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  Accurate Computation of the Absorption Spectrum of Chlorophyll a with Pair Natural Orbital Coupled Cluster Methods

Sirohiwal, A., Berraud-Pache, R., Neese, F., Izsák, R., & Pantazis, D. A. (2020). Accurate Computation of the Absorption Spectrum of Chlorophyll a with Pair Natural Orbital Coupled Cluster Methods. The Journal of Physical Chemistry B, 124(40), 8761-8771. doi:10.1021/acs.jpcb.0c05761.

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Sirohiwal, Abhishek1, 2, Author           
Berraud-Pache, Romain3, Author           
Neese, Frank4, Author           
Izsák, Róbert3, Author           
Pantazis, Dimitrios A.1, Author           
Affiliations:
1Research Group Pantazis, Max-Planck-Institut für Kohlenforschung, Max Planck Society, ou_2541711              
2Fakultät für Chemie und Biochemie, Ruhr-Universität Bochum, 44780 Bochum, Germany, ou_persistent22              
3Research Group Izsák, Max-Planck-Institut für Kohlenforschung, Max Planck Society, ou_2541707              
4Research Department Neese, Max-Planck-Institut für Kohlenforschung, Max Planck Society, ou_2541710              

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 Abstract: The ability to accurately compute low-energy excited states of chlorophylls is critically important for understanding the vital roles they play in light harvesting, energy transfer, and photosynthetic charge separation. The challenge for quantum chemical methods arises both from the intrinsic complexity of the electronic structure problem and, in the case of biological models, from the need to account for protein–pigment interactions. In this work, we report electronic structure calculations of unprecedented accuracy for the low-energy excited states in the Q and B bands of chlorophyll a. This is achieved by using the newly developed domain-based local pair natural orbital (DLPNO) implementation of the similarity transformed equation of motion coupled cluster theory with single and double excitations (STEOM-CCSD) in combination with sufficiently large and flexible basis sets. The results of our DLPNO–STEOM-CCSD calculations are compared with more approximate approaches. The results demonstrate that, in contrast to time-dependent density functional theory, the DLPNO–STEOM-CCSD method provides a balanced performance for both absorption bands. In addition to vertical excitation energies, we have calculated the vibronic spectrum for the Q and B bands through a combination of DLPNO–STEOM-CCSD and ground-state density functional theory frequency calculations. These results serve as a basis for comparison with gas-phase experiments.

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Language(s): eng - English
 Dates: 2020-06-242020-09-152020-10-08
 Publication Status: Published in print
 Pages: 11
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1021/acs.jpcb.0c05761
 Degree: -

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Title: The Journal of Physical Chemistry B
  Abbreviation : J. Phys. Chem. B
Source Genre: Journal
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Publ. Info: Washington, D.C. : American Chemical Society
Pages: - Volume / Issue: 124 (40) Sequence Number: - Start / End Page: 8761 - 8771 Identifier: ISSN: 1520-6106
CoNE: https://pure.mpg.de/cone/journals/resource/1000000000293370_1