A laser optical method for the determination of tropospheric OH concentrations

A long-path absorption procedure for the determination of tropospheric OH concentrations is described in detail. Initial measurements using this method were carried out in Frankfurt a. M. By including in the evaluation the visible radiation of a frequencydoubled dye laser used in the measurements, it was possible to mathematically reduce the signal fluctuations caused by the scattering and density fluctuations of tropospheric air. The resulting detection limit was 3×10⁶ OH per cm³. SO₂ concentrations which had to be simultaneously determined in order to eliminate an interference effect, could be detected in the range of 1–40 ppb on the absorption path.     

Two-Frequency waveguide CO2 laser for atmospheric pollution monitoring

The present paper suggests and discusses a method allowing one to produce a two-frequency switching mode between any two adjacent transitions of a CO₂ laser. Switching is achieved by means of simple modulation of the resonator length by a piezoelement. The use of conventional electronic circuits ensures the maintainance of a high power balance (10^–2–10^–1%) vs. switching rate) at the generation frequencies. The data of the two-frequency CO₂ laser with a waveguide resonator used for various systems, based on a differential absorption technique and designed to control the atmospheric pollutions, are presented.     

Intra-cavity spectroscopy with diode lasers

A multi-mode diode laser with an external cavity is studied experimentally and theoretically for its application to intra-cavity spectroscopy. One facet of a typical Ga_0.89Al_0.11As laser diode was antireflection-coated by deposition of HfO₂ such that 10^–3 residual reflectivity was left over. This diode was placed in an external optical cavity. The emission spectrum of this diode laser is highly sensitive to any frequency-dependent loss in the cavity, and the detectivity of such a loss grows with the pump rate. Even close to threshold, the absorption at 780 nm of Rb atoms with a density of 5×10¹⁰ cm^–3 has been detected. An adequate model for diode lasers based on rate equations and including frequency-dependent gain saturation is developed and applied to the calculations of output spectra. The sensitivity of these spectra to intra-cavity absorption is determined by the overall cavity loss — which is rather high — and the fraction of spontaneous emission in the total emission, in contrast with dye lasers where it is limited by nonlinear mode coupling. Various criteria for the sensitivity are suggested. The smallest detectable absorption with a perfectly antireflection-coated laser is 10^–6 cm^–1. Improvement of the characteristics of the laser diode would increase the sensitivity.     

A two-wavelength oscillation CO2 laser for differential absorption measurements of atmospheric trace molecules

A two-wavelength oscillation C0₂ laser was constructed for the differential absorption measurement of low concentrations of atmospheric trace molecules and pollution molecules. A diffraction grating was alternately angle-modulated for the two-branch oscillation using a single C0₂ laser. The output power of the two wavelengths was balanced to be equal. With these characteristics, the phase-sensitive detection technique can be applied to give highly sensitive detection of the received power difference, which is proportional to the absorption in the optical path of the transmitted beams. A differential absorption spectrometer was used to demonstrate the usefulness of this two-wavelength laser oscillation method incorporating the output power balancing technique. The concentration of ethylene molecules was detected in a calibration cell and was also measured in real time in the exhaust of a combustion engine. From these results it has been shown that this differential absorption scheme offers a minimum detectable absorption of approximately 0.8%.     

Relaxation oscillations and damping factors of 1.3 μm In(Ga)As/GaAs quantum-dot lasers

In(Ga)As/GaAs quantum-dot (QD) lasers with emission wavelength at 1295 nm at room temperature are fabricated. The laser active region contains a threefold stack of QD layers with surface dot density of 4.56 × 10¹⁰ cm^–2. The laser structure is aluminum-free with InGaP as cladding layers. Threshold current density of a narrow stripe laser of 8 m wide and 3.5 mm long is 152.5 A/cm². The highest relaxation oscillation frequency measured at room temperature is 1.8 GHz, corresponding to a modulation bandwidth of 2.8 GHz due to the small damping factor. From the above measurement, the differential gain and gain compression factor were extracted to be 4.3 × 10^–16 cm² and 3.4 × 10 ^–17 cm ³, respectively. Using these parameters, the maximum modulation bandwidth f _{3 dB max} is estimated as 7.9 GHz.     

2-μm high-power multiple-frequency single-mode Q-switched Ho:YLF laser for DIAL application

We report on the development and the demonstration of a two-wavelength single-frequency laser oscillator based on Ho:YLF crystal. This laser is especially suitable for application as a transmitter in differential absorption lidar (DIAL)/integrated path differential absorption (IPDA) measurements of atmospheric carbon dioxide (CO₂) using the R30 CO₂ absorption line at 2,050.967 nm. The oscillator consists in a fiber-coupled and free-space solid-state hybrid system and can be used in high-energy middle-rate or moderate-energy high-rate configurations. The latter produced On and Off sequentially single-frequency laser pulses with 13 mJ of energy at a repetition rate of 2 kHz and pulse duration of 42 ns. The pulse energy and frequency stabilities are specially documented in free-running, single-frequency and two-frequency seeding single-mode operations. Standard deviation is 7.7 % for pulse energy and 2 MHz for frequency stability for the two-wavelength seeding operation. Allan variance plot shows that frequency fluctuations are reduced below 70 kHz for 10 s of averaging which is suitable for accurate CO₂ DIAL or IPDA measurements.     

