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5. Flame thermometry based on spectral line-shape It is clear that the composite transition width shows little sensitivity to temperature change, especially at more elevated temperatures, where the increasing Doppler width compensates for the falling Lorentzian width to result in no overall change. By contrast, a substantial change in the spectral shape is apparent from the large variation in the peak-to-trough ratio. The contrast is that the lower line in Figure 5.3 refers to changes in the spectral width of the transition, whereas the upper line describes changes in the relative intensity between two points on the spectrum. Therefore, the choice of a transition system with several appropriately spaced hyperfine lines allows for greater temperature sensitivity than would be possible with a single hyperfine line, where the location of the line flanks would need to be determined very accurately. The fidelity of the indium LIF spectra obtained during this study, and the corresponding quality of the spectral fits (see Figure 5.5) mean that the technique is sensitive even to small changes around typical flame temperatures.

5. Flame thermometry based on spectral line-shape transition have already been presented in Chapter 3, and their use together with fluorescence spectra of the 5²P3/2→6²S1/2 transition of indium (near 451.1 nm) to determine two-line temperatures has been addressed in Chapter 4. The laser wavelength scans were performed at a rate of 20 Hz, and the laser power varied between approximately 1.4 mW to 0.8 mW during the scan, due to tuning of the injection current. The experimental set-up for the thermometry experiment is shown in Figure 5.4. The main difference from the set-up for the TLAF experiments described in Chapter 4 is that, in this case, only one extended cavity diode laser is required. The substantial difference from the forgoing chapter is not in the experimental method, but in the way in which the data are analysed.

Figure 5.4 The experimental set-up for the OLAF thermometry experiments (L:

lens; IF: interference filter centred around 451.1 nm; PMT: photomultiplier tube; PD: photodiode; BS: beamsplitter; ECDL: extended cavity diode laser)

The output beam of the extended cavity diode laser was focussed (f = 300 mm) to a beam diameter of around 100 µm on the central axis of the flame.

The burner was mounted on a translation stage which allowed for the adjustment of its height. Prior to passing through the flame, part of the laser beam was reflected by a glass plate towards a quartz etalon (FSR = 3.02 GHz); the transmitted fringe pattern of this etalon was used to ensure that the laser scans were mode-hop free, and also made it possible to compensate for

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5. Flame thermometry based on spectral line-shape slight non-linearities in the wavelength scanning rate. A second glass plate was used to reflect part of the laser beam to a photodiode as a reference power measurement, which was used to normalise the fluorescence intensity.

Another photodiode was used to measure the power of the laser beam after the flame. This allowed the absorbance spectrum to be evaluated, and thus to be used to compensate the LIF spectra for attenuation of the laser beam prior to the measurement volume. The fluorescence signal was imaged at f^# = 2.4 through a pin-hole (d = 500 µm) and an interference filter centred around 451.1 nm (CVI, ∆λ = 3 nm) onto a photomultiplier tube (Hamamatsu, R3788); the photomultiplier signal was pre-amplified (Gain = 10⁵; bandwidth

= 20 kHz). This resulted in a measurement volume defined by a cylinder with a diameter of 0.1 mm and length of 0.5 mm. The detection of non-resonant fluorescence in the 5²P3/2→6²S1/2 transition, at around 451.1 nm, avoided any interference that could otherwise have resulted from scattered laser light from the surface of the burner plate. The electronic signals were digitised using an oscilloscope, and the averages of 128 individual wavelength scans were stored. Measurements of the background readings were taken and were subtracted from the experimental data. It has previously been confirmed that the values of laser irradiance such as that used here are well within the linear excitation regime (Hult et al. 2005a).

The line-shape thermometry experiments were performed in a one-dimensional laminar flame of CH4 and air, stabilised on the Mèker burner described in Chapter 3. Seeding of indium atoms was done by passing a portion of the air stream through a nebuliser containing an aqueous solution of InCl3 (~0.05 M), which resulted in a concentration of indium atoms in the flame of approximately 100 ppb. The unseeded co-flow flame (d=60 mm)

5. Flame thermometry based on spectral line-shape which was run at the same stoichiometry as the inner seeded flame (d=40 mm), which meant that the seeded region was homogeneous in temperature, thus allowing accurate path-integrated temperature measurements to be performed by the Na-line reversal technique, for the purpose of comparison.

Reference temperature measurements were made, at precisely the same flow conditions, by Na-line reversal, and by vibrational coherent anti-Stokes Raman scattering (CARS) of N2. The characterisation of the Mèker burner by CARS, Na-line reversal, and numerical simulation were performed by Mr G.

Hartung of the Laser Analytics Group, and are presented here solely for the purpose of comparison to the diode laser LIF measurements.

Due to the long path length and flat flame front of the burner used during these experiments, there was non-negligible absorption of the laser beam by atomic indium as it passed through the flame (typically around 10%);

absorbance spectra have been presented in Chapter 3. This could be thoroughly compensated for, however, because of the homogeneity of the flame, which meant that the laser power at the measurement volume could be determined. Signal trapping did not influence the line-shape of the acquired spectra since these experiments involved an excitation scan and broadband detection. Spectra were taken at a range of stoichiometries at 12 mm height above burner (HAB), and at a range of heights above the burner for φ = 1.0.

Theoretical spectra comprising the sum of four Voigt profiles were fitted to the experimental data for each of the flames conditions studied. In the case of both the φ scan and the height scan, the point at φ = 1.0 and HAB = 12 mm was used as a calibration point. For these points, ∆νD was fixed to the temperature that was measured at the same conditions by the Na-line reversal method. The relative spectral positions and relative intensities of the four

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5. Flame thermometry based on spectral line-shape hyperfine lines are well-known (Hult et al. 2005a). The four fitted parameters were: the spectral location and intensity of the leftmost hyperfine component,

∆νL, and the background. The calibration therefore allowed a relationship to be developed for ∆νL at other temperatures:

L L

ref 0.7 ref T

∆ν =∆ν

T

⎛ ⎞

⎜ ⎟

⎝ ⎠ (5.7)

Thus for the rest of the measurements, T was a fitted parameter and ∆νD and

∆νL were related to T by Eqn. 5.1 and by Eqn. 5.7, respectively. The resulting temperature data are presented and discussed in the following section.