jp412782n_si_001.pdf (673.6 kB)
Nonadiabatic Molecular Dynamics Modeling of the Intrachain Charge Transport in Conjugated Diketopyrrolo-pyrrole Polymers
journal contribution
posted on 2014-04-03, 00:00 authored by Xing Gao, Hua Geng, Qian Peng, Jiajun Ren, Yuanping Yi, Dong Wang, Zhigang ShuaiUnderstanding the carrier transport
processes and predicting the
carrier mobility from first principle in organic electronic materials
has been a longstanding challenge. We have applied the nonadiabatic
Ehrenfest dynamics coupled with density functional tight binding (DFTB)
to investigate the carrier motion in the donor–acceptor type
polymer for photovoltaics. The equations of motion for the electrons
are evolved under the fixed subspace spanned by the active molecular
orbitals during each nuclear time step, and the feedback from charge
to the nuclei motions, namely, the polaronic effect, is considered.
We then use this methodology to investigate the charge transport dynamics
for the ladder-type poly(p-phenylenes) (LPPP) and
poly(diketopyrrolo-pyrrole (DPP)) series with ∼2 × 103 atoms. The carrier mobilities are evaluated via the diffusion
process. It was found that the diffusion abilities are determined
by the magnitude of transfer integrals and localization length for
frontier orbital, which is caused by the self-trapping effects (polaron)
arising from the double bond stretching and twisting motions. This
method can be useful in exploring the underlying charge transport
behavior and improving the structure design of materials in organic
electronics.
History
Usage metrics
Categories
Keywords
DFTBLPPPnuclei motionscharge transport dynamicsmaterialcarrier mobilitylocalization lengthpolaronic effectNonadiabatic Molecular Dynamics Modelingpolytransfer integralsnonadiabatic Ehrenfest dynamicscarrier motionstructure designIntrachain Charge TransportDPPcarrier transport processescharge transport behaviordiffusion abilitiesdiffusion processcarrier mobilitiestime step
Licence
Exports
RefWorks
BibTeX
Ref. manager
Endnote
DataCite
NLM
DC