New frontier of electronic structure calculations for strongly correlated molecular sciences from the fusion of deterministic and stochastic methodologies

• Project/Area Number: 18H03900
• Research Category: Grant-in-Aid for Scientific Research (A)
• Allocation Type: Single-year Grants
• Section: 一般
• Review Section: Medium-sized Section 32:Physical chemistry, functional solid state chemistry, and related fields
• Research Institution: Kobe University
• Principal Investigator: Ten-no Seiichiro 神戸大学, 科学技術イノベーション研究科, 教授 (00270471)
• Project Period (FY): 2018-04-01 – 2022-03-31
• Project Status: Completed (Fiscal Year 2022)
• Budget Amount: ¥40,560,000 (Direct Cost: ¥31,200,000、Indirect Cost: ¥9,360,000); Fiscal Year 2021: ¥9,880,000 (Direct Cost: ¥7,600,000、Indirect Cost: ¥2,280,000); Fiscal Year 2020: ¥9,490,000 (Direct Cost: ¥7,300,000、Indirect Cost: ¥2,190,000); Fiscal Year 2019: ¥9,490,000 (Direct Cost: ¥7,300,000、Indirect Cost: ¥2,190,000); Fiscal Year 2018: ¥11,700,000 (Direct Cost: ¥9,000,000、Indirect Cost: ¥2,700,000)
• Keywords: 結合クラスター理論 / 量子モンテカルロ法 / 完全CI / 強電子相関 / スピン状態 / 強相関 / 結合クラスター / モンテカルロ / スピン射影 / 固体 / 量子モンテカルロ / 多核遷移金属 / 励起状態 / イニシエーター誤差 / サイズ無矛盾 / サイズ矛盾

Outline of Final Research Achievements

We implemented the full coupled-cluster (FCC) expansion to develop an adaptive FCC reduction (FCCR) approach using screenings for excitation manifolds and nonlinear CC operations. The second order perturbative correction using the FCCR reference (FCCR(2)) along with extrapolations efficiently provides near-exact solutions of strongly correlated electronic systems. We further attempted to mitigate the initiator error of configuration space QMC with respect to the system size using the ideas in CC and many-body perturbation theories. A powerful means from spin-projection including the treatment of dynamic correlation and second-order optimizer is also developed to treat transition metal complexes.

Academic Significance and Societal Importance of the Research Achievements

触媒やレドックス作用の重要な役割を担う電子相関の強い物質は、複雑な電子配置のために理論的な取り扱いが困難である。この問題の解決を目指して、決定論と確率論に基づく最先端の電子状態計算手法の開発を総合的に行った。得られた研究成果は理論の独創性と幅広い応用を持ち、基礎学問と社会的な双方の意義を備えている。

