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PHOTOEXCITATION OF CESIUM THROUGH DISSOCIATIVE STATES OF THE CESIUM DIMER

C. W. Walter

Published Jan 1, 1987• 0 citations
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Abstract

The two-photon excitation of cesium to high-n Rydberg levels through resonant dissociative states of the dimer is investigated over the wavelength range 6000-5900A. Highly vibrationally excited $\\sp1\\Sigma\\sb{\\rm g}\\sp+$ ground state molecules are excited to the continuum of $\\sp1\\Pi\\sb{\\rm u}$ bound states which dissociate to give 5D atoms. The 5D atoms are subsequently photoexcited to high-n Rydberg states which are detected by selective field ionization techniques. Series corresponding to both (5D $\\to$ nF) and (5D $\\to$ nP) transitions with components up to n = 150 were observed. The photoexcitation process appears to be very efficient and produces copious quantities of Cs Rydberg atoms.

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A new method for studying dissociative molecular states, complementary to standard spectroscopy techniques, is discussed and its application to the specific case of $Cs_{2}$ is reported. Previous multi-photon ionization $experiments^{1,2}$ revealed the existence of hybrid absorption resonance, in which one photon causes a molecular transition to a dissociative state and a second photon is absorbed by one of the resulting dissociation fragments. The method of dissociation excitation spectroscopy uses two synchronized pulsed lasers to sequentially excite a dissociative molecular state and then detect the dissociation fragments through atomic excitation followed by collisional ionization. By scanning the wavelength of the laser probing the molecule it is possible to obtain a spectrum giving the relative probability that a specific dissociation product will be formed after photo-absorption in the molecule. The dissociation excitation spectrum, including the fine-structure branching ratio, has been obtained for the case \\[ Cs_{2} + \\gamma \\rightarrow Cs_{2}^{*} \\rightarrow Cs(6^{2}S_{1/2}) + Cs(5^{2}D_{3/2,5/2}) \\] over the wavelength region 4575-6050 $\\AA$. This spectrum shows marked similarities to the standard absorption spectrum of $Cs_{2}$. The implications for the molecular potentials of $Cs_{2}$ will be discussed.

