SEARCH
Search Details
KOBORI YasuhiroMolecular Photoscience Research CenterProfessor
Researcher basic information
■ Research news- 24 Sep. 2019, Converting absorbed photons into twice as many excitons: successful high-efficiency energy conversion with organic monolayer on gold nanocluster surface
- 14 May 2018, Shedding light on a cyclic molecule with a twist
- 06 Apr. 2017, Mechanism behind the electric charges generated by photosynthesis -A step towards artificial photosynthesis
Research activity information
■ Award- Jul. 2023 ACS The Journal of Physical Chemistry Letters Poster Award, Time-Resolved EPR Study on Conformational Changes in Triplet-Triplet Dissociation and Annihilation after Intramolecular Singlet Fission
- Nov. 2022 神戸大学, 学長表彰(財務貢献者), 学長表彰(財務貢献者)財務貢献者
- Nov. 2021 神戸大学, 学長表彰, 財務貢献者財務貢献
- Sep. 2019 光化学協会, 第33回光化学協会賞, 電子スピン分極イメージング法の開発による光エネルギー変換機構の解明小堀康博氏は、植物光合成による光エネルギー変換過程の根源的な仕組みを理解し、超高効率な人工光合成や有機太陽電池に代表される光を入力としたエネルギー変換デバイスの設計指針を得ることを目的とし、時間分解電子スピン共鳴法を用い、I:常磁性サイト間の電子的相互作用メカニズム、II:光電荷分離および一重項励起子分裂による中間体の電子状態、立体構造および運動性を明らかにする実験的手法を確立した。結晶生成が困難であるにもかかわらず、次世代のクリーンエネルギー創出に向け分子機構の解明が必要な様々な反応系で、反応初期過程の仕組みをオングストローム領域の三次元映像化によって明らかにする画期的な実験的方法論を開発した。1) 植物PSIIタンパク質や太陽電池において生成する初期電荷分離状態の不対電子軌道を特定し、2) 中間体分子の距離および位置と分子配向を高い空間分解能にて画像化し、3)不対電子軌道間の重なり、トラップ深さと運動性を特徴付けた。高等植物が光合成による水分解を可能にした初期電荷分離過程における分子論的進化の仕組みが初めて明らかとなった。さらに一重項分裂による多重励起子生成機構の解明を行った。連結二量体の一重項分裂で生成する強相関五重項多重励起子生成の置換位置依存性を見いだし、スピン変換による再結合抑制効果を示した。種々の系で強相関五重項生成過程を調べ、励起子拡散のエントロピー効果によるスピン副準位選択性と多重励起子立体配向を世界に先駆け示すと共に、分子内多重励起子量子ダイナミクスの分子運動効果を特徴づけた。これらの業績は、光化学協会賞に値するものとして認められた。
- Sep. 2019 分子科学会, 第4回分子科学国際学術賞, 電子スピン分極イメージング法による光エネルギー変換機構の解明分子科学研究分野において量ではなく質的に優れた研究業績をあげ、国際的に高く評価されている研究者として高い水準の研究業績をあげ、国を超える分子科学の発展に大きな貢献を果たした功績が認められ、小堀教授が分子科学会{会員数1506名(2019年)}より第4回分子科学国際学術賞を授与されました。小堀教授は生体や太陽電池の様々な系で生成する励起子・電荷による光エネルギー変換機構の詳細を明らかにしました。次世代エネルギー源の分子設計に極めて重要な独創的成果を挙げたことが国際的にも評価され受賞につながりました。 2013年より本学理学研究科化学専攻教授に着任し、光合成タンパク質や太陽電池を対象とする励起子・光電荷分離構造解析と電子スピン分極イメージング法の開発を進めました。2017年に中間体分子の距離および位置と分子配向を高い空間分解能にて画像化し、さらに電子軌道の重なりや運動性を特徴付けたことにより、高等植物が光合成による水分解を可能にした初期電荷分離過程における分子論的進化の仕組みを示しました。さらに近年では、一重項励起子分裂による多重励起子生成機構の解明でも顕著な研究業績を次々と挙げています。これらは太陽電池の超高効率化に道を拓く多重励起子生成機構(DOI: doi.org/10.1073/pnas.1820932116他)や量子コンピューティングの先端領域(DOI:10.1021/jacs.8b13155他)で国際的に大きな影響を与えています。これらの成果は超高効率な人工光合成や有機太陽電池などの光エネルギー変換デバイスの開発に大きな契機をもたらすものです。
- Nov. 2017 電子スピンサイエンス学会, 第56回電子スピンサイエンス学会年会(SEST2017) 優秀ポスター賞2, アフリカツメガエル由来クリプトクロムに生成する光電荷分離状態の電子的相互作用
- Oct. 2017 化学フェスタ実行委員会, 最優秀ポスター発表賞(CSJ 化学フェスタ賞), 時間分解EPR 法による室温リン光発光性有機包接結晶の励起三重項状態の電子構造
- Sep. 2017 光化学協会, 2017年光化学討論会 優秀学生発表賞(ポスター)2, Time-Resolved EPR Study on Photoinduced Charge-Transfer Trap State in Thiophene-Thiazolothiazole Copolymer Film
- Nov. 2016 一般社団法人 電子スピンサイエンス学会, 第55回電子スピンサイエンス学会年会 優秀発表賞, 時間分解EPR 法による有機包接室温強リン光発光結晶の励起三重項状態の電子構造
- Sep. 2016 光化学協会, 2016年光化学討論会 優秀学生発表賞(ポスター発表), 時間分解電子スピン共鳴法によるチオフェンーチアゾロチアゾールコポリマー:PCBM有機薄膜における電荷分離状態の立体構造とダイナミクス
- Aug. 2016 Organizing Committee of Asia-Pacific EPR/ESR Symposium 2016, The 2016 APES AWARD for best talk among young scientists, Electronic Structure of the Excited Triplet State of Hexaphyrins with twisted Mobious Conformation as Studied by TR EPR
- Jun. 2016 AWEST2016, 2016 The International EPR (ESR) Society Poster Award, Time-domain EPR observations of changes in protein binding structures induced by the amyloid fibrillation of human insulin
- Nov. 2014 The Society of Electron Spin Science and Technology (SEST), SEST Student Research Award of APES-IES-SEST2014, Time-resolved EPR study on the Electronic Structure of the Excited Triplet State of [26] and [28] Hexaphyrins
- Nov. 2014 International EPR/ESR Society, International EPR/ESR Society Poster Award of APES-IES-SEST2014, Time-resolved EPR study on the Electronic Structure of the Excited Triplet State of [26] and [28] Hexaphyrins
- Oct. 2014 International Meeting on Spins in Organic Semiconductors, Poster Award of 5th International Meeting on Spin in Organic Semiconductors, Morphology effect of the geometry of the photoinduced charge-separated states in RR-P3HT:PCBM blend films studied by time-resolved EPR
- May 2014 科学技術振興機構さきがけ「太陽光と光電変換機能」研究領域, 科学技術振興機構さきがけ「太陽光と光電変換機能」領域 総括賞, 第10回領域会議 発表
- Aug. 2009 公益信託分子科学研究奨励森野基金, 公益信託分子科学研究奨励森野基金研究助成, 時間分解磁気共鳴分光法を用いた人工光合成およびタンパク質の機能の解明
- Nov. 2006 電子スピンサイエンス学会, 電子スピンサイエンス学会奨励賞, 光電荷分離状態の電子スピン間相互作用機構の解明
- Abstract Photon upconversion via triplet‐triplet annihilation (TTA‐UC) is a well‐known process that converts low‐energy light into higher‐energy light. This process has attracted attention for its potential in various fields, including light‐emitting devices, power generation and medical applications. It is desirable to develop TTA‐UC materials of TTA emitters with large TTA rate constants (kTTA). However, molecular design to accelerate the bimolecular rate constant of kTTA has not been considered. We present a strategy to manipulate kTTA by assembling multiple chromophores linked to a boron in a rotationally symmetric manner, causing asymmetric motions by a localized triplet exciton. We have studied tri(9‐anthryl)borane, which consists of three anthracenes linked via boron, as a TTA emitter. Time‐resolved luminescence measurements confirmed that kTTA is improved compared to the conventional TTA‐UC system using DPA, an anthracene‐based monomer. Time‐resolved electron paramagnetic resonance measurements showed that the improvement in kTTA is due to fast intramolecular triplet exciton hopping coupled with vibrational motions in the trimer molecule, which extends the reactivity at the collision distance between the excitons through the pseudo‐rotational motions. This molecular design that enhances TTA reactivity is expected to contribute to the future development of TTA‐UC materials for sensing fluid environment.Wiley, Jun. 2025, Angewandte Chemie International Edition, e202503846
- The effect of nonplanarity on the electronic properties of π-systems has been difficult to study systematically because of the limited availability of suitable model compounds. Our group recently synthesized a series of end-to-end bent perylene bisimide (PBI) cyclophanes, whose degree of bending is adjustable by modifying the internal alkyl tethers. Herein, we subjected these bent PBI derivatives to theoretical calculations and time-resolved spectroscopy. The current study has offered rational explanations for several unique photophysical characteristics of bent PBIs: (1) the redshifts of the S0–S1 transitions, (2) the decrease in extinction coefficients, (3) the broadening of spectral shapes, and (4) the suppression of nonradiative decay processes. Furthermore, the investigation of the S1 states and radical anions has revealed that structural bending also substantially alters the energy levels of upper molecular orbitals such as LUMO+2.AIP Publishing, Mar. 2025, The Journal of Chemical Physics, 162(11) (11)
- Elsevier BV, Mar. 2025, Journal of Magnetic Resonance Open, 22, 100181 - 100181
- Carbazol-3-olate photosensitizers with long-wavelength absorption and strong reducing ability have been developed.Royal Society of Chemistry (RSC), Mar. 2025, Organic Chemistry Frontiers
- Feb. 2025, Journal of Chemical Physics, 162(5) (5), 054505-1 - 054505-10
- American Chemical Society (ACS), Jan. 2025, Journal of the American Chemical Society, 147(5) (5), 4365 - 4374
- The advancement of an effective hydrogen liberation tech-nology from liquid organic hydrogen carriers (LOHCs), such as cyclohexane and methylcyclohexane (MCH), holds significance in realizing a hydrogen-centric society. However, the attainment of homogeneous catalytic acceptorless dehydrogenation (CAD) characterized by elevated selectivity for thorough aromatization under mild conditions remains unrealized. In this study, a catalyst system, facilitated by a double hydrogen atom transfer (HAT) processes, has been devised for the CAD of inert cycloalkanes at ambient temperature under visible light irradiation. Through the synergistic utilization of tetrabutylammonium chloride (TBACl) and thiophosphoric acid (TPA) HAT catalysts, successful CAD with comprehensive aromatization has been accomplished with high functional group tolerance.Springer Science and Business Media LLC, Jan. 2025, Nature Communications, 16(1) (1)
- American Chemical Society (ACS), Nov. 2024, ACS Sustainable Chemistry & Engineering, 12(47) (47), 17328 - 17335
- American Chemical Society (ACS), Sep. 2024, Journal of the American Chemical Society, 146(37) (37), 25527 - 25535
- The development of nonfullerene acceptors (NFAs), represented by ITIC, has contributed to improving the power conversion efficiency (PCE) of organic solar cells (OSCs). Although tuning the electronic structures to reduce the exciton binding energy (Eb) is considered to promote photocharge generation, a rational molecular design for NFAs has not been established. In this study, we designed and developed two ITIC-based NFAs bearing spiro-substituted bithiophene or biphenyl units (named SpiroT-DCI and SpiroF-DCI) to tune the frontier molecular orbital (FMO) distribution of NFAs. While the highest occupied molecular orbitals (HOMOs) of SpiroF-DCI and ITIC are delocalized in the main π-conjugated framework, the HOMO of SpiroT-DCI is distributed on the bithiophene unit. Reflecting this difference, SpiroT-DCI exhibits a smaller Eb than either SpiroF-DCI or ITIC, and exhibits greater external quantum efficiency in single-component OSCs. Furthermore, SpiroT-DCI shows improved PCEs for bulk-heterojunction OSCs with a donor of PBDB-T, compared with that of either SpiroT-DCI or ITIC. Time-resolved spectroscopy measurements show that the photo-induced intermolecular charge separation is effective even in pristine SpiroT-DCI films. This study highlights the introduction of spiro-substituted bithiophene units that are effective in tuning the FMOs of ITIC, which is desirable for reducing the Eb and improving the PCE in OSCs.Aug. 2024, Angewandte Chemie (International ed. in English), e202412691
- American Chemical Society (ACS), May 2024, Journal of the American Chemical Society
- American Chemical Society (ACS), Mar. 2024, The Journal of Physical Chemistry Letters, 15(11) (11), 2966 - 2975
- A series of ferrocene (Fc)-bridged pentacene (Pc)-dimers [Fc-Ph(2,n)-(Pc)2: n shows the number of phenylene spacers] were synthesized to examine the tortional motion effect of Fc-terminated phenylene linkers on the strongly coupled quintet multiexciton (5TT) formation through intramolecular singlet fission (ISF). Fc-Ph(2,4)-(Pc)2 has the relatively small electronic coupling and large conformational flexibility according to spectroscopic and theoretical analyses. Fc-Ph(2,4)-(Pc)2 exhibits high-yield 5TT together with quantitative singlet TT (1TT) generation through ISF. This demonstrates much more efficient ISF than those of the other less flexible Pc-dimers. The activation entropy in 1TT spin conversion of Fc-Ph(2,4)-(Pc)2 is larger than those of the other systems due to the larger conformational flexibility, associated with the torsional motion of the linkers. The torsional motion of linkers in 1TT is attributable to weakened metal-ligand bonding in the Fc due to hybridization of hole level of Pc to Fc in 1TT unpaired orbitals.Jan. 2024, Angewandte Chemie (International ed. in English), 63(8) (8), e202315747
- Singlet fission (SF) can generate an exchange-coupled quintet triplet pair state 5TT, which could lead to the realization of quantum computing and quantum sensing using entangled multiple qubits even at room temperature. However, the observation of the quantum coherence of 5TT has been limited to cryogenic temperatures, and the fundamental question is what kind of material design will enable its room-temperature quantum coherence. Here we show that the quantum coherence of SF-derived 5TT in a chromophore-integrated metal-organic framework (MOF) can be over hundred nanoseconds at room temperature. The subtle motion of the chromophores in the MOF leads to the enough fluctuation of the exchange interaction necessary for 5TT generation, but at the same time does not cause severe 5TT decoherence. Furthermore, the phase and amplitude of quantum beating can be controlled by molecular motion, opening the way to room-temperature molecular quantum computing based on multiple quantum gate control.American Chemical Society (ACS), Jan. 2024, Science advances, 10(1) (1), eadi3147
- Neat ITIC films are found to facilitate charge transfer, dissociation, and free carrier formation without the need for donor layers. This process, driven by V-type molecular stacking, significantly boosts organic photovoltaic efficiency.Royal Society of Chemistry (RSC), 2024, Chemical Science, 15(32) (32), 12686 - 12694