Research Products

• [Int'l Joint Research] University of Illinois(米国)
• [Journal Article] Water?oxidation mechanism of cobalt phosphate co-catalyst in artificial photosynthesis: a theoretical study (2022)
  • Author(s): Tsuneda Takao、Ten-no Seiichiro L.
  • Journal Title: Physical Chemistry Chemical Physics Volume: 24 Issue: 7 Pages: 4674-4682
  • DOI: 10.1039/d1cp05816a
  • Peer Reviewed
• [Journal Article] Binary dopant segregation enables hematite-based heterostructures for highly efficient solar H2O2 synthesis (2022)
  • Author(s): Zhang Zhujun、Tsuchimochi Takashi、Ina Toshiaki、Kumabe Yoshitaka、Muto Shunsuke、Ohara Koji、Yamada Hiroki、Ten-no Seiichiro L.、Tachikawa Takashi
  • Journal Title: Nature Communications Volume: 13 Issue: 1 Pages: 1499-1499
  • DOI: 10.1038/s41467-022-28944-y
  • Peer Reviewed / Open Access
• [Journal Article] Improved Description and Efficient Implementation of Spin- Projected Perturbation Theory for Practical Applications (2021)
  • Author(s): Takashi Tsuchimochi, Kosuke Yoshimura, Yuma Shimomoto, and Seiichiro L. Ten-no
  • Journal Title: J. Chem. Theory Comput. Volume: 17 Issue: 6 Pages: 3471-3482
  • DOI: 10.1021/acs.jctc.1c00324
  • Peer Reviewed
• [Journal Article] First-Principles Investigation on the Heterostructure Photocatalyst Comprising BiVO4 and Few-Layer Black Phosphorus (2021)
  • Author(s): Takashi Tsuchimochi, Kaname Takaoki, Kazutaka Nishiguchi, and Seiichiro L. Ten-no
  • Journal Title: J. Phys. Chem. C Volume: 125 Issue: 40 Pages: 21840-21850
  • DOI: 10.1021/acs.jpcc.1c06247
  • Peer Reviewed
• [Journal Article] Spin-projection for quantum computation: A low-depth approach to strong correlation (2020)
  • Author(s): Tsuchimochi Takashi、Mori Yuto、Ten-no Seiichiro L.
  • Journal Title: Physical Review Research Volume: 2 Issue: 4 Pages: 043142-043142
  • DOI: 10.1103/physrevresearch.2.043142
  • Peer Reviewed
• [Journal Article] Third-order Epstein?Nesbet perturbative correction to the initiator approximation of configuration space quantum Monte Carlo (2020)
  • Author(s): Ladoczki Bence、Uejima Motoyuki、Ten-no Seiichiro L.
  • Journal Title: The Journal of Chemical Physics Volume: 153 Issue: 11 Pages: 114112-114112
  • DOI: 10.1063/5.0022101
  • Peer Reviewed
• [Journal Article] The Ground State Electronic Energy of Benzene (2020)
  • Author(s): Eriksen Janus J. et al.
  • Journal Title: The Journal of Physical Chemistry Letters Volume: 11 Issue: 20 Pages: 8922-8929
  • DOI: 10.1021/acs.jpclett.0c02621
  • Peer Reviewed
• [Journal Article] Quadratically convergent self-consistent field of projected Hartree?Fock (2020)
  • Author(s): Uejima Motoyuki、Ten-no Seiichiro L.
  • Journal Title: The Journal of Chemical Physics Volume: 153 Issue: 16 Pages: 164103-164103
  • DOI: 10.1063/5.0025280
  • Peer Reviewed
• [Journal Article] Towards Near-Exact Solutions of Molecular Electronic Structure: Full Coupled-Cluster Reduction with a Second-Order Perturbative Correction (2020)
  • Author(s): Xu Enhua、Uejima Motoyuki、Ten-no Seiichiro L.
  • Journal Title: The Journal of Physical Chemistry Letters Volume: 11 Issue: 22 Pages: 9775-9780
  • DOI: 10.1021/acs.jpclett.0c03084
• [Journal Article] Effect of Molecular Orientational Correlations on Solvation Free Energy Computed by Reference Interaction Site Model Theory (2019)
  • Author(s): Tanimoto Shoichi、Yoshida Norio、Yamaguchi Tsuyoshi、Ten-no Seiichiro L.、Nakano Haruyuki
  • Journal Title: Journal of Chemical Information and Modeling Volume: 59 Issue: 9 Pages: 3770-3781
  • DOI: 10.1021/acs.jcim.9b00330
  • Peer Reviewed
• [Journal Article] Stochastic perturbation theory in a limited configuration space (2019)
  • Author(s): Ladoczki Bence、Ten-no Seiichiro L.
  • Journal Title: The Journal of Chemical Physics Volume: 151 Issue: 11 Pages: 114113-114113
  • DOI: 10.1063/1.5109820
  • Peer Reviewed
• [Journal Article] Second-order perturbation theory with spin-symmetry projected Hartree-Fock (2019)
  • Author(s): Takashi Tsuchimochi, Seiichiro L. Ten-no
  • Journal Title: Journal of Chemical Theory and Computation Volume: 15 Issue: 12 Pages: 6688-6702
  • DOI: 10.1021/acs.jctc.9b00897
  • NAID: 120006954047
  • Peer Reviewed
• [Journal Article] Extending spin‐symmetry projected coupled‐cluster to large model spaces using an iterative null‐space projection technique (2019)
  • Author(s): Takashi Tsuchimochi and Seiichiro L. Ten-no
  • Journal Title: Journal of Computational Chemistry Volume: 40 Issue: 1 Pages: 265-278
  • DOI: 10.1002/jcc.25587
  • Peer Reviewed
• [Journal Article] Orbital-invariant spin-extended approximate coupled-cluster for multi-reference systems (2018)
  • Author(s): Takashi Tsuchimochi and Seiichiro L. Ten-no
