Multiphoton Single Ionization Research Articles

Doubly excited electron-ion angular momentum transfer in parity-unfavored multiphoton ionization

We observe the parity-unfavored photoelectron emission in multiphoton single ionization of krypton atoms in an intense ultraviolet laser field. With systematic experiments of successively varying the light ellipticity and intensity, we identify that this parity-unfavored emission is associated with the first excited ionic state via a resonant pathway. We reveal an abnormal Coulomb asymmetry of the parity-unfavored photoelectron emission in elliptically polarized fields when the ellipticity is less than 0.3. The simulation using the time-dependent Schr\odinger equation based on single-active-electron approximation fails to reproduce the experiment. We attribute the experimental observations to the angular momentum correlation between the resonantly excited electron and the spin-orbit excited ion. Our results demonstrate that the well-known picture of the angular momentum transfer in multiphoton ionization is broken and instead that the electron shares the spin angular momenta of photons with the ion as an effect of electron correlations.

Photon Energy Deposition in Strong-Field Single Ionization of Multielectron Molecules

Molecules exposed to strong laser fields may coherently absorb multiple photons and deposit the energy into electrons and nuclei, triggering the succeeding dynamics as the primary stage of the light-molecule interaction. We experimentally explore the electron-nuclear sharing of the absorbed photon energy in above-threshold multiphoton single ionization of multielectron molecules. Using CO as a prototype, vibrational and orbital resolved electron-nuclear sharing of the photon energy is observed. Different from the simplest one- or two-electron systems, the participation of the multiple orbitals and the coupling of various electronic states in the strong-field ionization and dissociation processes alter the photon energy deposition dynamics of the multielectron molecule. The population of numerous vibrational states of the molecular cation as the energy reservoir in the ionization process plays an important role in photon energy sharing between the emitted electron and the nuclear fragments.

Multiphoton single ionization of two-electron systems in intense laser fields

Multiphoton single-ionization of a two-electron system (He and He-like ions) in intense circularly polarized laser field is reported in a relativistic field theoretic method. Coulomb-correction factor is introduced to estimate the effect of the Coulomb field of the residual ion on the rate. Antisymmetric wave function is considered both in the initial and in the final state. The spin-specific currents are calculated. Angular asymmetry in current generation is noted with the change in the spin direction of the ionized electron. Coulomb-corrected relativistic-result for total rate is compared with the Coulomb-corrected nonrelativistic KFR rate. At the high-intensity regime nonrelativistic rate overestimates the relativistic rate. Formation of orthopositronium and parapositronium from positronium negative ion by multiphoton ionization is discussed.

Theory of multiphoton single and double ionization of two-electron atomic systems driven by short-wavelength electric fields: Anab initiotreatment

We give a detailed account of an ab initio computational treatment of multiphoton single ionization (with or without excitation) as well as double ionization of two-electron atoms exposed to short-wavelength electric fields. This treatment is time dependent and based on a spectral method of configuration interaction type combined with Jacobi or $J$-matrix calculations. It involves a complete treatment of electron-electron correlation in the initial and final states as well as during the time propagation. The atom eigenvalue problem is first solved by means of the spectral method. It consists of expanding the atom wave function in a basis of products of complex Coulomb-Sturmian functions of the electron radial coordinates and bipolar harmonics of the angular coordinates. This method allows a high-resolution study of many atomic states, in particular high-lying singly excited states as well as many doubly excited states. Results for He are presented and discussed in detail. The time-dependent Schr\"odinger equation is then solved by means of an explicit scheme of Runge-Kutta type. An accurate calculation of the probability of single and double ionization is carried out by projecting the ionizing wave packet on fully correlated multichannel scattering wave functions generated by means of the $J$-matrix method. After a detailed analysis of the accuracy of this method, we show that our results for the total cross section of one-photon single and double ionization of He and ${\mathrm{H}}^{\ensuremath{-}}$ are in very good agreement with those obtained by the most sophisticated approaches. Two-photon double ionization of He is then considered, and results are presented in a frequency regime where substantial discrepancies subsist between all existing calculations. Our results demonstrate that electron correlations in the final state play a significant role.

Ionization rates for He, Ne, and Ar subjected to laser light with wavelengths between 248.6 and390nm

Using the $R$-matrix Floquet approach, we have investigated multiphoton single ionization of helium, neon, and argon subjected to laser light with a wavelength between 248.6 and $390\phantom{\rule{0.3em}{0ex}}\mathrm{nm}$. For a wavelength of $390\phantom{\rule{0.3em}{0ex}}\mathrm{nm}$, we have investigated ionization rates for Ne and Ar at intensities up to $2.5\ifmmode\times\else\texttimes\fi{}{10}^{14}\phantom{\rule{0.3em}{0ex}}\mathrm{W}∕{\mathrm{cm}}^{2}$. In this intensity regime, the ionization rates no longer follow the multiphoton ${I}^{N}$ power law. At an intensity of $2\ifmmode\times\else\texttimes\fi{}{10}^{14}\phantom{\rule{0.3em}{0ex}}\mathrm{W}∕{\mathrm{cm}}^{2}$, a tunneling model approximates the Ar ionization rates within a factor 3, but the differences are much larger for Ne. The ionization rates at $390\phantom{\rule{0.3em}{0ex}}\mathrm{nm}$ are affected by intermediate resonances, with these resonances both enhancing and inhibiting ionization. Multiphoton ionization cross sections for Ne and Ar at $248.6\phantom{\rule{0.3em}{0ex}}\mathrm{nm}$ have also been determined.