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We present a theory of vibrational modulation of two-dimensional coherent Fourier transformed electronic spectra. Based on an expansion of the system's energy gap correlation function in terms of Huang-Rhys factors, we explain the…

Methods for reconstructing the spectral density of a vibrational environment from experimental data can yield key insights into the impact of the environment on molecular function. Although such experimental methods exist, they generally…

Chemical Physics · Physics 2025-09-11 Roosmarijn de Wit , Jonathan Keeling , Brendon W. Lovett , Alex W. Chin

The prevalence of long-lasting oscillatory signals in the 2d echo-spectroscopy of light-harvesting complexes has led to a search for possible mechanisms. We investigate how two causes of oscillatory signals are intertwined: (i) electronic…

Biological Physics · Physics 2013-08-20 Christoph Kreisbeck , Tobias Kramer , Alan Aspuru-Guzik

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

Electronic energy transfer in photosynthesis occurs over a range of time scales and under a variety of intermolecular coupling conditions. Recent work has shown that electronic coupling between chromophores can lead to coherent oscillations…

Advances in light sources and time resolved spectroscopy have made it possible to excite specific atomic vibrations in solids and to observe the resulting changes in electronic properties but the mechanism by which phonon excitation causes…

Superconductivity · Physics 2017-05-05 Dante M. Kennes , Eli Y. Wilner , David R. Reichman , Andrew J. Millis

Multidimensional coherent optical spectroscopy is one of the most powerful tools for investigating complex quantum mechanical systems. While it was conceived decades ago in magnetic resonance spectroscopy using micro- and radio-waves, it…

We demonstrate a two-dimensional time-domain spectroscopy method to extract amplitude and phase modifications of excited atomic states caused by the interaction with ultrashort laser pulses. The technique is based on Fourier analysis of the…

Atomic Physics · Physics 2015-06-19 Alexander Blättermann , Christian Ott , Andreas Kaldun , Thomas Ding , Thomas Pfeifer

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

We investigate how correlated fluctuations affect oscillatory features in rephasing and non-rephasing two-dimensional (2D) electronic spectra of a model dimer system. Based on a beating map analysis, we show that non-secular environmental…

The non-equilibrium dynamics of matter excited by light may produce electronic phases that do not exist in equilibrium, such as laser-induced high-transition-temperature superconductivity. Here we simulate the dynamics of a metal driven at…

Strongly Correlated Electrons · Physics 2022-12-05 John Sous , Benedikt Kloss , Dante M. Kennes , David R. Reichman , Andrew J. Millis

We demonstrate that the coupling of excitonic and vibrational motion in biological complexes can provide mechanisms to explain the long-lived oscillations that have been obtained in non linear spectroscopic signals of different…

Chemical Physics · Physics 2015-06-17 M. B. Plenio , J. Almeida , S. F. Huelga

We perform two-dimensional coherent spectroscopy on CdSe/CdZnS core/shell colloidal quantum dots at cryogenic temperatures. In the two-dimensonal spectra, sidebands due to electronic coupling with CdSe lattice LO-phonon modes are observed…

Materials Science · Physics 2019-08-16 A. Liu , D. B. Almeida , W. K. Bae , L. A. Padilha , S. T. Cundiff

Standard rheometers assess mechanical properties of viscoelastic samples up to 100~Hz, which often hinders the assessment of the local-scale dynamics. We demonstrate that high-frequency analysis can be achieved by inducing broadband…

Two-photon excitation spectroscopy is a nonlinear technique that has gained rapidly in interest and significance for studying the complex energy-level structure and transition probabilities of materials. While the conventional spectroscopy…

Quantum Physics · Physics 2022-11-23 Yuanyuan Chen , Roberto de J. León-Montiel , Lixiang Chen

The interplay of nuclear and electronic dynamics characterizes the multi-dimensional electronic spectra of various molecular and solid-state systems. Theoretically, the observable effect of such interplay can be accounted for by response…

Quantum Physics · Physics 2023-02-07 Filippo Troiani

Time and angular resolved photoelectron spectroscopy is a powerful technique to measure electron dynamics in solids. Recent advances in this technique have facilitated band and energy resolved observations of the effect that excited…

Materials Science · Physics 2020-09-30 Umberto De Giovannini , Hannes Hübener , Shunsuke A. Sato , Angel Rubio

We investigate two-color photon correlations in the light emitted by strongly coupled two-level emitters. Spectral filtering allows us to manipulate the collected light statistics and we show that the resonances induced by dipole-dipole…

Quantum Physics · Physics 2021-05-12 Elnaz Darsheshdar , Mathilde Hugbart , Romain Bachelard , Celso Jorge Villas-Boas

Raman spectra obtained by the inelastic scattering of light by crystalline solids contain contributions from first-order vibrational processes (e.g. the emission or absorption of one phonon, a quantum of vibration) as well as higher-order…

Materials Science · Physics 2017-08-22 Yannick Gillet , Stefan Kontur , Matteo Giantomassi , Claudia Draxl , Xavier Gonze

The two-dimensional spectroscopy has recently revealed oscillatory behavior of excitation dynamics in molecular systems. However, in the majority of cases it is strongly debated if excitonic or vibrational wavepackets, or evidences of…

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