Abstract
The exact factorization of the time-dependent electron–nuclear wavefunction has been employed successfully in the field of quantum molecular dynamics simulations for interpreting and simulating light-induced ultrafast processes. In this work, we summarize the major developments leading to the formulation of a trajectory-based approach, derived from the exact factorization equations, capable of dealing with nonadiabatic electronic processes, and including spin-orbit coupling and the non-perturbative effect of an external time-dependent field. This trajectory-based quantum-classical approach has been dubbed coupled-trajectory mixed quantum-classical (CT-MQC) algorithm, whose performance is tested here to study the photo-dissociation dynamics of IBr.Graphic abstract
Highlights
The theoretical description of nonequilibrium processes at the microscopic scale poses continuous challenges in many fields, such as molecular and chemical physics, condensed matter physics, and theoretical chemistry
In the domain of quantum molecular dynamics, approximations can be intended in various way, (i) to reduce the complexity of the original problem via simplified models, (ii) to make the underlying equations of motion computationally tractable based on mathematical or physical observations, or (iii) to neglect some effects in favor of others depending on the situations
While a comprehensive discussion on these points is beyond the scope of this work, we focus here on the possibility of capturing nonadiabatic effects and quantum decoherence during photo-induced ultrafast processes, by means of the quantum-classical scheme derived from the exact factorization
Summary
The theoretical description of nonequilibrium processes at the microscopic scale poses continuous challenges in many fields, such as molecular and chemical physics, condensed matter physics, and theoretical chemistry. We will provide examples on these three strategies, limiting our study to lightinduced ultrafast phenomena in isolated molecular systems, and employing the formalism of the exact factorization of the time-dependent electron–nuclear wavefunction [23,24,25]. Using this theoretical framework, particular attention is devoted to present the procedures yielding simplified equations of motion, i.e., point (ii). The exact factorization naturally lends itself for such a quantum-classical scheme because the original problem, i.e., the molecular time-dependent Schrodinger equation, is decomposed into a (single) electronic and nuclear part without invoking any approximations.
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