FIR Laser Lines from CH3OD: A Review

The methanol isotopic species CH₃OD has also proved to be an efficient and powerful medium to generate radiation in the far infrared (FIR) region. After the critical review of 1994, six papers have been published dealing with new FIR laser lines from this molecule. As a consequence of the use of wide tunability waveguide CO₂ lasers as well as a new pulsed CO₂ laser operating at hot and sequential bands, as of optical pumping sources, the total number of the FIR laser lines increased from 122 in 1994 to 227 today. In this communication we present an updated and complete catalogue of FIR laser lines generated from CH₃OD. Information on wavelength, offset, relative polarization, intensity, and optimum operation pressure is generally available.     

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.     

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.     

Optically pumped cw CH2DOH fir laser: New lines and frequency measurements

We have measured the output powers and relative polarizations of 66 cw FIR laser lines from CH₂DOH (including 50 not previously reported), which were optically pumped by a CO₂ laser. The frequencies of 43 of these lines were measured relative to stabilized CO₂ lasers.     

Submillimeter laser action of CW optically pumped CF2Cl2 (Fluorocarbon 12)

Eleven new CW far infrared (FIR) laser lines have been observed in the 600 m–1200 m range from the CF₂Cl₂ (Fluorocarbon 12) molecule optically pumped by a CO₂ laser. A 510^–4–10^–3 accuracy is achieved in the measurement of the FIR wavelengths.The frequency offset between the CO₂ pump center and the absorption line centers are measured using the transferred Lamb dip technique. Owing to a recent spectroscopic study of the CF₂ ³⁵Cl₂ molecule three lines may be assigned with great confidence as rotational transitions in thev ₆ vibrational band 923 cm^–1 of this main isotope.     

Far infrared cw raman lasing in NH3

We report evidence that two FIR laser lines generated by cw optical pumping of ¹⁴NH₃ with CO₂ laser lines are due to stimulated Raman emission instead of the usual resonant absorption-emission process.     

Detailed vibrational population distributions in a CO2 laser discharge as measured with a tunable diode laser

A tunable diode laser (TDL) operating in the 2150–2350 cm^–1 wavenumber region is used to probe a conventional cw CO₂ laser discharge. Absorption lines in more than 25 different vibrational bands are observed, enabling us to determine absolute vibrational populations inall levels of concern to the dynamics of the 10 m CO₂ laser. Levels in thev ₃ mode of CO₂ as high as 00°9 are monitored, and it is found that anharmonic effects play a significant role in the populations of such levels. Thev ₁ andv ₂ mode populations are also investigated in detail, and it is found that these modes are strongly coupled and maintain a common vibrational temperature under all discharge conditions. The use of a TDL is shown to be a powerful technique for investigating the dynamics of infrared molecular lasers.This work was supported in part by the National Science and Engineering Research Council, Canada     

High resolution infrared spectrum of the CD2 wagging band of methanol-D2 (CHD2OH) for the lowest lying torsional vibrational state (e0)

This paper reports the analysis of the high resolution (0.0019 cm⁻¹) Fourier transform infrared (FTIR) spectrum for asymmetrically deuterated methanol CHD₂OH (methanol-D₂) at a low temperature for the CD₂ wagging band for the lowest lying trans-species (e₀). In spite of the complexity and perturbation in the spectra, assignments were possible for the CD₂ wagging band for a maximum K value of 10. In total, about 500 spectral lines have been assigned. Analysis of the spectral lines has been performed in terms of state dependent molecular parameters, Q-branch origins and asymmetry splitting. Assignments have been thoroughly confirmed using combination relations (see text). The catalogue of the assigned transition wavenumbers will help identification and prediction of far infrared (FIR) optically pumped CO₂ lasers. The absorption lines close to the several 10R and 10P CO₂ laser lines have also been identified. These should help experimentalists to optimize the power of the emission FIR laser lines and to predict new lines and should prove valuable as a laboratory support for interstellar detection in “Radio Astronomy”. To our knowledge this is the first time such vibrational infrared (IR) high resolution study in CHD₂OH is being performed.     

Determination of absorption length of CO2 and high power diode laser radiation for ordinary Portland cement and its influence on the depth of melting

The laser beam absorption lengths of CO₂ and a high power diode laser (HPDL) radiation for concrete have been determined. By employing Beer–Lambert’s law the absorption lengths for concrete of CO₂ and a HPDL radiation were 470±22 μm and 177±15 μm, respectively. Indeed, this was borne out somewhat from a cross-sectional analysis of the melt region produced by both lasers which showed melting occurred to a greater depth when the CO₂ laser was used.     

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.     

Methanol laser lines from torsionally excited co stretch states, and from OH-bend, CH3-rock, and CH3-deformation states

Using a quasi-CW CO₂ oscillator-amplifier combination with peak power 300 Watt, we have generated FIR laser emission in weak absorption bands of CH₃OH. 40 new lines are reported, and their wavelengths are measured with a relative accuracy of 5×10^–5. A total of 72 lines are assigned. 34 of these involve torsional n=1, 2, and 3 states of the CO stretch and the vibrational ground state. The remaining lines are associated with the CH₃-rock, OH-bend, and CH₃-deformation modes. The latter are located 1460 cm^–1 above the ground state, and are pumped by simultaneous vibrational excitation and torsional deexcitation.     

