The formation of an intense secondary pulsed molecular beam and obtaining accelerated molecules and radicals in it

A method for obtaining an intense secondary pulsed molecular beam is described. The kinetic energy of molecules in the beam can be controlled by vibrational excitation of the molecules in the source under high-power IR laser radiation. A compression shock (shock wave) is used as a source of secondary beams. The shock wave is formed in interaction between an intense pulsed supersonic molecular beam (or flow) and a solid surface. The characteristics of the secondary beam were studied. Its intensity and the degree of gas cooling in it were comparable with the corresponding characteristics of the unperturbed primary beam. Vibrational excitation of molecules in the shock wave and subsequent vibrational-translational relaxation, which occurs when a gas is expanded in a vacuum, allow the kinetic energy of molecules in the secondary beam to be substantially increased. Intense [≥10²⁰ molecules/(sr s)] beams of SF₆ and CF₃I molecules with kinetic energies approximately equal to 1.5 and 1.2 eV, respectively, were generated in the absence of carrier gases, and SF₆ molecular beams with kinetic energies approximately equal to 2.5 and 2.7 eV with He (SF₆/He=1/10) and H₂ (SF₆/H₂=1/10) as carrier gases, respectively, were obtained. The spectral and energy characteristics of acceleration of SF₆ molecules in the secondary beams were studied. The optimal conditions were found for obtaining high-energy molecules. The possibility of accelerating radicals in secondary molecular beams was demonstrated.     

Photoassociation experiments with ultracold metastable helium

The present article gives a review of various photoassociation (PA) experiments performed at ENS with a gas of ultracold atoms of metastable helium in the 2³S₁ state, using a PA laser beam red-detuned from the 2³S₁-2³P transitions. Molecular spectra close to the D₂ atomic line (2³S P₂) are presented. All the measured lines are identified as a signature of molecular bound states having a strong (if not pure) quintet spin character at short interatomic distance. Close to the D₀ atomic line (2³S P₀), giant helium dimers can be produced [see Phys. Rev. Lett. 91, 073203 (2003)]. A laser set-up improved recently allows us to measure very accurately the binding energy of the ro-vibrational ground state of the 0 _u ⁺ purely long-range potential and the agreement with the theory published previously is excellent. Finally, preliminary results on 2 photon PA spectroscopy are given.Received: 1 July 2004, Published online: 26 October 2004PACS: 32.80.Pj Optical cooling of atoms trapping - 33.20.Kf Visible molecular spectra - 34.50.Gb Electronic excitation and ionization of molecules - 34.20.Cf Interatomic potentials and forcesJ. Léonard: Present address: Van der Waals-Zeeman Institute, Universiteit van Amsterdam, The Netherlands.M. Walhout: Permanent address: Calvin College, Grand Rapids, MI, USA.     

Improved molecular constants for the and states of NaH

Improved molecular constants for the and states of the NaH molecule are presented. NaH molecules are produced by reactive scattering of H and Na₂ in a crossed beam experiment. High vibrational levels (6 9) of the NaH molecules are predominantly populated. Their excitation spectrum in the range has been measured using a new variant of Doppler spectroscopy. The transition frequencies involving the vibrational levels 2 8 in the and 6 9 in the state have been determined with an accuracy of better than . Using also previously published data a new set of molecular constants for the and state is derived. In particular, the vibrational dependence of the rotational constants B, D and H as well as some of v”-v' band origins for and is determined. The transition frequencies measured here or published previously are reproduced by these new coefficients with an accuracy of 0.1 cm^-1 [rms value] with a maximum deviation of 0.4 cm^-1. New RKR potential energy curves have been calculated up to the turning points of the levels v” = 9 in the state and v' = 25 in the state. Received 21 August 1999     

