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We report the first experimental two-dimensional infrared (2D IR) spectra of novel molecular photonic excitations - vibrational-polaritons. The application of advanced 2D IR spectroscopy onto novel vibrational-polariton challenges and…

A general theory of electronic excitations in aggregates of molecules coupled to intramolecular vibrations and the harmonic environment is developed for simulation of the third-order nonlinear spectroscopy signals. The model is applied in…

Chemical Physics · Physics 2014-01-17 Vytautas Butkus , Leonas Valkunas , Darius Abramavicius

Two-dimensional (2D) vibrational spectroscopy is a powerful means of investigating the structure and dynamics of complex molecules in condensed phases. However, even in theory, analysis of 2D spectra resulting from complex inter- and…

Chemical Physics · Physics 2025-01-07 Ryotaro Hoshino , Yoshitaka Tanimura

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

Understanding the vibrational and thermal properties of amorphous solids is one of the most discussed and long-standing issues in condensed matter physics. Recent works have made significant steps towards understanding harmonic vibrational…

Soft Condensed Matter · Physics 2020-02-28 Hideyuki Mizuno , Masanari Shimada , Atsushi Ikeda

We develop a first-principles approach for the treatment of vibronic interactions in solids that overcomes the main limitations of state-of-the-art electron-phonon coupling formalisms. In particular, anharmonic effects in the nuclear…

Materials Science · Physics 2020-07-29 Marios Zacharias , Matthias Scheffler , Christian Carbogno

Double-$\gamma$ vibrations in deformed nuclei are analyzed in the context of the interacting boson model. A simple extension of the original version of the model towards higher-order interactions is required to explain the observed…

Nuclear Theory · Physics 2009-11-06 J. E. Garcia-Ramos , J. M Arias , P. Van Isacker

Quantum beats in nonlinear spectroscopy of molecular aggregates are often attributed to electronic phenomena of excitonic systems, while nuclear degrees of freedom are commonly included into models as overdamped oscillations of bath…

Chemical Physics · Physics 2012-11-27 Vytautas Butkus , Leonas Valkunas , Darius Abramavicius

Vibrational polaritons are formed by strong coupling of molecular vibrations and photon modes in an optical cavity. Experiments have demonstrated that vibrational strong coupling can change molecular properties and even affect chemical…

Quantum Physics · Physics 2025-01-14 Thomas Schnappinger , Cyril Falvo , Markus Kowalewski

Understanding the molecular vibrations underlying each of the unknown infrared emission (UIE) bands (such as those found at 3.3, 3.4, 3.5, 6.2, 6.9, 7.7, 11.3, 15.8, 16.4, 18.9 mm) observed in or towards astronomical objects is a vital link…

Astrophysics of Galaxies · Physics 2018-11-22 SeyedAbdolreza Sadjadi , Quentin Andrew Parker

We model, simulate, and analyze the intramolecular modes of liquid H2O and D2O to elucidate how energy excitation, relaxation, and vibrational dephasing interplay through anharmonic mode-mode coupling. Our analysis employs two-dimensional…

Chemical Physics · Physics 2026-03-20 Kwanghee Park , Ryotaro Hoshino , Yoshitaka Tanimura

We study the collective behavior of molecules placed in an infrared (IR) microcavity, incorporating the local fluctuations, i.e., dynamical disorder. The cooperative feature in vibrational polaritons is shown to be dynamically eroded, due…

Quantum Physics · Physics 2018-06-19 Zhedong Zhang , Kai Wang , Zhenhuan Yi , Shaul Mukamel , Marlan O. Scully

Two dimensional spectroscopy is a powerful dynamical study method that has been developed in the last two decades. In 2D IR there are three experimental time periods during which the system vibrational modes of interest are excited, evolved…

Chemical Physics · Physics 2021-04-12 S. Tahereh Alavi

Coherent dynamics of coupled molecules are effectively characterized by the two-dimensional (2D) electronic coherent spectroscopy. Depending on the coupling between electronic and vibrational states, oscillating signals of purely…

Chemical Physics · Physics 2013-10-17 Vytautas Butkus , Donatas Zigmantas , Darius Abramavicius , Leonas Valkunas

Photonic resonance modes can be spectrally coupled to the vibrational modes of molecules in the mid-infrared regime through interactions between localized electric fields and nearby molecules. According to recent studies, radiative loss…

We introduce the Anharmonic Oscillator Symmetry Model to describe vibrational excitations in molecular systems exhibiting high degree of symmetry. A systematic procedure is proposed to establish the relation between the algebraic and…

chem-ph · Physics 2009-10-28 A. Frank , R. Lemus , R. Bijker , F. Perez-Bernal , J. M. Arias

Two-dimensional infrared (2DIR) spectroscopy is widely used to study molecular dynamics but it is typically restricted to solid and liquid phase samples and modest spectral resolution. Only recently, its potential to study gas-phase…

Optics · Physics 2022-11-01 Grzegorz Kowzan , Thomas K. Allison

Cavity dressing of molecular vibrational dynamics expands the role of characteristic vibrations as spectroscopic markers of underlying ultrafast dynamics. Interacting vibrational modes exhibit a pronounced excited state delocalization due…

Quantum Physics · Physics 2026-01-06 Arunangshu Debnath

Experimental and theoretical evidence point out to the crucial role of specific resonant intramolecular vibrational modes in the interpretation of long-lived coherences observed in two-dimensional spectra of some natural and synthetic light…

Chemical Physics · Physics 2020-07-15 Leonardo F. Calderón , Leonardo A. Pachón

This is the first in a series of two papers investigating the effect of electron-phonon coupling in two-dimensional Fourier transformed electronic spectroscopy. We present a series of one- and two-dimensional nonlinear spectroscopic…

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