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Applied Optics

Optical Excitation of Mercury Vapor for the Production of Isolated Fluorescence

Ralph Zito, A. E. Schraeder

Published Dec 1, 1963• 5 citations
Publisher

Abstract

Empirical data are presented for the preliminary intensity and resolution measurements made in the multiple-step induced fluorescence of mercury vapor. The primary application contemplated for such a process is the production of an isolated source of visible radiation in three-dimensional space. A dual optical excitation process is employed in conjunction with inelastic foreign gas molecule collision for the resultant spontaneous, visible fluorescence of excited mercury atoms. Details of the experimental apparatus and techniques employed are also given.

DOI
10.1364/ao.2.001323

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A new type of electron/photon coincidence experiment is presented which utilises a laser -electron stepwise excitation technique to prepare atoms in an excited state. An electron collision initially excites an atom from the ground state to an intermediate state. Following this electron excitation process, coherent single mode laser radiation further excites the atom to an upper state, from which the fluorescence is observed. The nature of the laser excitation transfers both amplitude and phase information about the electron excited state to the upper excited state in a coherent way. This information is extracted from the upper state fluorescence by analysis of the fluorescence polarization in coincidence with the electron scattered from the atom for particular polarizations of the laser radiation. The coincidence technique allows an identically prepared sub -ensemble of excited atoms to be selected for measurement. The electron excited state studied was the 61131 state of mercury, excited by a beam of unpolarized electrons at an impact energy of 16 eV. The mercury atomic beam was isotopically selected following electron excitation using the narrow bandwidth of the laser radiation. Excitation from the electron excited 61P1 state was via 579 nm laser radiation to the 61D2 state and fluorescence was monitored from this state to the 63P1 state via a 313 nm transition. Stokes parameters were measured for two different laser polarization angles, since this allowed a complete set of collision parameters to be deduced for a single experimental geometry. Results for three different scattering angles at this energy are presented. The laser excitation process was modelled in both the weak and the strong laser excitation regimes. A perturbation approach developed to model single photon laser excitation allowed the collision parameters to be extracted from the measured coincidence Stokes parameters analytically, whereas a Quantum Electrodynamic model allowed high laser intensity effects on the coincidence signal to be explored theoretically. The Quantum Electrodynamic model indicated that the weak excitation model could be used to extract the collision parameters from the Stokes parameters at the laser intensities used in the experiment. Effects due to variation of the laser intensity were predicted from the Quantum Electrodynamic model and experiments conducted to test these predictions are presented. Collision parameters deduced from the measured stepwise coincidence Stokes parameters following optimization of the experimental conditions are presented. These parameters are compared qualitatively with existing data from heavy atomic systems and with a theoretical model based upon the Distorted Wave Born Approximation. Similarities between the experimental data are found, however significant discrepancies are noted between the parameters obtained here and with the predictions of the theoretical model.

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Sensitized fluorescence in thallium induced in collisions with Hg(63P1) atoms

Murray K Wade, M. Czajkowski, L. Krause

The transfer of excitation from excited mercury atoms to ground-state thallium atoms was investigated using techniques of sensitized fluorescence. A Hg–Tl vapor mixture contained in a quartz cell was irradiated with Hg 2537 Å resonance radiation which caused the mercury atoms to become excited to the 63P1, state. Subsequent collisions between the Hg(63P1) and Tl(62P1/2) atoms resulted in the population of the 82S1/2, 62D, and 72S1/2 thallium states, whose decay gave rise to sensitized fluorescence of wavelengths 3231, 3520, 3776, and 5352 Å. Intensity measurements on the sensitized fluorescence and on the Hg 2537 Å resonance fluorescence, observed at right angles to the direction of excitation, yielded cross sections of 3.0, 0.3, and 0.05 Å2 for collisional excitation transfer from Hg(63P1) to the 82S1/2, 62D, and 72S1/2 states in thallium, respectively. The results are fully consistent with previously determined cross sections for excitation transfer in other binary metallic vapor systems.