Slow ammonia molecules in an electrostatic quadrupole guide

An electrostatic quadrupole is used to filter slow dipolar ND₃ molecules from an effusive source and to guide them into ultrahigh vacuum. The molecules in the electrostatic quadrupole experience a Stark interaction which allows filtering of small velocities in the linear and bent sections of the quadrupole. With this technique we demonstrate a flux of /s with a longitudinal temperature of a few K. The technique and the set-up are discussed in detail, and the guided gas as well as the output beam are characterized. Improvements in the set-up are highlighted, as for instance cooling of the effusive source to below 150 K.Received: 1 July 2004, Published online: 28 September 2004PACS: 33.55.Be Zeeman and Stark effects - 39.10. + j Atomic and molecular beam sources and techniques     

Formation of ultracold polar molecules via Raman excitation

Alkali hydride molecules are very polar, exhibiting large ground-state dipole moments. As ultracold sources of alkali atoms, as well as hydrogen, have been created in the laboratory, we explore theoretically the feasibility of forming such molecules from a mixture of the ultracold atomic gases, employing a two-photon stimulated radiative association process -- Raman excitation. Using accurate molecular potential energy curves and dipole transition moments, we have calculated the rate coefficients for populating all the vibrational levels of the X state of LiH via the excited A state. We have found that significant molecule formation rates can be realized with laser intensities and atomic densities that are attainable experimentally. Because of the large X state dipole moment, rapid cascade occurs down the ladder of vibrational levels to v = 0. The calculated recoil momentum imparted to the molecule is small, and thus negligible trap loss results from the cascade process. This allows for the build-up of a large population of v = 0 trapped molecules.Received: 31 August 2004, Published online: 23 November 2004PACS: 34.50.Rk Laser-modified scattering and reactions - 32.80.Pj Optical cooling of atoms; trapping - 33.20.Vq Vibration-rotation analysis     

Plasma parameter diagnosis using hydrogen emission spectra of a quartz-chamber 2.45 GHz ECRIS at Peking University

A quartz-chamber 2.45 GHz electron cyclotron resonance ion source(ECRIS) was designed for diagnostic purposes at Peking University [Patent Number: ZL 201110026605.4]. This ion source can produce a maximum 84 m A hydrogen ion beam at 50 k V with a duty factor of 10%. The root-mean-square(RMS) emittance of this beam is less than 0.12π mm mrad. In our initial work,the electron temperature and electron density inside the plasma chamber had been measured with the line intensity ratio of noble gases. Based on these results, the atomic and molecular emission spectra of hydrogen were applied to determine the dissociation degree of hydrogen and the vibrational temperature of hydrogen molecules in the ground state, respectively. Measurements were performed at gas pressures from 4×10~(-4) to 1×10~(-3) Pa and at input peak RF power ranging from 1000 to 1800 W. The dissociation degree of hydrogen in the range of 0.5%-10% and the vibrational temperature of hydrogen molecules in the ground state in the range of 3500-8500 K were obtained. The plasma processes inside this ECRIS chamber were discussed based on these results.     

Rotational structures of long-range diatomic molecules

We present a systematic understanding of the rotational structure of a long-range (vibrationally highly-excited) diatomic molecule. For example, we show that depending on a quantum defect, the least-bound vibrational state of a diatomic molecule with -C _n /r ⁿ (n > 2) asymptotic interaction can have only 1, 2, and up to a maximum of n-2 rotational levels. A classification scheme of diatomic molecules is proposed, in which each class has a distinctive rotational structure and corresponds to different atom-atom scattering properties above the dissociation limit.Received: 15 June 2004, Published online: 28 September 2004PACS: 33.15.Mt Rotation, vibration, and vibration-rotation constants - 34.10. + x General theories and models of atomic and molecular collisions and interactions (including statistical theories, transition state, stochastic and trajectory models, etc.) - 03.75.Nt Other Bose-Einstein condensation phenomena - 03.75.Ss Degenerate Fermi gases     

Collisions between molecules in the <Emphasis Type="Italic">J</Emphasis> = 0 state

