Wituschek Andreas, Bruder Lukas, Allaria Enrico, Bangert Ulrich, Binz Marcel, Borghes Roberto, Callegari Carlo, Cerullo Giulio, Cinquegrana Paolo, Giannessi Luca, Danailov Miltcho, Demidovich Alexander, Di Fraia Michele, Drabbels Marcel, Feifel Raimund, Laarmann Tim, Michiels Rupert, Mirian Najmeh Sadat, Mudrich Marcel, Nikolov Ivaylo, O'Shea Finn H, Penco Giuseppe, Piseri Paolo, Plekan Oksana, Prince Kevin Charles, Przystawik Andreas, Ribič Primož Rebernik, Sansone Giuseppe, Sigalotti Paolo, Spampinati Simone, Spezzani Carlo, Squibb Richard James, Stranges Stefano, Uhl Daniel, Stienkemeier Frank
Institute of Physics, University of Freiburg, Hermann-Herder-Str. 3, 79104, Freiburg, Germany.
Chemical Physics, Lund University, Naturvetarvägen 16, 22362, Lund, Sweden.
Nat Commun. 2020 Feb 14;11(1):883. doi: 10.1038/s41467-020-14721-2.
The recent development of ultrafast extreme ultraviolet (XUV) coherent light sources bears great potential for a better understanding of the structure and dynamics of matter. Promising routes are advanced coherent control and nonlinear spectroscopy schemes in the XUV energy range, yielding unprecedented spatial and temporal resolution. However, their implementation has been hampered by the experimental challenge of generating XUV pulse sequences with precisely controlled timing and phase properties. In particular, direct control and manipulation of the phase of individual pulses within an XUV pulse sequence opens exciting possibilities for coherent control and multidimensional spectroscopy, but has not been accomplished. Here, we overcome these constraints in a highly time-stabilized and phase-modulated XUV-pump, XUV-probe experiment, which directly probes the evolution and dephasing of an inner subshell electronic coherence. This approach, avoiding any XUV optics for direct pulse manipulation, opens up extensive applications of advanced nonlinear optics and spectroscopy at XUV wavelengths.
超快极紫外（XUV）相干光源的最新发展对于更好地理解物质的结构和动力学具有巨大潜力。在XUV能量范围内，先进的相干控制和非线性光谱方案是很有前景的途径，可产生前所未有的空间和时间分辨率。然而，它们的实施受到了产生具有精确控制的定时和相位特性的XUV脉冲序列这一实验挑战的阻碍。特别是，直接控制和操纵XUV脉冲序列中单个脉冲的相位为相干控制和多维光谱学带来了令人兴奋的可能性，但尚未实现。在此，我们在一个高度时间稳定且相位调制的XUV泵浦-XUV探测实验中克服了这些限制，该实验直接探测内壳层电子相干的演化和退相。这种方法避免了用于直接脉冲操纵的任何XUV光学元件，为XUV波长下先进的非线性光学和光谱学开辟了广泛的应用。
