Research on ultracold cesium molecule long-range states by high-resolution photoassociative spectroscopy

In this paper, an ultra-high resolution photoassociation spectroscopy study on photoassociation of cesium atoms is reported. The cold cesium gas in the magneto-optical trap is illuminated by a photoassociation laser with red-tuning as large as 40 cm⁻¹ below the 6S _1/2 + 6P _3/2 dissociation limit, and the photoassociation to the excited state ultracold molecule is detected. High signal-to-noise ratio is obtained by using the lock-in detection of the fluorescence from the modulated cold Cs atoms. The 0 _g ⁻ , 1_g and 0 _u ⁺ long-range states which correspond to 6S _1/2 + 6P _3/2 dissociation limit are present in the photoassociation spectrum. The effective coefficients of leading long-range interactions and the corresponding vibrational quantum number are obtained using LeRoy-Bernstein Law. It is found that photoassociation process creates rotating molecules and the high J value is a hint that higher partial waves participate in the PA process in the presence of trapping laser. Supported by 973 Program of China (Grant. No. 2006CB921603), the National Natural Science Foundation of China (Grant Nos. 10574084, 60678003, and 60778008), the Special Foundation for State Major Basic Research Program of China (Grant No. 2005CCA06300), and the Youth Science Foundation of Shanxi Province of China (Grant No. 20041013)     

Electronic and vibrational spectroscopy of the low-lying states of potassium mono-sulphide KS,and comparison in the series of MS (M = Li,Na, K,Rb, Cs)

ABSTRACT

Potential energy curves (PECs) of the lowest electronic states of the potassium mono-sulphide KS have been determined with highly correlated ab initio calculations, using internally contracted multi reference interaction configuration methods including Davidson correction (MRCI?+?Q) with and without considering spin-orbit effects. For the three low-lying bound states, we report a set of spectroscopic parameters including equilibrium distances, dissociation energies, vibrational and rotational constants. The effects of spin-orbit-induced changes on these parameters are also discussed. An analysis of the properties of the three bound states, X²Π, 1²Σ⁺ and 2²Π, illustrates the common characteristics of the whole series of compounds in the MS family (M?=?Li, Na, K, Rb, Cs). Indeed, the shapes of the PECs of these bound states are strongly affected by the interactions between the two ionic states, ²Σ⁺ and ²Π, correlating at large internuclear separations (R_MS) to the first ionic dissociation limit [M⁺?+?S^?] and the electronic states correlating to the three/four lowest dissociation limits. The spectroscopy of these low-lying electronic states and the lifetime of their vibrational levels are thus affected by the spin-orbit interactions which are mainly related to the S atom and consequently common to all alkali-metal mono-sulphides.     

High sensitive photoassociation spectroscopy based on modulated ultra-cold Cs atoms

In this paper, a high sensitive photoassociation spectroscopy based on modulated ultra-cold cesium atoms is reported. The cold cesium gas in the magneto-optical trap is illuminated by a photoassociation laser with red detuning 40 cm^-1 below the 6S _1/2+6P _3/2 dissociation limit and photoassociation to the excited state ultra-cold molecules is observed. The rotationally bound levels of 0_g ^- state are well resolved using the lock-in detection. The 0_g ^-, 1_g and 0_u ⁺ long range states which connect to this dissociation limit are measured. The long-range dipole–dipole interaction constants are determined through a fit of the experimental energy levels. PACS 33.15.Mt; 33.20.Vq; 32.80.Pj     

Ultra-high resolution trap-loss spectroscopy of ultracold <Superscript>133</Superscript>Cs atom long-range states in a magnetooptical trap

We present an ultra-high resolution spectroscopic study of the photoassociation of cesium atoms inside a magnetooptical trap using trap-loss detection with photoassociation laser slow scanning. The photoassociation spectra show vibrational levels of three molecular symmetries below the 6S _1/2 + 6P _3/2 dissociation limit. A dynamic model is derived to extract the photoassociation rate from the trap-loss spectrum. Many observed rotational levels are well resolved, which indicate d-wave and higher partial wave contributions to the photoassociation cross section.     

基于振幅调制的超冷铯原子高分辨光缔合光谱的实验研究

基于振幅调制的超冷铯原子高分辨光谱的实验研究，用相对于铯分子6S_1/2+6P_3/2离解限红失谐的光缔合激光作用于磁光阱中超冷铯原子，观察到通过光缔合产生的激发态超冷分子.在实验中，为了得到高信号-噪声比的光缔合光谱，利用声光调制器对俘获光进行振幅调制，将探测到的超冷铯原子的荧光信号利用lock-in技术解调.同时利用密度矩阵方程系统地分析了实验结果.     