  • Journal Title: The Journal of Chemical Physics Volume: 149 Issue: 4 Pages: 044109-044109
  • DOI: 10.1063/1.5036542
  • NAID: 120006796536
  • Peer Reviewed
• [Journal Article] Full Coupled-Cluster Reduction for Accurate Description of Strong Electron Correlation (2018)
  • Author(s): Xu Enhua、Uejima Motoyuki、Ten-no Seiichiro Lenka
  • Journal Title: Physical Review Letters Volume: 121 Issue: 11 Pages: 113001-113001
  • DOI: 10.1103/physrevlett.121.113001
• [Journal Article] Monte Carlo explicitly correlated many-body Green’s function theory (2018)
  • Author(s): Johnson Cole M.、Doran Alexander E.、Ten-no Seiichiro L.、Hirata So
  • Journal Title: The Journal of Chemical Physics Volume: 149 Issue: 17 Pages: 174112-174112
  • DOI: 10.1063/1.5054610
• [Presentation] The full coupled-cluster approach for accurate treatment of strongly correlaed electrons (2020)
  • Author(s): Seiichiro L. Ten-no
  • Organizer: New Horizons in Scientific Software: from Legacy Codes to Modular Environments
  • Int'l Joint Research / Invited
• [Presentation] Selected coupled-cluster for strong electron correlation (2019)
  • Author(s): Seiichiro L. Ten-no
  • Organizer: Workshop on Strongly Correlated Electrons
  • Int'l Joint Research
• [Presentation] ull coupled-cluster reduction for strongly correlated electrons (2019)
  • Author(s): Seiichiro L. Ten-no
  • Organizer: The Ninth Conference of the Asia-Pacific Association of Theoretical and Computational Chemists (APATCC 2019)
  • Int'l Joint Research
• [Presentation] Explicitly correlated F12 theory on modern electronic structure calculations (2019)
  • Author(s): Seiichiro L. Ten-no
  • Organizer: 10th Triennial Congress of the International Society for Theoretical Chemical Physics (ISTCP2019)
  • Int'l Joint Research
• [Presentation] Full coupled-cluster reduction for strongly correlated electrons (2019)
  • Author(s): Seiichiro L. Ten-no
  • Organizer: 9th Molecular Quantum Mechanics Conference (MQM2019)
  • Int'l Joint Research
• [Presentation] Selected coupled-cluster and stochastic perturbation theory (2019)
  • Author(s): Seiichiro L. Ten-no
  • Organizer: New Frontiers in Electron Correlation Workshop
• [Presentation] Stochastic perturbation theory in a limited configuration space (2019)
  • Author(s): Bence Ladoczki、Seiichiro L. Ten-no
  • Organizer: 第22回理論化学討論会
• [Presentation] First-principles study of the interfaces of SrTiO3 with mediator and cocatalyst for the hydrogen evolution in the Z-scheme artificial photosynthesis (2019)
  • Author(s): Shotaro Sakurai, Kotaro Okano, Kazutaka Nishiguchi, Seiichiro Ten-no
  • Organizer: International Workshop on Frontier of Science and Technology for Solar Energy Conversion
• [Presentation] 強電子相関系のイオン化ポテンシャル (2019)
  • Author(s): 土持崇嗣、天能精一郎
  • Organizer: 第13回分子科学討論会
• [Presentation] Ionization potentials for multi-reference systems via post-PHF: Extended Koopmans Theorem (2019)
  • Author(s): Takashi Tsuchimochi and Seiichiro L. Ten-no
  • Organizer: 9th Molecular Quantum Mechanics Conference (MQM2019)
• [Presentation] 拡張 Koopmans 定理を用いた強相関系におけるイオン化ポテンシャルの計算 (2019)
  • Author(s): 土持崇嗣、天能精一郎
  • Organizer: 第22回理論化学討論会
• [Presentation] 確率論的手法とUnlinked図形の寄与に関する研究 (2018)
  • Author(s): Ladoczki Bence、天能精一郎
  • Organizer: 第21回理論化学討論会
• [Presentation] Selected coupled-cluster approaches from stochastic and deterministic algorithms (2018)
  • Author(s): Seiichiro L. Ten-no
  • Organizer: The 7th (Japan-Czech-Slovakia) Symposium on Theoretical Chemistry
  • Int'l Joint Research / Invited
• [Presentation] Selected coupled-cluster approaches from stochastic and deterministic algorithms (2018)
  • Author(s): Seiichiro L. Ten-no
  • Organizer: Low-scaling and Unconventional Electronic Structure Techniques (LUEST2018)
  • Int'l Joint Research / Invited
• [Presentation] Selected coupled-cluster approaches from stochastic and deterministic algorithms (2018)
  • Author(s): Seiichiro L. Ten-no
  • Organizer: The Molecular Electronic Structure in Metz (MESM)
  • Int'l Joint Research / Invited
• [Presentation] イニシエーター近似の摂動補正に関する研究 (2018)
  • Author(s): Ladoczki Bence、天能精一郎
  • Organizer: 第12回分子科学討論会
• [Presentation] 量子化学プログラムGELLANの開発 (2018)
  • Author(s): 上島基之、天能精一郎
  • Organizer: 第12回分子科学討論会
• [Presentation] Full coupled cluster reduction (2018)
  • Author(s): Seiichiro L. Ten-no
  • Organizer: Mainz-Kobe joint workshop on solving the full configuration interaction problem
  • Int'l Joint Research / Invited
• [Presentation] Stochastic and deterministic coupled-cluster approaches for accurate treatment of strong electron correlations (2018)
  • Author(s): Seiichiro L. Ten-no
  • Organizer: Quantum Simulations: From Chemistry to Materials Science
  • Int'l Joint Research / Invited