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.     

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.     

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.     

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.     

Importance of pre-ionisation for the non-chain discharge-pumped HF laser

The importance of pre-ionisation for the non-chain discharge-pumped HF laser is studied through experiments on an X-ray photo-triggered laser using mixtures of Ne, SF₆, and ethane. The discharge dynamic in Ne/SF₆ mixtures or pure SF₆, as well as the stabilisation effect induced by C₂H₆ and consequences for the laser performance, are investigated for pre-ionisation electron density values, n_eo, ranging from 10⁶ cm^-3 up to 10⁹ cm^-3, as well as for the so-called discharge self-breakdown mode. Without ethane, the minimum n_eo value which is needed to complete 100% homogeneous charge deposition in the plasma is a very sharply increasing function of the SF₆ pressure. This hinders performance optimisation when the molecule used to react with F-atoms, for instance H₂, has no effect on the discharge dynamic. The minimum ethane partial pressure that is needed to stabilise the discharge depends on n_eo, the pumping pulse duration, the deposited electric charge, and the SF₆ pressure. Discharges in Ne/SF₆ can be much more efficiently stabilised by addition of a small amount of ethane than by an increase of n_eo. A pre-ionisation density as low as 10⁶ cm^-3 is sufficient to achieve the maximum laser energy value, but total suppression of the pre-ionisation has a detrimental effect on the active medium homogeneity. Received: 30 May 2000 / Revised version: 9 October 2000 / Published online: 9 February 2001     

High-efficiency,high-energy performance of a pulsed HF laser pumped by phototriggered discharge

A comparison of the performance of pulsed infrared HF lasers pumped by phototriggered discharges using either Ne/SF₆/H₂ or Ne/SF₆/C₂H₆ mixtures are presented. For an active volume of 50 cm³, a specific output energy as high as 11 J/ has been achieved with an efficiency higher than 3% when C₂H₆ is used as H atom fuel. The replacement of ethane by molecular hydrogen reduces the laser performance by 40%. The investigation of the temporal evolution of the laser intensity shows that this dramatic decrease results from a shortening of the laser pulse duration rather than from a decrease of the peak power. Indications are given that this behavior is correlated to a very different temporal evolution of the discharge parameters, especially at low reduced electric field E/N.     

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.     

Laser control of the capture of chromophore molecules by nanoclusters of noble gases in crossed molecular and cluster beams

The infrared-laser-radiation-controlled capture of chromophore molecules (on an example of SF₆) by cold nanoclusters of noble gases (Xe _N , N ≥ 100–1000 is the number of atoms in a cluster) in the crossed molecular and cluster beams has been investigated by a new method based on the selective vibrational excitation of molecules by an intense infrared laser pulse before their capture by clusters, which leads to a significant increase in the probability of their desorption from the surface of clusters as compared to the unexcited molecules. The possibility of using the proposed method for the selective doping of clusters with molecules, laser separation of isotopes, and selective transport of molecules to the surface has been discussed.     

A KrF fast discharge laser in mixtures containing NF3, N2F4 or SF6

A fast discharge KrF laser system (λ = 248.5 nm) has been operated at 25 mJ/pulse, 3.0 MW peak power in high pressure He: Kr: fluoride mixtures containing low concentrations of both krypton and the fluorine donors N₂F₄, NF₃ and SF₆. Lasing action is reported for the first time in N₂F₄ and SF₆ with optimum energy output at 750 and 160 mJ/l respectively.     

Interaction of intense beams of highly vibrationally excited molecules with molecules (clusters) condensed on a cold surface

The interaction of intense beams of SF₆ and CF₃I molecules, excited by powerful IR laser radiation to high vibrational states (0.3 eV ≤ E _vib ≤ 2.0 eV), with molecules (clusters) condensed on a cold surface (T _s ≈ 80–85 K) has been studied. The probability that the excited and unexcited molecules are reflected from the cold metal surface covered by condensed molecules (clusters), as well as the probability that such excited and unexcited molecules are transmitted through a cooled multichannel metal plate and a converging cone oriented at an angle relative to the molecular beam axis, has been determined. Expressions for these probabilities of reflection and transmission as functions of the angle of incidence and the parameters of the exciting laser radiation and the molecular beam are obtained. It is shown that highly vibrationally excited molecules are reflected from the surface and transmitted through the plates and cones with a much higher probability than unexcited molecules. The results suggest that this phenomenon can be used for the separation of molecules in a beam with respect to isotope (or atomic) composition.     

Diode-laser spectroscopy of supersonic free jets

A supersonic-free-jet infrared spectrometer has been constructed for investigation of molecular vibrational spectra at low rotational and vibrational temperatures. The sensitivity of measurement in a pulsed jet is increased by employing a phase-sensitive detection method synchronized with the pulse frequency. The performance of the spectrometer is examined for the absorption lines of the NH₃ v ₂ band. A rotational temperature as low as 16K is attained when seeded in He. Cold-jet spectra are demonstrated for thev ₃ bands of PF₅,³⁴SF₆, and¹⁸²WF₆.     

