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Accurate vibrational spectra are essential for understanding how molecules behave, yet their computation remains challenging and benchmark data to reliably compare different methods are sparse. Here, we present high-accuracy eigenstate…

Chemical Physics · Physics 2025-04-16 Henrik R. Larsson

Vibrational spectra and wavefunctions of polyatomic molecules can be calculated at low memory cost using low-rank sum-of-product (SOP) decompositions to represent basis functions generated using an iterative eigensolver. Using a SOP tensor…

Chemical Physics · Physics 2017-08-02 Arnaud Leclerc , Phillip S. Thomas , Tucker Carrington

Present day computers do not have enough memory to store the high-dimensional tensors required when using a direct product basis to compute vibrational energy levels of a polyatomic molecule with more than about 5 atoms. One way to deal…

Computational Physics · Physics 2024-06-19 Sangeeth Das Kallullathil , Tucker Carrington

We present how to compute vibrational eigenstates with tree tensor network states (TTNSs), the underlying ansatz behind the multilayer multiconfiguration time-dependent Hartree (ML-MCTDH) method. The eigenstates are computed with an…

Chemical Physics · Physics 2019-11-27 Henrik R. Larsson

Quantum computers are ideal for solving chemistry problems due to their polynomial scaling with system size in contrast to classical computers which scale exponentially. Until now molecular energy calculations using quantum computing…

Quantum Physics · Physics 2019-08-15 Alexander Teplukhin , Brian K. Kendrick , Dmitri Babikov

Vibrational spectroscopy is a key technique to elucidate microscopic structure and dynamics. Without the aid of theoretical approaches, it is however, often difficult to understand such spectra at a microscopic level. Ab initio molecular…

Chemical Physics · Physics 2023-03-14 Philipp Schienbein

We present a practical method to compute the vibrational resonant Raman spectra in solids with delocalized excitations. We apply this approach to the study of tetrahedrous amorphous carbon. We determine the vibrational eigenmodes and…

Materials Science · Physics 2009-11-07 Mickael Profeta , Francesco Mauri

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 propose an iterative method for computing vibrational spectra that significantly reduces the memory cost of calculations. It uses a direct product primitive basis, but does not require storing vectors with as many components as there are…

Computational Physics · Physics 2014-05-13 Arnaud Leclerc , Tucker Carrington

The vibrational behavior of molecules serves as a crucial fingerprint of their structure, chemical state, and surrounding environment. Neutron vibrational spectroscopy provides comprehensive measurements of vibrational modes without…

Chemical Physics · Physics 2025-02-19 Bowen Han , Pei Zhang , Kshitij Mehta , Massimiliano Lupo Pasini , Mingda Li , Yongqiang Cheng

We propose an accurate and efficient method to compute vibrational spectra of molecules, based on exact diagonalization of an algebraically calculated matrix based on powers of Morse coordinate. The present work focuses on the 1D potential…

Chemical Physics · Physics 2009-11-13 Andrea Bordoni , Nicola Manini

The behavior of polyatomic molecules around their equilibrium positions can be regarded as quantum coupled anharmonic oscillators. Solving the corresponding Schr\"odinger equations can interpret or predict experimental spectra of molecules.…

Chemical Physics · Physics 2024-07-10 Qi Zhang , Rui-Si Wang , Lei Wang

Quantum computation of vibrational properties of molecules is a promising platform to obtain computational advantages for computational chemistry. However, fault-tolerant quantum computations of vibrational properties remain a relatively…

A combined approach that uses the vibrational self-consistent field (VSCF) and vibrational configuration interaction (VCI) method together with the semiclassical instanton theory was developed to study vibrational tunneling spectra of…

Chemical Physics · Physics 2022-02-07 Mihael Eraković , Marko T. Cvitaš

This article covers few selected aspects of quantum theory of molecular rotations and vibrations. Triatomic molecules are the simplest systems, which show qualitative characteristics of larger polyatomic molecules. On the minimal example of…

Chemical Physics · Physics 2022-03-18 Emil J. Zak

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…

Chemical Physics · Physics 2014-01-03 Kiran Sankar Maiti , Christoph Scheurer

Machine learning has revolutionized the high-dimensional representations for molecular properties such as potential energy. However, there are scarce machine learning models targeting tensorial properties, which are rotationally covariant.…

Chemical Physics · Physics 2020-08-11 Yaolong Zhang , Sheng Ye , Jinxiao Zhang , Ce Hu , Jun Jiang , Bin Jiang

We present an efficient method of calculating the vibrational spectrum of a magnetic molecule adsorbed on a superconductor, directly related to the first derivative of the tunneling $IV$ curve. The work is motivated by a recent…

Mesoscale and Nanoscale Physics · Physics 2025-01-14 Athanasios Koliogiorgos , Richard Korytár

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…

Chemical Physics · Physics 2019-05-23 Xiao-Gang Wang , Tucker Carrington

We describe a new approach based on semiclassical molecular dynamics that allows to simulate infrared absorption or emission spectra of molecular systems with inclusion of anharmonic intensities. This is achieved from semiclassical power…

Chemical Physics · Physics 2018-11-12 Marco Micciarelli , Riccardo Conte , Jaime Suarez , Michele Ceotto
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