Domain-based local pair natural orbital CCSD(T) calculations of strongly correlated electron systems: Examination of dynamic equilibrium models based on multiple intermediates in S1 state of photosystem II*

K. Miyagawa, T. Kawakami, Y. Suzuki, H. Isobe, M. Shoji, S. Yamanaka, M. Okumura, T. Nakajima, K. Yamaguchi

Research output: Contribution to journalArticle

Abstract

Domain-based local pair natural orbital (DLPNO) coupled cluster single and double (CCSD) methods with perturbative triples (T) correction with NormalPNO were used to compute energies for twelve different S1 structures of the CaMn4O5 cluster in the oxygen evolving complex (OEC) of photosystem II (PSII). The DLPNO-CCSD(T0) calculations with TightPNO for the important six structures among them revealed that the right (R)-opened S1XYZW structures were more stable than the corresponding left (L)-opened structures (X = O(5), Y = W2, Z = W1, and W = O(4)) of CaMn4O5. The three different S1 structures belonging to the R-opened type (S1acca, S1bbca, and S1abcb, where O2-= a, OH-= b and H2O = c) were found nearly degenerated in energy, indicating the possibility of the coexistence of different structures in the S1 state. The DLPNO-CCSD(T0) calculations with TightPNO supported the proposal of a dynamic equilibrium model based on the multi-intermediate structures for the S1 state, which is also in agreement with EPR and other experimental and hybrid DFT computational results. Implications of the computational results are discussed in relation to scope and applicability of NormalPNO and TightPNO for the CCSD(T0) calculations of strongly correlated electron systems such as 3d transition-metal complexes.

Original languageEnglish
Article number1666171
JournalMolecular Physics
DOIs
Publication statusAccepted/In press - Jan 1 2019

Fingerprint

Photosystem II Protein Complex
Coordination Complexes
examination
Electrons
Oxygen
orbitals
electrons
Discrete Fourier transforms
Transition metals
Paramagnetic resonance
proposals
transition metals
hydroxide ion
energy
oxygen

Keywords

  • CaMnO cluster
  • hybrid DFT method
  • LPNO-CC method
  • OEC PSII

ASJC Scopus subject areas

  • Biophysics
  • Molecular Biology
  • Condensed Matter Physics
  • Physical and Theoretical Chemistry

Cite this

Domain-based local pair natural orbital CCSD(T) calculations of strongly correlated electron systems : Examination of dynamic equilibrium models based on multiple intermediates in S1 state of photosystem II*. / Miyagawa, K.; Kawakami, T.; Suzuki, Y.; Isobe, H.; Shoji, M.; Yamanaka, S.; Okumura, M.; Nakajima, T.; Yamaguchi, K.

In: Molecular Physics, 01.01.2019.

Research output: Contribution to journalArticle

@article{0decf664c06b42e393ad54240c675c70,
title = "Domain-based local pair natural orbital CCSD(T) calculations of strongly correlated electron systems: Examination of dynamic equilibrium models based on multiple intermediates in S1 state of photosystem II*",
abstract = "Domain-based local pair natural orbital (DLPNO) coupled cluster single and double (CCSD) methods with perturbative triples (T) correction with NormalPNO were used to compute energies for twelve different S1 structures of the CaMn4O5 cluster in the oxygen evolving complex (OEC) of photosystem II (PSII). The DLPNO-CCSD(T0) calculations with TightPNO for the important six structures among them revealed that the right (R)-opened S1XYZW structures were more stable than the corresponding left (L)-opened structures (X = O(5), Y = W2, Z = W1, and W = O(4)) of CaMn4O5. The three different S1 structures belonging to the R-opened type (S1acca, S1bbca, and S1abcb, where O2-= a, OH-= b and H2O = c) were found nearly degenerated in energy, indicating the possibility of the coexistence of different structures in the S1 state. The DLPNO-CCSD(T0) calculations with TightPNO supported the proposal of a dynamic equilibrium model based on the multi-intermediate structures for the S1 state, which is also in agreement with EPR and other experimental and hybrid DFT computational results. Implications of the computational results are discussed in relation to scope and applicability of NormalPNO and TightPNO for the CCSD(T0) calculations of strongly correlated electron systems such as 3d transition-metal complexes.",
keywords = "CaMnO cluster, hybrid DFT method, LPNO-CC method, OEC PSII",
author = "K. Miyagawa and T. Kawakami and Y. Suzuki and H. Isobe and M. Shoji and S. Yamanaka and M. Okumura and T. Nakajima and K. Yamaguchi",
year = "2019",
month = "1",
day = "1",
doi = "10.1080/00268976.2019.1666171",
language = "English",
journal = "Molecular Physics",
issn = "0026-8976",
publisher = "Taylor and Francis Ltd.",

