Generation of intense pulsed low-kinetic-energy molecular beams

A method for the generation of intense pulsed low-kinetic-energy molecular beams is described. The method is based on the formation of a cold (≈77 K) pressure shock as a result of interaction between an intense pulsed gas-dynamically cooled molecular beam with a solid surface. The pressure shock is used as a source of a secondary beam for generating low-energy molecules. The suggested method was used to obtain intense molecular beams of H₂, He, CH₄, N₂, and Kr with kinetic energies lower than or equal to 10 meV and H₂/Kr and He/Kr molecular beams with kinetic energies of H₂ and He molecules lower than 1 meV. The energy (velocity) of molecules in low-energy beams can be controlled by varying the intensity of the initial beam or temperature in the pressure shock.     

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.     

Pressure-shock-controlled pulsed molecular beams

A method of controlling the duration of pulses of intense molecular beams is suggested. The idea of the method is the shortening of an initial molecular beam pulse by producing a pressure shock in front of a solid surface through which the beam passes. Experiments on shortening H₂, He, SF₆, SF₆/H₂(1/10), and SF₆/He(1/10) molecular beam pulses are reported. The parameters of the beams incident on, and transmitted through, the surface are studied. The gas density in the initial beam and in the pressure shock before the surface is estimated. The intensity and duration of shortened molecular pulses are found as a function of the initial intensity, angle of incidence, and the diameter of a hole on the surface through which the beam passes. It is established that the duration of the shortened beam decreases greatly with increasing incident intensity and decreasing hole diameter. It is shown that intense pulsed H₂, He, SF₆, SF₆/H₂(1/10), and SF₆/He(1/10) molecular beams with a pulse duration of ≤10–15 μs and an extent of ≤1–2 cm can be generated with the method suggested.     

Generation of high-energy secondary pulsed molecular beams

A method is suggested for generating high-intensity secondary pulsed molecular beams in which the kinetic energy of molecules can be controlled by an intense laser IR radiation through the vibrational excitation of molecules in the source. High-intensity [≥10²⁰ molecule/(sr s)] SF₆ molecular beams with a kinetic energy of ?1.0 eV without carrier gas and of ?1.9 and ?2.4 eV with carrier He (SF₆/He=1/10) and H₂ (SF₆/H₂=1/10) gases, respectively, were obtained.     

On the depolarization of ultracold neutrons in traps

The method of pulse duration control is proposed for intense molecular beams. The method is based on the shortening of a primary molecular-beam pulse through the formation of a pressure shock ahead of a solid surface through which the beam is passed. The method was used to obtain intense SF₆, H₂, He, SF₆/H₂ (1/10), and SF₆/He (1/10) molecular beams with a pulse duration of ≤10?15 μs and a spatial length of ≤1?2 cm.     

Inelastic neutron scattering from H2 on vapour deposited CO2

Inelastic neutron scattering spectra at 17 meV and 68 meV incident energies of molecular hydrogen adsorbed on vapour deposited substrates of pure CO₂, 90:10 and 50:50 CO₂:Kr are reported. The ortho-para transition is shifted from 14.7 meV in the free H₂-molecule to 9.4 meV in a presumably commensurate ortho-H₂ monolayer on the CO₂ surface. The quadrupole-quadrupole interaction of ortho-H₂ molecules with the CO₂ substrate results in a strongly anisotropic potential. In addition to rotations the dynamics of this layer comprise a local Einstein mode and phonons in resonance with the substrate, giving rise to intense multiphonon transitions. Quasielastic scattering on warmer samples is assigned to a liquidlike adsorption layer, in which the H₂ rotations are strongly perturbed. Received: 15 October 1996 / Revised: 25 August 1997 / Accepted: 24 October 1997     

Diagnostics of pulsed molecular beams and free jets with pyroelectric detectors and TEA CO2 lasers

A pyroelectric detector with a time resolution of 3–5 s and a TEA CO₂ laser have been used in diagnostics of a pulsed molecular beam (a free jet). The kinetic energy distribution of molecules was determined by using time-of-flight measurements both with a laser and without it. A combination of the laser with the pyroelectric detector makes it possible to determine the kinetic energy distribution of molecules in a selected internal state and to measure the energy absorted by the molecules of the beam from a laser pulse. The results obtained for pure SF₆ and the SF₆ seeded in He have been presented and analyzed. The advantages and the disadvantages of the method are being discussed in comparison with other available methods of diagnostics of molecular beams and free jets.     

