Highly sensitive detection of neutral Kr atoms was accomplished by the
use of laser-induced fluorescence. In one experiment, Kr at 40 parts
per 10(12) in He was detected at a signal-to-noise ratio of 500 by tim
e-resolved fluorescence measurements. The Kr metastable Iss level was
populated by cascade after two-photon excitation to the 2p(6) level by
the frequency-tripled output of a pulsed single-longitudinal-mode dye
laser. After a delay, when scattered laser light and cascade resonanc
e fluorescence became negligible, trace quantities of Kr were detected
by the use of a pulsed-laser pumping scheme. In a related experiment,
Kr-78/Kr-86 isotope ratios ranging from 1 to 0.1 were measured with a
resonant isotopic depletion technique first proposed by Makarov [Sov.
J. Quantum Electron. 13, 722 (1983)]. The Kr-86 metastable population
was selectively depleted by optical pumping to a higher-lying state t
hat relaxed to the ground state by means of radiative cascade. After t
he Kr-78/Kr-86 ratio of metastables had been enriched by a factor of 1
0, the Kr-78 population was probed by pulsed excitation. Premixed Kr-7
8/Kr-86 ratios were measured to within an accuracy of 10%, even for un
resolved, Doppler-broadened transitions.