We describe a set of experiments that investigate excitation transfer among the barium 6s5d
3DJ metastable levels due to collisions with argon perturber atoms, and quenching of atoms in these levels by nitrogen perturber molecules. The metastable levels were populated through optical pumping of the 6
s2 1S0\ensuremath{\rightarrow}6s6p
3P1o intercombination transition with a pulsed laser, followed by stimulated emission or stimulated Raman scattering into the 6s5d
3D1,2 levels. Collisional mixing then distributed population throughout the
3DJ levels. Time-dependent absorption coefficients were obtained by measuring the transmission of a weak cw probe laser beam (after the pulsed laser fired) at several perturber number densities. Argon buffer gas was used to investigate fine-structure mixing, and nitrogen was used to study quenching. The time-dependent absorption coefficients were fitted to appropriate fitting functions, obtained by solving the set of coupled rate equations used to model the time evolution of the metastable level populations. The buildup rates of the initially unpopulated
3D3 and underpopulated
3D1 levels were used to determine the collisional mixing rates, while the measured decay rates of the
3DJ level populations yielded the quenching rates. From plots of buildup rates versus argon number density for the
3D1,3 states, we were able to determine four of the six fine-structure mixing rate coefficients
kij.The results are
k12=(1.71\ifmmode\pm\else\textpm\fi{}0.18),
k21=(1.39\ifmmode\pm\else\textpm\fi{}0.13),
k23=(1.42\ifmmode\pm\else\textpm\fi{}0.13), and
k32=(1.92\ifmmode\pm\else\textpm\fi{}0.16)\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}13}$
cm3 ${\mathrm{s}}^{\mathrm{\ensuremath{-}}1}$. The experiment is not sensitive to the values of
k13 and
k31. Estimated rate coefficients for excitation transfer among the
3DJ levels due to collisions with barium atoms are
k21Ba=1.3\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}10}$
cm3 ${\mathrm{s}}^{\mathrm{\ensuremath{-}}1}$ and
k23Ba=5.8\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}10}$
cm3 ${\mathrm{s}}^{\mathrm{\ensuremath{-}}1}$. A plot of the population decay rates versus
N2 number density for each of the three metastable levels yielded the average nitrogen quenching rate coefficient
kq=(3.14\ifmmode\pm\else\textpm\fi{}0.19)\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}11}$
cm3 ${\mathrm{s}}^{\mathrm{\ensuremath{-}}1}$.
The authors have studied collisional redistribution of near-resonance radiation in thallium vapour caused by collisions with argon buffer gas. Electronic Raman scattering and collision-induced fluorescence were spectrally resolved, both to the weakly populated metastable 6 2 P 3/2 level in thallium. Thus the problem with radiative trapping encountered in previous experiments is partially avoided. By measuring the total collision-induced fluorescence as a function of the incident laser frequency, the absolute collisional redistribution line shape is obtained.
We have measured the atomic lifetime of the argon 2 p 4 level by the laser-induced-fluorescence spectroscopy to be 30.5 ns. This contradicts the recent measurement using the high-frequency plused electron-beam excitation. We conjecture that, in their experiment, the radiation trapping not only affects the decay of the upper-level population but also relaxes the alignment initially produced by the electron-collision excitation in the upper-level population. Thus, the directly observed decay of the emission-line intensity is different from the decay of the upper-level population. We have observed the radiative relaxation of alignment on the neon 2 p 2 level which is a complementary effect to coherence narrowing.