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The spatial phase and direction of extreme-ultraviolet light are controlled by an all-optical modulator based on argon gas. It works by using an infrared pulse to control the spatial and spectral phase of the free induction decay in the gas system.

We extend the recently developed technique of opto-optical modulation (OOM) to probe state-resolved ac-Stark-induced phase variations of a coherently excited ensemble of helium atoms. In a joint experimental and theoretical study, we find that the spatial redirection of the resonant emission from the OOM process is different for the low-lying 1s2p state as compared with the higher-lying Rydberg states, and that this redirection can be controlled through the spatial characteristics of the infrared (IR) probe beam. In particular, we observe that the intensity dependence of the IR-induced Stark phase on the 1s2p emission is nonlinear, and that the phase accumulation changes sign for moderate intensities. Our results suggest that OOM, combined with precise experimental shaping of the probe beam, could be used to measure the Stark-induced phase shifts of excited states., 5 pages, 4 figures. Updated version addressing referee comments and editorial changes. Reprinted with permission from [Phys. Rev. A 100, 023403 (2019)]. Copyright (2019) by the American Physical Society

Nonlinear spectroscopies are utilized extensively for selective measurements of chemical dynamics in the optical, infrared, and radio-frequency regimes. The development of these techniques for extreme ultraviolet (XUV) light sources facilitates measurements of electronic dynamics on attosecond timescales. Here, we elucidate the temporal dynamics of nonlinear signal generation by utilizing a transient grating scheme with a subfemtosecond XUV pulse train and two few-cycle near-infrared pulses in atomic helium. Simultaneous detection of multiple diffraction orders reveals delays of ≥1.5 fs in higher-order XUV signal generation, which are reproduced theoretically by solving the coupled Maxwell–Schrödinger equations and with a phase grating model. The delays result in measurable order-dependent differences in the energies of transient light induced states. As nonlinear methods are extended into the attosecond regime, the observed higher-order signal generation delays will significantly impact and aid temporal and spectral measurements of dynamic processes., Ultrafast dynamics following light-matter interaction are governed by nonlinear processes. Here the authors show that initial nonlinear signal time-evolution is a consequence of phase grating accumulation using transient grating measurements with attosecond and near-infrared pulses.

Synopsis There is a profound, almost symbiotic relation between electrons and photons. When light interacts with matter the electrons in the material will start to move and oscillate. When a charged particle, such as an electron, oscillates it will act as a dipole and emit light. We utilize this symbiotic relation and extend the control of light to the extreme ultraviolet (XUV) region using the newly developed XUV opto-optical modulator.

We study attosecond XUV transient absorption in dense gases to investigate the interplay between resonant pulse propagation and laser induced phase shifts. We observe lineshape modifications due to laser-imposed phase and temporal reshaping of XUV

We investigate the role of excited states in High-order Harmonic Generation by studying the spectral, spatial and temporal characteristics of the radiation produced near the ionization threshold of argon by few-cycle laser pulses. We show that the population of excited states can lead either to direct XUV emission through Free Induction Decay or to the generation of high-order harmonics through ionization from these states and recombination to the ground state. By using the attosecond lighthouse technique, we demonstrate that the high-harmonic emission from excited states is temporally delayed by a few femtoseconds compared to the usual harmonics, leading to a strong nonadiabatic spectral redshift., Comment: Accepted at Physical Review Letters

In the infinite square well, any wave function will return to its initial state at integer multiples of the revival time. Most quantum systems do not exhibit perfect revivals, but some exhibit partial revivals in which the wave function returns close to its initial state. Subsequent partial revivals usually deteriorate in quality. We discuss the reasons for the perfect revivals in the infinite square well and how a small change in the potential disrupts the revivals. As an example, we examine partial revivals of a Gaussian wave packet in an infinite square well with a step. First-order and second-order perturbation theory show that the rate at which revivals decay depends on the location of the step.

Attosecond transient absorption is one of the promising new techniques being developed to exploit the availability of sub-femtosecond extreme ultraviolet (XUV) pulses to study the dynamics of the electron on its natural time scale. The temporal resolution in a transient absorption setup comes from the control of the relative delay and coherence between pump and probe pulses, while the spectral resolution comes from the characteristic width of the features that are being probed. In this review we focus on transient absorption scenarios where an attosecond pulse of XUV radiation creates a broadband excitation that is subsequently probed by a few cycle infrared (IR) laser. Because the attosecond XUV pulses are locked to the IR field cycle, the exchange of energy in the laser–matter interaction can be studied with unprecedented precision. We focus on the transient absorption by helium atoms of XUV radiation around the first ionization threshold, where we can simultaneoulsy solve the time-dependent Schrodinger equation for the single atom response and the Maxwell wave equation for the collective response of the nonlinear medium. We use a time-domain method that allows us to treat on an equal footing all the different linear and nonlinear processes by which the medium can exchange energy with the fields. We present several simple models, based on a few-level system interacting with a strong IR field, to explain many of the novel features found in attosecond transient absorption spectrograms. These include the presence of light-induced states, which demonstrate the ability to probe the dressed states of the atom. We also present a time-domain interpretation of the resonant pulse propagation features that appear in absorption spectra in dense, macroscopic media. We close by reviewing several recent experimental results that can be explained in terms of the models we discuss. Our aim is to present a road map for understanding future attosecond transient absorption experiments in more complex systems.