Abstract

Time-resolved and spatially resolved temperature measurements, by pure rotational picosecond broadband coherent anti-Stokes Raman spectroscopy (CARS), and kinetic modeling calculations are used to study kinetics of energy thermalization in nanosecond pulse discharges in air and hydrogen–air mixtures. The diffuse filament, nanosecond pulse discharge (pulse duration ∼100 ns) is sustained between two spherical electrodes and is operated at a low pulse repetition rate to enable temperature measurements over a wide range of time scales after the discharge pulse. The experimental results demonstrate high accuracy of pure rotational ps CARS for thermometry measurements in highly transient non-equilibrium plasmas. Rotational–translational temperatures are measured for time delays after the pulse ranging from tens of ns to tens of ms, spanning several orders of magnitude of time scales for energy thermalization in non-equilibrium plasmas. In addition, radial temperature distributions across the plasma filament are measured for several time delays after the discharge pulse. Kinetic modeling calculations using a state-specific master equation kinetic model of reacting hydrogen–air plasmas show good agreement with experimental data. The results demonstrate that energy thermalization and temperature rise in these plasmas occur in two clearly defined stages, (i) ‘rapid’ heating, caused by collisional quenching of excited electronic states of N2 molecules by O2, and (ii) ‘slow’ heating, caused primarily by N2 vibrational relaxation by O atoms (in air) and by chemical energy release during partial oxidation of hydrogen (in H2–air). The results have major implications for plasma assisted combustion and plasma flow control.

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