Quantum Dynamics of Exciton Transport and Dissociation in Multichromophoric Systems.
Quantum Dynamics of Exciton Transport and Dissociation in Multichromophoric Systems.
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DOI：
10.1146/annurev-physchem-090419-040306
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发表时间：
2021-02
影响因子：
14.7
通讯作者：
W. Popp;D. Brey;R. Binder;I. Burghardt
中科院分区：
文献类型：
--
作者：
W. Popp;D. Brey;R. Binder;I. Burghardt
由于站点到站点的电子耦合，激子离域，非绝热效应和振动耦合的微妙的相互作用，需要量子动力学研究来阐明超快的光诱导能量和电荷转移事件在有机多色系统的细节。在这方面，我们回顾了一种方法，结合第一性原理参数化晶格哈密顿与精确的量子动力学模拟，使用先进的多组态方法。重点关注有机分子材料中的基元转移步骤，我们解决了均聚物（特别是代表聚（3-己基噻吩）聚合物的聚噻吩型材料）中相干激子迁移和电荷转移激子的产生，以及聚合物中的激子解离：富勒烯异质结。我们强调相干转移的作用，由于高频声子模式的捕获效应，以及由于驱动扩散动力学的低频软模式的热激活。预计物理化学年度评论的最终在线出版日期，第72卷是2021年4月。请访问http://www.annualreviews.org/page/journal/pubdates了解修订后的估计数。
Due to the subtle interplay of site-to-site electronic couplings, exciton delocalization, nonadiabatic effects, and vibronic couplings, quantum dynamical studies are needed to elucidate the details of ultrafast photoinduced energy and charge transfer events in organic multichromophoric systems. In this vein, we review an approach that combines first-principles parameterized lattice Hamiltonians with accurate quantum dynamical simulations using advanced multiconfigurational methods. Focusing on the elementary transfer steps in organic molecular materials, we address coherent exciton migration and creation of charge transfer excitons in homopolymers, notably polythiophene-type materials representative of the poly(3-hexylthiophene) polymer, as well as exciton dissociation at polymer:fullerene heterojunctions. We emphasize the role of coherent transfer, trapping effects due to high-frequency phonon modes, and thermal activation due to low-frequency soft modes that drive a diffusive dynamics.Expected final online publication date for the Annual Review of Physical Chemistry, Volume 72 is April 2021. Please see http://www.annualreviews.org/page/journal/pubdates for revised estimates.