SUGIMOTO Hiroshi | ![]() |
Graduate School of Engineering / Department of Electrical and Electronic Engineering | |
Associate Professor | |
Engineering / Other Field |
Oct. 2021 神戸大学, 令和3年度 学長表彰
Nov. 2020 神戸大学, 優秀若手研究者賞・学長賞
Nov. 2017 応用物理学会, 応用物理学会講演奨励賞, コロイド状シリコンナノ粒子の広範囲サイズ制御とその光学特性
May 2013 European Materials Research Society, Young Scientist Award
The 19th International Microscopy Congress, Best Poster Award
Scientific journal
[Refereed]
Scientific journal
Scientific journal
Scientific journal
A dielectric core-metal shell nanosphere has attracted scientific and technological interests due to the unique optical resonances arising from the hybridization of surface plasmon modes and cavity modes. The previous studies focus on a low-index dielectric core without its own optical resonances. Here, optical resonances of a core-shell nanosphere with a high refractive index (n approximate to 4) core with the lowest order Mie resonances in the visible range are investigated theoretically and experimentally. Scattering and absorption spectra of a core-shell nanosphere for different values of the core refractive index are first analyzed, and there is a transition of the hybridization scheme around n approximate to 2. Above the value, a characteristic hybridized mode with strong absorption and weak scattering emerges in the near-infrared range. A core-shell nanosphere composed of a silicon core and a gold shell is prepared, and the resonance modes are studied by single particle scattering spectroscopy and electron energy loss spectroscopy (EELS) in a transmission electron microscope. The core-shell nanospheres exhibit the hybridized modes depending on the core diameter. The hybridized mode as well as the higher order one that is not observable in the scattering spectroscopy is observed in the EELS.
Wiley, 26 Sep. 2022, Small, 18 (45), 2204890 - 2204890, EnglishScientific journal
Controlling ultraviolet light at the nanoscale using optical Mie resonances holds great promise for a diverse set of applications, such as lithography, sterilization, and biospectroscopy. Access to the ultraviolet requires materials with a high refractive index and wide band gap energy. Here, the authors systematically search for such materials by computing the frequency-dependent optical permittivity of 338 binary semiconductors and insulators from first principles, and evaluate their scattering properties using Mie theory. This analysis reveals several interesting candidate materials among which boron phosphide (BP) appears most promising. Then BP nanoparticles are prepared and it is demonstrated that they support Mie resonances at visible and ultraviolet wavelengths using both far-field optical measurements and near-field electron energy-loss spectroscopy. A laser reshaping method is also presented to realize spherical Mie-resonant BP nanoparticles. With a refractive index over three and low absorption losses in a broad spectral range spanning from the infrared to the near ultraviolet, BP is an appealing material for a broad range of applications in dielectric nanophotonics.
Wiley, Aug. 2022, Advanced Optical Materials, 10 (16), 2200422 - 2200422, EnglishScientific journal
[Invited]
Scientific journal
Scientific journal
Scientific journal
[Refereed]
Scientific journal
Scientific journal
Scientific journal
The photoelectrochemical response of a photocathode made from a colloidal solution of boron (B) and phosphorus (P) codoped silicon (Si) quantum dots (QDs) 2-11 nm in diameters is studied. Since codoped Si QDs are dispersible in alcohol and water due to the hydrophilic surface, a photoelectrode with a smooth surface is produced by drop-coating the QD solution on an indium tin oxide substrate. The codoping provides high oxidation resistance to Si QDs and makes the electrode operate as a photocathode. The photoelectrochemical response of a Si QD photoelectrode depends strongly on the size of QDs; there is a transition from anodic to cathodic photocurrent around 4 nm in diameter. Below the size, anodic photocurrent due to self-oxidation of Si QDs is observed, while above the size, cathodic photocurrent due to electron transfer across the interface is observed. The cathodic photocurrent increases with increasing the size, and in some samples, it is observed for more than 3000 s under intermittent light irradiation.
