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Coherent all X-ray four wave mixing at core shell resonances

Authors :
Morillo-Candas, Ana Sofia
Augustin, Sven Martin
Prat, Eduard
Sarracini, Antoine
Knurr, Jonas
Zerdane, Serhane
Sun, Zhibin
Yang, Ningchen
Rebholz, Marc
Zhang, Hankai
Deng, Yunpei
Xie, Xinhua
Cannizzo, Andrea
Al-Haddad, Andre
Schnorr, Kirsten Andrea
Ott, Christian
Feurer, Thomas
Bostedt, Christoph
Pfeifer, Thomas
Knopp, Gregor
Publication Year :
2024

Abstract

Nonlinear wave mixing in the X-ray range can provide valuable insights into the structural and electron dynamics of atomic and molecular systems on ultrafast time scales, with state- and site-selectivity and atomic resolution. This promising experimental toolbox was so far limited by requiring at least one near-visible laser, thus preventing core-shell two-dimensional X-ray spectroscopy. In this work, we demonstrate the generation of background-free all-X-ray four-wave mixing (XFWM) signals from a dilute gaseous sample (Ne). The measured and simulated two-dimensional spectral maps ($\omega_{\text{in}},\omega_{\text{out}}$) show multiple contributions involving the coherent response from core electrons. Notably, two-color resonant XFWM signals, essential for generalized multi-color schemes that allow to locally probe the electronic excitation of matter, are observed in neutral Ne. Moreover, stimulated Ne$^+$ emission in each of the propagating X-ray pulses leads to an increase of the temporal coherence in a narrow-bandwidth, which results in the coherent mixing of three X-ray lasers. Preliminary X-ray excitation experiments making use of multi-color time-delayed X-ray pulses demonstrate temporal resolution capability and show a time dependency consistent with a signal dominated by resonant XFWM processes. This first all-X-ray four-wave-mixing approach represents a major breakthrough towards multidimensional X-ray correlation spectroscopy and the general application of nonlinear all-X-ray wave-mixing.

Details

Database :
arXiv
Publication Type :
Report
Accession number :
edsarx.2408.11881
Document Type :
Working Paper