Predictive Study of Charge Transport in Disordered Semiconducting Polymers

Athanasopoulos, Stavros; Kirkpatrick, James; Martínez, Diego; Frost, Jarvist M.; Foden, Clare; Walker, Alison B.; Nelson, Jenny

doi:10.1021/nl0708718

Cited by 83 publications

(102 citation statements)

References 21 publications

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“…The ability to obtain device-scale characteristics, such as the power conversion efficiency or the J-V curve, comes at the price of abstracting out much of molecular interaction behavior that occurs on lengthscales <1 nm. Instead, the disordered energetic landscape resulting from these sub-lattice interactions is estimated using alternative methods [125,126]. Commonly, a Gaussian Disorder Model is used, which applies a perturbation to a site's energy, selected randomly from a Gaussian distribution with a typical standard deviation of σ = 100 meV [127,128], inspired by explicit QCCs of charge carrier densities within the material [129,130].…”

Section: Charge Mobilitymentioning

confidence: 99%

Computationally connecting organic photovoltaic performance to atomistic arrangements and bulk morphology

Jones

Jankowski

2017

Molecular Simulation

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Rationally designing roll-to-roll printed organic photovoltaics requires a fundamental understanding of active layer morphologies optimized for charge separation and transport, and which ingredients can be used to self-assemble those morphologies. In this review article we discuss advances in three areas of computational modeling that provide insight into active layer morphology and the charge transport properties that result. We explain the computational bottlenecks prohibiting atomistically-detailed simulations of device-scale active layers and the coarse-graining and hardware acceleration strategies for overcoming them. We review coarse-grained simulations of organic photovoltaic active layers and show that high throughput simulations of experimentally-relevant length scales are now accessible. We describe a new Python package diffractometer that permits grazing-incidence X-ray scattering patterns of simulated active layers to be compared against experiments. We explain the accurate calculation of charge-carrier mobilities from coarse-grained active layer morphologies by using atomistic backmapping, quantum chemical calculations, and kinetic Monte Carlo simulations. We employ these simulations to show that ordering of poly(3-hexylthiophene-2,5-diyl) explains a factor of 1000 improvement in charge mobility. In concert, we present a suite of computational tools enabling large-scale electronic properties of organic photovoltaics to be studied and screened for by molecular simulations.

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Section: Charge Mobilitymentioning

confidence: 99%

Computationally connecting organic photovoltaic performance to atomistic arrangements and bulk morphology

Jones

Jankowski

2017

Molecular Simulation

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“…Therefore a successful theory of the charge transport should include ingredients of both models and describe the dynamic and static disorders in a realistic manner. Toward this goal, significant advances have been made recently, including the Marcus theory with ab initio determined microscopic parameters, [16][17][18][19][20] the construction of model Hamiltonians with the transfer integrals evaluated quantum mechanically, [21][22][23] and using time-dependent perturbation theory to determine the phonon-assisted transition rate, 24,25 among others. However, all these methods have certain elements of empiricism, relying on classical force fields to compute material structure and/or phonon spectrum.…”

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confidence: 99%

First-principles determination of charge carrier mobility in disordered semiconducting polymers

Zhang

Lü

2010

Phys. Rev. B

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“…Most of existing theoretical work has been focused on the characteristics of optical and transport properties of isolated PFO oligomers, 5,20,21 with few efforts on studying intermolecular interactions in crystalline packing. 14,[22][23][24] Unfortunately, simulations of realistic disordered materials as used in devices are scarce. 19 The main reason is the computationally unmanageable number of atoms in realistic amorphous polymer systems.…”

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confidence: 99%

Electronic Structure of Self-Assembled Amorphous Polyfluorenes

et al. 2008

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We investigate the role of conformational disorder and intermolecular interactions on the electronic structure of amorphous clusters of polyfluorenes. Classical molecular dynamics simulations are used to determine probable molecular geometries and chain packing, and first-principles density functional theory calculations are employed to determine electronic structure and orbital localization properties. Intramolecular and intermolecular effects are disentangled by contrasting results for densely packed oligomer clusters and for ensembles of isolated oligomers with the same intramolecular geometries. Our simulations show that intermolecular disorder allows for nearly planar configurations of interacting fluorenes compared to the isolated molecules. This rationalizes the experimentally detected formation of the planar crystalline morphologies that frequently accompany twisted glassy configurations in fluorene films. The energy gap (HOMO−LUMO gap) significantly decreases for planar configurations. The electron and hole orbital energies are strongly dependent on both torsional angles and intermolecular interactions. This leads to strong localization of electronic states in amorphous polymer aggregates, which is analyzed by examining the respective orbital participation ratios. Notably, the energies of unoccupied levels show stronger dependence on the conformational disorder, compared to that of occupied levels. This results in the more probable formation of trap states near the edge of the conduction band than near the valence band.

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Predictive Study of Charge Transport in Disordered Semiconducting Polymers

Cited by 83 publications

References 21 publications

Computationally connecting organic photovoltaic performance to atomistic arrangements and bulk morphology

Computationally connecting organic photovoltaic performance to atomistic arrangements and bulk morphology

First-principles determination of charge carrier mobility in disordered semiconducting polymers

Electronic Structure of Self-Assembled Amorphous Polyfluorenes

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