New short-wavelength laser emissions from partially deuterated methanol isotopes

The partially deuterated isotopes of methanol, CH₂DOH and CHD₂OH, have been reinvestigated as sources of far-infrared (FIR) laser emissions using an optically pumped molecular laser (OPML) system recently designed for wavelengths below 150 μm. With this system, 10 new FIR laser emissions from these isotopes ranging from 32.8 to 174.6 μm have been discovered. This includes the shortest known OPML emission from CHD₂OH, at 32.8 μm. These lines are reported with their operating pressure, polarizations relative to the CO₂ pump laser and wavelengths, measured to ±0.5 μm. In addition, polarizations for three previously observed FIR laser lines from CHD₂OH were measured for the first time. This paper is dedicated to the memory of Dr. K.M. Evenson, a pioneer in the field for his role in the development of optically pumped molecular lasers and their use in laser frequency measurements and the laser magnetic resonance technique. His scientific expertise, guidance, mentoring and friendship will be greatly missed. Received: 27 March 2002 / Published online: 8 May 2002     

Discovery and frequency measurement of far-infrared laser emissions generated by optically pumped CH2DOH

A recently improved three-laser heterodyne system was used to frequency measure ten previously observed optically pumped far-infrared (FIR) laser emissions from the partially deuterated methanol isotopologue CH₂DOH. Also, a 64.0 μm FIR emission generated by the 9P32 line of the carbon dioxide (CO₂) laser was discovered and frequency measured. These newly measured frequencies have fractional uncertainties on the order of ±2×10^-7 and correspond to laser wavelengths ranging from 42.6 to 152.7 μm. The offset frequency for the CO₂ pump laser was measured for twenty-two CH₂DOH FIR laser emissions. PACS 07.57.Hm; 42.55Lt; 42.62.Eh     

Short-wavelength far-infrared laser cavity yielding new laser emissions in CD3OH

A significantly improved far-infrared laser has been used to generate optically pumped laser emissions from 26 to 150 μm for CD₃OH. Using an X–V-pumping geometry, several new laser emissions have been found for CD₃OH. In addition, an increase in power, by factors from 10 to 1000, for many of the previously known shorter-wavelength laser lines, below 100 μm, has been observed. Frequency measurements for several lines have also been performed and have been reported to a fractional uncertainty up to ±2×10^-7, permitting the spectroscopic assignment of the laser transition. One of the frequency-measured lines, 44.256 μm observed using the 10R34 pump, has confirmed the assignment of the previously reported FIR emission (n,K;J)=(1,7;20)?(0,8;20)A in the ground vibrational state. Received: 26 October 2000 / Published online: 7 February 2001     

Efficient and widely step-tunable terahertz generation with a dual-wavelength CO<Subscript>2</Subscript> laser

Coherent terahertz radiation in a widely step-tunable range of 72.3–2706 μm (0.11–4.15 THz) has been generated in GaAs crystal by difference-frequency generation using one CO₂ laser with dual-wavelength output. The peak power of THz pulse reaches 35 W at the wavelength of 236.3 μm, which corresponds to a pulse energy of 2.1 μJ. An average power of 10 μW has been achieved when working repetitively. This efficient terahertz radiation source is more compact and widely tunable than other THz sources pumped by CO₂ laser.     

CH<Subscript>3</Subscript>OH optically pumped by a <Superscript>13</Superscript>CO<Subscript>2</Subscript> laser: new laser lines and assignments

We report 12 new THz (far-infrared) laser lines from methanol (CH₃OH), ranging from 58.1 μm (5.2 THz) to 624.6 μm (0.5 THz). A ¹³CO₂ laser of wide tunability (110 MHz) has been used for optical pumping, allowing access to previously unexplored spectral regions. Optoacoustic absorption spectra were used as a guide to search for new THz laser lines, which have been characterized in wavelength, polarization, offset, relative intensity, and optimum operation pressure. For 20 laser lines previously observed, we have measured the absorption offset with respect to the ¹³CO₂ laser line center. PACS 33.20.Ea; 33.20.Vq; 33.80.-b     

Discovery and frequency measurement of short-wavelength far-infrared laser emissions from optically pumped <Superscript>13</Superscript>CD<Subscript>3</Subscript>OH and CHD<Subscript>2</Subscript>OH

A three-laser heterodyne system was used to measure the frequencies of twelve previously observed far-infrared laser emissions from the partially deuterated methanol isotopologues ¹³CD₃OH and CHD₂OH. Two laser emissions, a 53.773 μm line from ¹³CD₃OH and a 74.939 μm line from CHD₂OH, have also been discovered and frequency measured. The CO₂ pump laser offset frequency was measured with respect to its center frequency for twenty-four FIR laser emissions from CH₃OH, ¹³CD₃OH and CHD₂OH. PACS 07.57.Hm; 42.55.Lt; 42.62.Eh     

Infrared laser emission in two-photon pumped sodium vapour

We report infrared laser emission in the region of 3 to 5 μm from sodium vapour optically pumped by a pulsed dye laser with wavelengths ranging from 585 to 610nm. Twophoton excitation processes are believed to be responsible for the primary excitation. Both molecular transitions (4 to 5 μm) between high lying states, and atomic transitions (5² S _1/2−4² P _3/2,1/2 at 3.41 μm) have been identified.     

