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Using time dependent density functional theory (TDDFT) we examine the energy, angular and time-resolved photoelectron spectra (TRPES) of ethylene in a pump-probe setup. To simulate TRPES we expose ethylene to an ultraviolet (UV) femtosecond…

Atomic and Molecular Clusters · Physics 2014-08-28 Alison Crawford-Uranga , Umberto De Giovannini , Duncan John Mowbray , Stefan Kurth , Angel Rubio

Studies of ultrafast dynamics along with femtosecond-pulse metrology rely on non-linear processes, induced solely by the exciting/probing pulses or the pulses to be characterized. Extension of these approaches to the extreme-ultraviolet…

Atomic Physics · Physics 2015-05-27 P. Tzallas , E. Skantzakis , L. A. A. Nikolopoulos , G. D. Tsakiris , D. Charalambidis

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…

The capability of generating two intense, femtosecond x-ray pulses with controlled time delay opens the possibility of performing time-resolved experiments for x-ray induced phenomena. We have applied this capability to study the…

Imaging in real time the complete dynamics of a process as fundamental as photoemission has long been out of reach due to the difficulty of combining attosecond temporal resolution with fine spectral and angular resolutions. Here, we…

We present the extension of the time-dependent configuration interaction singles (TDCIS) method to the computation of the electron kinetic-energy spectrum in photoionization processes. Especially for strong and long ionizing light pulses…

Atomic Physics · Physics 2014-04-17 Antonia Karamatskou , Stefan Pabst , Yi-Jen Chen , Robin Santra

Split-pulse x-ray photon correlation spectroscopy has been proposed as one of the unique capabilities made possible with the x-ray free electron lasers. It enables characterization of atomic scale structural dynamics that dictates the…

Instrumentation and Detectors · Physics 2020-05-06 Yanwen Sun , Mike Dunne , Paul Fuoss , Taito Osaka , Aymeric Robert , Mark Sutton , Makina Yabashi , Diling Zhu

We propose a new scenario to apply IR-pump-XUV-probe schemes to resolving strong field ionization induced and attosecond pulse driven electron-hole dynamics and coherence in real time. The coherent driving of both the infrared laser and the…

Atomic Physics · Physics 2016-02-26 Jing Zhao , Jianmin Yuan , Zengxiu Zhao

We report two schemes to generate perfect anisotropy in the photoelectron angular distribution of a randomly oriented ensemble of polyatomic molecules. In order to exert full control over the anisotropy of photoelectron emission, we exploit…

Quantum Physics · Physics 2020-02-24 R. Esteban Goetz , Christiane P. Koch , Loren Greenman

We demonstrate the breakdown of molecular-frame dynamics induced by the uncoupling of molecular rotation from electronic motion in molecular Rydberg states. We observe this non-Born-Oppenheimer regime in the time domain through…

Atomic and Molecular Clusters · Physics 2017-07-05 Lucas J. Zipp , Adi Natan , Philip H. Bucksbaum

Recent advances in attosecond spectroscopy techniques have fueled the interest in the theoretical description of electronic processes taking place in the subfemtosecond time scale. Here we study the coupled dynamic screening of a localized…

Atomic and Molecular Clusters · Physics 2013-01-28 N. E. Koval , D. Sánchez-Portal , A. G. Borisov , R. Díez Muiño

We employ ultrafast pump-probe spectroscopy to directly monitor electron tunneling between discrete orbital states in a pair of spatially separated quantum dots. Immediately after excitation, several peaks are observed in the pump-probe…

In this research, we employ accurate time-dependent density functional calculations for ultrashort laser spectroscopy of nitrogen molecule. Laser pulses with different frequencies, intensities, and durations are applied to the molecule and…

Atomic and Molecular Clusters · Physics 2019-01-01 Mohammad Reza Jangrouei , S. Javad Hashemifar

We present a new extension of the UKRmol electron-molecule scattering code suite, which allows one to compute ab initio photoionization and photorecombination amplitudes for complex molecules, resolved both on the molecular alignment…

Chemical Physics · Physics 2014-02-18 Alex G Harvey , Danilo S Brambila , Felipe Morales , Olga Smirnova

Classical time-resolved optical spectroscopy experiments are performed using sequences of ultrashort light pulses, with photon fluxes incident on the sample which are many orders of magnitude higher than real-world conditions corresponding…

Time-resolved pump-probe measurements of Xe, pumped at 133~nm and probed at 266~nm, are presented. The pump pulse prepared a long-lived hyperfine wavepacket, in the Xe $5p^5(^2P^{\circ}_{1/2})6s~^2[1/2]^{\circ}_1$ manifold ($E=$77185…

We analyze Photo-Electron Spectra (PES) for a variety of excitation mechanisms from a simple mono-frequency laser pulse to involved combination of pulses as used, e.g., in attosecond experiments. In the case of simple pulses, the peaks in…

Atomic and Molecular Clusters · Physics 2015-05-20 C. -Z. Gao , P. M. Dinh , P. -G. Reinhard , E. Suraud

Time-resolved photoemission orbital tomography (tr-POT) offers unique possibilities for tracing molecular electron dynamics. The recorded pump-induced changes of the angle-resolved photoemission intensities allow to characterize unoccupied…

Electron motion on the (sub-)femtosecond time scale constitutes the fastest response in many natural phenomena such as light-induced phase transitions and chemical reactions. Whereas static electron densities in single molecules can be…