Related papers: Nonadiabatic ring-polymer instanton rate theory: a…
We investigate a simple and robust scheme for choosing the phases of adiabatic electronic states smoothly (as a function of geometry) so as to maximize the performance of ab initio non-adiabatic dynamics methods. Our approach is based upon…
This paper provides the first ab-initio on-the-fly example of using the Quasi-Diabatic (QD) scheme for non-adiabatic simulations with diabatic dynamics approaches. The QD scheme provides a seamless interface between diabatic quantum…
Chemical relaxation phenomena, including photochemistry and electron transfer processes, form a vigorous area of research in which nonadiabatic dynamics plays a fundamental role. Here, we show that for nonadiabatic dynamics with two…
Mean-field Ring Polymer Molecular Dynamics (MF-RPMD) offers a computationally efficient method for the simulation of reaction rates in multi-level systems. Previous work has established that, to model a nonadiabatic state-to-state reaction…
The adiabatic approximation exhibits wide applicability in quantum mechanics, providing a simple approach for nontransitional dynamics in quantum systems governed by slowly varying time-dependent Hamiltonians. However, the standard…
We shall revisit the conventional adiabatic or Markov approximation, showing its intrinsic failure in describing the proper quantum-mechanical evolution of a generic subsystem interacting with its environment. In particular, we shall show…
Non-adiabatic decay rates for a radio-frequency dressed magnetic trap are calculated using Fermi's Golden Rule: that is, we examine the probability for a single atom to make transitions out of the dressed trap and into a continuum in the…
The ring-polymer instanton approach is applied to compute the ground-state tunnelling splitting of four isotopomers of the formic acid dimer using the accurate PES of Qu and Bowman [Phys. Chem. Chem. Phys., 2016, 18, 24835]. As well as…
Diabatization of the molecular Hamiltonian is a standard approach to removing the singularities of nonadiabatic couplings at conical intersections of adiabatic potential energy surfaces. In general, it is impossible to eliminate the…
The thorough treatment of electron-lattice interactions from first principles is one of the main goals in condensed matter physics. While the commonly applied adiabatic Born-Oppenheimer approximation is sufficient for describing many…
We propose a nonadiabatic approach to quantum annealing, in which we repeat quantum annealing in nonadiabatic time scales, and collect the final states of many realizations to find the ground state among them. In this way, we replace the…
Counter-diabatic driving protocols were proposed as a means to do fast changes in the Hamiltonian without exciting transitions. Such driving in principle allows one to realize arbitrarily fast annealing protocols or implement fast…
Instanton rate theory is used to study tunneling events in a wide range of systems including low-temperature chemical reactions. Despite many successful applications, the method has never been obtained from first principles, relying instead…
In this article we propose a novel method to accelerate adiabatic passage in a two-level system with only longitudinal field (detuning) control, while the transverse field is kept constant. The suggested method is a modification of the…
A general quantum adiabatic theorem with and without the time-dependent orthogonalization is proven, which can be applied to understand the origin of activation energies in chemical reactions. Further proofs are also developed for the…
At present, several models for quantum computation have been proposed. Adiabatic quantum computation scheme particularly offers this possibility and is based on a slow enough time evolution of the system, where no transitions take place. In…
We develop and implement an exact conical intersection nonadiabatic wave packet dynamics method that combines the local diabatic representation, Strang splitting for the total molecular propagator, and discrete variable representation with…
We explore the relation between the quantum and semiclassical instanton approximations for the reaction rate constant. From the quantum instanton expression, we analyze the contributions to the rate constant in terms of minimum-action paths…
Mixed-quantum-classical molecular dynamics simulation implies an effective measurement on the electronic states owing to continuously tracking the atomic forces.Based on this insight, we propose a quantum trajectory mean-field approach for…
Periodically driven systems have emerged as a useful technique to engineer the properties of quantum systems, and are in the process of being developed into a standard toolbox for quantum simulation. An outstanding challenge that leaves…