Siナノドットの非線形光学特性変化に対する動力学的解析

• Project Area: Materials Design through Computics: Complex Correlation and Non-equilibrium Dynamics
• Project/Area Number: 25104716
• Research Category: Grant-in-Aid for Scientific Research on Innovative Areas (Research in a proposed research area)
• Allocation Type: Single-year Grants
• Review Section: Science and Engineering
• Research Institution: University of Tsukuba (2014); Osaka University (2013)
• Principal Investigator: 重田 育照 筑波大学, 数理物質系, 教授 (80376483)
• Project Period (FY): 2013-04-01 – 2015-03-31
• Project Status: Discontinued (Fiscal Year 2014)
• Budget Amount: ¥3,900,000 (Direct Cost: ¥3,000,000、Indirect Cost: ¥900,000); Fiscal Year 2014: ¥1,950,000 (Direct Cost: ¥1,500,000、Indirect Cost: ¥450,000); Fiscal Year 2013: ¥1,950,000 (Direct Cost: ¥1,500,000、Indirect Cost: ¥450,000)
• Keywords: 非線形光学応答量 / ジラジカル

Outline of Annual Research Achievements

物質にレーザー光のような非常に強い光が照射されると、光電場に非線形に応答する分極が観測される。この非線形光学応答特性に優れた材料は、超高速スイッチや大容量記憶装置等の光デバイスに利用される基盤物質として大変重要である。一方、現代の高度情報化社会を支える基盤物質の一つはシリコンであり、その微細化技術の進展により、ナノサイズのシリコンを合成できるようになってきた。その中でも半導体の超微粒子であるナノ結晶は、光学的・電気的・磁気的物性がサイズによって著しく変化し、分子や固体とは異なる挙動を示すため、新しい機能性材料として注目されている。本申請課題では、光応答メモリの実現に向けた基礎研究を行う。25年度は低次元周期系RSDFTおよびRS-CPMDのプログラム開発を行った。特に後者のRS-CPMDの研究開発に関しては、京コンピュータにおいて有機溶媒1600原子系のベンチマークを行い、1024CPU(8192cores)を用いて、1ステップ6秒程度、64CPUに対して30%のストロングスケーリングを達成した。これらの低次元周期系RSDFTおよびRS-CPMDに関しては、現在、論文をまとめている所である。また、光学材料の研究に関して、ジラジカル系の光吸収スペクトルを計算し、スピン平均を取ることで実験のスペクトルを再現することに成功し、その業績に関してはMolecularPhysics誌に掲載予定である。

