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Physical Review A

Orientation observed by Zeeman spectra of dissociated atoms and the interference in photoexcitations

Yasuyuki Kimura, Shunji Kasahara, Hajime Katô, Masaaki Baba

Published Jun 27, 2003• 2 citations
Publisher

Abstract

In a magnetic field, the wave number of a pump laser light polarized along the field was fixed to the isolated ${\mathrm{Cs}}_{2}D{}^{1}{\ensuremath{\Sigma}}_{u}^{+}(v=46,J=54)\ensuremath{\leftarrow}X{}^{1}{\ensuremath{\Sigma}}_{g}^{+}(v=0,J=55)$ line, and the excitation spectrum of the dissociated $\mathrm{Cs}(6p{}^{2}{P}_{3/2})$ atoms was measured by scanning the wave number of a probe laser light polarized perpendicular to the field. The population of each sublevel $6p{}^{2}{P}_{{3/2,m}_{j}}$ of the dissociated atoms was determined from the line intensities in the ${m}_{j}$-resolved excitation spectrum. The unequal population between the $6p{}^{2}{P}_{3/2,+|{m}_{j}|}$ and $6p{}^{2}{P}_{3/2,\ensuremath{-}|{m}_{j}|}$ levels (atomic orientation) was observed and it was enhanced as the magnetic-field strength was increased. The atomic orientation is shown to be induced by the interference between the indirect predissociation, which occurs by a combination of the spin-orbit coupling of the $D{}^{1}{\ensuremath{\Sigma}}_{u}^{+}$ state with the ${(2)}^{3}{\ensuremath{\Pi}}_{0u}$ state and the L-uncoupling and Zeeman interactions between the ${(2)}^{3}{\ensuremath{\Pi}}_{0u}$ and dissociative ${(2)}^{3}{\ensuremath{\Sigma}}_{u}^{+}$ states, and the dissociation following a direct excitation to the ${(2)}^{3}{\ensuremath{\Sigma}}_{u}^{+}$ state, which is allowed by spin-orbit coupling of the ${(2)}^{3}{\ensuremath{\Sigma}}_{u}^{+}$ state with the $B{}^{1}{\ensuremath{\Pi}}_{u}$ state. It is demonstrated that the atomic orientation is produced by the photodissociation in the presence of an external magnetic field even when all degenerated molecular $M=J,\dots{},0,\dots{},\ensuremath{-}J$ sublevels are excited by a light polarized linearly along the field.

