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International Laser Science Conference

Radiative scattering close-coupled calculations for isotope dependence of fine-structure branching in 3He-Na and 4He-Na optical collisions

Linda L. Vahala, Paul S. Julienne

Published Jan 1, 1986• 0 citations
Publisher

Abstract

Assume that collisional redistribution occurs in a collision of two atoms in scattering state i by absorption of a photon through an isolated molecular state a to an isolated molecular state b, followed by separation to excited product scattering state f. If the separation velocity of the two atoms is sufficiently large, the final state can be approximated by the same recoil limit which has been developed for photofragmentation.1 Our close coupling calculations on Na + He systems show how the recoil limit for fine-structure branching rations is approached for both red and blue detuning as product separation velocity increases. Comparisons are made between the lighter Na-He system at thermal energies and the heavier Na-He system.

DOI
10.1364/ils.1986.fd5

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Nonadiabatic theory of fine-structure branching cross sections for Na-He, Na-Ne, and Na-Ar optical collisions

Linda L. Vahala, Paul S. Julienne, Mark D. Havey

The nonadiabatic close-coupled theory of atomic collisions in a radiation field is generalized to include electron spin and is used to consider the weak-field Na--rare-gas (RG) optical collision Na${(}^{2}$${S}_{1/2}$)+RG+nh\ensuremath{\nu} \ensuremath{\mu}Na${(}^{2}$${\mathrm{P}}_{\mathrm{j}}$)+RG+(n-1)h\ensuremath{\nu}. The effects of detuning and incident energy on the branching into the atomic Na 3${p}^{2}$${P}_{3/2}$ and 3p $^{2}P_{1/2}$ states are examined. The cross sections \ensuremath{\sigma}(j) are found to have a strong asymmetry between red and blue detuning as well as a complex threshold and resonance structure dependence on energy. A partial cross-section analysis of \ensuremath{\sigma}(j) shows a significant difference between contributions from states of e and f molecular parity. The theoretically calculated detuning dependence of the branching ratio into each fine-structure state is in good agreement with available experimental data for Na-Ar, Na-Ne, and Na-He, as well as the total absorption coefficient for the production of Na 3p atoms. The fine-structure branching ratio for thermal energy collisions shows considerable variation with a rare-gas collision partner, due to the different interaction potentials. For sufficiently high collision energy, the branching approaches a recoil limit which is independent of collision partner.

Physical Review A•Sep 1, 1986•41 citations

Experimental fine-structure branching ratios for Na–rare-gas optical collisions

Mark D. Havey, F. T. Delahanty, Linda L. Vahala +1 more

Experimental ratios for branching into the fine-structure levels of the Na 3p multiplet, as a consequence of an optical collision with He, Ne, Ar, Kr, or Xe, are reported. The process studied is Na(3s $^{2}S_{1/2}$)+scrR+nh\ensuremath{\nu}\ensuremath{\rightarrow} Na(3p $^{2}P_{j}$)+scrR+(n-1)h\ensuremath{\nu} , where scrR represents a rare-gas atom and where the laser frequency \ensuremath{\nu} is tuned in the wings of the Na resonance transitions. The branching ratios are defined as I(D1)/I(D2) where I(D1) and I(D2) are measured intensities of the atomic Na D1 and D2 lines. The ratios are determined for detunings ranging from about 650 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$ in the blue wing to 170 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$ in the red wing of the Na 3p multiplet. The branching is found to be strongly detuning dependent in the vicinity of the NaAr, NaKr, and NaXe near-red-wing satellites. The blue-wing branching ratios show a detuning-dependent approach to a recoil, or sudden statistical, limit of 0.5, irrespective of the rare gas. Fine-structure changing cross sections have also been measured for resonant excitation of the Na 3p $^{2}P_{j}$ state; the results are consistent with cross sections obtained from wing excitation.