Method of Measuring the Spectral Shape of the Radiation Line of a Three-Micron Long-Path Laser Gas Analyzer

A new method to experimentally determine the spectral shape of the radiation line of a tunable long-path absorption laser gas analyzer operating in a three-micron range ( = 2.5–4.5 m) on the basis of a difference-frequency generator is suggested. The method is based on measurement of the transmission function of a gas medium upon modulation of its optical thickness or pressure. Specific vibrational–rotational transitions and also optimal pressures of CO₂, N₂O, and CH₄ are recommended for carrying out experiments.     

Sensitive intracavity photoacoustic measurements with a CO2 waveguide laser

A photoacoustic intracavity configuration is presented; a resonant photoacoustic cell excited in its first longitudinal mode is placed inside the cavity of a CO₂ waveguide laser. Due to the high laser power and the sharp intracavity focus, saturation effects occur in the excitation and relaxation process of absorbing C₂H₄ molecules. A more optimal configuration is applied to measure the C₂H₄ emission of several Rumex species. A detection sensitivity of 6 ppt (parts per trillion) C₂H₄ is reached, equivalent to a minimal detectable absorption of 1.8×10^–10 cm^–1.     

Infrared laser stark shift spectroscopy in ammonia

The Stark effect in ammonia has been theoretically and experimentally analyzed using lead salt tunable diode laser absorption spectroscopy and CO₂ laser absorption spectroscopy of several absorption lines around 1050 cm^–1 applied to an all-optical sensor for measuring of electric field strength. Measurements of the Stark splitting effect of theaR(5,K) ammonia lines forK=1–5 as well as for the sR(3,K) lines forK=0–3 have been made at Doppler broadening pressures and for several different electric field strengths. Theoretical electric field dependent energy levels have been evaluated by diagonalization of a 6×6 energy matrix constructed using both electric field independent and dependent terms. From the theoretical analysis the resolution can be predicted and optimized both in the Doppler broadened and in the pressure broadened regimes. The predicted resolution is 0.5% at an electric field strength of 20 kV/cm. The theoretical calculations and the experimental data recorded with the tunable diode laser system were compared with independent measurements made with a CO₂ laser system. The agreement between experimentally recorded and theoretically calculated spectra is good which indicates that the theoretical model is satisfactory for our purposes. The contribution from the normally forbidden ssR(5, 3) ammonia line to the absorption at theP(12) CO₂ laser line in the 9 m band is briefly discussed.     

Infrared absorption of silane,ammonia, acetylene and diborane in the range of the CO2 laser emission lines: Measurements and modelling

Absorption spectra of the gases SiH₄, NH₃, C₂H₂ and of SiH₄/Ar and SiH₄/B₂H₆ mixtures have been measured in the spectral range of the CO₂ laser from 9.2 to 10.8 µm. In agreement with literature, silane shows the highest absorption (absorption coefficient = 3.3 × 10^–2 Pa^–1 m^–1). The deviation of the measured absorption behaviour of silane from literature, as far as the pressure dependence is concerned, can be explained by the enhanced spectral energy density in our experiment. This is confirmed by a rate-equation model involving the basic mechanisms of V-V and V-T energy transfer between vibrationally excited silane molecules. In contrast to silane, the absorption coefficient of NH₃ at the 10P(20) laser line is 4.5 × 10^–4 Pa^–1 m^–1 atp = 20 kPa and has its maximum of 4.5 × 10^–3 Pa^–1 m^–1 at the 10R(6) laser line. For C₂H₂ and B₂H₆, is even less ( 2.1 Ò 10^–5 Pa^–1 m^–1 for C₂H₂).     

Absorption of CO 2 laser emission by freon-12

The infrared (IR) absorption of freon-12 (CF₂Cl₂) was studied in the emission range of a 3-W tunable CW CO₂ laser by using a brass cell with KBr windows that was located outside the laser resonator. The results show that CF₂Cl₂ absorbs all CO₂ laser emission lines in the ranges of 1073–1083 cm^-1 and 937–943 cm^-1. The most strongly absorbed laser line was 10P (28) ( 937.21 cm^-1). Absorption coefficient values were obtained for all available wavelengths of the CO₂ laser as the CF₂Cl₂ pressure was varied from 5 to 1000 mbar. By using the HITRAN database for freon-12, the absorption coefficients were calculated at the 10P (28) and 9R (28) lines as functions of the gas pressure and compared with the experimental values. The calculated results are in reasonable agreement with the experiment. PACS 33.20.Ea; 42.55.-f; 42.55.Lt     

