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Physical Review Letters

Theoretical Determination of Fine-Structure Transitions Occurring in Collisional Redistribution of Light

K. C. Kulander, Frank Rebentrost

Published Oct 3, 1983• 19 citations
Publisher

Abstract

Recent experimental results of Havey, Copeland, and Wang on the collisional redistribution of light by Na in Ar showed a dependence of the relative intensities of the Na ${D}_{1}$ and ${D}_{2}$ resonance lines on laser detuning. Calculations of these intensity ratios are reported here. The agreement between theory and experiment obtained here shows the importance of fine-structure transitions occurring during the dissociation of the excited-state molecule.

DOI
10.1103/physrevlett.51.1262

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Fine-Structure Transitions Occurring in Collisional Redistribution of Light

Mark D. Havey, Gary E. Copeland, W. J. Wang

Experimental results on fine-structure transitions occurring in collisional redistribution of far---off-resonant radiation are presented. Measurements on Na-Ar atomic collisions illustrate that electronically nonadiabatic transitions occurring in the final state, following absorption, are important for describing the redistribution process. The results also provide details of the fine-structure transition process that are not obtainable from the usual resonant scattering experiments.

Physical Review Letters•May 30, 1983•22 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.

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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

Experimental fine-structure branching ratio for R b -A r optical collision

Yifan Shen, A Pulati, Silayi Huerxida

Experimental ratio for branching into the fine structure levels of the Rb52P multiplet, as a consequence of an optical collision with Ar, is reported. An optically thin gaseous mixture of Rb and low-density Ar is excited by a cw dye laser. The excited RbAr molecule is dissociated into the Rb5P1/2 or Rb5P3/2, the branching ratio is defined as I(D1)/I(D2) where 1(D1) and I(D2) are measured intensities of the atomic RbD1 and D2 lines. The branching is determined for tuning ranging from 600 nm to 570 nm and in the Ar density range 2 to 8 X 1017 cm-3. The ratio of the dissociation rates and the fine structure changing cross section are obtained. The ratio of the dissociation rates approaches 0.7 as a limit which is independent of the laser frequency.© (1999) COPYRIGHT SPIE--The International Society for Optical Engineering. Downloading of the abstract is permitted for personal use only.

Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE•Sep 8, 1999•0 citations

Depolarisation in Na-Ar optical collisions

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[Measurement of fine-structure branching ratios for Rb-He optical collisions].

Lei Lü, Lin Li, Yu-Hua Deng +3 more

Experimental ratios of branching in the fine-structure levels of the Rb5P multiplet, as a consequence of an optical collision with He, are reported. The process studied is Rb(5S1/2 )+ He + hrv --> Rb(5P(J)) +He, where the pulsed laser frequency v is tuned in the wings of the Rb resonance transitions. The authors defined the detuning delta to be v-v (D2 )(delta > 0) for laser frequency v highter than that of RbD2 transition and to be v-v (D1)(delta < 0) for v lower than the RbD1 transition. As RbHe molecular states are correlated to the two 5 2P(J) states, there is some likelihood that the molecule will dissociate into 5 2P1/2 or 5P3/2 state. The dissociation results in a nonuniform distribution of atomic Rb5P(J) states. The branching ratios are defined as n1/n2, where n1 and n2 are densities of the 5P1/2 and 5P3/2 states dissociated. To determine experimentally the relative cross section for scattering into the two fine-structure states, the relative time-intergrated intensities of the resulting Rb emission lines, I(5P3/2 --> 5P1/2 )[I(D2)] and I(5P1/2 --> 5P3/2) ) [I(D1)], were measured. The ratios are determined by detunings from about 200 cm(-1) in the blue wing to -180 cm(-1) in the red wing of the Rb5P multiplet. A rate equation analysis of the pressure dependence was yielded. The branching ratios and cross sections for collisional 5P1/2 --> 5P3/2 transition were obtained from the slope and intercept. The blue-wing branching ratios show a detuning-dependent approach to limit of 0. 2. The branching was found to be very large (-40) in the red wing, irrespective of the detuning. Fine structure changing cross section (1.1 +/- 0.3) x 10(-17) cm2 was measured from wing excitation, and the result is consistent with the cross section obtained from resonant excitation of the Rb5P(J) state. The measurements show a strong sensitivity to interatomic potentials and to nonadiabatic effects in dissociation dynamics.

•Jul 1, 2009•0 citations
Recent experimental results of Havey, Copeland, and Wang on the collisional redistribution of light by Na in Ar showed a dependence of the relative intensities of the Na D1{D}_{1}D1​ and D2{D}_{2}D2​ resonance lines on laser detuning. Calculations of these intensity ratios are reported here. The agreement between theory and experiment obtained here shows the importance of fine-structure transitions occurring during the dissociation of the excited-state molecule.
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.
Experimental ratio for branching into the fine structure levels of the Rb52P multiplet, as a consequence of an optical collision with Ar, is reported. An optically thin gaseous mixture of Rb and low-density Ar is excited by a cw dye laser. The excited RbAr molecule is dissociated into the Rb5P1/2 or Rb5P3/2, the branching ratio is defined as I(D1)/I(D2) where 1(D1) and I(D2) are measured intensities of the atomic RbD1 and D2 lines. The branching is determined for tuning ranging from 600 nm to 570 nm and in the Ar density range 2 to 8 X 1017 cm-3. The ratio of the dissociation rates and the fine structure changing cross section are obtained. The ratio of the dissociation rates approaches 0.7 as a limit which is independent of the laser frequency.© (1999) COPYRIGHT SPIE--The International Society for Optical Engineering. Downloading of the abstract is permitted for personal use only.
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.
Experimental ratios of branching in the fine-structure levels of the Rb5P multiplet, as a consequence of an optical collision with He, are reported. The process studied is Rb(5S1/2 )+ He + hrv --> Rb(5P(J)) +He, where the pulsed laser frequency v is tuned in the wings of the Rb resonance transitions. The authors defined the detuning delta to be v-v (D2 )(delta > 0) for laser frequency v highter than that of RbD2 transition and to be v-v (D1)(delta < 0) for v lower than the RbD1 transition. As RbHe molecular states are correlated to the two 5 2P(J) states, there is some likelihood that the molecule will dissociate into 5 2P1/2 or 5P3/2 state. The dissociation results in a nonuniform distribution of atomic Rb5P(J) states. The branching ratios are defined as n1/n2, where n1 and n2 are densities of the 5P1/2 and 5P3/2 states dissociated. To determine experimentally the relative cross section for scattering into the two fine-structure states, the relative time-intergrated intensities of the resulting Rb emission lines, I(5P3/2 --> 5P1/2 )[I(D2)] and I(5P1/2 --> 5P3/2) ) [I(D1)], were measured. The ratios are determined by detunings from about 200 cm(-1) in the blue wing to -180 cm(-1) in the red wing of the Rb5P multiplet. A rate equation analysis of the pressure dependence was yielded. The branching ratios and cross sections for collisional 5P1/2 --> 5P3/2 transition were obtained from the slope and intercept. The blue-wing branching ratios show a detuning-dependent approach to limit of 0. 2. The branching was found to be very large (-40) in the red wing, irrespective of the detuning. Fine structure changing cross section (1.1 +/- 0.3) x 10(-17) cm2 was measured from wing excitation, and the result is consistent with the cross section obtained from resonant excitation of the Rb5P(J) state. The measurements show a strong sensitivity to interatomic potentials and to nonadiabatic effects in dissociation dynamics.