Related papers: Quantum Quality with Classical Cost: Ab Initio Non…
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…
Experiments indicate that collective coupling of molecular ensembles to confined optical modes can modify excited-state dynamics and photochemical reactivity. To describe such cavity-induced effects at atomic resolution, semi-classical…
We present a new approach to carry out non-adiabatic molecular dynamics to study the carrier mobility in an organic monolayer. This approach allows the calculation of a 4802 atom system for 825 fs in about three hours using 51,744 computer…
We explain the concept of superadiabatic approximations and show how in the context of the Born- Oppenheimer approximation they lead to an explicit formula that can be used to predict transitions at avoided crossings. Based on this formula,…
We present a detailed derivation and numerical tests of a new mixed quantum-classical scheme to deal with non-adiabatic processes. The method is presented as the zero-th order approximation to the exact coupled dynamics of electrons and…
In quantum information processing, the development of fast and robust control schemes remains a central challenge. Although quantum adiabatic evolution is inherently robust against control errors, it typically demands long evolution times.…
The research project has been made for mathematical modeling of aerospace system Space-to-Surface for avoid intercepting process by flight objects Surface-to-Air. The research has been completed and created mathematical models which used…
We present an open-source MLatom@XACS software ecosystem for on-the-fly surface hopping nonadiabatic dynamics based on the Landau-Zener-Belyaev-Lebedev (LZBL) algorithm. The dynamics can be performed via Python API with a wide range of…
We present a new partially linearized mapping-based approach for approximating real-time quantum correlation functions in condensed-phase nonadiabatic systems, called spin-PLDM. Within a classical trajectory picture, partially linearized…
Energy transfer during molecular collisions on metal surfaces plays a pivotal role in a host of critical interfacial processes. Despite significant efforts, our understanding of relevant energy transfer mechanisms, even in an…
We generalise the celebrated semiclassical wavepacket approach from the adiabatic to the non-adiabatic regime. A unified description covering both of these regimes is particularly desired for systems with spatially varying band structures…
Collisions of atoms and molecules with metal surfaces create electronic excitations in the metal, leading to nonadiabatic energy dissipation, inelastic scattering, and sticking. Mixed quantum-classical molecular dynamics simulation methods,…
In recent years, plasmonic nanocavities have emerged as powerful tools for controlling and enhancing light-matter interactions at the nanoscale. This study explores the role of plasmonic nanocavities in manipulating nonadiabatic dynamics,…
Here we outline and test an extension of the energy grained master equation (EGME) for treating nonadiabatic (NA) hopping between different potential energy surfaces, which enables us to model the competition between stepwise collisional…
In this paper, we propose a novel Gaussian process-based moving horizon estimation (MHE) framework for unknown nonlinear systems. On the one hand, we approximate the system dynamics by the posterior means of the learned Gaussian processes…
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…
I give an overview of rare event simulation techniques to generate dynamical pathways across high free energy barriers. The methods on which I will concentrate are the reactive flux approach, transition path sampling, (replica-exchange)…
The diagonal Born-Oppenheimer correction (DBOC) stems from the diagonal second derivative coupling term in the adiabatic representation, and it can have an arbitrary large magnitude when a gap between neighbouring Born-Oppenheimer (BO)…
For years, theoretical calculations and scalable computer simulations have complemented ultrafast experiments as they offer the advantage to overcome experimental restrictions and have access to the whole dynamics. This synergy between…
The choice of the electronic representation in on-the-fly quantum dynamics is crucial. The adiabatic representation is appealing since adiabatic states are readily available from quantum chemistry packages. The nuclear wavepackets are then…