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Experimental observations of multi-quantum relaxation of highly vibrationally excited NO scattering from Au(111) are a benchmark for the breakdown of Born-Oppenheimer approximation in molecule-surface systems. This remarkable vibrational…

Chemical Physics · Physics 2019-10-23 Rongrong Yin , Yaolong Zhang , Bin Jiang

We present a perturbation approach rooted in time-dependent density-functional theory to calculate electron hole (eh)-pair excitation spectra during the non-adiabatic vibrational damping of adsorbates on metal surfaces. Our analysis for the…

Chemical Physics · Physics 2017-11-22 Simon P. Rittmeyer , Jörg Meyer , Karsten Reuter

We introduce a general technique to compute finite temperature electronic properties by a novel covariant formulation of the electronic partition function. By using a rigorous variational upper bound to the free energy we are led to the…

Strongly Correlated Electrons · Physics 2013-06-19 Guglielmo Mazzola , Andrea Zen , Sandro Sorella

We investigate the accuracy and efficiency of the semiclassical Frozen Gaussian method in describing electron dynamics in real time. Model systems of two soft-Coulomb-interacting electrons are used to study correlated dynamics under…

Chemical Physics · Physics 2015-05-30 Peter Elliott , Neepa T. Maitra

The atomistic resolution recently achieved by ultrafast spectroscopies demands corresponding theoretical advances. Real-time time-dependent density-functional theory (RT-TDDFT) with Ehrenfest dynamics offers an optimal trade-off between…

Materials Science · Physics 2022-10-19 Jannis Krumland , Matheus Jacobs , Caterina Cocchi

Ultrafast laser excitation can trigger multiplex coherent dynamics in molecules. Here, we report attosecond transient absorption experiments addressing simultaneous probing of electronic and vibrational dynamics in a prototype molecule,…

Potential energy surfaces of electron dynamics (ePES) are constructed from a model of localized electron wave packets (eWP) with non-orthogonal valence-bond (VB) spin coupling and applied to quantum dynamics simulations of high harmonic…

Chemical Physics · Physics 2023-03-28 Koji Ando

Understanding protein flexibility and its dynamic interactions with other molecules is essential for studying protein function. Although cryogenic electron microscopy(cryo-EM) provides an opportunity to observe macromolecular dynamics…

Computer Vision and Pattern Recognition · Computer Science 2026-02-03 Bintao He , Yiran Cheng , Hongjia Li , Xiang Gao , Xin Gao , Fa Zhang , Renmin Han

Extended Lagrangian Born-Oppenheimer molecular dynamics [Niklasson, Phys. Rev. Lett. 100 123004 (2008)] has been generalized to the propagation of the electronic wavefunctions. The technique allows highly efficient first principles…

Materials Science · Physics 2011-10-07 Peter Steneteg , Igor A. Abrikosov , Valery Weber , Anders M. N. Niklasson

Parameter estimation and trajectory reconstruction for data-driven dynamical systems governed by ordinary differential equations (ODEs) are essential tasks in fields such as biology, engineering, and physics. These inverse problems --…

Machine Learning · Statistics 2025-01-27 Jianhong Chen , Shihao Yang

Based on optical medium analogy, we establish a formalism to describe the interaction between an electromagnetic (EM) system with gravitational waves (GWs) background. After a full discussion on the classical treatment of the EM-GW…

General Relativity and Quantum Cosmology · Physics 2023-11-16 F. Shojaei Arani , M. Bagheri Harouni , B. Lamine , A. Blanchard

The Born--Oppenheimer approximation is the standard tool for the study of molecular systems. It is founded on the observation that the energy scale of the electron dynamics in a molecule is larger than that of the nuclei. A very similar…

High Energy Physics - Phenomenology · Physics 2018-01-31 Nora Brambilla , Gastão Krein , Jaume Tarrús Castellà , Antonio Vairo

We formulate a time-dependent density functional theory for the coupled dynamics of electrons and nuclei that goes beyond the Born-Oppenheimer (BO) approximation. We prove that the time-dependent marginal nuclear probability density…

Chemical Physics · Physics 2025-11-14 Chen Li , Ryan Requist , E. K. U. Gross

We study a general problem of the translational/rotational/vibrational/electronic dynamics of a diatomic molecule exposed to an interaction with an arbitrary external electromagnetic field. The theory developed in this paper is relevant to…

Quantum Physics · Physics 2016-09-28 Milan Sindelka , Nimrod Moiseyev

It is well known that Electroencephalography(EEG) and the respective evoked potentials have deep implications corresponding to specific cognitive tasks and in the diagnosis of several diseases such as epilepsy and schizophrenia. Some recent…

Neurons and Cognition · Quantitative Biology 2007-05-23 I. Mitra

We develop a phase-space electronic structure theory of molecules in magnetic fields. For a system of electrons in a magnetic field with vector potential $\bf{A}(\hat{\bf{r}})$, the usual Born-Oppenheimer Hamiltonian is the sum of the…

Chemical Physics · Physics 2024-11-25 Mansi Bhati , Zhen Tao , Xuezhi Bian , Jonathan Rawlinson , Robert Littlejohn , Joseph E. Subotnik

Controlling the wave function of free electrons is important to improve the spatial resolution of electron microscopes, the efficiency of electron interaction with sample modes of interest, and our ability to probe ultrafast materials…

Quantum Physics · Physics 2021-01-27 Valerio Di Giulio , F. Javier García de Abajo

We develop and experimentally demonstrate a methodology for a full molecular frame quantum tomography (MFQT) of dynamical polyatomic systems. We exemplify this approach through the complete characterization of an electronically…

A relativistic quantum mechanical model to describe the quantum FEL dynamics has been developed. Neglecting the spin of electrons in the impacting beam, this model is based on the Klein-Gordon equation coupled to the Poisson equation for…

Plasma Physics · Physics 2023-10-20 Stephan I. Tzenov , Zhichu Chen

Analytic consideration of the Bohr-Oppenheimer (BO) approximation for diatomic molecules is proposed: accurate analytic interpolation for potential curve consistent with its rovibrational spectra is found. It is shown that in the…

Atomic Physics · Physics 2019-08-07 Horacio Olivares-Pilón , Alexander V. Turbiner