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Journal of the Chemical Society Faraday Transactions 2 Molecular and Chemical Physics

M j selectivity in collisional energy transfer between alkali-metal atoms

Masaaki Baba, Hajime Katô

Published Jan 1, 1989• 4 citations
Publisher

Abstract

Na atoms in the magnetic field have been selectively excited to each Zeeman sub-level of either the 3p2P1/2 or 3p 2P3/2 state by a tunable dye laser and the Zeeman spectra of the fluorescence from the collisional populated 3p 2P levels have been measured. From the intensities of the Zeeman lines, the selectivity in the collisional transitions between the Zeeman sub-levels of the 3p 2P1/2 and 3p 2P3/2 states has been directly specified. The time evolution of the σ-polarized fluorescence intensity of the Na(3p 2P1/2→ 3s 2S1/2) transition has been measured following the Na(3p 2P3/2â†� 3s 2S1/2) excitation by a σ-polarized short light pulse at H= 129 G. An amplitude modulation was found in the fluorescence from the collisional energy transferred state Na(3p 2P1/2). This is the first observation of quantum beats in collision-induced fluorescence. The frequency of the modulation coincides very well with that of the quantum beats of the resonance fluorescence Na(3p 2P3/2→ 3s 2S1/2), but the phases are opposite. These results are explained by assuming the conservation of coherence during collisional energy transfer.

DOI
10.1039/f29898500965

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Inelastic collisions between excited alkali atoms and molecules. V. Sensitized fluorescence in mixtures of sodium with N2, H2, HD, and D2

M. Stupavsky, L. Krause

3 2P1/2 ↔ 3 2P3/2 excitation transfer in sodium, induced in inelastic collisions with ground-state N2, H2, HD, and D2 molecules, has been investigated in a series of sensitized fluorescence experiments. Mixtures of sodium vapor at a pressure of 5 × 10−7 Torr, and the gases, were irradiated with each NaD component in turn, and the fluorescence which contained both D components was monitored at right angles to the direction of the exciting beam. Measurements of the relative intensities of the NaD fluorescent components yielded the following collision cross sections for excitation transfer. For Na–N2 collisions: Q12(2P1/2 → P3/2) = 144 Å2, Q21(2P1,2 ← 2P3/2) = 76 Å2 for Na–H2 collisions: Q12 = 80 Å2, Q21 = 42 Å2. For Na–HD collisions: Q12 = 84 Å2, Q21 = 44 Å2. For Na–D2 collisions: Q12 = 98 Å2, Q21 = 52 Å2. The cross sections Q21 exhibit a slight resonance effect between the atomic and molecular rotational transitions.

