Rovibrational State-Selectivity in Photoassociation through Multi-photon Transitions

The rovibrational state-selectivity in photoassociation （PA） is investigated for the ground electronic state of OH radical. The calculated results show that population can be transferred from continuum state to the target states through three-, four-, and nine-photon transitions by choosing suitable pulse parameters and initial collision energy. To control population transfer to a lower rovibrational state, a shorter pulse frequency has to be chosen and the photon number transferred to target state should be increased. In PA process, some associated OH radicals can be dissociated via intermediate and background states, which decreases the nal population of the target state.

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.

Suppressing the weakly bound states in the photoassociation dynamics by using a frequency cut-off laser pulse

The photoassociation dynamics of ultracold lithium atoms controlled by a cut-off pulse has been investigated theoretically by solving numerically the time-dependent Schr6dinger equation using the mapped Fourier grid method. The frequency components of the laser pulse close to the atomic resonance are partly cut off. Compared with the typical Gauss-type pulses, the cut-off pulse is helpful to suppress efficiently the weakly bound states and prepare the associated molecules in the lower vibrational states. Especially, the dependence of photoassociation probability on the cut-off position of the laser pulse is explored.

High-resolution photoassociation spectroscopy of ultracold Cs_2 long-range 0_g~- state: The external well potential depth

High-resolution photoassociation spectroscopy is reported using a modulation spectroscopy technology in a cesium atomic magneto-optical trap. The two lowest vibrational levels have been experimentally observed which have been theo- retically predicted in [Phys. Rev. A 75 052501 （2007）]. A new potential curve is obtained by using the Rydberg-Klein-Ress method with a well depth of -82,384 ＋ 0,026 cm-1, which is deeper than the result of previous experiment （-77.909 cm-1） and the theoretical prediction （-81.6445 cm- l ）.

Reanalysis of the photoassociation spectrum of ^(133)Cs_2 (6P_(3/2)) 1_g state

Reanalysis of the photoassociation spectrum of the weakly binding （6S1/2 ＋ 6P3/2） lg 133Cs2 levels, reported in the previous study [J. Mol. Spectro. 255 （2009） 106], is performed by using a Lu-Fano graph coupled to the improved LeRoy- Bernstein formula including two additional modified terms. A more accurate coefficient （c3） is obtained for the leading long-range potential （-c3/R3） of a diatomic molecule.

High resolution photoassociation spectra of an ultracold Cs_2 long-range 0_u^+ (6S_(1/2)+6P_(1/2) ) state

In this paper, ultracold cesium molecules are formed through photoassociation technology, which is carried out in a magneto-optical trap. High resolution photoassociaion spectra with the rotational progressions up to J = 7 are obtained. Three rovibrational levels of the long-range 0＋ state of Cs2 below the （6S1/2 ＋ 6P1/2） dissociation limit are specifically investigated. By fitting their binding energy intervals to the non-rigid rotational model, the rotational constant of the long- range 0u＋ state is determined. A proportional dependence of the value of the rotational constant on the vibrational quantum number is demonstrated.

Highly sensitive photoassociation spectroscopy of ultracold 23Na133Cs molecular long-range states below the 3S1/2＋6P3/2 limit

We present high resolution photoassociation spectroscopy of ultracold 23Na133Cs molecules in a long-range c3∑＋ state below the （3S1/2 ＋ 6P3/2） asymptote. We perform photoassociation spectroscopy in a dual-species magneto-optical trap （MOT） and detect the photoassociation resonances using trap-loss spectroscopy. By fitting the experimental data with the semi-classical LeRoy-Bernstein formula, we deduce the long-range molecular coefficient C6 and derive the empirical potential energy curve in the long-range region.

Photoassociation spectra of ultracold(85)Rb2 molecule in 0u+long range state near the 5S(1/2)+5P(1/2)asymptote

We investigate the high resolution photoassociation spectra of ^（85）Rb_2 molecules in 0~＋_u long range state below the（5S_（1/2）＋ 5P_（1/2）） asymptote. The ^（85）Rb atomic samples are trapped in a dark magneto–optical trap（MOT） and prepared in the dark state. With the help of trap loss technique, we obtain considerable photoassociation spectroscopy with rovibrational resolution, some of which have never been observed before. The observed spectrum is fitted by a rigid rotation model, and the rotational constants of ultracold ^（85）Rb_2 molecule in long range 0~＋_u are obtained for different vibrational states. By applying the Le Roy–Bernstein method, we assign the vibrational quantum numbers and derive C_3 coefficient, which is used to obtain the potential energy curve.

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＋ state below the 6S1/2 ＋ 6PI/2 limit is presented in this paper. The saturation of the photoassociation scattering probability is observed from the depen dence 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 con sistency with the theoretical saturation model of Bohn and Julienne [Bohn J L and Julienne P S 1999 Phys. Rev. A 60 1].

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→HF is theoret- ically 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.

Enhancement of the photoassociation of ultracold atoms via a non-resonant magnetic field

We report an effective method for enhancing the photoassociation of ultracold atoms using a non-resonant magnetic field,which enables the manipulation of the coupling between the wavefunctions of the colliding atomic pairs and the excited molecules.A series of photoassociation spectra are measured for different magnetic fields.We show that the photoassociation rate is significantly dependent on the non-resonant magnetic field.A qualitatively theoretical explanation is provided,and shows a good agreement with the experimental result.