Research Progress Status

26年度が最終年度であるため、記入しない。

Strategy for Future Research Activity

26年度が最終年度であるため、記入しない。

Research Products

• [Journal Article] Substitution effects on optical properties of iminonitroxide-substituted iminonitroxide diradical (2015)
  • Author(s): 中村亮太、重田育照、奥野克樹、長谷川美貴、福嶋真由子、鈴木修一、小嵜正敏、岡田恵次、中野雅由
  • Journal Title: Molecular Physics Volume: 113 Issue: 3-4 Pages: 267-273
  • DOI: 10.1080/00268976.2014.937777
  • Peer Reviewed
• [Journal Article] Open-Shell Character and Second Hyperpolarizabilities of One-Dimensional Chromium(II) Chains: Size Dependence and Bond-Length Alternation Effect (2014)
  • Author(s): H. Fukui, S. Takamuku, T. Yamada, K. Fukuda, T. Takebayashi, T. Shigeta, R. Kishi, B. Champagne, M. Nakano
  • Journal Title: Inorg. Chem. Volume: 53 Issue: 16 Pages: 8700-8707
  • DOI: 10.1021/ic501334p
  • Peer Reviewed / Acknowledgement Compliant
• [Journal Article] Theoretical studies of electronic structures, magnetic properties and electron conductivities of one-dimensional Nin (n= 3,5,7) com plexes (2013)
  • Author(s): Y. Kitagawa, T. Matsui, Y. Nakanishi, Y. Shigeta, T. Kawakami, M. Okumura and K. Yamaguchi
  • Journal Title: Dalton Transaction Volume: 42 Issue: 45 Pages: 16200-16208
  • DOI: 10.1039/c3dt51466h
  • Peer Reviewed
• [Journal Article] New Type of Organic-Inorganic Hybrid NLO-Phores with Large Off-Diagonal First Hyperpolarizability Tensors : A Two-Dimensional Approach (2013)
  • Author(s): Muhammad Shabbir, Hongliang Xu, Zhong-Min Su, Kotaro Fukuda, Ryohei Kishi, Yasuteru Shigeta and Masayoshi Nakano
  • Journal Title: Dalton Trans. Volume: 42 Issue: 42 Pages: 15053-15062
  • DOI: 10.1039/c3dt51331a
  • Peer Reviewed
• [Journal Article] Binding of a Positron to Nucleic Base Molecules and Their Pairs (2013)
  • Author(s): K. Koyanagi, Y. Kita, Y. Shigeta, M. Tachikawa
  • Journal Title: ChemPhysChem Volume: 14 Issue: 15 Pages: 3458-3462
  • DOI: 10.1002/cphc.201300549
  • Peer Reviewed
• [Journal Article] Finite-field method with unbiased polarizable continuum model for evaluation of the second hyperpolarizability of an open-shell singlet molecule in solvents (2013)
  • Author(s): 乾 智也、重田育照、奥野克樹、馬場剛史、岸 亮平、中野雅由
  • Journal Title: Journal of Compulational Chemistry Volume: 34 Issue: 27 Pages: 2345-2352
  • DOI: 10.1002/jcc.23395
  • Peer Reviewed
• [Journal Article] Non-empirical tuning of CAM-B3LYP functional in time-dependent density functional theory for excitation energies of diarylethene derivatives (2013)
  • Author(s): 奥野克樹、重田育照、岸 亮平、中野雅由
  • Journal Title: Chemical Physics Letters Volume: 585 Pages: 201-206
  • DOI: 10.1016/j.cplett.2013.09.013
  • Peer Reviewed
• [Journal Article] Photochromic Switching of Diradical Character : Design of Efficient Nonlinear Optical Switches (2013)
  • Author(s): 奥野克樹、重田育照、岸亮平、中野雅由
  • Journal Title: The Journal of Physical Chemistry Letters Volume: 4 Issue: 15 Pages: 2418-2422
  • DOI: 10.1021/jz401228c
  • Peer Reviewed
• [Journal Article] A Density Functional Theory Based Protocol to Compute the Red ox Potential of Transition Metal Complex with the Correction of Pseudo-Counter Ion : General Theory and Applications (2013)
  • Author(s): T. Matsui, Y. Kitagawa, Y Shigeta, and M. Okumura
  • Journal Title: Journal of Chemical Theory and Computation Volume: 9 Issue: 7 Pages: 2974-2980
  • DOI: 10.1021/ct4002653
  • Peer Reviewed
• [Journal Article] Atom-Scale Reaction Pathways and Free-Energy Landscapes in Oxygen Plasma Etching of Graphene (2013)
  • Author(s): K. Koizumi, M. Boero, Y. Shigeta, and A. Oshiyama
  • Journal Title: J. Phys. Chem. Letters Volume: 4 Issue: 10 Pages: 1592-1592
