Related papers: Robust non-adiabatic molecular dynamics for metals…
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…
A non-adiabatic nuclear wavepacket dynamics simulation of the H$_2$O$^+$ de-excitation process is performed based on electronic structure calculations using the variational quantum eigensolver. The adiabatic potential energy surfaces and…
We consider an implementation of the adiabatic spin dynamics approach in a tight-binding description of the electronic structure. The adiabatic approximation for spin-degrees of freedom assumes that the faster electronic degrees of freedom…
The quasi-neutral hybrid model with kinetic ions and fluid electrons is a promising approach for bridging the inherent multi-scale nature of many problems in space and laboratory plasmas. Here, a novel, implicit, particle-in-cell based…
On-the-fly quantum nonadiabatic dynamics for large systems greatly benefits from the adiabatic representation readily available from the electronic structure programs. However, frequently occurring in this representation conical…
We develop a density matrix formalism to describe coupled electron-nuclear dynamics. To this end we introduce an effective Hamiltonian formalism that describes electronic transitions and small (quantum) nuclear fluctuations along a…
Based on quantum reactive-scattering theory, we propose a method for studying the electronic nonadiabaticity in collision processes involving electron-ion rearrangements. We investigate the state-to-state transition probability for…
A novel mixed quantum-classical approach to simulating nonadiabatic dynamics of molecules at metal surfaces is presented. The method combines the numerically exact hierarchical equations of motion approach for the quantum electronic degrees…
This work identifies geometric effects on dynamics due to nonadiabatic couplings in Born Oppenheimer systems and provides a systematic method for deriving corrections to mixed quantum-classical methods. Specifically, an exact path integral…
We introduce EChemDID, a model to describe electrochemical driving force in reactive molecular dynamics simulations. The method describes the equilibration of external electrochemical potentials (voltage) within metallic structures and…
A first-principles coupled electron-nuclear dynamics simulation based on real-time, time-dependent density functional theory and Ehrenfest dynamics quantitatively repro-duces bimodal translational energy loss and angular distributions…
The exact nuclear time-dependent potential energy surface arises from the exact decomposition of electronic and nuclear motion, recently presented in [A. Abedi, N. T. Maitra, and E. K. U. Gross, Phys. Rev. Lett. 105, 123002 (2010)]. Such…
Incorporating nuclear quantum effects into nonadiabatic dynamics remains a significant challenge. Herein we introduce new nonadiabatic dynamics approaches based on the recently developed constrained nuclear-electronic orbital (CNEO) theory.…
In radiation damage cascade displacement spikes ions and electrons can reach very high temperatures and be out of thermal equilibrium. Correct modelling of cascades with molecular dynamics should allow for the non-adiabatic exchange of…
A novel method of coherent manipulation of the electron tunneling in quantum-dots is proposed, which utilizes the quantum interference in nonadiabatic double-crossing of the discrete energy levels. In this method, we need only a smoothly…
We propose mixed quantum-classical equations of motion that unify electronic coherence and phase evolution simultaneously within the exact factorization framework. Our derivation shows that incorporating the second-order electron-nuclear…
Most microscopic descriptions of structural dynamics assume the Born-Oppenheimer separation, where electrons adjust adiabatically to ionic motion. When this separation breaks down, electronic and lattice degrees of freedom can evolve on…
We propose a novel method to describe realistically ionization processes with absorbing boundary conditions in basis expansion within the formalism of the so-called Non-Adiabatic Quantum Molecular Dynamics. This theory couples…
Quantum simulation has begun to penetrate the field of quantum chemistry in hopes of efficiently calculating ground state energies and approximating real-time evolution. With modern research highlighting nonadiabatic dynamics, tunably…
We present in detail the recently derived ab-initio molecular dynamics (AIMD) formalism [Phys. Rev. Lett. 101 096403 (2008)], which due to its numerical properties, is ideal for simulating the dynamics of systems containing thousands of…