{IOP} Publishing, 26 Nov. 2021, Nanotechnology, 32 (48), 485709 - 485709, English, International magazineScientific journal
Scientific journal
Scientific journal
Scientific journal
Scientific journal
Scientific journal
Scientific journal
Scientific journal
Scientific journal
Scientific journal
Scientific journal
Scientific journal
Scientific journal
Scientific journal
The photocatalytic hydrogen (H-2) generation by boron (B) and phosphorus (P) codoped silicon quantum dots (Si QDs) with diameters in the quantum confinement regime is investigated. The codoped Si QDs have an amorphous shell made from B, Si and P. The shell induces negative potential on the surface and makes codoped Si QDs dispersible in water. The hydrophilic shell offers enhanced stability and efficiency in photocatalytic H(2)generation and provides the opportunity to study the size dependence of the H(2)generation rate. A drastic increase of H(2)generation rate with decreasing QD size is observed. Analyses based on the Marcus theory reveal that the upper shift of the lowest unoccupied molecular orbital level of Si QDs by the quantum confinement effect is responsible for the enhanced photocatalytic activity.
ROYAL SOC CHEMISTRY, Aug. 2020, JOURNAL OF MATERIALS CHEMISTRY A, 8 (31), 15789 - 15794, English[Refereed]
Scientific journal
[Refereed]
Scientific journal
Luminescent solar concentrator (LSC) is a promising technology to integrate semitransparent photovoltaic (PV) systems into modern buildings and vehicles. Silicon quantum dots (QDs) are good candidates as fluorophores in LSCs, due to the absence of overlap between absorption and emission spectra, high photoluminescence quantum yield (PLQY), good stability, nontoxicity, and element abundance. Herein, LSCs based on Si QDs/polymer nanocomposites are fabricated in a triplex glass configuration. A special polymer matrix (off-stoichiometric thiol-ene, OSTE) is used, which improves Si nanocrystal quantum yield. Herein, a comprehensive investigation to improve the performance of LSCs by exploring different strategies under the guidance of a theoretical description is conducted. Among these strategies, the systematical enhancement of PLQY of the nanocomposite is achieved by tuning the thiol/allyl group ratio in the OSTE matrix. In addition, ligand selection and loading optimization for QDs reduce the total scattering loss in the device. Finally, an optical power efficiency of 7.9% is achieved for an optimized LSC prototype (9 x 9 x 0.6 cm(3), transmittance approximate to 62% at 500 nm) based on Si QDs/OSTE nanocomposite, which shows good potential of this material system in LSC fabrication.
WILEY-V C H VERLAG GMBH, Jun. 2020, SOLAR RRL, English[Refereed]
Scientific journal
A crystalline silicon (Si) nanoparticle (NP) of 100-200 nm in diameter exhibits a highly saturated color owing to Mie resonance, and can be a component to realize angle-insensitive structural color covering the entire visible range. However, to date, coloring a substrate by Si nanostructures has only been achieved in a very small area by using electron beam lithography and dry etching processes. In this work, a Si NP color ink capable of coloring a flexible substrate by a painting process is developed. The sphericity of Si NPs is very high; the circularity factor obtained from a transmission electron microscope image reaches 0.97. The average diameter of Si nanospheres is controlled from 95 to 200 nm, and the polydispersity defined by the standard deviation divided by the average diameter is as small as 6%. Because of the high sphericity, high crystallinity, high size purity, and perfect dispersion in solution, the Si nanosphere solutions exhibit vivid colors recognizable by naked eye in a range of blue to orange. The Si nanosphere color inks combined with a polymer binder are capable of coloring flexible substrates by a painting process.
WILEY-V C H VERLAG GMBH, Jun. 2020, ADVANCED OPTICAL MATERIALS, 8 (12), English[Refereed]
Scientific journal
[Refereed]
Scientific journal
Gel electrophoresis, which is a standard method for separation and analysis of macromolecules such as DNA, RNA and proteins, is applied for the first time to silicon (Si) quantum dots (QDs) for size separation. In the Si QDs studied, boron (B) and phosphorus (P) are simultaneously doped. Codoping induces a negative potential on the surface of a Si QD and makes it dispersible in water. Si QDs with different B and P concentrations and grown at different temperatures (950 degrees C-1200 degrees C) are studied. It is shown that native polyacrylamide gel electrophoresis can separate codoped Si QDs by size. The capability of gel electrophoresis to immobilize size-separated QDs in a solid matrix makes detailed analyses of size-purified Si QDs possible. For example, the photoluminescence (PL) studies of the dried gel of Si QDs grown at 1100 degrees C demonstrate that a PL spectrum of a Si QD solution with the PL maximum around 1.4 eV can be separated into more than 15 spectra with the PL maximum changing from 1.2 to 1.8 eV depending on the migration distance. It is found that the relationship between the PL peak energy and the migration distance depends on the growth temperature of Si QDs as well as the B and P concentration. For all the samples with different impurity concentrations and grown at different temperatures, a clear trend is observed in the relationship between the full width at half maximum (FWHM) and the peak energy of the PL spectra in a wide energy range. The FWHM increases with the increasing peak energy and it is nearly twice larger than those observed for undoped Si QDs. The large PL FWHM of codoped Si QDs suggests that excitons are further localized in codoped Si QDs due to the existence of charged impurities.