}

TY - JOUR

T1 - Domain-based local pair natural orbital CCSD(T) calculations of strongly correlated electron systems

T2 - Examination of dynamic equilibrium models based on multiple intermediates in S1 state of photosystem II*

AU - Miyagawa, K.

AU - Kawakami, T.

AU - Suzuki, Y.

AU - Isobe, H.

AU - Shoji, M.

AU - Yamanaka, S.

AU - Okumura, M.

AU - Nakajima, T.

AU - Yamaguchi, K.

PY - 2019/1/1

Y1 - 2019/1/1

N2 - Domain-based local pair natural orbital (DLPNO) coupled cluster single and double (CCSD) methods with perturbative triples (T) correction with NormalPNO were used to compute energies for twelve different S1 structures of the CaMn4O5 cluster in the oxygen evolving complex (OEC) of photosystem II (PSII). The DLPNO-CCSD(T0) calculations with TightPNO for the important six structures among them revealed that the right (R)-opened S1XYZW structures were more stable than the corresponding left (L)-opened structures (X = O(5), Y = W2, Z = W1, and W = O(4)) of CaMn4O5. The three different S1 structures belonging to the R-opened type (S1acca, S1bbca, and S1abcb, where O2-= a, OH-= b and H2O = c) were found nearly degenerated in energy, indicating the possibility of the coexistence of different structures in the S1 state. The DLPNO-CCSD(T0) calculations with TightPNO supported the proposal of a dynamic equilibrium model based on the multi-intermediate structures for the S1 state, which is also in agreement with EPR and other experimental and hybrid DFT computational results. Implications of the computational results are discussed in relation to scope and applicability of NormalPNO and TightPNO for the CCSD(T0) calculations of strongly correlated electron systems such as 3d transition-metal complexes.

AB - Domain-based local pair natural orbital (DLPNO) coupled cluster single and double (CCSD) methods with perturbative triples (T) correction with NormalPNO were used to compute energies for twelve different S1 structures of the CaMn4O5 cluster in the oxygen evolving complex (OEC) of photosystem II (PSII). The DLPNO-CCSD(T0) calculations with TightPNO for the important six structures among them revealed that the right (R)-opened S1XYZW structures were more stable than the corresponding left (L)-opened structures (X = O(5), Y = W2, Z = W1, and W = O(4)) of CaMn4O5. The three different S1 structures belonging to the R-opened type (S1acca, S1bbca, and S1abcb, where O2-= a, OH-= b and H2O = c) were found nearly degenerated in energy, indicating the possibility of the coexistence of different structures in the S1 state. The DLPNO-CCSD(T0) calculations with TightPNO supported the proposal of a dynamic equilibrium model based on the multi-intermediate structures for the S1 state, which is also in agreement with EPR and other experimental and hybrid DFT computational results. Implications of the computational results are discussed in relation to scope and applicability of NormalPNO and TightPNO for the CCSD(T0) calculations of strongly correlated electron systems such as 3d transition-metal complexes.

KW - CaMnO cluster

KW - hybrid DFT method

KW - LPNO-CC method

KW - OEC PSII

UR - http://www.scopus.com/inward/record.url?scp=85073966065&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=85073966065&partnerID=8YFLogxK

U2 - 10.1080/00268976.2019.1666171

DO - 10.1080/00268976.2019.1666171

M3 - Article

AN - SCOPUS:85073966065

JO - Molecular Physics

JF - Molecular Physics

SN - 0026-8976

M1 - 1666171

ER -