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Molecular absorption and photo-electron spectra can be efficiently predicted with real-time time-dependent density-functional theory (TDDFT). We show here how these techniques can be easily extended to study time-resolved pump-probe…

Atomic and Molecular Clusters · Physics 2013-01-10 Umberto De Giovannini , Gustavo Brunetto , Alberto Castro , Jessica Walkenhorst , Angel Rubio

Multidimensional optical spectroscopy observes transient excitation dynamics through the time evolution of spectral correlations. Its action-detected variants offer several advantages over the coherent detection and are thus becoming…

Chemical Physics · Physics 2024-12-31 Kateřina Charvátová , Pavel Malý

Time-resolved photoemission spectroscopy is the key technique to probe the real-time non-equilibrium dynamics of electronic states. Theoretical predictions of the time dependent spectral function for realistic systems is however, a…

Computational Physics · Physics 2024-05-24 Cian Reeves , Vojtech Vlcek

We present a two-dimensional electronic spectroscopy (2DES) platform driven by a novel Coherent Loop-based Integrated Modulating and Beamsplitting System (CLIMBS). Coupled with an octave-spanning multiple-plate continuum (MPC) source,…

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…

Two-dimensional electronic spectra (2DES) provide unique ways to track the energy transfer dynamics in light-harvesting complexes. The interpretation of the peaks and structures found in experimentally recorded 2DES is often not…

Biological Physics · Physics 2020-01-07 Tobias Kramer , Mirta Rodríguez

Programmable electron-beam scanning offers new opportunities to improve dose efficiency and suppress scan-induced artifacts in scanning transmission electron microscopy. Here, we systematically benchmark the impact of non-raster…

Nonadiabatic effects in chemical reaction at metal surfaces, due to excitation of electron-hole pairs, stand at the frontier of the studies of gas-surface reaction dynamics. However, the first principles description of electronic excitation…

Chemical Physics · Physics 2019-12-20 Yaolong Zhang , Reinhard J. Maurer , Bin Jiang

We use projected entangled-pair states (PEPS) to calculate the large deviations (LD) statistics of the dynamical activity of the two dimensional East model, and the two dimensional symmetric simple exclusion process (SSEP) with open…

Statistical Mechanics · Physics 2025-02-06 Luke Causer , Mari Carmen Bañuls , Juan P. Garrahan

We consider an implementation of the adiabatic spin dynamics approach in a tight-binding description of the electronic structure. The adiabatic approximation for spin-degrees of freedom assumes that the faster electronic degrees of freedom…

Two-dimensional coherent spectroscopy (2DCS) with terahertz radiation offers a promising new avenue for the exploration of many-body phenomena in quantum magnets. This includes the potential diagnosis of fractionalized excitations, for…

Strongly Correlated Electrons · Physics 2024-10-29 Yoshito Watanabe , Simon Trebst , Ciarán Hickey

Two-dimensional electronic spectroscopy has become one of the main experimental tools for analyzing the dynamics of excitonic energy transfer in large molecular complexes. Simplified theoretical models are usually employed to extract model…

Chemical Physics · Physics 2019-01-17 Mirta Rodríguez , Tobias Kramer

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

How atoms and electrons in a molecule move during a chemical reaction and how rapidly energy is transferred to or from the surroundings can be studied with flashes of laser light. However, despite prolonged efforts to develop various…

Chemical Physics · Physics 2022-01-05 JunWoo Kim , Jonggu Jeon , Tai Hyun Yoon , Minhaeng Cho

Chemical relaxation phenomena, including photochemistry and electron transfer processes, form a vigorous area of research in which nonadiabatic dynamics plays a fundamental role. Here, we show that for nonadiabatic dynamics with two…

Chemical Physics · Physics 2022-07-20 Yanze Wu , Xuezhi Bian , Jonathan Rawlinson , Robert G. Littlejohn , Joseph E. Subotnik

A general theoretical framework is derived for the recently developed multi-state trajectory (MST) approach from the time dependent Schr\"odinger equation, resulting in equations of motion for coupled nuclear-electronic dynamics equivalent…

Chemical Physics · Physics 2017-09-13 Guohua Tao

Coherent spin resonance methods, such as nuclear magnetic resonance and electron spin resonance spectroscopy, have led to spectrally highly sensitive, non-invasive quantum imaging techniques. Here, we propose a pump-probe spin resonance…

Quantum Physics · Physics 2024-12-02 Philipp Haslinger , Stefan Nimmrichter , Dennis Rätzel

The meromorphic functional calculus developed in Part I overcomes the nondiagonalizability of linear operators that arises often in the temporal evolution of complex systems and is generic to the metadynamics of predicting their behavior.…

Chaotic Dynamics · Physics 2018-04-18 Paul M. Riechers , James P. Crutchfield

Ultrafast two-dimensional spectroscopy utilizes correlated multiple light-matter interactions for retrieving dynamic features that may otherwise be hidden under the linear spectrum. Its extension to the terahertz regime of the…

We study the semiclassical Ehrenfest trajectories in open quantum systems. We first derive in explicit form the Fokker-Planck equation that governs the time evolution of the mixing measure for a Gaussian mixture. Then, we embed the…

Quantum Physics · Physics 2026-05-01 Xiao-Kan Guo