Charge transport along phenylenevinylene molecular wires

Prins, P.R.; Grozema, Ferdinand C.; Siebbeles, L. D. A.

doi:10.1080/08927020600835657

Cited by 14 publications

(24 citation statements)

References 49 publications

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“…Here we obtain the density of states (DOS) by first partitioning the system onto localization units, and subsequently evaluating the ionization energy for each unit, taking into account electrostatic and inductive contributions that result from the interaction of the hole with the molecular environment. Other approaches include a combination of atomistic molecular dynamics simulations with calculations of electronic structure using tight‐binding, fragment molecular orbital, charge‐patching, tight‐binding DFT, as well as semi‐empirical approaches . More details can be found in ref.…”

Section: Resultsmentioning

confidence: 99%

Effect of Mesoscale Ordering on the Density of States of Polymeric Semiconductors

Gemünden

Poelking

Kremer

et al. 2015

Macromol. Rapid Commun.

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A multiscale simulation scheme, which incorporates both long-range conformational disorder and local molecular ordering, is proposed for predicting large-scale morphologies and charge transport properties of polymeric semiconductors. Using poly(3-hexylthiophene) as an example, it is illustrated how the energy landscape and its spatial correlations evolve with increasing degree of structural order in mesophases with amorphous, uniaxial, and biaxial nematic ordering. It is shown that the formation of low-lying energy states in more ordered systems is mostly due to larger (on average) conjugation lengths and not due to electrostatic interactions. The proposed scheme is general and can be applied to a wide range of polymeric organic materials.

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Section: Resultsmentioning

confidence: 99%

Effect of Mesoscale Ordering on the Density of States of Polymeric Semiconductors

Gemünden

Poelking

Kremer

et al. 2015

Macromol. Rapid Commun.

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show abstract

“…The fluctuations induced by the solvent are then the primary driving force for charge motion. In wavepacket propagation, the role of rotational diffusion is to enhance mobility by removing twists near 90 o that restrict charge motion 5 . This leads to a weaker dependence on t rot , such that changing t rot from 10 to 100 ps changes the mobility by less than a factor of 4 5 , as opposed to the factor of 10 predicted here based on the inverse relationship between  and t rot .…”

Section: Discussionmentioning

confidence: 99%

“…One factor is the large difference in time scales of the two computational approaches. In the wavepacket propagation methods, t rot is taken as about 60 ps and a few hundred simulations are run, each with a length of about 25 ps 3,5 .…”

Section: Discussionmentioning

confidence: 99%

“…Current theoretical models of solution-phase mobility use the time-dependent Schrödinger equation to propagate the charge along a polymer chain [2][3][4][5][6] . For poly(para-phenylene vinylene) (PPV), and microwaves with a frequency of 34 GHz, such models estimate the mobility to be about 60 cm 2 /Vs on a long chain.…”

Section: Introductionmentioning

confidence: 99%

“…Here, we use a quantum chemical model of the polymer that is equivalent to that used above [2][3][4][5][6] , but start from the opposite extreme of incoherent motion of the charge along the polymer. Within the adiabatic approximation considered here, the motion of the charge can be viewed as follows.…”

Section: Introductionmentioning

confidence: 99%

See 2 more Smart Citations

Brownian dynamics simulations of charge mobility on conjugated polymers in solution

Albu

Yaron

2013

The Journal of Chemical Physics

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A model is developed for the mobility of a charge carrier along a conjugated polymer dissolved in solution, as measured by time-resolved microwave conductivity. Each unit cell of the polymer is assigned a torsional degree of freedom, with Brownian dynamics used to include the effects of solvent on the torsions. The barrier to torsional motion is substantially enhanced in the vicinity of the charge, leading to self-trapping of the charge onto a planarized region of the polymer chain. Within the adiabatic approximation used here, motion arises when regions of the polymer on either side of the charge fluctuate into planarity and the wavefunction spreads in the corresponding direction. Well-converged estimates for the mobility are obtained for model parameters where the adiabatic approximation holds. For the parameters expected for conjugated polymers, where crossing between electronic surfaces may lead to breakdown in the adiabatic approximation, estimates for the mobility are obtained via extrapolation. Nonadiabatic contributions from hopping between electronic surfaces are therefore ignored. The resulting mobility is inversely proportional to the rotational diffusion time, trot, of a single unit cell about the polymer axis in the absence of intramolecular forces. For trot of 75 ps, the long-chain mobility of poly(para-phenylene vinylene) is estimated to be between 0.09 and 0.4 cm(2)∕Vs. This is in reasonable agreement with experimental values for the polymer, however, the nonadiabatic contribution to the mobility is not considered, nor are effects arising from stretching degrees of freedom or breaks in conjugation.

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Charge Transport along Isolated Conjugated Molecular Wires Measured by Pulse Radiolysis Time‐Resolved Microwave Conductivity

Grozema

Siebbeles

2011

Charge and Exciton Transport Through Molecular Wires

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Charge transport along phenylenevinylene molecular wires

Cited by 14 publications

References 49 publications

Effect of Mesoscale Ordering on the Density of States of Polymeric Semiconductors

Effect of Mesoscale Ordering on the Density of States of Polymeric Semiconductors

Brownian dynamics simulations of charge mobility on conjugated polymers in solution

Charge Transport along Isolated Conjugated Molecular Wires Measured by Pulse Radiolysis Time‐Resolved Microwave Conductivity

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