Related papers: Coupled Wavepackets for Non-Adiabatic Molecular Dy…

Many processes in chemistry and physics take place on timescales that cannot be explored using standard molecular dynamics simulations. This renders the use of enhanced sampling mandatory. Here we introduce an enhanced sampling method that…

The dynamics of an electronic system interacting with an electromagnetic field is investigated within mixed quantum-classical theory. Beyond the classical path approximation (where we ignore all feedback from the electronic system on the…

We introduce a simple ansatz for the wavefunction of a many-body system based on coupled forward and backward-propagating semiclassical trajectories. This method is primarily aimed at, but not limited to, treating nonequilibrium dynamics in…

We demonstrate that ultrashort pulses carry the possibility for a new regime of light-matter interaction with nonadiabatic electron processes sensitive to the envelope-derivative of the light pulse. A standard single pulse with its two…

Nonadiabatic molecular dynamics offers a powerful tool for studying the photochemistry of molecular systems. Key to any nonadiabatic molecular dynamics simulation is the definition of its initial conditions, ideally representing the initial…

We introduce a computational framework for simulating non-adiabatic vibronic dynamics on circuit quantum electrodynamics (cQED) platforms. Our approach leverages hybrid oscillator-qubit quantum hardware with mid-circuit measurements and…

We introduce a novel methodology for simulating the excited-state dynamics of extensive molecular aggregates in the framework of the long-range corrected time-dependent density-functional tight-binding fragment molecular orbital method…

One-dimensional integrable and quasi-integrable systems display, on macroscopic scales, a universal form of transport known as Generalized Hydrodynamics (GHD). In its standard Euler-scale formulation, GHD mirrors the equations of a…

In mixed quantum-classical simulations of molecule-metal surface interactions, the discretization of the metallic electronic continuum typically results in a closed-system representation that fails to capture the open-system nature of the…

This report presents a new approach for treating the coupling of electrons and nuclei in quantum mechanical calculations for molecules and condensed matter. It includes the standard "Born-Oppenheimer approximation" as a special case but…

We study a partially ionized hydrogen plasma by means of quantum molecular dynamics, which is based on wave packets. We introduce a new model which distinguishes between free and bound electrons. The free electrons are modelled as Gaussian…

Quantum simulations of photoexcited low-dimensional systems are pivotal for understanding how to functionalize and integrate novel two-dimensional (2D) materials in next-generation optoelectronic devices. First principles predictions are…

We describe a new approach based on semiclassical molecular dynamics that allows to simulate infrared absorption or emission spectra of molecular systems with inclusion of anharmonic intensities. This is achieved from semiclassical power…

Understanding complex quantum dynamics in realistic materials requires insight into the underlying correlations dominating the interactions between the participating particles. Due to the wealth of information involved in these processes,…

We generalize our earlier work on the symplectic/Hamiltonian formulation of the dynamics of the Gaussian wave packet to non-Gaussian semiclassical wave packets. We find the symplectic forms and asymptotic expansions of the Hamiltonians…

In the cuprates, the opening of a d-wave superconducting (SC) gap is accompanied by a redistribution of spectral weight at energies two orders of magnitude larger than this gap. This indicates the importance to the pairing mechanism of…

We present a method to sample reactive pathways via biased molecular dynamics simulations in trajectory space. We show that the use of enhanced sampling techniques enables unconstrained exploration of multiple reaction routes. Time…

Non-adiabatic molecular dynamics simulations are used to analyze the role of different solvent degrees of freedom in the non-radiative relaxation of the first excited state of the hydrated electron. The relaxation occurs through a…

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…

Ab initio methods for electronic structure of molecules have reached a satisfactory accuracy for calculation of static properties, but remain too expensive for quantum dynamical calculations. We propose an efficient semiclassical method for…