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Within a 2-D scattering model, we investigate the vibrational relaxation of an idealized molecule colliding with a metal surface. Two perturbative nonadiabatic dynamics schemes are compared: $(i)$ electronic friction (EF) and $(ii)$…

Chemical Physics · Physics 2018-01-17 Gaohan Miao , Wenjie Dou , Joseph Eli Subotnik

We investigate detailed balance for a quantum system interacting with thermal radiation within mixed quantum-classical theory. For a two-level system coupled to classical radiation fields, three semiclassical methods are benchmarked: (1)…

Chemical Physics · Physics 2019-07-17 Hsing-Ta Chen , Tao E. Li , Abraham Nitzan , Joseph E. Subotnik

We design a quantum molecular dynamics method for strongly correlated electron metals. The strong electronic correlation effects are treated within a real-space version of the Gutzwiller variational approximation (GA), which is suitable for…

Strongly Correlated Electrons · Physics 2017-07-12 Jean-Pierre Julien , Joel D. Kress , Jian-Xin Zhu

We address the nonadiabatic quantum dynamics of macrosystems with several coupled electronic states, taking into account the possibility of multi-state conical intersections. The general situation of an arbitrary number of states and…

Chemical Physics · Physics 2009-11-13 Etienne Gindensperger , Lorenz S. Cederbaum

Multi-configurational electronic structure theory delivers the most versatile approximations to many-electron wavefunctions, flexible enough to deal with all sorts of transformations, ranging from electronic excitations, to open-shell…

Chemical Physics · Physics 2024-05-07 Kalman Szenes , Maximilian Moerchen , Paul Fischill , Markus Reiher

Molecular adsorbates on metal surfaces exchange energy with substrate phonons and low-lying electron-hole pair excitations. In the limit of weak coupling, electron-hole pair excitations can be seen as exerting frictional forces on…

Materials Science · Physics 2016-09-28 Reinhard J. Maurer , Mikhail Askerka , Victor S. Batista , John C. Tully

Controlling polymorphism in molecular crystals is crucial in the pharmaceutical, dye, and pesticide industries. However, its theoretical description is extremely challenging, due to the associated long timescales ($ > 1 \, \mu s$). We…

Chemical Physics · Physics 2023-02-09 Oren Elishav , Roy Podgaetsky , Olga Meikler , Barak Hirshberg

Understanding the electron dynamics and transport in metallic and semiconductor nanostructures -- such as metallic nanoparticles, thin films, quantum wells and quantum dots -- represents a considerable challenge for today's condensed matter…

Strongly Correlated Electrons · Physics 2008-10-20 G. Manfredi , P. -A. Hervieux , Y. Yin , N. Crouseilles

Due to the exponential growth of the state space of coupled quantum systems it is not possible, in general, to numerically store the state of a very large number of quantum systems within a classical computer. We demonstrate a method for…

Quantum Physics · Physics 2017-02-07 J. J. Bowen , V. M. Dwyer , I. W. Phillips , M. J. Everitt

Quantum computers have the potential to simulate chemical systems beyond the capability of classical computers. Recent developments in hybrid quantum-classical approaches enable the determinations of the ground or low energy states of…

Quantum Physics · Physics 2021-12-06 Chee-Kong Lee , Jonathan Wei Zhong Lau , Liang Shi , Leong Chuan Kwek

Generating a data set that is representative of the accessible configuration space of a molecular system is crucial for the robustness of machine learned interatomic potentials (MLIP). However, the complexity of molecular systems,…

Machine Learning · Computer Science 2025-01-28 Aik Rui Tan , Johannes C. B. Dietschreit , Rafael Gomez-Bombarelli

The dynamics of an electronic two-level system coupled to an electromagnetic field are simulated explicitly for one and three dimensional systems through semiclassical propagation of the Maxwell-Liouville equations. We consider three…

In this paper we propose an ab initio method to solve quantum many-body problems of molecular dynamics where both the electronic and the nuclear degrees are represented by ensembles of trajectories and guiding waves in physical space. Both…

Atomic Physics · Physics 2025-01-28 Ivan P. Christov

Advances in manufacturing and characterization of complex molecular systems have created a need for new methods for design at molecular length scales. Emerging approaches are increasingly relying on the use of Artificial Intelligence (AI),…

Soft Condensed Matter · Physics 2022-08-17 Dan Mendels , Fabian Byléhn , Timothy W. Sirk , Juan J. de Pablo

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…

Chemical Physics · Physics 2015-06-22 Federica Agostini , Ali Abedi , E. K. U. Gross

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…

Chemical Physics · Physics 2024-08-20 Jonathan R. Mannouch , Aaron Kelly

Understanding kinetics and thermodynamics profile of biomolecules is necessary to understand their functional roles which has a major impact in mechanism driven drug discovery. Molecular dynamics simulation has been routinely used to…

Biomolecules · Quantitative Biology 2021-12-07 Soumendranath Bhakat

We discuss nuclear dynamics at molecule-metal interfaces including non-equilibrium molecular junctions. Starting from the many-body states (pseudoparticle) formulation of the molecule-metal system in the molecular vibronic basis, we…

Mesoscale and Nanoscale Physics · Physics 2015-11-30 Michael Galperin , Abraham Nitzan

Exposing a molecule to intense light pulses may bring this molecule to a nonstationary quantum state, thus launching correlated dynamics of electronic and nuclear subsystems. Although much had been achieved in the understanding of…

Chemical Physics · Physics 2024-04-11 Nikolay V. Golubev , Jiří Vaníček

An approach to non-adiabatic dynamics of atoms in molecular and condensed matter systems under general non-equilibrium conditions is proposed. In this method interaction between nuclei and electrons is considered explicitly up to the second…

Materials Science · Physics 2018-08-01 L. Kantorovich