Far-infrared laser emission from deuterated ammonia

By optically pumping the deuterated isotopomers of ¹⁴NH₃ and ¹⁵NH₃ using ¹²C¹⁶O₂, ¹³C¹⁶O₂, ¹²C¹⁸O₂, and ¹³C¹⁸O₂ lasers, several new far-infrared (FIR) emission lines between 65 μm and 125 μm have been detected. The existing spectroscopy of ¹⁴N-ammonia isotopomers has been used to identify many of these lines, as well as some previously observed but unidentified. The spectroscopic data have been analyzed to predict over 20 additional FIR laser lines that could be pumped by a more capable CO₂ laser. This effort was motivated by a need for strong laser lines in frequency coincidence with molecular transitions of astrophysical interest. Of particularnote is the measurement of the 2680-GHz line of ¹⁴NHD₂, whose frequency is 4.9 GHz higher than that of the important J=1-0 line of interstellar HD. Received: 25 July 2002 / Published online: 20 December 2002 RID="*" ID="*"Corresponding author. Fax: +1-303/492-5941, E-mail: boreiko@spot.colorado.edu     

Stimulated rotational Raman scattering at multiwavelength under tea CO2 laser pumping with a multiple-pass cell

Stimulated rotational Raman scattering (SRRS) at multiwavelength pumped by TEA CO₂ laser was demonstrated in this paper. Raman mediums were cooled by liquid-N₂ and a multiple-pass cell (MPC) with 25 passes was designed and used. When the para-H2 was pumped by single-longitudinal-mode (SLM) circular polarized TEA CO₂ laser on 10P(20), 9P(20), and 10R(20), 50 mJ 16.95 μm, 350 mJ 14.44 μm, and 536 mJ 16.9 μm radiations were obtained, corresponding to energy conversion efficiency of 1.2, 11.7, and 13.4%, respectively. When the ortho-D₂ was pumped by CO₂ laser on 10R(18), 108 mJ 12.57 μm Raman laser was obtained with energy conversion efficiency of 2.9%.     

Resonant pumping far-infrared NH3 laser

A far-infrared (FIR) NH₃ laser was resonantly pumped with a line-tunable infrared (IR) NH₃ laser. The number of the observed FIR laser lines amounted to 33. Most of them belonged toaR(J,K) rotation-inversion transition in (0, 1, 0, 0) vibrational state. The line tunability of sealed-off FIR NH₃ laser was almost achieved in 90, 115, 150, and 220 m wavelength regions by the selective line tuning of the pumping IR NH₃ laser.     

Investigation of 13CH3OH methanol: new laser lines and assignments

We have reinvestigated ¹³CH₃OH as a source of far-infrared (FIR) laser emission using a CO₂ laser as a pumping source. Thirty new FIR laser lines in the range 36.5 μm to 202.6 μm were observed and characterized. Five of them have wavelengths between 36.5 and 75 μm and have sufficient intensity to be used in LMR spectroscopy. Using Fourier-transform spectroscopic data in the infrared (IR) and FIR regions we have determined the assignment for 10 FIR laser transitions and predict nine frequencies for laser lines which have yet to be observed. Received: 17 July 2000 / Published online: 6 December 2000     

Reinvestigation of far-infrared laser emissions from hydrazine and deuterated isotopes of difluoromethane and methanol

Hydrazine (N₂H₄) and the deuterated isotopes of difluoromethane (CD₂F₂) and methanol (CH₃OD and CD₃OH) have been reinvestigated as sources of far-infrared (FIR) laser emissions using an optically pumped molecular laser system designed for wavelengths below 150 microns. With this system, seven FIR laser emissions from optically pumped N₂H₄, CH₃OD and CD₃OH were discovered with wavelengths ranging from 54.0 to 185.0 m. In addition, the polarizations of eight previously observed laser emissions from optically pumped N₂H₄, CH₃OD and CD₂F₂ were measured for the first time. All laser emissions are reported with their operating pressures, relative polarizations and wavelengths, measured to ±0.5 m. The effectiveness of this particular system in generating short-wavelength laser emissions has been further demonstrated by the improvement in output power observed from nine known FIR laser emissions. PACS 07.57.Hm; 42.55.Lt     

