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The basic properties of atoms, molecules and solids are governed by electron dynamics which take place on extremely short time scales. To measure and control these dynamics therefore requires ultrafast sources of radiation combined with…

Atomic Physics · Physics 2008-02-27 J. Mauritsson , P. Johnsson , E. Gustafsson , M. Swoboda , T. Ruchon , A. LHuillier , K. J. Schafer

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…

Chemical Physics · Physics 2017-05-18 David Ayuso

We explore long lived electronic coherences in molecules using shaped ultrafast laser pulses to launch and probe entangled nuclear-electronic wave packets. We find that under certain conditions, the electronic phase remains well defined…

Quantum Physics · Physics 2023-11-20 Brian Kaufman , Philipp Marquetand , Tamas Rozgonyi , Thomas Weinacht

Streaking of photoelectrons has long been used for the temporal characterization of attosecond extreme ultraviolet pulses. When the time-resolved photoelectrons originate from a coherent superposition of electronic states, they carry an…

Chemical Physics · Physics 2016-07-27 Markus Kowalewski , Kochise Bennett , Jérémy R. Rouxel , Shaul Mukamel

The coupling of electronic and nuclear motion in polyatomic molecules is at the heart of attochemistry. The molecular properties, transient structures and reaction mechanism of these many-body quantum objects are defined on the level of…

Chemical Physics · Physics 2024-03-12 David Schwickert , Andreas Przystawik , Dian Diaman , Detlef Kip , Jon P. Marangos , Tim Laarmann

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,…

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…

Atomic and Molecular Clusters · Physics 2015-06-22 Aurelie Perveaux , David Lauvergnat , Fabien Gatti , Gabor Halasz , Agnes Vibok , Benjamin Lasorne

We introduce and experimentally demonstrate a method, where the two intrinsic time scales of a molecule, the slow nuclear motion and the fast electronic motion, are simultaneously measured in a photo-electron photo-ion coincidence…

Exposing a molecule to intense light pulses may bring this molecule to a nonstationary quantum state, thus launching correlated dynamics of electronic and nuclear subsystems. Although much had been achieved in the understanding of…

Chemical Physics · Physics 2024-04-11 Nikolay V. Golubev , Jiří Vaníček

We explore the novel capabilities offered by attosecond extreme ultraviolet and x-ray pulses that can be now generated by free-electron lasers and high-harmonics generation sources for probing photon-induced electron dynamics in molecules.…

Quantum Physics · Physics 2023-02-15 Marvin Reuner , Daria Popova-Gorelova

We propose a protocol to probe the ultrafast evolution and dephasing of coherent electronic excitation in molecules in the time domain by the intrinsic streaking field generated by the molecule itself. Coherent electronic motion in the…

Short-in-time, broad-in-energy attosecond or few-femtosecond pulses can excite coherent superpositions of several electronic states in molecules. This results in ultrafast charge oscillations known as charge migration. A key open question…

Chemical Physics · Physics 2025-09-12 Lina Fransén , Sandra Gomez , Morgane Vacher

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…

Atomic and Molecular Clusters · Physics 2016-10-24 P. Decleva , N. Quadri , A. Perveaux , D. Lauvergnat , F. Gatti , B. Lasorne , G. J. Halász , Á. Vibók

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…

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…

Optics · Physics 2018-12-11 Daria Popova-Gorelova , Jochen Küpper , Robin Santra

We introduce and demonstrate a new approach to measuring coherent electron wave packets using high-harmonic spectroscopy. By preparing a molecule in a coherent superposition of electronic states, we show that electronic coherence opens…

Chemical Physics · Physics 2014-07-09 P. M. Kraus , S. B. Zhang , A. Gijsbertsen , R. R. Lucchese , N. Rohringer , H. J. Wörner

Quantum coherence between electronic states of a photoionized molecule and the resulting process of ultrafast electron-hole migration have been put forward as a possible quantum mechanism of charge-directed reactivity governing the…

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…

Atomic Physics · Physics 2013-05-14 Stefan Pabst

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.…

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