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Physica Scripta•Jan 1, 2000•0 citations
The two-photon excitation of cesium to high-n Rydberg levels through resonant dissociative states of the dimer is investigated over the wavelength range 6000-5900A. Highly vibrationally excited sp1Sigmasbrmgsp+\\sp1\\Sigma\\sb{\\rm g}\\sp+sp1Sigmasbrmgsp+ ground state molecules are excited to the continuum of sp1Pisbrmu\\sp1\\Pi\\sb{\\rm u}sp1Pisbrmu bound states which dissociate to give 5D atoms. The 5D atoms are subsequently photoexcited to high-n Rydberg states which are detected by selective field ionization techniques. Series corresponding to both (5D to\\toto nF) and (5D to\\toto nP) transitions with components up to n = 150 were observed. The photoexcitation process appears to be very efficient and produces copious quantities of Cs Rydberg atoms.
Cesium molecules are pumped by a CW dye laser. Some of the excited molecules then pre-dissociate or collisionally transfer excitation to produce excited atoms at the 5D and 6P levels. The cross sections (in units of 10-14cm2) for the excitation transfer process Cs(6P)+Cs(5D) →Cs(7DJ)+Cs(6S)for J being 5/2 and 3/2 are 5. 4 ± 50% and 4. 9 ± 50%, respectively. The cross sections (in units of 10-14cm2) for the excitation transfer out of the 7D doublet [i. e. , Cs(7DJ)+Cs(6S) →states other than Cs(7D)] for J being 5/2 and 3/2 are 1. 6 ±50% and 0. 34±50%, respectively. To obtain these cross sections, the intensities of 7D and 5D fluorescence emissions and the 6P atom density are measured by using the absorption equivalent width technique. The results are discussed in eomparison with those of other experiments.
DISSOCIATIVE EXCITATION SPECTROSCOPY OF Cs2:Cs2+γ→Cs2∗→Cs(62S)+Cs(52D)Cs_{2}: Cs_{2} + \gamma \to Cs_{2}{^{*}} \to Cs(6^{2}S) + Cs(5^{2}D)Cs2​:Cs2​+γ→Cs2​∗→Cs(62S)+Cs(52D)
A new method for studying dissociative molecular states, complementary to standard spectroscopy techniques, is discussed and its application to the specific case of Cs2Cs_{2}Cs2​ is reported. Previous multi-photon ionization experiments1,2experiments^{1,2}experiments1,2 revealed the existence of hybrid absorption resonance, in which one photon causes a molecular transition to a dissociative state and a second photon is absorbed by one of the resulting dissociation fragments. The method of dissociation excitation spectroscopy uses two synchronized pulsed lasers to sequentially excite a dissociative molecular state and then detect the dissociation fragments through atomic excitation followed by collisional ionization. By scanning the wavelength of the laser probing the molecule it is possible to obtain a spectrum giving the relative probability that a specific dissociation product will be formed after photo-absorption in the molecule. The dissociation excitation spectrum, including the fine-structure branching ratio, has been obtained for the case \\[ Cs_{2} + \\gamma \\rightarrow Cs_{2}^{*} \\rightarrow Cs(6^{2}S_{1/2}) + Cs(5^{2}D_{3/2,5/2}) \\] over the wavelength region 4575-6050 AA\\AAAA. This spectrum shows marked similarities to the standard absorption spectrum of Cs2Cs_{2}Cs2​. The implications for the molecular potentials of Cs2Cs_{2}Cs2​ will be discussed.
Very highly excited p states of Cs with principal quantum numbers 30<or=n<or=85 were produced by one-step photoexcitation with frequency-doubled light from a flash-lamp-pumped dye laser. Field ionization was employed for selective detection. Ionization occurs at field strengths E>or=E min with a sharp threshold. The relation E min (n*) varies as (n*) -4 was verified over a wide range. Two-photon excitation to a very high state via a virtual intermediate state leads to immediate ionization of most of the excited atoms; in this case the ion signal as a function of the light intensity I is not proportional to I k , k>or=2, whereas a direct two-photon transition into the continuum yields proportionality with I 2 .
The multiphoton excitation of rubidium has been investigated over the 4600-6500-\AA{} wavelength region with a tunable dye-laser source having a linewidth better than 0.1 \AA{} and a space-charge ionization detector sensitive to a few ions per second. Multiphoton transitions have been observed to occur both through intermediate atomic states and through intermediate continuum states of the rubidium molecule. In the former case two-photon transitions have been observed from the 52S5^{2}S52S ground state of atomic rubidium to higher-lying n2Dn^{2}Dn2D levels for values of nnn ranging from 9 to 34 and to n2Sn^{2}Sn2S levels for values of nnn from 11 through 20. The fine-structure intervals of the n2Dn^{2}Dn2D levels for n=9toc13n=9 \mathrm{to}c 13n=9toc13 were measured together with the line-strength ratios and were found to be in good agreement with the predictions of a simple theoretical model. At the shorter wavelengths hybrid two-photon resonances were observed to be excited through resonant intermediate continuum states of Rb2{\mathrm{Rb}}_{2}Rb2​. As a result the dispersion curve for two-photon absorption in rubidium showed what appears to be resonant intermediate $p\ensuremath{\pi}(^{3}\ensuremath{\Sigma}_{u1})$ and 0g+{0}_{g}^{+}0g+​ terms dissociating to give a 5P325{P}_{\frac{3}{2}}5P23​​ atom and resulting in the strong development of features corresponding to the $5^{2}P_{\frac{3}{2}}\ensuremath{\rightarrow}n^{2}D_{\frac{3}{2},\frac{5}{2}}$ part of the diffuse series, for $n\ensuremath{\le}50$ in absorption and the $5^{2}P_{\frac{3}{2}}\ensuremath{\rightarrow}n^{2}S_{\frac{1}{2}}$ part of the sharp series. Components to 322D32^{2}D322D and 302S30^{2}S302S were recorded to a precision of 0.3 ${\mathrm{cm}}^{\ensuremath{-}1}$ and quantum defects for these previously unobserved terms were derived. The corresponding hybrid two-photon resonances involving intermediate states dissociating to give a 52P125^{2}P_{\frac{1}{2}}52P21​​ atom were not observed in the wavelength interval available in this experiment.
The two-photon excitation and three-photon ionization of atomic cesium is investigated over the 6550-6950-\AA{} wavelength region with a tunable-dye-laser source having a 0.06-0.08-\AA{} linewidth and a space-charge ionization detector sensitive to a few ions per second. An online data-acquisition computer provides significant signal-to-noise recovery. The resulting dispersion curve for photoionization is interpreted in terms of the two-photon transitions from the ground 62S126^{2}S_{\frac{1}{2}}62S21​​ level to resonant n2Dn^{2}Dn2D and n2Sn^{2}Sn2S intermediate states, and represents, to the authors' knowledge, the first such two-photon absorption spectrum of Cs. Transitions from n=9to13n=9\mathrm{to}13n=9to13 have been recorded for the $6^{2}S_{\frac{1}{2}}\ensuremath{-}n^{2}D_{\frac{5}{2},\frac{3}{2}}$ series and from n=11to14n=11\mathrm{to}14n=11to14 for the $6^{2}S_{\frac{1}{2}}\ensuremath{-}n^{2}S_{\frac{1}{2}}$ series.
In the molecular photoassociation process, two free cold atoms absorb one photon by a resonant way, to create an excited molecule in a well defined ro-vibrational state. The photoassociative spectroscopy of alkaline dimers yields accurate determinations for the long-range parts of molecular potential curves correlated to the first s + p asymptote. In contrast to atoms, laser cooling of molecules is very difficult because of the lack of a closed two-level scheme for recycling the population. The molecular photoassociation of cold atoms opens also a promising alternative for the formation of cold ground state molecules. Photoassociation of cold cesium atoms has permitted the first observation of translationally cold ground state molecules. The case of the cesium atom is very favorable because the 0 g - and 1 u purely long-range states below the dissociation limit 6s 1/2 +6p 3/2 present Condon points at intermediate distances. Such configurations offer rather efficient channels for the creation of singlet or triplet ground state Cs 2 molecules after spontaneous decay.