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We present three schemes to go beyond the electric-dipole approximation in X-ray absorption spectroscopy calculations within a four-component relativistic framework. The first is based on the full semi-classical light-matter interaction…

Chemical Physics · Physics 2021-07-02 Nanna Holmgaard List , Timothé Romain Léo Melin , Martin van Horn , Trond Saue

A relativistic transient absorption theory is derived, implemented and validated within the dipole approximation based on the time-dependent Dirac equation. Time-dependent simulations have been performed using the Dirac equation and the…

Atomic Physics · Physics 2020-10-14 Felipe Zapata , Jimmy Vinbladh , Eva Lindroth , Jan Marcus Dahlström

We present a spin-adapted time-dependent coupled cluster singles and doubles model for the molecular response to a sequence of ultrashort laser pulses. The implementation is used to calculate the electronic response to a valence-exciting…

Chemical Physics · Physics 2020-08-28 Andreas S. Skeidsvoll , Alice Balbi , Henrik Koch

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…

We present a novel function fitting method for approximating the propagation of the time-dependent electric dipole moment from real-time electronic structure calculations. Real-time calculations of the electronic absorption spectrum require…

Time-resolved spectroscopy provides the main tool for analyzing the dynamics of excitonic energy transfer in light-harvesting complexes. To infer time-scales and effective coupling parameters from experimental data requires to develop…

Chemical Physics · Physics 2018-11-28 Tobias Kramer , Mirta Rodriguez , Yaroslav Zelinskyy

We derive a time-dependent density functional theory appropriate for calculating the near-edge X-ray absorption spectrum in molecules and condensed matter. The basic assumption is to increase the space of many-body wave functions from one…

Strongly Correlated Electrons · Physics 2015-06-16 G. F. Bertsch , A. Lee

Transient absorption is a very powerful observable in attosecond experiments on atoms, molecules and solids and is frequently used in experiments employing phase-locked few-cycle infrared and XUV laser pulses derived from high harmonic…

Atomic Physics · Physics 2020-08-26 Lorenz Drescher , Marc J. J. Vrakking , Jochen Mikosch

We study light absorption in many-electron interacting systems beyond the linear regime by using a {\em single} broadband impulse of an electric field in the instantaneous limit. We determine non-pertubatively the absorption cross section…

Chemical Physics · Physics 2021-04-20 Alberto Guandalini , Caterina Cocchi , Stefano Pittalis , Alice Ruini , Carlo Andrea Rozzi

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

Laser assisted photoemission by a chirped subfemtosecond extreme ultraviolet (XUV) pulse is considered within an exactly solvable quantum-mechanical model. Special emphasis is given to the energy dependence of photoexcitation cross-section.…

Atomic Physics · Physics 2015-05-13 E. E. Krasovskii , M. Bonitz

Strong field photoemission and electron recollision provide a viable route to extract electronic and nuclear dynamics from molecular targets with attosecond temporal resolution. However, since an {\em ab-initio} treatment of even the…

Atomic Physics · Physics 2016-11-02 N. Suárez , A. Chacón , M. F. Ciappina , B. Wolter , J. Biegert , M. Lewenstein

While providing a highly accurate framework for simulating laser-induced many-electron dynamics in atom and molecules, including linear and nonlinear steady-state and transient absorption spectra, time-dependent coupled-cluster theory does…

We develop a new approach to electron transport in mesoscopic systems by using a particular single-particle basis. Although this basis generates redundant many-particle amplitudes, it greatly simplifies the treatment. By using our method…

Mesoscale and Nanoscale Physics · Physics 2015-10-28 Shmuel Gurvitz

The physical interpretation of time-resolved photoabsorption experiments is not as straightforward as for the more conventional photoabsorption experiments conducted on equilibrium systems. In fact, the relation between the transient…

Atomic Physics · Physics 2015-06-24 E. Perfetto , G. Stefanucci

Absorption and emission in inorganic bipolar solar cells based on low dimensional structures exhibiting the effects of quantum confinement is investigated in the framework of a comprehensive microscopic theory of the optical and electronic…

Mesoscale and Nanoscale Physics · Physics 2009-12-09 U. Aeberhard , U. Rau

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

Transient absorption spectroscopy (TAS) is among the most common ultrafast photochemical experiments, but its interpretation remains challenging. In this work, we present an efficient and robust method for simulating TAS signals from first…

In this manuscript we present a theoretical framework and its numerical implementation to simulate the out-of-equilibrium electron dynamics induced by the interaction of ultrashort laser pulses in condensed-matter systems. Our approach is…

Based on our earlier works [Phys. Rev. B 75, 195127 (2007) & J. Chem. Phys. 128, 234703 (2008)], we propose a formally exact and numerically convenient approach to simulate time-dependent quantum transport from first-principles. The…

Chemical Physics · Physics 2015-05-18 Xiao Zheng , GuanHua Chen , Yan Mo , SiuKong Koo , Heng Tian , ChiYung Yam , YiJing Yan
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