Compact, high-power FIR NH3laser pumped in a CO2laser cavity

A compact CO2-NH3FIR laser system, with an NH3laser cavity inserted in the pump CO2laser cavity, was designed. Temporally smooth and reproducible single mode NH3laser pulses with an energy of 5 mJ (20 kW peak power) were obtained at the 152 μm line when optically pumped by the injection-locked single-mode CO2laser with a pulse energy of 0.3 J.     

A time-resolved study of rotational and vibrational excitation and relaxation in the13CH3F optically pumped far-infrared laser

The rotational and vibrational energy transfer processes of the¹³CH3F optically pumped far-infrared (OPFIR) laser have been studied in a time-resolved experiment. The experiment uses a tunable millimeter and submillimeter spectroscopic technique as a diagnostic probe. Included are observations of the fastDelta Jprocesses that closely connect otherJstates withinK = 3to the directly pumpedJ = 5level, a vibrational swapping mechanism that transfers excitation fromK = 3to otherKstates, vibrational relaxation due to both wall collisions and molecule-molecule collisions, the nonunity probability of vibrational deactivation in a wall collision, and pump saturation and hole burning effects due to the CO2pump laser. All of these observations are accounted for in the context of a numerical simulation. This results in a complete map of all of the collision-induced rotation-vibration transitions of importance to this basic OPFIR system including quantitative cross sections for the relevant processes.     

Far-infrared raman laser with high intensity laser pumping

Theoretical and experimental results are presented for a pulsed far-infrared (FIR) molecular gas laser with high intensity laser pumping. In these FIR lasers, high intensity pumping is found to produce stimulated Raman emission at very large offsets (up to 30 GHz) from resonance with the intermediate state. A theoretical, density matrix model is developed for these lasers to account for simultaneous Raman emission on rotational levels in the ground and excited vibrational states (double Raman resonance). This theoretical approach is necessary in the case of off-resonant, high intensity pumping. Theory predicts the FIR emission frequency, the FIR laser gain, and the pump threshold intensity as a function of pump laser frequency. Experimental results are obtained onP-,Q-, andR-branch transitions in¹²CH3F and¹³CH3F using a single-mode, grating tuned CO2TEA pump laser with an intensity of up to 40 MW/cm². Good agreement is obtained between theory and experiment for the observed values of FIR emission frequency and pump threshold intensity. These results indicate that a widely tunable (150-1200 mum), pulsed FIR CH3F laser could be constructed with a tunable, multiatmospheric CO2pump laser of modest power (about 2-5 MW).     

Sub-T2optical pulse generation: Application to optically pumped far-infrared lasers

Several polar molecules possessing strong far-infrared (FIR) transitions have been optically pumped by a mode-locked CO2TEA laser in a single-pass configuration. All the resulting FIR pulses are shorter than the sub-T2pump pulses; subnanosecond FIR pulses are observed. These short FIR pulses exhibit lethargic gain, stimulated Raman emission, and multiple-pulse superradiance. The experimental results are modeled by numerical solution of the Maxwell-density matrix equations for two fields interacting with a three-level system. Level degeneracy is included, and the pump is described by a multimode power spectrum with a parabolic envelope, resulting in a periodic train of pulses. Variation of the detuning of the pump from resonance allows simulation of the superradiant or Raman cases. This fully coherent model, which is the major contribution of this paper, explains key experimental observations such as the noncoincidence of the Raman peak with the pump modulation minimum and the enhancement of multiple-pulse superradiance due to remanent polarization.     

Continuously tunable optically pumped high-pressure DF → CO2transfer laser

The operational characteristics of a continuously tunable DF → CO2transfer laser optically pumped with radiation from a pulsed DF laser are experimentally and theoretically studied. The pump radiation is absorbed by DF in a high-pressure DF/CO2/He gas mixture, and subsequent V-V energy transfer to the CO2ν3mode provides the CO2laser population inversion. Continuous tuning of the CO2laser frequency between five CO2line centers from 29.14 to 29.30 THz has been demonstrated, using a 12 atm gas mixture. The maximum pulse energy was about 0.8 mJ. In experiments with a two-mirror CO2laser resonator, pulse energies up to 6 mJ and 35 percent slope quantum efficiency have been obtained at 10 atm gas pressure. The gas mixture typically contained 0.5 percent DF, 5 percent CO2, and 94.5 percent He, but this was not critical. Computer simulations based on a rate equation model of the laser have given results which are in reasonable agreement with those obtained experimentally.     

Assignments of the high power optically pumped CW laser lines of CH3OH

Thirteen far IR laser lines in CH3OH, optically pumped by a CO2laser, have been assigned toa- andb-type transitions in ν5CO-stretch band. Identification procedures used were: a frequency match between the CO2pump and CH3OH absorption, frequency match of laser lines and CH3OH ν5transitions, polarization of far IR radiation, cascade and competition effects between far IR laser lines, and frequency consistencies. An improved set of molecular constants for ν5transitions were also obtained.     