- Polycyclic aromatic hydrocarbons (PAHs) are fragments of graphene that have attracted considerable attention as a new class of carbon-based materials. The functionalization of edge positions in PAHs is important to...Royal Society of Chemistry (RSC), 2024, Chemical Science, 15(27) (27), 10592 - 10599
- Invited for the cover of this issue are the groups of Kazuteru Usui and Satoru Karasawa at Showa Pharmaceutical University and Yasuhiro Kobori of Kobe University. The image depicts chirality control of helical compounds through cycles of photocleavage and recombination under sunlight with a "Jack and the Beanstalk" motif. Read the full text of the article at 10.1002/chem.202302413.Nov. 2023, Chemistry (Weinheim an der Bergstrasse, Germany), 29(62) (62), e202303311
- The biomimetic design of a transition metal complex based on the iron(iv)-oxo porphyrin π-cation radical species in cytochrome P450 enzymes has been studied extensively. Herein, we translate the functions of this iron(iv)-oxo porphyrin π-cation radical species to an α-ketoacyl phosphonium species comprised of non-metal atoms and utilize it as a light-activated oxygenation auxiliary for ortho-selective oxygenation of anilines. Visible light irradiation converts the α-ketoacyl phosphonium species to the excited state, which acts as a transiently generated oxidant. The intramolecular nature of the process ensures high regioselectivity and chemoselectivity. The auxiliary is easily removable. A one-pot protocol is also described.Oct. 2023, Chemical science, 14(38) (38), 10488 - 10493
- Increasing levels of CO2 in the atmosphere is a problem that must be urgently resolved if the rise in current global temperatures is to be slowed. Chemically reducing CO2 into compounds that are useful as energy sources and carbon-based materials could be helpful in this regard. However, for the CO2 reduction reaction (CO2RR) to be operational on a global scale, the catalyst system must: use only renewable energy, be built from abundantly available elements and not require high-energy reactants. Although light is an attractive renewable energy source, most existing CO2RR methods use electricity and many of the catalysts used are based on rare heavy metals. Here we present a transition-metal-free catalyst system that uses an organohydride catalyst based on benzimidazoline for the CO2RR that can be regenerated using a carbazole photosensitizer and visible light. The system is capable of producing formate with a turnover number exceeding 8,000 and generates no other reduced products (such as H2 and CO).Mar. 2023, Nature chemistry
- Recent remarkable developments on nonfullerene solar cells have reached a photoelectric conversion efficiency (PCE) of 18% by tuning the band energy levels in small molecular acceptors. In this regard, understanding the impact of small donor molecules on nonpolymer solar cells is essential. Here, we systematically investigated mechanisms of solar cell performance using diketopyrrolopyrrole (DPP)-tetrabenzoporphyrin (BP) conjugates of C4-DPP-H2BP and C4-DPP-ZnBP, where C4 represents the butyl group substituted at the DPP unit as small p-type molecules, while an acceptor of [6,6]-phenyl-C61-buthylic acid methyl ester is employed. We clarified the microscopic origins of the photocarrier caused by phonon-assisted one-dimensional (1D) electron-hole dissociations at the donor-acceptor interface. Using a time-resolved electron paramagnetic resonance, we have characterized controlled charge-recombination by manipulating disorders in π-π donor stacking. This ensures carrier transport through stacking molecular conformations to suppress nonradiative voltage loss capturing specific interfacial radical pairs separated by 1.8 nm in bulk-heterojunction solar cells. We show that, while disordered lattice motions by the π-π stackings via zinc ligation are essential to enhance the entropy for charge dissociations at the interface, too much ordered crystallinity causes the backscattering phonon to reduce the open-circuit voltage by geminate charge-recombination.Mar. 2023, ACS physical chemistry Au, 3(2) (2), 207 - 221
- Elsevier BV, Mar. 2023, Journal of Photochemistry and Photobiology A: Chemistry, 437, 114479 - 114479
- Abstract Singlet fission (SF), converting a singlet excited state into a spin-correlated triplet-pair state, is an effective way to generate a spin quintet state in organic materials. Although its application to photovoltaics as an exciton multiplier has been extensively studied, the use of its unique spin degree of freedom has been largely unexplored. Here, we demonstrate that the spin polarization of the quintet multiexcitons generated by SF improves the sensitivity of magnetic resonance of water molecules through dynamic nuclear polarization (DNP). We form supramolecular assemblies of a few pentacene chromophores and use SF-born quintet spins to achieve DNP of water-glycerol, the most basic biological matrix, as evidenced by the dependence of nuclear polarization enhancement on magnetic field and microwave power. Our demonstration opens a use of SF as a polarized spin generator in bio-quantum technology.Springer Science and Business Media LLC, Mar. 2023, Nature Communications, 14(1) (1), 1056
- Wiley, Jan. 2023, Angewandte Chemie International Edition, 62(8) (8), e202217704
- Abstract Singlet oxygen (1O2), one of the most sought-after species in oxidative chemical reactions and photodynamic cancer therapy, is activated and neutralized in the atmosphere and living cells. It is essential to see "when" and "where" 1O2 is produced and delivered to understand and utilize it. There is an increasing demand for molecular sensor tools to capture, store, and supply 1O2, controlled by light and engineered singlet and triplet states, indicating the 1O2-capturing-releasing state. Here, we demonstrate the outstanding potential of an aminocoumarin-methylanthracene-based electron donor–acceptor molecule (1). Spectroscopic measurements confirm the formation of an endoperoxide (1-O2) which is not strongly fluorescent and remarkably different from previously reported 1O2 sensor molecules. Moreover, the photoexcitation on the dye in 1-O2 triggers fluorescence enhancement by the oxidative rearrangement and a competing 1O2 release. The unique ability of 1 will pave the way for the spatially and temporally controlled utilization of 1O2 in various areas such as chemical reactions and phototherapies.Springer Science and Business Media LLC, Dec. 2022, Scientific Reports, 12(1) (1), 11371
- American Chemical Society ({ACS}), Nov. 2022, ACS Omega, 7(44) (44), 40364 - 40373
- Springer Science and Business Media LLC, Jul. 2022, Photochemical and Photobiological Sciences, 21, 1781 - 1791
- American Chemical Society ({ACS}), Jun. 2022, Langmuir, 38, 1781 - 1791
- Non-fused electron-accepting π-conjugated compounds have been investigated recently for application to nonfullerene acceptors (NFAs) in organic solar cells (OSCs).Royal Society of Chemistry (RSC), Jun. 2022, Journal of Materials Chemistry A, 10(37) (37), 20035 - 20047
- We developed organocatalyst systems to promote the cleavage of stable C-H bonds, such as formyl, α-hydroxy, and benzylic C-H bonds, through a hydrogen atom transfer (HAT) process without the use of exogenous photosensitizers. An electronically tuned thiophosphoric acid, 7,7'-OMe-TPA, was assembled with substrate or co-catalyst N-heteroaromatics through hydrogen bonding and π-π interactions to form electron donor-acceptor (EDA) complexes. Photoirradiation of the EDA complex induced stepwise, sequential single-electron transfer (SET) processes to generate a HAT-active thiyl radical. The first SET was from the electron-rich naphthyl group of 7,7'-OMe-TPA to the protonated N-heteroaromatics and the second proton-coupled SET (PCET) from the thiophosphoric acid moiety of 7,7'-OMe-TPA to the resulting naphthyl radical cation. Spectroscopic studies and theoretical calculations characterized the stepwise SET process mediated by short-lived intermediates. This organocatalytic HAT system was applied to four different carbon-hydrogen (C-H) functionalization reactions, hydroxyalkylation and alkylation of N-heteroaromatics, acceptorless dehydrogenation of alcohols, and benzylation of imines, with high functional group tolerance.Mar. 2022, J. Am. Chem. Soc., 144(14) (14), 6566 - 6574
- American Chemical Society (ACS), Dec. 2021, ACS Energy Letters, 7(1) (1), 390 - 400
- Dec. 2021, Communications Materials, 2(1) (1)
- Springer Science and Business Media LLC, Dec. 2021, Communications Chemistry, 4(1) (1)
Abstract In the biological magnetic compass, blue-light photoreceptor protein of cryptochrome is thought to conduct the sensing of the Earth’s magnetic field by photoinduced sequential long-range charge-separation (CS) through a cascade of tryptophan residues, WA(H), WB(H) and WC(H). Mechanism of generating the weak-field sensitive radical pair (RP) is poorly understood because geometries, electronic couplings and their modulations by molecular motion have not been investigated in the secondary CS states generated prior to the terminal RP states. In this study, water dynamics control of the electronic coupling is revealed to be a key concept for sensing the direction of weak magnetic field. Geometry and exchange coupling (singlet–triplet energy gap: 2J ) of photoinducedsecondary CS states composed of flavin adenine dinucleotide radical anion (FAD−•) and radical cation WB(H)+• in the cryptochrome DASH fromXenopus laevis were clarified by time-resolved electron paramagnetic resonance. We found a time-dependent energetic disorder in 2J and was interpreted by a trap CS state capturing one reorientated water molecule at 120 K. Enhanced electron-tunneling by water-libration was revealed for the terminal charge-separation event at elevated temperature. This highlights importance of optimizing the electronic coupling for regulation of the anisotropic RP yield on the possible magnetic compass senses. - American Chemical Society (ACS), Aug. 2021, The Journal of Physical Chemistry C, 125(33) (33), 18287 - 18296
- American Chemical Society (ACS), Jul. 2021, Accounts of Materials Research, 2(7) (7), 501 - 514
- Hexacene (Hc) is highly promising for singlet fission (SF). However, the number of SFs in Hc is extremely limited. As far as Hc dimers in solution are concerned, there is no report on the observation of the dissociation process from a correlated triplet pair (TT) to an individual one. The emphasis in this study is on the first observation of the quantitative TT generation together with the orientation-dependent photophysical discussions for TT dissociation using para- and meta-phenyl-bridged Hc dimers. Moreover, the activation enthalpies of Hc dimers in TT dissociation are smaller than those of pentacene (Pc) dimers, whereas the relative entropic contributions for Gibbs free energy of activation are much larger than the enthalpic ones in both Hc and Pc dimers. This implies that the vibrational motions are responsible for the intramolecular conformation changes associated with the TT dissociation. Consequently, "enthalpy-entropy compensation" has a large impact on the rate constants and quantum yields.Jul. 2021, The journal of physical chemistry letters, 12(28) (28), 6457 - 6463
- This paper reports on durable and nearly temperature-independent (at 298-328 K) T-type photochromism of colloidal Cu-doped ZnS nanocrystals (NCs). The color of Cu-doped ZnS NC powder changes from pale yellow to dark gray by UV light irradiation, and the color changes back to pale yellow on a time scale of several tens of seconds to minutes after stopping the light irradiation, while the decoloration reaction is accelerated to submillisecond in solutions. This decoloration reaction is much faster than those of conventional inorganic photochromic materials. The origin of the reversible photoinduced coloration is revealed to be a strong optical transition involving a delocalized surface hole which survives over a minute after escaping from intraparticle carrier recombination due to electron-hopping dissociation. ZnS NCs can be easily prepared in a water-mediated one-pot synthesis and are less toxic. Therefore, they are promising for large-scale photochromic applications such as windows and building materials in addition to conventional photochromic applications. Moreover, the present study demonstrates the importance of excited carrier dynamics and trap depths, resulting in coloration over minutes not only for photochromic nanomaterials but also for various advanced photofunctional materials, such as long persistent luminescent materials and photocatalytic nanomaterials.American Chemical Society (ACS), Feb. 2021, Journal of the American Chemical Society, 143(5) (5), 2239 - 2249
