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The introduction of femto-chemistry has made it a primary goal to follow the nuclear and electronic evolution of a molecule in time and space as it undergoes a chemical reaction. Using Coulomb Explosion Imaging we have shot the first…

Among polycyclic aromatic hydrocarbons, pyrene is widely used as an optical probe thanks to peculiar ultraviolet absorption and infrared emission features. Interestingly, this molecule is also an abundant component of the interstellar…

Chemical Physics · Physics 2021-11-19 Katherine R. Herperger , Jannis Krumland , Caterina Cocchi

Attosecond pulses can be used to initiate and control electron dynamics on a sub-femtosecond time scale. The first step in this process occurs when an atom absorbs an ultraviolet photon leading to the formation of an attosecond electron…

Atomic Physics · Physics 2007-12-11 P. Johnsson , J. Mauritsson , T. Remetter , A. LHuillier , K. J. Schafer

Charge migration is the electronic response that immediately follows localized ionization or excitation in a molecule, before the nuclei have time to move. It typically unfolds on sub-femtosecond time scales and most often corresponds to…

Atomic and Molecular Clusters · Physics 2022-03-07 Francois Mauger , Aderonke Folorunso , Kyle Hamer , Cristel Chandre , Mette Gaarde , Kenneth Lopata , Kenneth Schafer

The present review addresses the technical advances and the theoretical developments to realize and rationalize attosecond-science experiments that reveal a new dynamical time scale ($10^{-15}$-$10^{-18}$ s), with a particular emphasis on…

Chemical Physics · Physics 2020-02-07 Denitsa Baykusheva , Hans Jakob Wörner

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

A nonadiabatic scheme for the description of the coupled electron and nuclear motions in the ozone molecule was proposed recently. An initial coherent nonstationary state was prepared as a superposition of the ground state and the excited…

Atomic and Molecular Clusters · Physics 2015-06-18 A. Perveaux , D. Lauvergnat , B. Lasorne , F. Gatti , M. A. Robb , G. J. Halász , Á. Vibók

Photoelectron spectroscopy is a powerful method that provides insight into the quantum mechanical properties of a wide range of systems. The ionized electron wavefunction carries information on the structure of the bound orbital, the ionic…

We illustrate how attosecond light pulses can be used to directly mapping out the time-dependence of the correlated motion of two excited atomic electrons, discuss how the two-electron correlations manifest themselves in realistic…

Atomic Physics · Physics 2007-05-23 Toru Morishita , Shinichi Watanabe , C. D. Lin

Imaging the quantum motion of electrons not only in real-time, but also in real-space is essential to understand for example bond breaking and formation in molecules, and charge migration in peptides and biological systems. Time-resolved…

Atomic Physics · Physics 2012-07-20 Gopal Dixit , Oriol Vendrell , Robin Santra

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 investigate the characteristic effects of nuclear motion on attosecond transient absorption spectra in molecules by calculating the spectrum for different model systems. Two models of the hydrogen molecular ion are considered: one where…

Atomic Physics · Physics 2015-04-16 Jens E. Bækhøj , Lun Yue , Lars Bojer Madsen

The motion of electrons in or near solids, liquids and gases can be tracked by forcing their ejection with attosecond x-ray pulses, derived from femtosecond lasers. The momentum of these emitted electrons carries the imprint of the…

Mesoscale and Nanoscale Physics · Physics 2017-06-14 C. W. Barlow-Myers , N. J. Pine , W. A. Bryan

The coupling of light to electrical charge carriers in semiconductors is the foundation of many technological applications. Attosecond transient absorption spectroscopy measures simultaneously how excited electrons and the vacancies they…

Materials Science · Physics 2023-05-03 Z. Schumacher , S. A. Sato , S. Neb , A. Niedermayr , L. Gallmann , A. Rubio , U. Keller

In ultrafast experiments with gas phase molecules, the alignment of the molecular axis relative to the polarization of the interacting laser pulses plays a crucial role in determining the dynamics following this light-matter interaction.…

Chemical Physics · Physics 2025-04-14 Shashank Kumar , Eric Liu , Liang Z. Tan , Varun Makhija , Niranjan Shivaram

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…

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…

Tracing the motion of electrons has enormous relevance to understanding ubiquitous phenomena in ultrafast science, such as the dynamical evolution of the electron density during complex chemical and biological processes. Scattering of…

Atomic Physics · Physics 2013-03-28 Gopal Dixit , Jan Malte Slowik , Robin Santra

Attosecond science is based on steering of electrons with the electric field of well-controlled femtosecond laser pulses. It has led to, for example, the generation of XUV light pulses with a duration in the sub-100-attosecond regime, to…

Quantum Physics · Physics 2011-07-11 Michael Krüger , Markus Schenk , Peter Hommelhoff

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