Canadian Journal of Physics•Jul 1, 1978•10 citations
Empirical data are presented for the preliminary intensity and resolution measurements made in the multiple-step induced fluorescence of mercury vapor. The primary application contemplated for such a process is the production of an isolated source of visible radiation in three-dimensional space. A dual optical excitation process is employed in conjunction with inelastic foreign gas molecule collision for the resultant spontaneous, visible fluorescence of excited mercury atoms. Details of the experimental apparatus and techniques employed are also given.
Empirical data are presented for the preliminary intensity and resolution measurements made in the multiple-step induced fluorescencof mercury vapor. The primary contemplated application for such a process is the production of an isolated source of visible radiation in three-dimensional space. A dual optical excitation process is employed in conjunction with inelastic foreign gas molecule collision for the resultant spontaneous, visible fluorescence of excited mercury atoms. Details of the experimental apparatus and techniques employed are also given. (Author)
In the course of studying a multiple-step excitation process in mercury vapor for the possible application to a three-dimensional display of data, an analysis of the fluorescence mechanism was made. A dual optical-excitation process is employed by which mercury vapor is caused to radiate at a localized region in space. The radiation is in the ultraviolet and visible portions of the spectrum. A partial analysis and pertinent literature review is presented here for the resonance absorption and reradiation of light energy by mercury vapor at room temperature.
Effect of nitrogen and of mixtures of nitrogen and carbon dioxide upon the fluorescence of mercury vapor. By "stepwise" optical excitation, unexcited mercury atoms are raised to the 23S12^{3}S_{1}23S1​ state. They may leave this level upon the emission of radiation by four paths---the first to the 21P12^{1}P_{1}21P1​ state, a transition of relatively low probability, and the other three to the 23P22^{3}P_{2}23P2​, 23P12^{3}P_{1}23P1​, and 23P02^{3}P_{0}23P0​ states with the emission of 5461A, 4358A and 4046A, respectively. Measurements, by totally independent methods, of the mean life of the 23S12^{3}S_{1}23S1​ state yielded values, when measured by the line 5461A, equal to approximately four times those when measured by either 4358A or 4046A. Upon the addition of foreign gas, then, the intensity ratio of 5461A to either 4358A or 4046A should decrease with increasing pressure while that of 4046A to 4358A should remain constant. However, these ratios were all found to be invariant with pressure, up to 400 mm in the case of nitrogen and up to 100 mm in the case of the nitrogen-carbon dioxide mixtures.
Collisional transfer of excitation from mercury to sodium was investigated using methods of sensitized fluorescence. A mixture of mercury and sodium vapors at low pressure was irradiated with Hg 2537 Å resonance radiation, producing a population of Hg(63P1) atoms whose inelastic collisions with ground-state sodium atoms resulted in a transfer of excitation energy to close-lying S, P, and D states in sodium. The subsequent decay of these states manifested itself in the emission of a sensitized fluorescent spectrum. Absolute intensity measurements on the components of the spectrum yielded 21 cross sections whose magnitudes range from 0.02 to 38.5 Å2 and which exhibit a pronounced resonance with ΔE, the energy defect between Hg (63P1) and the appropriate level in sodium.
A new type of electron/photon coincidence experiment is presented which utilises a laser -electron stepwise excitation technique to prepare atoms in an excited state. An electron collision initially excites an atom from the ground state to an intermediate state. Following this electron excitation process, coherent single mode laser radiation further excites the atom to an upper state, from which the fluorescence is observed. The nature of the laser excitation transfers both amplitude and phase information about the electron excited state to the upper excited state in a coherent way. This information is extracted from the upper state fluorescence by analysis of the fluorescence polarization in coincidence with the electron scattered from the atom for particular polarizations of the laser radiation. The coincidence technique allows an identically prepared sub -ensemble of excited atoms to be selected for measurement. The electron excited state studied was the 61131 state of mercury, excited by a beam of unpolarized electrons at an impact energy of 16 eV. The mercury atomic beam was isotopically selected following electron excitation using the narrow bandwidth of the laser radiation. Excitation from the electron excited 61P1 state was via 579 nm laser radiation to the 61D2 state and fluorescence was monitored from this state to the 63P1 state via a 313 nm transition. Stokes parameters were measured for two different laser polarization angles, since this allowed a complete set of collision parameters to be deduced for a single experimental geometry. Results for three different scattering angles at this energy are presented. The laser excitation process was modelled in both the weak and the strong laser excitation regimes. A perturbation approach developed to model single photon laser excitation allowed the collision parameters to be extracted from the measured coincidence Stokes parameters analytically, whereas a Quantum Electrodynamic model allowed high laser intensity effects on the coincidence signal to be explored theoretically. The Quantum Electrodynamic model indicated that the weak excitation model could be used to extract the collision parameters from the Stokes parameters at the laser intensities used in the experiment. Effects due to variation of the laser intensity were predicted from the Quantum Electrodynamic model and experiments conducted to test these predictions are presented. Collision parameters deduced from the measured stepwise coincidence Stokes parameters following optimization of the experimental conditions are presented. These parameters are compared qualitatively with existing data from heavy atomic systems and with a theoretical model based upon the Distorted Wave Born Approximation. Similarities between the experimental data are found, however significant discrepancies are noted between the parameters obtained here and with the predictions of the theoretical model.
The transfer of excitation from excited mercury atoms to ground-state thallium atoms was investigated using techniques of sensitized fluorescence. A Hg–Tl vapor mixture contained in a quartz cell was irradiated with Hg 2537 Å resonance radiation which caused the mercury atoms to become excited to the 63P1, state. Subsequent collisions between the Hg(63P1) and Tl(62P1/2) atoms resulted in the population of the 82S1/2, 62D, and 72S1/2 thallium states, whose decay gave rise to sensitized fluorescence of wavelengths 3231, 3520, 3776, and 5352 Å. Intensity measurements on the sensitized fluorescence and on the Hg 2537 Å resonance fluorescence, observed at right angles to the direction of excitation, yielded cross sections of 3.0, 0.3, and 0.05 Å2 for collisional excitation transfer from Hg(63P1) to the 82S1/2, 62D, and 72S1/2 states in thallium, respectively. The results are fully consistent with previously determined cross sections for excitation transfer in other binary metallic vapor systems.