Department of Physics and Astronomy, University College London, Gower Street, London WC1E 6BT, United Kingdom.
Phys Rev Lett. 2009 Oct 2;103(14):146404. doi: 10.1103/PhysRevLett.103.146404. Epub 2009 Oct 1.
I investigate energy transfer in a donor-acceptor pair beyond weak system-bath coupling. I identify a transition from coherent to incoherent dynamics with increasing temperature, due to multiphonon effects not captured by a standard weak-coupling treatment. The crossover temperature has a marked dependence on the degree of spatial correlation between fluctuations experienced at the two system sites. For strong correlations, this leads to the possibility of coherence surviving into a high-temperature regime.
我研究了在 donor-acceptor 对中超越弱系统-浴耦合的能量转移。我发现,随着温度的升高,由于标准弱耦合处理无法捕捉到的多声子效应,动力学从相干态向非相干态转变。交叉温度与两个系统位置经历的涨落之间的空间相关性程度有明显的依赖关系。对于强相关性,这导致相干性有可能在高温范围内存在。