Mid-infrared trace gas detection using continuous-wave difference frequency generation in periodically poled RbTiOAsO4

A tunable mid-infrared continuous-wave (cw) spectroscopic source in the 3.4–4.5 μm region is reported, based on difference frequency generation (DFG) in a quasi-phase-matched periodically poled RbTiOAsO₄ (PPRTA) crystal, DFG power levels of 10 μW were generated at approximately 4 μm in a 20-mm long PPRTA crystal by mixing two cw single-frequency Ti:Al₂O₃ lasers operating near 713 nm and 871 nm, respectively, using a laser pump power of 300 mW. A quasi-phase-matched infrared wavelength-tuning bandwidth (FWHM) of ∼12 cm^-1 and a temperature tuning rate of 1.02 cm^-1/°C were achieved. Experimental details regarding the feasibility of trace gas detection based on absorption spectroscopy of CO₂ in ambient air using this DFG radiation source are also described. Received: 23 October 2000 / Revised version: 22 January 2001 / Published online: 27 April 2001     

Heterodyne performance of a quasioptical Schottky diode detector: Theoretical and experimental results

A detailed theoretical and experimental study of the heterodyne performance of a quasioptical Schottky diode detector is presented. The experimental results have been obtained by mixing the radiation from a FIR laser with the output of a 67–73 GHz Klystron. The heterodyne signal variation versus various parameters and its relation to the special case of two lasers mixing are described. The mixer characteristics are a NEP value of 2×10^–19W/Hz and a detector bandwidth of at least 9 GHz. Experimental evidence of harmonics generation of submillimetric frequencies at the diode junction is also presented.     

Efficient generation of FIR radiation by optical pumping of D2 18O

In this paper we show that D₂ ¹⁸O vapour, optically pumped with a continuously tunable high pressure CO₂ laser, is an excellent source for far infrared radiation. Both high photon conversion coefficients and broad Raman gain regions were found for a large number of new laser transitions spread over the frequency range from 25 cm^–1 to 240 cm^–1. We demonstrate that these Raman gain regions can be used to generate far infrared laser pulses with high intensity and durations of about 100 ps.     

The Rotational Spectrum of H2Te

In the present work, we study the spectrum of the H₂Te molecule in the submillimeter-wave and far infrared region. An important aim of this investigation is the further experimental characterization of the anomalous “four-fold cluster effect” exhibited by the rotational energy levels in the vibrational ground state of H₂Te. The spectrum in the region 90–472 GHz was measured with a source-modulated millimeter-wave spectrometer and that between 600 and 1600 GHz with a far-infrared sideband spectrometer. The far infrared spectrum from 30 to 360 cm⁻¹was measured with a Bruker IFS 120 HR interferometer attached to a 3 m long cell. We have assigned 224 submillimeter-wave lines and 1695 FIR lines. These observed data were supplemented by a large number of ground state combination differences derived from rotation–vibration bands of H₂Te, and the resulting large data set was analyzed by means of a modified Watson Hamiltonian. Accurate sets of rotational and centrifugal distortion constants for all eight tellurium isotopomers were obtained.     

Optical pumping by CO2 and N2O lasers: New cw FIR emissions in vinyl cyanide

A systematical study of optical pumping by CO₂ and N₂O lasers using a FIR metallic waveguide has been undertaken in vinyl cyanide. 97 new FIR laser lines are reported in the wavelength range 400 m–1,5 mm.Unité associée au CNRS (UA 836).     

Diffusion of excited state molecules in FIR- and CO2-lasers

Both standing waves in laser oscillators and spatially inhomogenous cross sections of laser beam and pumprate cause a non-uniform distribution of excited state molecules in longitudinal and transversal direction, respectively. This spatial hole burning however is smoothed by diffusion of the excited molecules. The effect of diffusion is investigated theoretically for an optically pumped far infrared laser as well as the corresponding CO₂ pump laser. It is found, that the remaining spatial hole burning in the direction of wave propagation is negligible within CO₂ lasers but not within FIR lasers. Concerning the transversal direction it can be shown that in the FIR laser diffusion takes no effect, whereas the transversal distribution of the excited molecules in the CO₂ laser is significantly influenced by diffusion.FIR ring lasers avoid longitudinal spatial hole burning, which leads to the common assumption that they use the active medium more efficient than conventional standing wave lasers, hence delivering higher output powers. This expected advantage is levelled out to a great extent by diffusion.     

Observation of exciton surface polaritons at room temperature

10 new cw far infrared laser lines have been observed by optically pumping the CD₃ deformation vibration band of CD₃OH with 9 μm CO₂-laser lines     

R branch tuning characteristics of the13CH3F Raman FIR laser

Summary We described a¹³CH₃F Raman laser pumped by a grating tuned 20 atmospheres CO₂ laser. The emission characteristics of the¹³CH₃F laser extends from 14 cm^–1–35 cm^–1 and from 49 cm^–1–72 cm^–1; about 65% of these frequency ranges can be covered with tunable radiation. The characteristics shows a strong dependence on the rotaional quantum numbers of the states involved in the Raman laser transitions and, within each tuning interval, on the frequency offset with respect to the frequencies of resonant transitions. We obtained, at 51 cm^–1, a maximum FIR laser pulse energy of about 800 J (at a pump energy of 200 mJ), corresponding to a photon conversion of about 8%. In some cases we have observed simultaneous emission at a Raman and a cascade frequency. In addition, FIR emission power dependence on¹³CH₃F gas pressure and pump pulse power were investigated for different J quantum numbers.