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Laser-induced phosphorescence (LIP) is a relatively recent and versatile development for studying flow dynamics. This work investigates certain lanthanide-based molecular complexes for their use in LIP for high-speed sprays. Lanthanide complexes in solutions have been shown to possess long phosphorescence lifetimes (∼1-2 ms) and to emit light in the visible wavelength range. In particular, europium and terbium complexes are investigated using fluorescence/phosphorescence spectrometry, showing that europium-thenoyltrifluoracetone-trioctylphosphineoxide (Eu-TTA-TOPO) can be easily and efficiently excited using a standard frequency-tripled Nd:YAG laser. The emitted spectrum, with maximum intensity at a wavelength of 614 nm, is shown not to vary strongly with temperature (293-383 K). The decay constant of the phosphorescence, while independent of ambient pressure, decreases by approximately 12 μs/K between 323 and 373 K, with the base level of the decay constant dependent on the used solvent. The complex does not luminesce in the gas or solid state, meaning only the liquid phase is visualized, even in an evaporating spray. By using an internally excited spray containing the phosphorescent complex, the effect of vaporization is shown through the decrease in measured intensity over the length of the spray, together with droplet size measurements using interferometric particle imaging. This study shows that LIP, using the Eu-TTA-TOPO complex, can be used with different solvents, including diesel surrogates. Furthermore, it can be easily handled and used in sprays to investigate spray breakup and evaporation.

We evaluate various molecular tagging velocimetry (MTV) techniques for application in turbulent flows of gases where the smallest length scales must be resolved. We argue that tracer diffusion dictates the use of large complex molecules and discuss a few candidate molecules. The accuracy of MTV is determined by the profile of written lines which widen due to molecular dynamics, including both diffusion and chemical reaction. We evaluate these profiles for tagging with phosphorescing biacetyl molecules, which is a commonly used probe in MTV. For relatively large laser power, these profiles are determined not by molecular diffusion, but by the triplet-triplet annihilation reaction of excited biacetyl molecules. We identify a new reaction pathway, and present a model for the observed line shapes. The rapid widening of tagged lines of biacetyl molecules due to chemical reaction restricts this MTV technique to large-scale turbulent motion in gases of comparable molecular weight.

Coherent Rayleigh-Brillouin scattering is a four-wave mixing technique that provides information on various physical properties of the scattering medium in the spectral domain. Being based on density gratings generated by dipole forces, the method requires two pump beams of sufficient spectral width to span the full response bandwidth of the scattering medium. We provide experimental data on the scattered spectrum as a function of the coherence between the two pump beams and derive the corresponding pump beam spectrum. We argue that all experiments on coherent Rayleigh-Brillouin scattering to date, have, in fact, been performed in the incoherent regime and show that orders of magnitude in scattering efficiency are to be expected when the experiments are performed with bandwidth-limited picosecond laser pulses., (© 2011 American Physical Society)

We investigate coherent Rayleigh-Brillouin spectroscopy as an efficient process to measure the bulk viscosity of gases at gigahertz frequencies. Scattered spectral distributions are measured using a Fizeau spectrometer. We discuss the statistical error due to the fluctuating mode structure of the used pump laser. Experiments were done for both polar and nonpolar gases and the bulk viscosity was obtained from the spectra using the Tenti S6 model. Results are compared to simple classical kinetic models of molecules with internal degrees of freedom. At the extremely high (gigahertz) frequencies of our experiment, most internal vibrational modes remain frozen and the bulk viscosity is dominated by the rotational degrees of freedom. Our measurements show that the molecular dipole moments have unexpectedly little influence on the bulk viscosity at room temperature and moderate pressure.

The cyanonitrene radical, NCN, is detected by laser-induced fluorescence in laminar, adiabatic, flat phi=1.3 methane-air flames at 200 hPa and atmospheric pressure. Laser excitation of the A approximately 3Piu(020)-X approximately 3Sigmag-(000) band at 317 nm allows off-resonant fluorescence to be detected at 326 nm. Excitation and dispersed fluorescence spectra are presented, as well as profiles of NCN and CH versus height above burner.

The Bayesian deconvolution algorithm described in a preceding paper [Appl. Opt. 43, 5669-5681 (2004)] is applied to measurement of the two-dimensional stoichiometry field in a combustible methane-air mixture by Raman imaging through a spectrograph. Stoichiometry (fuel equivalence ratio) is derived from the number density fields of methane and nitrogen, with a signal-to-noise ratio of approximately 10 in a 600-laser-shot average. Prospects for single-shot Raman imaging are discussed.

A grating spectrograph can be used for spectrally selective two-dimensional imaging if it is operated with a broad entrance slit. The resulting intensity distribution in its exit plane is a one-dimensional convolution of the spatial and spectral distributions of incident light. We present a dedicated deconvolution filter to reconstruct the spatial image from the spectrograph output. The algorithm is illustrated on Raman imaging of an underexpanded dry air jet. Recorded Raman images correspond to density maps convolved with the Raman spectrum of air; the latter essentially acts as a blurring function for the density map. The deconvolution filter combines the individual images recorded in the O2 and N2 Raman bands into a single image of relative air density.

Raman imaging is shown to be a very suitable technique for simultaneous density mapping of different species in dry air and N(2) supersonic nozzle flows. The salient features of Raman scattering are its molecular sensitivity and the fact that it can be spectrally separated from strong reflections and Mie scattering. We collected Raman images of both N(2) and O(2) concurrently by imaging the flow through an imaging spectrograph with a broad entrance slit onto a CCD camera. The main advantage of this method is that different species can be imaged under exactly the same flow conditions.