- Importance of vibronic effects has been highlighted for the singlet-fission (SF) that converts one high-energy singlet exciton into doubled triplet excitons, as strongly coupled multiexcitons. However, molecular mechanisms of spin conversion processes and ultimate decouplings in the multiexcitons are poorly understood. We have analyzed geometries and exchange couplings (singlet-quintet energy gaps: 6J) of the photoinduced multiexcitons in the pentacene dimers bridged by a phenylene at ortho and meta positions [denoted as o-(Pc)2 and m-(Pc)2] by simulations of the time-resolved electron paramagnetic resonance spectra. We clarified that terahertz molecular conformation dynamics play roles on the spin conversion from the singlet strongly coupled multiexcitons 1(TT) to the quintet multiexcitons 5(TT) and on the intramolecular decouplings in the 6J to form spin correlated triplet pairs (T+T). The strongly coupled 5(TT) multiexcitons are revealed to possess entirely planar conformations stabilized by mutually delocalized spin distributions, while the intramolecular decoupled spin-correlated triplet pairs generated at 1 μs are also stabilized by distorted conformations resulting in two separately localized biradical characters.Oct. 2020, The journal of physical chemistry. B, 124(42) (42), 9411 - 9419
- American Chemical Society (ACS), Oct. 2020, The Journal of Physical Chemistry C, 124(39) (39), 21502 - 21511
- Photostimulated luminescence, which allows energy or data to be stored and released using electromagnetic waves as both the input and output, has attracted considerable interest in the fields of biomedical and informatics technologies, but this phenomenon is mostly limited to solid inorganic materials. Here, we report photostimulated luminescence from purely organic blend films composed of electron donor, acceptor, and trap/emitter molecules. In the films, charges are accumulated as radical ions by ultraviolet light irradiation and then extracted by near infrared light irradiation to produce visible light. Films are capable of multiple cycles (>10 times) of organic photostimulated luminescence, which was still observable from films left in the dark at room temperature for one week after excitation, and emission color could be varied by changing the trap/emitter molecules. These findings will broadly impact existing applications and provide new prospects for innovative flexible devices.American Chemical Society (ACS), Sep. 2020
- Feb. 2020, Nanoscale, 12, 6420 - 6428TiO2 superstructures with oriented nanospaces: a strategy for efficient and selective photocatalysis
- Singlet fission (SF) is expected to exceed the Shockley-Queisser theoretical limit of efficiency of organic solar cells. Transport of spin-entanglement in the triplet-triplet pair state via one singlet exciton is a promising phenomenon for several energy conversion applications including quantum information science. However, direct observation of electron spin polarization by transport of entangled spin-states has not been presented. In this study, time-resolved electron paramagnetic resonance has been utilized to observe the transportation of singlet and quintet characters generating correlated triplet-triplet (T + T) exciton-pair states by probing the electron spin polarization (ESP) generated in thin films of 6,13-bis(triisopropylsilylethynyl)pentacene. We have clearly demonstrated that the ESP detected at the resonance field positions of individual triplet excitons is dependent on the morphology and on the detection delay time after laser flash to cause SF. ESP was clearly explained by quantum superposition of singlet-triplet-quintet wavefunctions via picosecond triplet-exciton dissociation as the electron spin polarization transfer from strongly exchange-coupled singlet and quintet TT states to weakly-coupled spin-correlated triplet pair states. Although the coherent superposition of spin eigenstates was not directly detected, the present interpretation of the spin correlation of the separated T + T exciton pair may pave new avenues not only for elucidating the vibronic role in the de-coupling between two excitons but also for scalable quantum information processing using quick T + T dissociation via one-photon excitation.Feb. 2020, Chemical Science, 11(11) (11), 2934 - 2942
- Lipid bilayer membranes are known to exist as heterogeneous and dynamic structures where the molecules are always moving and fluctuating under physiological conditions. Magnetic field effects (MFEs) studied herein are phenomena in which the exciplex emission from an electron donor-acceptor dyad increases or decreases by applying an external magnetic field. The characteristic dependence of MFEs on the viscosity and polarity of the surrounding medium has been applied to investigate the local environments around the probe molecule. In this study, a novel MFE-based fluorescence microscopy technique was developed to explore the structural dynamics of lipid bilayer membranes. The vesicle formation during the membrane deformation was selectively visualized through the MFEs, thus allowing the extraction of information on the cellular dynamics at high temporal and spatial resolutions. This highly versatile and powerful technique is applicable to a wide range of areas, such as biology and material science.Dec. 2019, The journal of physical chemistry. B, 123(50) (50), 10896 - 10902
- Dec. 2019, Electrostatic Interaction with Anionic Polymer Activates Berberine, 40, 4 - 7Electrostatic Interaction with Anionic Polymer Activates Berberine
- Sep. 2019, J. Am. Chem. Soc., 141(37) (37), 14720 - 14727
- Aug. 2019, Journal of Physical Chemistry C, 123(31) (31), 18813 - 18823
- Aug. 2019, Photomedicine and Photobiology, 40, 7 - 10Photosensitizing Activity of Berberine-Cyclodextrin Inclusion Complexes
- Jun. 2019, JOURNAL OF PHYSICAL CHEMISTRY C, 123(22) (22), 13472 - 13481
- May 2019, JOURNAL OF PHYSICAL CHEMISTRY C, 123(20) (20), 12592 - 12598
- American Chemical Society ({ACS}), Mar. 2019
- Mechanistic Insights into Photochemical Reactions on CH3NH3PbBr3 Perovskite Nanoparticles from Single-Particle Photoluminescence SpectroscopyMetal halide perovskites have attracted considerable attention in applications such as photovoltaic cells and light-emitting diodes. The performance and durability of perovskite devices are significantly dependent on the nature of structural defects, but the underlying mechanisms of structure-related photochemical reactions are not yet fully elucidated. This study demonstrates that the photoluminescence (PL) from individual perovskite nanoparticles (NPs) can be utilized to resolve the different trapping pathways of the photogenerated charges, and hence, obtain a correlation between the pathways. PL deactivation and activation were observed and mainly attributed to nonradiative Auger recombination by the trapped charges and the passivation of surface traps by oxygen, respectively. Single-particle spectroelectrochemical techniques were further employed to explore the possible origin of the effective charge trap states and the reversibility of redox events under electrical bias. Consequently, this study unravels the complex effects of the structural defects on the charge carrier dynamics in perovskites.Wiley‐VCH Verlag, Mar. 2019, ChemNanoMat, 5(3) (3), 340 - 345
- American Chemical Society (ACS), Nov. 2018, ACS Energy Lett., 2019((4)) ((4)), 26 - 31
- Partial halide substitution in organolead halide perovskites MAPbX3 (MA = CH3NH3+, X = Cl-, Br-, or I-) leads to semiconductor heterostructures with precisely tuned band-gap energies, which facilitates efficient charge extraction or separation for high-performance solar cells and optoelectronic devices. In this study, partially iodide-substituted MAPbBr3 perovskites were prepared through a halide-exchange reaction in the liquid phase, and in situ space- and time-resolved photoluminescence profiles were acquired by means of confocal microscopy. The rates of charge transfer from the bulk MAPbBr3 to the surface MAPbBr3- xI x domains, which are widely distributed over a single crystal, were found to greatly depend on the excitation-power density. In particular, an abnormally slow charge-transfer process, lasting a few nanoseconds, was observed at higher excitation density. To explain the dependence of this rate on the excitation density, and its correlation with the charge-trapping rate in the bulk MAPbBr3, we propose a plausible mechanism in which trap filling associated with surface-trapped holes induces band bending within the space charge region. This band bending modulates carrier dynamics near the surface, thereby leading to efficient charge extraction from the bulk. To validate the mechanism, the carrier dynamics was numerically simulated using a diffusion model that includes the effect of the localized electric field. Our findings provide significantly deeper insight into the carrier dynamics within heterostructured perovskites with nanoscale heterogeneities, and a robust route for manipulating the photogenerated charges in various types of perovskite devices.Oct. 2018, ACS applied materials & interfaces, 10(43) (43), 37057 - 37066
- Sep. 2018, The Journal of Physical Chemistry Letters, 9(19) (19), 5855–5861Singlet-Fission-Born Quintet State: Sublevel Selections and Trapping by Multiexciton Thermodynamics
- American Chemical Society, Jun. 2018, Journal of Physical Chemistry Letters, 9(12) (12), 3354 - 3360
- Möbius aromatic molecules have attracted great attention as new functional materials because of their π-orbital cyclic conjugations lying along the twisted Möbius topology. To elucidate the electronic character of the lowest excited triplet (T1) state of a Möbius aromatic [28]hexaphyrin, we employed a time-resolved electron paramagnetic resonance (TREPR) method with applied magnetophotoselection measurements at 77 K. Analyses of the EPR parameters have revealed that the T1 state possesses intramolecular charge-transfer (CT) character together with local excitation character residing at one side in the Möbius strip ring. We have also demonstrated that the CT character between orthogonal unpaired orbitals triggers quick triplet deactivation by spin-orbit coupling. This deactivation can be an important barometer to represent the "antiaromaticity" because of a connection between the orthogonal CT character and instability by a weakened spin-spin exchange coupling in the T1 state.May 2018, The journal of physical chemistry letters, 9(10) (10), 2685 - 2690
- 2018, J. Org. Chem., 83, 9381 - 9390UVA- and visible light-mediated generation of carbon radicals from organochlorides using non-metal photocatalyst
- Building efficient triplet-harvesting layers for photovoltaic applications requires a deep understanding of the microscopic properties of the components involved and their dynamics. Singlet fission is a particularly appealing mechanism as it generates two excitons from a single photon. However, the pathways of the coupled triplets into free species, and their dependence on the intermolecular geometry, has not been fully explored. In this work, we produce highly ordered dilute pentacene films with distinct parallel and herringbone dimers and aggregates. Using electron paramagnetic resonance spectroscopy, we provide compelling evidence for the formation of distinct quintet excitons in ambient conditions, with intrinsically distinctive electronic and kinetic properties. We find that the ability of quintets to separate into free triplets is promoted in the parallel dimers and this provides molecular design rules to control the triplets, favouring either enhanced photovoltaic efficiency (parallel) or strongly bound pairs that could be exploited for logic applications (herringbone).2018, Nature Communications, 9(1) (1), 4222 - 4222
- Jan. 2018, arXiv:1801.00603Multiple Quintets via Singlet Fission in Ordered Films at Room Temperature
- 2018, JOURNAL OF PHOTOPOLYMER SCIENCE AND TECHNOLOGY, 31(2) (2), 163 - 167
- Organolead halide perovskites MAPbX3 (MA = CH3NH3+, X = Cl-, Br-, or I-) are known to undergo reversible halide exchange reactions, enabling bandgap tuning over the visible light region. Using single-particle photoluminescence (PL) imaging for in situ observation, we have studied the structure-dependent charge dynamics during halide exchange with iodide ions on an MAPbBr3 crystal. In particular, we optically detected nanometer-scale iodide-rich domains (i.e., MAPbBrI2) and found that their lifetimes of several tens of milliseconds are limited by reaction with diffusing vacancies. Furthermore, it was discovered that these domains effectively collect the charge carriers from the bulk crystal, thus resulting in amplified spontaneous emission (ASE) under continuous-wave laser irradiation. Our findings will provide direction for development of perovskite heterostructures with enhanced charge utilization.Mar. 2017, Journal of Physical Chemistry Letters, 8(8) (8), 1724 - 1728
