Quantitative concentration measurements of atomic sodium in an atmospheric hydrocarbon flame with asynchronous optical sampling.

We report the development of a pump-probe instrument that uses a high-repetition-rate (82-MHz) picosecond laser. To maximize laser power and to minimize jitter between the pump- and the probe-pulse trains, we choose the asynchronous optical sampling (ASOPS) configuration. Verification of the method is obtained through concentration measurements of atomic sodium in an atmospheric methane-air flame. For the first time to our knowledge, ASOPS measurements are made on a quantitative basis. This is accomplished by calibration of the sodium concentration with atomic absorption spectroscopy. ASOPS measurements are taken at a rate of 155.7 kHz with only 128 averages, resulting in a corresponding detection limit of 5 × 10(9) cm(-3). The quenching-rate coefficient is obtained in a single measurement with a variation of ASOPS, which we call dual-beam ASOPS. The value of this coefficient is in excellent agreement with literature values for the present flame conditions. Based on our quantitative results for detection of atomic sodium, a detection limit of 2 × 10(17) cm(-3) is predicted for the Q(1) (9) line of A (2)Σ(+) (v = 0)-X(2)II (v = 0) hydroxyl at 2000 K. Although this value is too large for practical flame studies, a number of improvements that should lower the ASOPS detection limit are suggested.