Physical Review A•Oct 1, 1986•21 citations

Experimental fine-structure branching ratios for Na-rare gas optical collisions

Mark D. Havey, F. T. Delahanty, Linda L. Vahala +1 more

Experimental ratios for branching into the fine‐structure levels of the Na 3p multiplet, as a consequence of an optical collision with He, Ne, Ar, Kr, or Xe, are reported. The process studied is Na(3s2S1/2) +RG+nhν → Na(3p2 Pj)+RG+(n−1)hν, where RG represents a rare gas atom and where the laser frequency ν is tuned in the wings of the Na resonance transitions. The branching ratios are defined as I(D1)/I(D2) where I(D1) and I(D2) are measured intensities of the atomic Na D1 and D2 lines. The ratios are determined for detunings ranging from about 650 cm−1 blue to 170 cm−1 red of the Na 3p multiplet. The branching is found to be strongly detuning dependent in the vicinity of the NaKr and NaXe near red‐wing satellites. The blue wing branching ratios show a detuning‐dependent approach to a recoil or sudden statistical limit of 0.5, irrespective of the rare gas.

AIP conference proceedings•Jan 1, 1986•0 citations

Nonadiabatic theory of atomic line broadening: Final-state distributions and the polarization of redistributed radiation

Paul S. Julienne, Frederick H. Mies

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Journal of the Optical Society of America B•Feb 1, 1987•0 citations

Depolarisation in Na-Ar optical collisions

Wolfgang Behmenburg, V. Kroop, Frank Rebentrost

The depolarisation of the redistributed Na D1and D2line fluorescence caused by Na-Ar collisions after far-wing excitation was investigated. In the limit of zero Ar density the J=1/2orientation and J=3/2alignment reflect the distribution among Zeeman sublevels of Na 32PJproduced after absorption of a photon into one or several excited Na-Ar molecular states at small internuclear separation, followed by a mixing between these states during dissociation. Measurements of these quantities as functions of the detuning up to Delta omegaJ=50 cm-1in the red wings are compared with quantum-mechanical coupled-channel (CC) calculations using realistic molecular potentials and thermal averaging, and with predictions from the factorisation approximation (FA) of the theory of redistribution. Fair agreement with CC calculations and FA predictions was obtained within the impact region, proving the validity of the factorisation assumption there. Outside this region the overall depolarisation is primarily due to reorientation of the Na 3P electronic angular momentum and is reproduced qualitatively by the CC calculations but not by the FA theory. Additional depolarisation connected with the fine-structure coupling was observed.