- In initial events of the photosynthesis by higher plants, the photosystem II (PSII) generates photoinduced primary charge-separated (CS) state composed of reduced pheophytin (PheoD1-•) and oxidized special pair (P+•) in chlorophyll a (Chla) PD1/PD2 in the D1/D2 heterodimer, ultimately leading to the water oxidation at the oxygen-evolving Mn4CaO5 cluster by P+•. To understand the mechanism of the efficient generation of initially localized CS state (PD1+• PheoD1-•), we have characterized cofactor geometries and electronic coupling of the photoinduced primary CS state in quinone prereduced membrane of PSII from spinach using the time-resolved electron paramagnetic resonance method. It has been revealed that the electronic coupling between the charges is significantly weak in the CS state separated by 1.5 nm, showing the importance of regulated cofactor-cofactor electronic interaction between a vinyl substituent in PheoD1 and an accessory chlorophyll to inhibit the energy-wasting charge recombination after the primary electron-transfer processes.Feb. 2017, The Journal of Physical Chemistry Letters, 8(6) (6), 1179 - 1184
- 2017, RSC ADVANCES, 7(5) (5), 2403 - 2406
- Wiley-VCH Verlag, 2017, Angewandte Chemie - International Edition, 56(19) (19), 5299 - 5303
- 2017, JOURNAL OF PHOTOPOLYMER SCIENCE AND TECHNOLOGY, 30(5) (5), 551 - 555
- Sep. 2016, JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 138(38) (38), 12564 - 12577
- Jul. 2016, CHEMISTRY-AN ASIAN JOURNAL, 11(14) (14), 2006 - 2010
- American Chemical Society, May 2016, Journal of Physical Chemistry B, 120(19) (19), 4365 - 4372
- May 2016, JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 138(18) (18), 5879 - 5885
- Feb. 2016, ACS Catal., 6(4) (4), 2250 - 2256Crystal-Face-Dependent Charge Dynamics on a BiVO4 Photocatalyst Revealed by Single-Particle Spectroelectrochemistry
- Jan. 2016, ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 55(2) (2), 629 - 633
- 2016, JOURNAL OF PHOTOPOLYMER SCIENCE AND TECHNOLOGY, 29(4) (4), 561 - 564
- Aug. 2015, JOURNAL OF PHYSICAL CHEMISTRY LETTERS, 6(16) (16), 3195 - 3201
- Apr. 2015, JOURNAL OF PHYSICAL CHEMISTRY C, 119(15) (15), 8078 - 8088
- Jan. 2015, JOURNAL OF PHYSICAL CHEMISTRY LETTERS, 6(1) (1), 113 - 123
- Time-resolved electron paramagnetic resonance (TREPR) spectroscopy has been utilized at T = 77 K to characterize geometries and electronic couplings (VCR) of transient charge-separated (CS) states in photoactive layers in organic thin film solar cells fabricated by spin-coating of mixed solutions of polyalkylthiophenes (RR-P3AT) and [6, 6]-C61-butyric acid methyl ester (PCBM). Electron-hole distance of the interfacial transient CS states has been revealed to be modulated by alkyl side-chain number in P3AT. This result is explained by a coupling of a hole dissociation to polymer librations by the side-chains. From an exponential decay of VCR with respect to the CS distance, an attenuation factor (βe) of the decay has been determined to be βe=0.2 Å−1. Such a long-range tunneling feature is explained by generations of shallowly trapped, delocalized electron-hole pairs by the dissociations of the hole toward π-stacking directions at the organic photovoltaic interface.The Surface Science Society of Japan, Nov. 2014, e-J. Surf. Sci. Nanotech., 35(11) (11), 621 - 626
- Jan. 2014, JOURNAL OF PHYSICAL CHEMISTRY LETTERS, 5(1) (1), 30 - 35
- Jan. 2013, JOURNAL OF PHYSICAL CHEMISTRY C, 117(4) (4), 1589 - 1599
- Jul. 2012, Journal of the American Chemical Society, 134(27) (27), 11251 - 11260
- Oct. 2011, JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 133(42) (42), 16770 - 16773
- 2011, ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 50(29) (29), 6583 - 6586
- Nov. 2010, JOURNAL OF PHYSICAL CHEMISTRY B, 114(45) (45), 14621 - 14630
- Jan. 2010, APPLIED MAGNETIC RESONANCE, 37(1-4) (1-4), 177 - 189
- Jun. 2009, PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 106(26) (26), 10444 - 10448
- Feb. 2009, JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 131(5) (5), 1624 - +
- The Biophysical Society of Japan General Incorporated Association, 2009, Seibutsu Butsuri, 49, S10
- Jan. 2009, JOURNAL OF PHYSICAL CHEMISTRY A, 113(4) (4), 633 - 638
- Jan. 2006, JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 128(1) (1), 4 - 5
- Aug. 2005, JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 127(32) (32), 11220 - 11221
- Aug. 2005, ABSTRACTS OF PAPERS OF THE AMERICAN CHEMICAL SOCIETY, 230(25) (25), U2941 - U2941Primary charge-recombination in an artificial photosynthetic reaction center
- NATL ACAD SCIENCES, Jul. 2005, PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 102(29) (29), 10017 - 10022Primary charge-recombination in an artificial photosynthetic reaction center
- Jun. 2005, PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 102(25) (25), 8978 - 8983
- Nov. 2004, BULLETIN OF THE CHEMICAL SOCIETY OF JAPAN, 77(11) (11), 1997 - 2001
- Jul. 2004, JOURNAL OF PHYSICAL CHEMISTRY B, 108(29) (29), 10226 - 10240
- Feb. 2004, JOURNAL OF PHYSICAL CHEMISTRY A, 108(7) (7), 1120 - 1126
- 2004, J. Phys. Chem. B, 108(31) (31), 10709 - 11715Theoretical Study on Electronic and Solvent Reorganization Associated with a Charging Process of Organic Compounds. 2. A New Decomposition Procedure into Electrostatic and Nonelectrostatic Responses
- 2004, J. Phys. Chem. B, 108(31) (31), 10709 - 11715Superexchange Electron Tunneling Mediated by Solvent Molecules: Pulsed Electron Paramagnetic Resonance Study on Electronic Coupling in Solvent-Separated Radical Ion Pairs
- Jan. 2004, JOURNAL OF PHYSICAL CHEMISTRY A, 108(4) (4), 524 - 531
- 2004, APPLIED MAGNETIC RESONANCE, 26(1-2) (1-2), 145 - 154
- Dec. 2003, JOURNAL OF PHYSICAL CHEMISTRY B, 107(48) (48), 13255 - 13257
- Feb. 2003, CHEMICAL PHYSICS LETTERS, 369(1-2) (1-2), 49 - 54
- 2003, J. Chem. Phys., 119(5) (5), 2753 - 2760Theoretical Study of Electronic and Solvent Reorganization Associated with a Charging Process of Organic Compounds. I. Molecular and Atomic Level Description of Solvent Reorganization
- 2003, J. Am. Chem. Soc., 125(16) (16), 4722 - 4723Long-Range Jump versus Stepwise Hops: Magnetic Field Effects on the Charge-Transfer Fluorescence from Photoconductive Polymer Films
- 2003, APPLIED MAGNETIC RESONANCE, 23(3-4) (3-4), 269 - 287
- Oct. 2002, Journal of Physical Chemistry B, 106(39) (39), 10074 - 10081
- Oct. 2002, JOURNAL OF PHYSICAL CHEMISTRY B, 106(39) (39), 10074 - 10081
- Jul. 2002, CHEMICAL PHYSICS LETTERS, 360(1-2) (1-2), 13 - 21Spin dynamics and zero-field splitting constants of the triplet exciplex generated by photoinduced electron transfer reaction between erythrosin B and duroquinone
- May 2002, MOLECULAR PHYSICS, 100(9) (9), 1413 - 1420
- Oct. 2001, JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 123(39) (39), 9722 - 9723Determination of electron-transfer reorganization energy in nanometer-separated radical ion pair by time-resolved EPR spectroscopy
- 2001, J. Photochem. Photobiol. C, 2(1) (1), 17 - 33Spin-Orbit Coupling Induced Electron Polarization in Photoinduced Electron Transfer Reactions
- 2001, RESEARCH ON CHEMICAL INTERMEDIATES, 27(1-2) (1-2), 155 - 164Magnetic field effects on the triplet exciplex dynamics in the duroquinone-N, N-dimethylaniline derivative systems
- 2001, Mol. Phys., 100(8) (8), 1245 - 1259Magnetic Field and Spin Effects from Sequential p-Type and d-Type Triplet Mechanisms
- Jul. 2000, JOURNAL OF CHEMICAL PHYSICS, 113(2) (2), 465 - 468Theoretical analysis of singlet-triplet energy splitting generated by charge-transfer interaction in electron donor-acceptor radical pair systems
- Jul. 1999, JOURNAL OF PHYSICAL CHEMISTRY A, 103(28) (28), 5416 - 5424Chemically induced dynamic electron polarization study on the mechanism of exchange interaction in radical ion pairs generated by photoinduced electron transfer reactions
- Oct. 1998, JOURNAL OF PHYSICAL CHEMISTRY A, 102(42) (42), 8078 - 8083Intrinsic enhancement factors of the spin-orbit coupling mechanism polarization in the duroquinone-N,N-dimethylaniline derivative systems
- Jul. 1998, JOURNAL OF PHYSICAL CHEMISTRY A, 102(27) (27), 5160 - 5170Exchange interaction in radical-triplet pairs: Evidences for CIDEP generation by level crossings in triplet-doublet interactions
- Feb. 1998, JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 120(6) (6), 1325 - 1326Marcus free energy dependence of the sign of exchange interactions in radical ion pairs generated by photoinduced electron transfer reactions
- 1998, Proceedings of the Joint 29th AMPERE-13th ISMAR. International Conference on Magnetic Resonance and Related Phenomena, Berlin, vol. II, 929CIDEP Studies on the Signs of Exchange Interactions in Radical Ion Pairs Generated by Photoinduced Electron Transfer Reactions
- 1997, APPLIED MAGNETIC RESONANCE, 12(4) (4), 405 - 410CIDEP in radical-singlet molecular oxygen system
- Nov. 1996, CHEMICAL PHYSICS LETTERS, 262(1-2) (1-2), 125 - 130The first observation of CIDEP generated through the interaction between an excited singlet oxygen molecule and a free radical
- Jun. 1996, JOURNAL OF PHYSICAL CHEMISTRY, 100(24) (24), 10021 - 10026Time-resolved ESR studies on ketyl type radical-amine complexes
- Apr. 1996, CHEMICAL PHYSICS LETTERS, 252(5-6) (5-6), 355 - 361Absolute magnitude of spin polarization in the radical-triplet pair mechanism: CIDEP generation by level crossings in a triplet-doublet interaction
- Jun. 1994, JOURNAL OF PHYSICAL CHEMISTRY, 98(26) (26), 6425 - 6429DIRECT OBSERVATION OF CIDEP GENERATED THROUGH ENHANCED INTERSYSTEM CROSSING
- Nov. 1993, CHEMICAL PHYSICS LETTERS, 215(1-3) (1-3), 203 - 208TIME-RESOLVED ESR-SPECTRA OF THE ALPHA-HYDROXYBENZYL AMINE COMPLEX
- ニュー・サイエンス社, Mar. 2023, 細胞, 55(3) (3), 45 - 47光受容クリプトクロムによる磁気コンパス機構:タンパク質結合水のゆらぎの役割
- 北隆館, Mar. 2023, アグリバイオ, 7(4) (4), 77 - 80光受容クリプトクロムによる磁気コンパス機構:タンパク質結合水のゆらぎの役割
- 2022, 日本化学会春季年会講演予稿集(Web), 102ndDynamics of triplet exciton formed at the donor/acceptor interface of organic semiconductor photon upconversion materials by electron spin resonance
- 光化学協会誌誌, Dec. 2019, 光化学協会誌, 50(3) (3), 177 - 184Electron Spin Polarization Imaging Method Applied for Elucidating Photon-to-Energy Conversion Mechanism in Organic Thin Film Solar Cells
- 電子スピンサイエンス学会, Oct. 2017, 電子スピンサイエンス研究室訪問「神戸着任から新規な中間体磁気イメージング法の開発まで」
- 電子スピンサイエンス学会, Oct. 2016, 電子スピンサイエンス有機半導体界面の光電荷解離機構
- 光化学協会, Dec. 2012, 光化学協会誌「光化学」, 43(3) (3), 134 - 141タンパク質の光エネルギー変換機構:光電荷分離のダイナミクスと構造解析の最前線
- エヌ・ティー・エス, Mar. 2024, 83-93, ISBN: 9784860438821量子生命科学ハンドブック (瀬藤;光利;荒牧, 修平)
- 15.4 電子スピン共鳴スペクトル, 丸善出版(株), Mar. 2021化学便覧 基礎編 改訂6版
- 解説, 月刊「化学」(化学同人), Mar. 2020Roles of orbitals and molecular motions on the light-energy conversions studied by 3D visualization of electron spin polarization
- シーエムシー出版, Feb. 2016「電子スピンコヒーレンスによる有機太陽電池基板の電子伝達機能の解明」in: 「太陽光と光電変換機能-分野融合から生まれる次世代太陽電池-」
- 株式会社エヌ・ティー・エス, Dec. 2014「有機薄膜太陽電池の電子伝達機構:光合成反応中心との比較」光合成研究と産業応用最前線
- 丸善, Jul. 2013Translation of sections of 2.22-2.40 and of 3.12-3.27 in “Principle of Moderen Molecular Photochemistry: An Introduction” by N.J. Turro, V. Ramamurthy, J. C. Scaiano,
- 光技術コンタクト, Mar. 2012, 植物の光合成やDNAの修復など、さまざまな生命活動でタンパク質は、光を利用して電子伝達を行う中間体分子を効率よく生み出し、エネルギー生産へとつなぐ重要な役割を持つ。光エネルギー変換初期過程では、光の吸収によって電子軌道エネルギーが励起された生体分子が、その近傍の分子に電子あるいは正孔のどちらかを与える。このため生成する中間体分子は、軌道に収容される電子対の内の1つの電子が不足した状態(ラジカル)であり、磁性を持つ。ある励起分子が近傍の分子に電子1個を与えると、両分子が不対電子を持つ状態(電荷分離状態)になる。このような光電荷分離状態は不安定であり、電子あるいは正孔を戻して元の安定な状態に戻ろうとするはずであるが、これではエネルギー変換にはならない。生命が高い効率で光エネルギー変換を行うために、タンパク質は光照射直後に生成した中間体分子の位置や向きを巧タンパク質による光エネルギー変換機構:レーザー励起時間分解電子スピン共鳴法を用いた立体構造解析
- 日本化学会第105春季年会(2025), Mar. 2025時間分解EPR法を用いた分子内一重項励起子分裂の機構解析
- 日本化学会第105春季年会, Mar. 2025時間分解 EPR 法による脱炭酸光触媒の反応機構の解明
- 日本化学会第105回春季年会(2025), Mar. 2025Effect of molecular motion on electron spin polarization in the photo-excited chromophore radical systems of molecular spin-qubit candidates
- 日本化学会春季年会特別企画「エキシトン操作の新展開と展望」, Mar. 2025ノイズが生み出すコヒーレンス:高速分子運動による光エネルギー変換
- 13th IDyEx, Jan. 2025Conformation Dynamics of Molecular Spin Qubits by Exciton Pairs
- 12th International Symposium in Dynamic Exciton, Dec. 2024Exciton Spin Dynamics in Triplet Pairs
- 第63回電子スピンサイエンス学会年会, Nov. 2024時間分解 EPR 法による脱炭酸光触媒の反応機構の解明
- 第63回電子スピンサイエンス学会年会, Nov. 2024時間分解EPR法を用いたテトラセンオリゴマーにおける分子内一重項励起子分裂の機構解析
- 第63回電子スピンサイエンス学会年会, Nov. 2024Y構造非フラーレンアクセプターを用いた有機薄膜太陽電池の光電荷分離構造:時間分解EPR法とパルスEPR法による観測