Application of a CW helium neon laser for measurement of gaseous hydrogen fluoride concentration

The concentration of gaseous hydrogen fluoride in air can be measured by the use of a close coincidence between the 3P ₄–2s ₂ cascade cw helium neon laser line and the 1R5 hydrogen fluoride absorption line. A nearby cw HeNe laser line (3p ₂–2s ₂) is not absorbed by hydrogen fluoride and may be used to compensate for transmission losses in a long-path measurement system. Most of the HFv=0 tov=1 absorption lines lie in a region in which there is strong attenuation caused by atmospheric water vapour, but the 1R5 line is almost free of interference from H₂O, CO₂ or CO.     

Fiber laser intracavity absorption spectroscopy for in situ multicomponent gas analysis in the atmosphere and combustion environments

Intracavity absorption spectroscopy with a broadband Er³⁺-doped fiber laser is applied for the measurements of several molecular species revealing quantitative information about the gas concentration, temperature and chemical reactions in flames. The spectral range of measurements extends from 6200 cm⁻¹ to 6550 cm⁻¹ with the proper choice of the fiber length and by moving an intracavity lens. With a pulsed laser applied in this experiment, the sensitivity to absorption corresponds to an effective absorption path length of 3 km assuming the cavity is completely filled with the sample. For a cw laser, the effective absorption path length is estimated to be 50 km. Absorption spectra of various molecules such as CO₂, CO, H₂O, H₂S, C₂H₂ and OH were recorded separately in the cell and/or in low-pressure methane and propane flames. The presented measurements demonstrate simultaneous in situ detection of three molecular products of chemical reactions at different flame locations. Variation of the relative strengths of OH absorption lines with the temperature enables the estimation of the local flame temperature. The sensitivity of this laser does not depend on the broadband cavity losses and it can be used for in situ measurements of absorption spectra in hostile environments such as contaminated samples, flames or combustion engines. The presented technique can be applied for various diagnostic purposes, such as in environmental, combustion and plasma research, in medicine and in the determination of stable isotope ratios.     

Numerical modeling of a fast-axial-flow CW–CO2 laser

A four-temperature model has been applied on a fast axial flow, longitudinal discharge CO₂ laser. Using Runge–Kutta method, a set of differential equations of the model is numericaly solved. These equations describe the operation of the laser with certain ratio 1:3:6 of the mixture CO₂:N₂: He and average output power of 550 W.The temporal behaviour of the output power and photon density was obtained. The effects of kinetic temperature, coupled mirror reflectivity, gas flow speed, and cavity loss on the output power were studied.Calculated output power was compared with its measured value taken from experiment and a good agreement was observed.     

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.     

A study of the methanol laser with a 500 MHz tunable CO2 pump laser

The absorption spectrum of CH₃OH is measured optoacoustically over a 500 MHz tuning range in 84 different CO₂ laser lines, and 19 assigned CO-stretch absorptions are used for establishing the linearity of the measurements over two decades of absorption coefficient. 40 new FIR laser lines originating from large offset absorption, are reported in the wavelength range between 40 and 400 m, and their wavelengths are given with a relative accuracy of 5×10^–5. 30 lines are assigned, involving CO-stretch transitions in torsionaln=0, 1, and 2 states, as well as transitions inn=3 of the vibrational ground state, pumped by transitions to Fermi interacting states.Work supported by the Danish National Science Research Council grant No. 11-5375     

Practical separation of silicon isotopes by IRMPD of Si2F6

Large-scale silicon isotope separation based on the IRMPD of natural Si₂F₆ has been carried out using a commercially available high power CO₂ TEA laser and a flow reaction system. The decomposition product SiF₄ containing 19–33% of ³⁰Si was obtained at a production rate of 1.5×10^–2–2.6×10^–2 mol·h^–1, depending on experimental parameters such as laser wavelength, laser fluence, pressure, and flow rate. SiF₄ containing 12% of ²⁹Si was obtained under slightly different conditions, i.e., at a shorter wavelength than that for ³⁰Si. When 39% of Si₂F₆ was decomposed at a slow flow rate, residual Si₂F₆ was found to have 99.7% of ²⁸Si. The production rate was 4.2×10^–2 mol·h^–1.     

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.     

Nonlinear refraction and nonlinear absorption of As2S3 aqueous solution

We report for the first time to our knowledge on the preparation of colloidal solution of chalcogenide semiconductor As₂S₃ by laser ablation and the measurements of its nonlinear-optical characteristics using Z-scan method at the wavelength of Nd:YAG laser radiation ( = 1064 nm, = 25 ns). The nonlinear refractive index was measured to be –7.5 × 10^–18 m² W^–1. Nonlinear absorption coefficient of chalcogenide solution was measured to be 1 cm GW^–1.