ROYAL SOC CHEMISTRY, Apr. 2020, NANOSCALE, 12 (16), 9266 - 9271, English[Refereed]
Scientific journal
The microstructure of boron (B) and phosphorus (P) codoped silicon (Si) nanocrystals (NCs), cubic boron phosphide (BP) NCs and their mixed NCs (BxSiyPz NCs) has been studied using atom probe tomography (APT), transmission electron microscopy (TEM), and Raman scattering spectroscopy. The BxSiyPz NCs inherit superior properties of B and P codoped Si NCs such as high dispersibility in aqueous media and near infrared (NIR) luminescence and those of cubic BP NCs such as high chemical stability. The microanalyses revealed that BxSiyPz NCs are composed of a crystalline core and an amorphous shell. The core possesses a lattice constant between that of Si (diamond-cubic) and BP (cubic). The amorphous shell is comprised of B, Si and P, though the composition is not uniform and there are local B-rich, Si-rich and P-rich domains connected contiguously. The amorphous shell is proposed to be responsible for their superior chemical properties such as high dispersibility in polar solvents and high resistance to acids, and the crystalline core is responsible for the stable NIR luminescence.
ROYAL SOC CHEMISTRY, Apr. 2020, NANOSCALE, 12 (13), 7256 - 7262, English[Refereed]
Scientific journal
Although the study of nonradiating anapoles has long been part of fundamental physics, the dynamic anapole at optical frequencies was only recently experimentally demonstrated in a specialized silicon nanodisk structure. We report excitation of the electrodynamic anapole state in isotropic silicon nanospheres using radially polarized beam illumination. The superposition of equal and out-of-phase amplitudes of the Cartesian electric and toroidal dipoles produces a pronounced dip in the scattering spectra with the scattering intensity almost reaching zero-a signature of anapole excitation. The total scattering intensity associated with the anapole excitation is found to be more than 10 times weaker for illumination with radially vs linearly polarized beams. Our approach provides a simple, straightforward alternative path to realizing nonradiating anapole states at the optical frequencies.
AMER PHYSICAL SOC, Mar. 2020, PHYSICAL REVIEW LETTERS, 124 (9), English[Refereed]
Scientific journal
[Refereed]
Scientific journal
Scientific journal
Scientific journal
Resonant excitation and manipulation of complex interactions among two or more resonances in high-index dielectric nanostructures provide great opportunities for engineering novel optical phenomena and applications. However, difficulties often arise when interpreting the observed spectra because of the overlap of the broad resonances contributed by many factors such as particle size, shape, and background index. Therefore, selective excitation of resonances that spectrally overlap with each other provides a gateway towards an improved understanding of the complex interactions. Here, we demonstrate selective excitation and enhancement of multipolar resonances of silicon nanospheres using cylindrical vector beams (CVBs) with different diameters of nanospheres and numerical apertures (NAs) of the excitations. By combining single particle spectroscopy and electrodynamic simulations, we show that the radially polarized beam can selectively excite the electric multipoles, whereas the azimuthally polarized beam can selectively excite the magnetic multipoles even though multipolar resonances are convoluted together due to their spectral overlap. Moreover, focusing the CVBs with high NA can lead to a dominant longitudinal polarization of the electric or magnetic field. We show that the enhanced longitudinal polarization with increasing NA of the radially and azimuthally polarized beams can selectively enhance the electric and magnetic multipolar resonances, respectively. Our approach can be used as a spectroscopy tool to enhance and identify multipolar resonances leading to a better understanding of light-matter interactions in other dielectric nanostructures as well as serve as a first step toward excitation of dark mode and Fano resonances in dielectric oligomers by breaking the symmetry of the nanostructures. Published under license by AIP Publishing.
