Exciton Dissociation and Charge Separation at Donor-Acceptor Interfaces from Quantum-Classical Dynamics Simulations

Abstract

In organic photovoltaic (OPV) systems, exciton dissociation and ultrafast charge separation at donor-acceptor heterojunctions both play a key role in controlling the efficiency of the conversion of excitation energy into free charge carriers. In this work, nonadiabatic dynamics simulations based on the quantum-classical Liouville equation, are employed to study the real-time dynamics of exciton dissociation and charge separation at a model donor-acceptor interface. Benchmark comparisons for a variety of low dimensional donor-acceptor chain models are performed to assess the accuracy of the quantum classical dynamics technique referred to as the forward-backward trajectory solution (FBTS). Although not always quantitative, the FBTS approach offers a reasonable balance between accuracy and computational cost. The short-time dynamics of exciton dissociation in related higher-dimensional lattice models for the interface are also investigated to assess the effect of the dimensionality on the first steps in the mechanism of charge carrier generation.

References in corpus (16)

• The Role of Driving Energy and Delocalised States for Charge Separation in Organic Semiconductors
• Origin of the Efficient Polaron Pair Dissociation in Polymer--Fullerene Blends
• Exact quantum master equation via the calculus on path integrals
• Entropy and disorder enable charge separation in organic solar cells
• Direct observation of ultrafast long-range charge separation at polymer:fullerene heterojunctions
• Quantum-Classical Liouville Dynamics in the Mapping Basis
• Noise-induced quantum coherence drives photocarrier generation dynamics at polymeric semiconductor heterojunctions
• Nonadiabatic Dynamics in Open Quantum-Classical Systems: Forward-Backward Trajectory Solution
• Phonon-driven ultrafast exciton dissociation at donor-acceptor polymer heterojunctions
• Generalized Quantum Master Equations In and Out of Equilibrium: When Can One Win?
• On the identity of the identity operator in nonadiabatic linearized semiclassical dynamics
• Analysis of the Forward-Backward Trajectory Solution for the Mixed Quantum-Classical Liouville Equation
• Accurate nonadiabatic quantum dynamics on the cheap: making the most of mean field theory with master equations
• Phonon-Assisted Ultrafast Charge Separation in a Realistic PCBM Aggregate
• Ultrafast Charge Separation and Nongeminate Electron-Hole Recombination in Organic Photovoltaics
• Non-Markovian quantum-classical ratchet for ultrafast long-range electron-hole separation in condensed phases

Cited by in corpus (4)

• A partially linearized spin-mapping approach for nonadiabatic dynamics. I. Derivation of the theory
• Even a little delocalization produces large kinetic enhancements of charge-separation efficiency in organic photovoltaics
• A partially linearized spin-mapping approach for nonadiabatic dynamics. II. Analysis and comparison with related approaches
• A partially linearized spin-mapping approach for simulating nonlinear optical spectra