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The detection of vibrational excitations of individual molecules on surfaces by scanning tunneling spectroscopy does not obey strict selection rules but rather propensity rules. The experimental verification of these is challenging because…

The potential energy surface (PES) is crucial for interpreting a variety of chemical reaction processes. However, predicting accurate PESs with high-level electronic structure methods is a challenging task due to the high computational…

化学物理 · 物理学 2022-06-09 Yanxian Tao , Xiongzhi Zeng , Yi Fan , Jie Liu , Zhenyu Li , Jinlong Yang

The role of numerical accuracy in training and evaluating neural network-based potential energy surfaces is examined for different experimental observables. For observables that require third- and fourth-order derivatives of the total…

化学物理 · 物理学 2023-11-30 Silvan Käser , Markus Meuwly

Full-dimensional reactive potential energy surfaces (PESs) for the OCS$^+$ cation are constructed to describe S$^+$ loss in the electronic ground state and seven low-lying electronically excited states. High-level \textit{ab initio}…

化学物理 · 物理学 2026-05-15 Cangtao Yin , Stefan Willitsch , Markus Meuwly

We introduce a new method for computing spectra of molecules for which a spin-spin term in the Hamiltonian has an important effect. In previous calculations, matrix elements of the spin-spin term and of the potential were obtained by…

化学物理 · 物理学 2019-05-23 Xiao-Gang Wang , Tucker Carrington

Accurately simulating molecular vibronic spectra remains computationally challenging due to the exponential scaling of required calculations. Here, we show that employing the linear coupling model within the gaussian boson sampling…

量子物理 · 物理学 2025-08-07 I. Konyshev , R. Pradip , O. Page , C. Ünlüer , R. T. Nasibullin , V. V. Rybkin , W. Pernice , S. Ferrari

An algebraic model of Boson-realization is proposed to study the vibrational spectra of a tetrahedral molecule, where ten sets of boson creation and annihilation operators are used to construct the Hamiltonian with $T_{d}$ symmetry. There…

chem-ph · 物理学 2009-10-28 Zhong-Qi Ma , Xi-Wen Hou , Mi Xie

The vibrational excitations of ozone, including both bending and stretching vibrations, are studied in the framework of a symmetry-adapted algebraic approach. This method is based on the isomorphism between the U(2) algebra and the…

chem-ph · 物理学 2015-06-24 F. Perez-Bernal , J. M. Arias , A. Frank , R. Lemus , R. Bijker

The precise theoretical determination of the geometrical parameters of molecules at the minima of their potential energy surface and of the corresponding vibrational properties are of fundamental importance for the interpretation of…

强关联电子 · 物理学 2013-06-19 Andrea Zen , Delyan Zhelyazov , Leonardo Guidoni

Electric dipole and polarizability surfaces are developed for the methanol (CH$_3$OH) molecule using ab initio electronic structure data, computed at the CCSD/aug-cc-pVTZ level of theory, and equivariant neural networks. These property…

化学物理 · 物理学 2026-05-01 Ayaki Sunaga , Albert P. Bartók , Edit Mátyus

Monitoring ozone concentrations in the Earth's atmosphere using spectroscopic methods is a major activity which undertaken both from the ground and from space. However there are long-running issues of consistency between measurements made…

We generalise the non-affine theory of viscoelasticity for use with large, well-sampled systems of arbitrary chemical complexity. Having in mind predictions of mechanical and vibrational properties of amorphous systems with atomistic…

无序系统与神经网络 · 物理学 2020-07-27 Ivan Kriuchevskyi , Vladimir V. Palyulin , Rico Milkus , Robert M. Elder , Timothy W. Sirk , Alessio Zaccone

Methyl benzoate (MB) is studied as a model compound for the development of new IR pulse schemes with possible applicability to biomolecules. Anharmonic vibrational modes of MB are calculated on different level (MP2, SCS, CCSD(T) with…

化学物理 · 物理学 2014-01-03 Kiran Sankar Maiti , Christoph Scheurer

A potential energy curve (PEC) accurate to a fraction of 1 ppm ($1:10^6$) is computed for the $^3\Sigma_\mathrm{u}^+$ state of He$_2$ endowed with relativistic and QED corrections. The nuclear Schr\"odinger equation is solved on this PEC…

化学物理 · 物理学 2026-02-25 Ádám Margócsy , Balázs Rácsai , Péter Jeszenszki , Edit Mátyus

There has been a veritable explosion of methods and software to perform machine-learned regression on datasets of electronic energies and forces to develop high-dimensional machine learned potential energy surfaces (ML-PESs). A major, but…

A very accurate, (HF)$_2$ potential energy surface (PES) is constructed based on \ai\ calculations performed using the MOLPRO package at the CCSD(T) level of theory with an aug-cc-pvQz-F12 basis set at about 161~000 points. a higher…

原子与分子团簇 · 物理学 2021-07-27 Roman I. Ovsyannikov , Vladimir Yu. Makhnev , Nikolai F. Zobov , Jacek Koput , Jonathan Tennyson

We present in detail and validate an effective Monte Carlo approach for the calculation of the nuclear vibrational densities via integration of molecular eigenfunctions that we have preliminary employed to calculate the densities of the…

化学物理 · 物理学 2020-12-08 Chiara Aieta , Gianluca Bertaina , Marco Micciarelli , Michele Ceotto

The determination of thermal and vibrational relaxation rates of triatomic systems suitable for application in hypersonic model calculations is discussed. For this, potential energy surfaces for ground and electronically excited state…

化学物理 · 物理学 2020-11-06 Debasish Koner , Raymond J. Bemish , Markus Meuwly

We present a 3D isotropic ab initio three-body (para-H$_2$)$_3$ interaction potential energy surface (PES). The electronic structure calculations are carried out at the correlated coupled-cluster theory level, with single, double, and…

化学物理 · 物理学 2025-06-05 Alexander Ibrahim , Pierre-Nicholas Roy

Amorphous solids, like metallic glasses, exhibit an excess of low frequency vibrational states reflecting the break-up of sound due to the strong structural disorder inherent to these materials. Referred to as the boson peak regime of…

计算物理 · 物理学 2019-02-20 Giuseppe Accaputo , Peter M. Derlet , Peter Arbenz