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THE 6s5d 1 D2 ! 6s5d 3 DJ EXCITATION ENERGY TRANSFER IN BARIUM INDUCED BY COLLISIONS WITH He, Ar AND Xe ATOMS

Cedomil Vadla, Vlasta Horvatić

Published Jan 1, 1995• 3 citations
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Abstract

the description of the population and depopulation processes of the Ba metastable states in noble gas atmosphere. The analysis of the experimental results, within the assumed model, yields the following cross-section values for the investigated

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Excitation transfer in barium by collisions with noble gases

J. Brust, Alan C. Gallagher

We present a time resolved study of excitation transfer processes between the low lying excited states of barium (6s6p $^{3}$${\mathit{P}}_{\mathit{J}}$, 6s5d $^{1}$${\mathit{D}}_{2}$, 6s5d $^{3}$${\mathit{D}}_{\mathit{J}}$) induced by collisions with noble gases. The transient excited state populations have been measured by means of fluorescence and absorption spectroscopy. Cross sections for spin-changing collisions from $^{3}$${\mathit{P}}_{1}$ to $^{1}$${\mathit{D}}_{2}$ and from $^{1}$${\mathit{D}}_{2}$ to $^{3}$${\mathit{D}}_{3}$ as well as for fine-structure mixing within the $^{3}$D multiplet were obtained by fitting the numerical solution of a seven-state system of rate equations including diffusion to the experimental data. We compare our results to experimental findings for other alkaline earth metals and report an improved value of the lifetime of the 6s6p $^{3}$${\mathit{P}}_{1}$ state of barium.

Physical Review A•Sep 1, 1995•34 citations

Diffusion of barium atoms in the 6s5d 3 DJ metastable levels and the 6 s2 1 S0 ground state through noble-gas perturbers

R. K. Namiotka, E. Ehrlacher, J. Sagle +5 more

We describe a set of experiments that investigate diffusion of barium 6s5d${\mathrm{}}^{3}$${\mathit{D}}_{\mathit{J}}$ metastable level and 6${\mathit{s}}^{2}$${\mathrm{}}^{1}$${\mathit{S}}_{0}$ ground-state atoms through the noble gases: He, Ne, Ar, Kr, and Xe. The barium metastable levels were populated through optical pumping of the 6${\mathit{s}}^{2}$${\mathrm{}}^{1}$${\mathit{S}}_{0}$\ensuremath{\rightarrow}6s6p${\mathrm{}}^{3}$${\mathit{P}}_{1}^{\mathit{o}}$ intercombination transition with a pulsed laser, followed by spontaneous or stimulated emission into the 6s5d${\mathrm{}}^{3}$${\mathit{D}}_{1,2}$ levels. Collisional mixing then distributed population throughout the 6s5d${\mathrm{}}^{3}$${\mathit{D}}_{\mathit{J}}$ levels. A weak narrow-band cw laser was tuned to appropriate transitions to probe the spatial distribution of metastable level atoms, as well as the hole created in the ground-state spatial distribution, by the pulsed laser. Time-dependent absorption coefficients were obtained by measuring the transmission of the probe laser at several different pump-probe spatial separations. From these absorption data, spatial number density profiles were mapped out for various times following the firing of the pump laser. These density profiles were used to determine the diffusion coefficient for each state at a particular buffer-gas pressure and temperature. From these pressure- and temperature-dependent diffusion coefficients D, we determined the thermally averaged diffusion cross sections ${\mathrm{\ensuremath{\sigma}}}_{\mathit{D}}$(6s5d${\mathrm{}}^{3}$${\mathit{D}}_{\mathit{J}}$) and ${\mathrm{\ensuremath{\sigma}}}_{\mathit{D}}$(6${\mathit{s}}^{2}$${\mathrm{}}^{1}$${\mathit{S}}_{0}$) for the metastable and ground-state atoms diffusing through the noble gases, respectively. We also report values for the scaled standard diffusion coefficients ${\mathit{D}}_{0}$. Our experimental values of the thermally averaged diffusion cross sections ${\mathrm{\ensuremath{\sigma}}}_{\mathit{D}}$(6s5d${\mathrm{}}^{3}$${\mathit{D}}_{\mathit{J}}$) and ${\mathrm{\ensuremath{\sigma}}}_{\mathit{D}}$(6${\mathit{s}}^{2}$${\mathrm{}}^{1}$${\mathit{S}}_{0}$) for the barium-helium system are compared with values calculated from published, theoretical barium-helium potentials and the agreement is excellent. \textcopyright{} 1996 The American Physical Society.

