Electronic coherence lifetimes of the Fenna-Matthews-Olson complex and light harvesting complex II

被引:17
作者
Irgen-Gioro, Shawn [1 ]
Gururangan, Karthik [1 ]
Saer, Rafael G. [2 ]
Blankenship, Robert E. [2 ]
Harel, Elad [1 ,3 ]
机构
[1] Northwestern Univ, Dept Chem, 2145 Sheridan Rd, Evanston, IL 60208 USA
[2] Washington Univ, Dept Biol, One Brookings Dr, St Louis, MO 63130 USA
[3] Michigan State Univ, Dept Chem, E Lansing, MI 48824 USA
关键词
LH2 ANTENNA COMPLEX; QUANTUM COHERENCE; ENERGY-TRANSFER; SPECTROSCOPY; DYNAMICS; FEMTOSECOND; PROTEIN; SYSTEM;
D O I
10.1039/c9sc03501j
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The study of coherence between excitonic states in naturally occurring photosynthetic systems offers tantalizing prospects of uncovering mechanisms of efficient energy transport. However, experimental evidence of functionally relevant coherences in wild-type proteins has been tentative, leading to uncertainty in their importance at physiological conditions. Here, we extract the electronic coherence lifetime and frequency using a signal subtraction procedure in two model pigment-protein-complexes (PPCs), light harvesting complex II (LH2) and the Fenna-Matthews-Olson complex (FMO), and find that the coherence lifetimes occur at the same timescale (<100 fs) as energy transport between states at the energy level difference equal to the coherence energy. The pigment monomer bacteriochlorophyll a (BChla) shows no electronic coherences, supporting our methodology of removing long-lived vibrational coherences that have obfuscated previous assignments. This correlation of timescales and energy between coherences and energy transport reestablishes the time and energy scales that quantum processes may play a role in energy transport.
引用
收藏
页码:10503 / 10509
页数:7
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