Combined Electronic Structure and Quantum Dynamical Study of Organic Photovoltaics

• Project/Area Number: 15K05374
• Research Category: Grant-in-Aid for Scientific Research (C)
• Allocation Type: Multi-year Fund
• Section: 一般
• Research Field: Physical chemistry
• Research Institution: The University of Tokyo (2016-2017); Tohoku University (2015)
• Principal Investigator: Tamura Hiroyuki 東京大学, 大学院工学系研究科(工学部), 特任准教授 (60390655)
• Project Period (FY): 2015-04-01 – 2018-03-31
• Project Status: Completed (Fiscal Year 2017)
• Budget Amount: ¥4,940,000 (Direct Cost: ¥3,800,000、Indirect Cost: ¥1,140,000); Fiscal Year 2017: ¥650,000 (Direct Cost: ¥500,000、Indirect Cost: ¥150,000); Fiscal Year 2016: ¥650,000 (Direct Cost: ¥500,000、Indirect Cost: ¥150,000); Fiscal Year 2015: ¥3,640,000 (Direct Cost: ¥2,800,000、Indirect Cost: ¥840,000)
• Keywords: 有機太陽電池 / 励起子 / 電荷分離 / 有機系太陽電池 / シングレットフィッション / 有機薄膜太陽電池 / 第一原理計算 / 量子ダイナミックス

Outline of Final Research Achievements

In organic photovoltaics, charge separation from photo-generated exciton occurs at donor-acceptor interfaces on a time scale of few hundred second despite the small permittivity of organic materials. Our quantum dynamics calculations revealed the role of charge delocalization and hot exciton in the ultrafast charge separation.