The study of ungerade electronic states of the Xe2 molecules in the region of Xe*(5p 56p, 5d, 7s, 6d) by the resonance multiphoton ionization method

Electronic spectra of the Xe2 molecules in the energy range of 77700?C89300 cm^?1 are recorded. The method of resonance enhanced multiphoton ionization of molecules in a supersonic molecular beam was used, in which excitation of the molecules by three photons was followed by ionization caused by a fourth photon (the (3+1) REMPI method). Analysis of the vibrational structure of observed systems of bands yielded information about the dissociation energy and the molecular constants for ungerade states of molecules. On the basis of the Franck-Condon principle, the equilibrium distances for potential curves were estimated from the relative intensities in vibrational progressions. Data on 16 new electronic states of diatomic xenon molecules with the dissociation limits Xe ₂ ^* ?? XE(5p ^{6 1} S ₀) + Xe*(5p ⁵6p,5d, 7s, 7p) were obtained.     

All-optical formation of molecules with spin degree of freedom in an atomic Bose-Einstein condensate

We have performed a two-photon photoassociation experiment in an atomic Bose-Einstein condensate of ⁸⁷Rb with the spin degree of freedom, which is created by an all-optical method with CO₂ lasers. The spinor character of the created molecules has been revealed by the photoassociation spectrum with a new structure. The hyperfine structure of the created molecules near the dissociation limit is identified by observations of the Zeeman and AC-Stark effects of the molecules. We have also demonstrated the spin-selective creation of molecules. This result would open the new possibility of research on novel molecular spinor BEC.     

Multiphoton mass spectra of XeKr molecules in the range of excited Xe*6<Emphasis Type="Italic">p</Emphasis>[5/2]<Subscript>2, 3</Subscript> atoms

Data on excited states of XeKr molecules in the energy range 78280–77600 cm^?1 are obtained. Using the method of multiphoton laser photoionization of molecules in a supersonic jet, five vibrational progressions of XeKr molecules are obtained, which are attributed to five electronic-vibrational transitions from the ground state of the XeKr molecule of the symmetry 0⁺ to excited states of the symmetry Ω = 0⁺, 1, 2 with the dissociation limit Kr¹ S ₀ + Xe*6p[5/2]₂ and of the symmetry Ω = 1, 2 with the dissociation limit Kr + Xe*6 p [5/2]₃. The molecular constants of the corresponding excited states of the XeKr molecule are estimated.     

Spectroscopic characterization and potential energy functions of the six low-lying electronic states of ArKr+

Pulsed-field-ionization zero-kinetic-energy (PFI-ZEKE) photoelectron spectra of ArKr have been recorded in the wavenumber range 108,000–118,000 cm^?1 using a 1 + 1′ two-photon resonant excitation scheme from the ground X 0⁺ state of ArKr via selected intermediate states located just below the Ar(¹S₀) + Kr([5p[1/2]₀) dissociation limit. The positions of ionic vibrational levels with quantum numbers from 1 to 30, from 0 to 8 and from 0 to 6 were determined for the X(1/2), A₁(3/2) and A₂(1/2) states, respectively. The assignment of absolute vibrational quantum numbers of the ionic states was derived from the isotopic shifts of the spectral lines. Combining these data with literature data on the B(1/2) → X(1/2), C₁(3/2) → A₁(3/2) and C₂(1/2) → A₂(1/2) band systems of ArKr⁺ enabled the derivation of potential energy functions for the lowest six electronic states of ArKr⁺ using a global potential model that includes the effects of the spin-orbit, charge-exchange and long-range interactions.     

Spinor molecule in atomic Bose–Einstein condensate

We have performed two-photon photoassociation experiments in atomic Bose–Einstein condensate (BEC) of ⁸⁷Rb with spin degree of freedom which is created by all-optical method with CO₂ lasers. The spinor character of the molecules has been revealed by the photoassociation spectrum with a new structure. The hyperfine structure of the molecules near the dissociation limit is identified by observations of the Zeeman and AC-Stark effects of the molecules. The molecules have been spin-selectively probed by the use of the light shift. This result would open the new possibility of research on novel spinor molecular BEC.     

