超低频调制光缔合光谱的实验研究

通过激光冷却技术在磁光阱中俘获原子数约107,温度约200 μK,直径约400 μm的超冷铯原子,利用超冷铯原子光缔合方法制备了激发态的超冷铯分子。实验研究了光缔合光不同扫描速率对铯分子振转光谱分辨率的影响,发现光缔合光扫描速率较慢时,铯分子振转光谱分辨率较高。通过高灵敏的雪崩光电探测器探测冷原子荧光,获得了超冷铯分子第一激发态6S_1/2+6P_3/2离解限0-_g长程态高分辨振转光谱。为了实现受控拉曼光缔合制备超冷基态分子,光缔合激光频率需要锁定在原子-分子共振跃迁线,对超冷原子光缔合光谱进行了超低频波长调制,通过改变调制幅度和调制频率获得最优化的一阶微分信号,将该信号反馈回激光器,实现闭合环路稳频,满足了受控拉曼光缔合制备振转能级可控的基态分子的实验要求,该工作对研究受限空间中的超冷原子分子具有很重要的意义。     

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     

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.     

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)     

The laser-intensity dependence of the photoassociation spectrum of the ultracold Cs_2(6S_(1/2) + 6P_(1/2))0_u~+ long-range molecular state

The high-resolution photoassociation spectrum of the ultracold cesium molecular 0_u~+ state below the 6S 1/2 + 6P 1/2 limit is presented in this paper. The saturation of the photoassociation scattering probability is observed from the dependence of the trap-loss probability on the photoassociation laser intensity. The corresponding resonant line width is also demonstrated to increase linearly with increasing photoassociation laser intensity. Our experimental data have good consistency with the theoretical saturation model of Bohn and Julienne Bohn J L and Julienne P S 1999 Phys. Rev. A 60 1].     

Photoassociative spectroscopy as a self-sufficient tool for the determination of the Cs triplet scattering length

In photoassociation spectroscopy, the line intensities of a given vibrational progression exhibit zero-signal modulation reflecting the node structure of the s-wave ground state wave function of two free colliding atoms. This leads to the determination of the scattering length. We performed photoassociation of cold Cs atoms polarized in the Zeeman sublevel f = 4, m(f) = 4. We analyzed the intensities of the lines associated with the Cs2 0(-)(g) state dissociating to the 6s(1/2)+6p(3/2) asymptote. This yields a value of the Cs triplet state scattering length, a(T) = -530a(0), while consistency requirements impose a value of the multipole ground state molecular coefficient, C6 = 6510 a.u.     

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     

Prospects for the formation of ultracold ground state polar molecules from mixed alkali atom pairs

Photoassociation rates of mixed cold alkali atom pairs and formation rates of cold heteronuclear alkali dimers in their ground state are computed within an approach where the wave functions are calculated exactly, and the laser field is treated as a perturbation. These rates are predicted to have the same magnitude for all heteronuclear species involving either Rb or Cs atoms. Moreover, these rates are found slightly smaller than, or similar to, the same rates for Cs₂ molecules, which is encouraging for future experiments. We studied the specific case of the photoassociation into excited molecular states coupled with spin-orbit interaction, emphasizing the role of the so-called resonant coupling in the formation of stable ultracold molecules with low vibrational levels. The comparison with recent experimental results on RbCs photoassociation and cold molecule formation show their reasonable agreement with our calculations.Received: 2 July 2004, Published online: 23 November 2004PACS: 32.80.Pj Optical cooling of atoms; trapping - 33.20.Tp Vibrational analysis - 33.70.Ca Oscillator and band strengths, lifetimes, transition moments, and Franck-Condon factors     

Creating, detecting and locating ultracold molecules in a surface trap

Ultracold molecules have been produced by photoassociation of Cs atoms trapped in a mirror magneto-optical trap. The molecules were detected by resonantly enhanced multi-photon ionization followed by time-of-flight mass spectroscopy. The time-of-flight ofatomic and molecular ions was investigated in the presence of a dc bias voltageapplied to the conducting mirror. This technique provides a new tool for determining the distance between the cold molecules and the mirror surface. This revised version was published online in August 2005 with a corrected cover date.     

Anomalous frequency shift in the photoassociation spectrum of a Bose-Einstein condensate

We theoretically investigate the effect of anomalous quantum correlations on the light-induced frequency shift in the photoassociation spectrum of a Bose-Einstein condensate. Anomalous quantum correlations arise because, although formed from a pair of zero-momentum condensate atoms, a condensate molecule need not dissociate back to the atomic condensate, but may just as well form a noncondensate atom pair with equal and opposite momentum, i.e., due to rogue photodissociation. The uncorrelated frequency shift of the photoassociation spectrum is to the red and linearly dependent on the laser intensity I. In contrast, anomalous correlations due to rogue dissociation lead to a blueshifted photoassociation spectrum. For sufficiently low light intensities, the rogue blueshift is dominant and proportional to sqrt[I].     

