In most applications helium-based plasma jets operate in an open-air environment. The presence of humid air in the plasma jet will influence the plasma chemistry and can lead to the production of a broader range of reactive species. We explore the influence of humid air on the reactive species in radio frequency (rf)-driven atmospheric-pressure helium-oxygen mixture plasmas (He-O 2 , helium with 5000 ppm admixture of oxygen) for wide air impurity levels of 0-500 ppm with relative humidities of from 0% to 100% using a zero-dimensional, time-dependent global model. Comparisons are made with experimental measurements in an rf-driven micro-scale atmospheric pressure plasma jet and with one-dimensional semi-kinetic simulations of the same plasma jet. These suggest that the plausible air impurity level is not more than hundreds of ppm in such systems. The evolution of species concentration is described for reactive oxygen species, metastable species, radical species and positively and negatively charged ions (and their clusters). Effects of the air impurity containing water humidity on electronegativity and overall plasma reactivity are clarified with particular emphasis on reactive oxygen species.
The formation of reactive species in the afterglow of a radio-frequency-driven atmospheric-pressure plasma in a fixed helium-oxygen feed gas mixture (He+0.5%O 2 ) with humid air impurity (a few hundred ppm) is investigated by means of an extensive global plasma chemical kinetics model. As an original objective, we explore the effects of humid air impurity on the biologically relevant reactive species in an oxygen-dependent system. After a few milliseconds in the afterglow environment, the densities of atomic oxygen (O) decreases from 10 15 to 10 13 cm −3 and singlet delta molecular oxygen (O 2 ( 1 D)) of the order of 10 15 cm −3 decreases by a factor of two, while the ozone (O 3 ) density increases from 10 14 to 10 15 cm −3 . Electrons and oxygen ionic species, initially of the order of 10 11 cm −3 , recombine much faster on the time scale of some microseconds. The formation of atomic hydrogen (H), hydroxyl radical (OH), hydroperoxyl (HO 2 ), hydrogen peroxide (H 2 O 2 ), nitric oxide (NO) and nitric acid (HNO 3 ) resulting from the humid air impurity as well as the influence on the afterglow chemistry is clarified with particular emphasis on the formation of dominant reactive oxygen species (ROS). The model suggests that the reactive species predominantly formed in the afterglow are major ROS O 2 ( 1 D) and O 3 (of the order of 10 15 cm −3 ) and rather minor hydrogen-and nitrogen-based reactive species OH, H 2 O 2 , HNO 3 and NO 2 /NO 3 , of which densities are comparable to the O-atom density (of the order of 10 13 cm −3 ). Furthermore, the model quantitatively reproduces the experimental results of independent O and O 3 density measurements.
We unravel the complex chemistry in both the neutral and ionic systems of a radio-frequency-driven atmospheric-pressure plasma in a helium-oxygen mixture (He-0.5%O 2 ) with air impurity levels from 0 to 500 ppm of relative humidity from 0% to 100% using a zero-dimensional, time-dependent global model. Effects of humid air impurity on absolute densities and the dominant production and destruction pathways of biologically relevant reactive neutral species are clarified. A few hundred ppm of air impurity crucially changes the plasma from a simple oxygen-dependent plasma to a complex oxygen-nitrogen-hydrogen plasma. The density of reactive oxygen species decreases from 10 16 to 10 15 cm −3 , which in turn results in a decrease in the overall chemical reactivity. Reactive nitrogen species (10 13 cm −3 ), atomic hydrogen and hydroxyl radicals (10 11 -10 14 cm −3 ) are generated in the plasma. With 500 ppm of humid air impurity, the densities of positively charged ions and negatively charged ions slightly increase and the electron density slightly decreases (to the order of 10 11 cm −3 ). The electronegativity increases up to 2.3 compared with 1.5 without air admixture. Atomic hydrogen, hydroxyl radicals and oxygen ions significantly contribute to the production and destruction of reactive oxygen and reactive nitrogen species.
The density and temperature of electrons and key heavy particles were measured in an atmospheric-pressure pulsed-dc helium discharge plasma with a nitrogen molecular impurity generated using system with a liquid or metal anode and a metal cathode. To obtain these parameters, we conducted experiments using several laser-aided methods: Thomson scattering spectroscopy to obtain the spatial profiles of electron density and temperature, Raman scattering spectroscopy to obtain the neutral molecular nitrogen rotational temperature, phase-modulated dispersion interferometry to determine the temporal variation of the electron density, and time-resolved laser absorption spectroscopy to analyze the temporal variation of the helium metastable atom density. The electron density and temperature measured by Thomson scattering varied from 2.4 × 10 14 cm −3 and 1.8 eV at the center of the discharge to 0.8 × 10 14 cm −3 and 1.5 eV near the outer edge of the plasma in the case of the metal anode, respectively. The electron density obtained with the liquid anode was approximately 20% smaller than that obtained with the metal anode, while the electron temperature was not significantly affected by the anode material. The molecular nitrogen rotational temperatures were 1200 K with the metal anode and 1650 K with the liquid anode at the outer edge of the plasma column. The density of helium metastable atoms decreased by a factor of two when using the liquid anode.
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