期刊
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
卷 3, 期 21, 页码 3136-3142出版社
AMER CHEMICAL SOC
DOI: 10.1021/jz3010317
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资金
- DARPA (QuBE)
- United States Air Force Office of Scientific Research [FA9550-10-1-0260]
- Natural Sciences and Engineering Research Council of Canada
- EPSRC
- EPSRC [EP/G005222/1] Funding Source: UKRI
- Engineering and Physical Sciences Research Council [EP/G005222/1] Funding Source: researchfish
Recent two-dimensional electronic spectroscopy (2DES) experiments have reported evidence of coherent dynamics of electronic excitations in several light-harvesting antennae. However, 2DES uses ultrafast coherent laser pulses as an excitation source; therefore, there is a current debate on whether coherent excitation dynamics is present under natural sunlight - incoherent - illumination conditions. In this letter, we show that even if incoherent light excites an electronic state with no initial quantum superpositions among excitonic states, energy transfer can proceed quantum coherently if nonequilibrium dynamics of the phonon environment takes place. Such nonequilibrium behavior manifests itself in non-Markovian evolution of electronic excitations and is typical of many photosynthetic systems. We therefore argue that light-harvesting antennae have mechanisms that could support coherent evolution under incoherent illumination.
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