从头计算研究BCl+基态和激发态的势能曲线和光谱性质

基于相关一致极化4zeta(aug-cc-pVQZ)基组, 应用量子化学从头计算中高水平的多参考组态相互作用方法计算了BCl⁺ 两个离解极限B⁺(¹S_g)+Cl(²P_u)和B (²P_u)+Cl⁺ (³P_g)的14个Λ-S态势能曲线. 在计算中考虑了Davidson修正(+Q)和标量相对论效应, 并首次在计算中考虑了BCl⁺ 的旋轨耦合效应, 获得了由能量最低的4个Λ-S态分裂出的7个Ω 态. 计算结果表明相同对称性的Ω 态的势能曲线存在着非常明显的避免交叉. 通过分析Λ-S态的电子结构, 得到了各态的电子跃迁特性, 并确认了电子态的多组态性质. 使用LEVEL程序通过求解径向的Schrödinger方程得到了束缚Λ-S 和Ω态的光谱参数D_e, R_e, T_e, ω_e, ω_eχ_e和B_e. 通过和已有的Λ-S态X²∑⁺ 的实验数据进行对比发现, 本文所得的计算结果与实验结果非常一致. 而文中其他电子态的光谱参数均为首次报道. 关键词： 势能曲线 光谱参数 多参考组态相互作用方法 旋轨耦合     

Time-dependent analysis of tunneling effect in the formation of ultracold molecules via photoassociation of laser-cooled atoms

The paper contains a time-dependent investigation of the tunneling effect observed in the photoassociation spectrum of Cs₂ and attributed to the 0_g ^-(6s, 6p _3/2) double well. When by photoassociation of two cold cesium atoms a vibrational level of the outer well is populated, tunneling is an efficient mechanism for transferring the population to the inner well (R < 15a ₀), where spontaneous emission may lead to formation of cold molecules in low vibrational levels of the a ³Σ⁺ _u(6s, 6s) electronic state. This tunneling effect is analyzed by wavepackets propagation, first considering the double well potential alone, and following a packet made by a superposition of states initially located at large distances. Characteristic times for the vibration dynamics, corresponding to a beating phenomenon between the two wells, to partial “revival” at large distances, and to maxima in the population localized in the inner well are reported and discussed. Second, we simulate the two-channels a ³Σ⁺ _u(6s, 6s)↦0_g ^-(6s, 6p _3/2) photoassociation at detunings around 2.9 cm^-1: the inner well can be populated either by the excitation of a vibrational level of the external well (resonant excitation), or by tuning the photoassociation laser at the energy of the inner well level which displays tunneling (“off-resonance excitation”). In the first case the photoassociation is efficient, while the tunneling probability is small; in the second, the tunneling probability is large, so that despite the poor efficiency of the photoassociation process, more population can be transferred to the inner well. This second choice is shown to be very sensitive to the laser intensity, which could be used to control the population of the inner well and hence the formation of ultracold molecules in low vibrational levels. Received 19 April 2002 Published online 1st October 2002 RID="a" ID="a"e-mail: francoise.masnou@lac.u-psud.fr     

Cold rubidium molecule formation through photoassociation: A spectroscopic study of the 0 g - long-range state of 87 Rb 2

We report the detailed analysis of translationally cold rubidium molecule formation through photoassociation. Cold molecules are formed after spontaneous decay of photoexcited molecules from a laser cooled atomic sample, and are detected by selective mass spectroscopy after two-photon ionization into Rb ₂ ⁺ ions. A spectroscopic study of the 0 _g ^- (5 S + 5 P _3/2 ) pure long-range state of ⁸⁷Rb₂ is performed by detecting the ion yield as a function of the photoassociation laser frequency; the spectral data are theoretically analyzed within the semiclassical RKR approach. Molecular ionization is resonantly enhanced through either the 2 ³ Π _g or the 2 ³ Σ ⁺ _g intermediate molecular states. Some vibrational levels of the latter electronic state are observed and assigned here for the first time. Finally, cold molecules formation rates are calculated and compared to the experimentally measured ones, and the vibrational distribution of the formed molecules in the a ³ Σ ⁺ _u ground triplet state is discussed. Received 18 January 2001 and Received in final form 10 April 2001     

Resonant coupling in the formation of ultracold ground state molecules via photoassociation

We demonstrate the existence of a new mechanism for the formation of ultracold molecules via photoassociation of cold cesium atoms. The experimental results, interpreted with numerical calculations, suggest that a resonant coupling between vibrational levels of the 0+u (6s+6p1/2) and (6s+6p3/2) states enables formation of ultracold molecules in vibrational levels of the ground state well below the 6s+6s dissociation limit. Such a scheme should be observable with many other electronic states and atomic species.     

Laser induced collisional energy transfer processes in a rubidium-potassium mixture

Two laser induced collisional energy transfer processes in alkali vapours are investigated. For process K(4²S_1/2)+ Rb(5²P_3/2)+?ω_T→K(6²S_1/2)+Rb(5²S_1/2), a population inversion between the final state K(6²S_1/2) and lower states, leading to a superradiant emission has been observed. Comparison between experiment and theory shows a qualitative agreement in the limit of low atomic densities and laser power. However the transfer profile width is about two times larger than the calculated one for both processes.     