Collisions between electrostatically trapped molecules in the J = 0 state are theoretically investigated. Molecules in this state are advantageous for the evaporative cooling, because inelastic collision is impossible at ultra-low temperature. However, inelastic collision is more significant than elastic collision at high temperature, because the off-diagonal dipole matrix elements are much larger than the diagonal elements. The elastic and inelastic collision cross-sections are calculated under the condition that the collisional kinetic energy is larger than the energy gap between the rotational states. The dependencies of the collision cross-sections on the collisional kinetic energy and molecular constants are examined.Received: 29 July 2004, Published online: 21 September 2004PACS: 31.15.Qg Molecular dynamics and other numerical methods - 33.80.Ps Optical cooling of molecules; trapping - 33.90. + h Other topics in molecular properties and interactions with photons     

Optimizing the photoassociation of cold atoms by use of chirped laser pulses

Photoassociation of ultracold atoms induced by chirped picosecond pulses is analyzed in a non-perturbative treatment by following the wavepacket dynamics on the ground and excited surfaces. The initial state is described by a Boltzmann distribution of stationary continuum states. The chosen example is photoassociation of cesium atoms at temperature K from the continuum to bound levels in the external well of the 0 _g ^-(6s + 6p _3/2) potential. We study how the modification of the pulse characteristics (carrier frequency, duration, linear chirp rate and intensity) can enhance the number of photoassociated molecules and suggest ways of optimizing the production of stable molecules.Received: 30 June 2004, Published online: 23 November 2004PACS: 33.80.Ps Optical cooling of molecules; trapping - 33.80.-b Photon interactions with molecules - 33.90. + h Other topics in molecular properties and interactions with photons - 33.80.Gj Diffuse spectra; predissociation, photodissociation     

Density functional study of the molecular structures,infrared and Raman spectra of carbon suboxide,its sulfur and selenium analogues

Carbon suboxide, and its sulfur and selenium analogues in D _∞h symmetry have been studied in the gas phase by a density functional method using B3LYP as the functional. The basis sets employed are 6-31++G(d,p), 6-311++G(d,p), cc-pVDZ and all calculations have been carried out using Gaussian 03W. Molecular parameters, namely bond lengths, rotational constants, quadrupole moments, and infrared and Raman frequencies are predicted for these molecules. Atomization energies have also been predicted. The calculated molecular parameters and vibrational spectra of the parent molecule, namely carbon suboxide, are in good agreement with literature data. Therefore, data from the present theoretical gas phase study are expected to be valid for the molecular structures and vibrational spectra of carbon subsulfide and carbon subselenide. The results from this study could be used as a reference for these molecules.     

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.     

FTIR spectroscopic and quantum-chemical studies on some tribromoindenes and their isomers

Combined experimental and computational studies on molecular structure of newly synthesised transtirans 1,2,3-tribromo-1,2,3-trihydro-¹H-benz[f]indene (TTTBI) were reported. Also, only computational studies were done for cis-trans-1,2,3-tribromo-1,2,3-trihydro-¹H-benz[f]indene (CTTBI) and cis-cis-1,2,3-tribromo-1,2,3-trihydro-¹H-benz[f]indene (CCTBI) in order to understand the vibrational spectra and molecular parameters of them. The geometry optimization and vibrational wave numbers of the title molecules were carried out with the Gaussian98 program package by using Hartree-Fock (HF) and Density Functional Theory (DFT) with B3LYP functional and 6–31G (d) basis set. All calculations were done for the title compounds in their ground states. Especially for CTTBI and CCTBI, which could not be synthesized yet, these kind of pre-calculations take an important role for their synthesis process. Also crystal structural parameters of TTTBI by single-crystal X-ray diffraction method was used as input for computational study of it. Observed and calculated vibrational wave numbers were compared. Because the use of benz[f]indene as a cyclopentadienyl ligand attracted much attention because an annulated benzo ring might increase both the stereocontrol and productivity of catalytic system, TTTBI and other computationally studied and modeled two molecules may play an important role of other types of compounds as a starting structures.     

