FIR Stark spectroscopy on optically pumped CH3OH laser

An extensive theoretical and experimental analysis of the absorption and emission spectrum of a CH₃OH FIR-laser excited by a conventional CO₂ laser is presented. Particular interest is devoted to the Stark shifts of the pump and lasing lines and to the electric field dependence of the Fir-laser output of the various lines. The offsets with respect to the exciting radiation and the Stark shifts of the IR absorption (pump) lines are measured by means of the transferred Lamb dip technique. The theoretical behaviours of the Stark patterns are calculated for several choices of the quantum numbers and selection rules involved in the transitions. A large variety of experimental results are reported and compared to theory. Non-linear Stark shifts have been observed for the 37.5m FIR laser line and for the IR-pump transitions excited by the 9-P(38) and 10-R(38) CO₂ laser Lines. Line assignments are proposed and new FIR laser lines are reported.     

Short wavelength operation of the CH3F Raman FIR laser

Using the isotopic species¹³CH₃F in the methyl-fluoride Raman laser, we have observed kilowatt-level laser pulses which can be tuned over a series of intervals that are centered on pure-rotational transitions in thev ₃ ground state with initial-state J values between 35 and 43, inclusively. Taken together, these tuning intervals cover 35% of the spectrum between 142 and 174 m. Several straightforward improvements in the experimental setup, including the use of isotopically purer¹³CH₃F, should enhance the spectral coverage in this region.     

Wavelengths for new CH3OH laser lines

Using a grating-tuned CO₂-TEA laser to pump CH₃OH in a metallic-wave-guide resonator, submillimeter laser emissions have been produced by pumping with 36 lines in the 9.4m CO₂ band and with 23 lines in the 10.6m band. Several dozen new SMM laser lines were observed. Wavelengths accurate to within 0.1% are given for 12 previously unmeasured lines between 34m and 225m.     

New FIR laser lines and frequency measurements for optically pumped CD3OH

Twenty new cw FIR laser lines in CD₃OH, optically pumped by a CO₂ laser, are reported. The frequencies of 39 of the stronger laser lines were measured relative to stabilized CO₂ lasers with a fractional uncertainty, as determined by the reproducibility of the FIR frequency itself, of 2 parts in 10⁷.Contribution of the U.S. Government, not subject to copyright.     

Far infrared laser lines and assignments of CH3OH: a review

Methyl alcohol is the most important lasing molecule in the Far-Infrared (FIR) spectral region, and the most widely used for investigation and for applications. Since the last critical review of 1984, over seventy papers have been published dealing with the FIR laser lines and the infrared spectroscopy of CH₃OH. In 1984 we could list about 330 FIR laser lines, 98 of which were measured in frequency and 105 assigned. Since then more than 70 papers were published increasing the number of the known laser lines to 575 (103 measured in frequency). Also the FIR and IR spectroscopy was largely improved thanks to the analysis of high resolution FT spectra, and the number of the correctly assigned laser lines has been increased to 224. The wavenumbers of the assigned lines can now be predicted with an accuracy of about 0.001 cm^–1 or better, thus approaching the accuracy of the experimental frequency measurements.     

Far-infrared laser stark spectroscopy of CH3OH and13CH3OH

The high resolution laser Stark spectra of methanol and¹³C-substituted methanol have been studied up to Stark fields of about 60 000V/cm with the HCN and DCN lasers. Numerous families of absorption lines have been observed in both parallel and perpendicular polarizations. For methanol, the transitions J _k =7₅ 6₄ A, _t=0; J _k =11₄ 10₃ E _l , _t=0; and J _k =17₃ 16₂ E₂, _t=0 have been identified while the assignments for¹³C-substituted methanol are J _k =14₈ 15₇ A, _t=0; J _k =15₃ 14₂ A⁺, _t=0; J _k =10₇ 9₆ A, _t=0; and J _k =27₉ 27₈ E₁, _t=0. Zero-field frequencies for the assigned transitions are given with improved accuracy over those calculated from available molecular constants, especially for¹³CH₃OH.     

