Related papers: Mixed quantum-classical dynamics using collective …
We present a novel learning framework that consistently embeds underlying physics while bypassing a significant drawback of most modern, data-driven coarse-grained approaches in the context of molecular dynamics (MD), i.e., the availability…
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…
While the treatment of chemically relevant systems containing hundreds or even thousands of electrons remains beyond the reach of quantum devices, the development of quantum-classical hybrid algorithms to resolve electronic correlation…
A theory of electronic friction is developed using the exact factorization of the electron-nuclear wavefunction. No assumption is made regarding the electronic bath, which can be made of independent or interacting electrons, and the nuclei…
The mapping approach addresses the mismatch between the continuous nuclear phase space and discrete electronic states by creating an extended, fully continuous phase space using a set of harmonic oscillators to encode the populations and…
We develop a unified quantum geometric framework to understand reactive quantum dynamics. The critical roles of the quantum geometry of adiabatic electronic states in both adiabatic and non-adiabatic quantum dynamics are unveiled. A…
A recent proposal for mixed dynamics of classical and quantum ensembles is shown, in contrast to other proposals, to satisfy the minimal algebraic requirements proposed by Salcedo for any consistent formulation of such dynamics. Generalised…
We analyze a mixed quantum-classical algorithm recently derived from the exact factorization equations [Min, Agostini, Gross, PRL {\bf 115}, 073001 (2015)] to show the role of the different terms in the algorithm in bringing about…
We propose a trajectory-based method for simulating nonadiabatic dynamics in molecular systems with two coupled electronic states. Employing a quantum-mechanically exact mapping of the two-level problem to a spin-1/2 coherent state, we…
Adiabatic mixed quantum/classical molecular dynamics simulations were used to generate snapshots of the hydrated electron (e-) in liquid water at 300 K. Water cluster anions that include two complete solvation shells centered on the e- were…
An accurate description of strong correlation is quintessential for the exploration of emerging chemical phenomena. While near-term variational quantum algorithms provide a theoretically scalable framework for quantum chemical problems, the…
Electronic friction-Langevin dynamics (EF-LD) provides an efficient framework for capturing nonadiabatic effects at solid surfaces, with particular relevance to electrochemistry and molecular electronics. In this work, we investigate…
Accurate simulation of the non-adiabatic dynamics of molecules in excited electronic states is key to understanding molecular photo-physical processes. Here we present a novel method, based on a semiclassical approximation, that is as…
The quantum master equation (QME), used to describe the Markov process of interaction between atoms and field, has a number of significant drawbacks. It is extremely memory intensive, and also inapplicable to the case of long-term memory in…
We develop a classical mapping approach suitable to describe vibrationally coupled charge transport in molecular junctions based on the Cartesian mapping for many-electron systems [J. Chem. Phys. 137, 154107 (2012)]. To properly describe…
Simulating molecules using the Variational Quantum Eigensolver method is one of the promising applications for NISQ-era quantum computers. Designing an efficient ansatz to represent the electronic wave function is crucial in such…
We introduce a new method to accurately and efficiently estimate the effective dynamics of collective variables in molecular simulations. Such reduced dynamics play an essential role in the study of a broad class of processes, ranging from…
We propose the powerful integration of the Hybrid Monte Carlo (hybridMC) algorithm and Well-Tempered Metadynamics. This new algorithm, hybridMC-MetaD, enhances the flexibility and applicability of metadynamics by allowing for the…
In molecular dynamics (MD) simulations, transitions between states are often rare events due to energy barriers that exceed the thermal temperature. Because of their infrequent occurrence and the huge number of degrees of freedom in…
We derive the fundamental equations of an optimal control theory for systems containing both quantum electrons and classical ions. The system is modeled with Ehrenfest dynamics, a non-adiabatic variant of molecular dynamics. The general…