$R$-matrix with Time-dependence Theory for Ultrafast Atomic Processes in Arbitrary Light Fields

Abstract

We describe an ab initio and non-perturbative $R$-matrix with time-dependence theory for ultrafast atomic processes in light fields of arbitrary polarization. The theory is applicable to complex, multielectron atoms and atomic ions subject to ultrashort (particularly few-femtosecond and attosecond) laser pulses with any given ellipticity, and generalizes previous time-dependent $R$-matrix techniques restricted to linearly polarized fields. We discuss both the fundamental equations, required to propagate the multielectron wavefunction in time, as well as the computational developments necessary for their efficient numerical solution. To verify the accuracy of our approach, we investigate the two-photon ionization of He, irradiated by a pair of time-delayed, circularly polarized, femtosecond laser pulses, and compare photoelectron momentum distributions, in the polarization plane, with those obtained from recent time-dependent close-coupling calculations. The predictive capabilities of our approach are further demonstrated through a study of single-photon detachment from F${}^{-}$ in a circularly polarized, femtosecond laser pulse, where the relative contribution of the co- and counter-rotating $2p$ electrons is quantified.

16 pages, 3 figures

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• It is all about phases: ultrafast holographic photoelectron imaging
• RMT: R-matrix with time-dependence. Solving the semi-relativistic, time-dependent Schrodinger equation for general, multi-electron atoms and molecules in intense, ultrashort, arbitrarily polarized laser pulses
• Manipulating Twisted Electrons in Strong-Field Ionization
• Dialogue on analytical and ab initio methods in attoscience
• Modeling tomographic measurements of photoelectron vortices in counter-rotating circularly polarized laser pulses
• Conservation laws for Electron Vortices in Strong-Field Ionisation
• Atomic photoionization dynamics in ultrashort cycloidal laser fields
• Electron rotational asymmetry in strong-field photodetachment from F${}^{-}$ by circularly polarized laser pulses
• Density-based one-dimensional model potentials for strong-field simulations in $\text{He}$, ${\text{H}}_2^{+}$ and ${\text{H}}_2$
• Electron correlation and short-range dynamics in attosecond angular streaking
• Ellipticity Dependence of Excitation and Ionization of Argon Atoms by Short-Pulse Infrared Radiation
• Implementation of gauge-invariant time-dependent configuration interaction singles method for three-dimensional atoms
• Ionization and excitation of low-lying circular states of the hydrogen atom in strong circularly polarized laser fields
• Enhancing spin polarization using ultrafast angular streaking
• Time-dependent Hole States in Multiconfigurational Time-Dependent Hartree-Fock Approaches: Applications in Photoionization of Water Molecule