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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…

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

Problems in the field of open quantum systems often involve an environment that strongly influences the dynamics of excited states. Here we present a numerical method to model optical spectra of non-Markovian open quantum systems. The…

Quantum Physics · Physics 2025-05-01 Roosmarijn de Wit , Jonathan Keeling , Brendon W. Lovett , Alex W. Chin

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

Electron energy loss spectroscopy is consolidating as a powerful tool to explore electronic (as well as vibrational) excitations of matter, including molecules. Performed in a scanning transmission electron microscope, this technique is…

Chemical Physics · Physics 2021-03-05 Ciro A. Guido , Enzo Rotunno , Matteo Zanfrognini , Stefano Corni , Vincenzo Grillo

Two-dimensional electronic spectroscopy (2DES) provides rich information about how the electronic states of molecules, proteins, and solid-state materials interact with each other and their surrounding environment. Atomistic molecular…

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…

Quantum Physics · Physics 2023-08-28 Frank Ernesto Quintela Rodriguez , Filippo Troiani

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

The spectral representation is an effecient tool to explore electrical properties of material mixtures. It separates the contributions of geometrical topology and intrinsic properties of the constituents in the system. The aim of this paper…

Materials Science · Physics 2007-05-23 Enis Tuncer

The light-harvesting efficiency of a photoactive molecular complex is largely determined by the properties of its electronic quantum states. Those, in turn, are influenced by molecular vibrational states of the nuclear degrees of freedom.…

Biological Physics · Physics 2019-10-23 Hong-Guang Duan , Michael Thorwart , R. J. Dwayne Miller

Terahertz molecular motions are often probed by high-frequency molecular oscillators in different types of non-linear vibrational spectroscopy. Recently developed two-dimensional terahertz-infrared-visible spectroscopy allows direct…

Chemical Physics · Physics 2023-04-19 Pankaj Seliya , Mischa Bonn , Maksim Grechko

Virtual excitations, inherent to ultrastrongly coupled light-matter systems, induce measurable modifications in system properties, offering a novel resource for quantum technologies. In this work, we demonstrate how these virtual…

Quantum Physics · Physics 2025-09-12 Christoph Hotter , Adam Miranowicz , Karol Gietka

Vibrational density of states of a classical two-dimensional electron system obtained with a molecular-dynamics simulation is shown to have a peak in both solid and liquid phases. From an exact diagonalisation of the dynamical matrix, the…

Strongly Correlated Electrons · Physics 2009-10-31 Satoru Muto , Hideo Aoki

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

Spectral densities encode the relevant information characterising the system-environment interaction in an open-quantum system problem. Such information is key to determining the system's dynamics. In this work, we leverage the potential of…

Quantum Physics · Physics 2024-03-13 Jessica Barr , Giorgio Zicari , Alessandro Ferraro , Mauro Paternostro

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

A procedure is developed to rigorously decompose experimental loss spectra of medium-energy electrons reflected from solid surfaces into contributions due to surface and volume electronic excitations. This can be achieved by analysis of two…

Materials Science · Physics 2009-11-11 Wolfgang S. M. Werner

Vibrational-excitation cross sections of ground electronic state of carbon dioxide molecule by electron-impact through the CO2-(2\Pi) shape resonance is considered in the separation of the normal modes approximation. Resonance curves and…

Chemical Physics · Physics 2016-11-01 V. Laporta , J. Tennyson , R. Celiberto

We present a review of the basic ideas and techniques of the spectral density functional theory which are currently used in electronic structure calculations of strongly-correlated materials where the one-electron description breaks down.…

Strongly Correlated Electrons · Physics 2009-11-11 G. Kotliar , S. Y. Savrasov , K. Haule , V. S. Oudovenko , O. Parcollet , C. A. Marianetti

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…

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