Effects of anharmonic splitting upon collisionless multiple-photon laser excitation of SF6

Qualitative agreement of the dependence of molecular excitation upon laser frequency, between non-perturbative quantum-mechanical calculations and experimental measurements of the collisionless multiple-photon excitation of a few vibrational quanta in SF₆ by a CO₂ laser, results when anharmonic splitting of the vibrational energy levels is taken into account.     

Effect of mode-locking on the multiple-photon reaction of SF6

The effect of mode locking on the CO₂ laser-induced reaction of SF₆ is reported. A mode-locked laser pulse enhances the SF₆ reaction yield by a small (8%) but significant amount. The mode-locked pulse also decreases the isotopic selectivity of the reaction. This small effect is greater for enrichment of ³³SF₆ than for ³⁴SF₆. These results suggest that absorption mechanisms that have high power dependence play a minor role in the multiple-photon reaction.     

Molecular dissociation of SF6 by ultra-short CO2 laser pulses

We have measured the absolute dissociation probability of SF₆ gas irradiated by CO₂ laser pulses varying in duration from 0.5 nsec to 100 nsec. We find a threshold for dissociation of ? 1.4 J/cm², independent of pulse duration. For fixed energy density, the dissociation probability increases as the pulse duration decreases, but not nearly to the degree expected from theory. We have also determined the dissociation probability in the ν₂ + ν₆ combination band and find it to be 10³ times less than in the ν₃ band, in contradiction to some conclusions recently reported by Ambartzumian et al. The dissociation mechanism takes place without collisions, and if collisions occur, they tend to be detrimental to the dissociation rate.     

Collisionless dissociation of SF6 using two resonant frequency CO2 laser fields

The collisionless dissociation of SF₆ has been studied using simultaneous irradiation by two frequencies from a CO₂ laser which are both nearly resonant with the SF_6v3 absorption band. It was found that the dissociation was enhanced, and occurred over a wider frequency range, than for single frequency dissociation. No threshold effect was observed for a weak resonant and a much higher energy field pumping slightly off-resonance. For such two frequency irradiation, the peak in the dissociation curve was found to be shifted to lower frequencies with respect to that for single frequency dissociation.     

Infrared multiple-photon dissociation of CDCl3 induced by a TEA CO2 laser

Infrared multiple-photon dissociation (IRMPD) of CDCl₃ was studied using a tunable TEA CO₂ laser. Effects of number of irradiation pulses, wavelength and energy fluence as well as of sample pressure on the reaction yield are reported.     

Selective T/H separation by NH3 laser multiple-photon dissociation of CTCL3

The multiple-photon dissociation (MPD) of CTCL₃ and the selectivity of T/H separation were investigated using a pulsed NH₃ laser, whose radiation contained a few lines depending on operating conditions. When Xe was added to chloroform, the dissociation rate of CTCL₃ increased at chloroform pressures below 2 Torr as a consequence of the removal of multiple-photon absorption bottleneck by collisions with Xe. The dissociation rate of CTCl₃ decreased monotonically with increasing chloroform pressure from 0.2 to 7 Torr. The depletion of CHCl₃ was not observed within experimental errors. The lower limit of the tritium enrichment factor in photo-products produced by one pulse irradiation was 570 at chloroform pressure of 2 Torr.     

Infrared multiple-photon dissociation of ion-molecules in a beam

First experiments on the infrared multiple-photon dissociation with ion molecules in beams have been carried out. A mass selected beam of SF⁺₅ parent ions is crossed with a focused pulsed CO₂ laser beam. Using mass spectroscopy for the detection, fragmentation into SF⁺₄ and SF⁺₃ has been observed. The relative yield and power dependence have been measured. Features of the MPD of ions in beams are discussed.     

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)     

Experimental selection of molecules for isotope separation by multiple-photon dissociation in an intense IR field

Consideration is given to selectivity estimation methods during polyatomic molecules dissociation by multiple photon absorption. Taking the CH₃NO₂ molecule as an example, the possibilities of selectivity estimations made on the electron-excited dissociation products (luminescence) are shown, as well as on the measurements of the energy absorbed in a strong IR field being transformed into heat. Some advantages of the last method of the selectivity estimation are discussed. The experiments on nitrogen-isotopes separation in the mixture of CH₃ ¹⁴NO₂ and CH₃ ¹⁵NO₂ molecules are carried out when exciting thev ₇ vibration with the isotope shift of about 7 cm⁻¹ and thev ₁₃ vibration with no isotope shift in the linear absorption spectrum. The contribution of secondary chemical reactions to the separation process is discussed.     

