Generating intense beams of low-energy molecules

A method for obtaining intense pulsed beams of molecules possessing low kinetic energies is proposed. The method is based on the formation of a cold pressure shock (shock wave) in an intense pulsed molecular beam interacting with a solid surface, which serves as a source of the secondary beam of low-energy molecules. The proposed method was successfully used to obtain intense beams of H₂, He, CH₄, and Kr molecules with kinetic energies not exceeding 10 meV, and H₂/Kr and He/Kr beams with kinetic energies of H₂ and He molecules below 1 meV.     

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.     

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.     

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.     

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     

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.     

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.     

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.     

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.     

Organic thin-film transistors of pentacene films fabricated from a supersonic molecular beam source

Top-contact organic thin-film transistors (OTFTs) of pentacene have been fabricated on bare SiO₂ and SiO₂ modified with hexamethyldisilazane (HMDS) and octadecyltrichlorosilane (OTS). The pentacene films were deposited from a supersonic molecular beam source with kinetic energy of incident molecules ranging from 1.5 to 6.7 eV. The field-effect mobility of OTFTs was found to increase systematically with increasing kinetic energy of the molecular beam. The improvements are more important on HMDS- and OTS-treated surfaces than on bare SiO₂. Tapping mode atomic force microscopy images reveal that pentacene thin films deposited at high kinetic energy form with significantly larger grains—independent of surface treatment—than films deposited using low-energy beams.     

Laser-heating diamond anvil cell studies of simple molecular systems at high pressures and temperatures

We report the application of new laser-heating techniques and sample preparation procedures for simple molecular materials (diatomic molecules and water) under high pressure in the diamond anvil cell (DAC). Both continuous and pulsed laser heating was employed. We probed the materials using Raman spectroscopy and also by analyzing the time evolution of the temperature of the metallic coupler that is used to absorb laser radiation and heat the sample. Raman measurements of H₂, D₂, N₂, H₂O and O₂ show a broadening of intramolecular vibrations at high P−T conditions, indicating a decreasing molecular lifetime, and hence suggest an increasing molecular dissociation. In diatomic molecules the intramolecular bonding can be further probed by observations of sidebands corresponding to vibrational transitions from excited states; the energies of these sidebands imply intramolecular potentials that become increasingly less anharmonic as pressure is increased. We also show that the pulsed heating technique combined with instantaneous radiative temperature measurements provides a useful tool for studies of thermochemical properties and phase transformation boundaries.     

On the relative strength of He and H2 diffraction from Ag(111)

Under equivalent incident conditions, H₂ diffraction beams on Ag(111) have recently been observed to be about one order of magnitude stronger than He beams. We show that this effect can be attributed to details of the interaction, in particular, the exponential increase of the corrugation amplitude towards the surface. By extending a previously developed theory for the interaction between He and a metal surface, we show that the H₂Ag(111) repulsion is roughly 1.5 times larger than for He. However, the Van der Waals attraction is about three times stronger for H₂, so that the classical turning points of low-energy H₂ particles lie closer to the surface. Because of the stronger corrugation at short distances, H₂ diffraction intensities can be up to an order of magnitude larger than for He.     

Molekularstrahlmessungen von Stoßquerschnitten für Übergänge zwischen definierten Rotationszuständen zwei-atomiger Moleküle

Inelastic collision cross sections for transitions between specified rotational states designated by (J, M) have been measured in a molecular beam apparatus. With an electrostatic four pole field molecules in a specified rotational state are separated out of a molecular beam and focussed into a gas filled scattering chamber. Molecules which have been scattered by less than 1/2° are then collected in a second four pole field, located directly behind the scattering chamber, and are analyzed for their rotational state. From a comparison of the measured pressure dependence with calculated curves a determination of inelastic collision cross sections for specified quantum jumps is possible. Measured inelastic scattering cross sections for the transitions (2,0→3,0) are reported for the gases He, Ne, Ar, Kr, CH₄, SF₆, H₂, O₂, Air, N₂O, H₂O, CF₂Cl₂. The values range between about 5 and 100 Ų in the order indicated. The scattering gases NH₃ und ND₃ yielded larger cross sections of about 600 Ų and, in addition, the transitions (3,0)→(2,0),(1,0)→(2,0), (2,0)→(1,0) and (3,0)→(1,0) were observed. Total cross sections for the same gases were also measured with the apparatus.     