DOI
10.1103/physreva.67.062717

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In a magnetic field, the wave number of a pump laser light polarized along the field was fixed to the isolated Cs2D1\ensuremathΣu+(v=46,J=54)\ensuremath←X1\ensuremathΣg+(v=0,J=55){\mathrm{Cs}}_{2}D{}^{1}{\ensuremath{\Sigma}}_{u}^{+}(v=46,J=54)\ensuremath{\leftarrow}X{}^{1}{\ensuremath{\Sigma}}_{g}^{+}(v=0,J=55)Cs2​D1\ensuremathΣu+​(v=46,J=54)\ensuremath←X1\ensuremathΣg+​(v=0,J=55) line, and the excitation spectrum of the dissociated Cs(6p2P3/2)\mathrm{Cs}(6p{}^{2}{P}_{3/2})Cs(6p2P3/2​) atoms was measured by scanning the wave number of a probe laser light polarized perpendicular to the field. The population of each sublevel 6p2P3/2,mj6p{}^{2}{P}_{{3/2,m}_{j}}6p2P3/2,mj​​ of the dissociated atoms was determined from the line intensities in the mj{m}_{j}mj​-resolved excitation spectrum. The unequal population between the 6p2P3/2,+∣mj∣6p{}^{2}{P}_{3/2,+|{m}_{j}|}6p2P3/2,+∣mj​∣​ and 6p2P3/2,\ensuremath−∣mj∣6p{}^{2}{P}_{3/2,\ensuremath{-}|{m}_{j}|}6p2P3/2,\ensuremath−∣mj​∣​ levels (atomic orientation) was observed and it was enhanced as the magnetic-field strength was increased. The atomic orientation is shown to be induced by the interference between the indirect predissociation, which occurs by a combination of the spin-orbit coupling of the D1\ensuremathΣu+D{}^{1}{\ensuremath{\Sigma}}_{u}^{+}D1\ensuremathΣu+​ state with the (2)3\ensuremathΠ0u{(2)}^{3}{\ensuremath{\Pi}}_{0u}(2)3\ensuremathΠ0u​ state and the L-uncoupling and Zeeman interactions between the (2)3\ensuremathΠ0u{(2)}^{3}{\ensuremath{\Pi}}_{0u}(2)3\ensuremathΠ0u​ and dissociative (2)3\ensuremathΣu+{(2)}^{3}{\ensuremath{\Sigma}}_{u}^{+}(2)3\ensuremathΣu+​ states, and the dissociation following a direct excitation to the (2)3\ensuremathΣu+{(2)}^{3}{\ensuremath{\Sigma}}_{u}^{+}(2)3\ensuremathΣu+​ state, which is allowed by spin-orbit coupling of the (2)3\ensuremathΣu+{(2)}^{3}{\ensuremath{\Sigma}}_{u}^{+}(2)3\ensuremathΣu+​ state with the B1\ensuremathΠuB{}^{1}{\ensuremath{\Pi}}_{u}B1\ensuremathΠu​ state. It is demonstrated that the atomic orientation is produced by the photodissociation in the presence of an external magnetic field even when all degenerated molecular M=J,…,0,…,\ensuremath−JM=J,\dots{},0,\dots{},\ensuremath{-}JM=J,…,0,…,\ensuremath−J sublevels are excited by a light polarized linearly along the field.
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.
Preferential population of the magnetic sublevels of Cs(6p 2P3/2) atoms produced by predissociation of the C 1Πu state of the Cs2 molecule along the repulsive molecular state b 3Σ+u , has been found by observing the polarization of the atomic fluorescence Cs(6p 2Pm3/2→6s 2S1/2). By applying an external magnetic field, we have determined the population of the magnetic sublevels Cs(6p 2Pm3/2) directly from the intensities of the fluorescence lines Cs(6p 2Pm3/2 →6s 2Sm±11/2 ) split by the Zeeman effect. The results are analyzed theoretically by assuming the separability of electronic and nuclear motion for the dissociation along the repulsive potential curve. The effect of the external magnetic field on the photodissociation has been made clear, and the observed results could be fully explained on the basis of the adiabatic approximation.
Abstract In a plane perpendicular to a magnetic field a collimated cesium beam was crossed at right angles by a pump laser beam. Cs2 molecules were excited to the D1Σu+ (v = 46, J = 54) level, which predissociated selectively to Cs(6s2S1/2) + Cs(6p2P3/2) atoms. The mj-resolved excitation spectra of the Cs(8s2S1/2,m′j ← 6p2P3/2,mj) transitions at a magnetic field of 1.91 kG were measured using a probe laser beam propagated either along the magnetic field or along the pump beam. The population of Cs(6p2P3/2,mj) atoms was found to be in the ratio 77 : 136 : 100 : 46 for mj = 3/2, 1/2, −1/2, and −3/2 based on an analysis of the line intensities. From the line shapes of the excitation spectra, Cs(6p2P3/2,±1/2) atoms were found to recoil predominantly parallel to the magnetic field H, and Cs(6p2P3/2,±3/2) atoms were found to recoil predominantly perpendicular to H.
In the optical excitation of atoms with polarized light, producing excited atoms, only some of the Zeeman sublevels of the excited state are actually reached, so that large differences of population can be built up between Zeeman sublevels or between hyperfine structure (hfs) levels. This property can be used to detect radio-frequency resonance in optically excited atomic states. These resonances produce a characteristic change in intensity or in the degree of polarization of the light re-emitted. Zeeman intervals, Stark effects, and hfs intervals can be measured in this manner. (The Stark constant of the 63P1 level of Hg and the electric quadrupole moments of the alkali atoms have been obtained in this way.)The technique of “optical pumping” gives a way to concentrate atoms in some of the Zeeman sublevels of one of the hfs levels of the ground state.Atomic orientation has been obtained with the Na atom, in an atomic beam and in the vapor in equilibrium with the metal. The orientation effects have been studied by detection of radio-frequency resonance signals in the ground state. Orientation can be increased many times by adding a variable pressure of a foreign gas to the pure Na vapor. Because of the coupling between nuclear spin and electron spin, nuclear orientation is produced at the same time as atomic orientation.
Anisotropic coherent radiation has been generated from an isotropic medium, in the absence of an external magnetic field, by the spin polarization of an atomic excited state. Lasing on specific hyperfine lines of the 6p2P32→6s2S12 (D2) transition of Cs at 852.1 nm has been realized by photoexciting Cs-rare gas thermal collision pairs with a circularly-polarized (σ+) optical field. Subsequent dissociation of the transient Cs-rare gas B2Σ12+ diatomic molecule selectively populates theF= 4, 5 hyperfine levels of the Cs 6p2P32 state. Not only does electronic spin polarization of the upper laser level yield circularly-polarized coherent emission, but the effective degeneracy (g2) of the 6p2P32 state is altered by the non-statistical hyperfine state population distribution, thereby permitting control of the laser small signal gain with an elliptically-polarized pump optical field. TheD2laser efficiency and output power correlate directly with the molecular orbital structure of the Cs-rare gasB2Σ+state in the region of internuclear separation at which the diatomic complex is born.
The theory of how excited-state hyperfine structure can be determined using a magnetic field to decouple the nuclear and electronic angular momentum is presented. The initial excited state is assumed to have an anisotropic Zeeman sublevel population distribution, which can be conveniently created by a laser-induced multiphoton excitation of an unpolarized atom. The Zeeman sublevel populations are subsequently mixed by the hyperfine interaction. The degree of mixing is controlled by a magnetic field applied along the quantization axis. The relative Zeeman sublevel populations can be monitored by detecting the polarization of fluorescence emitted when the excited state radiatively decays. It is convenient to take the ratio of two time-integrated fluorescent signals measured for orthogonal linear polarizations, since this is independent of the excited-state number density. The plot of this ratio versus magnetic field is very well approximated by a Lorentzian curve whose half-width is proportional to the magnetic dipole hyperfine coupling constant. This method was used to determine the magnitude of the magnetic dipole constant of the cesium 8D3/2{\mathit{D}}_{3/2}D3/2​ state to be 3.92\ifmmode\pm\else\textpm\fi{}0.10 MHz, which is in excellent agreement with previous results.