Sensitivity of the dynamics of Na + Na$\mathsf{_2}$ collisions on the three-body interaction at ultralow energies

We have studied the quantum dynamics of collisions between spin-stretched Na atoms and Na₂ molecules. Cross-sections and rate coefficients for vibrational relaxation of Na₂(v,j = 0) have been computed in the 1 nK-0.1 mK energy range using an accurate time-independent method based on hyperspherical coordinates. The complex scattering length and the extension of the Wigner region have been determined. A detailed study of the sensitivity of collisional quantities on the three-body interaction at short distance has been performed. They are very sensitive to three-body effects for the vibrational state v = 1 of Na₂. Rotational distributions have also been calculated and show a more pronounced sensitivity on the three-body interaction, even for v = 2 and 3.Received: 29 March 2004, Published online: 22 June 2004PACS: 34.50.-s Scattering of atoms and molecules     

The fate of the OH radical in molecular beam sampling experiments

The collisional history of ionized molecules in a molecular beam mass spectrometric flame experiment is target of our present investigation. Measurements in a double imaging photoelectron photoion coincidence spectroscopy (i²PEPICO) were performed at the Swiss Light Source (SLS) of the Paul Scherrer Institute to use the ion imaging device for separating the molecular beam ions from rethermalized ions. This enables the precise composition study of the individual types of ions. Results show clearly for the OH radical that the complete signal is obtained from the molecular beam, while the signal from other combustion compounds features additional rethermalized molecules. As for OH radicals, the mole fraction is reduced by sampling effects and contact with the ionization vessel walls significantly. Consequently, this leads to signal loss and lower mole fractions, when using ionization cross sections for the quantification. To improve on this, a beam fraction (BF) factor is presented. The factor describes the ratio of the separated beam signal without rethermalized ions with the total ion signal, consisting of the mass to charge ratio from the molecular beam and additional rethermalized ions. Since the detected OH radicals are solely from the molecular beam, a new method of comparing two molecular beam alignments using the OH to H₂O signal ratio is presented. This method has a decent potential for the optimization of the quality of molecular beams. Finally, the separated beam signal (without the rethermalized ions) was used to determine mole fraction profiles for the OH radical using ionization cross sections. These profiles are in good agreement with model predictions of the USC-II and the Aramco Mech 2.0 mechanisms, while the total signal leads to factor of 12 smaller OH mole fractions.     

Electronic spectra of XeNe molecules in the range 77100-90100 cm-1 near Xe* (6p, 5d, 6p’, 7s, 7p, 6d) obtained by the (3 + 1) REMPI and (2 + 1) REMPI methods

The electronic spectra of XeNe molecules in the range of 77100-90100 cm^-1 are measured by the method of laser resonance multiphoton ionization in a supersonic jet. The photoionization spectra are obtained upon two- and three-photon excitations of molecules and their ionization by the next photon. In the range of 80300-90100 cm^-1 near Xe*(5d, 6p’, 6d, 7s, and 7p), the spectra are obtained for the first time. A whole number of vibrational systems are measured in this range. The majority of vibrational systems near Xe* (5d, 6d, 7p, and 7s) are located in the red range with respect to their dissociation limits. In the blue range with respect to the dissociation limits, continua corresponding to transitions of molecules from the ground state to repulsive potential curves of excited states are detected. For a number of excited states of XeNe molecules, the vibrational analysis is performed and molecular constants are estimated.     

Monte Carlo calculations of reaction rates and energy distributions among reaction products. Reactions of HF and DF with H and D-atoms

