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Title: Attosecond transient absorption of argon atoms in the vacuum ultraviolet region: line energy shifts versus coherent population transfer

Abstract

Using attosecond transient absorption, the dipole response of an argon atom in the vacuum ultraviolet (VUV) region is studied when an external electromagnetic field is present. An isolated attosecond VUV pulse populates Rydberg states lying 15 eV above the argon ground state. A synchronized few-cycle near infrared (NIR) pulse modifies the oscillating dipoles of argon impulsively, leading to alterations in the VUV absorption spectra. As the NIR pulse is delayed with respect to the VUV pulse, multiple features in the absorption profile emerge simultaneously including line broadening, sideband structure, sub-cycle fast modulations, and 5-10 fs slow modulations. These features indicate the coexistence of two general processes of the light-matter interaction: the energy shift of individual atomic levels and coherent population transfer between atomic eigenstates, revealing coherent superpositions. Finally, an intuitive formula is derived to treat both effects in a unifying framework, allowing one to identify and quantify the two processes in a single absorption spectrogram.

Authors:
 [1];  [2];  [2];  [1]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division; Univ. of California, Berkeley, CA (United States). Dept. of Chemistry; Univ. of California, Berkeley, CA (United States). Dept. of Physics
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division; Univ. of California, Berkeley, CA (United States). Dept. of Chemistry
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1415950
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
New Journal of Physics
Additional Journal Information:
Journal Volume: 18; Journal Issue: 1; Journal ID: ISSN 1367-2630
Publisher:
IOP Publishing
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; attosecond transient absorption; population transfer; Stark shift; Rydberg states

Citation Formats

Cao, Wei, Warrick, Erika R., Neumark, Daniel M., and Leone, Stephen R. Attosecond transient absorption of argon atoms in the vacuum ultraviolet region: line energy shifts versus coherent population transfer. United States: N. p., 2016. Web. doi:10.1088/1367-2630/18/1/013041.
Cao, Wei, Warrick, Erika R., Neumark, Daniel M., & Leone, Stephen R. Attosecond transient absorption of argon atoms in the vacuum ultraviolet region: line energy shifts versus coherent population transfer. United States. doi:10.1088/1367-2630/18/1/013041.
Cao, Wei, Warrick, Erika R., Neumark, Daniel M., and Leone, Stephen R. Mon . "Attosecond transient absorption of argon atoms in the vacuum ultraviolet region: line energy shifts versus coherent population transfer". United States. doi:10.1088/1367-2630/18/1/013041. https://www.osti.gov/servlets/purl/1415950.
@article{osti_1415950,
title = {Attosecond transient absorption of argon atoms in the vacuum ultraviolet region: line energy shifts versus coherent population transfer},
author = {Cao, Wei and Warrick, Erika R. and Neumark, Daniel M. and Leone, Stephen R.},
abstractNote = {Using attosecond transient absorption, the dipole response of an argon atom in the vacuum ultraviolet (VUV) region is studied when an external electromagnetic field is present. An isolated attosecond VUV pulse populates Rydberg states lying 15 eV above the argon ground state. A synchronized few-cycle near infrared (NIR) pulse modifies the oscillating dipoles of argon impulsively, leading to alterations in the VUV absorption spectra. As the NIR pulse is delayed with respect to the VUV pulse, multiple features in the absorption profile emerge simultaneously including line broadening, sideband structure, sub-cycle fast modulations, and 5-10 fs slow modulations. These features indicate the coexistence of two general processes of the light-matter interaction: the energy shift of individual atomic levels and coherent population transfer between atomic eigenstates, revealing coherent superpositions. Finally, an intuitive formula is derived to treat both effects in a unifying framework, allowing one to identify and quantify the two processes in a single absorption spectrogram.},
doi = {10.1088/1367-2630/18/1/013041},
journal = {New Journal of Physics},
number = 1,
volume = 18,
place = {United States},
year = {2016},
month = {1}
}

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Cited by: 14 works
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    Works referencing / citing this record:

    Analytical Theory of Attosecond Transient Absorption Spectroscopy of Perturbatively Dressed Systems
    journal, March 2019

    • Kolbasova, Daria; Santra, Robin
    • Applied Sciences, Vol. 9, Issue 7
    • DOI: 10.3390/app9071350