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Accurate prediction of molecular vibrational frequencies is important to identify spectroscopic signatures and reaction thermodynamics. In this work, we develop a method to quantify uncertainty associated with density functional theory…

Chemical Physics · Physics 2019-03-13 Holden L. Parks , Alan. J. H. McGaughey , Venkatasubramanian Viswanathan

We demonstrate that a near-dissociation photoassociation resonance can be used to create a deeply bound molecular sample of ultracold NaCs. To probe the resulting vibrational distribution of the sample, we use a new technique that can be…

A reliable and efficient computation of the entire single-particle spectrum of correlated molecules is an outstanding challenge in the field of quantum chemistry, with standard density functional theory approaches often giving an inadequate…

Chemical Physics · Physics 2021-10-08 Oliver J. Backhouse , Alejandro Santana-Bonilla , George H. Booth

In this paper, we investigate periodic vibrations of a group of particles with a dihedral configuration in the plane governed by the Lennard-Jones and Coulomb forces. Using the gradient equivariant degree, we provide a full topological…

Dynamical Systems · Mathematics 2017-02-15 Irina Berezovik , Qingwen Hu , Wieslaw Krawcewicz

A general variational approach for computing the rovibrational dynamics of polyatomic molecules in the presence of external electric fields is presented. Highly accurate, full-dimensional variational calculations provide a basis of…

Chemical Physics · Physics 2018-04-18 Alec Owens , Andrey Yachmenev

The purpose of this article is to present theoretical values for the vibrational and rotational g-factors of several diatomic molecules. The calculations have been carried out at the Multi-Configurational Self-Consistent Field (MCSCF) level…

Chemical Physics · Physics 2025-09-24 Anna Thorn Ekstrøm , Stephan P. A. Sauer

A variational solution to the rovibrational problem in curvilinear vibrational coordinates has been implemented and used to investigate the nuclear motions in several linear triatomic molecules, like HCN, OCS, and HCP. The dependence of the…

Chemical Physics · Physics 2011-11-15 Leonid Shirkov , Tatiana Korona , Robert Moszynski

The main motivation for this work is the exploration of rotational-vibrational states corresponding to electronic excitations in a pre-Born-Oppenheimer quantum theory of molecules. These states are often embedded in the continuum of the…

Chemical Physics · Physics 2018-10-15 Edit Mátyus

The motion of chemical bonds within molecules can be observed in real time, in the form of vibrational wavepackets prepared and interrogated through ultrafast nonlinear spectroscopy. Such nonlinear optical measurements are commonly…

We introduce a hybrid classical-quantum algorithm to compute dynamical correlation functions and excitation spectra in many-body quantum systems, with a focus on molecular systems. The method combines classical preparation of a perturbed…

Quantum Physics · Physics 2025-10-30 Alessandro Santini , Stefano Barison , Filippo Vicentini

Vibrational spectra can be computed without storing full-dimensional vectors by using low-rank sum-of-products (SOP) basis functions. We introduce symmetry constraints in the SOP basis functions to make it possible to separately calculate…

Chemical Physics · Physics 2016-01-05 Arnaud Leclerc , Tucker Carrington

We show how the path-integral formulation of quantum statistical mechanics can be used to construct practical {\em ab initio} techniques for computing the chemical potential of molecules adsorbed on surfaces, with full inclusion of quantum…

Materials Science · Physics 2015-05-18 D. Alfe` , M. J. Gillan

In this paper there is presented method for ab initio calculation of the phonon spectra. The method is based upon a direct calculation of the dynamical matrix via second derivatives of the total energy. The pseudopotential technique in…

Materials Science · Physics 2007-05-23 Marek Hytha , Antonin Simunek

Variational ab-initio methods in quantum chemistry stand out among other methods in providing direct access to the wave function. This allows in principle straightforward extraction of any other observable of interest, besides the energy,…

A full-dimensional \emph{ab initio} potential energy surface of spectroscopic quality is developed for the van-der-Waals complex of a methane molecule and an argon atom. Variational vibrational states are computed on this surface including…

Chemical Physics · Physics 2020-03-18 Gustavo Avila , Dóra Papp , Gábor Czakó , Edit Mátyus

The vibrational properties of two-dimensional phononic crystals are studied with large-scale molecular dynamics simulations and finite element method calculation. The vibrational band structure derived from the molecular dynamics…

Materials Science · Physics 2017-11-28 Ralf Meyer

Some of us have recently reported in Science 321 232 (2008) vibrational cooling of translationally cold Cs_2 molecules into the lowest vibrational level v=0 of the singlet X 1Sigma_g ground electronic state. Starting from a sample of cold…

Multidimensional spectroscopy unveils the interplay of nuclear and electronic dynamics, which characterizes the ultrafast dynamics of various molecular and solid-state systems. In a class of models widely used for the simulation of such…

Quantum Physics · Physics 2023-08-28 Frank Ernesto Quintela Rodriguez , Filippo Troiani

We present a computer program to calculate the quantised rotational and hyperfine energy levels of $^{1}\Sigma $ diatomic molecules in the presence of dc electric, dc magnetic, and off-resonant optical fields. Our program is applicable to…

Computational Physics · Physics 2022-09-28 Jacob A. Blackmore , Philip D. Gregory , Jeremy M. Hutson , Simon L. Cornish

An algorithm and a system of quantum circuits is developed and applied to compute accurately the S matrix for the transitions between vibrational states of H2 for collisions with H. The algorithm was applied to 100 eV laboratory collision…

Quantum Physics · Physics 2023-01-05 Yulun Wang , Predrag S. Krstic