  • DOI: 10.1021/jz400666h
  • Peer Reviewed
• [Journal Article] Antidot Effects on the Open-Shell Characters and Second Hyperpolarizabilities of Rectangular Graphene Nanoflakes (2013)
  • Author(s): Kyohei Yoneda
  • Journal Title: Int J. Quantum Chem. Volume: 113 Issue: 4 Pages: 605-611
  • DOI: 10.1002/qua.24089
  • Peer Reviewed
• [Journal Article] Synthesis and Characterization of Quarteranthene : Elucidating the Characteristics of the Edge State of Graphene Nanoribbons at the Molecular Level (2013)
  • Author(s): Akihito Konishi
  • Journal Title: Journal of American Chemical Society Volume: 135 Issue: 4 Pages: 1430-1437
  • DOI: 10.1021/ja309599m
  • Peer Reviewed
• [Journal Article] Consistent Scheme for Computing Standard Hydrogen Electrode and Redox Potentials (2013)
  • Author(s): Toru Matsui, Yasutaka Kitagawa, Mitsutaka Okumura, Yasuteru Shigeta, and Shigeyoshi Sakaki
  • Journal Title: Journal of Computational Chemistry Volume: 34 Issue: 1 Pages: 21-26
  • DOI: 10.1002/jcc.23100
  • Peer Reviewed
• [Journal Article] Interplay between the Diradical Character and Third-Order Nonlinear Optical Properties in Fullerene Systems雑 誌 名 (2013)
  • Author(s): Shabbir Muhammad
  • Journal Title: Chem. Eur. J. Volume: 19 Issue: 5 Pages: 1677-1685
  • DOI: 10.1002/chem.201203463
  • Peer Reviewed
• [Journal Article] Diradicalology in Third-Order Nonlinear Optical Systems : Second Hyperpolarizabilities of Acetylene-Linked Phenalenyl-Based Superpolyenes (2012)
  • Author(s): Masayoshi Nakano, Hitoshi Fukui
  • Journal Title: Int.J.Quantum Chem. Volume: (in press) Issue: 4 Pages: 585-591
  • DOI: 10.1002/qua.24035
  • Peer Reviewed
• [Journal Article] Comparative Study of Diradical Characters and Third-Order Nonlinear Optical Properties of Linear/Cyclic Acenes Versus Phenylenes (2012)
  • Author(s): S.Muhammad, T.Minami, et al
  • Journal Title: International Journal of Quantum Chemistry Volume: (in press) Issue: 4 Pages: 592-598
  • DOI: 10.1002/qua.24032
  • Peer Reviewed
• [Journal Article] Functional Dependence of Excitation Energy for Pentacene/C60 Model Complex in the Nonempirically Tuned Long-Range Corrected Density Functional Theory (2012)
  • Author(s): T.Minami, et al
  • Journal Title: International Journal of Quantum Chemistry Volume: (In press) Issue: 3 Pages: 252-256
  • DOI: 10.1002/qua.24023
  • Peer Reviewed
• [Presentation] Computational Studies on Redox Potential of Metal Complexes and Model Cofactors (2014)
  • Author(s): Y. Shigeta
  • Organizer: International Conference on Synthetic Metals
  • Place of Presentation: Turku, Finland
  • Year and Date: 2014-06-30 – 2014-07-05
  • Invited
• [Presentation] Theoretical Studies on Reaction Mechanism of An Enzyme Cleaving Unnatural Amide Compound (2014)
  • Author(s): Yasuteru Shigeta
  • Organizer: Symposium on Molecular Science and Synthesis of Functional Molecules for Next Generation
  • Place of Presentation: 広島大学
  • Invited
• [Presentation] Quantum chemical studies for estimation of pKa and redox potential (2013)
  • Author(s): Yasuteru Shigeta
  • Organizer: 2nd World Congress on Petrochemistry and Chemical Engineering
  • Place of Presentation: San Antonio, USA
  • Invited
• [Presentation] Free Energy Analyses on Cluster Deformations by Cumulant Mechanics (2013)
  • Author(s): Yasuteru Shigeta
  • Organizer: 8th Congress of the International Society for Theoretical Chemical Physics
  • Place of Presentation: Budapest, Hungary
  • Invited
• [Presentation] 構造ゆらぎと化学反応に関する理論的研究 (2013)
  • Author(s): 重田育照
  • Organizer: 分子科学会奨励賞受賞講演
  • Place of Presentation: 京都
  • Invited