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arXiv:1602.01526 · Physical Review A

Attosecond transient absorption in dense gases: Exploring the interplay between resonant pulse propagation and laser-induced line-shape control

Chen-Ting Liao, Arvinder S. Sandhu, Seth Camp, Kenneth J. Schäfer, Mette B. Gaarde

Published Mar 4, 2016• 24 citations
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Abstract

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.

DOI
10.1103/physreva.93.033405

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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.
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.
We show that by combining strong-field dressing and resonant propagation of XUV pulses, the transition of absorption lines from their natural Lorentzian profiles through Fano and complex multipeak shapes all the way back to broadened near-Lorentzian profiles can be achieved, in the limit of optically thick samples. The final stage of this spectral modification can be understood in terms of a significant temporal stretching and delay of the resonant XUV pulse as it propagates through the dense gas, which alters the ultrafast absorption that is modified by the time-synchronized few-femtosecond laser pulse. We first demonstrate this concept in numerical calculations, both using a model system and through a fully coupled solution of the time-dependent Schrödinger equation and the Maxwell wave equation. The applicability and generality of the underlying mechanism is then illustrated in proof-of-principle attosecond transient absorption measurements in a helium gas with a widely varying atomic density. These results provide insights into the interaction of ultrashort laser pulses with dense media and its coherent control.
We employ an extreme ultraviolet (XUV) pulse to impulsively excite dipole polarization in atoms or molecules, which corresponds to coherently prepared superposition of excited states. A delayed near infrared (NIR) pulse then perturbs the fast evolving polarization, and the resultant absorbance change is monitored in dilute helium, dense helium, and sulfur hexafluoride (SF6) molecules. We observe and quantify the time-dependence of various transient phenomena in helium atoms,includinglaser-inducedphase(LIP),time-varying(AC)Starkshift,quantumpathinterference, and laser-induced continuum structure. In the case of dense helium targets, we discuss nonlinear macroscopic propagation effects pertaining to LIP and resonant pulse propagation, which accoun tfor the appearance of new spectral features in transient lineshapes. We then use tunable NIR photons to demonstrate the wavelength dependence of the transient laser induced effects. In the case of molecular polarization experiment in SF6, we show suppression of XUV photoabsorption corresponding to inter-valence transitions in the presence of a strong NIR field. In each case, the temporal evolution of transient absorption spectra allows us to observe and understand the transient laser induced modifications of the electronic structure of atoms and molecules.
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.
Recording the transmitted spectrum of a weak attosecond pulse through a medium, while a strong femtosecond pulse copropagates at variable delay, probes the strong-field dynamics of atoms, molecules, and solids. Usually, the interpretation of these measurements is based on the assumption of a thin medium. Here, the propagation through a macroscopic medium of helium atoms in the region of fully allowed resonances is investigated both theoretically and experimentally. The propagation has dramatic effects on the transient spectrum even at relatively low pressures (50 mbar) and short propagation lengths (1 mm). The absorption does not evolve monotonically with the product of propagation distance and pressure, but regions with characteristics of Lorentz line shapes and characteristics of Fano line shapes alternate. Criteria are deduced to estimate whether macroscopic effects can be neglected or not in a transient absorption experiment. Furthermore, the theory in the limit of single-atom response yields a general equation for Lorentz- and Fano-type line shapes at variable pulse delay.