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In single vibronic level (SVL) fluorescence experiments, the electronically excited initial state is also excited in one or several vibrational modes. Whereas computing all contributing Franck-Condon factors individually becomes impractical…

Chemical Physics · Physics 2024-12-17 Zhan Tong Zhang , Jiří J. L. Vaníček

Hagedorn wavepackets have been used to compute single vibronic level (SVL) spectra efficiently in model harmonic potentials. To make the Hagedorn approach practical for realistic polyatomic molecules with anharmonicity, here we combine…

Chemical Physics · Physics 2025-01-09 Zhan Tong Zhang , Máté Visegrádi , Jiří J. L. Vaníček

Hagedorn wavepacket dynamics yields exact single vibronic level (SVL) fluorescence spectra in global harmonic models. To partially describe the effects of anharmonicity, important in the spectra of real molecules, we describe a combination…

Chemical Physics · Physics 2025-10-14 Zhan Tong Zhang , Máté Visegrádi , Jiří J. L. Vaníček

Simulating vibrationally resolved electronic spectra of anharmonic systems, especially those involving double-well potential energy surfaces, often requires expensive quantum dynamics methods. Here, we explore the applicability and…

Chemical Physics · Physics 2022-05-12 Tomislav Begušić , Enrico Tapavicza , Jiří Vaníček

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…

Quantum Physics · Physics 2025-08-07 I. Konyshev , R. Pradip , O. Page , C. Ünlüer , R. T. Nasibullin , V. V. Rybkin , W. Pernice , S. Ferrari

Single-Hessian Gaussian wavepacket dynamics (GWD) significantly reduces the computational burden of Heller's local harmonic GWD, while maintaining comparable accuracy in approximating vibronic spectra. Here, we provide a new, symplectic…

Chemical Physics · Physics 2026-05-11 Davide Barbiero , Jiří J. L. Vaníček

Excitation-energy transfer (EET) and relaxation in an optically excited building block of poly(phenylene ethynylene) (PPE) dendrimers are simulated using wavepackets with the multilayer multiconfiguration time-dependent Hartree (ML-MCTDH)…

Chemical Physics · Physics 2025-07-01 Joachim Galiana , Michèle Desouter-Lecomte , Benjamin Lasorne

Vibrational levels of the electronic ground states in dye molecules have not been previously explored at high resolution in solid matrices. We present new spectroscopic measurements on single polycyclic aromatic molecules of…

Energy spectroscopy is a powerful tool with diverse applications across various disciplines. The advent of programmable digital quantum simulators opens new possibilities for conducting spectroscopy on various models using a single device.…

We describe a simple automated method to extract and quantify transient heterogeneous dynamical changes from large datasets generated in single molecule/particle tracking experiments. Based on wavelet transform, the method transforms raw…

Data Analysis, Statistics and Probability · Physics 2013-06-04 Kejia Chen , Bo Wang , Juan Guan , Steve Granick

Highly excited vibrational states of an isolated molecule encode the vibrational energy flow pathways in the molecule. Recent studies have had spectacular success in understanding the nature of the excited states mainly due to the extensive…

Chemical Physics · Physics 2009-11-07 A. Semparithi , V. Charulatha , S. Keshavamurthy

The article presents the result of an extended in silico experiment on computational vibrational spectroscopy of graphene molecules performed using the virtual vibrational spectrometer UHF VVS, previously proposed in the first part of the…

Materials Science · Physics 2020-08-26 Elena F. Sheka , Nadezhda A. Popova

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

A virtual vibrational spectrometer, based on efficient software exploring unrestricted Hartree-Fock approximation, has been proposed to perform computational spectroscopy of radicals. The computational device allows obtaining spectra of IR…

Chemical Physics · Physics 2020-08-26 Elena F. Sheka , V. A. Popova

The simple ultraviolet absorption spectrum of thiophene is investigated using a combination of a vibronic coupling model Hamiltonian with multi-configuration time-dependent Hartree quantum dynamics simulations. The model includes five…

Chemical Physics · Physics 2024-07-30 Michael A. Parkes , Graham A. Worth

Hagedorn functions are carefully constructed generalizations of Hermite functions to the setting of many-dimensional squeezed and coupled harmonic systems. Wavepackets formed by superpositions of Hagedorn functions have been successfully…

Quantum Physics · Physics 2025-08-18 Jiří J. L. Vaníček , Zhan Tong Zhang

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

In this article, we develop and analyse a new spectral method to solve the semi-classical Schr\"odinger equation based on the Gaussian wave-packet transform (GWPT) and Hagedorn's semi-classical wave-packets (HWP). The GWPT equivalently…

Numerical Analysis · Mathematics 2021-10-12 Borui Miao , Giovanni Russo , Zhennan Zhou

We show how vibronic spectra in molecular systems can be simulated in an efficient and accurate way using first principles approaches without relying on the explicit use of multiple Born-Oppenheimer potential energy surfaces. We demonstrate…

Chemical Physics · Physics 2024-03-01 Kevin Lively , Guillermo Albareda , Shunsuke A. Sato , Aaron Kelly , Angel Rubio

We theoretically propose a multidimensional high-harmonic echo spectroscopy technique which utilizes strong optical fields to resolve coherent electron dynamics spanning an energy range of multiple electron Volts. Using our recently…

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