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Title: Noncollinear wave mixing of attosecond XUV and few-cycle optical laser pulses in gas-phase atoms: Toward multidimensional spectroscopy involving XUV excitations

Journal Article · · Physical Review A
 [1];  [2];  [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 and 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

Ultrafast nonlinear spectroscopy, which records transient wave-mixing signals in a medium, is a robust tool to access microscopic information using light sources in the radio-frequency and optical regimes. The extension of this technique towards the extreme ultraviolet (XUV) or even x-ray regimes holds the promise to uncover rich structural or dynamical information with even higher spatial or temporal resolution. In this report, we demonstrate noncollinear wave mixing between weak XUV attosecond pulses and a strong near-infrared (NIR) few-cycle laser pulse in gas phase atoms (one photon of XUV and two photons of NIR). In the noncollinear geometry the attosecond and either one or two NIR pulses interact with argon atoms. Nonlinear XUV signals are generated in a spatially resolved fashion as required by phase matching. Different transition pathways can be identified from these background-free nonlinear signals according to the specific phase-matching conditions. Time-resolved measurements of the spatially gated XUV signals reveal electronic coherences of Rydberg wave packets prepared by a single XUV photon or XUV-NIR two-photon excitation, depending on the applied pulse sequences. These measurements open possible applications of tabletop multidimensional spectroscopy to the research of dynamics associated with valence or core excitation with XUV photons.

Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC02-05CH11231
OSTI ID:
1580076
Alternate ID(s):
OSTI ID: 1333341
Journal Information:
Physical Review A, Vol. 94, Issue 5; ISSN 2469-9926
Publisher:
American Physical Society (APS)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 45 works
Citation information provided by
Web of Science

References (34)

Time-resolved four-wave-mixing spectroscopy for inner-valence transitions journal January 2016
Nonlinear optics and spectroscopy journal July 1982
Sub-cycle Oscillations in Virtual States Brought to Light journal January 2013
Observation of a Photon Echo journal November 1964
Two-dimensional spectral interpretation of time-dependent absorption near laser-coupled resonances journal June 2014
A Review of the Theory and Application of Coherent Anti-Stokes Raman Spectroscopy (CARS) journal July 1977
Structure of the Amide I Band of Peptides Measured by Femtosecond Nonlinear-Infrared Spectroscopy journal July 1998
Optimizing High Harmonic Generation in Absorbing Gases: Model and Experiment journal February 1999
Femtosecond time‐resolved studies of coherent vibrational Raman scattering in large gas‐phase molecules journal December 1995
Laser-imposed phase in resonant absorption of an isolated attosecond pulse journal September 2013
Four-wave mixing experiments with extreme ultraviolet transient gratings journal April 2015
Observation of autoionization dynamics and sub-cycle quantum beating in electronic molecular wave packets journal February 2016
Quantum interference in attosecond transient absorption of laser-dressed helium atoms journal March 2013
Femtosecond time-resolved four-wave mixing spectroscopy in iodine vapour journal December 1997
Coherent Ultrafast Core-Hole Correlation Spectroscopy: X-Ray Analogues of Multidimensional NMR journal October 2007
Near-resonant four-wave mixing of attosecond extreme-ultraviolet pulses with near-infrared pulses in neon: Detection of electronic coherences journal August 2016
Two‐dimensional spectroscopy. Application to nuclear magnetic resonance journal March 1976
Coherent X-Ray Raman Spectroscopy: A Nonlinear Local Probe for Electronic Excitations journal July 2002
Attosecond Pulse Trains Using High–Order Harmonics journal August 1996
Observation of a Train of Attosecond Pulses from High Harmonic Generation journal June 2001
Attosecond transient absorption probing of electronic superpositions of bound states in neon: detection of quantum beats journal November 2014
Probing the Dynamics of Rydberg and Valence States of Molecular Nitrogen with Attosecond Transient Absorption Spectroscopy journal February 2016
Quantum Path Interference in the Wavelength Dependence of High-Harmonic Generation journal December 2007
Multidimensional Attosecond Resonant X-Ray Spectroscopy of Molecules: Lessons from the Optical Regime journal April 2013
Femtosecond time-resolved coherent anti-Stokes Raman scattering for the simultaneous study of ultrafast ground and excited state dynamics: iodine vapour journal May 1997
M ULTIDIMENSIONAL F EMTOSECOND C ORRELATION S PECTROSCOPIES OF E LECTRONIC AND V IBRATIONAL E XCITATIONS journal October 2000
Nuclear-motion effects in attosecond transient-absorption spectroscopy of molecules journal April 2015
Concepts and Methods of 2D Infrared Spectroscopy book January 2011
Probing ultrafast dynamics with attosecond transient absorption journal March 2015
Lorentz Meets Fano in Spectral Line Shapes: A Universal Phase and Its Laser Control journal May 2013
Multiresonant Coherent Multidimensional Spectroscopy journal May 2011
Time-resolved x-ray spectroscopies: Nonlinear response functions and Liouville-space pathways journal May 2001
Attosecond transient absorption of argon atoms in the vacuum ultraviolet region: line energy shifts versus coherent population transfer journal January 2016
Femtosecond transient-grating techniques: Population and coherence dynamics involving ground and excited states journal March 1999

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Autoionization dynamics of ( 2 P 1/2 ) ns/d states in krypton probed by noncollinear wave mixing with attosecond extreme ultraviolet and few-cycle near infrared pulses journal September 2019
Double-resonance studies of electronically autoionizing states of molecular nitrogen journal January 2019
Roadmap of ultrafast x-ray atomic and molecular physics journal January 2018
Ultrafast control and opto-optical modulation of extreme ultraviolet light journal March 2019
Transient absorption spectroscopy using high harmonic generation: a review of ultrafast X-ray dynamics in molecules and solids
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  • Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 377, Issue 2145 https://doi.org/10.1098/rsta.2017.0463
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Perturbed ac Stark Effect for Attosecond Optical-Waveform Sampling journal January 2020
Multidimensional spectroscopy with attosecond extreme ultraviolet and shaped near-infrared pulses journal September 2018
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Roadmap of ultrafast x-ray atomic and molecular physics text January 2019
Double-resonance studies of electronically autoionizing states of molecular nitrogen text January 2019
Double-resonance studies of electronically autoionizing states of molecular nitrogen text January 2019
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