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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE

Temporal analysis of processes induced by a resonant laser in a dense In vapor

Paola Bicchi, Claudio Marinelli, Mario Meucci, L. Moi

Published Sep 24, 1993• 0 citations
Publisher

Abstract

This work illustrates the temporal analysis we have done on the fluorescence signals originating from levels with pecularly different characteristics populated either via Energy Pooling Collision (EPC) or via Energy Pooling Ionization (EPI). The fluorescence from the first excited level (S ia) gives informations about the limited radiation trapping due the fine structure of the ground state l/2 3/2 the ones from the 1 1P and 5D levels allow to discriminate between the different population mechanism, EPC and EPI respectively. The cross sections for the two different processes may also be obtained.

DOI
10.1117/12.155682

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The quantitative investigation of the energy pooling collision (EPC) process between resonantly laser excited In atoms is reported. The process is studied in a laser induced fluorescence (LIF) experiment where the nP populations, with n=11, 10 and 9, are monitored. The population mechanism for these levels is verified via a temporal analysis of the fluorescence signals. This is possible in In due to the strongly reduced self trapping of the resonant radiation. The cross section for energy pooling collision to these nP levels has been derived by considering the Rydberg character of these levels.

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[Collisional energy transfer between excited Rb atoms].

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Energy pooling (EP) was observed in Rb vapor following pulsed optical excitation to the 5P1/2 state. The 5P3/2 state was populated by the energy transfer process: Rb(5P1/2)+Rb(5S1/2) --> Rb(5P3/2)+Rb(5Sl/2). The resulting densities of Rb atoms at the 5P1/2 level were obtained from the absorption of narrow spectral line from a Rb hollow cathode lamp, connecting the 5P1/2 state to 7S state. Since the effective lifetimes of the 5P1/2 and 5P3/2 states are approximately equal, the densities of the 5P3/2 level were obtained from the D2 to D1 fluorescence ratios where D1 and D2 are lines of the 5P1/2 --> 5S1/2 and 5P3/2 --> 5S1/2 transition. Because the time of the fine structure exchanging is much shorter than the lifetime of the 5D state, the fluorescence originating from the 5D state produced by the 5P1/2 + 5P3/2 and 5P3/2 + 5P3/2 processes follows the instantaneous production rate of the 5P1/2 + 5P1/2 process. It is clear that 5P/2 + 5P3/2 and 5P3/2 + 5P3/2 collisions can significantly influence the results obtained for the 5P1/2 + 5P1/2 rate since the energy defect for 5D state is much smaller for 5P1/2 + 5P3/2 and 5P3/2 + 5P3/2 collisions than for 5P1/2 + 5P1/2 collisions. Effective lifetimes of the 5P levels were calculated using radiation trapping theory. The time-integrated populations and signals were studied and analyzed. The resulting fluorescence included the direct component emitted in the decay of the optically excited 5P1/2 state and the sensitized component arising from the collisions for populating 5D state at different cell temperature. These relative intensities were combined with the measured excited atom densities to yield absolute energy-pooling rate coefficients. The cross sections (in units of 10(-14) cm2) for the energy-pooling collisions [i. e. , 5P1/2 + 5P1/2, 5P1/2 + 5P3/2, 5P3/2 + 5P3/2] are 0.78, 2.9 and 3.1, respectively. The dependence of the rates upon energy defect deltaE was examined, but the 5D3/2 level was approximately equally populated in 5P3/2 + 5P3/2 (deltaE = 68 cm(-1)) and 5P3/2 + 5P1/2 (deltaE = 306 cm(-1)) collisions. The 5P1/2 + 5P3/2 collisions are as efficient as 5P3/2 + 5P3/2 for populating 5D3/2 state.

