Diabatic States of Charge Transfer with Constrained Charge Equilibration DOI
Sohang Kundu,

Hong‐Zhou Ye,

Timothy C. Berkelbach

et al.

Journal of Chemical Theory and Computation, Journal Year: 2025, Volume and Issue: unknown

Published: March 20, 2025

Charge transfer (CT) processes that are electronically nonadiabatic ubiquitous in chemistry, biology, and materials science, but their theoretical description requires diabatic states or adiabatic excited states. For complex systems, these latter more difficult to calculate than the ground state. Here, we propose a simple method obtain states, including energies charges, by constraining atomic charges within charge equilibration framework. two-state exact coupling can be determined, from which excited-state energy also calculated. The viewed as an affordable alternative constrained density functional theory (CDFT), so call it (CQEq). We test CQEq on anthracene-tetracyanoethylene CT reductive decomposition of ethylene carbonate lithium metal surface. find predicts energies, excitation good agreement with CDFT, is promising for combination machine learning force fields study condensed phase.

Language: Английский

Diabatic States of Charge Transfer with Constrained Charge Equilibration DOI
Sohang Kundu,

Hong‐Zhou Ye,

Timothy C. Berkelbach

et al.

Journal of Chemical Theory and Computation, Journal Year: 2025, Volume and Issue: unknown

Published: March 20, 2025

Charge transfer (CT) processes that are electronically nonadiabatic ubiquitous in chemistry, biology, and materials science, but their theoretical description requires diabatic states or adiabatic excited states. For complex systems, these latter more difficult to calculate than the ground state. Here, we propose a simple method obtain states, including energies charges, by constraining atomic charges within charge equilibration framework. two-state exact coupling can be determined, from which excited-state energy also calculated. The viewed as an affordable alternative constrained density functional theory (CDFT), so call it (CQEq). We test CQEq on anthracene-tetracyanoethylene CT reductive decomposition of ethylene carbonate lithium metal surface. find predicts energies, excitation good agreement with CDFT, is promising for combination machine learning force fields study condensed phase.

Language: Английский

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