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Title: Nonlinear coherence effects in transient-absorption ion spectroscopy with stochastic extreme-ultraviolet free-electron laser pulses
Authors: Ding, Thomas
Rebholz, Marc
Aufleger, Lennart
Hartmann, Maximilian
Meyer, Kristina
Stooß, Veit
Magunia, Alexander
Wachs, David
Birk, Paul
Mi, Yonghao
Borisova, Gergana Dimitrova
da Costa Castanheira, Carina
Rupprecht, Patrick
Loh, Zhi Heng
Attar, Andrew R.
Gaumnitz, Thomas
Roling, Sebastian
Butz, Marco
Zacharias, Helmut
Düsterer, Stefan
Treusch, Rolf
Cavaletto, Stefano Michele
Ott, Christian
Pfeifer, Thomas
Keywords: Science::Chemistry
Issue Date: 2019
Source: Ding, T., Rebholz, M., Aufleger, L., Hartmann, M., Meyer, K., Stooß, V., . . . Pfeifer, T. (2019). Nonlinear coherence effects in transient-absorption ion spectroscopy with stochastic extreme-ultraviolet free-electron laser pulses. Physical Review Letters, 123(10), 103001-. doi:10.1103/physrevlett.123.103001
Journal: Physical Review Letters
Abstract: We demonstrate time-resolved nonlinear extreme-ultraviolet absorption spectroscopy on multiply charged ions, here applied to the doubly charged neon ion, driven by a phase-locked sequence of two intense free-electron laser pulses. Absorption signatures of resonance lines due to 2p-3d bound-bound transitions between the spin-orbit multiplets ^{3}P_{0,1,2} and ^{3}D_{1,2,3} of the transiently produced doubly charged Ne^{2+} ion are revealed, with time-dependent spectral changes over a time-delay range of (2.4±0.3)  fs. Furthermore, we observe 10-meV-scale spectral shifts of these resonances owing to the ac Stark effect. We use a time-dependent quantum model to explain the observations by an enhanced coupling of the ionic quantum states with the partially coherent free-electron laser radiation when the phase-locked pump and probe pulses precisely overlap in time.
ISSN: 0031-9007
DOI: 10.1103/PhysRevLett.123.103001
Rights: © 2019 American Physical Society. All rights reserved. This paper was published in Physical Review Letters and is made available with permission of American Physical Society.
Fulltext Permission: open
Fulltext Availability: With Fulltext
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