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We introduce a novel computational framework for excited-states molecular quantum dynamics simulations driven by quantum computing-based electronic-structure calculations. This framework leverages the fewest-switches surface-hopping method…
Simulating the irreversible quantum dynamics of exciton and electron transfer problems poses a nontrivial challenge. Because the irreversibility of the system dynamics is a result of quantum thermal activation and dissipation caused by the…
The role of quantum coherence loss in mixed quantum-classical dynamical systems is explored in the context of the theory of quantum decoherence introduced recently by Bittner and Rossky. (J. Chem. Phys. {\bf 103}, 8130 (1995)). This theory,…
We present an approach for carrying out non-adiabatic molecular dynamics simulations of systems in which non-adiabatic transitions arise from the coupling between the classical atomic motions and a quasi-continuum of electronic quantum…
We present a novel quantum-classical approach to non-adiabatic dynamics, deduced from the coupled electronic and nuclear equations in the framework of the exact factorization of the electron-nuclear wave function. The method is based on the…
The combined quantum electron-nuclear dynamics is often associated with the Born-Huang expansion of the molecular wave function and the appearance of nonadiabatic effects as a perturbation. On the other hand, native multicomponent…
Several methods in nonadiabatic molecular dynamics are based on Madelung's hydrodynamic description of nuclear motion, while the electronic component is treated as a finite-dimensional quantum system. In this context, the quantum potential…
The theoretical investigation of non-adiabatic processes is hampered by the complexity of the coupled electron-nuclear dynamics beyond the Born-Oppenheimer approximation. Classically, the simulation of such reactions is limited by the…
Many theoretical calculations of subtle coherent effects in quantum mechanics do not carefully consider the interface between their calculations and experiment. Calculations for gedanken experiments using initial states not satisfied in…
In many important cases, the rate of excitation of a system embedded in an environment is significantly smaller than the internal system relaxation rates. An important example is that of light-induced processes under natural conditions, in…
We propose an excited-state molecular dynamics simulation method based on variational quantum algorithms at a computational cost comparable to that of ground-state simulations. We utilize the feature that excited states can be obtained as…
Exploiting the relative entropy of coherence, we isolate the coherent contribution in the energetics of a driven non-equilibrium quantum system. We prove that a division of the irreversible work can be made into a coherent and incoherent…
Quantum computers have the potential to simulate chemical systems beyond the capability of classical computers. Recent developments in hybrid quantum-classical approaches enable the determinations of the ground or low energy states of…
We study spontaneous quantum coherence in an out of equilibrium system, coupled to multiple baths describing pumping and decay. For a range of parameters describing coupling to, and occupation of the baths, a stable steady-state condensed…
We present a framework for simulating relaxation dynamics through a conical intersection of an open quantum system that combines methods to approximate the motion of degrees of freedom with disparate time and energy scales. In the vicinity…
The conditions under which an open quantum mechanical system may be described by mixed quantum-classical dynamics are investigated. Decoherence is studied using influence functional methods in a model composite quantum system comprising two…
We study a quantum mechanical toy model that mimics some features of a quenched phase transition. Both by virtue of a time-dependent Hamiltonian or by changing the temperature of the bath we are able to show that even after classicalization…
We derive an exact solution of an explicitly time-dependent multichannel model of quantum mechanical nonadiabatic transitions. In the limit N >>1, where N is the number of states, we find that the survival probability of the initially…
The use of quantum computing to solve a problem in quantum mechanics is illustrated, step by step, by calculating energies and transition amplitudes in a nonrelativistic quark model. The quantum computations feature the use of variational…
Understanding the reactivity and spectroscopy of aqueous solutions at the atomistic level is crucial for the elucidation and design of chemical processes. However, the simulation of these systems requires addressing the formidable…