Computational Investigation of the Spin-Density Asymmetry in Photosynthetic Reaction Center Models from First Principles

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Computational Investigation of the Spin-Density Asymmetry in Photosynthetic Reaction Center Models from First Principles. / Artiukhin, Denis; Eschenbach, Patrick; Neugebauer, Johannes.

I: Journal of Physical Chemistry B, Bind 124, Nr. 24, 06.2020, s. 4873–4888.

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Artiukhin, Denis ; Eschenbach, Patrick ; Neugebauer, Johannes. / Computational Investigation of the Spin-Density Asymmetry in Photosynthetic Reaction Center Models from First Principles. I: Journal of Physical Chemistry B. 2020 ; Bind 124, Nr. 24. s. 4873–4888.

Bibtex

@article{c62eaccbe19c465a88ebeb3332407fd6,
title = "Computational Investigation of the Spin-Density Asymmetry in Photosynthetic Reaction Center Models from First Principles",
abstract = "We present a computational analysis of the spin-density asymmetry in cation radical states of reaction center models from photosystem I, photosystem II, and bacteria from Synechococcus elongatus, Thermococcus vulcanus, and Rhodobacter sphaeroides, respectively. The recently developed frozen-density embedding (FDE)-diab methodology [J. Chem. Phys., 2018, 148, 214104] allowed us to effectively avoid the spin-density overdelocalization error characteristic for the standard Kohn–Sham density functional theory and to reliably calculate spin-density distributions and electronic couplings for a number of molecular systems ranging from inner pairs of (bacterio)chlorophyll a molecules in vacuum to large proteins including up to about 2000 atoms. The calculated spin densities show a good agreement with available experimental results and were used to validate reaction center models reported in the literature. Here, we demonstrate that the applied theoretical approach is very sensitive to changes in molecular structures and the relative orientation of molecules. This makes FDE-diab a valuable tool for electronic structure calculations of large photosynthetic models effectively complementing the existing experimental techniques.",
author = "Denis Artiukhin and Patrick Eschenbach and Johannes Neugebauer",
year = "2020",
month = jun,
doi = "10.1021/acs.jpcb.0c02827",
language = "English",
volume = "124",
pages = "4873–4888",
journal = "Journal of Physical Chemistry Part B: Condensed Matter, Materials, Surfaces, Interfaces & Biophysical",
issn = "1520-6106",
publisher = "American Chemical Society",
number = "24",

}

RIS

TY - JOUR

T1 - Computational Investigation of the Spin-Density Asymmetry in Photosynthetic Reaction Center Models from First Principles

AU - Artiukhin, Denis

AU - Eschenbach, Patrick

AU - Neugebauer, Johannes

PY - 2020/6

Y1 - 2020/6

N2 - We present a computational analysis of the spin-density asymmetry in cation radical states of reaction center models from photosystem I, photosystem II, and bacteria from Synechococcus elongatus, Thermococcus vulcanus, and Rhodobacter sphaeroides, respectively. The recently developed frozen-density embedding (FDE)-diab methodology [J. Chem. Phys., 2018, 148, 214104] allowed us to effectively avoid the spin-density overdelocalization error characteristic for the standard Kohn–Sham density functional theory and to reliably calculate spin-density distributions and electronic couplings for a number of molecular systems ranging from inner pairs of (bacterio)chlorophyll a molecules in vacuum to large proteins including up to about 2000 atoms. The calculated spin densities show a good agreement with available experimental results and were used to validate reaction center models reported in the literature. Here, we demonstrate that the applied theoretical approach is very sensitive to changes in molecular structures and the relative orientation of molecules. This makes FDE-diab a valuable tool for electronic structure calculations of large photosynthetic models effectively complementing the existing experimental techniques.

AB - We present a computational analysis of the spin-density asymmetry in cation radical states of reaction center models from photosystem I, photosystem II, and bacteria from Synechococcus elongatus, Thermococcus vulcanus, and Rhodobacter sphaeroides, respectively. The recently developed frozen-density embedding (FDE)-diab methodology [J. Chem. Phys., 2018, 148, 214104] allowed us to effectively avoid the spin-density overdelocalization error characteristic for the standard Kohn–Sham density functional theory and to reliably calculate spin-density distributions and electronic couplings for a number of molecular systems ranging from inner pairs of (bacterio)chlorophyll a molecules in vacuum to large proteins including up to about 2000 atoms. The calculated spin densities show a good agreement with available experimental results and were used to validate reaction center models reported in the literature. Here, we demonstrate that the applied theoretical approach is very sensitive to changes in molecular structures and the relative orientation of molecules. This makes FDE-diab a valuable tool for electronic structure calculations of large photosynthetic models effectively complementing the existing experimental techniques.

U2 - 10.1021/acs.jpcb.0c02827

DO - 10.1021/acs.jpcb.0c02827

M3 - Journal article

C2 - 32449852

VL - 124

SP - 4873

EP - 4888

JO - Journal of Physical Chemistry Part B: Condensed Matter, Materials, Surfaces, Interfaces & Biophysical

JF - Journal of Physical Chemistry Part B: Condensed Matter, Materials, Surfaces, Interfaces & Biophysical

SN - 1520-6106

IS - 24

ER -