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Physical Review A

Laser-imposed phase in resonant absorption of an isolated attosecond pulse

Shaohao Chen, Mengxi Wu, Mette B. Gaarde, Kenneth J. Schäfer

Published Sep 9, 2013• 56 citations
Publisher

Abstract

We calculate resonant absorption line shapes in helium atoms subject to the combination of an attosecond pulse of XUV radiation and a delayed, few-cycle infrared (IR) laser pulse. We are in particular interested in how the resonant features evolve with the delay between the fields and with increasing IR intensity. We first compare the single-atom absorption calculated by a nonperturbative solution of the time-dependent Schr\"odinger equation (TDSE) to a simple model in which the resonant absorption is modified only by a laser-imposed phase (LIP) that originates in the instantaneous ac Stark shift of the resonant state. We find that the LIP model can explain many features of the resonant absorption, including the direction of the resonance energy shift and the onset of dispersive line shapes with increasing IR intensity. We also find, however, that the LIP model predicts the energy shifts and the line shapes only qualitatively when the resonant states are strongly IR coupled to nearby states. We then use a coupled solution of the Maxwell wave equation and the TDSE to examine how the line shapes are modified by propagation effects at helium densities such that the resonant absorption is strong. We find that when the resonant absorption saturates, their line shapes are strongly modified due to reshaping of the attosecond pulse time profile during propagation. This in turn alters the ultrafast absorption and emission dynamics.

DOI
10.1103/physreva.88.033409

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We calculate resonant absorption line shapes in helium atoms subject to the combination of an attosecond pulse of XUV radiation and a delayed, few-cycle infrared (IR) laser pulse. We are in particular interested in how the resonant features evolve with the delay between the fields and with increasing IR intensity. We first compare the single-atom absorption calculated by a nonperturbative solution of the time-dependent Schr"odinger equation (TDSE) to a simple model in which the resonant absorption is modified only by a laser-imposed phase (LIP) that originates in the instantaneous ac Stark shift of the resonant state. We find that the LIP model can explain many features of the resonant absorption, including the direction of the resonance energy shift and the onset of dispersive line shapes with increasing IR intensity. We also find, however, that the LIP model predicts the energy shifts and the line shapes only qualitatively when the resonant states are strongly IR coupled to nearby states. We then use a coupled solution of the Maxwell wave equation and the TDSE to examine how the line shapes are modified by propagation effects at helium densities such that the resonant absorption is strong. We find that when the resonant absorption saturates, their line shapes are strongly modified due to reshaping of the attosecond pulse time profile during propagation. This in turn alters the ultrafast absorption and emission dynamics.
In the present paper, we investigate the time-resolved transient absorption spectroscopy of doubly excited states of helium atoms by solving the time-dependent two-electron Schr\"odinger equation numerically based on a one-dimensional model. The helium atoms are subjected to an extreme ultraviolet (XUV) attosecond pulse and a time-delayed infrared (IR) few-cycle laser pulse. A superposition of doubly excited states populated by the XUV pulse is identified, which interferes with the direct ionization pathway leading to Fano resonance profiles in the photoabsorption spectrum. In the presence of an IR laser, however, the Fano line profiles are strongly modified: A shifting, splitting, and broadening of the original absorption lines is observed when the XUV attosecond pulse and infrared few-cycle laser pulse overlap in time, which is in good agreement with recent experimental results. At certain time delays, we observe symmetric Lorentz, inverted Fano profiles, and even negative absorption cross sections indicating that the XUV light can be amplified during the interaction with atoms. We further prove that the above pictures are general for different doubly excited states by suitably varying the frequency of the IR field to coherently couple the corresponding states.
We investigate the evolution of extreme ultraviolet (XUV) spectral line shapes in an optically thick helium gas under near-infrared (IR) perturbation. In our experimental and theoretical work, we systematically vary the IR intensity, time-delay, gas density, and IR polarization parameters to study line-shape modifications induced by collective interactions in a regime beyond the single-atom response of a thin, dilute gas. In both experiment and theory, we find that specific features in the frequency-domain absorption profile, and their evolution with propagation distance, can be attributed to the interplay between resonant attosecond pulse propagation and IR-induced phase shifts. Our calculations show that this interplay also manifests itself in the time domain, with the IR pulse influencing the reshaping of the XUV pulse propagating in the resonant medium.
We investigate the absorption line shapes of laser-dressed atoms beyond the single-atom response, by using extreme ultraviolet (XUV) attosecond pulse trains to probe an optically thick helium target under the influence of a strong infrared (IR) field. We study the interplay between the IR-induced phase shift of the microscopic time-dependent dipole moment and the resonant-propagation-induced reshaping of the macroscopic XUV pulse. Our experimental and theoretical results show that as the optical depth increases, this interplay leads initially to a broadening of the IR-modified line shape, and subsequently, to the appearance of new, narrow features in the absorption line.
Abstract We introduce a time-dependent generalized Floquet (TDGF) approach to calculate attosecond transient absorption spectra of helium atoms subjected to the combination of an attosecond extreme ultraviolet (XUV) pulse and a delayed few-cycle infrared (IR) laser pulse. This TDGF approach provides a Floquet understanding of the laser-induced change of resonant absorption lineshape. It is analytically demonstrated that the phase shift of the time-dependent dipole moment that results in the lineshape changes consists of two components, the adiabatic laser-induced phase (LIP) due to the IR-induced Stark shifts of adiabatic Floquet states and the non-adiabatic phase correction due to the non-adiabatic IR-induced coupling between adiabatic Floquet states. Comparisons of the spectral lineshape calculated based on the TDGF approach with the results obtained with the LIP model [ Phys. Rev. A 88 033409 (2013)] and the rotating-wave approximation (RWA) are presented for several typical cases, demonstrating that TDGF universally and accurately captures IR-induced lineshape changes. It is suggested that the LIP model works as long as the generalized adiabatic theorem [ PRX Quantum 2 030302 (2021)] holds, and the RWA works when the higher-order IR-coupling effect in the formation of adiabatic Floquet states is neglectable.
We present a theoretical study of transient absorption and reshaping of extreme ultraviolet (XUV) pulses by helium atoms dressed with a moderately strong infrared (IR) laser field. We formulate the atomic response using both the frequency-dependent absorption cross section and a time-frequency approach based on the time-dependent dipole induced by the light fields. The latter approach can be used in cases when an ultrafast dressing pulse induces transient effects, and/or when the atom exchanges energy with multiple frequency components of the XUV field. We first characterize the dressed atom response by calculating the frequency-dependent absorption cross section for XUV energies between 20 and 24 eV for several dressing wavelengths between 400 and 2000 nm and intensities up to 1012{}^{12}12 W/cm2{}^{2}2. We find that for dressing wavelengths near 1600 nm, there is an Autler-Townes splitting of the $1s\ensuremath{\rightarrow}2p$ transition that can potentially lead to transparency for absorption of XUV light tuned to this transition. We study the effect of this XUV transparency in a macroscopic helium gas by incorporating the time-frequency approach into a solution of the coupled Maxwell-Schr\"odinger equations. We find rich temporal reshaping dynamics when a 61-fs XUV pulse resonant with the $1s\ensuremath{\rightarrow}2p$ transition propagates through a helium gas dressed by an 11-fs, 1600-nm laser pulse.
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.