Related papers: Semiclassical Nonadiabatic Molecular Dynamics Usin…
Nonadiabatic ab initio molecular dynamics (MD) including spin-orbit coupling (SOC) and laser fields is investigated as a general tool for studies of excited-state processes. Up to now, SOCs are not included in standard ab initio MD…
We present a new methodology for the linear-response time-dependent density functional theory (LR-TDDFT) calculation of the dynamic density response function of warm dense matter in an adiabatic approximation that can be used with any…
We develop a trajectory-based approach for excited-state molecular dynamics simulations of systems subject to an external periodic drive. We combine the exact-factorization formalism, allowing to treat electron-nuclear systems in…
We present the theory and implementation of a fully variational wave function -- density functional theory (DFT) hybrid model, which is applicable to many cases of strong correlation. We denote this model the multiconfigurational…
We investigate the nonequilibrium dynamics of a laser-pumped two-dimensional spinless Holstein model within a semiclassical framework, focusing on the melting and recovery of long-range charge-density-wave order. Accurately describing this…
In this comparative study we benchmark a recently developed non-adiabatic exchange-correlation potential within time-dependent density functional theory (TDDFT) (Phys.\ Rev.\ Lett.\ {\bf 120}, 157701 (2018)) by (a) validating the transient…
Recently proposed non-adiabatic ring polymer molecular dynamics (NRPMD) approach has shown to provide accurate quantum dynamics by incorporating explicit electronic state descriptions and nuclear quantizations. Here, we present a rigorous…
The Landau--Zener (LZ) type classical-trajectory surface-hopping algorithm is applied to the nonadiabatic nuclear dynamics of the ammonia cation after photoionization of the ground-state neutral molecule to the excited states of the cation.…
Simulating the coupled electronic and nuclear response of a molecule to light excitation requires the application of nonadiabatic molecular dynamics. However, when faced with a specific photophysical or photochemical problem, selecting the…
Nonadiabatic effects in chemical reaction at metal surfaces, due to excitation of electron-hole pairs, stand at the frontier of the studies of gas-surface reaction dynamics. However, the first principles description of electronic excitation…
Nonadiabatic corrections in molecules composed of a few atoms are considered. It is demonstrated that a systematic perturbative expansion around the adiabatic solution is possible, with the expansion parameter being the electron-nucleus…
We formulate equations of time-dependent density functional theory (TDDFT) in the co-moving Lagrangian reference frame. The main advantage of the Lagrangian description of many-body dynamics is that in the co-moving frame the current…
At present there are two vastly different ab initio approaches to the description of the the many-body dynamics: the Density Functional Theory (DFT) and the functional integral (path integral) approaches. On one hand, if implemented…
In principle, we should not need the time-dependent extension of density-functional theory (TDDFT) for excitations, and in particular not for Molecular Dynamics (MD) studies: the theorem by Hohenberg and Kohn teaches us that for any…
Non-adiabatic molecular dynamics (NAMD) simulations have become an indispensable tool for investigating excited-state dynamics in solids. In this work, we propose a general framework, N$^2$AMD which employs an E(3)-equivariant deep neural…
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…
Real-time simulations of laser-driven electron dynamics contain information about molecular optical properties through all orders in response theory. These properties can be extracted by assuming convergence of the power series expansion of…
We present a systematic, quasi-automated methodology for generating electronic models in the framework of second-principles density functional theory (SPDFT). This approach enables the construction of accurate and computationally efficient…
We propose a method to compute free-energy differences from nonadiabatic alchemical transformations using flow-based generative models. The method, nonadiabatic force matching, hinges on estimating the dissipation along an alchemical…
Due to efficient scaling with electron number N, density functional theory (DFT) is widely used for studies of large molecules and solids. Restriction of an exact mean-field theory to local potential functions has recently been questioned.…