Sascha R. Engel

Gas phase temperature measurements in the liquid and particle regime of a flame spray pyrolysis process using O 2 -based pure rotational coherent anti-Stokes Raman scattering

For the production of oxide nanoparticles at a commercial scale, flame spray processes are frequently used where mostly oxygen is fed to the flame if high combustion temperatures and thus small primary particle sizes are desired. To improve the understanding of these complex processes in situ, noninvasive optical measurement techniques were applied to characterize the extremely turbulent and unsteady combustion field at those positions where the particles are formed from precursor containing organic solvent droplets. This particle-forming regime was identified by laser-induced breakdown detection. The gas phase temperatures in the surrounding of droplets and particles were measured with O(2)-based pure rotational coherent anti-Stokes Raman scattering (CARS). Pure rotational CARS measurements benefit from a polarization filtering technique that is essential in particle and droplet environments for acquiring CARS spectra suitable for temperature fitting. Due to different signal disturbing processes only the minority of the collected signals could be used for temperature evaluation. The selection of these suitable signals is one of the major problems to be solved for a reliable evaluation process. Applying these filtering and signal selection steps temperature measurements have successfully been conducted. Time-resolved, single-pulse measurements exhibit temperatures between near-room and combustion temperatures due to the strongly fluctuating and flickering behavior of the particle-generating flame. The mean flame temperatures determined from the single-pulse data are decreasing with increasing particle concentrations. They indicate the dissipation of large amounts of energy from the surrounding gas phase in the presence of particles.

Gas mixing analysis by simultaneous Raman imaging and particle image velocimetry

We report the combined application of Ramanography and particle image velocimetry (PIV) for the investigation of gas mixing processes. A droplet seeded hydrogen flow was injected as a free jet into pressurized nitrogen at 0.95 MPa. Ramanography and PIV were used to quantitatively image the mixture composition and the flow field of the mixing process, respectively.

Characterization of a CH planar laser-induced fluorescence imaging system using a kHz-rate multimode-pumped optical parametric oscillator

The performance characteristics of a new CH planar laser-induced fluorescence (PLIF) imaging system composed of a kHz-rate multimode-pumped optical parametric oscillator (OPO) and high-speed intensified CMOS camera are investigated in laminar and turbulent CH4-H2-air flames. A multi-channel Nd:YAG cluster that produces up to 225 mJ at 355 nm with multiple-pulse spacing of 100 μs (corresponding to 10 kHz) is used to pump an OPO to produce up to 6 mJ at 431 nm for direct excitation of the A-X (0, 0) band of the CH radical. Single-shot signal-to-noise ratios of 82:1 and 7.5:1 are recorded in laminar premixed flames relative to noise in the background and within the flame layer, respectively. The spatial resolution and image quality are sufficient to accurately measure the CH layer thickness of ~0.4 mm while imaging the detailed evolution of turbulent flame structures over a 20 mm span. Background interferences due to polycyclic-aromatic hydrocarbons and Rayleigh scattering are minimized and, along with signal linearity, allow semi-quantitative analysis of CH signals on a shot-to-shot basis. The effects of design features, such as cavity finesse and passive injection seeding, on conversion efficiency, stability, and linewidth of the OPO output are also discussed.

High-speed CH planar laser-induced fluorescence imaging using a multimode-pumped optical parametric oscillator.

We report on high-speed CH planar laser-induced fluorescence (PLIF) imaging in turbulent diffusion flames using a multimode-pumped optical parametric oscillator (OPO). The OPO is pumped by the third-harmonic output of a multimode Nd:YAG cluster for direct signal excitation in the A-X (0,0) band of the CH radical. The lasing threshold, conversion efficiency, and linewidth are shown to depend on the number of pump passes in the ring cavity of the OPO. Single-shot CH PLIF images are acquired at 10 kHz with excitation energy up to 6 mJ/pulse at 431.1 nm. Signal-to-noise ratios of ~25-35 are the highest yet reported for high-speed CH PLIF.

Simultaneous laser-induced fluorescence and Raman imaging inside a hydrogen engine

We report on the simultaneous and two-dimensional measurement of laser-induced fluorescence (LIF) and Raman scattering (Ramanography) applied inside a hydrogen internal combustion (IC) engine. Two different LIF tracer molecules, triethylamine (TEA) and trimethylamine (TMA), were used for the LIF experiments. The LIF and Raman results were found to be in very good agreement. The simultaneous application of Ramanography and LIF imaging indicated that TMA is the more suitable LIF tracer molecule, compared to TEA.

Raman mixture composition and flow velocity imaging with high repetition rates

A novel and completely tracer free strategy to image composition and velocity fields during the mixing process of two liquids is introduced. The achieved temporal resolution, spatial resolution and sampling rate of 30 ns, 54 x 54 µm2 and 10 kHz, respectively, are sufficient to resolve Kolmogorov time and length scales as well as transient mixing phenomena of many technical mixing processes. During the injection of liquid water into liquid ethanol, mixing was quantitatively observed by means of high repetition rate Raman imaging using a laser cluster for the excitation of the Raman process with 8 successive light sheet pulses. One high speed camera was used to detect the CH-vibration Raman band signal of ethanol, while a second one was used to detect the OH-vibration Raman band signal of water and ethanol. From the ratio of both, the mixture composition field was computed. The dense flow field was determined by processing the mixture composition images with a variational optical flow method.

Potential of two-line atomic fluorescence for temperature imaging in turbulent indium-oxide-producing flames

The applicability of two-line atomic fluorescence (TLAF) for temperature imaging in an indium-based flame spray pyrolysis (FSP) process is demonstrated using a single tunable optical parametric oscillator (OPO) to generate the required excitation wavelengths consecutively. Single-shot images of the detected fluorescence signals demonstrate that the signal levels in the flame are suitable for evaluation of temperature and verify the capability and potential of the measurement technique directly during particle formation without additional indium seeding. Qualitative averaged two-dimensional temperature distributions in the FSP flame are presented, showing the influence of varying sheath gas flow rates on the resulting temperature distribution. With the addition of a second OPO and detection system, the two fluorescence signals acquired consecutively in this work could be obtained simultaneously and enable spatio-temporally resolved single-shot temperature measurements in flame synthesis processes of indium-containing nanoparticles.

Characterization of gas phase temperatures in dependence of particle presence in the flame spray pyrolysis process

We introduce a novel strategy to acquire gas phase temperatures by O2 pure rotational CARS during flame spray pyrolysis (FSP) for silica production. RCARS benefits from a polarization filtering technique that is essential in particle and droplet environments. Particle containing regions were located by correlating laser-induced breakdown (LIB) in a particle-laden and a particle-free flame at different heights. Measured temperatures in the particle regime show significantly lower flame temperatures for particle-laden flames since energy is dissipated rapidly by radiation heat transfer in the presence of particles.

Simultaneous measurement of multiple gas species using a Nd 3+ :YAG laser combined with Raman scattering

Coherent anti-Stokes Raman scattering technique combined with a single pulsed Nd³⁺:YAG laser is proposed and demonstrated for simultaneous measurement of CO₂ and CH₄. The technique can be used in combustion measurement consisting of gas mixture.