Investigation of atomic and molecular clustering in a pulsed gas-dynamic jet with a pyroelectric detector

The clustering of atoms and molecules in a pulsed gas-dynamic jet has been investigated by the method of time-of-flight measurements performed with an uncooled pyroelectric detector (PED). The method is based on measuring the amplitude of the pyroelectric signal induced on the detector by a molecular (atomic) beam and the particle velocity in the beam as a function of the gas pressure above the nozzle. In addition, the number of molecules (atoms) emerging from the nozzle in a pulse has been measured. We describe the method and present the results of our studies on the clustering of He, Xe, CH₄, CO₂, and other gases. The peculiarities of the detection of molecular and cluster beams with PED are considered. We show that the described method allows the clustering threshold as a function of the gas pressure above the nozzle to be determined. We have established the threshold pressures at which particle clustering in the jet begins. Optimal conditions for the generation of intense cluster beams have been found.     

Molecular beam diagnostics by means of fast superconducting bolometer and pulsed infrared laser

The laser-bolometric infrared spectroscopy is an efficient method for measuring the internal energy distributions of molecular beams. Additional informations about the kinetic energy distribution of molecules in a selected internal state can be obtained from time resolved experiments. A fast superconducting bolometer and a pulsed infrared CO₂ laser have been used for testing the use of this technique as a universal tool for molecular beam diagnostics. Experimental results are presented and analyzed for pure SF₆ and helium seeded with 5% SF₆ beams. The efficiency of fast superconducting bolometers, used for molecular beam time-of-flight measurements, is discussed. A comparison is made between time resolved laser-bolometric technique and alternative molecular beam diagnostic methods.     

Kinetic energy of structural protons in silica xerogels

The kinetic energies of the protons in the silanol groups (Si–OH units) of silica xerogels were deduced by ab initio calculations using the basis set mp2/6-311G**. The silanol groups were simulated using the Si(OH)₄ unit. The calculated result of the H-kinetic energy was found to be 150 meV, which is ~ 50% smaller than a recently reported experimental value for porous silica xerogels. For comparison, the same calculations of the proton kinetic energies of other H-containing molecules such as H₂O and CH₄ (being also ~ 150 meV) were found to be in excellent agreement with measurements. Possible reasons for the huge deviations in the case of the silanols are discussed.     

Optical study of a pulsed molecular beam

By using absorption spectra in a pulsed molecular beam, the rotational temperature and the flow density of the jet are deduced. By using this technique, a comparison between a pulsed and a continuous beam is also reported for NH₃, CF₂Cl₂, and C₂H₃Cl molecular beams. Moreover, the behaviour of the temperature and density inside the pulsed beam is analyzed as a function of time for pure Ammonia. From these measurements, we deduce that a small improvement is obtained for absorption spectroscopy in the jet by using a pulsed molecular beam.     

Specular reflection of helium and hydrogen molecular beams from the (111) plane of silver

The Debye—Waller (DW) factor in the specular reflection intensity of He and H₂ molecular beams from the Ag (111) plane has been studied experimentally and theoretically. A new expression for the DW factor corrected for a stationary part of the gas—surface interaction potential is derived kinematically and semi-classically by the use of a Morse potential. An analysis of the experimental data through the above DW factor yields a surface Debye temperature of 251 ± 20 K, which is unusually high, and potential depths of 1.5 ± 1.0 meV for He and 6.4 ± 2.9 meV for H₂, which seem slightly too small. These results are discussed on the basis of the nature of gas-surface interactions and in comparison with the results deduced from the conventional DW factor corrected for a constant attractive potential depth.     