Physical Review A•Jul 1, 1996•16 citations

Population and deactivation of lowest lying barium levels by collisions with He, Ar, Xe and Ba ground state atoms

Cedomil Vadla, Kay Niemax, Vlasta Horvatić +1 more

Zeitschrift für Physik D Atoms Molecules and Clusters•Sep 1, 1995•34 citations

Diffusion of barium atoms in the 6s5d triplet-D(J) levels and the 6s(2) singlet-S(0) ground state through noble gas perturbers

Raychel Kristine Namiotka

•May 1, 1998•0 citations

Excitation transfer among, and quenching of, the barium 6s5d 3 DJ metastable levels due to collisions with argon, nitrogen, and barium perturbers

E. Ehrlacher, John Huennekens

We describe a set of experiments that investigate excitation transfer among the barium 6s5d $^{3}$${\mathit{D}}_{\mathit{J}}$ metastable levels due to collisions with argon perturber atoms, and quenching of atoms in these levels by nitrogen perturber molecules. The metastable levels were populated through optical pumping of the 6${\mathit{s}}^{2}$ $^{1}$${\mathit{S}}_{0}$\ensuremath{\rightarrow}6s6p $^{3}$${\mathit{P}}_{1}^{\mathit{o}}$ intercombination transition with a pulsed laser, followed by stimulated emission or stimulated Raman scattering into the 6s5d $^{3}$${\mathit{D}}_{1,2}$ levels. Collisional mixing then distributed population throughout the $^{3}$${\mathit{D}}_{\mathit{J}}$ levels. Time-dependent absorption coefficients were obtained by measuring the transmission of a weak cw probe laser beam (after the pulsed laser fired) at several perturber number densities. Argon buffer gas was used to investigate fine-structure mixing, and nitrogen was used to study quenching. The time-dependent absorption coefficients were fitted to appropriate fitting functions, obtained by solving the set of coupled rate equations used to model the time evolution of the metastable level populations. The buildup rates of the initially unpopulated $^{3}$${\mathit{D}}_{3}$ and underpopulated $^{3}$${\mathit{D}}_{1}$ levels were used to determine the collisional mixing rates, while the measured decay rates of the $^{3}$${\mathit{D}}_{\mathit{J}}$ level populations yielded the quenching rates. From plots of buildup rates versus argon number density for the $^{3}$${\mathit{D}}_{1,3}$ states, we were able to determine four of the six fine-structure mixing rate coefficients ${\mathit{k}}_{\mathit{i}\mathit{j}}$.The results are ${\mathit{k}}_{12}$=(1.71\ifmmode\pm\else\textpm\fi{}0.18), ${\mathit{k}}_{21}$=(1.39\ifmmode\pm\else\textpm\fi{}0.13), ${\mathit{k}}_{23}$=(1.42\ifmmode\pm\else\textpm\fi{}0.13), and ${\mathit{k}}_{32}$=(1.92\ifmmode\pm\else\textpm\fi{}0.16)\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}13}$ ${\mathrm{cm}}^{3}$ ${\mathrm{s}}^{\mathrm{\ensuremath{-}}1}$. The experiment is not sensitive to the values of ${\mathit{k}}_{13}$ and ${\mathit{k}}_{31}$. Estimated rate coefficients for excitation transfer among the $^{3}$${\mathit{D}}_{\mathit{J}}$ levels due to collisions with barium atoms are ${\mathit{k}}_{21}^{\mathrm{Ba}}$=1.3\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}10}$ ${\mathrm{cm}}^{3}$ ${\mathrm{s}}^{\mathrm{\ensuremath{-}}1}$ and ${\mathit{k}}_{23}^{\mathrm{Ba}}$=5.8\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}10}$ ${\mathrm{cm}}^{3}$ ${\mathrm{s}}^{\mathrm{\ensuremath{-}}1}$. A plot of the population decay rates versus ${\mathrm{N}}_{2}$ number density for each of the three metastable levels yielded the average nitrogen quenching rate coefficient ${\mathit{k}}_{\mathit{q}}$=(3.14\ifmmode\pm\else\textpm\fi{}0.19)\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}11}$ ${\mathrm{cm}}^{3}$ ${\mathrm{s}}^{\mathrm{\ensuremath{-}}1}$.

