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Journal of the Optical Society of America B

Observation of laser-enhanced radiative transfer of barium 6s6p^1P_1 to 6s5d^1D_2 by means of fluorescence-dip detection

Lei Xu, You-yuan Zhao, Guoyi Wang, Mao-Qi He, Zhaoyong Wang

Published Jul 1, 1992• 2 citations
Publisher

Abstract

We report that the nonspontaneous radiative (amplified spontaneous emission or superradiation) relaxation of barium 6s6p1P1 to 6s5d1D2 from the laser-excited upper state was enhanced by laser light that was set resonant with the 6s5d1D2–5d6p1F3 transition to deplete the lower-state population. To our knowledge, this was the first use of fluorescence-dip observation to investigate this laser-enhanced emission process.

DOI
10.1364/josab.9.001017

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We report that the nonspontaneous radiative (amplified spontaneous emission or superradiation) relaxation of barium 6s6p1P1 to 6s5d1D2 from the laser-excited upper state was enhanced by laser light that was set resonant with the 6s5d1D2–5d6p1F3 transition to deplete the lower-state population. To our knowledge, this was the first use of fluorescence-dip observation to investigate this laser-enhanced emission process.
This is the first reported demonstration of the use of pair-absorption transitions for optically pumping lasers. In a mixture of barium and thallium metal vapors, single-photon absorption of 3867-A laser light caused simultaneous excitation of colliding ground-state atoms to the Ba(6s6p 1P1(o)) and Tl(6p 2P(3/2)(o)) excited states. Excited-state densities of about 10(14) cm(-3) were created, and subsequent laser emission on the Ba(6s6p 1PI(o)) - Ba(6s5d 1D2) atomic transition at 1.5 microm was observed.
Time-resolved measurements of fluorescence and level populations have been made on barium vapour illuminated by an intense pulse of laser radiation (1 MW cm -2 , 50 ns FWHM) tuned to the resonance transition of Ba I, 6s 2 1 S 0 -6s6p 1 P 1 , at 5535 AA. Barium number densities between 10 13 -10 15 cm -3 were investigated, using a buffer gas of helium at 100 Torr. Fluorescence was measured with two different geometrical arrangements, one allowing partial spatial resolution. In neither case did the observed fluorescence saturate with increasing laser power, although the maximum flux was more than sufficient to burn through the vapour column, as confirmed by transmission measurements. The power loss from the laser beam was found to be compatible with the scattered radiation from the pumped column in the absence of radiation trapping. In contrast to other similar experiments, no significant ionisation was detected (<5%). Time-resolved population measurements by anomalous dispersion on the 6s6p 3 P 2 and 6s5d 1 D 2 metastable levels yielded quenching cross sections for both Ba-Ba and Ba-He collisions, but gave anomalous result for the peak populations. A qualitative explanation of the fluorescence anomaly is proposed on the basis of the AC Stark effect, and it is shown that the same effect can inhibit the onset of stimulated emission to the metastable D levels.
Using two CW dye lasers barium Rydberg states were populated by stepwise two-photon absorption via the 6s6p 1 P 1 intermediate level. Monitoring the transmission of the first laser beam, tuned to the resonance line, and scanning the second laser across the upper atomic transition, a greatly enhanced signal was observed. Taking optical pumping into account, a simple rate equation model can quantitatively describe the increase in sensitivity. This technique was applied to measure the hyperfine structure of the 6s15d 1 D 2 Rydberg state in barium.
We present a time resolved study of excitation transfer processes between the low lying excited states of barium (6s6p 3^{3}3PJ{\mathit{P}}_{\mathit{J}}PJ​, 6s5d 1^{1}1D2{\mathit{D}}_{2}D2​, 6s5d 3^{3}3DJ{\mathit{D}}_{\mathit{J}}DJ​) induced by collisions with noble gases. The transient excited state populations have been measured by means of fluorescence and absorption spectroscopy. Cross sections for spin-changing collisions from 3^{3}3P1{\mathit{P}}_{1}P1​ to 1^{1}1D2{\mathit{D}}_{2}D2​ and from 1^{1}1D2{\mathit{D}}_{2}D2​ to 3^{3}3D3{\mathit{D}}_{3}D3​ as well as for fine-structure mixing within the 3^{3}3D multiplet were obtained by fitting the numerical solution of a seven-state system of rate equations including diffusion to the experimental data. We compare our results to experimental findings for other alkaline earth metals and report an improved value of the lifetime of the 6s6p 3^{3}3P1{\mathit{P}}_{1}P1​ state of barium.