Amplitude stability improvement of CW submiltimeter wave lasers with phase modulated optical pumping

An experimentally measured reduction of 4:1 in the amplitude fluctuation of an optically pumped CW-submillimeter wave laser was achieved using a mirror, vibrating at audio frequencies, to decouple the pump beam reflected back to a CO2pump laser. An expression is derived for the peak frequency deviation of the pump laser due to a phase modulated feedback signal.     

Small-signal gain and time-resolved spectroscopy of the D2-F2/CO2pulsed chemical transfer laser system

Measurements made of the small-signal gain and time-resolved spectral output of a flash-initiated D2-F2/CO2chemical transfer laser system are reported. Small-signal gain measurements indicate a possible lack of rotational equilibration among the rotational levels of the CO2during the DF-CO2V-V energy transfer process. Time-resolved spectral output of this system, operated as a laser oscillator, is presented as verification of the small-signal gain results.     

High-power operation and scaling behavior of CW optically pumped FIR waveguide lasers

High-power far infrared (FIR) laser operation at the 10- 100 mW level is described for wavelengths throughout the 40 μm-1.22 mm spectral region. These data correspond to order of magnitude improvements in converting CO2laser energy into FIR laser output. This improved FIR laser performance is attributed to a waveguide laser geometry with reduced losses for the CO2pump and also to a new method of output coupling. The basic design concept of the efficient laser resonator is discussed as well as the prospect for further increases in laser performance through improved efficiency and sealing.     

Continuous-wave CH3F waveguide laser at 496 µm: Theory and experiment

The kinetic processes controlling the conversion of CO2pump radiation into far-infrared (FIR) radiation in optically pumped waveguide lasers are discussed. It is found that pump saturation and excited-state FIR absorption play major roles in limiting the conversion. Good agreement between theory and experiment was obtained over a wide range of pump powers, gas pressures, and mirror reflectivities. For a well-optimized system, power-conversion efficiencies of 0.2-0.6 percent can be realistically achieved for CH3F.     

Assigment of the CH2F2laser lines associated with the 9R(34) CO2pumping transition

Two new submillimeter laser transitions are reported for CH2F2optically pumped by the 9R(34) CO2line. The new transitions allow us to assign molecular transitions to the complete group of laser lines observed with that pump transition.     

Vibrational energy transfer in CO2under laser conditions with and without water vapor

It is shown that in the case of a dry 1.5-torr CO2gas fill the upper laser level is indirectly excited by vibrationally excited CO produced during the discharge, whereas in the case of a 1.5-torr CO2and 0.2-torr H2O mixture the upper laser level is directly excited by the electrons in the discharge. The collision relaxation times measured under laser conditions for the symmetric valence vibration of CO2in a CO2-H2O mixture and in a CO2-CO mixture as produced during a discharge of an initially pure CO2fill were 19 and 73 μs, respectively. If the reasonable assumption was taken that half of the CO2was dissociated into CO then this result shows that H2O was 14 times more effective in depopulating the lower laser level than CO. The growth in laser intensity for the dry fill was shown to be due to the CO (nu = 1) transfer of energy to the asymmetric vibration of CO2(00°1) with a characteristic increase that was exponential strictly only for a time short compared with the relaxation time of the symmetric vibration. The characteristic transfer time for excitation of the asymmetric vibration was dependent upon the fraction of CO present. If we make the assumption of 50 percent dissociation, the intermolecular energy transfer time between CO and CO2was found to be 40 torr-μs. Results obtained with N2and He added to the laser mixture indicated that He was not more effective in relaxing the lower laser level than N2or CO and was less effective than H2O.     

Emission frequencies of the CF4laser

104 (nu_{2} + nu_{4}) leftarrow nu_{2}hot-band transitions, some of which correspond to known(nu_{2} + nu_{4}) leftarrow nu_{2}CF4laser lines, have been identified and measured in high-resolution Doppler-limited spectra of¹²CF4near 16 μm, obtained with a tunable diode laser. From an analysis of these frequencies, the rotational and tensor splitting constants for the ν2vibrational level have been determined. These constants, together with thenu_{2} + nu_{4}pump-band spectrum previously obtained, allow the laser emission frequencies for any given CO2pump line to be calculated with an accuracy of 0.01-0.003 cm^-1.     

Initiation of NF3-H2chemical reactions via CO2laser irradiation of NF4BF4

NF4BF4has been irradiated with a low-power CO2laser to produce reactive species which then initiate reactions in an ambient NF3-H2mixture. The laser-induced decomposition of NF4BF4in vacuum was measured as a function of laser power and energy. The laser-induced decomposition threshold was determined to be 40 mJ, which corresponds to a laser fluence of 20 J/cm². This same value was determined for the initiation threshold of NF3-H2reactions via CO2laser irradiation of NF4BF4. Visible and infrared emissions were observed from initiated NF3-H2mixtures. This radiative technique has attractive features for initiating reactions in solid-gas systems.     