Physical Review A•Dec 1, 1994•26 citations

Collisional Deactivation of Ba 5d7p 3D1 by Noble Gases

John E. Smedley, Sarah K. Coulter, Edward J. Felton +1 more

Collisional deactivation of the 5d7p (3)D1 state of Ba by noble gases is studied by time- and wavelength-resolved fluorescence techniques. A pulsed, frequency-doubled dye laser at 273.9 nm excites the 5d7p (3)D1 level from the ground state, and fluorescence at 364.1 and 366.6 nm from the 5d7p (3)D1 --> 6s5d (3)D1 and 5d7p (3)D1 --> 6s5d (3)D2 transitions, respectively, is monitored in real time to obtain the deactivation rate constants. At 835 K these rate constants are as follows: He, (1.69 +/- 0.08) x 10(-9) cm(3) s(-1); Ne, (3.93 +/- 0.14) x 10(-10) cm(3) s(-1); Ar, (4.53 +/- 0.15) x 10(-10) cm(3) s(-1); Kr, (4.64 +/- 0.13) x 10(-10) cm(3) s(-1); Xe, (5.59 +/- 0.22) x 10(-10) cm(3) s(-1). From time-resolved 5d7p (3)D1 emission in the absence of noble gas and from the intercepts of the quenching plots, the lifetime of this state is determined to be 100 +/- 1 ns. Using time- and wavelength-resolved Ba emission with a low background pressure of noble gas, radiative lifetimes of several near-resonant states are determined from the exponential rise of the fluorescence signals. These results are as follows: 5d6d (3)D3, 28 +/- 3 ns; 5d7p (3)P1, 46 +/- 2 ns; 5d6d (3)G3, 21.5 +/- 0.8 ns; 5d7p (3)F3, 48 +/- 1 ns. Integrated fluorescence signals are used to infer the relative rate constants for population transfer from the 5d7p (3)D1 state to eleven near-resonant fine structure states.