Electron beam-adsorbate interactions on silicon surfaces

The interactions which occur between electron beams in the energy range 0.5–2.5 keV, with currents of 0.1–1.0 microA and various adsorbates (H₂, CO, CH₄ and C₂H₄) on silicon surfaces have been investigated. The accumulation of beam induced dissociation products on the surface has been monitored by Auger spectroscopy, and the extent of electron stimulated desorption of neutral molecules has been determined mass spectroscopically. Thermal desorption spectra for various gases have also been obtained in order to compare adsorption behaviour with and without the presence of an electron beam. It is concluded that serious experimental errors may occur when LEED and AES are used in adsorption studies, particularly where comparatively weak binding energies are involved.     

Totale Streuquerschnitte für den Stoß von H2, D2 und He an den Edelgasen Ne,Ar, Kr und Xe im thermischen Energiebereich

The velocity dependence of the total elastic cross section has been measured for the scattering of H₂, D₂, and He beams by Ne, Ar, Kr, and Xe gases. Velocity-selected beams were attenuated by gas in a scattering chamber. A universal detector, with a magnetic mass separator, was used in conjunction with lock-in techniques. The results are compared with quantum mechanical calculations using a Lennard-Jones-(12.6)-potential, and employing suitable averaging over experimental velocity distributions. Potential parameters are presented. These are in good agreement with those expected from other methods of measurement.     

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.     

Scattered-wave calculations of photoionization cross-sections and asymmetry parameters for CO,H2O and H2S

Partial photoionization cross-sections and asymmetry parameters are calculated for the valence orbitals of the molecules CO, H₂O, and H₂S and of the atoms O and S using a recently developed extension of the self-cosistent field— Xα—scattered-wave method to continuum states. The convergence of the partial-wave expansions for both initial and final states is studied for electron kinetic energies in the range 2–1000 eV. Since convergence is very slow at high kinetic energies, the interesting region between 2 and 50 eV is emphasized, and comparisons are made with experimental UV photoemission results where such data are available. Overall the method appears to be far more reliable than previous calculations for polyatomic molecules which have used plane-wave or orthogonalized plane-wave final states.     

100 MW, 248.4 nm,KrF laser excited by an electron beam

Laser oscillations have been observed at 248.4 nm from excited KrF molecules. The excited KrF molecules were produced by injecting an intense electron beam into mixtures of Ar, Kr and F₂. A peak power of 1.15 × 10⁸ W with a total energy of 5.6 J has been observed. Up to 3% of the deposited e-beam energy was converted to laser-energy.     

Leading relativistic correction to the interaction coefficients between atoms and molecules using Borel integral II

Lower and upper bounds to the leading relativistic correction to the interaction coefficients between H, He, Ne, Kr, and Xe atoms, and H₂ and N₂ molecules have been evaluated by using Borel integral for the dynamic dipole polarizability. Our results for these bounds are in agreement with others.     

Sticking and displacement channels in the COg + O2/Pt(111) reaction

A molecular beam of CO, impinging on a Ft surface saturated with molecular oxygen, causes displacement of O₂ molecules into the gas phase. The kinetics of the displacement and associated CO sticking have been measured for CO kinetic energies in the range 0.06-1.83 eV. At low kinetic energies the main displacement channel is associated with the sticking of CO, which by dynamic energy and momentum transfer causes O₂ molecules to leave the surface, with a probability of 0.09 per stuck CO molecule. At the highest CO kinetic energies an additional displacement channel is appearing, namely inelastic (non-sticking) scattering of CO molecules, which deposit enough energy to displace adsorbed O₂ into the gas phase.     

High resolution angle-resolved photoelectron spectrum of CO2, excited with polarized resonance radiation

The He(I) excited and angle-resolved photoelectron spectrum of CO₂ is investigated using a focussing VUV-polarizer. High resolution combined with the additional information given by comparing spectra taken at different angles permits detailed analysis of the vibrational structure. β-values are given for all vibrational components hitherto observed in the photoelectron spectrum of the ≈X, ≈A,≈B and ≈C electronic bands. Single excitations of the v₃ mode with vibrational energies 181 meV in the estate and 279 meV in the ≈B-state are reported. The peak at 360 meV vibrational energy in the (≈C-state is reinterpreted as a single v₃ excitation. The β-values of the most intense peaks are also measured using Ne(I) (16.67 and 16.85 eV), Ne(II) (26.86 and 26.95 eV) and He(II) (40.81) resonance radiations.