- 18th International Symposium on Spin and Magnetic Field Effects in Chemistry and Related Phenomena, Sep. 2024Elucidation of Initial Charge Separation Structure in Y-series Non-Fullerene Acceptor Based Organic Thin Film Solar Cell by Time-Resolved EPR and Pulse EPR
- 18th International Symposium on Spin and Magnetic Field Effects in Chemistry and Related Phenomena, Sep. 2024Time-resolved EPR study of intramolecular exciton hopping contributing to triplet-triplet annihilation-based photon upconversion
- 2024年光化学討論会, Sep. 2024Transient EPR study of intramolecular exciton hopping contributing to triplet-triplet annihilation
- 2024年光化学討論会, Sep. 2024時間分解EPR法による脱炭酸光触媒の反応機構の解明
- 2024年 光化学討論会, Sep. 2024有機太陽電池の超長距離電荷分離:パルス電子スピン共鳴法による観測
- KJF-ICOMEF, Aug. 2024Vibronic Spin Effects on Singlet Fission in Linked Systems
- 24th International Conference on Photochemical Conversion and Storage of Solar Energy (IPS-24), Jul. 2024Molecular Vibronic Control of Exciton Pairs: Transient EPR Study
- 8th Japan-Czech-Slovakia (JCS) International Symposium on Theoretical Chemistry, Jul. 2024Photoinduced spin entanglement and decoherence in triplet pairs
- 7th QST International Symposium, Jul. 2024Quantum Biology Phenomena from the Spin-Anisotropic Effect
- ECS Meeting, May 2024Exciton Dynamics for Spin Qubits
- 57th RSC ESR Spectroscopy Group Meeting, Apr. 2024, University of Warwick, UKManipulating anisotropic conformation dynamics of exciton pairs: Transient and pulse EPR analyses
- 9th Kanto Spin Chemistry Meeting, Mar. 2024Spin conversion mechanism for efficient photon up-conversion in amorphous rubrene
- 9th Kanto Spin Chemistry Meeting, Mar. 2024Quantum decoherence in triplet-radical linked system
- 第2回DNP研究会, Mar. 2024ゆらぎによる励起子ペアのスピン偏極
- 日本化学会第104春季年会(2024), Mar. 2024パルスEPR法によるスピン相関三重項対のスピン量子コヒーレンス観測
- 日本化学会第104春季年会(2024), Mar. 2024時間分解電子スピン共鳴法とパルス電子スピン共鳴法による非フラーレン型有機薄膜太陽電池の界面電荷分離状態の解析
- The 9th International Symposium on Dynamic Exciton, Nov. 2023Molecular conformation dynamics effect in singlet-fissions
- The 8th International Symposium on Dynamic Exciton, Nov. 2023Spin-state dynamics and anisotropies in organic solar cells using transient EPR
- 第62回電子スピンサイエンス学会年会, Nov. 2023三重項ー三重項消滅を用いた光アップコンバージョンの時間分解EPR法による観測:分子内三重項励起子ホッピングの寄与
- 第62回電子スピンサイエンス学会年会, Nov. 2023非フラーレン型アクセプターを用いた有機薄膜太陽電池光活性層の初期電荷分離構造:時間分解EPR法による解析
- 第62回電子スピンサイエンス学会年会, Nov. 2023三重項-三重項消滅型光アップコンバータにおける励起子ダイナミクスの時間分解EPRによる解析
- 第62回電子スピンサイエンス学会年会, Nov. 2023フェロセンで連結したペンタセンダイマーにおける一重項分裂で生成する多重励起子
- 第62回電子スピンサイエンス学会, Nov. 2023熱活性化遅延蛍光に至る薄膜中三重項励起子の低振動運動:時間分解EPRによる観測
- 第73回錯体化学討論会, Sep. 2023Photoinduced spin entanglement and decoherence in functionality of complex molecular systems
- 第17回分子科学討論会2023, Sep. 2023分子内一重項励起子分裂に伴う構造変化と三重項消滅: 時間分解EPRと過渡吸収による解析
- 2023年光化学討論会, Sep. 2023Observation of photon upconversion by triplet-triplet annihilation using time-resolved EPR: Contribution of intramolecular triplet exciton rotation
- 2023年光化学討論会, Sep. 2023Elucidation of Initial Charge Separation Structure in ITIC-Based Organic Thin Film Solar Cell Studied by Time-Resolved EPR
- 2023年光化学討論会, Sep. 2023三重項-三重項消滅を用いた液体光アップコンバータに生成する電子スピン分極の時間発展
- 2023年光化学討論会, Sep. 2023フェロセンで連結したペンタセンダイマーにおける一重項分裂で生成する三重項励起子
- 2023年光化学討論会, Sep. 2023光エネルギー変換への鍵となる分子配向と低周波振動:時間分解EPRによる観測
- The 31st International Conference on Photochemistry, Jul. 2023Time-Resolved EPR Study on Conformational Changes in Triplet-Triplet Dissociation and Annihilation after Intramolecular Singlet Fission
- The 31st International Conference on Photochemistry, Jul. 2023Time-resolved EPR study of electron spin polarization in an efficient triplet-triplet annihilation upconversion system
- The 31st International Conference on Photochemistry, Jul. 2023Impact of Non-fullerene Acceptor Steric Structure on Photoinduced Charge-Separation in Bulkheterojunction Film Studied by Time-resolved EPR
- The 31st International Conference on Photochemistry, Jul. 2023Key conformation dynamics for light-induced energy conversions: Transient EPR study
- 高知化学シンポジウム2023, Jul. 2023有機薄膜太陽電池における電荷輸送機構への非フラーレンアクセプターの立体構造の効果
- 高知化学シンポジウム2023, Jul. 2023分子内一重項励起子分裂で生成する三重項励起子対の構造変化と三重項消滅 時間分解EPRと過渡吸収による解析
- ECS Meeting, May 2023Non-Polymer Organic Solar Cells: Microscopic Phonon Control to Suppress Non-Radiative Voltage Loss via Charge-Separated State
- Gordon Research Conference, Quantum Biology, Mar. 2023, Galveston, TXWater Dynamics Control of Charge Separation for Magnetoreception by Cryptochrome
- 日本化学会第103春季年会(2023), Mar. 2023, 東京理科大学電子スピン共鳴法を用いた液体光アップコンバータに生成する三重項励起子のダイナミクス解析
- 第61回電子スピンサイエンス学会, Dec. 2022, 熊本市民会館分子ゆらぎが起こす低分子有機太陽電池の電圧損失:時間分解 EPR 法による長距離電荷再結合機構
- 第61回電子スピンサイエンス学会年会, Dec. 2022, 熊本市民会館ESRによる非フラーレン型有機薄膜太陽電池における電荷輸送機構の解析
- 第61回電子スピンサイエンス学会年会, Dec. 2022, 熊本市民会館分子内一重項励起子分裂で生成する多重励起子の低温での構造変化とその機構:時間分解ESR法を用いた解析
- 第61回電子スピンサイエンス学会年会, Dec. 2022, 熊本市民会館9,10-ジフェニルアントラセンにおける三重項―三重項消滅過程の電子スピン分極
- 第61回電子スピンサイエンス学会年会, Dec. 2022, 熊本市民会館テトラセン分子ワイヤーにおける一重項分裂で生成した多重励起子と解離状態
- Asia Pacific EPR/ESR Symposium, Nov. 2022, Web上での発表Spin-Entanglement Transport during Singlet Fissions
- Spin Chemistry Meeting, Sep. 2022, Northwestern Univ. Evanston, ILConformation Change of Exciton Pairs: Spin-Entanglement Transport during Singlet Fissions Studied by Time-Resolved EPR
- 光化学討論会2022, Sep. 2022, 京都大学桂キャンパスNon-Fullerene Organic Photovoltaic: Effect of Introducing Spirofluorene Substituent to Acceptor on the Photoinduced Charge Separation Structure
- 光化学討論会2022, Sep. 2022, 京都大学桂キャンパス分子内一重項励起子分裂で生成する多重励起子の低温領域での構造変化:時間分解EPR法による解析
- 光化学討論会2022, Sep. 2022Spin Dynamics of Triplet-Triplet Annihilation in a Photon Upconversion System Using 9,10-diphenylanthracene
- 2022年光化学討論会, Sep. 2022, 京都大学桂キャンパステトラセン分子ワイヤーにおける一重項分裂で生成した三重項状態
- 光化学討論会2022, Sep. 2022, 京都大学桂キャンパス金属有機構造体の励起子分裂による多重励起子のスピン量子操作
- 61st Rocky Mountain Conference on Magnetic Resonance, Jul. 2022, Denver, ColoradoExciton Dynamics on Triplet-Triplet Annihilation Upconversion in Organic Semiconductors Revealed by Time-Resolved EPR
- ECS Meeting, May 2022, Vancouver, CAConformations of Exciton Pairs Associated with Spin-Entanglement Transports during Singlet Fissions
- 日本化学会第102春季年会(2022), Mar. 2022, Web上での発表時間分解電子スピン共鳴法による非フラーレン型太陽電池材料の界面電荷分離構造解析
- 日本化学会第102春季年会(2022), Mar. 2022, Web上での発表分子内一重項励起子分裂で生成する多重励起子の構造変化:時間分解EPR法による解析
- 日本化学会第102春季年会(2022), Mar. 2022, Web上での発表時間分解EPR法による熱活性化遅延蛍光分子の励起状態の解析
- 京都大学分子工学研究科特別講演会, Jan. 2022, 京都大学分子工学研究科電子スピン分極の空間映像化による動的エキシトン機構解析
- Pacifichem2021, Dec. 2021, Web上での発表Heterogeneous charge-separation geometries at bulk-heterojunction interfaces in organic solar cell studied by transient EPR
- 7th Kanto Area Spin Chemistry Meeting (KASC 7), Dec. 2021, Web上での発表Water dynamics control of the magnetic compass
- Pacifichem2021, Dec. 2021, Web上での発表Spin-entanglement transport via singlet-fission as studied by transient EPR
- 第15回物性科学領域横断研究会, Nov. 2021, Web上での発表動物の磁気コンパスにおける水和運動の役割: 光受容タンパク質の長距離電荷分離機構
- Modern Development of Magnetic Resonance, Nov. 2021, Web上での発表Vibronic Spins in Singlet Fissions
- ICFPE2021, Oct. 2021, Web上での発表Conformation change and electronic de-coupling via intramolecular singlet fissions
- 第15回 分子科学討論会, Sep. 2021, Web上での発表分子内励起子分裂に伴う立体構造変化と電子的デカップリング :電子スピン分極映像化による解析
- 量子生命科学会第3回大会, Sep. 2021, Web上での発表光合成光電荷分離のスピン量子コヒーレンスとデコヒーレンス
- 2021年光化学討論会, Sep. 2021, Web上での発表時間分解EPR法による熱活性化遅延蛍光分子の励起状態の解析
- 2021年光化学討論会, Sep. 2021, Web上での発表時間分解EPRによるビフェニル連結テトラセンダイマーの分子内励起子分裂機構の解明
- 2021年光化学討論会, Sep. 2021, Web上での発表ベンゾポルフィリン-ジケトピロロピロールをドナーとするバルクヘテロ接合界面の電荷移動と電荷解離:時間分解EPRによる解析
- 光化学討論会2021, Sep. 2021, Web上での発表結晶性薄膜の一重項励起子分裂 : 活性化多重励起子の構造と解離に対する動的効果
- 第19回ESR夏の学校講演会, Sep. 2021, Web上での発表電子スピン分極映像化による超高効率エネルギー変換機構の解明
- 第一回広帯域極限電磁波生命理工連携研究会, Sep. 2021, Web上での発表「電子スピン分極映像化による超高効率光エネルギー変換機構の解明」
- ISMAR-APNMR2021, Aug. 2021, Web上での発表Generation domain of quintet multiexcitons via singlet fission in organic thin films as studied by time-resolved EPR
- ECS Meeting, Jun. 2021, Web上での発表Vibronic Effect of Donor-Acceptor Interaction Determines Fate of Mutiexciton Spins Generated By Singlet Fission
- 6th Kanto Area Spin Chemistry Meeting, Dec. 2020, Web上での発表Conformation Changes in Intramolecular Multiexciton Spins
- “光”機到来!Qコロキウム, Dec. 2020, Web上での発表電子スピンの量子・動的効果で読み解く光エネルギー変換のしくみ
- 電子スピンサイエンス学会年会2020, Nov. 2020, Web上での発表植物PSIIの電荷再結合に対する活性化パラメータの再評価
- 電子スピンサイエンス学会年会2020, Nov. 2020, Web上での発表共有結合した二量体における一重項励起子分裂によって生成された五重項励起子の立体配置
- 電子スピンサイエンス学会年会2020, Nov. 2020, Web上での発表分子内一重項分裂によるスピン相関三重項対生成に対する振電効果
- 2020年光化学討論会, Sep. 2020, Web上での発表Fast T-Type Photochromism of Colloidal Cu-Doped ZnS Nanocrystals
- 2020年光化学討論会, Sep. 2020, Web上での発表有機薄膜中の一重項励起子分裂による五重項多重励起子の生成ドメイン
- 2020年光化学討論会, Sep. 2020, Web上での発表植物 PSII の初期光電荷分離による立体配置と電荷再結合に対する温度効果
- 2020年光化学討論会, Sep. 2020共有結合した二量体における一重項分裂によって生成された五重項励起子の立体配置
- 2020年光化学討論会, Sep. 2020, Web上での発表有機薄膜中のシングレットフィッションによる多重励起子解離機構:時間分解 EPR 法を用いた解析
- JPA Award 2019 Award Lecture, Sep. 2020, Web上での発表Photon-to-Energy Conversion Mechanisms Revealed by Quantum Effects on Electron Spin Polarization
- 5th Kanto Area Spin Chemistry Meeting (4th KASC), Dec. 2019, Saitama Univ.Electron Spin Polarization Transfers in Charge-Separation and in Singlet Fission
- 第58回電子スピンサイエンス学会年会(SEST2019), Nov. 2019TIPS ペンタセン薄膜の一重項分裂による室温での時間分解 EPR
- 第58回電子スピンサイエンス学会年会(SEST2019), Nov. 2019時間分解 EPR 法を用いた P3HT:PC70BM ブレンド膜における 光誘起電荷ダイナミクスの解明
- 第58回電子スピンサイエンス学会年会(SEST2019), Nov. 2019非フラーレンアクセプターを用いたブレンド膜の時間分解 EPR
- 第58回電子スピンサイエンス学会年会(SEST2019), Nov. 2019時間分解 EPR 法による一重項励起子分裂により生成した多重励起子解離機構の解明
- 第58回電子スピンサイエンス学会年会(SEST2019), Nov. 2019偏光励起による五重項状態の効率的形成に関する研究
- 2019年光化学討論会, Sep. 2019ハロゲン混合型有機無機ペロブスカイトにおける光誘起相分離
- 2019年光化学討論会, Sep. 2019植物 PSII の初期光電荷分離による立体配置と電荷再結合に対する温度効果
- Sep. 2019イオンダイナミクスが誘起する有機鉛ペロブス カイトの単一粒子発光スイッチング
- 2019年光化学討論会, Sep. 2019二色時間分解 EPR 測定法を用いた有機太陽電池 における電荷分離状態の観測
- Wasielewski Symposium (Wazapalooza2019), Sep. 2019, Northweastern University, Evanston, USATransport of Spin-Correlated Multiexciton via Singlet Fission
- 16th International Symposium on Spin and Magnetic Field Effects in Chemistry and Related Phenomena, Aug. 2019, Saint Petersburg, RussiaPhotoinduced charge recombination in P3HT:PC70BM blend film studied by TR-EPR
- 16th International Symposium on Spin and Magnetic Field Effects in Chemistry and Related Phenomena, Aug. 2019, Saint Petersburg, RussiaMolecular geometries and motions driving quintet multiexcitons via singlet fissions
- 16th International Symposium on Spin and Magnetic Field Effects in Chemistry and Related Phenomena, Aug. 2019, Saint Petersburg, RussiaMechanism of multiple multiexciton formation and triplet dissociation by singlet fission in thin films
- 6th Awaji International Workshop on “Electron Spin Science & Technology: Biological and Materials Science Oriented Applications” (6th AWEST 2019), Jun. 2019, Awaji Yumebutai International Conference CenterMolecular Geometries and Motions Drive Quintet Multiexcitons via Singlet Fissions
- 235th ECS Meeting, May 2019, Dallas(USA)Transient Electron Spin Polarization Imaging of Photoinduced Interfacial Charge Separation Geometries in Organic Photovoltaic Cell
- 235th ECS Meeting, May 2019, Dallas(USA)Geometry and Dynamics of Quintet Multiexciton Studied By Time-Resolved EPR
- Colloquium in Department of Applied Chemistry, National Chiao Tung University, Apr. 2019, National Chiao Tung University(台湾)Unveiling Primary Photo-Energy Conversion Mechanisms by Transient Electron Spin Polarization Imaging Spectroscopy
- 日本化学会 第99春季年会 (2019), Mar. 2019, 甲南大学 岡本キャンパス有機鉛ハロゲン化物ペロブスカイトにおける発光挙動の単一粒子発光観測
- 第19回分子分光研究会, Mar. 2019, 静岡大学 静岡キャンパス時間分解電子スピン共鳴法を用いた光エネルギー変換初期過程の観測
- 日本化学会 第99春季年会 (2019), Mar. 2019, 甲南大学 岡本キャンパス酸化チタンメソ結晶の制御されたナノ空間を利用した選択的光触媒反応
- 日本化学会 第99春季年会 (2019), Mar. 2019, 甲南大学 岡本キャンパスルテニウム色素吸着メソポーラスシリカの単一粒子蛍光顕微鏡観測:細孔内拡散と光触媒活性の関係
- 日本化学会 第99春季年会 (2019), Mar. 2019, 甲南大学 岡本キャンパスハロゲン混合型有機無機ペロブスカイトナノ粒子の単一粒子発光イメージング
- 日本化学会 第99春季年会 (2019), Mar. 2019, 甲南大学 岡本キャンパスソフトクリスタルにおける刺激応答構造変化の蛍光顕微鏡観測
- 6th OCU International Workshop on Quantum Chemistry/Quantum Chemical Calculations on Quantum Computers: Quantum Algorithms, Mar. 2019, OCU Media Center, Osaka City UniversityThree-Dimension Visualizations of Electron Spin Polarization for Elucidating Photo-Energy Conversion Mechanisms
- 日本化学会 第99春季年会 (2019), Mar. 2019, 甲南大学 岡本キャンパスSingle-Particle Photoluminescence Switching Induced by Ion Dynamics in Organic-Inorganic Perovskite Nanoparticles
- 日本化学会 第99春季年会 (2019), Mar. 2019, 甲南大学 岡本キャンパスObservation of Quantitative Intermolecular Two-Electron Transfer Process through Highly Efficient Singlet Fission in Tetracene Dimer
- 日本化学会 第99春季年会 (2019), Mar. 2019, 甲南大学 岡本キャンパスLong-lived Triplet Excitons Formed by Intramolecular Singlet Fission of Adamantane-linked Tetracene Dyad
- 日本化学会 第99春季年会 (2019), Mar. 2019, 甲南大学 岡本キャンパスLocal Environment of Lipid Bilayer Membrane Monitored by Magnetic Field Effect-Based Fluorescence Imaging
- 日本化学会 第99春季年会 (2019), Mar. 2019, 甲南大学 岡本キャンパスIntramolecular Singlet Fission Behavior of Adamantane-linked Tetracene Dyad
