Ab-initio Theory of Photoionization via Resonances

Abstract

We present an \emph{ab-initio} approach for computing the photoionization spectrum near autoionization resonances in multi-electron systems. While traditional (Hermitian) theories typically require computing the continuum states, which are difficult to obtain with high accuracy, our non-Hermitian approach requires only discrete bound and metastable states, which are accurately computed with advanced quantum chemistry tools. We derive a simple formula for the absorption lineshape near Fano resonances, which relates the asymmetry of the spectral peaks to the phase of the complex transition dipole moment. Additionally, we present a formula for the ionization spectrum of laser-driven targets and relate the `Autler-Townes' splitting of spectral lines to the existence of exceptional points in the Hamiltonian. We apply our formulas to compute the autoionization spectrum of helium, but our theory is also applicable for non-trivial multi-electron atoms and molecules.

arXiv comment10 pages, 3 figures. arXiv admin note: text overlap with arXiv:1809.02868

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Cited by in corpus (4)

• Quantum Computing for Atomic and Molecular Resonances
• Quasinormal mode as a foundational framework for all electromagnetic Fano resonances
• Equations of motion governing the dynamics of the exceptional points of parameterically dependent nonhermitian Hamiltonians
• Complex time method for quantum dynamics when an exceptional point is encircled in the parameter space