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.     

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.     

Detection of SF<Subscript>6</Subscript> molecules sublimating from the surface of (CO<Subscript>2</Subscript>)<Subscript><Emphasis Type="Italic">N</Emphasis></Subscript> nanoparticles in a cluster beam by the infrared multiphoton excitation method

It has been found that SF₆ molecules captured by large van der Waals clusters (CO₂) _N (where N ≥ 10² is the number of monomers in a cluster) in intersecting molecular and cluster beams sublimate from the surface of clusters after a certain time and carry information on the velocity and temperature (internal energy) of clusters. Experiments have been carried out for detecting these molecules by means of a pyroelectric detector and the infrared multiphoton excitation method. The multiphoton absorption spectra of molecules sublimating from the surface of clusters have been obtained. The temperature of the (CO₂) _N nanoparticles in the cluster beam has been estimated using these spectra and comparing them with the infrared multiphoton absorption spectra of SF₆ in the initial molecular beam.     

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 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.     

Influence of collisions and pulse intensity on multiple photon absorption in SF6

Using a pyroelectric detector, the multiple photon absorption (MPA) of the SF₆ molecule in a wide range of pressures (10^-3 -1 torr) has been studied. The significant role of collisions in MPA has been shown. The fraction of molecules excited under essentially collisionless conditions has been defined. It is shown that under collisionless excitation of SF₆ (p < 10^-2 torr) at energy fluences E < 10^-1 J/cm² the intensity of the laser pulse plays the essential role, while in presence of collisions MPA is determined mainly by the energy fluence in the pulse.     

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.     

Vibrational predissociation of SF6 dimers and trimers

IR photo-dissociation spectra of SF₆ clusters have been studied. A He-seeded molecular beam has been attenuated by crossing it with a line tunable cw CO₂ laser of moderate power. — In the electron bombardment beam ionizer (E _el=100eV) small neutral clusters are found to fragment predominantly to the main monomer mass (SF ₅ ⁺ ). — Predissociation spectra have been calculated for clusters containing up to six SF₆-molecules invoking the dipole-dipole resonance force to lift the degeneracy of the molecule — excited molecule interaction. On the basis of these spectra, dimer and trimer concentrations have been determined quantitatively, for different molecular beam conditions.     

Multiphoton excitation of molecules by single mode CW lasers

An intracavity laser interaction zone with molecules expanded in a molecular beam set-up permits multiphoton excitation under collision-free conditions by narrow band radiation. Two- and three-laser experiments are performed to study rapid adiabatic passage processes, stimulated de-excitation and hole burning effects. The detection of excitation occurs by means of a sensitive bolometric molecular beam detector. The essential information obtained for SF₆ concerns the vibrational bottleneck, the conservation of excited eigenstate characteristics for at least 1 ms, the ease with which about 15 photons can be deposited in the molecules with the help of two cw CO₂ lasers and the influence of simultaneous two-frequency radiation, yielding a significant extra-excitation. Other molecules where multiphoton excitation is observed utilizing the same set-up are CF₃I and CF₃Br.     

Raman spectroscopy of infrared multiple-photon excited molecules

The method of spectroscopy of spontaneous Raman scattering (RS) with time resolution has been applied for the first time to diagnose the process of multiphoton ir molecular excitation (MPE). Some aspects of RS diagnostics of MPE processes are being analyzed. It has been shown experimentally on SF₆ and CF₃I molecules that it is possible to study such important characteristics of excitation process as the fraction of molecules involved in the process of excitation, vibrational energy distribution of molecules, stochastization of inner molecular energy.     

Universal probe method for measuring the temperature of large clusters (nanoparticles) in a cluster beam

A universal probe method for measuring the temperature of large clusters (nanoparticles) in a cluster beam has been proposed and experimentally implemented. The temperature of large van der Waals clusters (nanoparticles) (CO₂) _N (where N ⩾ 10² is the number of monomers in a cluster) in the cluster beam is measured using this method with SF₆ molecules as miniature probe thermometers. The SF₆ molecules are captured by the (CO₂) _N clusters in intersecting cluster and molecular beams and sublimate from the surface of the clusters, carrying information on the velocity and temperature (internal energy) of the clusters. The velocity (kinetic energy) of SF₆ molecules sublimating from the surface of the clusters has been measured by the time-of-flight method and the temperature of the clusters has been determined as T _cl = (105 ± 15) K.     

Direct measurement of multiphoton molecular absorption of IR laser radiation by pyroelectric detector

The applicability of a pyroelectric detector (PED) to multiphoton absorption measurements (MPA) under ir laser excitation of molecules was examined. The possibility of MPA measurement of SF₆ molecules in the pressure range of 10⁻³÷10⁻¹ Torr with a time resolution of ∼ 7 μs has been shown. It has been demonstrated that the degree of vibrational relaxation of highly vibrationally excited molecules at PED surface does not depend on excitation level under the studied conditions.     

The characteristics of multiple-photon absorption of SF6 molecules cooled in free jet expansion from a pulsed supersonic nozzle

The multiple-photon absorption of pulsed TEA CO₂ laser radiation by SF₆ molecules cooled toT _R40K andT _v160K in the free jet expansion from a pulsed supersonic nozzle has been investigated at energy fluences of 0.1 to 3.0 J·cm^–2.For practically all laser lines which coincide with the linear absorption spectrum of thev ₃ vibrational mode of SF₆ [P(12)...P(28), 10,6 m], the dependence of the absorbed energyE _ab on the exciting energy fluence was found to be steeper than linearE _abⁿ, wheren=(1.1 to 1.8). Considerable increases of the absorption cross sections with increasing energy fluence were observed.The fraction of the molecules interacting with the laser radiation is estimated.     