High resolution study of anion formation in low-energy electron attachment to SF<Subscript>6</Subscript> molecules in a seeded supersonic beam

Using two variants of the Laser Photoelectron Attachment (LPA) method involving a differentially-pumped, seeded supersonic beam (0.05% and 12.5% of SF₆ molecules in helium carrier gas, nozzle temperatures T₀= 300–600 K, stagnation pressures p₀= 1–5 bar) and mass spectrometric ion detection, we have investigated the energy dependence of anion formation in low-energy electron collisions with SF₆ molecules at high energy resolution. Using the standard LPA method, the yield for SF₆^- as well as SF₅^- and F^- anions was studied with an energy width around 1 meV over the electron energy range 0–200 meV. In addition, a variant of the LPA method with extended energy range (denoted as EXLPA) was developed and applied to measure the yield for SF₆^- and SF₅^- formation over the energy range 0–1.5 eV with an energy width of about 20 meV. The cross-section for formation of SF₆^- decreases by five orders of magnitude over the range 1–500 meV and is only weakly dependent on nozzle temperature. The yield for SF₅^- formation shows — apart from a weak zero energy peak which grows strongly with rising temperature — a broad maximum (located around 0.6 eV for T₀= 300 K and shifting to lower energies with rising T₀) and a monotonical decrease towards higher energies. SF₅^- attachment spectra taken at elevated temperatures exhibit changes with rising stagnation pressure which directly reflect rovibrational cooling of the SF₆ molecules with rising pressure. The SF₅^-/SF₆^- intensity ratio at near-zero energy and the low-energy shape of the broad peak in the SF₅^- spectra are used as thermometers for the internal temperature of the SF₆ molecules in the seeded supersonic beam which (at p₀= 1 bar) are found to be 50–100 K lower than the nozzle temperature. The energy dependence of the yield for F^- formation is similar to that for SF₆^-, but the F^- signals are three to four orders of magnitude lower than those for SF₆^-; in view of the rather high endothermicity of F^- formation the origin of the F^- signals is discussed in some detail.     

Vibrational inelastic electron-H<Subscript>2</Subscript> scattering revisited: numerically converged coupled channels space frame calculations with model interactions

The collisional excitation of the lower vibrational levels of H₂(¹Σ_g⁺) molecules by low-energy electron impact is computed using an empirical model potential and by solving the coupled-channels scattering equations within a space-fixed (SF) frame of reference formulation. Numerically converged partial, integral inelastic and elastic cross-sections are obtained from what is an essentially exact treatment of the dynamics and the results are compared with measurements and with earlier calculations on the same system. The usefulness of the SF method for handling excitation processes at near-threshold collision energies is discussed and analyzed through the calculations of collisional superelastic partial cross-sections down to 10^-2 meV of collision energy.     

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.     

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.     

Interaction d'un jet moléculaire avec un gaz tampon : relaxation collisionnelle d'un système à deux niveaux d'énergie

Using a molecular beam, we study the transitions induced by collisions with molecules of a scattering gas. The experimental method uses a H₂CO beam apparatus which allows the observation of rotational transitions . The target gas is NH₃. The application of a static electric field E considerably modifies the collision induced transition probabilities; the transitions become forbidden when Eis intense. An experimental method is deduced to select transitions on a molecular beam. We initially prepare the system to be in the level (i) before entering the scattering chamber. After scattering, the population ratio n _f/n _i is measured as a function of the target gas pressure P _T. We determine the state to state cross-section of H₂CO. When the pressure P _T becomes intense, the effect is non linear. It is shown that this effect results of many collisions. We compare theory with experimental results. This experimental method gives a model for relaxation process studies in two energy level systems. Re?u le 30 juin 1999 et re?u sous forme finale le 14 décembre 1999     

Inelastic atom scattering from layers of atoms and molecules on Cu(110)

The vibrational properties of adsorbed layers have been studied using inelastic He atom scattering. The substrate was Cu(110) viewed along the [001] and [11&#x0304;0] azimuth. The adsorbates included, Kr, Xe, CH₄, CD₄, C₂H₆, CO, CO₂ and O₂ and covered the region of both physisorption and chemisorption. Despite a range of binding energies and mass ratios the vibrational frequencies showed no dependence on the momentum change, i.e. scattering was dispersionless, although intensity changes occurred in the inelastic peaks. There seemed to be no dependence of the adsorbate spectra on coverage below a monolayer. The peaks of CH₄ and C₂H₆ appeared broader than those of Kr and Xe suggesting molecular motions. Further, CH₄ and C₂H₆ gave very similar spectra. Both energy gain and loss events were observed in the inelastic spectrum. For those adsorbates which gave multilayer adsorption (Xe, C₂H₆) changes in the spectra were observed as the second layer developed. In the latter category also, mixed layers (Xe on C₂H₆, Xe on CO and C₂H₆ on Xe) were studied.