Influence of weak vibrational-electronic couplings on 2D electronic spectra and inter-site coherence in weakly coupled photosynthetic complexes

Monahan, Daniele M.; Whaley-Mayda, Lukas; Ishizaki, Akihito; Fleming, Graham R.

doi:10.1063/1.4928068

Title: Influence of weak vibrational-electronic couplings on 2D electronic spectra and inter-site coherence in weakly coupled photosynthetic complexes

Journal Article · Mon Aug 10 00:00:00 EDT 2015 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.4928068· OSTI ID:1407273

Monahan, Daniele M. ^[1]; Whaley-Mayda, Lukas ^[1]; Ishizaki, Akihito ^[2];

^[1]

Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Kavli Energy NanoSciences Inst. at Berkeley, CA (United States)
National Inst. of Natural Sciences, Okazaki (Japan)

Coherence oscillations measured in two-dimensional (2D) electronic spectra of pigment-protein complexes may have electronic, vibrational, or mixed-character vibronic origins, which depend on the degree of electronic-vibrational mixing. Oscillations from intrapigment vibrations can obscure the inter-site coherence lifetime of interest in elucidating the mechanisms of energy transfer in photosynthetic light-harvesting. Huang-Rhys factors (S) for low-frequency vibrations in Chlorophyll and Bacteriochlorophyll are quite small (S ≤ 0.05), therefore it is often assumed that these vibrations influence neither 2D spectra nor inter-site coherence dynamics. In this work, we explore the influence of S within this range on the oscillatory signatures in simulated 2D spectra of a pigment heterodimer. To visualize the inter-site coherence dynamics underlying the 2D spectra, we introduce a formalism which we call the "site-probe response." By comparing the calculated 2D spectra with the site-probe response, we show that an on-resonance vibration with Huang-Rhys factor as small as S = 0.005 and the most strongly coupled off-resonance vibrations (S = 0.05) give rise to long-lived, purely vibrational coherences at 77 K. We moreover calculate the correlation between optical pump interactions and subsequent entanglement between sites, as measured by the concurrence. At 77 K, greater long-lived inter-site coherence and entanglement appear with increasing S. This dependence all but vanishes at physiological temperature, as environmentally induced fluctuations destroy the vibronic mixing.e

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); University of California, Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; Japan Society for the Promotion of Science (JSPS); National Science Foundation (NSF)

Grant/Contract Number:: AC02-05CH11231; AC03-76SF00098; 25708003; DGE-1106400

OSTI ID:: 1407273

Alternate ID(s):: OSTI ID: 1229605

Journal Information:: Journal of Chemical Physics, Vol. 143, Issue 6; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 30 works

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74 ATOMIC AND MOLECULAR PHYSICS
Excitons
Photosynthetic light-harvesting
Coherence
Bacteriochlorophyll
Fluorescence resonance energy transfer
Protein complexes
Delocalization
Electronic coupling
Chlorophyll
Quantum optics

Title: Influence of weak vibrational-electronic couplings on 2D electronic spectra and inter-site coherence in weakly coupled photosynthetic complexes

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