Settersten, T.B.; Kronemayer, H.; Sick, V.; Bessler, W.G.; Schulz, Christof; Daily, J.W.:

Population cycling in saturated laser-induced fluorescence detection of nitric oxide

In: 4th Joint Meeting of the US Sections of the Combustion Institute
Drexel University in Philadelphia, PA on March 20-23, 2005: The combustion Institute (2005)
Buchaufsatz / Kapitel / Fach: Maschinenbau
Abstract:
We describe experiments designed to study population cycling in laser-induced fluorescence (LIF) detection of nitric oxide. Population cycling refers to the process by which a molecule is excited multiple times by the   same laser pulse. This cycling occurs when collisions rapidly quench laser-excited molecules to the ground state and subsequent rapid rotational energy transfer in the ground state refills the laser-pumped level. This can be a significant contribution to the overall LIF signal during a saturating laser pulse. Owing to extremely slow ground-state vibrational energy transfer in NO, population cycling is only significant when there is rapid and direct electronicquenching to NO X 2P(v??=0). This potential quenching channel was investigated for several collision partners by measuring recovery of the ground-state population following intense laser excitation. Experiments were conducted in a room-temperature flow cell containing dilute mixtures of NO in quenching gases. An intense nanosecond laser pulse, tuned to the NO A 2S+–X 2P(0,0) Q1+Q21 bandhead at 226.3 nm, depopulated more than 20% of the equilibrium population in the X 2P(v??=0) manifold. A weak, time-delayed, picosecond laser pulse, tuned to the A–X(1,0) Q1+Q21 bandhead at 214.9 nm, measured recovery of population in X(v??=0) under different quenching conditions. Results are presented for quenching gases: N2, CO2, O2, and H2O. The results are an important step toward providing a detailed understanding of the physics of saturated LIF, which is necessary to properly model detection strategies based on high laser fluences.