Investigation of coupling mechanisms in attosecond transient absorption of autoionizing states: comparison of theory and experiment in xenon

Xuan Li, Birgitta Bernhardt, Annelise R Beck, Erika R Warrick, Adrian N Pfeiffer, M Justine Bell, Daniel J Haxton, C William McCurdy, Daniel M Neumark, Stephen R Leone

Research output: Contribution to journalArticleResearchpeer-review

Abstract

Attosecond transient absorption spectra near the energies of autoionizing states are analyzed in terms of the photon coupling mechanisms to other states. In a recent experiment, the autoionization lifetimes of highly excited states of xenon were determined and compared to a simple expression based on a model of how quantum coherence determines the decay of a metastable state in the transient absorption spectrum. Here it is shown that this procedure for extracting lifetimes is more general and can be used in cases involving either resonant or nonresonant coupling of the attosecond-probed autoionizing state to either continua or discrete states by a time-delayed near infrared (NIR) pulse. The fits of theoretically simulated absorption signals for the 6p resonance in xenon (lifetime = 21.1 fs) to this expression yield the correct decay constant for all the coupling mechanisms considered, properly recovering the time signature of twice the autoionization lifetime due to the coherent nature of the transient absorption experiment. To distinguish between these two coupling cases, the characteristic dependencies of the transient absorption signals on both the photon energy and time delay are investigated. Additional oscillations versus delay-time in the measured spectrum are shown and quantum beat analysis is used to pinpoint the major photon-coupling mechanism induced by the NIR pulse in the current xenon experiment: the NIR pulse resonantly couples the attosecond-probed state, 6p, to an intermediate 8s (at 22.563 eV), and this 8s state is also coupled to a neighboring state (at 20.808 eV).
Original languageEnglish
Pages (from-to)12560
Number of pages10
JournalJournal of Physics / B
Volume48
Issue number12
DOIs
Publication statusPublished - 1 May 2015
Externally publishedYes

Fields of Expertise

  • Advanced Materials Science

Cite this

Investigation of coupling mechanisms in attosecond transient absorption of autoionizing states: comparison of theory and experiment in xenon. / Li, Xuan; Bernhardt, Birgitta; Beck, Annelise R; Warrick, Erika R; Pfeiffer, Adrian N; Bell, M Justine; Haxton, Daniel J; McCurdy, C William; Neumark, Daniel M; Leone, Stephen R.

In: Journal of Physics / B, Vol. 48, No. 12, 01.05.2015, p. 12560.

Research output: Contribution to journalArticleResearchpeer-review

Li, Xuan ; Bernhardt, Birgitta ; Beck, Annelise R ; Warrick, Erika R ; Pfeiffer, Adrian N ; Bell, M Justine ; Haxton, Daniel J ; McCurdy, C William ; Neumark, Daniel M ; Leone, Stephen R. / Investigation of coupling mechanisms in attosecond transient absorption of autoionizing states: comparison of theory and experiment in xenon. In: Journal of Physics / B. 2015 ; Vol. 48, No. 12. pp. 12560.
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author = "Xuan Li and Birgitta Bernhardt and Beck, {Annelise R} and Warrick, {Erika R} and Pfeiffer, {Adrian N} and Bell, {M Justine} and Haxton, {Daniel J} and McCurdy, {C William} and Neumark, {Daniel M} and Leone, {Stephen R}",
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AU - Pfeiffer, Adrian N

AU - Bell, M Justine

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AB - Attosecond transient absorption spectra near the energies of autoionizing states are analyzed in terms of the photon coupling mechanisms to other states. In a recent experiment, the autoionization lifetimes of highly excited states of xenon were determined and compared to a simple expression based on a model of how quantum coherence determines the decay of a metastable state in the transient absorption spectrum. Here it is shown that this procedure for extracting lifetimes is more general and can be used in cases involving either resonant or nonresonant coupling of the attosecond-probed autoionizing state to either continua or discrete states by a time-delayed near infrared (NIR) pulse. The fits of theoretically simulated absorption signals for the 6p resonance in xenon (lifetime = 21.1 fs) to this expression yield the correct decay constant for all the coupling mechanisms considered, properly recovering the time signature of twice the autoionization lifetime due to the coherent nature of the transient absorption experiment. To distinguish between these two coupling cases, the characteristic dependencies of the transient absorption signals on both the photon energy and time delay are investigated. Additional oscillations versus delay-time in the measured spectrum are shown and quantum beat analysis is used to pinpoint the major photon-coupling mechanism induced by the NIR pulse in the current xenon experiment: the NIR pulse resonantly couples the attosecond-probed state, 6p, to an intermediate 8s (at 22.563 eV), and this 8s state is also coupled to a neighboring state (at 20.808 eV).

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