Journal of Physics B Atomic and Molecular Physics•Jul 14, 1985•19 citations
Assume that collisional redistribution occurs in a collision of two atoms in scattering state i by absorption of a photon through an isolated molecular state a to an isolated molecular state b, followed by separation to excited product scattering state f. If the separation velocity of the two atoms is sufficiently large, the final state can be approximated by the same recoil limit which has been developed for photofragmentation.1 Our close coupling calculations on Na + He systems show how the recoil limit for fine-structure branching rations is approached for both red and blue detuning as product separation velocity increases. Comparisons are made between the lighter Na-He system at thermal energies and the heavier Na-He system.
The nonadiabatic close-coupled theory of atomic collisions in a radiation field is generalized to include electron spin and is used to consider the weak-field Na--rare-gas (RG) optical collision Na(2{(}^{2}(2S1/2{S}_{1/2}S1/2​)+RG+nh\ensuremath{\nu} \ensuremath{\mu}Na(2{(}^{2}(2Pj{\mathrm{P}}_{\mathrm{j}}Pj​)+RG+(n-1)h\ensuremath{\nu}. The effects of detuning and incident energy on the branching into the atomic Na 3p2{p}^{2}p2P3/2{P}_{3/2}P3/2​ and 3p 2P1/2^{2}P_{1/2}2P1/2​ states are examined. The cross sections \ensuremath{\sigma}(j) are found to have a strong asymmetry between red and blue detuning as well as a complex threshold and resonance structure dependence on energy. A partial cross-section analysis of \ensuremath{\sigma}(j) shows a significant difference between contributions from states of e and f molecular parity. The theoretically calculated detuning dependence of the branching ratio into each fine-structure state is in good agreement with available experimental data for Na-Ar, Na-Ne, and Na-He, as well as the total absorption coefficient for the production of Na 3p atoms. The fine-structure branching ratio for thermal energy collisions shows considerable variation with a rare-gas collision partner, due to the different interaction potentials. For sufficiently high collision energy, the branching approaches a recoil limit which is independent of collision partner.
Experimental ratios for branching into the fine-structure levels of the Na 3p multiplet, as a consequence of an optical collision with He, Ne, Ar, Kr, or Xe, are reported. The process studied is Na(3s 2S1/2^{2}S_{1/2}2S1/2​)+scrR+nh\ensuremath{\nu}\ensuremath{\rightarrow} Na(3p 2Pj^{2}P_{j}2Pj​)+scrR+(n-1)h\ensuremath{\nu} , where scrR represents a rare-gas atom and where the laser frequency \ensuremath{\nu} is tuned in the wings of the Na resonance transitions. The branching ratios are defined as I(D1)/I(D2) where I(D1) and I(D2) are measured intensities of the atomic Na D1 and D2 lines. The ratios are determined for detunings ranging from about 650 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$ in the blue wing to 170 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$ in the red wing of the Na 3p multiplet. The branching is found to be strongly detuning dependent in the vicinity of the NaAr, NaKr, and NaXe near-red-wing satellites. The blue-wing branching ratios show a detuning-dependent approach to a recoil, or sudden statistical, limit of 0.5, irrespective of the rare gas. Fine-structure changing cross sections have also been measured for resonant excitation of the Na 3p 2Pj^{2}P_{j}2Pj​ state; the results are consistent with cross sections obtained from wing excitation.
Experimental ratios for branching into the fine‐structure levels of the Na 3p multiplet, as a consequence of an optical collision with He, Ne, Ar, Kr, or Xe, are reported. The process studied is Na(3s2S1/2) +RG+nhν → Na(3p2 Pj)+RG+(n−1)hν, where RG represents a rare gas atom and where the laser frequency ν is tuned in the wings of the Na resonance transitions. The branching ratios are defined as I(D1)/I(D2) where I(D1) and I(D2) are measured intensities of the atomic Na D1 and D2 lines. The ratios are determined for detunings ranging from about 650 cm−1 blue to 170 cm−1 red of the Na 3p multiplet. The branching is found to be strongly detuning dependent in the vicinity of the NaKr and NaXe near red‐wing satellites. The blue wing branching ratios show a detuning‐dependent approach to a recoil or sudden statistical limit of 0.5, irrespective of the rare gas.
The close-coupled theory of atomic collisions in the presence of a radiation field may be used to calculate the distribution of final atomic states which results from absorption of polarized light during a collision. The theory applies equally well to optical collisions (line broadening) and to radiative collisions (laser-induced collisional energy transfer). For an optical collision the detuning $\ensuremath{\omega}\ensuremath{-}{\ensuremath{\omega}}_{\ensuremath{\infty}}$ is restricted to be larger than either the Rabi frequency or the widths due to natural, Doppler, or pressure broadening. The radiation field is assumed to be weak enough that the transition probabilities are linear in field intensity. The molecular picture is emphasized in which the wave function is expanded in a basis of field-free molecular states and the Hamiltonian is blocked in accordance with molecular quantum numbers. The quantities needed to predict experimental observables are reduced radiative scattering SSS-matrix elements ${s}_{\ensuremath{\omega}}$ in the asymptotic Hund's case-(e) representation. The theory of product orientation and alignment is equivalent to that which has been developed for molecular photodissociation. It requires coherent sums of ${s}_{\ensuremath{\omega}}$ matrix elements from different transition branches, that is, for PPP-, QQQ-, and RRR-type transitions corresponding to changes of -1, 0, and +1 in total molecular angular momentum. On the other hand, the total absorption coefficient and the branching ratio to different final fine-structure states irrespective of orientation or alignment depend on incoherent sums of the same matrix elements.
The depolarisation of the redistributed Na D1and D2line fluorescence caused by Na-Ar collisions after far-wing excitation was investigated. In the limit of zero Ar density the J=1/2orientation and J=3/2alignment reflect the distribution among Zeeman sublevels of Na 32PJproduced after absorption of a photon into one or several excited Na-Ar molecular states at small internuclear separation, followed by a mixing between these states during dissociation. Measurements of these quantities as functions of the detuning up to Delta omegaJ=50 cm-1in the red wings are compared with quantum-mechanical coupled-channel (CC) calculations using realistic molecular potentials and thermal averaging, and with predictions from the factorisation approximation (FA) of the theory of redistribution. Fair agreement with CC calculations and FA predictions was obtained within the impact region, proving the validity of the factorisation assumption there. Outside this region the overall depolarisation is primarily due to reorientation of the Na 3P electronic angular momentum and is reproduced qualitatively by the CC calculations but not by the FA theory. Additional depolarisation connected with the fine-structure coupling was observed.