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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…

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…

生物物理 · 物理学 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…

化学物理 · 物理学 2014-01-17 Vytautas Butkus , Leonas Valkunas , Darius Abramavicius

Vibrationally resolved electronic absorption spectra including the effect of vibrational pre-excitation are computed in order to interpret and predict vibronic transitions that are probed in the Vibrationally Promoted Electronic Resonance…

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…

化学物理 · 物理学 2012-11-27 Vytautas Butkus , Leonas Valkunas , Darius Abramavicius

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…

化学物理 · 物理学 2012-11-27 Vytautas Butkus , Donatas Zigmantas , Leonas Valkunas , Darius Abramavicius

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…

化学物理 · 物理学 2015-06-17 M. B. Plenio , J. Almeida , S. F. Huelga

A time-dependent approach is used to explore inelastic effects during electron transport through few-level systems. We study a tight-binding chain with one and two sites connected to vibrations. This simple but transparent model gives…

介观与纳米尺度物理 · 物理学 2009-11-13 S. Monturet , N. Lorente

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 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…

量子物理 · 物理学 2023-02-07 Filippo Troiani

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…

Using time as an additional design parameter in electromagnetism, photonics, and wave physics is attracting considerable research interest, motivated by the possibility to explore physical phenomena and engineering opportunities beyond the…

光学 · 物理学 2024-11-12 Matteo Ciabattoni , Zeki Hayran , Francesco Monticone

The time-development of photoexcitations in molecular aggregates exhibits specific dynamics of electronic states and vibrational wavefunction. We discuss the dynamical formation of entanglement between electronic and vibrational degrees of…

量子物理 · 物理学 2007-05-23 Dmitri S. Kilin , Jeffrey A. Cina , Oleg V. Prezhdo

The spatio-temporal dynamics of the deformation of a vibrated plate is measured by a high speed Fourier transform profilometry technique. The space-time Fourier spectrum is analyzed. It displays a behavior consistent with the premises of…

混沌动力学 · 物理学 2011-07-13 Nicolas Mordant

Recently, nuclear vibrational contribution signatures in 2D electronic spectroscopy have attracted considerable interest, in particular as regards interpretation of the oscillatory transients observed in light-harvesting complexes. These…

化学物理 · 物理学 2015-06-04 Yuta Fujihashi , Graham R. Fleming , Akihito Ishizaki

We present a perturbation approach rooted in time-dependent density-functional theory to calculate electron hole (eh)-pair excitation spectra during the non-adiabatic vibrational damping of adsorbates on metal surfaces. Our analysis for the…

化学物理 · 物理学 2017-11-22 Simon P. Rittmeyer , Jörg Meyer , Karsten Reuter

Multidimensional spectroscopy unveils the interplay of nuclear and electronic dynamics, which characterizes the ultrafast dynamics of various molecular and solid-state systems. In a class of models widely used for the simulation of such…

量子物理 · 物理学 2023-08-28 Frank Ernesto Quintela Rodriguez , Filippo Troiani

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…

化学物理 · 物理学 2025-09-11 Roosmarijn de Wit , Jonathan Keeling , Brendon W. Lovett , Alex W. Chin

A theory of vibrational excitations based on power-law spatial correlations in the elastic constants (or equivalently in the internal stress) is derived, in order to determine the vibrational density of states $D(\omega)$ of disordered…

无序系统与神经网络 · 物理学 2020-11-30 Bingyu Cui , Alessio Zaccone

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…

原子物理 · 物理学 2015-06-19 Alexander Blättermann , Christian Ott , Andreas Kaldun , Thomas Ding , Thomas Pfeifer
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