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Title: Self-heterodyned detection of dressed state coherences in helium by noncollinear extreme ultraviolet wave mixing with attosecond pulses

Abstract

Noncollinear wave-mixing spectroscopies with attosecond extreme ultraviolet (XUV) pulses provide unprecedented insight into electronic dynamics. In infrared and visible regimes, heterodyne detection techniques utilize a reference field to amplify wave-mixing signals while simultaneously allowing for phase-sensitive measurements. Here, we implement a self-heterodyned detection scheme in noncollinear wave-mixing measurements with a short attosecond XUV pulse train and two few-cycle near infrared (NIR) pulses. The initial spatiotemporally overlapped XUV and NIR pulses generate a coherence of both odd (1snp) and even (1sns and 1snd) parity states within gaseous helium. A variably delayed noncollinear NIR pulse generates angularly-dependent four-wave mixing signals that report on the evolution of this coherence. The diffuse angular structure of the XUV harmonics underlying these emission signals is used as a reference field for heterodyne detection, leading to cycle oscillations in the transient wave-mixing spectra. With this detection scheme, wave-mixing signals emitting from at least eight distinct light-induced, or dressed, states can be observed, in contrast to only one light induced state identified in a similar homodyne wave-mixing measurement. In conjunction with the self-heterodyned detection scheme, the noncollinear geometry permits the conclusive identification and angular separation of distinct wave-mixing pathways, reducing the complexity of transient spectra. These results demonstratemore » that the application of heterodyne detection schemes can provide signal amplification and phase-sensitivity, while maintaining the versatility and selectivity of noncollinear attosecond XUV wave-mixing spectroscopies. These techniques will be important tools in the study of ultrafast dynamics within complex chemical systems in the XUV regime.« less

Authors:
ORCiD logo; ; ORCiD logo; ; ORCiD logo; ORCiD logo
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1618511
Alternate Identifier(s):
OSTI ID: 1618512; OSTI ID: 1633288
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Published Article
Journal Name:
JPhys Photonics
Additional Journal Information:
Journal Name: JPhys Photonics Journal Volume: 2 Journal Issue: 3; Journal ID: ISSN 2515-7647
Publisher:
IOP Publishing
Country of Publication:
United Kingdom
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; attosecond; wave-mixing; self-heterodyne; light induced states

