Related papers: HORTENSIA, a program package for the simulation of…
We examine time-resolved X-ray diffraction from molecules in the gas phase which undergo nonadiabatic avoided-crossing dynamics involving strongly coupled electrons and nuclei. Several contributions to the signal are identified,…
By performing an ensemble of molecular dynamics simulations, the model-dependent ionisation state is computed for strongly interacting systems self-consistently. This is accomplished through a free energy minimisation framework based on the…
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…
Mixed quantum-classical mechanics descriptions are critical to modeling coupled electron-nuclear dynamics, i.e. non-adiabatic molecular dynamics, relevant to photochemical and photophysical processes. We argue that, for polyatomic…
A number of non-Markovian stochastic Schr\"odinger equations, ranging from the numerically exact hierarchical form towards a series of perturbative expressions sequentially presented in an ascending degrees of approximations are revisited…
Using a generalized energy-conserving transition probability, it is shown how nonadiabatic calculations, within the Wigner-Heisenberg representation of quantum mechanics, can be reliably extended to far longer times than those allowed by a…
We propose a simple quantum algorithm for simulating highly oscillatory quantum dynamics, which does not require complicated quantum control logic for handling time-ordering operators. To our knowledge, this is the first quantum algorithm…
We prove that for a combined system of classical and quantum particles, it is possible to write a dynamics for the classical particles that incorporates in a natural way the Boltzmann equilibrium population for the quantum subsystem. In…
A first principles quantum formalism to describe the non-adiabatic dynamics of electrons and nuclei based on a second quantization representation (SQR) of the electronic motion combined with the usual representation of the nuclear…
We present the molecular hyperdynamics algorithm and its implementation to the nonorthogonal tight-binding model NTBM and the corresponding software. Due to its multiscale structure, the proposed approach provides the long time scale…
Direct dynamics methods using Gaussian wavepackets have to rely only on local properties, such as gradients and hessians at the center of the wavepacket, so as to be compatible with the usual quantum chemistry methods. Matrix elements of…
In adiabatic quantum computing the aim is to track an eigenstate as the Hamiltonian changes. In the usual setup this is achieved using the natural time-dependent Hamiltonian evolution of the system and the main technical tool is the…
We develop a computational method to learn a molecular Hamiltonian matrix from matrix-valued time series of the electron density. As we demonstrate for three small molecules, the resulting Hamiltonians can be used for electron density…
The recent improvement in experimental capabilities for interrogating and controlling molecular systems with ultrafast coherent light sources calls for the development of theoretical approaches that can accurately and efficiently treat…
Streaking of photoelectrons has long been used for the temporal characterization of attosecond extreme ultraviolet pulses. When the time-resolved photoelectrons originate from a coherent superposition of electronic states, they carry an…
The leading nonadiabatic corrections to rovibrational levels of a diatomic molecule are expressed in terms of three functions of internuclear distance: corrections to the adiabatic potential, the effective nuclear mass, and the effective…
Dissociative chemisorption is a key process in hydrogen-metal surface chemistry, where nonadiabatic effects due to low-lying electron-hole-pair excitations may affect reaction outcomes. Molecular dynamics with electronic friction…
We take up the idea of Nelson's stochastic processes, the aim of which was to deduce Schr\"odinger's equation. We make two major changes here. The first one is to consider deterministic processes which are pseudo-random but which have the…
We outline a method based on successive canonical transformations which yields a product expansion for the evolution operator of a general (possibly non-Hermitian) Hamiltonian. For a class of such Hamiltonians this expansion involves a…
A numerical algorithm based on the probabilistic path integral approach for solving Schroedinger equation has been devised to treat molecular systems without Born-Oppenheimer approximation in the non relativistic limit at zero temperature…