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Title:
Influence of weak vibrational-electronic couplings on 2D electronic spectra and inter-site coherence in weakly coupled photosynthetic complexes
Authors:
Monahan, Daniele M.; Whaley-Mayda, Lukas; Ishizaki, Akihito; Fleming, Graham R.
Affiliation:
AA(Department of Chemistry, University of California, Berkeley, California 94720, USA; Physical Biosciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, USA; Kavli Energy NanoSciences Institute at Berkeley, Berkeley, California 94720, USA), AB(Department of Chemistry, University of California, Berkeley, California 94720, USA; Physical Biosciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, USA; Kavli Energy NanoSciences Institute at Berkeley, Berkeley, California 94720, USA), AC(Institute for Molecular Science, National Institutes of Natural Sciences, Okazaki 444-8585, Japan), AD(Department of Chemistry, University of California, Berkeley, California 94720, USA; Physical Biosciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, USA; Kavli Energy NanoSciences Institute at Berkeley, Berkeley, California 94720, USA 0000-0003-0847-1838)
Publication:
The Journal of Chemical Physics, Volume 143, Issue 6, id.065101 (JChPh Homepage)
Publication Date:
08/2015
Origin:
AIP
Abstract Copyright:
2015: AIP Publishing LLC
DOI:
10.1063/1.4928068
Bibliographic Code:
2015JChPh.143f5101M

Abstract

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), so 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.
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