title: "Watching" Polaron Pair Formation from First-Principles Electron-Nuclear Dynamics.
abstract: The formation of polaron pairs is one of the important photophysical processes that take place after the excitation in semiconducting organic polymers. First-principles Ehrenfest excited-state dynamics is a unique tool to investigate ultrafast photoinduced charge carrier dynamics and related nonequilibrium processes involving correlated electron-nuclear dynamics. In this work the formation of polaron pairs and their dynamical evolution in an oligomer of seven thiophene units is investigated with a combined approach of first-principles exciton-nuclear dynamics and wavelet analysis. The real-time formation of a polaron pair can be observed in the dipole evolution during the excited-state dynamics. The possible driving force of the polaron pair formation is investigated through qualitative correlation between the structural dynamics and the dipole evolution. The time-dependent characteristics and spectroscopic consequences of the polaron pair formation are probed using the wavelet analysis.
authors: Dipartimento di Scienze Chimiche, Università di Napoli 'Federico II', Complesso Universitario di M. S. Angelo , via Cintia, I-80126 Napoli, Italy.
authors: Greta
authors: G
authors: Donati
authors: Department of Chemistry, University of Washington , Seattle, Washington 98195, United States.
authors: David B
authors: DB
authors: Lingerfelt
authors: Department of Chemistry, University of Washington , Seattle, Washington 98195, United States.
authors: Alessio
authors: A
authors: Petrone
authors: Dipartimento di Scienze Chimiche, Università di Napoli 'Federico II', Complesso Universitario di M. S. Angelo , via Cintia, I-80126 Napoli, Italy.|Italian Institute of Technology, IIT@CRIB Center for Advanced Biomaterials for Healthcare, Largo Barsanti e Matteucci, I-80125 Napoli, Italy.
authors: Nadia
authors: N
authors: Rega
authors: Department of Chemistry, University of Washington , Seattle, Washington 98195, United States.
authors: Xiaosong
authors: X
authors: Li