Abstract

Recently, the $n{p}^3{\prod }_g\leftarrow 5s^3{\Sigma }_u^{+}$ Rydberg series of Kr₂ was observed in absorption.¹ Also, the higher members of the series were observed by dye laser excitation spectroscopy.² Both approaches examine the rare gas dimer states near the equilibrium internuclear separation. This paper describes the study of the $5p^3{\prod }_u{,}^3{\Sigma }_g^{+}\leftarrow 5s^3{\Sigma }_u^{+}$ inter-Rydberg transitions by dye laser excitation spectroscopy. These experiments involve producing the ${\text{Kr}}_2{}^3{\Sigma }_u^{+}$ species by two-photon excitation of atomic Kr followed by three-body formation of ${\text{Kr}}_2^{*}$. A subsequent dye laser pulse populates vibrational levels of the ${\text{Kr}}_{2}5p^3{\Sigma }_g^{+}$ and ³Π_g states. Production of a Rydberg state is detected by monitoring Kr 5p → 5s emission. The spectroscopy of the 5p³Π_g and ${}^3{\Sigma }_g^{+}$ states and their asymptotic structure are discussed. Also, the appearance of two-photon (sequential) absorption at high dye laser intensities is described.

© 1986 Optical Society of America