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Electronic-vibrational resonance does not alter steady-state transport in natural light-harvesting systems

Leonardo F. Calder\'onChern ChuangPaul Brumer
Dec 2022
摘要
Oscillations in time-dependent 2D electronic spectra appear as evidence ofquantum coherence in light-harvesting systems related to electronic-vibrationalresonant interactions. Nature, however, takes place in a non-equilibriumsteady-state, so the relevance of these arguments to the natural process isunclear. Here we examine the role of intramolecular vibrations in thenon-equilibrium steady-state of photosynthetic dimers in the natural scenarioof incoherent light excitation. It is found that vibrations resonant with theenergy difference between exciton states do not increase the quantum yield northe imaginary part of the intersite coherence that is relevant for transportcompared with non-resonant vibrations in the natural non-equilibrium steadystate. That is, the vibration-electronic resonance interaction does not alterenergy transport under natural incoherent-light excitation conditions.
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