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Nature Communications

Raman time-delay in attosecond transient absorption of strong-field created krypton vacancy

Li Wang, Guangru Bai, Xiaowei Wang, Jing Zhao, Cheng Gao, Jiacan Wang, Fan Xiao, Wenkai Tao, Pan Song, Qianyu Qiu, Jinlei Liu, Zengxiu Zhao

Published Mar 27, 2024• 20 citations
Publisher

Abstract

Strong field ionization injects a transient vacancy in the atom which is entangled to the outgoing photoelectron. When the electron is finally detached, the ion is populated at different excited states with part of coherence information lost. The preserved coherence of matter after interacting with intense short pulses has important consequences on the subsequent nonequilibrium evolution and energy relaxation. Here we employ attosecond transient absorption spectroscopy to measure the time-delay of resonant transitions of krypton vacancy during their creation. We have observed that the absorptions by the two spin-orbit split states are modulated at different paces when varying the time-delay between the near-infrared pumping pulse and the attosecond probing pulse. It is shown that the coupling of the ions with the remaining field leads to a suppression of ionic coherence. Comparison between theory and experiments uncovers that coherent Raman coupling induces time-delay between the resonant absorptions, which provides insight into laser-ion interactions enriching attosecond chronoscopy.

DOI
10.1038/s41467-024-47088-9

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Strong field ionization injects a transient vacancy in the atom which is entangled to the outgoing photoelectron. When the electron is finally detached, the ion is populated at different excited states with part of coherence information lost. The preserved coherence of matter after interacting with intense short pulses has important consequences on the subsequent nonequilibrium evolution and energy relaxation. Here we employ attosecond transient absorption spectroscopy to measure the time-delay of resonant transitions of krypton vacancy during their creation. We have observed that the absorptions by the two spin-orbit split states are modulated at different paces when varying the time-delay between the near-infrared pumping pulse and the attosecond probing pulse. It is shown that the coupling of the ions with the remaining field leads to a suppression of ionic coherence. Comparison between theory and experiments uncovers that coherent Raman coupling induces time-delay between the resonant absorptions, which provides insight into laser-ion interactions enriching attosecond chronoscopy.
Ultrafast spectroscopy with attosecond resolution has enabled the real time observation of ultrafast electron dynamics in atoms, molecules and solids. These experiments employ attosecond pulses or pulse trains and explore dynamical processes in a pump-probe scheme that is selectively sensitive to electronic state of matter via photoelectron or XUV absorption spectroscopy or that includes changes of the ionic state detected via photo-ion mass spectrometry. Here, we demonstrate how the implementation of combined photo-ion and absorption spectroscopy with attosecond resolution enables tracking the complex multidimensional excitation and decay cascade of an Auger auto-ionization process of a few femtoseconds in highly excited krypton. In tandem with theory, our study reveals the role of intermediate electronic states in the formation of multiply charged ions. Amplitude tuning of a dressing laser field addresses different groups of decay channels and allows exerting temporal and quantitative control over the ionization dynamics in rare gas atoms.
We calculate the transient absorption of an isolated attosecond pulse (IAP) by helium atoms subject to a delayed infrared (IR) laser pulse. With the central frequency of the broad attosecond spectrum near the ionization threshold, the absorption spectrum is strongly modulated at the sub-IR-cycle level. Given that the absorption spectrum results from a time-integrated measurement, we investigate the extent to which the delay dependence of the absorption yields information about the attosecond dynamics of the atom-field energy exchange. We find two configurations in which this is possible. The first involves multiphoton transitions between bound states that result in interference between different excitation pathways. The second involves the modification of the bound state absorption lines by the IR field, which we find can result in a subcycle time dependence only when ionization limits the duration of the strong-field interaction.
Abstract Attosecond transient absorption (ATA) has been developed as an all-optical technique for probing electron dynamics in matter. Here we present a scheme that can modify the laser-induced state and the corresponding ATA spectrum via excitation by a pair of XUV attosecond pulses and by a time-delayed mid-infrared (MIR) laser probe. Different from the scheme of the electronic excitation by a single XUV attosecond pulse, the application of a pair of XUV pulses provides extra degrees of freedom, such as the time delay and the intensity ratio between two XUV pulses, which make it possible to adjust the pump process, resulting in the modification of the ATA spectrum. We show that by varying the time delay between the two XUV pulses, the population of the dark state and the ATA spectrum of the laser-induced state have periodic modulations. We also demonstrate that the peak of the ATA spectrum of the laser-induced state appears at a fixed time delay between the XUV pair and the MIR laser when the intensity ratio is large, and it changes with the time delay when the intensity ratio is small, which can be related to either one of two peaks in the population of the dark state.