Discovery and characterization of optically pumped far-infrared laser emissions using laser magnetic resonance spectroscopy

A laser magnetic resonance spectrometer has been used to discover and subsequently measure a far-infrared laser emission: the 166.6-micron line of CH₂F₂, optically pumped by the 9P24 CO₂ laser. By recording spectra for the NH radical, the frequency of this laser emission has been determined to be 1799950±13 MHz. Spectra for the NH radical were also recorded with two other far-infrared laser emissions: the 160.4-micron line of N₂H₄ (9P46 CO₂ pump) and the 328.6-micron line of ¹³CH₃OH (9P12 CO₂ pump). From the NH spectra, a discrepancy of 2.1 GHz with the previously measured laser frequency was identified for the 160.4-micron line. A three-laser heterodyne system was then used to remeasure the frequency to be 1868475.5±0.5 MHz. The NH spectra were also used to determine the frequency for the 328.6-micron line to be 912366±7 MHz, in agreement with the value previously calculated from the Rydberg–Ritz combination principle. PACS 07.57.Hm; 32.60.+i; 42.62.Eh     

Continuous-wave tunable Cr2+:ZnS laser

We report the first continuous-wave tunable over ∼280 nm around 2.3 μm room-temperature operation of a chemical vapor transport-grown and diffusion-doped Cr²⁺:ZnS laser, pumped by a Co:MgF₂ laser at 1.67 μm and generating over 100 mW of output power at 16% slope efficiency. The self-consistent results of the laser and spectroscopic analysis demonstrate a large potential of this crystal as an active medium for diode-pumped tunable mid-infrared sources. Received: 7 January 2002 / Revised: 14 March 2002 / Published online: 2 May 2002     

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.     

Stark effect on CH3OH and CH3F FIR lasers: Large frequency tuning and resolved structures

The operation of a cw FIR laser in the presence of a strong electric field is described. A hybrid metal-dielectric waveguide is used and the cavity length is scanned to study how the frequency and power of the laser depend on the field strength. The results have also been checked by heterodyning with a conventional reference laser. We report the results obtained for the 496 μm line of CH₃F and the 70.5 μm and 119 μm lines of CH₃OH. A large frequency tunability of almost ±40 MHz is obtained in the best case with power levels in the mW range. A very simple theoretical model accounts for the experimental results. We also report the appearance of a new FIR line at about 204 μm when CH₃OH is pumped by the 9 μmP(34) of CO₂ in the presence of an electric field larger than 1.2 KV/cm.     

Limitations of an optically pumped rubidium laser imposed by atom recycle rate

A rubidium laser pumped on the 5²S_1/2–5²P_3/2 D₂ transition by a pulsed dye laser at pump intensities exceeding 3.5 MW/cm² (>1000 times threshold) has been demonstrated. Output energies as high as 12 μJ/pulse are limited by the rate for collision relaxation of the pumped ²P_3/2 state to the upper laser ²P_1/2 state. More than 250 photons are available for every rubidium atom in the pumped volume during each pulse. For modest alkali atom and ethane spin–orbit relaxer concentrations, the gain medium can only process about 50 photons/atom during the 2–8 ns pump pulse. At 110°C and 550 Torr of ethane, the system is bottlenecked in the ²P_3/2 state and all of the incident photons cannot be absorbed. The output energy is linearly dependent on pump pulse duration for a given pump energy. The highly saturated pump limit of the recently developed three-level model for diode pumped alkali lasers (DPALs) is developed. The system efficiency based on absorbed photons approaches 36% even for these extreme pump conditions.     

New NH2H4 far-infrared laser lines and their frequencies

We report 25 new far-infrared laser lines and 26 heterodyne frequency measurements in hydrazine. The frequencies range from 1.0 to 5.5 THz with most of the frequencies between 2.5 and 4.0 THz. The lines were generated in a high frequency, far-infrared Fabry-Perot laser cavity pumped by a CO₂ laser. The cavity has a high Q for wavelengths below 150 µm and uses variable coupling to optimize the power for each line.This work has been financed by the Brazilian Government - Conselho Nacional de Desenvolvimento Científico e Tecnológico (CNPq), and by the United States Government - NASA grant W-18, 623.Contribution of NIST, not subject to U.S. copyright.     

Multiwatt optically pumped ammonia laser operation in the 12–13 μm

Design and operating caracteristics of high pulse repetition rate NH₃ laser producing up to 20 W of average output power are described. The NH₃ laser, operating in the 12–13 μm region was optically pumped with a high pulse repetition rate TEA CO₂ laser. Dependences of the NH₃ laser output on the pump energy, ammonia and buffer gas pressures and pulse repetition rate have been studied. The conversion efficiency of up to 16% has been received.     

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.