Citation Formats

Fidler, Ashley P., Warrick, Erika R., Marroux, Hugo J. B., Bloch, Etienne, Neumark, Daniel M., and Leone, Stephen R. Self-heterodyned detection of dressed state coherences in helium by noncollinear extreme ultraviolet wave mixing with attosecond pulses. United Kingdom: N. p., 2020. Web. doi:10.1088/2515-7647/ab869c.
Fidler, Ashley P., Warrick, Erika R., Marroux, Hugo J. B., Bloch, Etienne, Neumark, Daniel M., & Leone, Stephen R. Self-heterodyned detection of dressed state coherences in helium by noncollinear extreme ultraviolet wave mixing with attosecond pulses. United Kingdom. doi:https://doi.org/10.1088/2515-7647/ab869c
Fidler, Ashley P., Warrick, Erika R., Marroux, Hugo J. B., Bloch, Etienne, Neumark, Daniel M., and Leone, Stephen R. Thu . "Self-heterodyned detection of dressed state coherences in helium by noncollinear extreme ultraviolet wave mixing with attosecond pulses". United Kingdom. doi:https://doi.org/10.1088/2515-7647/ab869c.
@article{osti_1618511,
title = {Self-heterodyned detection of dressed state coherences in helium by noncollinear extreme ultraviolet wave mixing with attosecond pulses},
author = {Fidler, Ashley P. and Warrick, Erika R. and Marroux, Hugo J. B. and Bloch, Etienne and Neumark, Daniel M. and Leone, Stephen R.},
abstractNote = {Noncollinear wave-mixing spectroscopies with attosecond extreme ultraviolet (XUV) pulses provide unprecedented insight into electronic dynamics. In infrared and visible regimes, heterodyne detection techniques utilize a reference field to amplify wave-mixing signals while simultaneously allowing for phase-sensitive measurements. Here, we implement a self-heterodyned detection scheme in noncollinear wave-mixing measurements with a short attosecond XUV pulse train and two few-cycle near infrared (NIR) pulses. The initial spatiotemporally overlapped XUV and NIR pulses generate a coherence of both odd (1snp) and even (1sns and 1snd) parity states within gaseous helium. A variably delayed noncollinear NIR pulse generates angularly-dependent four-wave mixing signals that report on the evolution of this coherence. The diffuse angular structure of the XUV harmonics underlying these emission signals is used as a reference field for heterodyne detection, leading to cycle oscillations in the transient wave-mixing spectra. With this detection scheme, wave-mixing signals emitting from at least eight distinct light-induced, or dressed, states can be observed, in contrast to only one light induced state identified in a similar homodyne wave-mixing measurement. In conjunction with the self-heterodyned detection scheme, the noncollinear geometry permits the conclusive identification and angular separation of distinct wave-mixing pathways, reducing the complexity of transient spectra. These results demonstrate that the application of heterodyne detection schemes can provide signal amplification and phase-sensitivity, while maintaining the versatility and selectivity of noncollinear attosecond XUV wave-mixing spectroscopies. These techniques will be important tools in the study of ultrafast dynamics within complex chemical systems in the XUV regime.},
doi = {10.1088/2515-7647/ab869c},
journal = {JPhys Photonics},
number = 3,
volume = 2,
place = {United Kingdom},
year = {2020},
month = {5}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
DOI: https://doi.org/10.1088/2515-7647/ab869c

Figures / Tables:

Figure 1 Figure 1: Experimental geometry and pulse sequence. (a) The experimental apparatus after spectral broadening and pulse compression used for noncollinear wave-mixing measurements with attosecond pulses. (b) A noncollinear NIR pulse crossing the axis defined by the propagation of the XUV pulse with an angle of 1° leads to wave-mixing emissionmore » at non-zero divergence angles. (c) The XUV and collinear NIR pulse are time-coincident and induce a polarization probed by the noncollinear NIR pulse.« less

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Works referenced in this record:

Time-resolved four-wave-mixing spectroscopy for inner-valence transitions
journal, January 2016

  • Ding, Thomas; Ott, Christian; Kaldun, Andreas
  • Optics Letters, Vol. 41, Issue 4
  • DOI: 10.1364/OL.41.000709

Self Referencing Heterodyne Transient Grating Spectroscopy with Short Wavelength
journal, April 2015


Sub-cycle Oscillations in Virtual States Brought to Light
journal, January 2013

  • Chini, Michael; Wang, Xiaowei; Cheng, Yan
  • Scientific Reports, Vol. 3, Issue 1
  • DOI: 10.1038/srep01105

Nonlinear XUV signal generation probed by transient grating spectroscopy with attosecond pulses
journal, March 2019


Multidimensional spectroscopy with attosecond extreme ultraviolet and shaped near-infrared pulses
journal, September 2018

  • Marroux, Hugo J. B.; Fidler, Ashley P.; Neumark, Daniel M.
  • Science Advances, Vol. 4, Issue 9
  • DOI: 10.1126/sciadv.aau3783

Ultrafast heterodyne-detected transient-grating spectroscopy using diffractive optics
journal, January 1998

  • Goodno, Gregory D.; Dadusc, Gami; Miller, R. J. Dwayne
  • Journal of the Optical Society of America B, Vol. 15, Issue 6, 1791-1794
  • DOI: 10.1364/JOSAB.15.001791

Transient Grating Optical Heterodyne Detected Impulsive Stimulated Raman Scattering in Simple Liquids
journal, March 1995

