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Australian Journal of Physics

New Data from Laser Interrogation of Electron-Atom Collisions Experiments

AT Masters, Robert T. Sang, W. R. MacGillivray, M. C. Standage

Published Apr 1, 1996• 1 citation
Publisher

Abstract

Recent data from two methods in which high resolution laser radiation is used to assist in determining electron-atom collision parameters are presented. The electron superelastic method has yielded the first measurement of Stokes parameters for electron de-excitation of the 32D5/2–32P3/2,1/2 transition of atomic Na, the upper level having been optically prepared by resonant, stepwise excitation from the 32S1/2 ground level via the 32P3/2 level using two single mode lasers. As well, we report on the development of a model to determine the optical pumping parameters for superelastic scattering from the 32P3/2 level when it is prepared by two lasers exciting from the F = 1 and F = 2 states respectively of the 32S1/ 2 ground level. Data are also presented for collision parameters for the excitation of the 61So–61 PI transition of the I = 0 isotope of Hg by electrons of 50 eV incident energy. The technique employed for these measurements is the stepwise electron–laser excitation coincidence method, in which the electron excited atom is further excited by resonant laser radiation, and fluorescence photons emitted by relaxation from the laser excited state are detected in coincidence with the scattered electron.

DOI
10.1071/ph960499

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Recent data from two methods in which high resolution laser radiation is used to assist in determining electron-atom collision parameters are presented. The electron superelastic method has yielded the first measurement of Stokes parameters for electron de-excitation of the 32D5/2–32P3/2,1/2 transition of atomic Na, the upper level having been optically prepared by resonant, stepwise excitation from the 32S1/2 ground level via the 32P3/2 level using two single mode lasers. As well, we report on the development of a model to determine the optical pumping parameters for superelastic scattering from the 32P3/2 level when it is prepared by two lasers exciting from the F = 1 and F = 2 states respectively of the 32S1/ 2 ground level. Data are also presented for collision parameters for the excitation of the 61So–61 PI transition of the I = 0 isotope of Hg by electrons of 50 eV incident energy. The technique employed for these measurements is the stepwise electron–laser excitation coincidence method, in which the electron excited atom is further excited by resonant laser radiation, and fluorescence photons emitted by relaxation from the laser excited state are detected in coincidence with the scattered electron.
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.
This thesis presents the results of a series of experiments in which electrons are superelastically scattered from various laser excited states of sodium. The atoms, once in the optically prepared state, are forced to relax via the superelastic collision with an electron. The rate of detection of superelastically scattered electrons was measured as a function of the laser polarisation which enabled pseudo Stokes parameters to be determined. These pseudo Stokes parameters are functions of both optical pumping parameters and atomic collision parameters. The optical pumping parameters describe the laser-atom interaction and the atomic collision parameters describe the electron-atom collision process. Three different laser excitation mechanisms were used to optically pump the atoms into various excited states. The first of these used a single laser tuned to the 32S 112(F'=2 hyperfine state)-~32P312 transition. The excited atoms underwent a superelastic collision with an electron leaving the atom in the ground state and pseudo Stokes parameters were measured as a function of both scattering angle and incident electron energy. The second superelastic experiment, utilised a folded step excitation mechanism which employed two lasers tuned from the two hypethne states of the 32S112 ground state respectively to the 32P312 excited state. Power broadening effects in the single laser experiment cause the atoms to be optically pumped into the F= 1 hyperfine ground state. The laser powers used were not great enough to power broaden the hyperfine ground states and as such the F'= 1 sublevel effectively acted as a sink. The folded step excitation method enabled the excited state population to be increased so that data at larger scattering angles could be obtained. Stokes parameters from both of these experiments which had an incident energy range of 10eV to 30eV and an angular range of 5°-25° were compared to three current electron-atom scattering theories and previous experimental data. Overall, fair to good agreement was found between theory and experiments for the individual Stokes parameters. Losses of coherence was observed at small scattering angles (50.200) at 20eV and 25eV incident electron energies which were poorly modelled by the three different theories. The third superelastic experiment