Canadian Journal of Physics•Oct 1, 1968•23 citations
Na atoms in the magnetic field have been selectively excited to each Zeeman sub-level of either the 3p2P1/2 or 3p 2P3/2 state by a tunable dye laser and the Zeeman spectra of the fluorescence from the collisional populated 3p 2P levels have been measured. From the intensities of the Zeeman lines, the selectivity in the collisional transitions between the Zeeman sub-levels of the 3p 2P1/2 and 3p 2P3/2 states has been directly specified. The time evolution of the σ-polarized fluorescence intensity of the Na(3p 2P1/2→ 3s 2S1/2) transition has been measured following the Na(3p 2P3/2â†� 3s 2S1/2) excitation by a σ-polarized short light pulse at H= 129 G. An amplitude modulation was found in the fluorescence from the collisional energy transferred state Na(3p 2P1/2). This is the first observation of quantum beats in collision-induced fluorescence. The frequency of the modulation coincides very well with that of the quantum beats of the resonance fluorescence Na(3p 2P3/2→ 3s 2S1/2), but the phases are opposite. These results are explained by assuming the conservation of coherence during collisional energy transfer.
Quantum beats of the Na(3 2P3/2–3 2S1/2) transition and their change with the magnetic field were observed in pure Na vapor and Na+He gas by using a picosecond laser system. The energies of the hyperfine and Zeeman sublevels of the 3 2P3/2 and 3 2S1/2 states were calculated by using the reported hyperfine constants and g factors, and the theoretical curve of the quantum beats was calculated. The results were in good agreement with the observed profile of the quantum beats in phase of modulation, but the difference of the amplitudes increased with time. By comparing the amplitude of the theoretical curve of the quantum beats with that of the experimental curve, we determined the relaxation time of coherence. The decay of amplitude of the modulation was found to become faster as the pressure of the foreign gas (He) was increased. The decay of amplitude, i.e., the decay of coherence arises from the dephasing, which occurs from the fluctuation of the level energies induced by the interatomic interaction.
By applying an external magnetic field, we have determined the population of the magnetic sublevels of photodissociated atoms from the intensities of atomic fluorescence lines split by the Zeeman effect. A preferential population of the magnetic sublevels of the atomic fragment Na(3 2P3/2), which arises from the direct photodissociation through the D1Π(continuum) state of the NaK molecule, has been observed. The results are explained by assuming the separability of electronic and nuclear motion during the dissociation. The observed results could be rationalized by the sum of the photodissociation amplitudes caused by excitation of the P, Q and R branches. The population of the magnetic sublevels of Rb(5 2P3/2) atoms produced by predissociation of the C1Πu state of the Rb2 molecule by the repulsive molecular state c3Σ+u has been determined from the Zeeman spectra of the emission Rb(5 2P3/2→ 5 2Sm′1/2). The observed results are interpreted by including the spin-orbit coupling between an excited level of the C1Πu state and levels of the c3Σ+u state and the effect of the external magnetic field.
The cross sections for the excitation energy transfer in the collisional processes Na*(3P 1 2/)+M(nS 1 2/) to or from Na*(3p 3 2/)+m(Ns 3 2/), m being ground-state Rb (n=5) or Cs (n=6) atom, have been measured by laser fluorescence method. With either of the two sodium 3P fine-structure states optically excited, the intensity ratio of the sensitized to direct fluorescence was measured. The polarization effects due to partially polarized and anisotropic direct fluorescence were investigated. The measured cross sections (T=530 K) for the sodium 3P fine-structure excitation transfer induced by collisions with Rb are: sigma ( 1 / 2 to 3 / 2 )=170 AA 2 , with an overall accuracy of 20%. The corresponding values in the Cs case are: sigma ( 1 / 2 to 3 / 2 )=140 AA 2 , sigma ( 3 / 2 to 1 / 2 )=83 AA 2 . The theoretical calculations reveal the decisive role of the dipole-quadrupole interaction. The obtained values are in satisfactory agreement with the experiment only if both the dipole-dipole and dipole-quadrupole interactions are taken into account, while the calculations involving the dipole-dipole term alone yield the cross section values which are as much as one order of magnitude lower than the experimentally observed ones.
The dependence of the circular polarization of the fluorescence of alkali atoms on the intensity and spectral composition of the σ+-polarized exciting D1 line has been investigated by considering the stationary solutions of rate equations for populations of the Zeeman sublevels. The calculations were performed for pumping-light intensities corresponding to those of classical light sources, e.g., radio frequency or microwave discharge lamps, and commonly accepted values of cross sections for collisional relaxation of ground-state and excited atoms. The systematic errors of cross sections for collisional disorientation of 2P1/2 alkali atoms due to the neglect of intensity and spectral composition of the exciting light are estimated.
We measured the cross section for the collision transfer process Na(4D)+Na (3S)Na(4F)+Na(3S). The 4D state was excited by two photon absorption using a tunable dye laser. Since the direct 4F→3D fluorescence can not be detected with our apparatus, we monitored instead the cascade 3D→3P and 4D→3P fluorescence. Relative intensity of the fluorescence, combined with the measurement of sodium density, yielded cross section σ_(4D)→(4F)=1.3×10~(-14)±28％(cm~2). Our result is compared to other experiments.
3 2P1/2 ↔ 3 2P3/2 excitation transfer in sodium, induced in inelastic collisions with ground-state N2, H2, HD, and D2 molecules, has been investigated in a series of sensitized fluorescence experiments. Mixtures of sodium vapor at a pressure of 5 × 10−7 Torr, and the gases, were irradiated with each NaD component in turn, and the fluorescence which contained both D components was monitored at right angles to the direction of the exciting beam. Measurements of the relative intensities of the NaD fluorescent components yielded the following collision cross sections for excitation transfer. For Na–N2 collisions: Q12(2P1/2 → P3/2) = 144 Å2, Q21(2P1,2 ← 2P3/2) = 76 Å2 for Na–H2 collisions: Q12 = 80 Å2, Q21 = 42 Å2. For Na–HD collisions: Q12 = 84 Å2, Q21 = 44 Å2. For Na–D2 collisions: Q12 = 98 Å2, Q21 = 52 Å2. The cross sections Q21 exhibit a slight resonance effect between the atomic and molecular rotational transitions.