Scalable High-Performance Algorithm for the Simulation of Exciton Dynamics. Application to the Light-Harvesting Complex II in the Presence of Resonant Vibrational Modes
Scalable High-Performance Algorithm for the Simulation of Exciton Dynamics. Application to the Light-Harvesting Complex II in the Presence of Resonant Vibrational Modes
复制标题
DOI：
10.1021/ct500629s
复制
发表时间：
2014-09-01
影响因子：
5.5
通讯作者：
Aspuru-Guzik, Alan
中科院分区：
文献类型：
--
作者：
Kreisbeck, Christoph;Kramer, Tobias;Aspuru-Guzik, Alan
精确模拟激子能量转移的分子复合物耦合的电子和振动自由度是必不可少的比较激子系统参数从头计算方法与测量的时间分辨光谱。几个精确的方法来计算激子动力学内的密度矩阵形式主义是已知的，但限于小系统，少于10个网站，由于它们的计算复杂性。为了研究更大系统中的激子能量转移，我们使用开放计算语言（OpenCL）将精确分层运动方程（HEOM）方法适应并扩展到各种高性能众核平台。对于在菠菜中发现的捕光复合物II（LHC II），HEOM结果偏离了近似理论的预测，并澄清了传输过程的时间尺度。我们调查的影响共振耦合振动的放松，并表明转移不依赖于特定模式的微调。
The accurate simulation of excitonic energy transfer in molecular complexes with coupled electronic and vibrational degrees of freedom is essential for comparing excitonic system parameters obtained from ab initio methods with measured time-resolved spectra. Several exact methods for computing the exciton dynamics within a density-matrix formalism are known but are restricted to small systems with less than 10 sites due to their computational complexity. To study the excitonic energy transfer in larger systems, we adapt and extend the exact hierarchical equation of motion (HEOM) method to various high-performance many-core platforms using the Open Compute Language (OpenCL). For the light-harvesting complex II (LHC II) found in spinach, the HEOM results deviate from predictions of approximate theories and clarify the time scale of the transfer process. We investigate the impact of resonantly coupled vibrations on the relaxation and show that the transfer does not rely on a fine-tuning of specific modes.