CO2 laser CVD of a-Si:H: in situ gas analysis and model calculations

4 and disilane Si₂H₆ induced by continuous wave CO₂ laser irradiation has been investigated under the conditions of chemical vapor deposition (CVD) of amorphous hydrogenated silicon a-Si:H. At the very position of depositing the thin film the stationary chemical composition of the processing gas is probed in situ by an effusive molecular beam which passes through a differential pumping stage into a quadrupole mass spectrometer (QMS). With SiH₄ as educt and SF₆ as a sensitizer, SiH₄ and Si₂H₆ are found in the processing gas while Si₃H₈ or higher silanes are lacking. Si₂H₆ and SF₆ lead to SiH₄, Si₂H₆, and Si₃H₈, but higher silanes are missing. The experimentally determined composition of the processing gas is semi-quantitatively reproduced by model calculations based on the assumption of stationary local equilibrium conditions and applying thermodynamic and spectroscopic data (molecular statistics). The mass balance of the processing gas entering and leaving the CVD chamber states an atomic ratio Si:H of 1:2 for the gas phase species forming the solid deposit on the reactor walls. This finding together with theoretical considerations indicates the intermediate Si₂H₄ to be the dominating gas phase species forming the a-Si:H thin films. Received: 17 July 1998/Accepted: 20 July 1998     

Disintegration of Ar N,Kr N,and (N2) N clusters during collisions with highly vibrationally excited SF6 molecules

It is shown that, when highly vibrationally excited SF₆ molecules (with vibrational energy E _vib ≥ 0.5–2 eV) collide with weakly bound van der Waals Ar _N , Kr _N , or (N₂) _N (N ≤ 30–40 atoms in a cluster) clusters in intersecting molecular and cluster beams, the molecules are trapped by the clusters, the clusters then undergo full disintegration, and the trapped molecules become free. The method of studying this process and the results obtained are described. The possibilities of application of this method for selective doping of clusters by molecules, laser separation of isotopes, and selective transportation of molecules to a surface are discussed.     

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.     

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.     

Observation of rotational population transfer effect for an HF chemical laser

When a CO₂ gas absorption cell was placed within the optical cavity of a low pressure pulsed HF laser, the specific vibration- rotation line of the HF laser disappeared, which influenced both the intensity and pulse duration of the neighbouring lines. This behavior strongly depends upon the rotational population transfer in HF. By measuring the time response of this behavior, it was found that the rate constant for the rotational population transfer was in the range of 10⁷ s^-1 torr^-1 for the SF₆/H₂ lasing mixture.     

Is the critical Reynolds number universal?

This paper is devoted to checking whether the critical Reynolds number is universal in identical conditions for the flow of different fluids. The laminar-turbulent transition in a circular pipe flow has been tested experimentally. The flows of inert gases (He, Ne, Ar, Kr, Xe), molecular gases (N₂, CO, CO₂, SF₆), and two similar liquids (H₂O, D₂O) have been tested. A considerable, up to 40%, difference in critical Reynolds numbers was observed. The possible reasons for nonuniversality of the critical Reynolds number are discussed.     

Dynamics and correlated performance of a photo-triggered discharge-pumped HF laser using SF6 with hydrogen or ethane

3 , has been performed in Ne/SF₆/H₂ and Ne/SF₆/C₂H₆ mixtures. Parameters involved have been the storage line capacitance and the circuit inductance, the capacitors charging voltage, the RH-molecule type and partial pressure, and the X-ray dose for the preionization. High laser performance has been achieved with C₂H₆: an output energy up to 3 J corresponding to a specific energy of 9.6 J/l at an efficiency of 4.7%, which strengthens the advantage of the photo-triggering technique to energize high-power HF lasers. However the optimum performance achieved with H₂, 5.75 J/l and 3.5%, are lower. It is shown, through a time-resolved study of the electrical discharge and spatial dynamics correlated to laser power and energy measurements, that discharge instabilities are responsible for the poor laser performance of the mixture with H₂. These instabilities, which lead to arc development, are characteristics of the discharge in Ne/SF₆. It is demonstrated for the first time that addition of a heavy hydrocarbon, such as C₂H₆, to that mixture induces the discharge stabilization so that the laser emission arises in a homogeneous active medium. This effect allows us to achieve better laser performance than with H₂. Received: 17 March 1998/Revised version: 13 July 1998     

Spectral characteristics of IR-multiphoton excitation in supersonic molecular beams

The multiphoton absorption of SF₆ was investigated in supersonic molecular beams in dependence on the fluence and the wavelength of the CO₂ laser. The temperatures of the SF₆ molecules have been reduced using seeded beams of different concentrations. The experimental results are discussed on the basis of the known spectroscopic data of SF₆ and provide some novel information about the spectral characteristics of the ir-multiphoton excitation of strongly cooled molecules in the collision-free case.