具有空间关联涨落的量子相干生物分子能量转移
Quantum coherent biomolecular energy transfer with spatially correlated fluctuations
摘要：
我们表明，生物分子发色团之间的量子相干转移的激发强烈的影响，由环境波动的空间相关性。后者是由于传播的环境模式或局部波动与有限的本地化长度。一个简单的玩具模型的一个单一的供体-受体对空间分离的发色团网站允许调查这些空间相关性的量子相干激发转移的影响。溶剂的声速决定了环境模式的波长，而环境模式的波长又必须与发色团位置的空间距离进行比较。当波长超过施主和受主位置之间的距离时，我们发现退相干受到强烈的抑制。此外，我们考虑两个空间分离的施主-受主对的影响下传播的环境模式。取决于它们的波长固定的声速的溶剂材料，相关性的空间范围可能会延伸到典型的对间距离，这可能会导致溶剂的散肩影响的增加。令人惊讶的是，这种影响被温度升高所抵消。
英文摘要：
We show that the quantum coherent transfer of excitations between biomolecular chromophores is strongly influenced by spatial correlations of the environmental fluctuations. The latter are due either to propagating environmental modes or to local fluctuations with a finite localization length. A simple toy model of a single donor-acceptor pair with spatially separated chromophore sites allows to investigate the influence of these spatial correlations on the quantum coherent excitation transfer. The sound velocity of the solvent determines the wave lengths of the environmental modes, which, in turn, has to be compared to the spatial distance of the chromophore sites. When the wave length exceeds the distance between donor and acceptor site, we find strong suppression of decoherence. In addition, we consider two spatially separated donor-acceptor pairs under the influence of propagating environmental modes. Depending on their wave lengths fixed by the sound velocity of the solvent material, the spatial range of correlations may extend over typical interpair distances, which can lead to an increase of the decohering influence of the solvent. Surprisingly, this effect is counteracted by increasing temperature.
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