Quantumness in light harvesting is determined by vibrational dynamics

被引:18
作者
Reppert, Mike [1 ]
Brumer, Paul [1 ,2 ]
机构
[1] Univ Toronto, Dept Chem, Chem Phys Theory Grp, Toronto, ON M5S 3H6, Canada
[2] Univ Toronto, Ctr Quantum Informat & Quantum Control, Toronto, ON M5S 3H6, Canada
基金
加拿大自然科学与工程研究理事会;
关键词
EXCITATION-ENERGY TRANSFER; CLASSICAL CORRESPONDENCE; SPECTRAL DENSITY; ENTANGLEMENT; CHLOROPHYLL; COHERENCES; TRANSPORT; MODELS;
D O I
10.1063/1.5058136
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
We demonstrate for the multi-level spin-boson (MLSB) Hamiltonian, typically used to describe biological light-harvesting, that the distinction between quantum and classical dynamics is determined entirely by the thermal environment. In particular, any MLSB model featuring classical interactions with a classical bath is exactly equivalent in its absorption and energy transfer dynamics to a classical model involving coupled harmonic oscillators. This result holds in the linear response regime for both pulsed and incoherent excitation. In the biological context, this finding highlights the centrality of vibrational dynamics in determining the "quantumness" of photosynthetic light-harvesting, particularly in the creation of the photosynthetic energy funnel where excitation energy concentrates near the reaction center via a series of downhill energy transfer events. These findings support the idea that this energy funnel is exclusively quantum-mechanical in origin, although it need not rely on entanglement. Published by AIP Publishing.
引用
收藏
页数:14
相关论文
共 62 条
[11]   Wigner functions and Weyl transforms for pedestrians [J].
Case, William B. .
AMERICAN JOURNAL OF PHYSICS, 2008, 76 (10) :937-946
[12]   COMMENTS ON CLASSICAL THEORY OF ENERGY-TRANSFER [J].
CHANCE, RR ;
PROCK, A ;
SILBEY, R .
JOURNAL OF CHEMICAL PHYSICS, 1975, 62 (06) :2245-2253
[13]   Dynamics of Light Harvesting in Photosynthesis [J].
Cheng, Yuan-Chung ;
Fleming, Graham R. .
ANNUAL REVIEW OF PHYSICAL CHEMISTRY, 2009, 60 :241-262
[14]   Origin of Long-Lived Coherences in Light-Harvesting Complexes [J].
Christensson, Niklas ;
Kauffmann, Harald F. ;
Pullerits, Tonu ;
Mancal, Tomas .
JOURNAL OF PHYSICAL CHEMISTRY B, 2012, 116 (25) :7449-7454
[15]  
Croce R, 2014, NAT CHEM BIOL, V10, P492, DOI [10.1038/NCHEMBIO.1555, 10.1038/nchembio.1555]
[16]   Nature does not rely on long-lived electronic quantum coherence for photosynthetic energy transfer [J].
Duan, Hong-Guang ;
Prokhorenko, Valentyn I. ;
Cogdell, Richard J. ;
Ashraf, Khuram ;
Stevens, Amy L. ;
Thorwart, Michael ;
Miller, R. J. Dwayne .
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2017, 114 (32) :8493-8498
[17]   Classical Approach to Multichromophoric Resonance Energy Transfer [J].
Duque, Sebastian ;
Brumer, Paul ;
Pachon, Leonardo A. .
PHYSICAL REVIEW LETTERS, 2015, 115 (11)
[18]   Classical master equation for excitonic transport under the influence of an environment [J].
Eisfeld, Alexander ;
Briggs, John S. .
PHYSICAL REVIEW E, 2012, 85 (04)
[19]   Evidence for wavelike energy transfer through quantum coherence in photosynthetic systems [J].
Engel, Gregory S. ;
Calhoun, Tessa R. ;
Read, Elizabeth L. ;
Ahn, Tae-Kyu ;
Mancal, Tomas ;
Cheng, Yuan-Chung ;
Blankenship, Robert E. ;
Fleming, Graham R. .
NATURE, 2007, 446 (7137) :782-786
[20]  
Forster T., 1960, Radiat. Res. Suppl., P326, DOI [10.2307/3583604, DOI 10.2307/3583604]