- 日本化学会 第99春季年会 (2019), Mar. 2019, 甲南大学 岡本キャンパスCuをドープした水溶性ZnSナノ結晶の光物性とフォトクロミズム
- 神戸大学先端融合研究環境環ワークショップ『非共有結合系の分子科学:計測技術から探る生体分子科学の新展開』, Jan. 2019, 神戸大学 六甲台キャンパス 理学部Z201, 205号室部位特異的スピンラベルEPR分光法によるABCトランスポーター; BhuUVの構造変化測定
- 神戸大学 研究基盤センター 若手フロンティア研究会2018, Dec. 2018, 神戸大学百年記念館部位特異的スピンラベルEPR分光法によるABCトランスポーター;BhuUVの構造変化の実時間測定
- 10th Asian Photochemistry Conference (APC2018), Dec. 2018, Howard Civil Service Internationl House(Taipei)Singlet-Fission-Born Quintet State: Sublevel Selections and Trapping by Entropy Enhancement in Disordered Aggregates
- 10th Asian Photochemistry Conference (APC2018), Dec. 2018, Howard Civil Service Internationl House(Taipei)Single-Particle Emission Observation of Ruthenium Complex Supported on Mesoporous Silica
- 10th Asian Photochemistry Conference (APC2018), Dec. 2018, Howard Civil Service Internationl House(Taipei)Single-Particle Emission Observation of NaTaO3 Photocatalysts Using Deep Ultraviolet Fluorescence Microscope
- 10th Asian Photochemistry Conference (APC2018), Dec. 2018, Howard Civil Service Internationl House(Taipei)Localized Trapped Charges Induce Slow Charge Transfer over a Few Nanoseconds on Heterostructured CH3NH3PbBr3-xIx
- 10th Asian Photochemistry Conference (APC2018), Dec. 2018, Howard Civil Service Internationl House(Taipei)Local Environment Mapping of Lipid Bilayer Membranes using Magnetic Field Effects
- 10th Asian Photochemistry Conference (APC2018), Dec. 2018, Howard Civil Service Internationl House(Taipei)Development of Titanium Dioxide Mesocrystals for Highly Efficient and Selective Photocatalysis: Role of Oriented Nano-Space
- 10th Asian Photochemistry Conference (APC2018), Dec. 2018, Howard Civil Service Internationl House(Taipei)Development of Hierarchical Mesocrystals for Efficient Photocatalysis
- 第57回電子スピンサイエンス学会年会(SEST2018), Nov. 2018, 北海道大学時間分解EPR法を用いたPC70BM薄膜中における励起子拡散の観測
- 第57回電子スピンサイエンス学会年会(SEST2018), Nov. 2018, 北海道大学時間分解EPR法を用いたP3HT:PC70BMブレンド膜に生成する光電荷分離状態の観測
- 2018年光化学討論会, Sep. 2018, 関西学院大学・上ケ原キャンパス有機包接結晶における室温リン光発光性三重項電荷移動状態のゲスト分子依存性
- 第21回分子科学討論会2018, Sep. 2018, 福岡国際会議場電子スピン共鳴によるSrドープNaTaO3光触媒の電子励起状態の研究
- 2018年光化学討論会, Sep. 2018, 関西学院大学・上ケ原キャンパス新規金属酸化物メソ結晶の開発と高効率・高選択的光触媒への応用
- 2018年光化学討論会, Sep. 2018, 関西学院大学・上ケ原キャンパス新規テトラセンダイアドで実現する分子内シングレットフィッション
- 2018年光化学討論会, Sep. 2018, 関西学院大学・上ケ原キャンパス時間分解EPR 法を用いたP3HT:PC70BM ブレンド膜に生成する光電荷分離状態の観測
- 第12回分子科学討論会2018, Sep. 2018, 福岡国際会議場時間分解EPRによる一重項分裂反応から生じた三重項励起子対のダイナミクスの解析
- 2018年光化学討論会, Sep. 2018, 関西学院大学・上ケ原キャンパス混合ハロゲン化物ペロブスカイトにおける電荷キャリアダイナミクス
- 2018年光化学討論会, Sep. 2018, 関西学院大学・上ケ原キャンパスメソポーラスシリカ担持ルテニウム錯体の単一粒子発光観測:細孔内拡散と光触媒活性の関係
- 2018年光化学討論会, Sep. 2018, 関西学院大学・上ケ原キャンパスハロゲン交換反応によるペロブスカイトナノ粒子のコアーシェル空間制御
- 2018年光化学討論会, Sep. 2018, 関西学院大学・上ケ原キャンパスタンタル酸ナトリウム光触媒の発光特性と金属ドープ濃度の関係性
- 2018年光化学討論会, Sep. 2018, 関西学院大学・上ケ原キャンパスクリプトクロムに生成する光電荷分離状態の立体構造の観測
- 2018年光化学討論会, Sep. 2018, 関西学院大学・上ケ原キャンパスTREPR 法によるシングレットフィッションにおける五重項状態の生成機構
- 3rd International conference SPIN PHYSICS, SPIN CHEMISTRY and SPIN TECHNOLOGY, Sep. 2018, Novosibirsk (Russia)Singlet-Fission-Born Quintet State: Sublevel Selections and Trapping by Multiexciton Thermodynamics
- 第56回日本生物物理学会年会, Sep. 2018, 岡山大学 津島キャンパスReal-time measurements of the conformational changes in ABC transporter; BhuUV, revealed by site-directed spin-labeling EPR spectroscopy
- The third joint conference of the Asia-Pacific EPR/ESR Society and the International EPR (ESR) Society (IES), Sep. 2018, BrisbaneAB18 - Electron Spin Polarization Imaging of Photoinduced Primary Charge-Separated States in PSII
- 第5回森野ディスカッション, Aug. 2018, 東京大学理学部 小柴ホール光合成初期反応の電子スピン画像解析
- 27th IUPAC International Symposium on Photochemistry, Jul. 2018, University College Dublin(Ireland)Correlated dynamics of photogenerated charges and ions in organolead mixed-halide perovskites
- 35th International Conference of Photopolymer Science and Technology(ICPST-35), Jun. 2018, 幕張メッセ国際会議場Time-Resolved EPR Study on Singlet Fission and Subsequent Triplet Dissociation Dynamics
- 233rd ECS MEETING, May 2018, Seattle, WA USATime Resolved EPR Study on Photoinduced Charge-Transfer Trap States in Thiophene-Thiazolothiazole Copolymers Films
- タンタル酸ナトリウム光触媒のダイナミズムに関する研究会2018, Feb. 2018, 石川県白山市NaTaO3光触媒に生成する光キャリアの運動と空間分布
- The third joint conference of the Asia-Pacific EPR/ESR Society and the International EPR (ESR) Society (IES), 2018, BrisbaneSpin convrsion of the singlet-fission-bornmultiexciton in the amorphous aggregates
- 10th Asian Photochemistry Conference (APC 2018), 2018, 台北Multiexciton dynamics in amorphous aggregates of singlet fission materials studied by time-Resolved EPR spectroscopy
- 先端的ESR研究Workshop2017, Dec. 2017, 弥彦温泉 四季の宿みのや (新潟県西蒲原郡弥彦村弥彦)巨大分子の光機能解明と時間発展
- 第56回電子スピンサイエンス学会年会(SEST2017), Nov. 2017, 東京工業大学電子スピン分極イメージング法によるクリプトクロム光電荷分離状態の立体構造解析
- 第56回電子スピンサイエンス学会年会(SEST2017), Nov. 2017, 東京工業大学時間分解EPR法による室温リン光発光性有機包接結晶の三重項電荷移動状態におけるゲスト分子依存性
- 第56回電子スピンサイエンス学会年会(SEST2017), Nov. 2017, 東京工業大学光誘起電子移動反応における磁場効果を利用した新規蛍光イメージング法の開発
- 第56回電子スピンサイエンス学会年会(SEST2017), Nov. 2017, 東京工業大学 大岡山キャンパス強磁場・テラヘルツ領域におけるヘミンの精密ESR分光
- 第56回電子スピンサイエンス学会年会(SEST2017), Nov. 2017, 東京工業大学ペンタセン・テトラセン誘導体における一重項分裂により生成した五重項状態の観測
- 第36回 固体・表面光化学討論会, Nov. 2017, 滋賀県立大学タンタル酸ナトリウム光触媒の発光挙動におけるドーピングの効果
- 第56回電子スピンサイエンス学会年会(SEST2017), Nov. 2017, 東京工業大学アフリカツメガエル由来クリプトクロムに生成する光電荷分離状態の電子的相互作用
- 第56回電子スピンサイエンス学会年会(SEST2017), Nov. 2017, 東京工業大学TREPR法によるチオフェン-チアゾロチアゾールポリマー薄膜に生成する光誘起キャリアトラップ状態の観測
- 11th Japanese-Russian Workshop on “Open Shell Compounds and Molecular Spin Devices”, Nov. 2017, Awaji Yumebutai International Conference CenterTime-Resolved EPR Study on Photoinduced Charge-Transfer Trap States in Thiophene-Thiazolothiazole Copolymer Films
- 第56回電子スピンサイエンス学会年会(SEST2017), Nov. 2017, 東京工業大学PSII反応中心の光電荷分離と励起子生成に対する励起波長依存性
- 第7回CSJ化学フェスタ2017, Oct. 2017, タワーホール船堀有機無機ペロブスカイトのハロゲン交換反応における過渡種生成と電荷捕集のその場観測
- 第7回CSJ化学フェスタ2017, Oct. 2017, タワーホール船堀有機金属ハロゲン化物ペロブスカイトにおける光反応挙動の単一粒子解析
- 第7回CSJ化学フェスタ2017, Oct. 2017, タワーホール船堀時間分解EPR法による室温リン光発光性有機包接結晶の励起三重項状態の電子構造
- 2017年光化学討論会, Sep. 2017, 東北大学青葉山キャンパス深紫外蛍光顕微鏡によるNaTaO3 光触媒の発光観測
- 2017年光化学討論会, Sep. 2017, 東北大学青葉山キャンパス時間分解EPR 法による室温リン光発光性有機包接結晶の励起三重項状態の電子構造
- 第55回日本生物物理学会年会, Sep. 2017, 熊本大学 黒髪北地区Regulation of Initial Charge Separation in Photosynthetic Reaction Center detected by Transient EPR
- 第55回日本生物物理学会年会, Sep. 2017, 熊本大学 黒髪北地区The mechanism of efficient charge separation reaction in photosystem II of higher plants
- 2017年光化学討論会, Sep. 2017, 東北大学青葉山キャンパス顕微分光法を用いた二酸化チタンメソ結晶の光機能性評価
- 第55回日本生物物理学会年会, Sep. 2017, 熊本大学 黒髪北地区Initial charge separated spin-polarized radical pair in reaction center of Heliobacterium modesticaldum
- 2017年光化学討論会, Sep. 2017, 東北大学青葉山キャンパスチタン酸ストロンチウムメソ結晶光触媒における特異な電荷移動挙動
- 2017年光化学討論会, Sep. 2017, 東北大学青葉山キャンパスアフリカツメガエル由来クリプトクロムに生成する光電荷分離状態の電子的相互作用
- 2017年光化学討論会, Sep. 2017, 東北大学青葉山キャンパスTime-Resolved EPR Study on Photoinduced Charge-Transfer Trap State in Thiophene-Thiazolothiazole Copolymer Film
- 2017年光化学討論会, Sep. 2017, 東北大学青葉山キャンパスTime-resolved and pulsed electron paramagnetic resonance study on the singlet-fission materials
- 第11回分子科学討論会2017仙台, Sep. 2017, 東北大学 川内北キャンパスSrドープNaTaO3光触媒の電子スピン共鳴による計測評価
- 2017年光化学討論会, Sep. 2017, 東北大学青葉山キャンパスSlow Charge Transfer Process over a Few Nanoseconds in Heterostructured CH3NH3PbBr3-xIx
- 2017年光化学討論会, Sep. 2017, 東北大学青葉山キャンパスPSII 反応中心の光電荷分離と励起子生成に対する励起波長依存性
- 2017年光化学討論会, Sep. 2017, 東北大学青葉山キャンパスElectron tunneling route of photoinduced primary charge-separated state in the PSII studied by electron spin polarization imaging method
- 15th International Symposium on Spin and Magnetic Field Effects in Chemistry and Related Phenomena(SCM2017), Sep. 2017, Schluchsee, GermanyElectron spin polarization imaging of photoinduced primary charge-separated states in PSII
- 第30回生物無機化学夏季セミナー, Aug. 2017, 白子・サンライズオーツカ時間分解電子スピン共鳴法による生体分子機能の解明
- 第4回森野ディスカッション, Jul. 2017, 東京大学理学部 小柴ホール光合成初期反応の電子スピン画像解析
- 第21回ESRフォーラム研究会2017 京都, Jul. 2017, 京都工芸繊維大学シロキ基を有する室温リン光発性有機結晶の三重項状態に対する時間分解EPR観測
- 第21回ESRフォーラム研究会2017 京都, Jul. 2017, 京都工芸繊維大学TREPR法によるチオフェン-チアゾロチアゾールポリマー簿膜に生成する光誘起キャリアトラップ状態の観測
- 第21回ESRフォーラム研究会2017 京都, Jul. 2017, 京都工芸繊維大学PSⅡ反応中心の光電荷分離と励起子生成に対する励起波長依存性
- 第36回光がかかわる触媒化学シンポジウム, Jun. 2017, 近畿大学チタン酸ストロウムメソ結晶の合成と水分解光触媒へ応用
- 5th Awaji International Workshop on “Electron Spin Science & Technology: Biological and Materials Science Oriented Applications” (5th AWEST 2017), Jun. 2017, Awaji Yumebutai International Conference CenterTime-resolved EPR Study on Photoinduced Electron Spin Polarization and Dynamics of Radicals at Bilayer Interface
- 34th International Conference of Photopolymer Science and Technology, Jun. 2017, Makuhari MesseTime Resolved EPR Study on Photoinduced Charge-Separations in Thin Films of Thiophene-Thiazolothiazole Copolymers
- 5th Awaji International Workshop on “Electron Spin Science & Technology: Biological and Materials Science Oriented Applications” (5th AWEST 2017), Jun. 2017, Awaji Yumebutai International Conference CenterTime-resolved EPR Study on Antiaromatic Excited Triplet State of [28]Hexaphyrin with Twisted Möbius Conformation
- 5th Awaji International Workshop on “Electron Spin Science & Technology: Biological and Materials Science Oriented Applications” (5th AWEST 2017), Jun. 2017, Awaji Yumebutai International Conference CenterElectron spin polarization imaging applied to primary charge separation in the PSII
- 231st ECS Meeting, May 2017, New Orleans, LATime-Resolved EPR Study on Charge Dynamics of Electron-Hole Pairs in Lead Iodide Perovskite Thin Film
- 231st ECS Meeting, May 2017, New Orleans, LAGeometries and Dynamics of Photoinduced Electron-Hole Pairs in Polyhexylthiophene-Fullerene Systems
- 日本化学会 第97春季年会 (2017), Mar. 2017, 慶應義塾大学 日吉キャンパス光誘起電子移動反応における磁場効果を利用した新規蛍光顕微鏡観察手法の開発
- 日本化学会 第97春季年会 (2017), Mar. 2017, 慶應義塾大学 日吉キャンパスCharge Carrier Dynamics of CH3NH3PbBr3-xIx with Hetero-Band Structures
- 分子研研究会-生体や物質機能の起源にせまる先端的電子スピン計測-, Dec. 2016, 自然科学研究機構 分子科学研究所電子スピン分極イメージング法の開発によるPSII 電荷分離構造の三次元映像化
- 第55回電子スピンサイエンス学会年会, Nov. 2016, 大阪市立大学時間分解EPR法による有機包接室温強リン光発光結晶の励起三重項状態の電子構造
- 第6回CSJ化学フェスタ2016, Nov. 2016, タワーホール船堀効率的な炭素ラジカルの生成を目指した有機分子触媒の開発
- 第6回 CSJ化学フェスタ 2016, Nov. 2016, 公益社団法人日本化学会, 東京•タワーホール船堀フォトクロミックキノンの光レドックス変換と化学反応への応用
- 第6回CSJ化学フェスタ2016, Nov. 2016, タワーホール船堀ねじれたメビウス構造を有するヘキサフィリンの励起三重項状態の電子構造
- 第54回日本生物物理学会年会, Nov. 2016, つくば国際会議場Time resolved EPR study on orientations and electronic couplings of the primary charge-separated state in the PSII reaction center
- 第54回日本生物物理学会年会, Nov. 2016, つくば国際会議場Effects of amyloid fibrillations on geometries of human insulin as studied by time-resolved EPR spectroscopy
- 2016年光化学討論会, Sep. 2016, 東京大学駒場第一キャンパス単一粒子顕微分光電気化学法によるSrTiO3メソ結晶の発光観測
- 2016年光化学討論会, Sep. 2016, 東京大学駒場第一キャンパス時間分解電子スピン共鳴法によるチオフェンーチアゾロチアゾールコポリマー:PCBM有機薄膜における電荷分離状態の立体構造とダイナミクス
- 第10回分子科学討論会, Sep. 2016, 神戸ファッションマート時間分解EPR法による二分子膜界面におけるビタミンCの抗酸化反応機構と スピンダイナミクス
- 2016年光化学討論会, Sep. 2016, 東京大学駒場第一キャンパス時間分解EPR法によるチオフェン-チアゾロチアゾールポリマー薄膜に生成する光電荷分離状態の観測
- 第10回分子科学討論会, Sep. 2016, 神戸ファッションマート時間分解EPR法によるPSII反応中心に生成する初期電荷分離構造の解析
- 2016年光化学討論会, Sep. 2016, 東京大学駒場第一キャンパスLong-range charge transfer and transient species formation during halide exchange reaction on an organolead halide perovskite crystal
- 2016 Electron Donor Acceptor Interactions Gordon Research Conference, Aug. 2016, Newport, USAPrimary Charge-Separation Mechanism in the Photosynthetic Reaction Center Studied by Time-Resolved EPR Spectroscopy
- Asia-Pacific EPR/ESR Symposium 2016, Aug. 2016, Irkutsk city, RussiaElectronic Structure of the Excited Triplet State of Hexaphyrins with twisted Mobious Conformation as Studied by TR EPR
- 第20回ESRフォーラム研究会 in 神戸, Jul. 2016, 神戸大学 瀧川記念学術交流会館有機包接室温強リン光発光結晶の三重項状態に対する時間分解 EPR 観測
- 第20回ESRフォーラム研究会 in 神戸, Jul. 2016, 神戸大学 瀧川記念学術交流会館電⼦スピン共鳴法を⽤いたヒトインスリンのアミロイド線維化による構造変化の観測
- 第20回ESRフォーラム研究会 in 神戸, Jul. 2016, 神戸大学 瀧川記念学術交流会館時間分解EPR 法によるチオフェンーチアゾロチアゾールコポリマー:PCBM有機薄膜に⽣成する光誘起キャリアのダイナミクス
- 第20回ESRフォーラム研究会 in 神戸, Jul. 2016, 神戸大学 瀧川記念学術交流会館時間分解EPR 法によるチオフェン-チアゾロチアゾールポリマー薄膜に⽣成する光電荷分離状態の構造解析
- 第20回ESRフォーラム研究会 in 神戸, Jul. 2016, 神戸大学 瀧川記念学術交流会館時間分解EPR 法によるPSII 反応中⼼に⽣成する初期電荷分離構造解析
- 第20回ESRフォーラム研究会 in 神戸, Jul. 2016, 神戸大学 瀧川記念学術交流会館光誘起電⼦移動反応における磁場効果の蛍光顕微鏡観察⼿法の開発
- 第5回 JACI/GSCシンポジウム, Jun. 2016, 公益社団法人 新化学技術推進協会, 神戸・ANAクラウンプラザ光によるキノンのレドックス変換
- 4th Awaji International Workshop on “Electron Spin Science & Technology: Biological and Materials Science Oriented Applications”, Jun. 2016, Awaji Yumebutai International Conference CenterTime-domain EPR observations of changes in protein binding structures induced by the amyloid fibrillation of human insulin
- The 33rd International Conference of Photopolymer Science and Technology, Jun. 2016, Makuhari Messe, ChibaMorphology Effect on the Geometry of the Photoinduced Charge-Separated State in P3HT:PCBM Brend Films as Studied by Time-Resolved EPR Spectroscopy
