Measurements of excited-state-to-excited-state transition probabilities and photoionization cross-sections using laser-induced fluorescence and photoionization signals

•Laser-induced photoionization and fluorescence signals have been simultaneously observed.•The density matrix formalism has been employed to analyze these signals.•Two-color laser-induced fluorescence was used to measure the second-step transition probability.•The second-step transition probability obtained was used to infer the photoionization cross-section.•Transition probability and photoionization cross-section have been measured in a single experiment.

Laser-induced photoionization and fluorescence signals were simultaneously observed in atomic samarium using Nd:YAG-pumped dye lasers. Two-color, three-photon photoionization and two-color fluorescence signals were recorded simultaneously as a function of the second-step laser power for two photoionization pathways. The density matrix formalism has been employed to analyze these signals. Two-color laser-induced fluorescence signal depends on the laser powers used for the first and second-step transitions as well as the first and second-step transition probability whereas two-color, three-photon photoionization signal depends on the third-step transition cross-section at the second-step laser wavelength along with the laser powers and transition probability for the first and second-step transitions. Two-color laser-induced fluorescence was used to measure the second-step transition probability. The second-step transition probability obtained was used to infer the photoionization cross-section. Thus, the methodology combining two-color, three-photon photoionization and two-color fluorescence signals in a single experiment has been established for the first time to measure the second-step transition probability as well as the photoionization cross-section.