AMER INST PHYSICS, Jan. 2020, JOURNAL OF APPLIED PHYSICS, 127 (3), English[Refereed]
Scientific journal
It has been demonstrated recently that a nanowire (NW) of high refractive index dielectric materials works as a nanoantenna because of the excitation of the Mie-type resonances. Here, we explore the capability of a silicon (Si) NW as an optical nanoantenna by combining it with an external metallic component. We investigate the light scattering property of a single Si NW placed on a gold (Au) mirror via a very thin dielectric spacer and demonstrate strong confinement of electromagnetic fields in the gap because of the coupling of the resonance modes with a Au mirror. We demonstrate that the resonance wavelength of the hybrid mode can be tuned by the gap length, and the hybrid gap mode strongly modifies the spectral shape of the emission from a quantum dot (QD) monolayer incorporated in the gap. Quantitative analyses of the data in combination with numerical simulations reveal that the enhancement and the polarization control of the QD emission are achieved by the coupling.
AMER CHEMICAL SOC, 2020, ACS Applied Nano Materials, 3 (7), 7223 - 7230, English[Refereed]
Scientific journal
© 2019 Author(s). Nanoimprinting followed by metal deposition is a low-cost, high-throughput, and highly reproducible process for the fabrication of large-size plasmonic substrates required for commercial products. However, the plasmonic substrates prepared by the process usually have very broad surface plasmon resonances, which cannot be well reproduced by numerical simulations. The poor agreement between experiments and calculations has prevented the detailed analysis of the field enhancement behavior and the improvement of the performance as plasmonic substrates. In this work, we demonstrate that large-area plasmonic substrates with sharp surface plasmon resonances, which can be well reproduced by numerical simulations, are produced by sputter-deposition of gold (Au) on a commercially available nanoimprinted substrate. The good agreement between experiments and simulations allow us to identify the locations and field distributions of the hot spots. The angle dependence of specular reflectance and diffuse reflectance measurements in combination with numerical simulations reveal that a dipolelike bright mode and a higher-order dark mode exist at gaps between Au nanorods. Finally, we demonstrate the application of the developed plasmonic substrates for surface-enhanced fluorescence in sandwich immunoassays for the detection of influenza virus nucleoprotein. We show that the sharp resonance and the capability of precise tuning of the resonance wavelength significantly enhance the luminescence signal.
AMER INST PHYSICS, 14 Dec. 2019, Journal of Applied Physics, 126 (22), English[Refereed]
Scientific journal
[Refereed]
Scientific journal
Copyright © 2019 American Chemical Society. A stand-alone plasmonic nanocomposite into which a metal nanostructure and an emitting material are integrated is a promising building block for optoelectronics and biophotonics devices. Here, we present the plasmonic property of a nanocomposite composed of a Au elongated nanocap and a β-NaYF4 dielectric nanorod. We show that elongation of a Au nanocap results in splitting of the magnetic dipole resonance, and the resonance wavelengths can be controlled in a wide wavelength range by the aspect ratio. As an application of the elongated nanocap, we demonstrate strong enhancement of the near-infrared to visible upconversion of an Er3+ and Yb3+ doped β-NaYF4 nanorod by tuning the resonance wavelength of a Au nanocap placed on it to the excitation wavelength.
24 Oct. 2019, Journal of Physical Chemistry C, 123 (42), 25809 - 25815, English[Refereed]
Scientific journal
[Refereed]
Scientific journal
[Refereed]
Scientific journal
[Refereed]
Scientific journal
Copyright © 2019 American Chemical Society. Cubic boron phosphide (BP) is an indirect band gap semiconductor with a band gap of 2.0 eV and promising for a highly stable photocatalyst to produce hydrogen from water under visible light irradiation. Here, we performed a comprehensive study on the energy-level structure and photocatalytic activity of BP nanocrystals (NCs) in the quantum confinement regime (<5 nm in diameter). First, we calculated the electronic structure of cubic BP NCs up to 2.8 nm in diameter, hexagonal BP nanoflakes, and cubic/hexagonal BP nanostructures by density functional theory and time-dependent density functional theory. We then synthesized BP NCs with 2-13 nm in diameters and performed detailed structural analyses and optical measurements. The photocatalytic bleaching experiments for dye molecules under visible light irradiation revealed that the bleaching rate depends strongly on the size of BP NCs; the increase in the band gap of BP NCs by the quantum size effects (QSE) enhanced the photocatalytic activity. The band gap increase by the QSE also enhanced the rate of photocatalytic hydrogen evolution in water.