Research Products

• [Int'l Joint Research] モンス大学(ベルギー)
• [Int'l Joint Research] ゲーテ大学(ドイツ)
• [Journal Article] Robust singlet fission in pentacene thin films with tuned charge transfer interactions (2018)
  • Author(s): K. Broch, J. Dieterle, F. Branchi, N.J. Hestand, Y. Olivier, H. Tamura, C. Cruz, V.M. Nichols, A. Hinderhofer, D. Beljonne, F.C. Spano, G. Cerullo, C.J. Bardeen, and F. Schreiber
  • Journal Title: Nature Communications Volume: 9 Issue: 1 Pages: 954-954
  • DOI: 10.1038/s41467-018-03300-1
  • Peer Reviewed / Open Access / Int'l Joint Research
• [Journal Article] The entangled triplet pair state in acene and heteroacene materials (2017)
  • Author(s): Yong Chaw Keong、Musser Andrew J.、Bayliss Sam L.、Lukman Steven、Tamura Hiroyuki、Bubnova Olga、Hallani Rawad K.、Meneau Aur?lie、Resel Roland、Maruyama Munetaka、Hotta Shu、Herz Laura M.、Beljonne David、Anthony John E.、Clark Jenny、Sirringhaus Henning
  • Journal Title: Nature Communications Volume: 8 Issue: 1 Pages: 15953-15953
  • DOI: 10.1038/ncomms15953
  • Peer Reviewed / Open Access / Int'l Joint Research
• [Journal Article] π-electron S =1/2 quantum spin-liquid state in an ionic polyaromatic hydrocarbon (2017)
  • Author(s): Takabayashi Y, Menelaou M, Tamura H, Takemori N, Koretsune T, Stefancic A, Klupp G, Buurma AJC, Nomura Y, Arita R,, Arcon D, Rosseinsky MJ, Prassides K
  • Journal Title: Nature Chemistry Volume: 9 Issue: 7 Pages: 635-643
  • DOI: 10.1038/nchem.2764
  • Peer Reviewed / Open Access / Int'l Joint Research
• [Journal Article] Quantum dynamical studies of ultrafast charge separation in nanostructured organic polymer materials: Effects of vibronic interactions and molecular packing (2017)
  • Author(s): Polkehn Matthias、Eisenbrandt Pierre、Tamura Hiroyuki、Burghardt Irene
  • Journal Title: International Journal of Quantum Chemistry Volume: 118 Issue: 1
  • DOI: 10.1002/qua.25502
  • Peer Reviewed / Int'l Joint Research
• [Journal Article] Impact of charge-transfer excitons in regioregular polythiophene on the charge separation at polythiophene-fullerene heterojunctions (2017)
  • Author(s): Polkehn M、Tamura H、Burghardt I
  • Journal Title: Journal of Physics B: Atomic, Molecular and Optical Physics Volume: 51 Issue: 1 Pages: 014003-014003
  • DOI: 10.1088/1361-6455/aa93d0
  • Peer Reviewed / Int'l Joint Research
• [Journal Article] The entangled triplet pair state in acene and heteroacene materials (2017)
  • Author(s): C. K. Yong, A. J. Musser, S. L. Bayliss, S. Lukman, H. Tamura, O. Bubnova, R. K. Hallani, A. Meneau, R. Resel, M. Maruyama, S. Hotta, L. M. Herz, D. Beljonne, J. E. Anthony, J. Clark, and H. Sirringhaus
  • Journal Title: Nature Communications「印刷中」 Volume: -
  • Peer Reviewed / Open Access / Int'l Joint Research
• [Journal Article] Dynamics of the triplet pair state reveals the likely co-existence of coherent and incoherent singlet fission in crystalline hexacene (2016)
  • Author(s): N. R. Monahan, D. Su, *H. Tamura, K. W. Williams, B. Xu, Y. Zhong, B. Kumar, C. Nuckolls, A. R. Harutyunyan, G. Chen, H.-L. Dai, D. Beljonne, Y. Rao, X.-Y. Zhu,
  • Journal Title: Nature Chemistry, in press. Volume: 9 Issue: 4 Pages: 341-346
  • DOI: 10.1038/nchem.2665
  • Peer Reviewed / Open Access / Int'l Joint Research / Acknowledgement Compliant
• [Journal Article] Diabatization for time-dependent density functional theory: Exciton transfers and related conical intersections (2016)
  • Author(s): *H. Tamura
  • Journal Title: J Phys. Chem. A, Volume: 120 Issue: 46 Pages: 9341-9347
  • DOI: 10.1021/acs.jpca.6b09854
  • Peer Reviewed / Open Access / Acknowledgement Compliant
• [Journal Article] Molecular packing determines charge separation in a liquid crystalline bisthiophene－perylene diimide donor－acceptor material (2016)
  • Author(s): M. Polkehn, H. Tamura, P. Eisenbrandt, S. Haacke, S. Meery, and I. Burghardt
  • Journal Title: J. Phys. Chem. Lett Volume: 7 Issue: 7 Pages: 1327-1334
  • DOI: 10.1021/acs.jpclett.6b00277
  • Peer Reviewed / Open Access / Int'l Joint Research
• [Journal Article] Concurrent effects of delocalization and internal conversion tune charge separation at regioregular polythiophene-fullerene heterojunctions (2015)
  • Author(s): M. Huix-Rotllant, H. Tamura, I. Burghardt
  • Journal Title: J. Phys. Chem. Lett Volume: 6 Issue: 9 Pages: 1702-1708
  • DOI: 10.1021/acs.jpclett.5b00336
  • Peer Reviewed / Open Access / Int'l Joint Research
• [Journal Article] First-principles quantum dynamics of singlet fission: coherent versus thermally activated mechanisms governed by molecular pi stacking (2015)
  • Author(s): H. Tamura, M. Huix-Rotllant, I. Burghardt, Y. Olivier, D. Beljonne
  • Journal Title: Phys. Rev. Lett. Volume: 115 Issue: 10
  • DOI: 10.1103/physrevlett.115.107401
  • Peer Reviewed / Int'l Joint Research
• [Presentation] Combined Electronic Structure and Quantum Dynamical Analysis for Charge Separation and Singlet Fission (2018)
  • Author(s): 田村宏之
  • Organizer: Nonadiabatica 2018: Theory of nonadiabatic processes
  • Int'l Joint Research / Invited
• [Presentation] Mechanism of Singlet Fission in π-stacked Molecules: First Principles Calculations and Quantum Dynamics Calculations (2017)
  • Author(s): 田村宏之
  • Organizer: International Conference on Molecular Electronics and Bio-electronics
  • Int'l Joint Research / Invited
• [Presentation] Charge and exciton dynamics in organic photovoltaic and singlet fission (2017)
  • Author(s): 田村宏之
  • Organizer: Quantum Dynamics and Spectroscopy of Functional Molecular Materials and Biological Photosystems
  • Int'l Joint Research / Invited
• [Presentation] Charge and exciton dynamics in organic photovoltaics and singlet fission (2016)
  • Author(s): H. Tamura
  • Organizer: Excited states bridging scale 2016
  • Place of Presentation: Marseille
  • Year and Date: 2016-08-31
  • Int'l Joint Research / Invited
• [Presentation] 有機薄膜太陽電池の光電変換機構の理論研究 (2016)
  • Author(s): 田村宏之
  • Organizer: 応用物理学会
  • Place of Presentation: 東京工業大学（東京都・大岡山）
  • Year and Date: 2016-03-21
  • Invited
• [Presentation] 第一原理計算と量子ダイナミックス計算を統合した有機光電変換系の理論研究 (2015)
  • Author(s): 田村宏之
  • Organizer: 次世代有機太陽電池シンポジウム「次世代有機太陽電池の動向と展望～実験と理論の連携～」
  • Place of Presentation: 首都大学東京（東京都・秋葉原）
  • Year and Date: 2015-09-29
  • Invited