Autoionization of argon atoms was studied experimentally by transient absorption spectroscopy with isolated attosecond pulses. The peak position, intensity, linewidth, and shape of the 3s3p⁶np ¹P Fano resonance series (26.6-29.2 eV) were modified by intense few-cycle near infrared laser pulses, while the delay between the attosecond pulse and the laser pulse was changed by a few femtoseconds. Numerical simulations revealed that the experimentally observed splitting of the 3s3p⁶4p ¹P line is caused by the coupling between two short-lived highly excited states in the strong laser field.
Within this work, electron dynamics inside argon atoms are observed by probing the autoionizing states of argon atoms, so-called window resonances, with both attosecond XUV and timed-delayed few-cycle femtosecond NIR laser pulses, using attosecond transient absorption spectroscopy. The window resonances in the energy region of 25 - 29.3 eV are first excited with the XUV pulse and then dressed by the NIR laser, where the natural decay process of the states is greatly affected by the strong-field of the NIR pulse. Preliminary results of the measurement are presented in this work, with a hypothetical description of some of the effects that are present. A comparison has been made with the experimental results from a paper publishing measurements of autoionizing states with attosecond transient absorption spectroscopy for the first time, where the same resonances were probed. The comparison is only partly possible due to different experimental parameters and conditions, where more pronounced and new effects have been observed in the here performed measurement.
This thesis investigates quantum dynamics induced in atoms by ultrashort pulses of light. The work is motivated by recent developments in free-electron lasers, which generate ultrashort pulses of intense, coherent light and enable coherent control of quantum dynamics. We develop theoretical models to study the processes of absorption and emission in laser-atom interactions. Additionally, we study photoionisation, which creates an ion and an electron, and the entanglement that can be generated between these particles. Finally, we have investigated how the spontaneous decay of the ion induces entanglement transfer from the ion-electron pair to the electron-photon pair.This thesis compiles seven papers. Paper I investigates the absorption of light from an attosecond pulse by an atom in a prepared coherent superposition of states. We show how the evolution of the phase of the superposition wave packet influences the attosecond transient absorption spectra. Paper II predicts the existence of Mollow-like triplets in the absorption spectra of strongly coupled atoms. We establish the conditions for the pulse envelope under which this triplet pattern can be supported.Paper III studies two-photon Rabi oscillations, establishing which systems can sustain such dynamics. We find that a two-photon Rabi oscillating system can induce giant counter-rotating oscillations in the population dynamics, enabling investigations of physical effects beyond the rotating-wave approximation.Paper IV studies ionisation from an atom strongly coupled by a dichromatic field, where interference between the two frequency components shapes the temporal symmetry of the atomic dynamics, allowing for coherent control of the photoelectron distribution.Paper V considers an experiment performed at a Free-Electron Laser facility where a helium atom is ionised and the resulting ion is subsequently strongly coupled. The photoelectron spectra are theoretically reproduced and the entanglement between the ion and photoelectron is studied. Paper VI investigates how the entanglement in the ion--electron pair, generated via photoionisation followed by strong coupling, can be coherently controlled by harnessing the time symmetry of the pulse. We find that the observable manifestation of the entanglement can be altered in such a way that the electron energy becomes associated with the ionic state, allowing the entanglement to be detected via coincidence measurements. Paper VII investigates how quantum correlations between the ion and the electron can be coherently controlled by sequential strong coupling of the ion. We find that both the build-up of entanglement and its manifestation can be controlled, and we establish a quantitative measure of the amplitude entanglement that explains the dynamics in an intuitive way. Paper VIII studies the process of entanglement transfer induced by the spontaneous decay of the ion. We find that the ion--electron entanglement generated during the ultrashort interaction with the laser field is transferred to the electron--photon system over the much longer timescale of fluorescence.