Molecular dynamics and charge transport in organic semiconductors: a classical approach to modeling electron transferElectronic supplementary information (ESI) available. See DOI: 10.1039/c6sc04547b
Organic photovoltaics (OPVs) are a promising carbon-neutral energy conversion technology, with recent improvements pushing power conversion efficiencies over 10%. A major factor limiting OPV performance is inefficiency of charge transport in organic semiconducting materials (OSCs). Due to strong cou...
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Format | Journal Article |
Language | English |
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28.03.2017
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Abstract | Organic photovoltaics (OPVs) are a promising carbon-neutral energy conversion technology, with recent improvements pushing power conversion efficiencies over 10%. A major factor limiting OPV performance is inefficiency of charge transport in organic semiconducting materials (OSCs). Due to strong coupling with lattice degrees of freedom, the charges form polarons, localized quasi-particles comprised of charges dressed with phonons. These polarons can be conceptualized as pseudo-atoms with a greater effective mass than a bare charge. We propose that due to this increased mass, polarons can be modeled with Langevin molecular dynamics (LMD), a classical approach with a computational cost much lower than most quantum mechanical methods. Here we present LMD simulations of charge transfer between a pair of fullerene molecules, which commonly serve as electron acceptors in OSCs. We find transfer rates consistent with experimental measurements of charge mobility, suggesting that this method may provide quantitative predictions of efficiency when used to simulate materials on the device scale. Our approach also offers information that is not captured in the overall transfer rate or mobility: in the simulation data, we observe exactly when and why intermolecular transfer events occur. In addition, we demonstrate that these simulations can shed light on the properties of polarons in OSCs. Much remains to be learned about these quasi-particles, and there are no widely accepted methods for calculating properties such as effective mass and friction. Our model offers a promising approach to exploring mass and friction as well as providing insight into the details of polaron transport in OSCs.
Using
ab initio
calculations of charges in PCBM fullerenes, a multiscale approach applies classical molecular dynamics to model charge transfer. |
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AbstractList | Organic photovoltaics (OPVs) are a promising carbon-neutral energy conversion technology, with recent improvements pushing power conversion efficiencies over 10%. A major factor limiting OPV performance is inefficiency of charge transport in organic semiconducting materials (OSCs). Due to strong coupling with lattice degrees of freedom, the charges form polarons, localized quasi-particles comprised of charges dressed with phonons. These polarons can be conceptualized as pseudo-atoms with a greater effective mass than a bare charge. We propose that due to this increased mass, polarons can be modeled with Langevin molecular dynamics (LMD), a classical approach with a computational cost much lower than most quantum mechanical methods. Here we present LMD simulations of charge transfer between a pair of fullerene molecules, which commonly serve as electron acceptors in OSCs. We find transfer rates consistent with experimental measurements of charge mobility, suggesting that this method may provide quantitative predictions of efficiency when used to simulate materials on the device scale. Our approach also offers information that is not captured in the overall transfer rate or mobility: in the simulation data, we observe exactly when and why intermolecular transfer events occur. In addition, we demonstrate that these simulations can shed light on the properties of polarons in OSCs. Much remains to be learned about these quasi-particles, and there are no widely accepted methods for calculating properties such as effective mass and friction. Our model offers a promising approach to exploring mass and friction as well as providing insight into the details of polaron transport in OSCs.
Using
ab initio
calculations of charges in PCBM fullerenes, a multiscale approach applies classical molecular dynamics to model charge transfer. |
Author | Van Voorhis, Troy Gray, Stephen K Larsen, Ross E Darling, Seth B Tretiak, Sergei Ratcliff, Laura E Bair, Raymond A Pelzer, Kenley M Vázquez-Mayagoitia, Álvaro |
AuthorAffiliation | University of Chicago Argonne Leadership Computing Facility Theoretical Division Computational Science Center Argonne National Laboratory Mathematics and Computer Science Division Institute for Molecular Engineering Department of Chemistry Massachusetts Institute of Technology Computer, Environment, and Life Sciences Computation Institute Center for Nanoscale Materials Center for Integrated Nanotechnologies Materials Science Division National Renewable Energy Laboratory Center for Nonlinear Studies Los Alamos National Laboratory |
AuthorAffiliation_xml | – name: Mathematics and Computer Science Division – name: Center for Nanoscale Materials – name: National Renewable Energy Laboratory – name: Department of Chemistry – name: Computer, Environment, and Life Sciences – name: Massachusetts Institute of Technology – name: Center for Integrated Nanotechnologies – name: Institute for Molecular Engineering – name: Materials Science Division – name: Theoretical Division – name: Argonne National Laboratory – name: Los Alamos National Laboratory – name: Computation Institute – name: Argonne Leadership Computing Facility – name: University of Chicago – name: Computational Science Center – name: Center for Nonlinear Studies |
Author_xml | – sequence: 1 givenname: Kenley M surname: Pelzer fullname: Pelzer, Kenley M – sequence: 2 givenname: Álvaro surname: Vázquez-Mayagoitia fullname: Vázquez-Mayagoitia, Álvaro – sequence: 3 givenname: Laura E surname: Ratcliff fullname: Ratcliff, Laura E – sequence: 4 givenname: Sergei surname: Tretiak fullname: Tretiak, Sergei – sequence: 5 givenname: Raymond A surname: Bair fullname: Bair, Raymond A – sequence: 6 givenname: Stephen K surname: Gray fullname: Gray, Stephen K – sequence: 7 givenname: Troy surname: Van Voorhis fullname: Van Voorhis, Troy – sequence: 8 givenname: Ross E surname: Larsen fullname: Larsen, Ross E – sequence: 9 givenname: Seth B surname: Darling fullname: Darling, Seth B |
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