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Register a new userTwo-photon finite-pulse model for resonant transitions in attosecond experiments
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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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We present an analytical model that characterizes two-photon transitions in the presence of autoionising states. We applied this model to interpret resonant RABITT spectra, and show that, as a harmonic traverses a resonance, the phase of the sideband beating significantly varies with photon energy. This phase variation is generally very different from the $pi$ jump observed in previous works, in which the direct path contribution was negligible. We illustrate the possible phase profiles arising in resonant two-photon transitions with an intuitive geometrical representation.
We present the first demonstration of two-photon double ionization of neon using an intense extreme ultraviolet (XUV) attosecond pulse train (APT) in a photon energy regime where both direct and sequential mechanisms are allowed. For an APT generated through high-order harmonic generation (HHG) in argon we achieve a total pulse energy close to 1 $mu$J, a central energy of 35 eV and a total bandwidth of $sim30$ eV. The APT is focused by broadband optics in a neon gas target to an intensity of $3cdot10^{12} $W$cdot$cm$^{-2}$. By tuning the photon energy across the threshold for the sequential process the double ionization signal can be turned on and off, indicating that the two-photon double ionization predominantly occurs through a sequential process. The demonstrated performance opens up possibilities for future XUV-XUV pump-probe experiments with attosecond temporal resolution in a photon energy range where it is possible to unravel the dynamics behind direct vs. sequential double ionization and the associated electron correlation effects.
A new theoretical approach to the description of the attosecond streaking measurements of atomic photoionization is presented. It is a fully quantum mechanical description based on numerical solving of the time-dependent Schroedinger equation which includes the atomic field as well as the fields of the XUV and IR pulses. Also a simple semiempirical description based on sudden approximation is suggested which agrees very well with the exact solution.
We theoretically explore a variant of RABBITT spectroscopy in which the attosecond-pulse train comprises isolated pairs of consecutive harmonics of the fundamental infrared probe frequency. In this scheme, one-photon and two-photon amplitudes interfere resulting in an asymmetric photoelectron emission. This interferometric principle has the potential of giving access to the time-resolved ionization of systems that exhibit autoionizing states, since it imprints the group delay of both one-photon and two-photon resonant transitions in the energy-resolved photoelectron anisotropy as a function of the pump-probe time delay. To bring to the fore the connection between the pump-probe ionization process and its perturbative analysis, on the the one side, and the underlying field-free scattering observables as well as the radiative couplings in the target system, on the other side, we test this scheme with an exactly solvable analytical one-dimensional model that supports both bound states and shape-resonances. The asymmetric photoelectron emission near a resonance is computed using perturbation theory as well as solving the time-dependent Schodinger equation; the results are in excellent agreement with the field-free resonant scattering properties of the model.
We investigate the interaction of Xe with isolated attosecond XUV pulses. Specifically, we calculate the ion yields and determine the pathways leading to the formation of ionic charged states up to Xe$^{5+}$. To do so, in our formulation we account for single-photon absorption, sequential multi-photon absorption, direct two-photon absorption, single and double Auger decays, and shake-off. We compare our results for the ion yields and for ion yield ratios with recent experimental results obtained for 93 eV and 115 eV attosecond XUV pulses. In particular, we investigate the role that a sequence of two single-photon ionization processes plays in the formation of Xe$^{4+}$. We find that each one of these two processes ionizes a core electron and thus leads to the formation of a double core-hole state. Remarkably, we find that the formation of Xe$^{5+}$ involves a direct two-photon absorption process and the absorption of a total of three photons.
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