Chen Lipeng, Gelin Maxim F, Domcke Wolfgang, Zhao Yang
Department of Chemistry , Technische Universität München , D-85747 Garching , Germany.
Division of Materials Science , Nanyang Technological University , Singapore 639798 , Singapore.
J Phys Chem Lett. 2018 Aug 16;9(16):4488-4494. doi: 10.1021/acs.jpclett.8b01887. Epub 2018 Jul 27.
Recent phase-locked femtosecond double-pump experiments on individual light-harvesting complexes LH2 of purple bacteria at ambient temperature revealed undamped oscillatory responses on a time scale of at least 400 fs [ Hildner et al. Science 2013 , 340 , 1448 ]. Using an excitonic Hamiltonian for LH2 available in the literature, we simulate these signals numerically by a method that treats excitonic couplings and exciton-phonon couplings in a nonperturbative manner. The simulations provide novel insights into the origin of coherent dynamics in individual LH2 complexes.
最近在室温下对单个紫色细菌光捕获复合物LH2进行的锁相飞秒双泵浦实验显示,在至少400飞秒的时间尺度上存在无阻尼振荡响应[希尔德纳等人,《科学》,2013年,第340卷,第1448页]。我们使用文献中可用的LH2激子哈密顿量,通过一种以非微扰方式处理激子耦合和激子-声子耦合的方法对这些信号进行数值模拟。这些模拟为单个LH2复合物中相干动力学的起源提供了新的见解。