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Title: Multidimensional spectroscopy with attosecond extreme ultraviolet and shaped near-infrared pulses

Abstract

Dynamics following excitation with attosecond extreme ultraviolet (XUV) pulses arise from enormous numbers of accessible excited states, complicating the retrieval of state-specific time evolutions. We develop attosecond XUV multidimensional spectroscopy here to separate interfering pathways on a near-infrared (NIR) energy axis, retrieving single state dynamics in argon atoms in a two-dimensional (2D) XUV-NIR spectrum. In this experiment, we measure four-wave mixing signal arising from the interaction of XUV attosecond pulses centered around 15 eV with two few-cycle NIR pulses. The 2D spectrum is created by measuring the emitted XUV signal field spectrum while applying narrowband amplitude and phase modulations to one of the NIR pulses. Application of such a technique to systems of high dimensionality will provide for the observation of state-resolved pure electronic dynamics, in direct analogy to phenomena unraveled by multidimensional spectroscopies at optical frequencies.

Authors:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [2]
  1. Univ. of California, Berkeley, CA (United States). Dept. of Chemistry; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division
  2. Univ. of California, Berkeley, CA (United States). Dept. of Chemistry, and Dept. of Physics; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division
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). Chemical Sciences, Geosciences & Biosciences Division
OSTI Identifier:
1506366
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Science Advances
Additional Journal Information:
Journal Volume: 4; Journal Issue: 9; Journal ID: ISSN 2375-2548
Publisher:
AAAS
Country of Publication:
United States
Language:
English
Subject:
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS

Citation Formats

Marroux, Hugo J. B., Fidler, Ashley P., Neumark, Daniel M., and Leone, Stephen R. Multidimensional spectroscopy with attosecond extreme ultraviolet and shaped near-infrared pulses. United States: N. p., 2018. Web. doi:10.1126/sciadv.aau3783.
Marroux, Hugo J. B., Fidler, Ashley P., Neumark, Daniel M., & Leone, Stephen R. Multidimensional spectroscopy with attosecond extreme ultraviolet and shaped near-infrared pulses. United States. doi:10.1126/sciadv.aau3783.
Marroux, Hugo J. B., Fidler, Ashley P., Neumark, Daniel M., and Leone, Stephen R. Fri . "Multidimensional spectroscopy with attosecond extreme ultraviolet and shaped near-infrared pulses". United States. doi:10.1126/sciadv.aau3783. https://www.osti.gov/servlets/purl/1506366.
@article{osti_1506366,
title = {Multidimensional spectroscopy with attosecond extreme ultraviolet and shaped near-infrared pulses},
author = {Marroux, Hugo J. B. and Fidler, Ashley P. and Neumark, Daniel M. and Leone, Stephen R.},
abstractNote = {Dynamics following excitation with attosecond extreme ultraviolet (XUV) pulses arise from enormous numbers of accessible excited states, complicating the retrieval of state-specific time evolutions. We develop attosecond XUV multidimensional spectroscopy here to separate interfering pathways on a near-infrared (NIR) energy axis, retrieving single state dynamics in argon atoms in a two-dimensional (2D) XUV-NIR spectrum. In this experiment, we measure four-wave mixing signal arising from the interaction of XUV attosecond pulses centered around 15 eV with two few-cycle NIR pulses. The 2D spectrum is created by measuring the emitted XUV signal field spectrum while applying narrowband amplitude and phase modulations to one of the NIR pulses. Application of such a technique to systems of high dimensionality will provide for the observation of state-resolved pure electronic dynamics, in direct analogy to phenomena unraveled by multidimensional spectroscopies at optical frequencies.},
doi = {10.1126/sciadv.aau3783},
journal = {Science Advances},
issn = {2375-2548},
number = 9,
volume = 4,
place = {United States},
year = {2018},
month = {9}
}

Journal Article:
Free Publicly Available Full Text
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Cited by: 2 works
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Figures / Tables:

Fig. 1 Fig. 1: Experiment description. (A) Experiment design. In the non-multidimensional experiment, the pulse shaper is bypassed. (B) Geometry and timing diagram used over the course of the study. (C) Energy diagram. The shaded areas represent the wave packet created by the corresponding broadband pulse. (D) Phase-matching geometry. (E) Example ofmore » a double-sided Feynman diagram leading to 4WM signal emission.« less

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Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.