Two-photon cross-section calculations for krypton in the 190–220 nm range

This paper presents multi-path, two-photon excitation cross-section calculations for krypton, using first-order perturbation theory. For evaluation of the two-photon-transition matrix element, this paper formulates the two-photon cross-section calculation as a matrix mechanics problem. From a finite basis of states, consisting of 4p, 5s, 6s, 7s, 5p, 6p, 4d, 5d, and 6d orbitals, electric dipole matrix elements are constructed, and a Green’s function is expressed as a truncated, spectral expansion of solutions, satisfying the Schrödinger equation. Electric dipole matrix elements are evaluated via tabulated oscillator strengths, and where those are unavailable, quantum-defect theory is used. The relative magnitudes of two-photon cross-sections for eight krypton lines in the 190–220 nm range are compared to experimental excitation spectra with good agreement. This work provides fundamental physical understanding of the Kr atom, which adds to experimental observations of relative fluorescence intensity. This is valuable when comparing excitation schemes in different environments for krypton fluorescence experiments. We conclude that two-photon excitation at 212.556 nm is optimal for single-laser, krypton tagging velocimetry or krypton planar laser-induced fluorescence.