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We use time-resolved momentum microscopy at a free-electron laser (FEL) and extend orbital tomography into the time domain to image the electronic wave functions of excited molecular orbitals. This technique provides unprecedented insight…

We theoretically study how time- and angle-resolved photoemission spectroscopy can be applied for imaging coherent electron dynamics in molecules. We consider a process in which a pump pulse triggers coherent electronic dynamics in a…

光学 · 物理学 2018-12-11 Daria Popova-Gorelova , Jochen Küpper , Robin Santra

The development of attosecond technology has enabled the real-time observation of coherent electron motion in atoms, molecules and condensed phases. Experimentally, it is now possible to generate laser pulses of durations of only a few tens…

化学物理 · 物理学 2017-05-18 David Ayuso

Numerical simulations are presented to validate the possible use of cutting-edge attosecond time- resolved photoelectron spectroscopy to observe in real time the creation of an electronic wavepacket and subsequent electronic motion in a…

原子与分子团簇 · 物理学 2015-06-22 Aurelie Perveaux , David Lauvergnat , Fabien Gatti , Gabor Halasz , Agnes Vibok , Benjamin Lasorne

The electron motion in atoms and molecules is at the heart of all phenomena in nature that occur outside the nucleus. Recently, ultrafast electron and X-ray imaging tools have been developed to image the ultrafast dynamics of matter in real…

Tracking the coupled motion of electrons and nuclei on their intrinsic timescales is essential to understanding and controlling photochemical transformations. While attosecond techniques have provided unprecedented insight into electronic…

Time-resolved investigations of ultrafast electronic and molecular dynamics were not possible until recently. The typical time scale of these processes is in the picosecond to attosecond realm. The tremendous technological progress in…

原子物理 · 物理学 2013-05-14 Stefan Pabst

Recently we reported a series of numerical simulations proving that it is possible in principle to create an electronic wave packet and subsequent electronic motion in a neutral molecule photoexcited by a UV pump pulse within a few…

原子与分子团簇 · 物理学 2016-10-24 P. Decleva , N. Quadri , A. Perveaux , D. Lauvergnat , F. Gatti , B. Lasorne , G. J. Halász , Á. Vibók

We explore stimulated photo-association in the context of attosecond pump-probe schemes of atomic matter. An attosecond pulse -- the probe -- is used to induce photo-association of an electronic wave packet which had been created before,…

原子物理 · 物理学 2009-11-13 Paula Rivière , Camilo Ruiz , Jan-Michael Rost

We report attosecond-scale probing of the laser-induced dynamics in molecules. We apply the method of high-harmonic spectroscopy, where laser-driven recolliding electrons on various trajec- tories record the motion of their parent ion.…

We present a time-dependent density-functional method able to describe the photoelectron spectrum of atoms and molecules when excited by laser pulses. This computationally feasible scheme is based on a geometrical partitioning that…

原子物理 · 物理学 2012-06-28 U. De Giovannini , D. Varsano , M. A. L. Marques , H. Appel , E. K. U. Gross , A. Rubio

Attosecond science has been transforming our understanding of electron dynamics in atoms, molecules and solids. However, to date almost all of the attoscience experiments have been based on spectroscopic measurements because attosecond…

Electrons photoemitted by extreme ultraviolet attosecond pulses derive spatially from the first few atomic surface layers and energetically from the valence band and highest atomic orbitals. As a result, it is possible to probe the emission…

Frontier orbitals, i.e., the highest occupied and lowest unoccupied orbitals of a molecule, generally determine molecular properties, such as chemical bonding and reactivities. Consequently, there has been a lot of interest in measuring…

Tracing ultrafast processes induced by interaction of light with matter is often very challenging. In molecular systems, the initially created electronic coherence becomes damped by the slow nuclear rearrangement on a femtosecond timescale…

化学物理 · 物理学 2021-09-20 Nikolay V. Golubev , Jiří Vaníček , Alexander I. Kuleff

The route towards manipulation of the optoelectronic properties of matter beyond the current limits of electronics starts from a comprehensive study of the ultrafast dynamics triggered by interaction with light. Among them, a fundamental…

We show that the complete photoemission dynamics in situations of electron-ion entanglement can be retrieved from photoelectron spectral measurements without information on the ion. To this end, we develop an energy-time analysis of the…

High harmonic light sources make it possible to access attosecond time-scales, thus opening up the prospect of manipulating electronic wave packets for steering molecular dynamics. However, two decades after the birth of attosecond physics,…

Attosecond laser pulses open the door to resolve microscopic electron dynamics in time. Experiments performed include the decay of a core hole, the time-resolved measurement of photo ionization and electron tunneling. The processes…

原子与分子团簇 · 物理学 2011-11-09 Ionut Georgescu , Ulf Saalmann , Jan M. Rost
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