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Recent advances in laser technology allow us to follow electronic motion at its natural time-scale with ultra-fast time resolution, leading the way towards attosecond physics experiments of extreme precision. In this work, we assess the use…

Other Condensed Matter · Physics 2016-06-22 Jessica Walkenhorst , Umberto De Giovannini , Alberto Castro , Angel Rubio

We present the first fully ab initio calculations for attosecond transient absorption spectroscopy of atomic krypton with overlapping pump and probe pulses. Within the time-dependent configuration interaction singles (TDCIS) approach, we…

The theory for time-resolved photoemission spectroscopy as applied to pump-probe experiments is developed and solved for the generic case of a strongly correlated material. The formal development incorporates all of the nonequilibrium…

Strongly Correlated Electrons · Physics 2009-07-09 J. K. Freericks , H. R. Krishnamurthy , Th. Pruschke

Optical pump-probe spectroscopy is a powerful tool for the study of non-equilibrium electronic dynamics and finds wide applications across a range of fields, from physics and chemistry to material science and biology. However, a shortcoming…

We derive the two-time linear response theory for out-of-equilibrium pumped systems, generic pump-probe delays and probe frequencies. Such a theory enormously simplifies the numerical calculations, for instance, of the optical conductivity…

Optics · Physics 2024-12-10 Amir Eskandari-asl , Adolfo Avella

We put forward a first-principle NonEquilibrium Green's Function (NEGF) approach to calculate the transient photoabsorption spectrum of optically thin samples. The method can deal with pump fields of arbitrary strength, frequency and…

Atomic Physics · Physics 2015-09-30 E. Perfetto , A. -M. Uimonen , R. van Leeuwen , G. Stefanucci

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

A theory of pump-probe spectroscopy is developed in which optical fields drive two-photon Raman transitions between ground states of an ensemble of three-level $\Lambda $ atoms. Effects related to the recoil the atoms undergo as a result of…

Atomic Physics · Physics 2009-11-06 C. P. Search , P. R. Berman

The quantum dynamics of a system of Rb atoms, modeled by a V-type three-level system interacting with intense probe and pump pulses, are studied. The time-delay-dependent transient-absorption spectrum of an intense probe pulse is thus…

Atomic Physics · Physics 2018-02-14 Vadim Becquet , Stefano M. Cavaletto

The nonlinear response of materials, an increasingly important aspect of light-matter interaction, can be challenging to measure in highly absorbing materials. Here, we introduce an interferometric technique that enables a direct…

Optics · Physics 2024-11-25 C. D. Cruz , J. C. Stephenson , J. K. Wahlstrand

Based on the work done by an electromagnetic field on an atomic or molecular electronic system, a general gauge invariant formulation of transient absorption spectroscopy is presented within the semi-classical approximation. Avoiding…

In this work we propose an accurate first-principle approach to calculate the transient photo--absorption spectrum measured in Pump\&\,Probe experiments. We formulate a condition of {\em adiabaticity} and thoroughly analyze the…

Other Condensed Matter · Physics 2016-07-19 E. Perfetto , D. Sangalli , A. Marini , G. Stefanucci

Causality implies that by measuring an absorption spectrum, the time-dependent linear response function can be retrieved. Recent experiments suggest a link between the shape of spectral lines observed in absorption spectroscopy with the…

In this paper, we present a theoretical simulation of 87Rb absorption spectrum in a thermal cm-cell which is adaptive to the experimental observation. In experiment, the coupling and probe beams are configured to copropagate but…

Atomic Physics · Physics 2017-03-09 Hong Cheng , Shan-Shan Zhang , Pei-Pei Xin , Yuan Cheng , Hong-Ping Liu

The transient-absorption spectrum of a $V$-type three-level system is investigated, when this is periodically excited by a train of equally spaced, $\delta$-like pump pulses as, e.g., from an optical-frequency-comb laser. We show that, even…

Atomic Physics · Physics 2019-01-30 Juliane Haug , Stefano M. Cavaletto

In recent years, ultrafast pump-probe spectroscopy has provided insightful information about nonequilibrium dynamics of excitations in materials. In a typical experiment of time-resolved x-ray absorption spectroscopy, the systems are…

Strongly Correlated Electrons · Physics 2019-05-29 Chen-Yen Lai , Jian-Xin Zhu

The last decade has witnessed a rapid advancement in laser technology, enabling the direct monitoring and control of electronic motion on its natural attosecond to sub-femtosecond timescales. Ultrafast processes are conventionally studied…

Chemical Physics · Physics 2026-05-27 Torsha Moitra

Time-resolved angle-resolved photoemission spectroscopy is one of the most powerful pump-probe measurements of materials driven far from equilibrium. Unlike the linear-response regime, where the frequency-dependent response function is…

Strongly Correlated Electrons · Physics 2021-09-29 J. K. Freericks , Alexander F. Kemper

The electronic structure of atomic quantum systems and their dynamical interaction with light is reflected in transition dipole matrix elements coupling the system's energy eigenstates. In this work, we measure phase shifts of the…

Many new types of sensing or imaging surfaces are based on periodic thin films. It is explained how the response of those surfaces to partially coherent fields can be fully characterized by a set of functions in the wavenumber spectrum…

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