- 4th Awaji International Workshop on “Electron Spin Science & Technology: Biological and Materials Science Oriented Applications”, Jun. 2016, Awaji Yumebutai International Conference CenterDynamics of Photoinduced Electron-Hole Pairs in Polyhexylthiophene-Fullerene Dyads Rigidly Linked by Oligophenylenes
- The XXVIth IUPAC Symposium on Photochemistry, Apr. 2016, Osaka City Central Public Hall, Osaka, JapanSINGLE-PARTICLE PHOTOLUMINESCENCE MEASUREMENTS REVEAL THE SURFACE CHARGE TRAPPING IN ORGANOLEAD BROMIDE PEROVSKITE
- The XXVIth IUPAC Symposium on Photochemistry, Apr. 2016, Osaka City Central Public Hall, Osaka, JapanCRYSTAL-FACE-DEPENDENT CHARGE DYNAMICS ON A BiVO 4 PHOTOCATALYST STUDIED BY SINGLE-PARTICLE PHOTOELECTROCHEMISTRY
- 日本化学会第96春季年会(2016), Mar. 2016, 同志社大学 京田辺キャンパス有機金属ハロゲン化物ペロブスカイトにおけるハロゲン交換反応の単一粒子分光
- 日本化学会第96春季年会(2016), Mar. 2016, 同志社大学 京田辺キャンパス単一粒子顕微分光電気化学法によるBiVO4光触媒の結晶面依存キャリアダイナミクス観測
- 日本化学会 第96春季年会 (2016), Mar. 2016, 同志社大学 京田辺キャンパス効率的な炭素ラジカルの生成を目指した有機分子触媒の開発
- 応用物理学会春期学術講演会, Mar. 2016, 東京工業大学大岡山キャンパスチオフェン−チアゾロチアゾールポリマー:PCBM有機薄膜における初期電荷分離機構
- Pacifichem 2015, Dec. 2015, Hawai, USASynthesis and single-particle photoluminescence observation of hybrid organic-inorganic perovskite nanoparticles
- 異分野融合ワークショップ「有機太陽電池開発の現状と展望」, Nov. 2015有機薄膜太陽電池の光電流生成初期過程:界面電子-正孔対の立体構造と電子状態
- 第54回電子スピンサイエンス学会年会, Nov. 2015, 朱鷺メッセ時間分解ERR法によるチオフェン−チアゾロチアゾールポリマー:PCBM有機薄膜における光電荷分離ダイナミクス
- 第54回電子スピンサイエンス学会年会, Nov. 2015, 朱鷺メッセ時間分解EPR法によるヘキサフィリン励起三重項状態の生成機構と電子状態の解明
- 第54回電子スピンサイエンス学会年会, Nov. 2015, 朱鷺メッセペロブスカイト型太陽電池の光活性層界面に生成する光電荷分離状態の時間分解EPR
- 2015年 光化学討論会, Sep. 2015, 大阪市立大学 杉本キャンパス有機-無機ハイブリッド型ペロブスカイトの単一粒子発光観察
- 2015年 光化学討論会, Sep. 2015, 大阪市立大学 杉本キャンパス有機-無機ハイブリッド型ペロブスカイトナノ粒子の発光ブリンキング挙動
- 2015年 光化学討論会, Sep. 2015, 大阪市立大学 杉本キャンパス時間分解EPR法を用いたアミロイド線維を形成するヒトインスリンにおけるアミノ酸残基局所構造の観測
- 第53回日本生物物理学会年会, Sep. 2015, 金沢大学角間キャンパスTime-Resolved EPR Study on Geometry and Dynamics of the Primary Charge-Separated State in the Photosystem II Reaction Center of Spinach
- 2015年 光化学討論会, Sep. 2015, 大阪市立大学 杉本キャンパス時間分解EPR法によるチオフェンーチアゾロチアゾールポリマー:PCBM有機薄膜における初期電荷分離状態の観測
- 2015年 光化学討論会, Sep. 2015, 大阪市立大学 杉本キャンパス蛍光プローブを用いたBiVO4光触媒のその場観察
- 2015年 光化学討論会, Sep. 2015, 大阪市立大学 杉本キャンパスホウレン草のPSII反応中心に生成する光電荷分離状態の時間分解EPR
- International Workshop for Green Photonics, Sep. 2015, 奈良先端科学技術大学院大学Primary Charge-Separation Mechanism in the Photosynthetic Reaction Center
- AWEST2015, Jun. 2015, Awaji, JapanTime-resolved EPR on primary charge separation and recombination in the photosynthetic reaction center: Impact of electronic couplings
- Colloquium at Freiburg Institute of Advanced Studies, Jun. 2015Orbital Functionalities on the Primary Charge-Separations in the Organic Photovoltaic Solar Cell: A Transient Electron Paramagnetic Resonance Study
- ナノ学会第13回大会, May 2015, 東北大学 片平さくらホール有機-無機ペロブスカイトナノ粒子の合成と単一粒子発光挙動
- 日本化学会第95春季年会2015, Mar. 2015, 公益社団法人 日本化学会, 日本大学 理工学部船橋キャンパス時間分解EPR法によるヘキサフィリン励起三重項状態の電子構造の解明
- 日本化学会第95春季年会2015, Mar. 2015, 公益社団法人 日本化学会, 日本大学 理工学部船橋キャンパス時間分解EPR法によるP3HT:PCBM有機薄膜太陽電池の光電流生成機構の解明
- 日本化学会第95春季年会2015, Mar. 2015, 公益社団法人 日本化学会, 日本大学 理工学部船橋キャンパスアミロイド線維化タンパク質-アントラキノンスルフォン酸イオン複合体の時間分解EPR
- SCM 2015 - 14th International Symposium on Spin and Magnetic Field Effects in Chemistry and Related Phenomena, Mar. 2015, Kolkata, IndiaTime-resolved EPR study on cofactor geometries and electronic couplings after primary charge-separations in the photosynthetic reaction center
- 2014光化学討論会, Nov. 2014, 北海道大学 札幌キャンパス時間分解EPR法による光合成反応中心の初期電荷分離構造と電子的相互作用の解析
- アジア太平洋EPR/ESR学会-国際EPR(ESR)学会-第53回電子スピンサイエンス学会年会合同国際会議(APES-IES-SEST2014), Nov. 2014Time-resolved EPR study on the Electronic Structure of the Excited Triplet State of [26] and [28] Hexaphyrins
- アジア太平洋EPR/ESR学会-国際EPR(ESR)学会-第53回電子スピンサイエンス学会年会合同国際会議(APES-IES-SEST2014), Nov. 2014Time resolved EPR study on photoinduced primary charge-separated state of the PSII reaction center from spinach
- アジア太平洋EPR/ESR学会-国際EPR(ESR)学会-第53回電子スピンサイエンス学会年会合同国際会議(APES-IES-SEST2014), Nov. 2014Time resolved EPR study on photoinduced intermediates in photoactive interface of the perovskite solar cell
- アジア太平洋EPR/ESR学会-国際EPR(ESR)学会-第53回電子スピンサイエンス学会年会合同国際会議(APES-IES-SEST2014), Nov. 2014Morphology effect on the geometry of the photoinduced charge-separated states in RR P3HT:PCBM blend films studied by time-resolved EPR
- アジア太平洋EPR/ESR学会-国際EPR(ESR)学会-第53回電子スピンサイエンス学会年会合同国際会議(APES-IES-SEST2014), Nov. 2014, 東大寺総合文化センターElectron-hole dissociations and electronic coupling influenced by alkyl side chains in the photovoltaic Polyalkylthiophene:PCBM interface
- 32nd Samahang Pisika ng Philipinas Physics Congress, Nov. 2014, フィリピン大学国立物理研究所Electron-hole dissociation influenced by alkyl side chains in the photovoltaic polyalkylthiophene:PCBM interfaces
- アジア太平洋EPR/ESR学会-国際EPR(ESR)学会-第53回電子スピンサイエンス学会年会合同国際会議(APES-IES-SEST2014), Nov. 2014Effect of glycerol concentration on structure of photoinduced chargeseparated states in 9,10-anthraquinone-1-sulfonate-human serum albumin system
- 5th International Meeting on Spin in Organic Semiconductors, Oct. 2014, HimejiMorphology effect on the geometry of the the photoinduced charge separated states in RR-P3HT:PCBM blend film studies by time-resolved EPR
- 32nd National Physics Congress of the Samahang Pisika ng Pilipinas, Oct. 2014, National Institute of Physics University of the Philippines, Quezon City, PhilippinesElectron-hole dissociations influenced by alkyl side chains in the photovoltaic Polyalkylthiophene:PCBM interface
- 2014年光化学討論会, Sep. 2014, 北海道大学 札幌キャンパス時間分解EPR法によるヘキサフィリン励起三重項状態の電子構造の解明
- 第8回分子科学討論会, Sep. 2014, 広島大学 東広島キャンパス光合成反応中心の初期電荷分離過程に伴う立体構造変化:時間分解EPR法による解析
- 2014年光化学討論会, Sep. 2014, 北海道大学 札幌キャンパスポリヘキシルチオフェン-フラーレンをオリゴフェニレンで連結した分子P3HT-Phm-C60に生成する光誘起電荷分離状態の時間分解EPR法による解析
- 2014年光化学討論会, Sep. 2014, 北海道大学 札幌キャンパスホウレン草のPSII反応中心に生成する光電荷分離状態の時間分解EPR
- 2014年光化学討論会, Sep. 2014, 北海道大学 札幌キャンパスぺロブスカイト型太陽電池の光活性層界面に生成する光電荷分離状態の時間分解EPR
- 2014年光化学討論会, Sep. 2014, 北海道大学 札幌キャンパスヒト血清アルブミンーアントラキノン-1-スルホン酸イオン複合体の電荷分離構造に対するグリセロール添加効果
- Grand Renewable Energy International Conference, Aug. 2014, Tokyo Big Sight, TokyoElectron-hole dissociations influenced by alkyl side chains in the photovoltaic Polyalkylthiophene:PCBM interface
- 2nd Awaji International Workshop on “Electron Spin Science & Technology: Biological and Materials Science Oriented Applications, Jun. 2014, Awaji Island, Hyogo, Japan.Time-Resolved EPR study on cofactor geometries and electronic couplings of primary charge-separated state inthe photosynthetic reaction center
- 次世代太陽電池の動向と展望 京を用いた新材料設計に向けて, Mar. 2014, 理化学研究所 計算科学研究機構時間分解電子スピン共鳴法による有機薄膜太陽電池の光電流生成初期過程の観測:界面電子-正孔対の立体構造と電子状態
- 第7回ESRフォーラム研究会, Jul. 2013, 九州大学医学部百年講堂有機分子による光エネルギー変換機能:光合成反応中心と有機薄膜太陽電池
- The Awaji International Workshop on Electron Spin Science & Technology: Biological and Materials Science Oriented Applications, Jun. 2013, 淡路夢舞台国際会議場Exploring Roles of Nanostructure and Entropy on Primary Charge Dissociation in Organic Photovoltaic Interfaces Using Transient EPR
- 日本化学会春季年会特別企画「光化学の新展開」電荷移動によるスピンの動きを捉える
- Japan Society for the Promotion of Science, Grants-in-Aid for Scientific Research Grant-in-Aid for Scientific Research (A), Grant-in-Aid for Scientific Research (A), Kobe University, 01 Apr. 2022 - 31 Mar. 2025Semiconductor Photocatalysts for Artificial Photosynthesis: Operando Characterization of Reaction Kinetics in Milliseconds
- Japan Society for the Promotion of Science, Grants-in-Aid for Scientific Research Grant-in-Aid for Transformative Research Areas (A), Grant-in-Aid for Transformative Research Areas (A), Kobe University, 19 Nov. 2020 - 31 Mar. 2025Interaction in Dynamic Exciton Studied by Electron Spin Polarization Imaging本研究では有機系分子を中心とした次世代の光エネルギー変換材料の創成に向け、分子機構の解明が重要な有機薄膜系や連結系において、動的エキシトンによるスピン系相互作用をオングストローム領域の三次元映像で可視化し、三重項励起子や電荷分離立体構造による動的機構・電子状態を明らかにした。領域内で連携して過渡種の運動性を特徴づけ、電子スピン分極の三次元画像から、時々刻々変化する励起子対、光電荷分離状態の立体配置、運動性による磁気的相互作用の変化を映像化すると共に、電子的カップリングを定量している。スピン変換、再結合性、電荷解離性や束縛性状態の立体配置と運動性を明らかにする。部位特異的分子運動とその周波数がどのようにスピン変換、電荷分離立体配置や電子的カップリングに寄与するかを紐解き、中間体電子軌道による再結合を有効に制御する電子状態など、分子論的特性によりデバイス高効率化や生命機能開拓への学理を拓いた。分子内シングレットフィッション系では、強く相関した多重励起子からの電子的相互作用による束縛を解く際にかかるねじれ振動モードと周波数を具体的に特徴づけるとともに、それによる解離多重励起子の立体構造の変化も明らかにした。さらに励起子解離による立体構造変化の分子論起源は不明であった。本研究では、電子構造論に基づき双性イオン構造による束縛励起子対からのテラヘルツ振動による開放として、具体的に記述することもできた。有機光触媒開発においては、光誘起電荷分離過程で生成する光触媒分子の電荷分離状態の中間体を特定し触媒サイクル機構を明らかにした。以上より、結晶性と非晶性を併せ持つ有機エレクトロニクス薄膜や有機光触媒のエントロピー効果と運動による電子的効果を用いるデバイス効率飛躍的向上化の知的基盤を獲得し、有機薄膜太陽電池開発で課題となっている超高効率化への指針を提示することができるようになってきた。
- Japan Society for the Promotion of Science, Grants-in-Aid for Scientific Research Grant-in-Aid for Transformative Research Areas (A), Grant-in-Aid for Transformative Research Areas (A), Kyoto University, 19 Nov. 2020 - 31 Mar. 2025Dynamic Exciton: Emerging Science and Innovation本学術変革領域では、従来の光化学における「静的エキシトン」の概念を打ち破る学術領域「動的エキシトン学」の構築にむけ、分野融合・統合的研究を推進する。そのために総括班では、本領域全体での「学問分野の枠を超えた有機的連携の堅持」を最重要課題と位置づけ、期間内に全ての計画班員12名が役割分担して領域の推進に貢献する。特に、班長及び研究課題代表者による共同研究支援に加えて、若手研究者育成支援、女性研究者育成支援、国際活動支援、産学連携支援の五つの支援を柱に、様々な具体的施策により、領域の目標と方針を計画班員に周知徹底し、目標の達成に向け先導的な役割を達成を目指す。 研究領域全体の研究方針の作成は領域代表者の今堀と各班長、研究課題代表1-4を中心に行った。拡大運営委員会、領域会議等で計画班、公募班員全員が集まる機会を複数回設け、領域目標の周知・確認を繰り返し行った。また、広報活動の一環として、また領域目標の共有に向けて、領域ホームページ、プレスリリース、学会発表、アウトリーチ等も積極的に活用した。これらの機会を利用して、計画班員全員が互いの動的エキシトン研究の進捗を密に共有した。計画、公募班員は二ヶ月に一回程度、メールやZoomなどのインターネット会議で研究の進捗を各班長、研究課題代表に報告し 、各班長、研究課題代表は班長会議、研究課題会議、サイトビジットにより、計画、公募班全体の研究の進捗を把握した。これにより、必要に応じて適切なタイミングで、機動的な共同研究の提案、開始、とりまとめを行えた。
- Japan Society for the Promotion of Science, Grants-in-Aid for Scientific Research Grant-in-Aid for Challenging Research (Exploratory), Grant-in-Aid for Challenging Research (Exploratory), Kobe University, 30 Jun. 2022 - 31 Mar. 2024Photon up-conversion promoted by molecular vibration
- Japan Society for the Promotion of Science, Grants-in-Aid for Scientific Research Fund for the Promotion of Joint International Research (Fostering Joint International Research (B)), Fund for the Promotion of Joint International Research (Fostering Joint International Research (B)), Keio University, 27 Oct. 2020 - 31 Mar. 2024一重項分裂を駆動力とする革新的光反応の開発一般に、分子の光吸収過程では一光子光学許容状態(1光子吸収→1励起子生成)のみが遷移可能であり、励起状態を介した化学反応の量子収率の最大値は100%である。さらに、分子会合体になると単量体と比較して励起子間の消滅により吸収した励起エネルギーが迅速かつ大幅に失活する。この光化学の重大な問題点の解決策として二分子近接下で1光子の吸収過程から2つの三重項励起子を生成する多励起子生成反応の一重項分裂(SF)が考えられ、三重項励起子の生成効率ΦTは200%まで向上する。この励起子の倍増が可能なSFを種々の反応系でより汎用性を高めるには材料開発を含む基礎物性評価と反応開発の両輪による基礎学理の構築が急務である。本研究では国際共同研究を通してSFを最大限活用できる逐次反応系の構築を目指す。 まず、SFで最も汎用性の高いペンタセンと比較して、T1のエネルギーがより高く、強相関の三重項対(TT)生成の発熱性がより乏しい特徴を有するテトラセンに着目した。従来的な構造パラメーターである電子カップリングだけでなく、新たに立体柔軟性に着目し、異なるスペーサー部位を有する計4種類の二分子連結体を合成した。その結果、小さな電子カップリングと大きな立体柔軟性を有する4,4’-ビフェニル基で連結したテトラセン二分子連結体において量論的な三重項量子収率(196 ± 12%)の実現に成功した。次に、ペンタセン修飾量子ドットの分子集合体系では光吸収後の量子ドットの励起状態からペンタセンへのS-Sエネルギーを介して近接ペンタセン間の量論的なSFが観測された。量子ドットの光吸収光子数に対する三重項量子励起子の収率はほぼ200%となり、量論的なS-Sエネルギー移動とSFの逐次反応の観測に成功した。
- Japan Society for the Promotion of Science, Grants-in-Aid for Scientific Research Grant-in-Aid for Scientific Research (A), Grant-in-Aid for Scientific Research (A), Kobe University, 01 Apr. 2019 - 31 Mar. 2023, Principal investigator単一の光子から複数の三重項励起子を生むシングレットフィッション(一重項分裂)は有機薄膜太陽電池において飛躍的に高い光エネルギー変換効率をもたらす現象として世界的に注目されている。本研究では、時間分解電子スピン共鳴法をベースに世界最高性能の空間分解能を持つ中間体構造解析の画期的ツールとして独自に開発してきた「電子スピン分極イメージング法」を主たる手法とし、時々刻々と変化する多重励起子や光電荷分離状態の立体配置とその分子運動効果をナノ秒領域の三次元動画 (映像化)として実験的に特徴づけた。分子内シングレットフィッション系では、強く相関した多重励起子からの電子的相互作用による束縛を解く際にかかるねじれ振動モードと周波数を具体的に特徴づけるとともに、それによる解離多重励起子の立体構造の変化も明らかにした。さらに励起子解離による立体構造変化の分子論起源は不明であった。本研究では、電子構造論に基づき双性イオン構造による束縛励起子対からのテラヘルツ振動による開放として、具体的に記述することもできた。動物による磁気コンパスの働きを持つものの起源と考えられているクリプトクロムにおいては、光誘起電荷分離過程で生成する電荷分離状態の立体構造と配位水のゆらぎ分子運動による電子伝達機構の詳細を明らかにした。以上より、結晶性と非晶性を併せ持つ有機エレクトロニクス薄膜や生体タンパク質のエントロピー効果と運動による電子的効果を用いるデバイス効率飛躍的向上化の知的基盤を獲得し、有機薄膜太陽電池開発で課題となっている超高効率化への指針を提示することができるようになってきた。Competitive research funding
- Japan Society for the Promotion of Science, Grants-in-Aid for Scientific Research Grant-in-Aid for Challenging Research (Exploratory), Grant-in-Aid for Challenging Research (Exploratory), Kobe University, 30 Jul. 2020 - 31 Mar. 2022Quantum Teleportation via Singlet FissionWe have characterized spin entanglement transportations in the singlet-quintet multiexciton spin system by using the time-resolved electron paramagnetic resonance (TREPR) detections for several singlet-fission reaction systems. We have newly constructed a spin correlated triplet-pair model to account for the electron spin polarization observed in the spin states generated by the transportations of the spin entanglement via the dissociation of the singlet and quintet strongly coupled multiexciton composed of the four qubits system resulting in the two of the individual triplet excitons. Using this model, we have elucidated the quantum mechanical spin teleportation of the multiexcitons caused by vibration motions in the strongly coupled multiexcitons to weaken the spin-spin exchange interactions generating the weakly coupled multiexcitons resulting in the conformation changes in the individual triplet chromophores.