Optically pumped 15.90 μm SF6 laser

Optically pumped vibrational transition lasing has been achieved for the first time in a nonlinear molecule. Laser radiation at 628.74 ± 0.02 cm^?1 was generated from SF₆ using CO₂ TEA laser excitation. The SF₆ pumping is shown to be via absorption of two photons.     

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.     

Self-focussing of CO2 laser radiation in SF6

Self-focussing of high-power TEA CO₂ laser pulses for a number of 10 m P-band lines is reported in SF₆ molecular gas. Application of this effect to estimating the intensity-dependent refractive index of the gas is demonstrated.     

Influence of SF6 on HF laser plasma parameters

Summary This paper presents the results of calculations of electron drift velocity, mean energy and ionization, and attachment coefficients in SF₆: C₃H₈: He mixtures performed according to the multiterm Boltzmann-equation analysis. The parameters for wide variation of gas mixture composition andE/N values are obtained. The results presented may be useful in studying the HF laser action, analysis of the gas discharge, and research, development and modelling of this type of lasers. The authors of this paper have agreed to not receive the proofs for correction.     

非链式HF激光器SF6气体介质放电特性

采用放电图像拍摄和放电波形测量两种方法研究了放电激励HF激光工作介质SF6气体的放电特性。实验结果表明：SF6气体放电可以分为主放电、剩余电压维持和电弧放电3个阶段。主放电阶段为均匀体放电,电容储能大部分在此阶段沉积于放电等离子体中;剩余电压维持阶段无明显放电;在电弧放电阶段激光器以电弧形式消耗剩余储能。通过对放电波形的分析,获得剩余电压及主放电阶段能量沉积效率随充电电压的变化规律。随着充电电压提高,剩余电压下降,沉积效率逐渐提高。沉积效率最大值对应于主放电与电弧放电相接的时刻。     

Observations on the spectral dependence andT/D isotope selectivity in the CO2 laser multiple-photon dissociation of trifluoromethane

Pulsed CO₂ laser multiple-photon dissociation of CTF₃ (v ₂ mode) bathed in argon and CDF₃, CHF₃ or CCl₄ is examined as a function of laser wavelength (9.2–9.6 m) and fluence. The dependence of the dissociation profile on wavelength is analyzed and comparisons are made to prior work. The single-stepT/D enrichment factor for infrared photolysis of trifluoromethane is measured; potential practical isotope separation is discussed. Pulsed infrared laser photolysis of CTF₃ (v ₅ mode) using a 12 m NH₃ laser is also attempted.     

Strong dependence of ir multiphoton absorption and dissociation yield of SF6 molecule on intensity (duration) of exciting laser pulse

The role of played by the intensity of the exciting TEA CO₂ laser pulses in the processes of ir multiphoton absorption (MPA) of SF₆ molecules cooled toT _R?40 K andT _v?160 K in a pulsed supersonic jet and the dissociation of SF₆ in a bulk atT?300 K under essentially collisionless conditions have been investigated. A strong dependence of MPA and the dissociation yield on pulse intensity were observed. The frequency dependences of the intensity effects were studied.     

Improved separation of the rare sulfur isotopes by infrared multiphoton dissociation of SF6

The dissociation probabilities of³²SF₆ and some of³⁴SF₆ have been measured at a large number of CO₂ laser lines both at room temperature and at 140 K. The longwavelength wing of this dissociation spectrum is exponential in the wavenumber. Its logarithmic slope is proportional to the inverse temperature. Selectivities are high enough at 140 K, that the photons are consumed only for the rare isotope in the case of³⁴SF₆ and nearly so for³⁶SF₆. For³³SF₆ further improvement of the selectivity would be desirable.     

Spectral characteristics of multiphoton IR dissociation of SF6 in a nonequilibrium pressure shock

The spectral characteristics and the selectivity of multiphoton IR dissociation of SF₆ are studied upon excitation of the molecules in a nonequilibrium pressure shock formed upon the interaction of a pulsed gas-dynamically cooled molecular flow with a solid surface, as well as in the flow incident on the surface and in an unperturbed flow. The results obtained are compared with each other and with the data available on the dissociation of SF₆ on a molecular beam. The measurements of spectral characteristics and the dissociation selectivity upon excitation of SF 6 in the pressure shock and in an unperturbed flow correlate well with each other. The influence of the rotational and vibrational temperatures of the molecules on the spectral characteristics of the dissociation yield is selectivity analyzed.