2018
DOI: 10.1103/physreva.98.063403
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Ultrafast nuclear dynamics in the doubly-core-ionized water molecule observed via Auger spectroscopy

Abstract: We present a combined experimental and theoretical study of the Auger-emission spectrum following double core ionization and excitation of gas-phase water molecules with hard-x-ray synchrotron radiation above the O K −2 threshold. We observe an indication of ultrafast proton motion occurring within the 1.5 fs lifetime of the double-core-hole (DCH) states in water. Furthermore, we have identified symmetric and antisymmetric dissociation modes characteristic for particular DCH states. Our results serve as a fund… Show more

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Cited by 24 publications
(28 citation statements)
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References 33 publications
(44 reference statements)
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“…To account for the finite width of the vibrational wave-packet evolving in time and following the arguments in Ref. 25, we employ…”
Section: Femtosecond Xps and Aes Of The Photodissociating Moleculementioning
confidence: 99%
“…To account for the finite width of the vibrational wave-packet evolving in time and following the arguments in Ref. 25, we employ…”
Section: Femtosecond Xps and Aes Of The Photodissociating Moleculementioning
confidence: 99%
“…The experimental spectra are compared with theoretical ones taking into account the nuclear dynamics (top panel) or at fixed geometry (bottom panel). The agreement is much better with the top panel, in particular for the spectral region above 560 eV, where there is a long tail attributed to the effect of nuclear motion (see [57] and references therein for more details). The different colours of the theoretical curves refer to the Auger decay of different DCH states (see [57] for a detailed assignment).…”
Section: Double-core-hole Studiesmentioning
confidence: 60%
“…The most recent molecule investigated is water [57]. A combined experimental and theoretical investigation is reported of the Auger emission processes following double core ionization and excitation of gas-phase water molecules with hard-x-ray synchrotron radiation in the photon energy region above the O K-edge double ionization.…”
Section: Double-core-hole Studiesmentioning
confidence: 99%
“…(8), we have neglected direct one-photon double-coreionization (i.e., K-shell hypersatellites), which has for K-shell ionization a negligible cross section. 46,47 We consider an x-ray pulse consisting of two subpulses, each of which has a Gaussian envelope. The first pulse is centered at time t = 0, and the second is centered at time t = t d .…”
Section: Theorymentioning
confidence: 99%