Advanced

Insights into the Charge Carrier Terahertz Mobility in Polyfluorenes from Large-Scale Atomistic Simulations and Time-Resolved Terahertz Spectroscopy

Vukmirovic, Nenad; Ponseca, Carlito LU ; Nemec, Hynek; Yartsev, Arkady LU and Sundström, Villy LU (2012) In Journal of Physical Chemistry C 116(37). p.19665-19672
Abstract
Multiscale atomistic simulations were used to. understand the factors that determine the charge carrier mobility spectrum obtained from time-resolved terahertz (THz) spectroscopy in conjugated polymers. The simulation approach combines classical molecular dynamics simulations of atomic structure, large-scale electronic structure calculations, and the evaluation of the THz mobility using Kubo's linear response formula. We found that THz radiation probes a single carrier hop at low temperatures and high frequencies, while the transport over somewhat longer distances is probed in the opposite cases. Our results indicate that charge carrier transport at THz frequencies is thermally activated but with a much smaller activation energy compared... (More)
Multiscale atomistic simulations were used to. understand the factors that determine the charge carrier mobility spectrum obtained from time-resolved terahertz (THz) spectroscopy in conjugated polymers. The simulation approach combines classical molecular dynamics simulations of atomic structure, large-scale electronic structure calculations, and the evaluation of the THz mobility using Kubo's linear response formula. We found that THz radiation probes a single carrier hop at low temperatures and high frequencies, while the transport over somewhat longer distances is probed in the opposite cases. Our results indicate that charge carrier transport at THz frequencies is thermally activated but with a much smaller activation energy compared to the dc case. The shape of the real and imaginary part of the mobility spectral curve reveals the presence of above THz hopping rates that are relevant for charge carrier transport. Strong differences of the mobilities in the polymer and the corresponding monomer material are largely caused by stronger energetic disorder of the monomer material. (Less)
Please use this url to cite or link to this publication:
author
organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Journal of Physical Chemistry C
volume
116
issue
37
pages
19665 - 19672
publisher
The American Chemical Society
external identifiers
  • wos:000308855600008
  • scopus:84866667018
ISSN
1932-7447
DOI
10.1021/jp3055262
language
English
LU publication?
yes
id
f952832d-3834-4d43-9a08-e01ef2d89999 (old id 3190164)
date added to LUP
2012-12-04 08:07:10
date last changed
2017-01-01 03:40:09
@article{f952832d-3834-4d43-9a08-e01ef2d89999,
  abstract     = {Multiscale atomistic simulations were used to. understand the factors that determine the charge carrier mobility spectrum obtained from time-resolved terahertz (THz) spectroscopy in conjugated polymers. The simulation approach combines classical molecular dynamics simulations of atomic structure, large-scale electronic structure calculations, and the evaluation of the THz mobility using Kubo's linear response formula. We found that THz radiation probes a single carrier hop at low temperatures and high frequencies, while the transport over somewhat longer distances is probed in the opposite cases. Our results indicate that charge carrier transport at THz frequencies is thermally activated but with a much smaller activation energy compared to the dc case. The shape of the real and imaginary part of the mobility spectral curve reveals the presence of above THz hopping rates that are relevant for charge carrier transport. Strong differences of the mobilities in the polymer and the corresponding monomer material are largely caused by stronger energetic disorder of the monomer material.},
  author       = {Vukmirovic, Nenad and Ponseca, Carlito and Nemec, Hynek and Yartsev, Arkady and Sundström, Villy},
  issn         = {1932-7447},
  language     = {eng},
  number       = {37},
  pages        = {19665--19672},
  publisher    = {The American Chemical Society},
  series       = {Journal of Physical Chemistry C},
  title        = {Insights into the Charge Carrier Terahertz Mobility in Polyfluorenes from Large-Scale Atomistic Simulations and Time-Resolved Terahertz Spectroscopy},
  url          = {http://dx.doi.org/10.1021/jp3055262},
  volume       = {116},
  year         = {2012},
}