Tracking attosecond electronic coherences using phase-manipulated extreme ultraviolet pulses

The 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. A. Wituschek et al. Nature Communications 11, 883 (2020)
 Shot-to-shot phase manipulation of XUV pulses for different high harmonics
The extension of coherent time-resolved spectroscopy to extreme ultraviolet (XUV) photon energies is highly desirable as it offers unprecedented site-specificity by accessing localized inner-shell states and opens the door to attosecond time resolution. However, these experiments are extremely challenging due to the required ultra-high phase stability and the lack of phase-matching/cycling schemes necessary to isolate subtle coherence signals. For these reasons, a real-time study of the evolution of an XUV electronic coherence has not been reported and only few examples of quantum beat and vibrational wave packet (WP) studies have been demonstrated so far. In the present work, we implement a phase modulation technique for XUV pulse sequences, which facilitates both flexible coherent control schemes, and advanced coherent nonlinear spectroscopy techniques.
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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 Petrov, O'Shea Finn Henry, Penco Giuseppe, Piseri Paolo, Plekan Oksana, Prince Kevin Charles, Przystawik Andreas, Rebernik Ribic Primoz, Sansone Giuseppe, Sigalotti Paolo, Spampinati Simone, Spezzani Carlo, Squibb Richard, Stranges Stefano, Uhl Daniel, Stienkemeier Frank
Nature Communications 11, 883 (2020)
doi: 10.1038/s41467-020-14721-2

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