Non-Markovian stochastic Schrödinger equation at finite temperatures for charge carrier dynamics in organic crystals.
Non-Markovian stochastic Schrödinger equation at finite temperatures for charge carrier dynamics in organic crystals.
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DOI：
10.1063/1.4773319
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发表时间：
2013-01
期刊：
影响因子：
--
通讯作者：
Xinxin Zhong;Yi Zhao
中科院分区：
文献类型：
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作者：
Xinxin Zhong;Yi Zhao
提出了有限温度下的新非马尔可夫随机薛定谔方程，以正确描述有机分子晶体中的载流子动力学。位点能量和电子耦合中的电子-声子相互作用是由相应的谱密度函数生成的随时间变化的复值随机波动合并的。因此，该方法很容易扩展到研究具有数千个分子位点的系统中的相干跳跃电荷转移。通过自旋玻色子模型和现实的 Fenna-Matthews-Olson 复合体中载流子动力学的数值模拟证明了本方法的能力。结果表明，非马尔可夫效应和复值随机力对于保证细节平衡至关重要。在长链供体-受体系统的应用中，从扩散系数的温度依赖性中发现相干到跳跃电荷转移的特性也很有趣。
A new non-Markovian stochastic Schrödinger equation at finite temperatures is presented to correctly describe charge carrier dynamics in organic molecular crystals. The electron-phonon interactions in both site energies and electronic couplings are incorporated by the time-dependent complex-valued random fluctuations which are generated from corresponding spectral density functions. The approach is thus easily extended to investigate coherent-to-hopping charge transfer in systems with thousands of molecular sites. The capability of present approach is demonstrated by numerical simulations of carrier dynamics in the spin-boson model and a realistic Fenna-Matthews-Olson complex. The results manifest that the non-Markovian effect and complex-valued random forces are essential to guarantee the detailed balance. In an application to a long-chain donor-acceptor system, it is also interesting to find a property of coherent-to-hopping charge transfer from temperature dependence of diffusion coefficients.