  • Voehringer, Peter; Scherer, Norbert F.
  • The Journal of Physical Chemistry, Vol. 99, Issue 9
  • DOI: 10.1021/j100009a027

Polarization control of absorption of virtual dressed states in helium
journal, September 2015


Heterodyne‐detected time‐domain measurement of I 2 predissociation and vibrational dynamics in solution
journal, April 1992

  • Scherer, N. F.; Ziegler, L. D.; Fleming, G. R.
  • The Journal of Chemical Physics, Vol. 96, Issue 7
  • DOI: 10.1063/1.462693

Experimental demonstration of a single-spike hard-X-ray free-electron laser starting from noise
journal, October 2017

  • Marinelli, A.; MacArthur, J.; Emma, P.
  • Applied Physics Letters, Vol. 111, Issue 15
  • DOI: 10.1063/1.4990716

Excited-state vibronic wave-packet dynamics in H 2 probed by XUV transient four-wave mixing
journal, February 2018


Multiple pulse coherent dynamics and wave packet control of the N 2 a′′ 1 Σ+g dark state by attosecond four-wave mixing
journal, January 2018

  • Warrick, Erika R.; Fidler, Ashley P.; Cao, Wei
  • Faraday Discussions, Vol. 212
  • DOI: 10.1039/C8FD00074C

Light-induced states in attosecond transient absorption spectra of laser-dressed helium
journal, December 2012


Direct mapping of curve-crossing dynamics in IBr by attosecond transient absorption spectroscopy
journal, July 2019


Attosecond physics
journal, February 2009


Observation of a Train of Attosecond Pulses from High Harmonic Generation
journal, June 2001


Multidimensional resonant nonlinear spectroscopy with coherent broadband x-ray pulses
journal, March 2016


Multidimensional Attosecond Resonant X-Ray Spectroscopy of Molecules: Lessons from the Optical Regime
journal, April 2013


Optical multidimensional coherent spectroscopy
journal, July 2013

  • Cundiff, Steven T.; Mukamel, Shaul
  • Physics Today, Vol. 66, Issue 7
  • DOI: 10.1063/PT.3.2047

Reconstruction and control of a time-dependent two-electron wave packet
journal, December 2014

  • Ott, Christian; Kaldun, Andreas; Argenti, Luca
  • Nature, Vol. 516, Issue 7531
  • DOI: 10.1038/nature14026

Intensity dependence of light-induced states in transient absorption of laser-dressed helium measured with isolated attosecond pulses
journal, October 2013


Generating Single-Spike Hard X-Ray Pulses with Nonlinear Bunch Compression in Free-Electron Lasers
journal, October 2017


Alternating absorption features during attosecond-pulse propagation in a laser-controlled gaseous medium
journal, November 2013


Probing ultrafast dynamics with attosecond transient absorption
journal, March 2015


Attosecond metrology
journal, November 2001

  • Hentschel, M.; Kienberger, R.; Spielmann, Ch.
  • Nature, Vol. 414, Issue 6863, p. 509-513
  • DOI: 10.1038/35107000

Tunable isolated attosecond X-ray pulses with gigawatt peak power from a free-electron laser
journal, December 2019


Absolute phase measurement in heterodyne detection of transient gratings
journal, January 2004


Ultrafast electron dynamics in phenylalanine initiated by attosecond pulses
journal, October 2014


Multiresonant Coherent Multidimensional Spectroscopy
journal, May 2011


Vibrational transitions in excited states of molecules using coherent stokes raman spectroscopy: application to ferrocytochrome-C
journal, November 1981


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

  • Fidler, Ashley P.; Marroux, Hugo J. B.; Warrick, Erika R.
  • The Journal of Chemical Physics, Vol. 151, Issue 11
  • DOI: 10.1063/1.5113912

Beyond the Single-Atom Response in Absorption Line Shapes: Probing a Dense, Laser-Dressed Helium Gas with Attosecond Pulse Trains
journal, April 2015


Attosecond band-gap dynamics in silicon
journal, December 2014


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