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We demonstrate that, rather than resorting to high-cost dynamic correlation methods, qualitative failures in excited-state potential energy surface predictions can often be remedied at no additional cost by ensuring that optimal molecular…

Chemical Physics · Physics 2020-06-18 Lan Nguyen Tran , Eric Neuscamman

We show that standard Ehrenfest dynamics does not conserve linear and angular momentum when using a basis of truncated adiabatic states. However, we also show that previously proposed effective Ehrenfest equations of…

Chemical Physics · Physics 2023-12-15 Zhen Tao , Xuezhi Bian , Yanze Wu , Jonathan Rawlinson , Robert G. Littlejohn , Joseph E. Subotnik

The recent development of multidimensional ultrafast spectroscopy techniques calls for the introduction of computational schemes that allow for the simulation of such experiments and the interpretation of the corresponding results from a…

Mesoscale and Nanoscale Physics · Physics 2023-10-30 Jannis Krumland , Michele Guerrini , Antonietta De Sio , Christoph Lienau , Caterina Cocchi

We present a model intended for rapid sampling of ground and excited state potential energy surfaces for first-row transition metal active sites. The method is computationally inexpensive and is suited for dynamics simulations where (1)…

Chemical Physics · Physics 2009-11-10 M. X. LaBute , R. G. Endres , D. L. Cox

Ultrafast multistage electron transfer (ET) in molecular systems with multiple redox centers is fundamental to photochemical energy conversion, including processes in natural photosynthesis, molecular optoelectronics, and organic…

Chemical Physics · Physics 2025-07-29 Serguei Feskov , Anatoly Ivanov

Adiabatic optimal control schemes are essential for advancing the practical implementation of quantum technologies. However, the vast array of possible adiabatic protocols, combined with their dependence on the particular quantum system and…

The calculation of a segment of eigenvalues and their corresponding eigenvectors of a Hermitian matrix or matrix pencil has many applications. A new density-matrix-based algorithm has been proposed recently and a software package FEAST has…

Numerical Analysis · Mathematics 2014-01-21 Ping Tak Peter Tang , Eric Polizzi

We present a self-contained theoretical and computational framework for dynamics following photoexcitation in quantum dots near planar interfaces. A microscopic Hamiltonian parameterized by first principles calculations is merged with a…

Mesoscale and Nanoscale Physics · Physics 2015-06-15 Kuljit S. Virk , Mark S. Hybertsen , David R. Reichman

Nonadiabatic coupling between electrons and molecular motion at metal surfaces leads to energy dissipation and dynamical steering effects during chemical surface dynamics. We present a theoretical approach to the scattering of molecules…

Real-time time-dependent density functional theory, in conjunction with the Ehrenfest molecular dynamics scheme, is becoming a popular methodology to investigate ultrafast phenomena on the nanoscale. Thanks to recent developments, it is…

Materials Science · Physics 2020-08-18 Jannis Krumland , Ana M. Valencia , Stefano Pittalis , Carlo A. Rozzi , Caterina Cocchi

An efficient hybrid numerical method for multiple scattering calculations is proposed. We use the well established doubling--adding method to find the reflection function of the lowermost homogeneous slab comprising the atmosphere of our…

Instrumentation and Methods for Astrophysics · Physics 2016-11-04 Kiyoshi Kawabata

A combined nonequilibrium Green functions-Ehrenfest dynamics approach is developed that allows for a time-dependent study of the energy loss of a charged particle penetrating a strongly correlated system at zero and finite temperature.…

Strongly Correlated Electrons · Physics 2016-12-21 Karsten Balzer , Niclas Schlünzen , Michael Bonitz

We carried out extensive studies to examine the performance of the fewest-switches surface hopping method in the description of the ultrafast intersystem crossing dynamic of various singlet-triplet (S-T) models by comparison with the…

Chemical Physics · Physics 2019-05-22 Jiawei Peng , Yu Xie , Deping Hu , Zhenggang Lan

We deal with a continuous-time Ehrenfest model defined over an extended star graph, defined as a lattice formed by the integers of $d$ semiaxis joined at the origin. The dynamics on each ray are regulated by linear transition rates, whereas…

Probability · Mathematics 2022-05-18 Antonio Di Crescenzo , Barbara Martinucci , Serena Spina

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…

Chemical Physics · Physics 2018-05-01 Shunsuke A. Sato , Aaron Kelly , Angel Rubio

Ehrenfest and Car-Parrinello molecular dynamics are computational alternatives to approximate Born-Oppenheimer molecular dynamics without solving the electron eigenvalue problem at each time-step. A non-trivial issue is to choose the…

Chemical Physics · Physics 2014-09-18 Ashraful Kadir , Mattias Sandberg , Anders Szepessy

Mean field theory is applied to nonequilibrium thermal energy transport in a model molecular junction. An approximation to the total time-dependent heat current in the junction is constructed using an ensemble of Ehrenfest trajectories, and…

Chemical Physics · Physics 2019-06-26 Aaron Kelly

Viscoelasticity and rate-dependent adhesion of soft matter lead to difficulties in modeling the 'relatively simple' problem of a rigid sphere in contact with a viscoelastic half-space. For this reason, approximations in describing surface…

Soft Condensed Matter · Physics 2021-12-08 Luciano Afferrante , Guido Violano

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

We derive Ehrenfest like equations for the coupled Gross Pitaevskii equations (CGPE) which describe the dynamics of the binary Bose-Einstein condensate (BBEC) both in the free particle regime and in the regime where condensate is well…

Quantum Gases · Physics 2017-12-06 Sukla Pal , Jayanta K. Bhattacharjee
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