Experimental study on miniature pulsed CH3OH far-infrared laser

Using a grating tuned TEA-CO₂ laser with 9P(16) line to pump a 10cm or 20cm long miniature Fabry-Perot cavity CH₃OH laser, pulsed far infrared(FIR) lines of 570.6um and 918um wavelengths were observed, the latter is a new line. Operation performance and spectral characteristics of the miniature CH₃OH laser were studied. The project was supported by the Special Research Foundation of Doctorate Station in University of P.R.C.     

Compact, high power FIR NH3 laser pumped in a three mirror CO2 laser cavity

A compact CO₂–NH₃ FIR laser system where an NH₃ laser cavity was inserted in pump, three mirror CO₂ laser cavity was designed. The total length of this system was about 1.8 m. Output energy of about 1 mJ (10 KW pea power) was obtained at the 152 m and 90 m lines in NH₃. Power conversion efficiency of 1.7 percent was obtained at the 90 m line.     

Theoretical study of multi-mode optically pumped NH3 FIR laser

The two or multi-mode optically pumped NH₃ FIR laser had been studied theoretically. The NH₃ molecular gas was assumed to be a three-level system and obeyed the time-dependent behavior of the density matrix equations. Considering the situation of playing the two or multi-mode optical pumping and the FIR laser field were same polarized. The gain coefficient and the output FIR power of the system could be calculated by using the iteration method.It had been predicted that the two or multiple longitudinal mode optically pumped NH₃ FIR laser could have a greater output power or higher lasing efficiency than single mode pumped FIR laser under suitable selected operating parameters of laser.Supported by The Education Foundation of PRC.     

Assignments of optically pumped CD3OH laser lines

Six FIR laser lines from CD₃OH pumped by the 10R(36) and the 10R(18) CO₂ laser lines are assigned to specific rotational energy levels in the excited C–0 stretch state. It is found that their upper laser levels are shifted by a Fermi resonance between the C–0 stretch vibration and the third and forth harmonics of the torsional mode. The Fermi resonance shifts are +0.332 cm^–1 and +2.251 cm^–1 for the upper laser levels pumped by the 10R(36) and the 10R(18) CO₂ laser lines, respectively. Calculated frequencies of the pump and the laser transitions agree with those of the pump CO₂ laser lines and the observed FIR laser lines within estimated accuracy.     

A twin optically-pumped far-infrared CH3OH laser for plasma diagnostics

A twin optically-pumped far-infrared CH₃OH laser has been constructed for use in plasma diagnostics. The antisymmetric doublet due to the Raman-type resonant two-photon transition is reproducibly observed at 118.8 m. With the 118.8-m line, it is obtained from the frequency separation of the anti-symmetric doublet that CH₃OH absorption line center is 16±1 MHz higher than the pump 9.7-m P(36) CO₂ laser line center. It is shown that the Raman-type resonant two-photon transition is useful in order to get several-MHz phase modulation for the far-infrared laser interferometer. Some preliminary performances of this twin laser for the modulated interferometer are described.This work was carried out under the collaborating research program at the Institute of Plasma Physics, Nagoya University, Nagoya 464, Japan.     

The Spectrum of Ground-State Reversed Transition of CH3OH Far-Infrared Laser

Using the CH₃OH molecular energy levels data base management program, we deduced that when a CH₃OH laser pumped by CO₂-9P(16) line, there should be a FIR laser line of 918m wavelength, which corresponding to a transition in ground-state reversed three-level energy system. For the first time, the spectra of ground-state reversed three-level system transitions were calculated by solving the density matrix equations, and the spectrum characteristics of 918m line were studied. Experimentally, the CH₃OH FIR laser line of 918m wavelength was obtained by pumping with a TEA-CO₂ laser. The experimental results were in good agreement with the theoretical calculations.     

Optoacoustic Laser Stark spectroscopy and FIR laser action on CH3Br using a waveguide CO2 laser

The optoacoustic spectrum of CH₃Br around 10 m band lines of a tunable cw waveguide CO₂ laser is investigated. Several new infrared absorptions are observed and most of the correspond ing molecular transitions are assigned. Far infra red laser action is reported by pumping with the same CO₂ laser: pump offsets are given using the Transferred Lambs dip (TLD) technique. A new FIR laser emission is obtained and assigned. An optoacoustic Laser Stark spectroscopy technique is used to investigate off resonance infrared tran sitions.     

