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Physical Review A

Controlling atomic structures and photoabsorption processes by an infrared laser

Xiao‐Min Tong, Naoki Toshima

Published Jun 7, 2010• 32 citations
Publisher

Abstract

We propose a theoretical method to calculate the infrared (IR) laser-assisted photoabsorption cross sections over a broad energy range by a single calculation. In this method we define an initial wave function as the product of the dipole operator and the atomic ground state, propagate the initial wave function in the IR laser field with different initial phases, then calculate the generalized autocorrelation function, which is defined as the averaged value of the autocorrelation function over the initial phase from 0 to $2\ensuremath{\pi}$ (or one IR optical cycle). The IR laser-assisted photoabsorption cross sections are obtained by the Fourier transform of the generalized autocorrelation function. We apply this method to study the IR laser-assisted photoabsorption of He atoms. From the simulation results, we see that the IR laser field affects not only the resonant position but also the lifetime or the width of the bound states. This photoabsorption cross section is an important quantity to analyze the IR-laser-assisted dynamical processes by an attosecond pulse, a pulse train, or a free-electron laser.

DOI
10.1103/physreva.81.063403

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We propose a theoretical method to calculate the infrared (IR) laser-assisted photoabsorption cross sections over a broad energy range by a single calculation. In this method we define an initial wave function as the product of the dipole operator and the atomic ground state, propagate the initial wave function in the IR laser field with different initial phases, then calculate the generalized autocorrelation function, which is defined as the averaged value of the autocorrelation function over the initial phase from 0 to 2\ensuremathπ2\ensuremath{\pi}2\ensuremathπ (or one IR optical cycle). The IR laser-assisted photoabsorption cross sections are obtained by the Fourier transform of the generalized autocorrelation function. We apply this method to study the IR laser-assisted photoabsorption of He atoms. From the simulation results, we see that the IR laser field affects not only the resonant position but also the lifetime or the width of the bound states. This photoabsorption cross section is an important quantity to analyze the IR-laser-assisted dynamical processes by an attosecond pulse, a pulse train, or a free-electron laser.
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.
In the present paper, the time-resolved transient absorption spectroscopy of helium atoms is investigated based on the three-level modeling. The helium atoms are subjected to an extreme ultraviolet (XUV) attosecond pulse and a time-delayed infrared (IR) few-cycle laser field. The odd excited state are populated from the ground state by the XUV pulse due to the dipole selection rule, and probed by the time-delayed IR laser. The time-resolved transient absorption spectroscopy based on the different coupling mechanism demonstrate some different features, the photoabsorption spectrum based on three-level model with rotating wave approximation (RWA) cannot repeat the fast oscillation and the sideband structure which have been observed in the previous experimental investigation. The dressing effect of IR laser pulse on the ground state can contribute new interference structures in the photoabsorption spectrum.
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.
We theoretically study the infrared (IR)-dressed photoionization of atoms excited by extreme ultraviolet attosecond pulse trains above ionization threshold. The initial state of atoms is treated perturbatively by the IR field, and the continuum states are considered as Coulomb–Volkov (CV) waves. CV waves can much reduce the gauge difference calculated with Volkov waves, and, in general, the contribution of ground-state perturbation to the photoelectron spectrum is negligible. Our calculations show qualitative agreement with the experimental results [Phys. Rev. Lett. 95, 013001 (2005)]. An evident dependence of the photoelectron spectrum on the delay phase between the IR field and the attosecond pulse train is exhibited in both helium and argon. The angular distribution of photoelectrons with various IR polarizations and the corresponding photoelectron spectra are presented. The linearly polarized IR fields are shown to have a higher controlling capability of the spectrum via IR delay phases than the circularly polarized fields. On the other hand, the circularly polarized IR fields have a fruitful angular dependence of photoelectrons with various IR delay phases.