Determination of temperature and concentration of molecular nitrogen,oxygen and methane with coherent anti-stokes raman scattering

Temperature and concentration measurements by Coherent Anti-Stokes Raman Scattering (CARS) of molecular nitrogen, oxygen and methane were carried out. A comparison of corrected thermocouple and CARS temperature measurements in a high-temperature furnace up to 2000 K is presented. The temperature dependent CARS spectra of N₂ and O₂ are evaluated by a simulation program. Agreement between CARS and thermocouple temperatures is obtained within 40 K for N₂ and 80 K for O₂. Good agreement is found between measurements and calculations of the decrease of CARS intensity with temperature. Various quick-fit methods for N₂-and O₂-temperature measurements from temperature sensitive spectral parameters were tested. Temperature dependent CARS spectra of thev ₁-fundamental of methane are recorded and the methane CARS intensity as function of temperature is measured.     

Coherent light scattering spectroscopy for supersonic flow measurements

A unified discussion on coherent light scattering spectroscopy and its spectral dependence on molecular gas velocity, temperature and density is presented. The feasibility of using coherent Raman spectroscopy techniques for nonintrusive measurements of supersonic flow parameters is demonstrated and recent laboratory as well as wind tunnel experiments are reviewed. In addition, the advantages of using coherent Rayleigh-Brillouin spectroscopy for measuring high pressure flows are discussed.     

Temperature and concentration measurements of molecular hydrogen in a filamentary discharge by coherent anti-stokes raman spectroscopy (CARS)

Coherent anti-Stokes Raman Spectroscopy (CARS) is applied to a filamentary discharge in H₂. Temperature and density profiles of molecular hydrogen are determined. The maximum temperature observed on the discharge axis is 5685 K. Vibrational and rotational transitions are analyzed and a difference in the evaluated temperatures is found which increases with pressure. In addition, the reactive thermal conductivity associated with dissociation is determined and compared with earlier work.     

A time-resolved study of sub-nanosecond pulse generation by the combined effects of stimulated brillouin scattering and laser-induced breakdown

The generation of subnanosecond pulses by the combined effects of stimulated Brillouin scattering (SBS) and laser-induced breakdown has been investigated by obtaining simultaneous streak photographs of the spark, the backscattered and the transmitted pulses. The results demonstrate that the output from an excimer pumped dye laser can yield subnanosecond pulses with a duration of 20ps. The pulse shortening effect results from the nonlinear reflection properties of the Brillouin mirror and the strong absorption of visible radiation by the laser-breakdown plasma.     

Non-quantum liquefaction of coherent gases

We show that a gas-to-liquid phase transition at zero temperature may occur in a coherent gas of bosons in the presence of competing nonlinear effects. This situation can take place in atomic systems like Bose-Einstein condensates in alkali gases with two-body and three-body interactions of opposite signs, as well as in laser beams which propagate through optical media with Kerr (focusing) and higher order (defocusing) nonlinear responses. The liquefaction process takes place in the absence of any quantum effect and can be formulated in the framework of a mean field theory, in terms of the minimization of a thermodynamic potential. We study from a thermodynamic point of view all the stationary solutions of the cubic-quintic nonlinear Schrödinger equation which describes our system. We show that solitonic localized solutions connect the gaseous and liquid phases. Furthermore, we also perform a numerical simulation in the presence of linear gain and three-body recombination where a rich dynamics, including the emergence of self-organization behavior, is found.     

Stimulated raman scattering of fuel droplets

The strong stimulated Raman scattering (SRS) from diesel fuel droplets has the potential of providing the relative concentration of multicomponent fuel and the absolute size of individual droplets. The morphology-dependent resonances (MDRs) of a sphere cause the droplet to act as an optical resonator which greatly lowers the SRS threshold. The number density, quality factor, and frequency shift of several MDRs are calculated as a function of the ratio of the index of refraction of the liquid and the surrounding gas, which approaches unity at the thermodynamic critical condition for the fuel spray. The SRS spectra of monodispersed droplets of toluene, pentane, Exxon-Aromatic-150, and Mobil D-2 are presented. The exponential growth region of the SRS intensity I _1S as a function of the input laser intensity I _input is investigated for the toluene carbon ring breathing mode v ₂ and the pentane C-H stretching region. The I _1S ratio of toluene and pentane is measured as a function of the ratio of the toluene and pentane concentration for monodispersed droplets. The reduced fluctuation in I _1S when I _input is changed from multimode to single-mode is displayed as a histogram of the I _1S of the v ₂ mode of toluene droplets.     

