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Physical Review A

Calculation of the optical pumping parameters for electron-superelastic-scattering experiments from the sodium 3 2 P3/2 level

Peter M. Farrell, W. R. MacGillivray, M. C. Standage

Published Aug 1, 1991• 28 citations
Publisher

Abstract

The optical pumping parameters that modify the pure-state pseudo-Stokes parameters in an electron-superelastic-scattering experiment are calculated for the 3 $^{2}$${\mathit{S}}_{1/2}$(F=2)--${3}^{2}$${\mathit{P}}_{3/2}$(F) transitions of Na. A QED model is used to describe the laser excitation. It is found, that while the magnitude of the pumping parameter K' associated with circularly polarized excitation is close to unity for other than weak laser intensities, the value of the parameter K, associated with linearly polarized light, differs significantly from unity and is dependent on such experimental conditions as laser intensity, laser detuning, laser beam profile, and the Doppler width of the atomic transition. Methods for measuring K are suggested.

DOI
10.1103/physreva.44.1828

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Superelastic electron scattering from the laser-excited 32P3/2 level of Na

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The atomic collision parameters ?, ?, ?, ?, P, |P| and |�| were determined from measurements of the pseudo Stokes parameters for superelastic scattering of 20 eV incident electrons at angles of 10� and 15� from the 32P312 excited state of sodium. Two depolarising factors K and K' for the pseudo Stokes parameters are defined for it and a laser excitation respectively to account for the depolarising influence due to optical pumping in the hyperfine structure of the 32P3t2 excited state. A theoretical model of the laser excitation of the sodium transition is developed to determine K and K'. The theory developed is a quantum -electrodynamic description of the resonant interaction of monochromatic light with the 32S in(F'=2) <-> 32P3a(F=3,2,1) hyperfine transitions of the sodium D2 line formualated in terms of the Heisenberg atomic operator. Off diagonal state coherences and all relaxation terms are included. It is found that the equations for the populations, optical coherences and certain state coherences form a closed subset of the total system of equations. This subset is sufficiently small to enable numerical computation. As well as K and K', the model is used to calculate the probability of occupation of the various atomic states and the polarisation of the sideways scattered fluorescence from the laser excited atoms. The results of this model are compared with the predictions of four other models, a rate equation model which includes only the F=3 excited state, a semiclassical model based on the density operator, a low light intensity approximation to the semiclassical model and a high intensity model which uses a transformed basis for the states. For both it and a laser excitation it is shown that the QED calculated values converge to the values predicted by the high and low intensity approximations in the appropriate limits.

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Collisions studies using optically state selected beams is discussed. Measurements of spin resolved differential cross sections for superelastic scattering of electrons from excited sodium atoms (3P) are reported. The excited states are prepared by laser optical pumping with circularly polarized light thus giving a pure atomic state before the collision. A crossed beam arrangement of sodium atoms and electrons is used with a scattered electron detector. Scattered electron intensity as a function of scattering angle, incident electron energy, and relative orientation of the incident electronic and atomic spins is measured. 8 refs., 10 figs.

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Electron scattering from the optically prepared 3P state of sodium

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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.

•Jan 1, 1998•0 citations
The optical pumping parameters that modify the pure-state pseudo-Stokes parameters in an electron-superelastic-scattering experiment are calculated for the 3 ^{2}$${\mathit{S}}_{1/2}(F=2)--{3}^{2}$${\mathit{P}}_{3/2}(F) transitions of Na. A QED model is used to describe the laser excitation. It is found, that while the magnitude of the pumping parameter K' associated with circularly polarized excitation is close to unity for other than weak laser intensities, the value of the parameter K, associated with linearly polarized light, differs significantly from unity and is dependent on such experimental conditions as laser intensity, laser detuning, laser beam profile, and the Doppler width of the atomic transition. Methods for measuring K are suggested.
The atomic collision parameters ?, ?, ?, ?, P, |P| and |�| were determined from measurements of the pseudo Stokes parameters for superelastic scattering of 20 eV incident electrons at angles of 10� and 15� from the 32P312 excited state of sodium. Two depolarising factors K and K' for the pseudo Stokes parameters are defined for it and a laser excitation respectively to account for the depolarising influence due to optical pumping in the hyperfine structure of the 32P3t2 excited state. A theoretical model of the laser excitation of the sodium transition is developed to determine K and K'. The theory developed is a quantum -electrodynamic description of the resonant interaction of monochromatic light with the 32S in(F'=2) <-> 32P3a(F=3,2,1) hyperfine transitions of the sodium D2 line formualated in terms of the Heisenberg atomic operator. Off diagonal state coherences and all relaxation terms are included. It is found that the equations for the populations, optical coherences and certain state coherences form a closed subset of the total system of equations. This subset is sufficiently small to enable numerical computation. As well as K and K', the model is used to calculate the probability of occupation of the various atomic states and the polarisation of the sideways scattered fluorescence from the laser excited atoms. The results of this model are compared with the predictions of four other models, a rate equation model which includes only the F=3 excited state, a semiclassical model based on the density operator, a low light intensity approximation to the semiclassical model and a high intensity model which uses a transformed basis for the states. For both it and a laser excitation it is shown that the QED calculated values converge to the values predicted by the high and low intensity approximations in the appropriate limits.
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.
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.
Collisions studies using optically state selected beams is discussed. Measurements of spin resolved differential cross sections for superelastic scattering of electrons from excited sodium atoms (3P) are reported. The excited states are prepared by laser optical pumping with circularly polarized light thus giving a pure atomic state before the collision. A crossed beam arrangement of sodium atoms and electrons is used with a scattered electron detector. Scattered electron intensity as a function of scattering angle, incident electron energy, and relative orientation of the incident electronic and atomic spins is measured. 8 refs., 10 figs.
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.
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.