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

Marroux, Hugo J.  B.; Fidler, Ashley P.; Neumark, Daniel M.; Leone, Stephen R.

doi:10.1126/sciadv.aau3783

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

Journal Article · Fri Sep 28 00:00:00 EDT 2018 · Science Advances

DOI:https://doi.org/10.1126/sciadv.aau3783· OSTI ID:1506366

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Univ. of California, Berkeley, CA (United States). Dept. of Chemistry; 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; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division

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.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1506366

Journal Information:: Science Advances, Vol. 4, Issue 9; ISSN 2375-2548

Publisher:: AAASCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 29 works

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Two-dimensional UV spectroscopy: a new insight into the structure and dynamics of biomolecules Borrego-Varillas, R.; Nenov, A.; Ganzer, L. Chemical Science, Vol. 10, Issue 43 https://doi.org/10.1039/c9sc03871j	journal	January 2019
Exploring the multiparameter nature of EUV-visible wave mixing at the FERMI FEL Foglia, L.; Capotondi, F.; Höppner, H. Structural Dynamics, Vol. 6, Issue 4 https://doi.org/10.1063/1.5111501	journal	July 2019
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 Fidler, Ashley P.; Marroux, Hugo J. B.; Warrick, Erika R. The Journal of Chemical Physics, Vol. 151, Issue 11 https://doi.org/10.1063/1.5113912	journal	September 2019
Transient absorption spectroscopy using high harmonic generation: a review of ultrafast X-ray dynamics in molecules and solids Geneaux, Romain; Marroux, Hugo J. B.; Guggenmos, Alexander Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 377, Issue 2145 https://doi.org/10.1098/rsta.2017.0463	journal	April 2019
IsoSense: frequency enhanced sensorless adaptive optics through structured illumination Žurauskas, Mantas; Dobbie, Ian M.; Parton, Richard M. Optica, Vol. 6, Issue 3 https://doi.org/10.1364/optica.6.000370	journal	January 2019

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