N2 laser frequency conversion by stimulated Raman scattering in H2

High-efficiency frequency conversion in H₂ of a nitrogen laser oscillator-amplifier system is described. The laser system provides about 1 MW output power with a very low intrinsic divergence. Up to 3 Stokes lines at 392, 468, and 581 nm and 3 Anti-Stokes at 296, 263, and 237 nm, respectively, have been observed at the output of the 60 cm long H₂ Raman cell. Peak power values of 500, 300, and 70 kW have been measured for the first 3 Stokes, respectively, corresponding to a 56% pump energy conversion efficiency.A comparison between free and guided propagation (in a hollow dielectric waveguide) is also reported, for various values of the pump intrinsic divergence.     

High-order stimulated electronic Raman scattering from lithium vapor

An intense radiation at 395.0 nm has been observed when lithium vapor is optically pumped in a heat pipe with a pulsed dye laser whose output wavelength is tuned near the Li 2s–4s two-photon resonance transition. The radiation is emitted in the direction along the pump laser beam. It is proposed that the 395.0 nm radiation is mainly generated through three-photon excitation and one-Raman-photon scattering followed by two-cascade (spontaneous) emission. The overall reaction mechanism can be described by a parametric six-wave mixing process. The quantum efficiency of the observed process is estimated to be of the order of 2 × 10^–6.This work was partially supported by the USC Faculty Research and Innovation Fund     

Nonstationary intracavity stimulated raman scattering by polaritons

Stimulated Raman scattering by polaritons when employing a nonlinear crystal inside the cavity of the laser with Q-switching and locked to fundamental frequency was theoretically studied. The equations were formulated describing the dynamics of the fundamental, Stokes and polariton waves under the assumption of instant Q-switching and uniformity of radiation except in the longitudinal direction. Numerical solutions of the equations were found and analysed. We demonstrate the influence, on generation characteristics, of the most important parameters, such as the effective nonlinearity, the initial level of population inversion, the feedback of the Stokes wave and the group mismatch between a Stokes and a pump wave. Optimum generation conditions are determined. Possibilities of the method are discussed for the generation of a) giant pulses which are controllable with regard to carrier frequency and duration but are unachievable with other methods, b) Stokes pulses of very small duration and high energy having sharp trailing edges, and c) analogous polariton pulses in the middle and far infrared range. The generation using a number of polariton branches in LiNbO₃ was considered as an example. Calculations are in qualitative agreement with experimental data.     

Experimental study of vibrational and pure rotational coherent anti-stokes Raman scattering (CARS) in molecular hydrogen

Using a specially designed excimer-laser-pumped dye laser of adjustable bandwidth high-lying pure rotational transitions of both, ortho-and para-hydrogen have been identified by coherent anti-Stokes Raman scattering (CARS). As an interesting application H₂-based CARS-thermometry is discussed.     

Stimulated raman scattering up to 10 orders in an optical fiber

This paper describes the experimental investigation of stimulated Raman scattering obtained from a multimode fiber. 10 orders of stimulated Stokes scattering of wavelengths in the 546–702 nm region were obtained from a 480m multimode, low-loss, graded-index quartz fiber pumped by a 532 nm frequency-doubled YAG-Nd laser beam with a pulse duration of 7 ns, output power of 0.7 MW and repetition rates of 5 and 10 pps.     

