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Title: Quantum state-resolved probing of strong-field-ionized xenon atoms using femtosecond high-order harmonic transient absorption spectroscopy.

Abstract

Femtosecond high-order harmonic transient absorption spectroscopy is used to resolve the complete |j,m{r_angle} quantum state distribution of Xe{sup +} produced by optical strong-field ionization of Xe atoms at 800 nm. Probing at the Xe N4/5 edge yields a population distribution {rho}j,|m| of {rho}3/2,1/2:{rho}1/2,1/2:{rho}3/2,3/2=75{+-}6 :12{+-}3 :13{+-}6%. The result is compared to a tunnel ionization calculation with the inclusion of spin-orbit coupling, revealing nonadiabatic ionization behavior. The sub-50-fs time resolution paves the way for tabletop extreme ultraviolet absorption probing of ultrafast dynamics.

Authors:
; ; ; ; ; ; ; ;
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC); National Science Foundation (NSF); Feodor Lynen Research Fellowship
OSTI Identifier:
914941
Report Number(s):
ANL/CHM/JA-58489
Journal ID: ISSN 0031-9007; PRLTAO; TRN: US200817%%24
DOE Contract Number:
DE-AC02-06CH11357
Resource Type:
Journal Article
Resource Relation:
Journal Name: Phys. Rev. Lett.; Journal Volume: 98; Journal Issue: Apr. 6, 2007
Country of Publication:
United States
Language:
ENGLISH
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; ABSORPTION SPECTROSCOPY; ATOMS; DISTRIBUTION; HARMONICS; IONIZATION; TIME RESOLUTION; XENON; XENON IONS; PROBES

Citation Formats

Loh, Z.-H., Khalil, M., Correa, R. E., Santra, R., Buth, C., Leone, S. R., Chemistry, Univ. of California, and LBNL. Quantum state-resolved probing of strong-field-ionized xenon atoms using femtosecond high-order harmonic transient absorption spectroscopy.. United States: N. p., 2007. Web. doi:10.1103/PhysRevLett.98.143601.
Loh, Z.-H., Khalil, M., Correa, R. E., Santra, R., Buth, C., Leone, S. R., Chemistry, Univ. of California, & LBNL. Quantum state-resolved probing of strong-field-ionized xenon atoms using femtosecond high-order harmonic transient absorption spectroscopy.. United States. doi:10.1103/PhysRevLett.98.143601.
Loh, Z.-H., Khalil, M., Correa, R. E., Santra, R., Buth, C., Leone, S. R., Chemistry, Univ. of California, and LBNL. Fri . "Quantum state-resolved probing of strong-field-ionized xenon atoms using femtosecond high-order harmonic transient absorption spectroscopy.". United States. doi:10.1103/PhysRevLett.98.143601.
@article{osti_914941,
title = {Quantum state-resolved probing of strong-field-ionized xenon atoms using femtosecond high-order harmonic transient absorption spectroscopy.},
author = {Loh, Z.-H. and Khalil, M. and Correa, R. E. and Santra, R. and Buth, C. and Leone, S. R. and Chemistry and Univ. of California and LBNL},
abstractNote = {Femtosecond high-order harmonic transient absorption spectroscopy is used to resolve the complete |j,m{r_angle} quantum state distribution of Xe{sup +} produced by optical strong-field ionization of Xe atoms at 800 nm. Probing at the Xe N4/5 edge yields a population distribution {rho}j,|m| of {rho}3/2,1/2:{rho}1/2,1/2:{rho}3/2,3/2=75{+-}6 :12{+-}3 :13{+-}6%. The result is compared to a tunnel ionization calculation with the inclusion of spin-orbit coupling, revealing nonadiabatic ionization behavior. The sub-50-fs time resolution paves the way for tabletop extreme ultraviolet absorption probing of ultrafast dynamics.},
doi = {10.1103/PhysRevLett.98.143601},
journal = {Phys. Rev. Lett.},
number = Apr. 6, 2007,
volume = 98,
place = {United States},
year = {Fri Apr 06 00:00:00 EDT 2007},
month = {Fri Apr 06 00:00:00 EDT 2007}
}
  • Femtosecond high-order harmonic transient absorption spectroscopy is used to resolve the complete vertical bar j,m> quantum state distribution of Xe{sup +} produced by optical strong-field ionization of Xe atoms at 800 nm. Probing at the Xe N{sub 4/5} edge yields a population distribution {rho}{sub j,vertic}a{sub lbarmverticalbar} of {rho}{sub 3/2,1/2} ratio {rho}{sub 1/2,1/2} ratio {rho}{sub 3/2,3/2}=75{+-}6 :12{+-}3 :13{+-}6%. The result is compared to a tunnel ionization calculation with the inclusion of spin-orbit coupling, revealing nonadiabatic ionization behavior. The sub-50-fs time resolution paves the way for tabletop extreme ultraviolet absorption probing of ultrafast dynamics.
  • The fundamental mechanism responsible for optically induced magnetization dynamics in ferromagnetic thin films has been under intense debate since almost two decades. Currently, numerous competing theoretical models are in strong need for a decisive experimental confirmation such as monitoring the triggered changes in the spin-dependent band structure on ultrashort time scales. Our approach explores the possibility of observing femtosecond band structure dynamics by giving access to extended parts of the Brillouin zone in a simultaneously time-, energy- and spin-resolved photoemission experiment. For this purpose, our setup uses a state-of-the-art, highly efficient spin detector and ultrashort, extreme ultraviolet light pulses createdmore » by laser-based high-order harmonic generation. In this paper, we present the setup and first spin-resolved spectra obtained with our experiment within an acquisition time short enough to allow pump-probe studies. Further, we characterize the influence of the excitation with femtosecond extreme ultraviolet pulses by comparing the results with data acquired using a continuous wave light source with similar photon energy. In addition, changes in the spectra induced by vacuum space-charge effects due to both the extreme ultraviolet probe- and near-infrared pump-pulses are studied by analyzing the resulting spectral distortions. The combination of energy resolution and electron count rate achieved in our setup confirms its suitability for spin-resolved studies of the band structure on ultrashort time scales.« less
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  • A laser-based tabletop approach to femtosecond time-resolved photoelectron spectroscopy with photons in the vacuum-ultraviolet (VUV) energy range is described. The femtosecond VUV pulses are produced by high-order harmonic generation (HHG) of an amplified femtosecond Ti:sapphire laser system. Two generations of the same setup and results from photoelectron spectroscopy in the gas phase are discussed. In both generations, a toroidal grating monochromator was used to select one harmonic in the photon energy range of 20-30 eV. The first generation of the setup was used to perform photoelectron spectroscopy in the gas phase to determine the bandwidth of the source. We findmore » that our HHG source has a bandwidth of 140 {+-} 40 meV. The second and current generation is optimized for femtosecond pump-probe photoelectron spectroscopy with high flux and a small spot size at the sample of the femtosecond probe pulses. The VUV radiation is focused into the interaction region with a toroidal mirror to a spot smaller than 100 x 100 {mu}m{sup 2} and the flux amounts to 10{sup 10} photons/s at the sample at a repetition rate of 1 kHz. The duration of the monochromatized VUV pulses is determined to be 120 fs resulting in an overall pump-probe time resolution of 135 {+-} 5 fs. We show how this setup can be used to map the transient valence electronic structure in molecular dissociation.« less