involved the use of two lasers of specified polarisation to stepwise excite the atoms to the 32D512 excited state. Superelastic collisions with incident electron energies of 20eV from the 32D512-*32P312~312 collision were studied at three different scattering angles and pseudo Stokes parameters for the case where the polarisations of the radiation from the lasers were parallel were measured. The single step and folded step laser-atom interactions for it excitation were modelled using a full quantum electrodynamical treatment so that the optical pumping parameters from the single and folded step experiments could be investigated. Equations of motion were derived in the Heisenberg picture and it is shown that for the single laser case 59 equations of motion are required to fully model the interaction and for the folded step ease 78 equations of motion are required. The results of calculations demonstrated that the optical pumping parameters were sensitive to laser intensity, laser detuning and the Doppler width of the atomic beam. The theoretical quantum electrodynamical calculation results were in good agreement with the experimental results.
A theoretical description is presented for the process in which photons emitted from atoms which have been stepwise excited firstly by electron impact and then by resonant interaction with coherent radiation are detected in coincidence with the inelastically scattered electrons. The optical excitation is modelled using a full quantum electrodynamic theory. Calculations of the Stokes parameters are performed for the Hg (I=0) scheme; electron excitation from the 6 1 S 0 ground state to the 6 1 P 1 state followed by resonant laser excitation to the 6 1 D 2 state, with analysis being performed on the fluorescence from the 6 1 D 2 -6 3 P 1 relaxation channel. It is found that for this case, even though manifestations of optical pumping are evident, the Stokes parameters do not vary by more than +or-4% from the weak intensity limit.
This paper reports on the extension of the electron superelastic scattering technique to three new situations. The first considers scattering from the 32P3/2 level of Na that has been excited by two laser modes tuned, respectively, to the transitions from the two hyperfine states of the 32S1/2 ground level. Both coherent and noncoherent modes are treated in a full quantum electrodynamic model of the laser excitation. Under certain conditions, the time-averaged probability of finding an atom in the 32P3/2 level exceeds 0.5. The second situation is electron superelastic scattering from the 32D5/2 level of Na that has been resonantly excited from the ground level via a resonant intermediate level. With the first observation of superelastically scattered electrons from this higher lying level recently recorded, this paper considers the extension of the quantum electrodynamics (QED) model to describe the optical excitation process. Application of superelastic scattering to the 52S1/2–52P3/2 transition of Rb is the third situation considered. The superelastic scattering formalism is extended to allow for a nonzero spin flip cross section for this transition. The resulting optical pumping terms are calculated using the QED model and the method of their determination for the superelastic scattering experiment described. The experimental design necessary to measure all of the collision parameters for this transition is discussed.
An experimental investigation of electron - impact induced transitions from the laser - excited 3P state of sodium atom to the 4S and 3D excited states is presented, the main objective being measurement of the atomic collision parameters ( ACPs ) that are related to individual scattering amplitudes. These parameters are complementary to the differential excitation cross - sections and provide finer details on the collisional excitation process. The experiment involved the preparation of the 3P - state with coherent laser radiation of a particular polarisation and measuring the rate of electrons scattered from the laser - excited state as function of laser polarisations. The ACPs were then deduced from these measurements and optical pumping parameters, which account for the optical preparation of the 3P - state. To formulate different measurement schemes, a measurement theory based on the general description of transitions between states of different angular momentum using density matrix formalism is derived. The investigation of the 3P - 4S transition is very similar to the studies of the 3S - 3P excitation performed by superelastic method involving the 3P - 3S scattering in the 'time - inverse' geometry. 'Standard' ACPs are used and, similarly to the superelastic method, the measurements for the 3P - 4S excitation performed in the 'time - inverse' geometry also reveal ACPs for the 4S - 3P de -excitation process. For the more complex 3P - 3D transition, however, the 'standard' ACPs may be less informative. It is shown that certain sums of individual magnetic sublevel excitation probabilities can be measured which may be considered as atomic collision parameters for transitions between P and D - states.