Atomistic Simulations of Charge Separation at a Nanohybrid Interface: Relevance of Photoinduced Initial State Preparation,The Journal of Physical Chemistry Letters

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Atomistic Simulations of Charge Separation at a Nanohybrid Interface: Relevance of Photoinduced Initial State Preparation
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2017-12-27 00:00:00 , DOI: 10.1021/acs.jpclett.7b02772
Thomas Plehn ₁ , Dirk Ziemann ₁ , Volkhard May ₁

Affiliation

Charge separation kinetics at a nanohybrid interface are investigated in their dependence on ultrafast optical excitation. A prototypical organic/inorganic interface is considered. It is formed by a vertical stacking of 20 para-sexiphenyl molecules physisorbed on a ZnO nanocluster of 3783 atoms. A first principle parametrized Hamiltonian is employed, and the photoinduced subpicosecond evolution of Frenkel-excitons in the organic part is analyzed besides the formation of charge separated states across the interface. The interface absorption spectrum is calculated. Together, the data indicate that the charge separation is based on the direct excitation of the charge separated states but also on the migration of created Frenkel excitons to the interface with subsequent decay. Further, the photoinduced interface dynamics are compared with data resulting from direct set-ups of an initially excited state. Mostly such set-ups lead to substantially different charge separation processes.

中文翻译：

纳米杂化界面电荷分离的原子模拟：光诱导初始状态制备的相关性

研究了纳米杂化界面上电荷分离动力学对超快光激发的依赖性。考虑了原型有机/无机界面。它是由20个标准杆的垂直堆叠形成的-sexiphenyl分子物理吸附在3783个原子的ZnO纳米簇上。首先采用参数化的哈密顿量原理，除了在界面上形成电荷分离态以外，还分析了有机部分中Frenkel-激子的光诱导亚皮秒演化。计算界面吸收光谱。总之，数据表明电荷分离是基于电荷分离态的直接激发，而且还基于产生的Frenkel激子向界面的迁移以及随后的衰减。此外，将光致界面动力学与直接激发初始激发态建立的数据进行比较。通常，这样的设置导致基本上不同的电荷分离过程。

更新日期：2017-12-27

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