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Photoelectron spectroscopy of laser-dressed atomic helium

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 Added by Severin Meister
 Publication date 2020
  fields Physics
and research's language is English




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Photoelectron emission from excited states of laser-dressed atomic helium is analyzed with respect to laser intensity-dependent excitation energy shifts and angular distributions. In the two-color XUV (exteme ultra-violet) -- IR (infrared) measurement, the XUV photon energy is scanned between SI{20.4}{electronvolt} and the ionization threshold at SI{24.6}{electronvolt}, revealing electric dipole-forbidden transitions for a temporally overlapping IR pulse ($sim!SI{e12}{wattper centimetersquared}$). The interpretation of the experimental results is supported by numerically solving the time-dependent Schrodinger equation in a single-active-electron approximation.



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314 - Luca Argenti , Eva Lindroth 2021
We describe a numerical method that simulates the interaction of the helium atom with sequences of femtosecond and attosecond light pulses. The method, which is based on the close-coupling expansion of the electronic configuration space in a B-spline bipolar spherical harmonic basis, can accurately reproduce the excitation and single ionization of the atom, within the electrostatic approximation. The time dependent Schrodinger equation is integrated with a sequence of second-order split-exponential unitary propagators. The asymptotic channel-, energy- and angularly-resolved photoelectron distributions are computed by projecting the wavepacket at the end of the simulation on the multichannel scattering states of the atom, which are separately computed within the same close-coupling basis. This method is applied to simulate the pump-probe ionization of helium in the vicinity of the $2s/2p$ excitation threshold of the He$^+$ ion. This work confirms the qualitative conclusions of one of our earliest publications [L Argenti and E Lindroth, Phys. Rev. Lett. {bf 105}, 53002 (2010)], in which we demonstrated the control of the $2s/2p$ ionization branching-ratio. Here, we take those calculations to convergence and show how correlation brings the periodic modulation of the branching ratios in almost phase opposition. The residual total ionization probability to the $2s+2p$ channels is dominated by the beating between the $sp_{2,3}^+$ and the $sp_{2,4}^+$ doubly excited states, which is consistent with the modulation of the complementary signal in the $1s$ channel, measured in 2010 by Chang and co-workers~[S Gilbertson~emph{et al.}, Phys. Rev. Lett. {bf 105}, 263003 (2010)].
The derivation of approximate wave functions for an electron submitted to both a coulomb and a time-dependent laser electric fields, the so-called Coulomb-Volkov (CV) state, is addressed. Despite its derivation for continuum states does not exhibit any particular problem within the framework of the standard theory of quantum mechanics (QM), difficulties arise when considering an initially bound atomic state. Indeed the natural way of translating the unperturbed momentum by the laser vector potential is no longer possible since a bound state does not exhibit a plane wave form including explicitely a momentum. The use of a fractal space permits to naturally define a momentum for a bound wave function. Within this framework, it is shown how the derivation of laser-dressed bound states can be performed. Based on a generalized eikonal approach, a new expression for the laser-dressed states is also derived, fully symmetric relative to the continuum or bound nature of the initial unperturbed wave function. It includes an additional crossed term in the Volkov phase which was not obtained within the standard theory of quantum mechanics. The derivations within this fractal framework have highlighted other possible ways to derive approximate laser-dressed states in QM. After comparing the various obtained wave functions, an application to the prediction of the ionization probability of hydrogen targets by attosecond XUV pulses within the sudden approximation is provided. This approach allows to make predictions in various regimes depending on the laser intensity, going from the non-resonant multiphoton absorption to tunneling and barrier-suppression ionization.
In dense atomic gases the interaction between transition dipoles and photons leads to the formation of many-body states with collective dissipation and long-ranged forces. Despite decades of research, a full understanding of this paradigmatic many-body problem is still lacking. Here, we put forward and explore a scenario in which a dense atomic gas is weakly excited by an off-resonant laser field. We develop the theory for describing such dressed many-body ensembles and show that collective excitations are responsible for the emergence of many-body interactions, i.e. effective potentials that cannot be represented as a sum of binary terms. We illustrate how interaction effects may be probed through microwave spectroscopy via the analysis of time-dependent line-shifts, and show that these signals are sensitive to the phase pattern of the dressing laser. Our study offers a new perspective on dense atomic ensembles interacting with light and promotes this platform as a setting for the exploration of rich non-equilibrium many-body physics.
We develop the theory of propagation of laser wave in a gas of two-level atoms (with an optical transition frequency $omega^{}_0$) under the condition of inhomogeneous Doppler broadening, considering the self-consistent solution of the Maxwell-Bloch equations in the mean-field approximation and for one-atomic density matrix. The nonlinear effects in the atomic density $n$, caused by the free motion of atoms, are found. These effects distort the lineshape (shift, asymmetry, broadening), but are not associated with atom-atom interaction. Moreover, in the case $nk^{-3}_0<1$ (where $k^{}_0=omega^{}_0/c$) and temperatures $Tgtrsim 300$~K, these quasi-collective effects exceed the well-known influence of the dipole-dipole interatomic interaction (e.g., Lorentz-Lorenz shift) by more than one order of magnitude. It was also found that for some area of parameters, the frequency interval appears, within which the non-trivial self-consistent solution of the Maxwell-Bloch equations is absent at all. Thus, the physical picture of collective effects in a gas medium should be substantially revised.
We analyze several possibilities for precisely measuring electronic transitions in atomic helium by the direct use of phase-stabilized femtosecond frequency combs. Because the comb is self-calibrating and can be shifted into the ultraviolet spectral region via harmonic generation, it offers the prospect of greatly improved accuracy for UV and far-UV transitions. To take advantage of this accuracy an ultracold helium sample is needed. For measurements of the triplet spectrum a magneto-optical trap (MOT) can be used to cool and trap metastable 2^3S state atoms. We analyze schemes for measuring the two-photon $2^3S to 4^3S$ interval, and for resonant two-photon excitation to high Rydberg states, $2^3S to 3^3P to n^3S,D$. We also analyze experiments on the singlet-state spectrum. To accomplish this we propose schemes for producing and trapping ultracold helium in the 1^1S or 2^1S state via intercombination transitions. A particularly intriguing scenario is the possibility of measuring the $1^1S to 2^1S$ transition with extremely high accuracy by use of two-photon excitation in a magic wavelength trap that operates identically for both states. We predict a ``triple magic wavelength at 412 nm that could facilitate numerous experiments on trapped helium atoms, because here the polarizabilities of the 1^1S, 2^1S and 2^3S states are all similar, small, and positive.
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