Modified scaled hierarchical equation of motion approach for the study of quantum coherence in photosynthetic complexes

Jing Zhu, Sabre Kais, Patrick Rebentrost, Alán Aspuru-Guzik

Research output: Contribution to journalArticle

91 Citations (Scopus)

Abstract

We present a detailed theoretical study of the transfer of electronic excitation energy through the Fenna-Matthews-Olson (FMO) pigment-protein complex, using the newly developed modified scaled hierarchical approach (Shi, Q.; et al. J. Chem. Phys.2009, 130, 084105). We show that this approach is computationally more efficient than the original hierarchical approach. The modified approach reduces the truncation levels of the auxiliary density operators and the correlation function. We provide a systematic study of how the number of auxiliary density operators and the higher-order correlation functions affect the exciton dynamics. The time scales of the coherent beating are consistent with experimental observations. Furthermore, our theoretical results exhibit population beating at physiological temperature. Additionally, the method does not require a low-temperature correction to obtain the correct thermal equilibrium at long times.

Original languageEnglish
Pages (from-to)1531-1537
Number of pages7
JournalJournal of Physical Chemistry B
Volume115
Issue number6
DOIs
Publication statusPublished - 17 Feb 2011
Externally publishedYes

Fingerprint

Photosynthetic Reaction Center Complex Proteins
Equations of motion
Mathematical operators
equations of motion
operators
Excitation energy
pigments
Pigments
Excitons
excitons
proteins
Proteins
Temperature
approximation
electronics
excitation
temperature
energy
Hot Temperature
LDS 751

ASJC Scopus subject areas

  • Physical and Theoretical Chemistry
  • Materials Chemistry
  • Surfaces, Coatings and Films

Cite this

Modified scaled hierarchical equation of motion approach for the study of quantum coherence in photosynthetic complexes. / Zhu, Jing; Kais, Sabre; Rebentrost, Patrick; Aspuru-Guzik, Alán.

In: Journal of Physical Chemistry B, Vol. 115, No. 6, 17.02.2011, p. 1531-1537.

Research output: Contribution to journalArticle

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