Determination of temperature by stimulated raman scattering of molecular nitrogen,oxygen, and carbon dioxide

We have determined the temperature from SRS spectra of N₂-N₂, N₂-CO₂, O₂-O₂, and CO₂-CO₂ recorded in wide pressure and temperature ranges. The fitting procedure takes simultaneously into account the Dicke effect and motional narrowing. We have quantified the accuracy of the MEG and ECS-P models for rotational relaxation. The temperature extracted from each model is compared with thermocouple measurements. The influence of vibrational broadening and shifting is discussed in detail.     

Stimulated IR- and vacuum-UV emission following two-photon-excitation of molecular hydrogen using an ArF laser

Hydrogen molecules are excited by two 193 nm-photons [X¹ _g ⁺ E,F¹ _g ⁺ ;Q₀₂(1)] generated with a commerical oscillator-amplifier ArF laser. Stimulated emission is subsequently observed in the IR (=752.4 nm to 836.6 nm;E, FB) and in the VUV (=134.0 nm to 160.9 nm;BX) with a VUV conversion efficiency of 0.2%. The rotational fine-structure, the saturation behaviour, pump depletion as well as SRS-onset on and off two-photon resonance are investigated.     

Soret effect in forced Rayleigh scattering

In forced Rayleigh scattering of mixtures or suspensions the temperature gratings generate, by the Soret effect, concentration gratings that may be very important since they produce both a phase and an amplitude grating superimposed on the principal one. The experimental evidence of their influence was given by Thyagarajan and Lallemand using a mixture of carbondisulfide and ethanol. In this paper we study the temporal behaviour of the concentration grating versus the sample properties and its effect on the detected diffracted beam. Explicit expressions are given for the output intensity taking into account both the generated amplitude and phase gratings.     

Resonance enhanced coherent anti-stokes raman scattering and laser induced fluorescence applied to CH radicals: a comparative study

Resonance enhanced CARS and LIF have been applied to the CH radicals in a microwave excited Ar/H/CH plasma ( Pa, kW). Both techniques yield similar nonthermal rotational population distributions of CH(X) in its vibrational ground state (), which can be described by two rotational temperatures, K being in the order of the gas temperature for rotational states with , and a considerably higher for the higher rotational states. This result is in good agreement with previous resonance CARS and LIF measurements in similar plasmas. With resonance CARS additional measurements on CH in the state could be performed yielding a vibrational temperature of 2440 K, the total CH density was about m. The detection limits of both techniques are determined, in our case about CH radicals per quantum state in the detection volume, and their advantages and disadvantages are discussed. Received: 29 April 1996 / Accepted: 19 June 1996     

A new method of assessing the efficiency of second harmonic generation by small samples of organic crystals

The intensity of optical second harmonic generation was measured from pressed KCl disks containing low concentrations (1%) of non-linear optical (NLO) materials. Comparison of the signals at 532 nm, with the known second order NLO coefficients exhibited a monotonic relationship. An estimate was made of the effect of light scattering at 532 nm, on the results.     

Coherent raman spectroscopy of nitrogen molecules and clusters in supersonic jets

Coherent Stokes and anti-Stokes Raman scattering CSRS and CARS have been employed to study the spectroscopy of nitrogen molecules and clusters in the expansion of a supersonic jet. In the vibrational spectrum, at strong stagnation conditions, an intense redshifted peak is observed which can be assigned to the intramolecular vibrations in large N₂ clusters having adopted the -phase structure. Another weak feature is assigned to nitrogen clusters in the -phase. In the rotational region of the spectrum only monomer features have been observed. The failing to observe librational motions is consistent with the finding that the nitrogen clusters are predominantly in the orientationally unordered -phase. The low rotational temperature suggests supercooling of the -phase.     

Test of an optical parametric oscillator (OPO) as a compact and fast tunable stokes source in coherent anti-stokes raman spectroscopy (CARS)

An optical parametric oscillator (OPO), as a novel kind of broadband Stokes source, is employed for coherent anti-Stokes Raman spectroscopy (CARS). Compared to the conventional dye laser configuration OPO-CARS offers practical advantages. The tunable OPO allows a fast and comfortable frequency tuning. The excitation bandwidth of about 35 cm^–1 (FWHM) limits the spectral range of effective and stable single pulse CARS generation but can be used to enhance selected spectral structures.