Experimental investigation of ultracold atom-molecule collisions

Ultracold collisions between Cs atoms and Cs2 dimers in the electronic ground state are observed in an optically trapped gas of atoms and molecules. The Cs2 molecules are formed in the triplet ground state by cw photoassociation through the outer well of the 0-(g) (P3/2) excited electronic state. Inelastic atom-molecule collisions converting internal excitation into kinetic energy lead to a loss of Cs2 molecules from the dipole trap. Rate coefficients are determined for collisions involving Cs atoms in either the F=3 or F=4 hyperfine ground state, and Cs2 molecules in either highly vibrationally excited states (nu'=32-47) or in low vibrational states (nu'=4-6) of the a3 summation(u)+ triplet ground state. The rate coefficients beta approximately 10(-10) cm3/s are found to be largely independent of the vibrational and rotational excitation indicating unitary limited cross sections.     

Simulation of emission spectra of the gas-discharge plasma of a krypton-xenon mixture

The narrow-band radiation observed in the range of the resonance line of xenon at 147 nm in the VUV emission spectra of the gas-discharge plasma of a krypton-xenon mixture is proposed to interpret as a manifestation of bound-bound transitions between the vibrational levels of the excited electronic states 0⁺(³ P ₁) and 1(³ P ₁) and the ground electronic state 0⁺(¹ S ₀) in the KrXe* molecule. A correction of the potential curves of the electronic states under consideration is proposed from a comparison of the calculated and experimental spectra.     

Resonant coupling in the van der Waals interaction between an excited alkali atom and a dielectric surface: an experimental study via stepwise selective reflection spectroscopy

We present a detailed experimental study of the evaluation of the van der Waals (vW) atom-surface interaction for high-lying excited states of alkali-metal atoms (Cs and Rb), notably when they couple resonantly with a surface-polariton mode of the neighbouring dielectric surface. This report extends our initial observation [Phys. Rev. Lett. 83, 5467 (1999)] of a vW repulsion between Cs(6D_3/2) and a sapphire surface. The experiment is based upon FM selective reflection spectroscopy, on a transition reaching a high-lying state from a resonance level, that has been thermally pumped by an initial one-photon step. Along with a strong vW repulsion fitted with a blue lineshift, -160±25 kHz μm³ for Cs(6D_3/2) in front of a sapphire surface (with a perpendicular c-axis), we demonstrate a weaker vW repulsion (-32±5 kHz μm³) for Cs(6D_3/2) in front of a YAG surface, as due to a similar resonant coupling at 12 μm between a virtual atomic emission (6D_3/2-7P_1/2) and the surface polariton modes. A resonant behaviour of Rb(6D_5/2) in front of a sapphire surface exists also because of analogous decay channels in the 12 μm range. Finally, one demonstrates that fused silica, nonresonant for a virtual transition in the 12 μm range and hence weakly attracting for Cs(6D_3/2), exhibits a resonant behaviour for Cs(9S_1/2) as due to its surface polariton resonance in the 8-9 μm range. The limiting factors that affect both the accuracy of the theoretical prediction, and that of the fitting method applied to the experimental data, are discussed in the conclusion. Received 16 January 2003 / Received in final form 25 March 2003 Published online 5 May 2003     

Formation of ultracold molecules via photoassociation with blue detuned laser light

We propose a new possibility to form ultracold molecules, via photoassociation of a pair of cold atoms into vibrational levels of the external well of an excited electronic state located at intermediate interatomic distance ( ≈ 20 Bohr radii), and embedded in the dissociation continuum above its dissociation limit. The existence of such a well is demonstrated by conventional free-free absorption spectroscopy at thermal energies. Estimation for cold atom photoassociation and cold molecule formation rates are obtained within a perturbative approach [Drag et al., IEEE J. Quant. Electr. 36, 1378 (2000)], and are found observable for usual conditions of photoassociation experiments. Received 1st March 2001     

Accurate studies on the full vibrational energy spectra and molecular dissociation energies for some electronic states of N<Subscript>2</Subscript> molecule

It is usually very difficult to directly obtain molecular dissociation energy D _e and all accurate high-lying vibrational energies for most diatomic electronic states using modern experimental techniques or quantum theories, and it, is also very difficult to give accurate analytical expression for diatomic molecular dissociation energy. This study proposes a new analytical formula for obtaining accurate molecular dissociation energy based on the LeRoy and Bernstein’s energy expression in dissociation limit. A set of full vibrational energy spectra for some electronic states of N₂ molecule are studied using the algebraic method (AM) suggested recently, and the corresponding accurate molecular dissociation energies are evaluated using the proposed new formula and high-lying AM vibrational energies. The results show that the AM spectra and the new theoretical dissociation energies agree excellently with experimental data, and thereby providing a new physical approach to generating accurate dissociation energies for electronic states of diatomic molecules.