- Japan Society for the Promotion of Science, Grants-in-Aid for Scientific Research Grant-in-Aid for Scientific Research (A), Grant-in-Aid for Scientific Research (A), Kobe University, 01 Apr. 2019 - 31 Mar. 2022Researchers in Japan have developed semiconductor photocatalysts highly efficient for the overall water splitting reaction to produce H2 and O2. Why are they active? This is the fundamental question that drives this three-year research project. We developed two methods for characterization of photocatalysts working under water. Time-resolved detection of O2 released into water was achieved with platinum microelectrode. Infrared light absorption of photocatalyst particles irradiated with ultraviolet light for excitation was monitored on a diamond prism. The developed methods were successfully applied to NaTaO3 and SrTiO3 photocatalysts.Competitive research funding
- Japan Society for the Promotion of Science, Grants-in-Aid for Scientific Research Grant-in-Aid for Challenging Research (Exploratory), Grant-in-Aid for Challenging Research (Exploratory), Kobe University, 30 Jun. 2017 - 31 Mar. 2020, Principal investigatorWe have developed a novel method of “3D spin polarization imaging” by which the anisotropic spin polarization is mapped to all possible magnetic field directions from the powder-pattern time-resolved electron paramagnetic resonance (EPR) spectra to obtain geometries of the photoinduced primary charge-separated (CS) state of quinone pre-reduced membranes of plant PSII from spinach in frozen solution and in oriented multilayers at 77 K. For this we have observed the primary CS states using an X-band time-resolved EPR method. From the imaging maps, we have characterized cofactor geometries and electronic coupling of the photoinduced primary CS state. It has been revealed that that the electronic coupling between the charges is significantly weak in the CS state separated by 1.5 nm, showing an importance of regulated cofactor-cofactor electronic interaction between a vinyl substituent and an accessory chlorophyll to inhibit the energy-wasting charge-recombination.Competitive research funding
- Japan Society for the Promotion of Science, Grants-in-Aid for Scientific Research Grant-in-Aid for Scientific Research (B), Grant-in-Aid for Scientific Research (B), Kobe University, 01 Apr. 2016 - 31 Mar. 2019, Principal investigatorTo understand the mechanism of navigating the Earth magnetic field by animals, we have clarified atomic-scale conformation changes in oxidized tryptophan residue in photoinduced charge-separated (CS) state in cryptochrome by using time-resolved electron paramagnetic resonance measurements with applying site directed mutagenesis for Xenopus laevis cryptochrome (Xcry) DASH. The intermediate charge-separated state as the secondary radical ion pair between reduced flavin adenine dinucleotide (FAD-) and the tryptophan377 (W377+) was characterized together with the terminal radical pair of FAD--W324+. The relative position and the orientation of the charges were precisely determined by our recently developed tool of the electron spin polarization imaging derived by the magnetophotoselection measurement at low temperature. We have clarified that the conformation changes in W377+ play important role for the hole-transfer reaction from the secondary intermediate of FAD--W377+.Competitive research funding
- Japan Society for the Promotion of Science, Grants-in-Aid for Scientific Research Grant-in-Aid for Scientific Research (A), Grant-in-Aid for Scientific Research (A), Kobe University, 01 Apr. 2016 - 31 Mar. 2019Sodium tantalate (NaTaO3) is the first semiconductor photocatalyst which produces hydrogen-oxygen mixed bubbles in the overall water splitting reaction, when properly doped with metal cations. This research project has been organized to answer the question of why doping with metal cations raised the quantum efficiency of the reaction. In-depth studies focused on Sr cation doping revealed that the electron-hole recombination rate was reduced when Ta cations were exchanged with Sr cations. Sodium cations were simultaneously exchanged to balance the cationic and anionic charges to form NaTaO3-Sr(Sr1/3Ta2/3)O3 solid solution. In addition, the intra-particle distribution of Sr cations played an essential role. Strontium cations segregated to produce graded composition from the Sr-rich surface to the Sr-poor core. The bottom of the conduction band lifted up at the Sr-rich surface, and the excited electrons were driven to the Sr-poor core leaving holes at the surface.Competitive research funding
- Japan Society for the Promotion of Science, Grants-in-Aid for Scientific Research Grant-in-Aid for Challenging Exploratory Research, Grant-in-Aid for Challenging Exploratory Research, Kobe University, 01 Apr. 2014 - 31 Mar. 2017, Principal investigatorIn recent years, great attentions have been attracted on the perovskite solar cells as the next generation thin-film photovoltaics that can be low-cost, flexible and light. In this study, we observed photoinduced separated charges in the photoactive layers in the perovskite (CH3NH3PbI3) solar cells by using the time-resolved electron paramagnetic resonance spectroscopy for the three layer thin films (Spiro-OMeTAD/CH3NH3PbI3/TiO2 on a glass substrate) composed of the organic hole transport layer (Spiro-OMeTAD), the CH3NH3PbI3 layer and the mesoporous TiO2 fabricated by spin coating method on the mesoporous TiO2 films. We have characterized the spin density distributions of the trapped holes of the CH3NH3PbI3 layer at 110 K. Furthermore, from the ESP generated in the trapped hole, we have estimated the J coupling in the primary electron-hole pairs which will give us an insight on the electronic coupling of the Wannier excitons.Competitive research funding
- Japan Society for the Promotion of Science, Grants-in-Aid for Scientific Research Grant-in-Aid for Challenging Exploratory Research, Grant-in-Aid for Challenging Exploratory Research, Kobe University, 01 Apr. 2014 - 31 Mar. 2016Photoexcited NaTaO3 photocatalysts observed with time-resolved ESR(1) Time-resolved electron spin resonance spectra of Sr-doped NaTaO3 photocatalysts were observed. A microwave absorption induced by bandgap excitation was identified at g=1.995 with an absorption line width of 2 mT. (2) Sr-doped NaTaO3 photocatalysts produced core-shell structured NaTaO3-SrSr1/3Ta2/3O3 solid solution. The photocatalysts were chemically etched to examine the different roles of the core and shell with respect to the recombination of electrons and holes. Under excitation by Hg-Xe lamp irradiation, the steady-state population of electrons in the core-shell-structured photocatalyst with a bulk Sr concentration of 5 mol% increased by 130 times relative to that of the undoped photocatalyst. During etching for the first 10 min, the shell detached from the top of the core, and the electron population in the uncovered core further increased by 40%. This population enhancement indicates that electrons are excited in the core and recombined in the shell.
- Japan Society for the Promotion of Science, Grants-in-Aid for Scientific Research Grant-in-Aid for Scientific Research (B), Grant-in-Aid for Scientific Research (B), Kobe University, 01 Apr. 2013 - 31 Mar. 2016, Principal investigatorWe have developed a method to analyze geometries and molecular orientations of photoinduced charge-separated states by detections of the magnetic interactions by using the time-resolved paramagnetic resonance (TREPR) methods. We have employed multi-frequency TREPR spectroscopy to characterize the geometries and the electronic coupling of the photoinduced primary charge-separated states generated in the photosynthetic reaction centers and in the photosystem II reaction center of spinach. We have clarified molecular mechanisms of the efficient charge generations and of the preventions of the energy-wasting charge-recombinations.Competitive research funding
- Japan Society for the Promotion of Science, Grants-in-Aid for Scientific Research Grant-in-Aid for Scientific Research (B), Grant-in-Aid for Scientific Research (B), Kyushu University, 01 Apr. 2012 - 31 Mar. 2015Development of imaging probe to detect lipid derived radicals from whole body to cellsLipid derived radicals and its metabolic products are closely involved in the pathogenesis of oxidative stress diseases such as inflammation and angiogenesis through the formation of protein or DNA complex. The starting point of lipid peroxide generation is lipid derived radicals which increase explosively via radical chain reaction. Therefore, the trapping of lipid derived radicals is useful to understanding the mechanism of formation of oxidative stress diseases, and to suppress the following chain reaction. On the other hands, nitroxides having stable unpaired electron allows spin trapping with carbon-centered radicals. Hence, in this study, we aimed to develop and evaluate lipid derived detection method using profluorescent nitroxide switching methods.
- 戦略的創造研究推進事業 個人型研究さきがけ, 2013, Principal investigatorさきがけ「電子スピンコヒーレンスによる有機太陽電池基板の電子伝達機能の解明」Competitive research funding
- Japan Society for the Promotion of Science, Grants-in-Aid for Scientific Research Grant-in-Aid for Scientific Research (C), Grant-in-Aid for Scientific Research (C), Shizuoka University, 2010 - 2012Electron Transport Functions for Solar Energy Conversions in Nanometer-Scaled Organic Molecular SystemsFor development of the molecular solar-energy conversion systems, it is crucial to investigate how both the molecular geometry and the electronic structure of electron donor-acceptor (D-A) molecules contribute to the electronic coupling for the charge-separation (CS) and for the charge-recombination (CR) processes. In this study, we have developed theoretical methods to analyze the electron spin polarization detected by the time-resolved electron paramagnetic resonance (TREPR) spectroscopy for D-A systems to systematically characterize both the molecular geometry and the electronic coupling of the photoinduced charge-separated state inthe electron donor-acceptor (D-A) molecular systems for several D-A systems in photoactive proteins and in the active layers of the organic thin-film solar cells.
- Japan Society for the Promotion of Science, Grants-in-Aid for Scientific Research Grant-in-Aid for Scientific Research (C), Grant-in-Aid for Scientific Research (C), Shizuoka University, 2007 - 2009Enzyme Activation Mechanism Probed by Photoinduced Radical Generation in Proteins Related to Nucleotides結核菌のカタラーゼ-ペロキシダーゼ(KatG)酵素における酵素反応初期過程を時間分解電子スピン共鳴法で室温において観測した。KatG-アントラキノンスルフォン酸イオン(薬物)の複合体において、レーザー光照射による光誘起電子移動反応を観測し、メチオニンカチオンラジカルと電子受容した薬物のアニオンラジカルで構成されるスピン相関ラジカル対をナノ秒領域で観測することに成功した。この薬物はKatGヘムポケット内部に存在し、近傍のヘム、トリプトファン、チロシン残基を介して高速の電荷分離過程が起こっていることが明らかになった。
- 日本学術振興会, 科学研究費助成事業 若手研究(B), 若手研究(B), 東北大学, 2001 - 2002光合成系分子のイノメートル電子移動反応における溶媒和形態変化液体中の遠距離電子移動系において、中間体ラジカルイオン対を取り巻く溶媒分子のナノスケール環境場からどのように静電的相互作用を受けているかを分子論的に解明することを目的とした。 光合成反応中心を構成するような比較的大きなサイズの分子として、亜鉛ポルフィリン-デュロキノン系に特に注目し、レーザー励起時間分解EPR法によりこれまで正確な測定が不可能であったクロロフィルやフラーレン分子の光誘起電子移動で生成する異常電子スピン分極を直接検出し、ラジカル対の電子スピン分極機構から、1ナノメートル程度の遠距離電子移動系における再配向エネルギー、一重項-三重項エネルギー差(J)の符号を得るため、溶質や溶媒に固有の値として精密にしかも一義的に定量した。 Jにおける電荷移動相互作用機構から、溶媒の極性や温度を変化させて電荷再結合自由エネルギーをチューニングすることによって符号が変化する結果を得られれば、J=0なる溶媒中でドナー、アセプターそれぞれの酸化還元電位を測定することにより、系に固有の再配向エネルギーλが一義的に決定される。そのため、数多くの溶質、溶媒系で測定し、溶質分子サイズ、溶質立体構造、置換基、溶媒極性などの効果を系統的に調べた。それぞれの分子系でマーカスの連続誘電体モデルがよく成り立っていることが明かとなった。
- 日本学術振興会, 科学研究費助成事業 萌芽的研究, 萌芽的研究, 東北大学, 1999 - 1999溶媒和ラジカルイオン対の交換相互作用検出による再配向エネルギーの精密測定光誘起電子移動反応過程の反応性を大きく支配する溶媒再配向エネルギーの値を精密に測定することを目的として電子供与体-受容体ラジカルイオン対系について以下の研究を行った。 1.時間分解EPR法を用いた溶媒和ラジカルイオン対の一重項-三重項エネルギー差(J)検出による溶媒再配向エネルギーの決定 (1)電荷移動型相互作用によるラジカルイオン対のJの理論を構築し、電荷再結合自由エネルギーと全再配向エネルギーが一致する点を境にラジカル間距離が約12Å離れたイオン対のJの符号が変化することを示した。 (2)時間分解EPR法によるJの符号に対する溶媒極性や温度効果から、デュロキノン-N,N-ジメチルアニリン等の電子供与体-受容体系に固有の溶媒再配向エネルギーの値を種々の溶媒中で精度良く決定した。溶媒再配向エネルギーの値がベンゼン誘導体の置換基の種類によって大きく異なることが見出された。 (3)時間分解蛍光分光測定による電荷移動錯体蛍光スペクトルから接触イオン対系の溶媒再配向エネルギーを得ることにより、(2)の結論を裏付けた。 2.溶媒再配向エネルギーの分子論的描像 以上の溶媒再配向エネルギーに対する置換基効果の結果はMarcusの連続誘電体モデルでは説明することができない。ベンゼン誘導体のイオン化に伴う置換基の構造変化が溶質と第一溶媒和圏の溶媒分子との静電相互作用に大きな影響を与えるため、溶媒再配向エネルギーが置換基の種類によって大きく異なることが示唆された。
- 日本学術振興会, 科学研究費助成事業 奨励研究(A), 奨励研究(A), 東北大学, 1997 - 1998外部磁場による励起分子-ラジカル系の反応制御1) 時間分析EPR法によるラジカルイオン対の交換相互作用機構(電荷移動型交換相互作用)の発見 光誘起電子移動反応で生成する様々な溶媒和ラジカルイオン対の交換相互作用(J)の符号が電荷再結合自由エネルギーに依存することを初めて見出した。この結果を統一的に説明するものとして、電子移動反応理論に基づく新しい交換相互作用の機構(電荷移動型交換相互作用)を提唱した。この機構から、Jの符号、大きさについての理論を確立した。 2) 時間分解EPR法によるラジカル-三重項分子間の交換相互作用 ラジカルと励起三重項分子間の相互作用で生成する電子スピン分極に対する温度効果を観測した。ラジカル-三重項対機構による電子スピン分極生成理論を構築し、それに基づく解析から、ラジカル-三重項対のJの大きさを見積もった。励起三重項種によってJが大きく異なることを初めて見出した。Jの大きさは、ラジカル誘起三重項消光過程が電子交換反応により進む系では、電子移動反応により進む系よりも1桁以上大きく、Jは消光機構の違いにより大きく影響を受けることが分かった。これは、電荷移動型交換相互作用で見積もられるJの大きさからも支持された。 3) 磁場効果測定によるラジカル-三重項分子間の交換相互作用 ラジカルによる励起三重項消光過程に対する外部磁場効果を時間分解蛍光法や過渡吸収法により観測した。様々な励起分子および、ラジカル種において、消光過程に対する磁場効果が見出され、外部磁場による反応制御が可能であることが明らかになった。ラジカル-三重項対機構に基づき磁場効果生成理論を構築し、それによる解析から、磁場効果生成機構が初めて明らかになった。消光過程が電子交換反応により進む系では、電子移動反応により進む系よりもJが1桁以上大きいことが磁場効果測定により直接的に示され、ラジカル-三重項対の交換相互作用機構が定量的に明らかになった。