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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…

化学物理 · 物理学 2014-07-09 P. M. Kraus , S. B. Zhang , A. Gijsbertsen , R. R. Lucchese , N. Rohringer , H. J. Wörner

We obtain continuum molecular wavefunctions for open-shell molecules in the Hartree-Fock framework. We do so while accounting for the singlet or triplet total spin symmetry of the molecular ion, that is, of the open-shell orbital and the…

原子物理 · 物理学 2023-07-04 M. E. Mountney , T. C. Driver , A. Marinelli , M. F. Kling , J. P. Cryan , A. Emmanouilidou

Photoelectron spectroscopy in intense laser fields has proven to be a powerful tool for providing detailed insights into molecular structure. The ionizing molecular orbital, however, has not been reconstructed from the photoelectron…

原子物理 · 物理学 2023-04-14 XuanYang Lai , RenPing Sun , ShaoGang Yu , YanLan Wang , Wei Quan , André Staudte , XiaoJun Liu

We present momentum resolved covariance measurements of entangled electronic-nuclear wave packets created and probed with octave spanning phaselocked ultrafast pulses. We launch vibrational wave packets on multiple electronic states via…

量子物理 · 物理学 2023-11-20 Gonenc Mogol , Brian Kaufman , Chuan Cheng , Itzik Ben-Itzhak , Thomas Weinacht

In recent years, ultrafast pump-probe spectroscopy has provided insightful information about nonequilibrium dynamics of excitations in materials. In a typical experiment of time-resolved x-ray absorption spectroscopy, the systems are…

强关联电子 · 物理学 2019-05-29 Chen-Yen Lai , Jian-Xin Zhu

State-of-the-art attosecond metrology deals with the detection and characterization of photon pulses with typical energies up to the hundreds of eV and time resolution of several tens of attoseconds. Such short pulses are used for example…

仪器与探测器 · 物理学 2015-06-04 Andreas Ipp , Jörg Evers , Christoph H. Keitel , Karen Z. Hatsagortsyan

Quantum coherence in quantum optics is an essential part of optical information processing and light manipulation. Alkali metal vapors, despite the numerous shortcomings, are traditionally used in quantum optics as a working medium due to…

The screening of a 2p core-hole in Na clusters is investigated using density functional theory applied to an extended jellium model with an all-electron atom in the center. The study is related to recent experiments at the free electron…

原子与分子团簇 · 物理学 2017-11-21 D. Bauer

A theoretical comparison of the electronic excitation and ionisation behaviour of molecular hydrogen oriented either parallel or perpendicular to a linear polarised laser pulse is performed. The investigation is based on a non-perturbative…

量子物理 · 物理学 2009-11-13 Yulian V. Vanne , Alejandro Saenz

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…

原子物理 · 物理学 2014-04-17 Antonia Karamatskou , Stefan Pabst , Yi-Jen Chen , Robin Santra

The pump-probe experiments enabled by X-ray free-electron lasers (XFEL) will allow us to directly observe correlated electronic motion with attosecond time resolution by detecting photoelectron pairs in coincidence. In helium, the…

In time-resolved photoemission experiments, more than one electron can be emitted from the solid by a single ultra-short pulse. We theoretically demonstrate how correlations between the momenta of outgoing electrons relate to time-dependent…

强关联电子 · 物理学 2019-06-26 Christopher Stahl , Martin Eckstein

Photoelectron interferometry with femto- and atto-second light pulses is a powerful probe of the fast electron wavepacket dynamics, albeit it has practical limitations on the energy resolution. We show that one can simultaneously obtain…

原子物理 · 物理学 2022-02-24 A. Plunkett , M. A. Alarcon , J. K. Wood , C. H. Greene , A. Sandhu

By analyzing ``exact'' theoretical results from solving the time-dependent Schr\"odinger equation of atoms in few-cycle laser pulses, we established the general conclusion that differential elastic scattering and photo-recombination cross…

原子物理 · 物理学 2008-04-04 Toru Morishita , Anh-Thu Le , Zhangjin Chen , C. D. Lin

Measuring and controlling the ionization dynamics by intense laser fields has recently led to important breakthroughs, from the investigation of tunneling time delays to attosecond molecular imaging by electron holography. In these…

We photoionize nitrogen molecules with a train of extreme ultraviolet attosecond pulses together with a weak infrared field. We measure the phase of the two-color two-photon ionization transition (molecular phase) for different states of…

The evolution of electron wavepackets determines the course of many physical and chemical phenomena and attosecond spectroscopy aims to measure and control such dynamics in real-time. Here, we investigate radial electron wavepacket motion…

原子物理 · 物理学 2015-09-04 Niranjan Shivaram , Xiao-Min Tong , Henry Timmers , Arvinder Sandhu

We analyze the photoelectron angular distribution in two-pathway interference between non\-resonant one-photon and resonant two-photon ionization of neon. We consider a bichromatic femtosecond XUV pulse whose fundamental frequency is tuned…

Nonstationary molecular states which contain electronic coherences can be impulsively created and manipulated by using recently-developed ultrashort optical and X-ray pulses via photoexcitation, photoionization and Auger processes. We…

化学物理 · 物理学 2015-09-02 Konstantin E. Dorfman , Kochise Bennett , Shaul Mukamel

We present a novel theory and implementation for computing coupled electronic and quantal nuclear subsystems on a single potential energy surface, moving beyond the standard Born-Oppenheimer (BO) separation of nuclei and electrons. We…

化学物理 · 物理学 2021-11-15 Ziyong Chen , Jun Yang