Spatially resolved measurement of singlet delta oxygen by radar resonance-enhanced multiphoton ionization.

Coherent microwave Rayleigh scattering (Radar) from resonance-enhanced multiphoton ionization (REMPI) was demonstrated to directly and nonintrusively measure singlet delta oxygen, O(2)(a(1)Δ(g)), with high spatial resolution. Two different approaches, photodissociation of ozone and microwave discharge plasma in an argon and oxygen flow, were utilized for O(2)(a(1)Δ(g)) generation. The d(1)Π(g)←a(1)Δ(g) (3-0) and d(1)Π(g)←a(1)Δ(g) (1-0) bands of O(2)(a(1)Δ(g)) were detected by Radar REMPI for two different flow conditions. Quantitative absorption measurements using sensitive off-axis integrated cavity output spectroscopy (ICOS) was used simultaneously to evaluate the accuracy and sensitivity of the Radar REMPI technique. The detection limit of Radar REMPI was found to be comparable to the ICOS technique with a detection threshold of approximately 10(14) molecules/cm(3) but with a spatial resolution that was 8 orders of magnitude smaller than the ICOS technique.

Direct measurement of methyl radicals in a methane/air flame at atmospheric pressure by radar REMPI.

We report the direct measurements of methyl radicals (CH(3)) in methane/air flames at atmospheric pressure by using coherent microwave Rayleigh scattering (Radar) from Resonance Enhanced Multi-Photon Ionization (REMPI), also known as the Radar REMPI technique. A tunable dye laser was used to selectively induce the (2 + 1) REMPI ionization of methyl radicals (CH(3), 3p(2)A(2)('')0(0)(0) band) in a near adiabatic and premixed laminar methane/air flame, generated by a Hencken burner. In situ measurements of the REMPI electrons were made by non-intrusively using a microwave homodyne transceiver detection system. The REMPI spectrum of the CH(3) radical was obtained and a spatial distribution of the radicals limited by focused laser beam geometry, approximately 20 µm normal to the flame front and 2.4 mm parallel to the flame, was determined. The measured CH(3) was in good agreement with numerical simulations performed using the detailed kinetic mechanism of GRI-3.0. To the authors' knowledge, these experiments represent the first directly-measured spatially-resolved CH(3) in a flame at atmospheric pressure.