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Nature Photonics

Coherent control of ultrafast extreme ultraviolet transient absorption

Peng Peng, Yonghao Mi, Marianna Lytova, Mathew A. Britton, Xiaoyan Ding, Andrei Yu Naumov, P. B. Corkum, David M. Villeneuve

Published Dec 13, 2021• 60 citations
Publisher
DOI
10.1038/s41566-021-00907-7

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Metastable states are important actors in the ionisation of atoms and molecules. Sub-femtosecond extreme ultraviolet pulses can coherently populate several transiently bound states at once, thus starting the attosecond clocks which are required to monitor and control ultrafast electronic evolution above the ionisation threshold. Here we illustrate, from a theoretical point of view, the effects coherent superpositions of 1 P o doubly excited states in the helium atom have on channel-resolved photoelectron spectra as well as on the transient absorption spectrum of the atom in the extreme ultraviolet region, when they are created by a single-attosecond pulse in the presence of a strong few-cycle near-infrared/visible pulse which acts as a probe. Interference fringes varying rapidly with the pump-probe time delay are visible in both photoelectron and transient absorption spectra. From such fringes, the wave packet itself can conceivably be reconstructed. Conversely, all observables are modulated by the characteristic beating periods of the wave packet, so that control of partial ionisation yields, branching ratios, and light absorption or amplification can be achieved.
We present a theoretical study of the transient absorption of an ultrafast, extreme ultraviolet (XUV) pulse in the presence of an infrared (IR) control pulse in a macroscopic three-level helium gas. We concentrate on cases in which the IR pulse is shorter than the XUV pulse and induces transient transparency and amplification of the XUV light via coherent control. We give a time-dependent picture of the absorption process through the time dependence of the populations and relative coherences of the three states. We show that the XUV absorption can be dynamically changed into emission via phase control of the XUV-resonant 2p2p2p state through IR-induced coupling between the 2p2p2p and the 2s2s2s states. This can lead to compression and amplification of the XUV pulse when propagating through a laser-dressed macroscopic medium. We discuss the influence of atomic decoherence times on the XUV reshaping and show that fast decoherence means that the laser dressing acts more like a passive transmission window and less like a dynamical redistribution of energy.
Studying the dynamics of dark states is challenging due to their inability to undergo single-photon emission or absorption. This challenge is made even more difficult for dark autoionizing states owing to their ultrashort lifetime of a few femtoseconds. High-order harmonic spectroscopy recently appeared as a novel method to probe the ultrafast dynamics of a single atomic or molecular state. Here, we demonstrate the emergence of a new type of ultrafast resonance state as a manifestation of coupling between Rydberg and a dark autoionizing state dressed by a laser photon. Through high-order harmonic generation, this resonance results in extreme ultraviolet light emission that is more than one order of magnitude stronger than for the off-resonance case. The induced resonance can be leveraged to study the dynamics of a single dark autoionizing state and the transient changes in the dynamics of real states due to their overlap with the virtual laser-dressed states. In addition, the present results allow the generation of coherent ultrafast extreme ultraviolet light for advanced ultrafast science applications.