New SMMW laser transitions optically pumped by a tunable CO2waveguide laser

Optical pumping of a submillimeter wave (SMMW) laser with a relatively compact RF-excited CW CO2laser is described. The increased frequency tunability of the waveguide pump laser has resulted in new low threshold SMMW emissions in C2H2F2, CDF3, and CD2F2by pumping into absorption lines which are beyond the tuning range of a conventional CO2laser. Frequency offsets and some assignments obtained with the aid of a tunable diode laser heterodyne spectrometer are reported.     

Some new FIR laser lines of optically pumped12CH316OH,12CH316OD, and12CH3I,12CH3Br,12CD2Cl2absorption spectroscopy of water and acetonitrile

The wavelength, polarization, and output power of several lines of the optically pumped CW FIR¹²CH3¹⁶OH (methanol) and¹²CH3¹⁶OD (1-D deuterated methanol), methyl iodide, methyl bromide, and deuterated methylene chloride lasers have been determined. In addition to lines already reported in the literature, seven strong lines have been observed. Optimum performance of the laser system is achieved by means of an improved coupling of the CO2pump power into the resonator and extraction of the FIR power from the resonator. Measurements on the power absorption coefficient of water using the laser indicate thatalpha(bar{nu})rises to almost 1100 Np ċ cm^-1at 170 cm^-1, and then shows a gradual fall with an increase in frequency. A strong temperature dependence of the 200 cm^-1peak inalpha(bar{nu})is predicted, with a decrease in the frequency of maximum power absorption coefficient with an increase in temperature. The range of measurements for acetonitrile is extended to lower frequencies so as to overlap with those determined from other millimeter wave techniques. For highly power-absorbing liquids,alpha(bar{nu})is estimated to be within ± 5 percent.     

4B2--Pulsed and steady-state infrared emission studies of CO2laser systems

Transient and steady-state infrared emission at 2.5 to 15 μ from low-lying vibrational-rotational levels of CO2has been studied using a dc discharge. The time-dependent behaviors of several levels important for laser excitation and relaxation were examined following a pulsed discharge. The decays were, in general, different and were not simple exponentials. Relaxation of vibrational energy of CO2appears to occur by collisions involving vibration-vibration exchange between different vibrational modes and vibration-translation relaxation of the bending mode. The rate of transfer of vibrational excitation from N2to various vibrational modes of CO2was investigated as a function of CO2pressure. The addition of He reduced the emission from the lower laser levels with respect to that from the upper laser level and increased the nonradiative decay rate of the lower vibrational levels by CO2-He collisions. Under pulsed excitation, in addition to CO2laser action nearly coincident with the pulse, a weaker, delayed output was observed.     

Direct optical pumping of high-pressure CO2and N2O lasers with a pulsed HF pump laser

Pulsed HF laser radiation has been used for direct optical excitation of CO2and N2O lasers at 10 and 5 atm gas pressures, respectively, which are the pressures required for continuous laser frequency tuning between the line centers in these gases. The maximum demonstrated quantum efficiency is about 14 percent, which seems to be limited by the formation of pressure waves in the gas, in addition to losses in the resonator optics. We find that quantum efficiencies close to unity are theoretically feasible with a low-loss resonator, and by using a sufficiently short pump pulse to avoid a serious influence from pressure waves. The excitation scheme can be used with any of the CO2and N2O laser isotopes.     

Relaxation of CO2laser levels by collisions with foreign gases

Relaxation time of the 00⁰1 upper and 10⁰0 lower CO2laser levels as a function of H2O, CO, and Xe gas pressure has been measured using the afterglow pulse-gain technique. Lifetime data for these gas mixtures and also for mixtures of CO2, CO2-H2, CO2-He, and CO2-N2, obtained previously, are analyzed and compared with available ultrasonic and fluorescence data. Results indicate that the 10⁰0 and 01¹0 levels of CO2are strongly coupled and depletion of the lower laser level population is essentially limited by the relaxation rate of the 01¹0 level. Other processes involving energy exchange between CO2and foreign gases are detailed.     

Gain and fluorescence characteristics of flowing CO2laser systems

Single-pass gain has been measured for flowing CO2, CO2-N2, CO2-He, CO2-N2-He, and CO2-N2-H2mixes. The gain for CO2-N2mixes varies as d^-0.9, wheredis the tube diameter. The diameter dependence of the gain is less pronounced for CO2- N2-He mixes; a peak gain of 4.7 dB/m was obtained in a 1/2 in diam tube. Fluorescence data indicate that the upper laser level population is saturated at 100 mA in all cases. The addition of He, H2, or O2depopulates the lower laser level; helium further increases the population of the upper laser level. The addition of CO increases the population of the upper laser level, probably by resonant transfer from the excited vibrational states of CO.