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Controlling laser-dressed resonance line shape using attosecond extreme-ultraviolet pulse with a spectral minimum.
Proc Natl Acad Sci U S A
January 2024
Department of Applied Physics, Nanjing University of Science and Technology, Nanjing, Jiangsu 210094, China.
High-harmonic generation from a gas target exhibits sharp spectral features and rapid phase variation near the Cooper minimum. By applying spectral filtering, shaped isolated attosecond pulses can be generated where the pulse is split into two in the time domain. Using such shaped extreme-ultraviolet (XUV) pulses, we theoretically study attosecond transient absorption (ATA) spectra of helium [Formula: see text] autoionizing state which is resonantly coupled to the [Formula: see text] dark state by a time-delayed infrared laser.
View Article and Find Full Text PDFAttosecond photoionization delays in the vicinity of molecular Feshbach resonances.
Sci Adv
April 2023
Departamento de Química, Módulo 13, Universidad Autónoma de Madrid, 28049 Madrid, Spain.
Temporal delays extracted from photoionization phases are currently determined with attosecond resolution by using interferometric methods. Such methods require special care when photoionization occurs near Feshbach resonances due to the interference between direct ionization and autoionization. Although theory can accurately handle these interferences in atoms, in molecules, it has to face an additional, so far insurmountable problem: Autoionization is slow, and nuclei move substantially while it happens, i.
View Article and Find Full Text PDFPhotoionization of the water molecule with XCHEM.
J Chem Phys
April 2023
Departamento de Química, Facultad de Ciencias, Universidad Autónoma de Madrid, Madrid, Spain.
We have evaluated total and partial photoionization cross sections, β asymmetry parameters, and molecular frame photoelectron angular distributions (MFPADs) of the water molecule by using the XCHEM methodology. This method accounts for electron correlation in the electronic continuum, which is crucial to describe Feshbach resonances and their autoionization decay. We have identified a large number of Feshbach resonances, some of them previously unknown, in the region between 12.
View Article and Find Full Text PDFExtreme Ultraviolet Wave Packet Interferometry of the Autoionizing HeNe Dimer.
J Phys Chem Lett
September 2022
Institute of Physics, University of Freiburg, Hermann-Herder-Str. 3, 79104 Freiburg, Germany.
Femtosecond extreme ultraviolet wave packet interferometry (XUV-WPI) was applied to study resonant interatomic Coulombic decay (ICD) in the HeNe dimer. The high demands on phase stability and sensitivity for vibronic XUV-WPI of molecular-beam targets are met using an XUV phase-cycling scheme. The detected quantum interferences exhibit vibronic dephasing and rephasing signatures along with an ultrafast decoherence assigned to the ICD process.
View Article and Find Full Text PDFRaman Interferometry between Autoionizing States to Probe Ultrafast Wave-Packet Dynamics with High Spectral Resolution.
Phys Rev Lett
February 2022
Department of Physics, University of Arizona, Tucson, Arizona 85721, USA.
Photoelectron interferometry with femtosecond and attosecond light pulses is a powerful probe of the fast electron wave-packet dynamics, albeit it has practical limitations on the energy resolution. We show that one can simultaneously obtain both high temporal and spectral resolution by stimulating Raman interferences with one light pulse and monitoring the modification of the electron yield in a separate step. Applying this spectroscopic approach to the autoionizing states of argon, we experimentally resolved its electronic composition and time evolution in exquisite detail.
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