Peng, Wei-Tao; Brey, Dominik; Giannini, Samuele; Dell'Angelo, David; Burghardt, Irene; Blumberger, Jochen; (2022) Exciton Dissociation in a Model Organic Interface: Excitonic State-Based Surface Hopping versus Multiconfigurational Time-Dependent Hartree. The Journal of Physical Chemistry Letters , 13 pp. 7105-7112. 10.1021/acs.jpclett.2c01928. (In press).

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Abstract

Quantum dynamical simulations are essential for a molecular-level understanding of light-induced processes in optoelectronic materials, but they tend to be computationally demanding. We introduce an efficient mixed quantum-classical nonadiabatic molecular dynamics method termed eXcitonic state-based Surface Hopping (X-SH), which propagates the electronic Schrödinger equation in the space of local excitonic and charge-transfer electronic states, coupled to the thermal motion of the nuclear degrees of freedom. The method is applied to exciton decay in a 1D model of a fullerene-oligothiophene junction, and the results are compared to the ones from a fully quantum dynamical treatment at the level of the Multilayer Multiconfigurational Time-Dependent Hartree (ML-MCTDH) approach. Both methods predict that charge-separated states are formed on the 10-100 fs time scale via multiple "hot-exciton dissociation" pathways. The results demonstrate that X-SH is a promising tool advancing the simulation of photoexcited processes from the molecular to the true nanomaterials scale.

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