19 Sep. 2019, Journal of Physical Chemistry C, 123 (37), 23226 - 23235, English[Refereed]
Scientific journal
© The Author(s) 2019. A process for bioconjugation of an IgG antibody and silicon quantum dots (Si-QDs) having the luminescence in the near-infrared (NIR) range was developed. For the bioconjugation, the surface of water-soluble all-inorganic Si-QDs was functionalized by using silane-coupling agents. In amino-functionalized Si-QDs, successful conjugation was achieved without strongly affecting the luminescence property. Detailed analyses revealed that Si-QDs are bound covalently to both the light and heavy chains of an IgG antibody. It was also confirmed that the binding property of an IgG antibody with antigen nucleoprotein was not ruined by the process. The successful conjugation of an IgG antibody and NIR luminescent Si-QDs paves the way for designing environmentally friendly bio-sensing and -imaging processes.
CAMBRIDGE UNIV PRESS, 01 Sep. 2019, MRS Communications, 9 (3), 1079 - 1086, English[Refereed]
Scientific journal
[Refereed]
Scientific journal
[Refereed]
Scientific journal
The antimicrobial activity of a hybrid nanoparticle (NP) composed of a silver (Ag) NP core decorated with silicon (Si) nanocrystals (NCs) on the exterior (Ag/Si NPs) is evaluated.
2019, RSC Advances, 9 (27), 15171 - 15176, English[Refereed]
Scientific journal
© 2018 American Chemical Society. Shallow impurity doping is an efficient route to tailor optical and electronic features of semiconductor quantum dots (QDs). However, the effect of doping is often smeared by the size, shape, and composition inhomogeneities. In this paper, we study optical properties of almost monodispersed spherical silicon (Si) QDs that are heavily doped with boron (B) and phosphorus (P). The narrow size distribution achieved by a size-separation process enables us to extract doping-induced phenomena clearly. The degree of doping-induced shrinkage of the optical band gap is obtained in a wide size range. Comparison of the optical band gap with theoretical calculations allow us to estimate the number of active donor-acceptor pairs in a QD. Furthermore, we found that the size and detection energy dependence of the luminescence decay rate is significantly modified below a critical diameter, that is ∼5.5 nm. In the diameter range above 5.5 nm, the luminescence decay rate is distributed in a wide range depending on the detection energy even in size-purified Si QDs. The distribution may arise from that of donor-acceptor distances. On the other hand, in the diameter range below 5.5 nm the detection energy dependence of the decay rate almost disappears. In this size range, which is smaller than twice of the effective Bohr radius of B and P in bulk Si crystal, the donor-acceptor distance is not a crucial factor to determine the recombination rate.
American Chemical Society ({ACS}), 14 Nov. 2018, Nano Letters, 18 (11), 7282 - 7288, English[Refereed]
Scientific journal
© 2018 OSA - The Optical Society. All rights reserved. We fabricate the colloidal Si nanoantenna exhibiting efficient Mie resonances in optical regime. The hybrid nanogap antenna structures prepared by a bottom-up approach showed the Purcell enhanced emission of QD layer integrated in the gap.