Formation of cold Cs ground state molecules through photoassociation in the pure long-range state

We report on the formation of translationally cold Cs₂ ground state molecules through photoassociation in the 1_u attractive molecular state below the 6 s _1/2 +6 p _3/2 dissociation limit. The cold molecules are obtained after spontaneous decay of photoassociated molecules in a MOT and in a dark SPOT. We also used polarized atoms, in the f =3, m f =+3Zeeman ground state. Purely asymptotic and adiabatic calculations including hyperfine interaction and rotation are in excellent agreement with observed structures. As expected, the 1_u state is actually a pure long-range state, consisting of paired atoms, uniquely linked by the first terms of the multipole expansion of the electrostatic interaction. A temperature of 20 K has been measured for the molecular cloud. Received 19 July 1999     

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     

Creation of a molecular condensate by dynamically melting a Mott insulator

We propose the creation of a molecular Bose-Einstein condensate by loading an atomic condensate into an optical lattice and driving it into a Mott insulator with exactly two atoms per site. Molecules in a Mott insulator state are then created under well defined conditions by photoassociation with essentially unit efficiency. Finally, the Mott insulator is melted and a superfluid state of the molecules is created. We study the dynamics of this process and photoassociation of tightly trapped atoms.     

Line shape analysis of two-colour photoassociation spectra on the example of the Cs ground state

Two-photon photoassociation spectra in a Λ-type excitation scheme are analysed under the systematically varied experimental conditions of frequency detunings and laser intensities. Line shape fits are presented as well as the investigation of intensity and detuning dependent line shifts. From both we determine the attained spectroscopic precision, that is corrected for a systematic line shift due to the thermal distribution of atoms in the trap. An energy correction for this effect is given. Information about the feasibility of generating translationally cold molecules in a well defined rotational and vibrational level by the photoassociation process is derived from the analysis. Received 21 May 2002 Published online 15 October 2002 RID="a" ID="a"Current address e-mail: christian.lisdat@ptb.de RID="b" ID="b"e-mail: pierre.pillet@lac.u-psud.fr     

Continuously transferring cold atoms in caesium double magneto-optical trap

We have established a caesium double magneto-optical trap (MOT) system for cavity-QED experiment, and demonstrated the continuous transfer of cold caesium atoms from the vapour-cell MOT with a pressure of ～ 1×10^-6 Pa to the ultra-high-vacuum (UHV) MOT with a pressure of ～ 8×10^-8 Pa via a focused continuous-wave transfer laser beam. The effect of frequency detuning as well as the intensity of the transfer beam is systematically investigated, which makes the transverse cooling adequate before the atoms leak out of the vapour-cell MOT to reduce divergence of the cold atomic beam. The typical cold atomic flux got from vapour-cell MOT is ～2×10⁷ atoms/s. About 5×10⁶ caesium atoms are recaptured in the UHV MOT.     

超冷铯分子0g-长程态的振转光谱研究

通过超冷铯原子光缔合制备激发态的超冷铯分子. 利用冷原子荧光频率调制技术获得了超冷铯分子第一激发态6S_1/2+6P_3/2离解限0_g^-长程态高分辨振转光谱, 计算得到0_g^- 长程态振动量子数从0到51的不同振动能级的转动常数, 和Daniel研究小组的理论结果符合得很好. 关键词： 超冷铯分子 光缔合 振转光谱     

Effect of external magnetic field on the shift of resonant frequency in photoassociation of ultracold Cs atoms

We study the influence of external magnetic field on the shift of the resonant frequency in the photoassociation of ultracold Cs atoms, which are captured in a magnetically levitated optical crossed dipole trap. With the increase of the photoassociation laser intensity, the linear variation of the frequency shift is measured by recording the photoassociation spectra of the long-range 0_u~+ state of Cs molecule below the 6S_(1/2)+ 6P_(1/2) dissociation limit at different magnetic fields.The slope of the frequency shift to the intensity of the photoassociation laser exhibits a strong dependence on the external magnetic field. The experimental data is simulated with an analytic theory model, in which a single channel rectangular potential with the tunable well depth is introduced to acquire the influence of the magnetic field on the atomic behavior in the effective range where photoassociation occurs.     

Formation of ultracold polar molecules in the rovibrational ground state

Ultracold LiCs molecules in the absolute ground state X1Sigma+, v' = 0, J' = 0 are formed via a single photoassociation step starting from laser-cooled atoms. The selective production of v' = 0, J' = 2 molecules with a 50-fold higher rate is also demonstrated. The rotational and vibrational state of the ground state molecules is determined in a setup combining depletion spectroscopy with resonant-enhanced multiphoton ionization time-of-flight spectroscopy. Using the determined production rate of up to 5 x 10(3) molecules/s, we describe a simple scheme which can provide large samples of externally and internally cold dipolar molecules.     

Coherent transfer of photoassociated molecules into the rovibrational ground state

We report on the direct conversion of laser-cooled 41K and 87Rb atoms into ultracold 41K87Rb molecules in the rovibrational ground state via photoassociation followed by stimulated Raman adiabatic passage. High-resolution spectroscopy based on the coherent transfer revealed the hyperfine structure of weakly bound molecules in an unexplored region. Our results show that a rovibrationally pure sample of ultracold ground-state molecules is achieved via the all-optical association of laser-cooled atoms, opening possibilities to coherently manipulate a wide variety of molecules.     

Control of photoassociation reaction F+H→HF with ultrashort laser pulse

The laser-induced vibrational state-selectivity of product HF in photoassociation reaction H+F$\rightarrow$HF is theoretically investigated by using the time-dependent quantum wave packet method. The population transfer process from the continuum state down to the bound vibrational states can be controlled by the driving laser. The effects of laser pulse parameters and the initial momentum of the two collision atoms on the vibrational population of the product HF are discussed in detail. Photodissociation accompanied with the photoassociation process is also described.