Measurement of collisional multiphoton energy deposition by a new optothermal detector

The infrared multiphoton absorption of SF₆ under collisional condition has been measured by a new optothermal detector which is based on measuring the change of resistance of a platinum filament. The optothermal signal, i.e., the absorbance of CO₂ laser energy by SF₆, was enhanced by the addition of Ar or NH₃. But the increase of optothermal signal caused by adding NH₃ is much greater than that caused by adding Ar, mainly due to the energy siphoning from excited SF₆ molecules to NH₃ molecules.     

Selective multiphoton IR dissociation of SF6 molecules under nonequilibrium conditions of a pulsed gasodynamically cooled molecular flow interacting with a solid surface

The process of the isotope-selective multiphoton IR dissociation of SF₆ molecules under the non-equilibrium conditions of a pulsed gasodynamically cooled molecular flow interacting with a solid surface was experimentally studied. The SF₆ molecules dissociate as a result of excitation in a shock wave generated in the flow, in the flow incident onto the sold surface, and in an unperturbed flow (in the absence of the solid). The experiment was based on detecting the luminescence from HF^* molecules (λ ≈ 2.5) μm) accompanying the SF₆ dissociation in the presence of H₂ or CH₄, the emission intensity being a measure of the SF₆ dissociation yield. The molecular beam parameters were studied. The time-of-flight spectra of SF₆ in the flow interacting with the surface were measured under various experimental conditions. The spectral and energy characteristics of the SF₆ dissociation process were determined in the flow interacting with the solid surface and in the unperturbed flow. The dissociation product (SF₄) yield was measured and the coefficient of its enrichment with the ³⁴S isotope was determined. It is demonstrated that, using the shock wave formation, it is possible to increase the efficiency of the isotope-selective dissociation of SF₆ molecules. An explanation of the observed results is proposed. The gas density and temperature in the incident flow and in the shock wave were estimated. The results are analyzed and compared to the other published data on the SF₆ dissociation in a molecular beam.     

Spectral and energetic characteristics of passing vibrationally excited SF6 molecules through a cooled multichannel plate

We study the spectral and energetic characteristics of SF₆ molecules excited in a pulsed molecular beam by intense IR laser radiation into high-lying vibrational states (with the energy E _v ≥ 0.3–2.0 eV) that pass through a multichannel metal plate that is cooled to T _s ? 80–85 K and is inclined to the beam axis. From comparison of the measured characteristics with the spectral and energetic characteristics of the IR multiphoton absorption of these molecules, we find that they correlate rather well with each other. The results obtained allow us to conclude that, due to different probabilities of passing vibrationally excited and unexcited molecules through the multichannel plate, it is possible to separate molecules in the beam with respect to their isotopic (component) composition.     

The influence of vibrational excitation on the burning voltage of a pulsed electric discharge in HF laser working media

The burning voltages of an intermediate pressure self-sustained volume discharge (SSVD) in SF₆ and SF₆-C₂H₆ mixtures irradiated by a 10.6 μm pulse TEA CO₂ laser, have been measured on varying the laser fluences over a wide range. The delay between the voltage application and the laser pulse onset is 4 μs, and the laser pulse lasts ∼3 μs. The considerable rise observed in the discharge voltages with increasing absorbed specific laser radiation energy, is due to electron attachment to vibrationally excited molecules of SF₆. Different processes of relaxation of the vibrational energy stored in SF₆ molecules are analyzed and the relevant characteristic times are numerically assessed. The gas heating process owing to vibration-translation energy exchange is qualitatively described in terms of the “thermal explosion”. The relation between the “explosion” and delay times determines the peculiarities of electron attachment to vibrationally excited SF₆ molecules. The burning voltages of a submicrosecond non-irradiated SSVD in the above-mentioned media versus the specific electric energy deposited are also measured. They are compared to those of a laser-illuminated SSVD at commensurable specific laser energy depositions. It is concluded that electron attachment to the discharge-produced vibrationally excited SF₆ molecules is not capable of noticeably affecting the discharge voltages of a submicrosecond non-irradiated SSVD. PACS 42.55 Ks; 52.80     

Efficiency of an electron-beam-pumped chemical laser with an SF6-H2 working mixture

Results are presented from a study of HF lasers pumped by non-chain chemical reactions initiated by a radially convergent and by a planar electron beam. The main channels of formation of vibrationally excited HF molecules are analyzed. The distribution of the energy density of the radiation in the output beam of a wide-aperture laser is measured. In 30 liters of a mixture of SF₆:H₂=8:1 at a pressure of 1.1 atm an output energy of ∼200 J is obtained at an ∼11% efficiency with respect to the energy deposition. It is shown that the admixture of a buffer gas of neon or argon improves the uniformity of the radiation energy distribution in the output beam of an HF laser pumped by a non-chain chemical reaction and initiated by an electron beam, and it also increases the output energy. Zh. Tekh. Fiz. 69, 76–81 (January 1999)     

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.     

Characteristics and efficiency of a compact HF laser initiated by an electron beam

A compact hydrogen fluoride laser is described and its efficiency is evaluated. The HF laser is initiated by injecting a 150 kV electron beam into a mixture of SF₆ and H₂ transversely to the laser cell axis. The optimum laser energy characteristics are determined as a function of the beam energy and gas pressure.