Rate coefficients are calculated for the reactions of H and D-atoms with vibrationally excited HF and DF molecules. Three-dimensional classical trajectories of the collision dynamics of these reactions have been calculated by means of the London-Eyring-Polanyi-Sato (LEPS) potential energy surface. The Monte Carlo procedure is used to start each collision trajectory. Results of this study indicate that (a) chemical exchange provides an efficient mechanism for relaxing vibrationally excited HF and DF molecules by H and D-atoms; (b) multiple-quantum transitions are important in the deactivation processes; and (c) both vibration-translation and vibration-rotation energy transfers contribute to vibrational relaxation of vibrationally excited HF and DF molecules by H and D-atoms. The vibrational relaxation of HF (v = 1) by H-atoms is faster than the vibrational relaxation of DF (v = 1) by H-atoms. A similar effect is indicated for D-atoms; i.e. the vibrational relaxation of DF (v = 1) by D-atoms is faster than the vibrational relaxation of HF (v = 1) by D-atoms. Room temperature vibration to translation-rotation (V → T, R) relaxation rates in units of (μsec Torr)^-1 are as follows: 13·8 × 10^-2 for HF (v = 1) by H, 3·1 × 10^-2 for DF (v = 1) by D, 5·5 × 10^-3 for HF (v = 1) by D, and 1·9 × 10^-2 for DF (v = 1) by H. Rates of deactivation of vibrationally excited HF and DF molecules by H and D-atoms are very fast. Rate coefficients are provided for many reactions that have not been measured experimentally.     

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     

Temperature determination of (CF<Subscript>3</Subscript>I)<Subscript><Emphasis Type="Italic">N</Emphasis></Subscript> clusters in a beam by time-of-flight measurements of IR-laser excited SF<Subscript>6</Subscript> molecules sublimating from the surface of clusters

The method is described and the experimental results are presented on the temperature determination of the (CF₃I) _N clusters in a beam (N ⩽ 10² is a number of monomers in a cluster) using SF₆ molecules from intersecting molecular beam as probe thermometers. The SF₆ molecules are captured by clusters in the crossed cluster and molecular beams and, after a certain time, sublimate from the surface of clusters carrying information on the velocity and temperature (internal energy) of clusters. Using time-of-flight (TOF) method the kinetic energy (velocity) of sublimated SF₆ molecules was measured and the temperature of clusters was determined to be T _cl = (88 ± 15) K.     

Measurement of nanoparticle temperature in a (CO2) N cluster beam using SF6 molecules as tiny probe thermometers

A temperature measurement technique using SF₆ molecules as tiny probe thermometers is described, and results are presented, for large (CO₂) _N van der Waals clusters (with N ≥ 10²) in a cluster beam. The SF₆ molecules captured by (CO₂) _N clusters in crossed cluster and molecular beams sublimate (evaporate) after a certain time, carrying information about the cluster velocity and internal temperature. Experiments are performed using detection of these molecules with an uncooled pyroelectric detector and infrared multiphoton excitation. The multiphoton absorption spectra of molecules sublimating from clusters are compared with the IR multiphoton absorption spectra of SF₆ in the incoming beam. As a result, the nanoparticle temperature in the (CO₂) _N cluster beam is estimated as T _cl < 150 K. Time-of-flight measurements using a pyroelectric detector and a pulsed CO₂ laser are performed to determine the velocity (kinetic energy) of SF₆ molecules sublimating from clusters, and the cluster temperature is found to be T _cl = 105 ± 15 K. The effects of various factors on the results of nanoparticle temperature measurements are analyzed. The potential use of the proposed technique for vibrational cooling of molecules to low temperatures is discussed.     

激光冷却获得高亮度的亚稳态惰性气体原子束和原子阱

高强度的亚稳态惰性原子束流在原子分子物理实验研究中具有广泛的应用.使用射频电离方法和激光横向冷却技术制备了高强度的亚稳态氪原子束流,并使用数值模拟方法对横向冷却激光场中的原子径迹进行了分析.通过激光诱导荧光光谱方法测量原子束的束流特性,结果显示,横向冷却后在束流源下游230 cm处的原子束流强度达1.6atoms/(s*sr),束流强度提高了两个量级.利用这种高强度原子束流,我们成功囚禁了1.3×10¹⁰个亚稳态⁸⁴Kr原子,同时冷原子装载速率达到了3.0×10¹¹atoms/s;并利用该装置成功地实现了高亮度的亚稳态氩原子束和原子阱. 关键词： 横向冷却 原子束 原子阱 惰性气体