2018, Optics InfoBase Conference Papers, Part F125-JSAP 2018[Refereed]
International conference proceedings
[Refereed]
Scientific journal
[Refereed]
Scientific journal
[Refereed]
Scientific journal
[Refereed]
Scientific journal
[Refereed]
Scientific journal
[Refereed]
Scientific journal
[Refereed]
Scientific journal
[Refereed]
Scientific journal
[Refereed]
Scientific journal
[Refereed]
Scientific journal
[Refereed]
Scientific journal
[Refereed]
Scientific journal
[Refereed]
Scientific journal
[Refereed]
Scientific journal
[Refereed]
Scientific journal
[Refereed]
Scientific journal
[Refereed]
Scientific journal
[Refereed]
Scientific journal
[Refereed]
Scientific journal
[Refereed]
Scientific journal
[Refereed]
Scientific journal
[Refereed]
Research institution
[Refereed]
Scientific journal
[Refereed]
Scientific journal
[Refereed]
Scientific journal
[Refereed]
Scientific journal
[Refereed]
Scientific journal
[Refereed]
Scientific journal
[Refereed]
Scientific journal
[Refereed]
Scientific journal
[Refereed]
Scientific journal
[Refereed]
Scientific journal
[Refereed]
Scientific journal
[Refereed]
Scientific journal
[Refereed]
Scientific journal
[Refereed]
Scientific journal
[Refereed]
Scientific journal
[Refereed]
Scientific journal
[Refereed]
Scientific journal
[Refereed]
Scientific journal
[Refereed]
Scientific journal
[Refereed]
Scientific journal
[Refereed]
Scientific journal
[Refereed]
Scientific journal
[Refereed]
Scientific journal
[Refereed]
Scientific journal
[Refereed]
Scientific journal
[Refereed]
Scientific journal
[Refereed]
Scientific journal
[Refereed]
Scientific journal
The surface structure of P and B codoped colloidal Si-NCs are studied by photoluminescence (PL) in hydrofluoric acid (HF) solution and X-ray photoelectron spectroscopy (XPS). We find that codoped Si-NCs are much more stable in HF solution than undoped, P-doped, and B-doped Si-NCs. The PL study combined with XPS results reveal that a high B concentration layer is formed on the surface of codoped Si-NCs and the layer acts as a kind of inorganic atomic ligands for Si-NCs. The high B concentration layer makes Si-NCs hydrophilic and dispersible in polar liquids. Furthermore, the layer effectively protects Si-NCs from oxidation in solution and in air. © 2013 American Chemical Society.
Apr. 2013, Journal of Physical Chemistry C, 117 (13), 6807 - 6813, English[Refereed]
Scientific journal
[Refereed]
Scientific journal
We demonstrate the formation of a new type of surfactant-free colloidal silicon nanocrystal (Si-NC). The characteristic structural feature of the Si-NCs is simultaneous doping of phosphorus (P) and boron (B) in and on the surface of Si-NCs. The codoped Si-NCs are stable in methanol for more than a year and exhibit luminescence in the near-infrared range. We perform comprehensive studies on the structure of codoped colloidal Si-NCs and discuss the mechanism of the high solution dispersibility. © 2012 American Chemical Society.
23 Aug. 2012, Journal of Physical Chemistry C, 116 (33), 17969 - 17974, English[Refereed]
Scientific journal
[Refereed]
Scientific journal
Si nanocrystals (Si-NCs) dispersible in polar liquid without surface functionalization by organic molecules have been realized by simultaneously doping n and p type impurities. We show that the codoped Si-NCs are stable in methanol for more than five months, while intrinsic Si-NCs prepared by the same procedure form large agglomerates. The different behavior of the intrinsic and codoped Si-NCs in solutions suggests that doped impurities exist on the surface of Si-NCs and the surface potential is large enough to prevent the agglomeration. The colloidal solution of codoped Si-NCs exhibits broad photoluminescence with the maximum in the near infrared range (1:1-1:3 eV). © 2011 Optical Society of America.
15 Oct. 2011, Optics Letters, 36 (20), 4026 - 4028, English[Refereed]
Scientific journal
[Refereed]
Scientific journal
Boron (B) doped Si nanocrystals (Si-ncs) dispersed in hydrofluoric (HF) acid solution are prepared by dissolving borosilicate films containing B-doped Si-ncs in HF solution. We find that the etching rate of B-doped Si-ncs is much smaller than that of undoped Si-ncs. The difference of the etching rate allows us to extract only doped Si-ncs in the mixture of doped and undoped Si-ncs and observe the photoluminescence (PL) due to the transition from the conduction band to the acceptor state. The PL was very broad with the maximum around 1.15 eV. From the analysis of the PL data obtained for the samples prepared under different conditions and different etching time, preferential doping sites of B atoms are estimated. The data suggests that B-doped Si-ncs consists of intrinsic cores and heavily B-doped shells. © 2011 American Institute of Physics.