The Journal of Physical Chemistry A•Jul 17, 2008•5 citations
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.
We describe a set of experiments that investigate diffusion of barium 6s5d3{\mathrm{}}^{3}3DJ{\mathit{D}}_{\mathit{J}}DJ​ metastable level and 6s2{\mathit{s}}^{2}s21{\mathrm{}}^{1}1S0{\mathit{S}}_{0}S0​ ground-state atoms through the noble gases: He, Ne, Ar, Kr, and Xe. The barium metastable levels were populated through optical pumping of the 6s2{\mathit{s}}^{2}s21{\mathrm{}}^{1}1S0{\mathit{S}}_{0}S0​\ensuremath{\rightarrow}6s6p3{\mathrm{}}^{3}3P1o{\mathit{P}}_{1}^{\mathit{o}}P1o​ intercombination transition with a pulsed laser, followed by spontaneous or stimulated emission into the 6s5d3{\mathrm{}}^{3}3D1,2{\mathit{D}}_{1,2}D1,2​ levels. Collisional mixing then distributed population throughout the 6s5d3{\mathrm{}}^{3}3DJ{\mathit{D}}_{\mathit{J}}DJ​ levels. A weak narrow-band cw laser was tuned to appropriate transitions to probe the spatial distribution of metastable level atoms, as well as the hole created in the ground-state spatial distribution, by the pulsed laser. Time-dependent absorption coefficients were obtained by measuring the transmission of the probe laser at several different pump-probe spatial separations. From these absorption data, spatial number density profiles were mapped out for various times following the firing of the pump laser. These density profiles were used to determine the diffusion coefficient for each state at a particular buffer-gas pressure and temperature. From these pressure- and temperature-dependent diffusion coefficients D, we determined the thermally averaged diffusion cross sections ${\mathrm{\ensuremath{\sigma}}}_{\mathit{D}}$(6s5d3{\mathrm{}}^{3}3DJ{\mathit{D}}_{\mathit{J}}DJ​) and ${\mathrm{\ensuremath{\sigma}}}_{\mathit{D}}$(6s2{\mathit{s}}^{2}s21{\mathrm{}}^{1}1S0{\mathit{S}}_{0}S0​) for the metastable and ground-state atoms diffusing through the noble gases, respectively. We also report values for the scaled standard diffusion coefficients D0{\mathit{D}}_{0}D0​. Our experimental values of the thermally averaged diffusion cross sections ${\mathrm{\ensuremath{\sigma}}}_{\mathit{D}}$(6s5d3{\mathrm{}}^{3}3DJ{\mathit{D}}_{\mathit{J}}DJ​) and ${\mathrm{\ensuremath{\sigma}}}_{\mathit{D}}$(6s2{\mathit{s}}^{2}s21{\mathrm{}}^{1}1S0{\mathit{S}}_{0}S0​) for the barium-helium system are compared with values calculated from published, theoretical barium-helium potentials and the agreement is excellent. \textcopyright{} 1996 The American Physical Society.
We describe a set of experiments that investigate excitation transfer among the barium 6s5d 3^{3}3DJ{\mathit{D}}_{\mathit{J}}DJ​ 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 6s2{\mathit{s}}^{2}s2 1^{1}1S0{\mathit{S}}_{0}S0​\ensuremath{\rightarrow}6s6p 3^{3}3P1o{\mathit{P}}_{1}^{\mathit{o}}P1o​ intercombination transition with a pulsed laser, followed by stimulated emission or stimulated Raman scattering into the 6s5d 3^{3}3D1,2{\mathit{D}}_{1,2}D1,2​ levels. Collisional mixing then distributed population throughout the 3^{3}3DJ{\mathit{D}}_{\mathit{J}}DJ​ 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 3^{3}3D3{\mathit{D}}_{3}D3​ and underpopulated 3^{3}3D1{\mathit{D}}_{1}D1​ levels were used to determine the collisional mixing rates, while the measured decay rates of the 3^{3}3DJ{\mathit{D}}_{\mathit{J}}DJ​ level populations yielded the quenching rates. From plots of buildup rates versus argon number density for the 3^{3}3D1,3{\mathit{D}}_{1,3}D1,3​ states, we were able to determine four of the six fine-structure mixing rate coefficients kij{\mathit{k}}_{\mathit{i}\mathit{j}}kij​.The results are k12{\mathit{k}}_{12}k12​=(1.71\ifmmode\pm\else\textpm\fi{}0.18), k21{\mathit{k}}_{21}k21​=(1.39\ifmmode\pm\else\textpm\fi{}0.13), k23{\mathit{k}}_{23}k23​=(1.42\ifmmode\pm\else\textpm\fi{}0.13), and k32{\mathit{k}}_{32}k32​=(1.92\ifmmode\pm\else\textpm\fi{}0.16)\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}13}$ cm3{\mathrm{cm}}^{3}cm3 ${\mathrm{s}}^{\mathrm{\ensuremath{-}}1}$. The experiment is not sensitive to the values of k13{\mathit{k}}_{13}k13​ and k31{\mathit{k}}_{31}k31​. Estimated rate coefficients for excitation transfer among the 3^{3}3DJ{\mathit{D}}_{\mathit{J}}DJ​ levels due to collisions with barium atoms are k21Ba{\mathit{k}}_{21}^{\mathrm{Ba}}k21Ba​=1.3\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}10}$ cm3{\mathrm{cm}}^{3}cm3 ${\mathrm{s}}^{\mathrm{\ensuremath{-}}1}$ and k23Ba{\mathit{k}}_{23}^{\mathrm{Ba}}k23Ba​=5.8\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}10}$ cm3{\mathrm{cm}}^{3}cm3 ${\mathrm{s}}^{\mathrm{\ensuremath{-}}1}$. A plot of the population decay rates versus N2{\mathrm{N}}_{2}N2​ number density for each of the three metastable levels yielded the average nitrogen quenching rate coefficient kq{\mathit{k}}_{\mathit{q}}kq​=(3.14\ifmmode\pm\else\textpm\fi{}0.19)\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}11}$ cm3{\mathrm{cm}}^{3}cm3 ${\mathrm{s}}^{\mathrm{\ensuremath{-}}1}$.
Collisional deactivation of the 5d7p (3)D1 state of Ba by noble gases is studied by time- and wavelength-resolved fluorescence techniques. A pulsed, frequency-doubled dye laser at 273.9 nm excites the 5d7p (3)D1 level from the ground state, and fluorescence at 364.1 and 366.6 nm from the 5d7p (3)D1 --> 6s5d (3)D1 and 5d7p (3)D1 --> 6s5d (3)D2 transitions, respectively, is monitored in real time to obtain the deactivation rate constants. At 835 K these rate constants are as follows: He, (1.69 +/- 0.08) x 10(-9) cm(3) s(-1); Ne, (3.93 +/- 0.14) x 10(-10) cm(3) s(-1); Ar, (4.53 +/- 0.15) x 10(-10) cm(3) s(-1); Kr, (4.64 +/- 0.13) x 10(-10) cm(3) s(-1); Xe, (5.59 +/- 0.22) x 10(-10) cm(3) s(-1). From time-resolved 5d7p (3)D1 emission in the absence of noble gas and from the intercepts of the quenching plots, the lifetime of this state is determined to be 100 +/- 1 ns. Using time- and wavelength-resolved Ba emission with a low background pressure of noble gas, radiative lifetimes of several near-resonant states are determined from the exponential rise of the fluorescence signals. These results are as follows: 5d6d (3)D3, 28 +/- 3 ns; 5d7p (3)P1, 46 +/- 2 ns; 5d6d (3)G3, 21.5 +/- 0.8 ns; 5d7p (3)F3, 48 +/- 1 ns. Integrated fluorescence signals are used to infer the relative rate constants for population transfer from the 5d7p (3)D1 state to eleven near-resonant fine structure states.