Photoassociation of ultracold RbCs molecules into the (2)0^- state (v = 189, 190) below the 5S_(1/2) + 6P_(1/2) dissociation limit

Ultracold polar RbCs molecules are produced via photoassociation in a laser-cooled mixture of ^85Rb and ^133Cs atoms. The a3∑＋ state molecules which decay from electronically excited （2）0- state RbCs molecules are detected by resonance- enhanced two-photon ionization. The new rovibrational levels （v = 189, 190） in the （2）0- state are also observed, which exist in theory and have not been observed in experiments yet. The corresponding rotational constants are measured by photoassociation spectroscopy, which are consistent with theoretical calculations using a nonrigid rotor model.

Theoretical simulation of the photoassociation process for NaCs

We investigate the two-step association process of NaCs using the time-dependent wave packet method.Ground state atoms can be photoassociated to the low vibrational levels of the ground state for an NaCs molecule by the two-step association.The time-dependent Schro¨dinger equation of the association process is solved within a three-state model and the wave packet is propagated with the ＂split operator-Fourier transform＂ scheme and the rotating-wave approximation（RWA）.The vibrational population distribution of the ground state can be obtained by projecting the wave packet to every vibrational level of the ground state.The results not only show that for NaCs achievement of photoassociation production is accompanied by the photodissociation of the higher vibrational molecules,but also show that the vibrational distribution in lower vibrational levels of the ground state changes with the laser parameters.

High sensitive detection of high-order partial wave scattering in photoassociation of ultralcold atoms

We report on the observation of enhanced high-order partial wave scattering from atom atom interaction via changing the temperature of a magneto optical trap in the process of photoassociation. The high-order scattering partial wave is directly manifested through the large signal amplitude of the rovibrational resonance levels of trap-loss spectroscopy from photoassociation.

Production and Detection of Ultracold Ground State 85Rb133Cs Molecules in the Lowest Vibrational Level by Short-Range Photoassociation

We investigate the production of ultracold ground state x^1∑7＋（u = 0） RbCs molecules in the lowest vibrational level via short-range photoassociation followed by spontaneous emission. The starting point is the laser cooled 85Rb and laa cs atoms in a dual species, forced dark magneto-optical trap. The special intermediate level （5）O＋ （u = 10） correlated to the （2）311 electric state is achieved by the photoassociation process. The formed ground state X1∑＋ （u = 0） molecule is resonantly excited to the 2111 intermediate state by a 651 nm pulse laser and is ionized by a 532nm pulse laser and then detected by the time-of-flight mass spectrum. Saturation of the photoionization spectroscopy at large ionization laser energy is observed and the ionization efficiency is obtained from the fitting. The production of ultracold ground state 85Rblaacs molecules is facilitative for the further research about the manipulation of ultracold molecules in the rovibrational ground state.

Photoassociation of NaRb with an asymmetric laser pulse

We investigate the photoassociation dynamics of cold NaRb molecule controlled by an asymmetric laser pulse called slowly-turned-on and rapidly-turned-off(STRT) laser pulse. This new shaped laser pulse has a remarkable merit, compared with the typical Gauss-type pulses, so that we can efficiently associate molecules with the state expected instead of going back to the continuum state. Using the three-state model, we solve the quantum mechanical equation with the "split operator-Fourier transform" method under the rotating-wave approximation(RWA) in propagation of the wave packet. By the projection of the obtained wave function onto each vibrational state, we can get the vibrational population of the ground electronic state. The results reveal that, with the STRT laser pulse, an efficient photoassociation process can be achieved and the vibrational distribution in the ground state can be controlled by the laser parameters.

Formation of NaH Molecules in the Lowest Rovibrational Level of the Ground Electronic State via Short-Range Photoassociation

The formation of NaH molecules in the lowest rovibrational level of the ground electronic state is investigated using a pump-dump photoassociation(PA)scheme.In short-range region,two colliding atoms Na and H are efficiently associated into the NaH molecule in the rovibrational|0,0i state of the ground electronic state via the intermediately rovibrational|10,1i state of the excited electronic state.The changes of populations with the electric field amplitudes,frequency detunings,dump pulse duration and delay time between two laser pulses are calculated and discussed.The PA probability reaches 0.623 with a high state-selectivity.

Cold cesium molecules produced directly in a magneto-optical trap

We report on the observation of ultracold ground electric-state cesium molecules produced directly in a magneto-optical trap with a good signal-to-noise ratio. These molecules arise from the photoassociation of magneto-optical trap lasers and they are detected by resonantly enhanced multiphoton ionization technology. The production rate of ultracold cesium molecules is up to 4× 10^4 s-1. We measure the characteristic time of the ground electric-state cesium molecules generated in the experiment and investigate the Cs2＋ molecular ion intensity as a function of the trapping laser intensity and the ionization pulse laser energy. We conclude that the production of cold cesium molecules may be enhanced by using appropriate experimental parameters, which is useful for future experiments involving the production and trapping of ultracold ground electric-state molecules.

Generation of Coherent Trimers from Bose-Condensed Atoms via a Generalized Stimulated Raman Adiabatic Passage

We propose to use a generalized technique of stimulated Raman adiabatic passage to create an atom-molecule dark state that permits the enhanced coherent creation of triatomic molecules in a repulsive atomic Bose-Einstein condensate. As an interesting comparison, the similar cases of creating heteronuclear （bosonic or fermionic） trimers are also briefly discussed.

The effect of field modulation on the vibrational population of the photoassociated NaK and its dynamics

This paper presents calculation results for the photoassociation of a NaK molecule with a two-color modulated laser and gives a detailed analysis about them.For the two-step photoassociation process in intense fields,the effect of two-color modulated laser parameters,such as relative phase,envelope period,and laser intensity,on the population of the molecular electronic state can be obtained by solving the time-dependent Schrodinger equation through the quantum wave packet method.The numerical simulation shows not only that the influence of laser parameters on the vibrational distribution presents some regularity,but also that a higher population in the ground electronic state can be realized through adjusting these laser parameters.