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Register a new userAttosecond Transient Absorption in Dense Gases: Exploring the Interplay between Resonant Pulse Propagation and Laser-Induced Line Shape Control
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We investigate the evolution of extreme ultraviolet (XUV) spectral lineshapes 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 lineshape 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.
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The recent demonstration of isolated attosecond pulses from an X-ray free-electron laser (XFEL) opens the possibility for probing ultrafast electron dynamics at X-ray wavelengths. An established experimental method for probing ultrafast dynamics is X-ray transient absorption spectroscopy, where the X-ray absorption spectrum is measured by scanning the central photon energy and recording the resultant photoproducts. The spectral bandwidth inherent to attosecond pulses is wide compared to the resonant features typically probed, which generally precludes the application of this technique in the attosecond regime. In this paper we propose and demonstrate a new technique to conduct transient absorption spectroscopy with broad bandwidth attosecond pulses with the aid of ghost imaging, recovering sub-bandwidth resolution in photoproduct-based absorption measurements.
We study the behavior of reduced models for the propagation of intense laser pulses in atomic gases. The models we consider incorporate ionization, blueshifting, and other nonlinear propagation effects in an ab initio manner, by explicitly taking into account the microscopic electron dynamics. Numerical simulations of the propagation of ultrashort linearly-polarized and elliptically-polarized laser pulses over experimentally-relevant propagation distances are presented. We compare the behavior of models where the electrons are treated classically with those where they are treated quantum-mechanically. A classical equivalent to the ground state is found, which maximizes the agreement between the quantum and classical predictions of the single-atom ionization probability as a function of laser intensity. We show that this translates into quantitative agreement between the quantum and classical models for the laser field evolution during propagation through gases of ground-state atoms. This agreement is exploited to provide a classical perspective on low- and high-order harmonic generation in linearly-polarized fields. In addition, we demonstrate the stability of the polarization of a nearly-linearly-polarized pulse using a two-dimensional model.
Transient absorption is a very powerful observable in attosecond experiments on atoms, molecules and solids and is frequently used in experiments employing phase-locked few-cycle infrared and XUV laser pulses derived from high harmonic generation. We show numerically and analytically that in non-centrosymmetric systems, such as many polyatomic molecules, which-way interference enabled by the lack of parity conservation leads to new spectral absorption features, which directly reveal the laser electric field. The extension of Attosecond Transient Absorption Spectroscopy (ATAS) to such targets hence becomes sensitive to global and local inversion symmetry. We anticipate that ATAS will find new applications in non-centrosymmetric systems, in which the carrier-to-envelope phase of the infrared pulse becomes a relevant parameter and in which the orientation of the sample and the electronic symmetry of the molecule can be addressed.
We simulate the transient absorption of attosecond pulses of infrared-laser-dressed atoms by considering a three-level system with the adiabatic approximation. The delay-dependent interference features are investigated from the perspective of the coherent interaction processes between the attosecond pulse and the quasi-harmonics. We find that many features of the interference fringes in the absorption spectra of the attosecond pulse can be attributed to the coherence phase difference. However, the modulation signals of laser-induced sidebands of the dark state is found related to the population dynamics of the dark state by the dressing field.
We present an analytical model capable of describing two-photon ionization of atoms with attosecond pulses in the presence of intermediate and final isolated autoionizing states. The model is based on the finite-pulse formulation of second-order time-dependent perturbation theory. It approximates the intermediate and final states with Fanos theory for resonant continua, and it depends on a small set of atomic parameters that can either be obtained from separate emph{ab initio} calculations, or be extracted from few selected experiments. We use the model to compute the two-photon resonant photoelectron spectrum of helium below the N=2 threshold for the RABITT (Reconstruction of Attosecond Beating by Interference of Two-photon Transitions) pump-probe scheme, in which an XUV attosecond pulse train is used in association to a weak IR probe, obtaining results in quantitative agreement with those from accurate emph{ab initio} simulations. In particular, we show that: i) Use of finite pulses results in a homogeneous red shift of the RABITT beating frequency, as well as a resonant modulation of the beating frequency in proximity of intermediate autoionizing states; ii) The phase of resonant two-photon amplitudes generally experiences a continuous excursion as a function of the intermediate detuning, with either zero or $2pi$ overall variation.
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