15 Sep. 2011, Journal of Applied Physics, 110 (6), 063528, English[Refereed]
Scientific journal
[Refereed]
Scientific journal
[Refereed][Invited]
[Invited]
[Refereed][Invited]
Introduction scientific journal
[Invited]
[Invited]
[Refereed]
Report scientific journal
Scholarly book
Scholarly book
Scholarly book
Scholarly book
Oral presentation
Oral presentation
Oral presentation
Poster presentation
Poster presentation
Poster presentation
Poster presentation
Poster presentation
Poster presentation
Oral presentation
Poster presentation
Poster presentation
Oral presentation
Oral presentation
Oral presentation
Oral presentation
Oral presentation
Oral presentation
Oral presentation
Oral presentation
Poster presentation
Poster presentation
[Invited]
Oral presentation
Oral presentation
Oral presentation
[Invited]
Oral presentation
Oral presentation
Oral presentation
Oral presentation
Oral presentation
Oral presentation
Poster presentation
Oral presentation
Poster presentation
Oral presentation
Poster presentation
Invited oral presentation
Poster presentation
Oral presentation
Oral presentation
Oral presentation
Poster presentation
Poster presentation
Oral presentation
Oral presentation
Oral presentation
Oral presentation
[Invited]
Invited oral presentation
Oral presentation
Oral presentation
Oral presentation
Poster presentation
Oral presentation
Oral presentation
Oral presentation
Oral presentation
Oral presentation
Oral presentation
Oral presentation
Oral presentation
Poster presentation
Oral presentation
Oral presentation
Oral presentation
Oral presentation
Oral presentation
Poster presentation
Poster presentation
Poster presentation
Poster presentation
Oral presentation
Poster presentation
Oral presentation
Oral presentation
Oral presentation
Public symposium
Public symposium
Public symposium
Public symposium
Poster presentation
Public symposium
Public symposium
半導体量子ドットへの不純物ドーピング技術は、量子効果に起因する特性をさらに高度化するための有望な手段である。本研究では、不純物ドーピングに加えて化学ドーピングを量子ドットに適用した技術により、シリコン量子ドットの高機能化と新機能創出を実現することを目的としている。本年度は,個々のドーピング技術に関して実験的な検討を行い、以下のi)-v)の成果を得た。i)置換型不純物ドーピングに関して、不純物濃度制御による発光波長制御および発光効率の改善に成功した。ii)不純物ドープシリコン量子ドットの成長初期段階のラマン散乱スペクトルおよび透過型電子顕微鏡観察を行い、成長メカニズムに関して知見を得た。iii)NREL(アメリカ合衆国)のグループと共同で、フェムト秒過渡吸収分光法により不純物ドープシリコン量子ドットの光励起キャリアダイナミクスを調べ、量子ドット内の自由キャリアの有無とサイズの関係を明らかにした。iv)貧溶媒添加法によるサイズ分離技術により、シリコン量子ドットのサイズ分布を10%以下に抑制し、発光線幅の抑制に成功した。また、ドナー・アクセプタ対発光のピークエネルギーと再結合レートのサイズ依存性を定量的に決定した。v)化学ドーピングの基礎技術として、電子供与体である亜硫酸イオンを溶解した液中のシリコン量子ドットの発光特性を詳細に調べ、亜硫酸イオンから量子ドットへの電荷移動により光励起により生成した余剰キャリアを補償できることを明らかにした。
本年度は、シリコンナノ結晶コロイドの基礎物性解明及び大面積電子デバイス・バイオフォトニクス応用を念頭に研究を行った。不純物ドープシリコンナノ結晶の基礎物性解明の一環として、(i) 3次元アトムプローブトモグラフィー法による原子スケールでの不純物分布の解明、(ii) 単一シリコンナノ結晶の発光特性解明に関する研究を行った。さらに、バイオ応用を見据えて、(iii) 生体分子を用いたシリコンナノ結晶-プラズモニックナノ粒子複合体形成、(iv) シリコンナノ結晶を用いたバイオイメージング応用実証に関する研究を行った。 (i) に関して、ニューサウスウェールズ大学・シドニー大学と共同で3次元アトムプローブによるシリコンナノ結晶内部の不純物分布を明らかにし、その粒径依存性や不純物の偏析状態を評価した。(ii) について、顕微分光法を用いて単一の不純物ドープシリコンナノ結晶の発光特性を評価した。これらの研究により、不純物ドープシリコンナノ結晶の構造及び発光起源が不純物をドープしていないナノ結晶と大きく異なることを明らかにした。 (iii) に関して、シリコンナノ結晶表面をアミノ基、チオール基で修飾し、DNAはハイブリダイゼーションにより金ナノ粒子と結合した。複合体は3-4倍の発光強度を示した。(iv)に関して、シリコンナノ結晶と骨芽細胞を24-48時間培養し、その毒性評価・発光特性評価を行った。シリコンナノ結晶は非常に毒性が低く、細胞内で長時間安定して近赤外発光を示すことを明らかにした。