Drift of charge carriers in crystalline organic semiconductors.
J Chem Phys
; 144(14): 144905, 2016 Apr 14.
Article
em En
| MEDLINE
| ID: mdl-27083750
ABSTRACT
We investigate the direct-current response of crystalline organic semiconductors in the presence of finite external electric fields by the quantum-classical Ehrenfest dynamics complemented with instantaneous decoherence corrections (IDC). The IDC is carried out in the real-space representation with the energy-dependent reweighing factors to account for both intermolecular decoherence and energy relaxation by which conduction occurs. In this way, both the diffusion and drift motion of charge carriers are described in a unified framework. Based on an off-diagonal electron-phonon coupling model for pentacene, we find that the drift velocity initially increases with the electric field and then decreases at higher fields due to the Wannier-Stark localization, and a negative electric-field dependence of mobility is observed. The Einstein relation, which is a manifestation of the fluctuation-dissipation theorem, is found to be restored in electric fields up to â¼10(5) V/cm for a wide temperature region studied. Furthermore, we show that the incorporated decoherence and energy relaxation could explain the large discrepancy between the mobilities calculated by the Ehrenfest dynamics and the full quantum methods, which proves the effectiveness of our approach to take back these missing processes.
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Base de dados:
MEDLINE
Tipo de estudo:
Prognostic_studies
Idioma:
En
Ano de publicação:
2016
Tipo de documento:
Article