Torsional refilling transitions in tea-pumped CH3OH fir lasers with associated high-resolution fir spectra

It is proposed that a number of the high-frequency far-infrared (FIR) laser lines observed when CH₃OH is optically pumped by high-power CO₂ TEA lasers can be identified as refilling torsional transitions within the vibrational ground state. Assignments are presented for 8 such TEA-pump/FIR-laser refilling systems. To provide support for the assigned laser frequencies, high-resolution Fourier transform FIR spectra of CH₃OH have been obtained and partially analyzed in the torsional transition region.     

Frequencies of cw FIR laser lines from optically pumped CH2F2

The frequencies of 48 optically pumped cw FIR CH₂F₂ laser lines have been measured relative to stabilized CO₂ lasers. Uncertainties are estimated to be about 5 parts in 10⁷.     

Acoustooptic extension of the frequency tunability of CW CO2 lasers: New FIR lasers emissions from CH3OH and13CH3OH

We have increased the frequency tunability of our CW waveguide CO₂ lasers by means of an acoustooptic amplitude modulator, operating at the fixed frequency of 90 MHz. The up-shifted, or down-shifted, laser optical sideband can be generated independently by adjusting the orientation of the modulator. The efficiency is larger than 50%. The frequency tunability of the CO₂ laser around each laser line is thus increased by 180 MHz. To demonstrate the possibilities of this method, a source composed of the above modulator and of a CW, 300 MHz tunable waveguide CO₂ laser has been used for the search of new large offset FIR laser lines from optically pumped CH₃OH and¹³CH₃OH molecules. As a result 15 and 10 new large offset laser lines were discovered respectively. New assignments of some laser lines are also proposed. We have also measured the Stark effect, the offset, and the polarization of other already known lines. In particular a Stark effect frequency tuning of about 1 GHz is demonstrated for a laser line at 208.399 m.     

Operating parameter optimization of optically pumped CH3OH far-infrared laser

By solving the density matrix equations of a quantum system, the output power intensity of an optically pumped CH₃OH FIR laser (CH₃OH-OPFIRL) was calculated by means of iteration method, and the spectral characteristics were got. Base on the calculation, optimization of operating parameters including operating gas pressure, pumped power and output coupling coefficient of the CH₃OH cavity laser were systematically studied. Experimental, a series of FIR emissions of the CH₃OH cavity laser pumped by TEA-CO₂ laser with 9P(16) line were measured. The experimental results were in good agreement with theoretical calculations. The project was supported by the Special Research Foundation of Doctorate Station in University of P.R.C.     

Assignments of optically pumped CH3OD laser lines

Fifteen laser lines from CH₃OD pumped by a CO₂ laser are assigned to specific rotational energy transitions. These assignments have been obtained from the approximation that, except for one constant, the molecular constants in the excited CO stretching state are same as those in the ground state.     

Applications of high resolution spectroscopy to the identification of far-infrared laser emission from optically pumped13CH3OH

High-resolution infrared (IR) and far infrared (FIR) Fourier transform absorption spectra have been employed to investigate assignments of FIR laser lines reported from optically-pumped¹³CH₃OH. The spectroscopic measurements are used in conjunction with the reported IR pump and FIR laser frequencies to form closed combination loops for several systems, serving to confirm the assignments and in some cases to improve the accuracy of the FIR laser frequencies. Frequency predictions from combination differences are also presented for a number of potential new FIR laser lines.     

Cavity operation of a pulsed C13H3F laser

Cavity operation of an optically pumped, pulsed, C¹³H₃F far-infrared laser is described. The use of a Fabry-Perot output coupler has resulted in selectable line emission at 1222, 1207, 1006, 388 and 412 m with power levels in the 1–20 kW range. In addition, single mode operation on the longer wavelength lines has been achieved. Experimental evidence is also presented for a collisionally coupled two-photon absorption process which is responsible for the observed short wavelength emission.