•Aug 1, 2009•1 citation
This work illustrates the temporal analysis we have done on the fluorescence signals originating from levels with pecularly different characteristics populated either via Energy Pooling Collision (EPC) or via Energy Pooling Ionization (EPI). The fluorescence from the first excited level (S ia) gives informations about the limited radiation trapping due the fine structure of the ground state l/2 3/2 the ones from the 1 1P and 5D levels allow to discriminate between the different population mechanism, EPC and EPI respectively. The cross sections for the two different processes may also be obtained.
The quantitative investigation of the energy pooling collision (EPC) process between resonantly laser excited In atoms is reported. The process is studied in a laser induced fluorescence (LIF) experiment where the nP populations, with n=11, 10 and 9, are monitored. The population mechanism for these levels is verified via a temporal analysis of the fluorescence signals. This is possible in In due to the strongly reduced self trapping of the resonant radiation. The cross section for energy pooling collision to these nP levels has been derived by considering the Rydberg character of these levels.
In this paper we report on the atomic population redistribution originating from the ionization that takes place in a dense Ga vapour kept in quartz cells and resonantly excited by laser radiation, in the collisions between two excited atoms. This ionization process is known as energy-pooling ionization (EPI). The electron/ion recombination that takes place in the low density plasma produced gives rise to population in the atomic Rydberg levels and from the latter via cascade transitions to lower lying ones. We have monitored the fluorescences relative to the radiative emissions from such levels, namely those corresponding to the n P → 5S 1/2 series, with 9 ≤ n ≤ 26, and the 4D → 4P 1/2,3/2 transitions. Their characteristics testify to their origin as being due to the EPI process. Further confirmation is obtained by performing a time-resolved analysis of such fluorescences, whose appearance and time evolution is strongly influenced by the dynamics of the process. The effect of the introduction of a few Torr of buffer gas inside the quartz cell, resulting in the quenching of all the fluorescences for n ≥ 12, is also discussed.
The production of Rydberg atoms via collisions in a resonantly laser excited dense In vapour is reported. When a dense In vapour confined in a quartz cell, whose temperature is raised above 820 °C, is excited by 100 kW cm−2 laser pulses at 410.3 nm, resonant with the fundamental transition 5 2P1/2 → 6 2S1/2, the fluorescence spectrum shows radiative emissions from Rydberg states, namely those corresponding to the n 2P → 6 2S1/2 series with 9 ≤ n ≤ 23. Fluorescences corresponding to the 5 2D → 5 2P1/2,3/2 transitions are also observed. Analysis of these signals' intensity as a function of several different experimental parameters, such as the atomic density and the laser power density, indicates that the population in the Rydberg levels is produced mainly by energy pooling collisions (EPC). The EPC cross section for the population of the Rydberg levels is also given. The influence on these effects of the presence of a fine structure in the In ground state (5 2P1/2,3/2) is also discussed, as well as the presence of a buffer gas inside the quartz cell.
We report on the electronic detection of the energy-pooling ionization (EPI) process in resonantly laser-excited gallium vapour. The formation of electrons and ions in the collision of two Ga atoms excited to the 5 2 S 1/2 level is analysed as a function of several different parameters such as the laser power density, the atomic density and the temperature. The influence of the strong chemical reactivity of Ga at high temperatures on the process is also evidenced. Finally the cross section for the EPI process is derived from the electronic signals detected. It turns out to be (1.1±0.5)×10 -15 cm 2 , a large value that states EPI as a very efficient process in Ga vapour.
Energy pooling (EP) was observed in Rb vapor following pulsed optical excitation to the 5P1/2 state. The 5P3/2 state was populated by the energy transfer process: Rb(5P1/2)+Rb(5S1/2) --> Rb(5P3/2)+Rb(5Sl/2). The resulting densities of Rb atoms at the 5P1/2 level were obtained from the absorption of narrow spectral line from a Rb hollow cathode lamp, connecting the 5P1/2 state to 7S state. Since the effective lifetimes of the 5P1/2 and 5P3/2 states are approximately equal, the densities of the 5P3/2 level were obtained from the D2 to D1 fluorescence ratios where D1 and D2 are lines of the 5P1/2 --> 5S1/2 and 5P3/2 --> 5S1/2 transition. Because the time of the fine structure exchanging is much shorter than the lifetime of the 5D state, the fluorescence originating from the 5D state produced by the 5P1/2 + 5P3/2 and 5P3/2 + 5P3/2 processes follows the instantaneous production rate of the 5P1/2 + 5P1/2 process. It is clear that 5P/2 + 5P3/2 and 5P3/2 + 5P3/2 collisions can significantly influence the results obtained for the 5P1/2 + 5P1/2 rate since the energy defect for 5D state is much smaller for 5P1/2 + 5P3/2 and 5P3/2 + 5P3/2 collisions than for 5P1/2 + 5P1/2 collisions. Effective lifetimes of the 5P levels were calculated using radiation trapping theory. The time-integrated populations and signals were studied and analyzed. The resulting fluorescence included the direct component emitted in the decay of the optically excited 5P1/2 state and the sensitized component arising from the collisions for populating 5D state at different cell temperature. These relative intensities were combined with the measured excited atom densities to yield absolute energy-pooling rate coefficients. The cross sections (in units of 10(-14) cm2) for the energy-pooling collisions [i. e. , 5P1/2 + 5P1/2, 5P1/2 + 5P3/2, 5P3/2 + 5P3/2] are 0.78, 2.9 and 3.1, respectively. The dependence of the rates upon energy defect deltaE was examined, but the 5D3/2 level was approximately equally populated in 5P3/2 + 5P3/2 (deltaE = 68 cm(-1)) and 5P3/2 + 5P1/2 (deltaE = 306 cm(-1)) collisions. The 5P1/2 + 5P3/2 collisions are as efficient as 5P3/2 + 5P3/2 for populating 5D3/2 state.