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New free-electron laser and high-harmonic generation X-ray light sources are capable of supplying pulses short and intense enough to perform resonant nonlinear time-resolved experiments in molecules. Valence-electron motions can be triggered impulsively by core excitations and monitored with high temporal and spatial resolution. We discuss possible experiments that employ attosecond X-ray pulses to probe the quantum coherence and correlations of valence electrons and holes, rather than the charge density alone, building on the analogy with existing studies of vibrational motions using femtosecond techniques in the visible regime.
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http://dx.doi.org/10.1146/annurev-physchem-040412-110021 | DOI Listing |
Sci Rep
January 2025
Instituto de Quimica, Universidad Nacional Autonoma de Mexico,Circuito Exterior, Ciudad Universitaria, Alcaldía Coyoacàn C.P., 04510, Mexico City, Mexico.
There is a growing interest in reconstructing the density matrix of photoelectron wavepackets, in particular in complex systems where decoherence can be introduced either by a partial measurement of the system or through coupling with a stochastic environment. To this end, several methods to reconstruct the density matrix, quantum state tomography protocols, have been developed and tested on photoelectrons ejected from noble gases following absorption of extreme ultraviolet (XUV) photons from attosecond pulses. It remains a challenge to obtain model-free, single scan protocols that can reconstruct the density matrix with high fidelities.
View Article and Find Full Text PDFPhys Rev E
June 2024
State Key Laboratory of Nuclear Physics and Technology, and Key Laboratory of HEDP of the Ministry of Education, CAPT, School of Physics, Peking University, Beijing 100871, China.
Collision between relativistic electron sheets and counterpropagating laser pulses is recognized as a promising way to produce intense attosecond x rays through coherent Thomson backscattering (TBS). In a double-layer scheme, the electrons in an ultrathin solid foil are first pushed out by an intense laser driver and then interact with the laser reflected off a second foil to form a high-density relativistic electron sheet with vanishing transverse momentum. However, the repulsion between these concentrated electrons can increase the thickness of the layer, reducing both its density and subsequently the coherent TBS.
View Article and Find Full Text PDFLight Sci Appl
August 2023
School of Optical and Electronic Information and Wuhan National Laboratory for Optoelectronics, Huazhong University of Science and Technology, Wuhan, 430074, China.
Femtosecond vortex beams are of great scientific and practical interest because of their unique phase properties in both the longitudinal and transverse modes, enabling multi-dimensional quantum control of light fields. Until now, generating femtosecond vortex beams for applications that simultaneously require ultrashort pulse duration, high power, high vortex order, and a low cost and compact laser source has been very challenging due to the limitations of available generation methods. Here, we present a compact apparatus that generates powerful high-order femtosecond vortex pulses via astigmatic mode conversion from a mode-locked Hermite-Gaussian Yb:KGW laser oscillator in a hybrid scheme using both the translation-based off-axis pumping and the angle-based non-collinear pumping techniques.
View Article and Find Full Text PDFFew-cycle, long-wavelength sources for generating isolated attosecond soft x ray pulses typically rely upon complex laser architectures. Here, we demonstrate a comparatively simple setup for generating sub-two-cycle pulses in the short-wave infrared based on multidimensional solitary states in an NO-filled hollow-core fiber and a two-channel light-field synthesizer. Due to the temporal phase imprinted by the rotational nonlinearity of the molecular gas, the redshifted (from 1.
View Article and Find Full Text PDFNon-linear processes such as four-wave-mixing have become instrumental in attosecond EUV spectroscopy. Using EUV high harmonics in conjunction with collinear near-infrared and mid-infrared fields, we extended this approach to high-order-mixing between three colors. Specifically, we find that atomic resonances in neon exhibit a significant cross section for six-wave mixing.
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