Tensor-Train Format Hierarchical Equations of Motion Formalism: Charge Transfer in Organic Semiconductors via Dissipative Holstein Models,Journal of Chemical Theory and Computation

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Tensor-Train Format Hierarchical Equations of Motion Formalism: Charge Transfer in Organic Semiconductors via Dissipative Holstein Models
Journal of Chemical Theory and Computation ( IF 5.7 ) Pub Date : 2024-08-17 , DOI: 10.1021/acs.jctc.4c00711
Hideaki Takahashi ₁ , Raffaele Borrelli ₁

Affiliation

Hierarchical Equations of Motion (HEOM) in the Tensor-Train (TT) representation is applied to study the charge-transfer dynamics in organic semiconductors (OSCs). The theoretical formulation as well as the basic computational aspects of HEOM-TT are discussed in detail. Charge transfer in OSCs is modeled using dissipative polaronic models that incorporate the effects of both high- and low-frequency molecular vibrations, and it is simulated in a fully quantum and nonperturbative manner, which has not been studied intensively. The capability of treating complex electron-vibrational systems is examined by analyzing and comparing the numerical behavior of the time-dependent variational approach and the time-Alternating Minimal Energy methods and by calculating the current autocorrelation function and diffusivity across various models. Our results indicate that the HEOM-TT framework offers a robust tool for the detailed analysis of complex polaronic systems, suggesting its potential for broader applications.

中文翻译：

张量序列格式运动形式的层次方程：通过耗散荷斯坦模型的有机半导体中的电荷转移

张量序列 (TT) 表示形式的分层运动方程 (HEOM) 用于研究有机半导体 (OSC) 中的电荷转移动力学。详细讨论了 HEOM-TT 的理论公式和基本计算方面。 OSC 中的电荷转移是使用耗散极化模型建模的，该模型结合了高频和低频分子振动的影响，并以完全量子和非微扰的方式进行模拟，但尚未得到深入研究。通过分析和比较瞬态变分法和时间交替最小能量法的数值行为，并计算各种模型的当前自相关函数和扩散率，检验处理复杂电子振动系统的能力。我们的结果表明，HEOM-TT 框架为复杂极化子系统的详细分析提供了强大的工具，表明其具有更广泛应用的潜力。

更新日期：2024-08-17

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