Cold atmospheric plasma devices have shown promise for a variety of plasma medical applications, including wound healing and bacterial inactivation often performed in liquids. In the latter application, plasma-produced reactive oxygen and nitrogen species (RONS) interact with and damage bacterial cells, though the exact mechanism by which cell damage occurs is unclear. Computational models can help elucidate relationships between plasma-produced RONS and cell killing by enabling direct comparison between dissimilar plasma devices and by examining the effects of changing operating parameters in these devices. In biological applications, computational models of plasma-liquid interactions would be most effective in design and optimization of plasma devices if there is a corresponding prediction of the biological outcome. In this work, we propose a hierarchal model for planktonic bacterial cell inactivation by plasma produced RONS in liquid. A previously developed reaction mechanism for plasma induced modification of cysteine was extended to provide a basis for cell killing by plasma-produced RONS. Results from the model are compared to literature values to provide proof of concept. Differences in time to bacterial inactivation as a function of plasma operating parameters including gas composition and plasma source configuration are discussed. Results indicate that optimizing gas-phase reactive nitrogen species production may be key in the design of plasma devices for disinfection.
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Abstract Remote plasmas are used in semiconductor device manufacturing as sources of radicals for chamber cleaning and isotropic etching. In these applications, large fluxes of neutral radicals (e.g. F, O, Cl, H) are desired with there being negligible fluxes of potentially damaging ions and photons. One remote plasma source (RPS) design employs toroidal, transformer coupling using ferrite cores to dissociate high flows of moderately high pressure (up to several Torr) electronegative gases. In this paper, results are discussed from a computational investigation of moderate pressure, toroidal transformer coupled RPS sustained in Ar and Ar/NF3mixtures. Operation of the RPS in 1 Torr (133 Pa) of argon with a power of 1.0 kW at 0.5 MHz and a single core produces a continuous toroidal plasma loop with current continuity being maintained dominantly by conduction current. Operation with dual cores introduces azimuthal asymmetries with local maxima in plasma density. Current continuity is maintained by a mix of conduction and displacement current. Operation in NF3for the same conditions produces essentially complete NF3dissociation. Electron depletion as a result of dissociative attachment of NF3and NF
x fragments significantly alters the discharge topology, confining the electron density to the downstream portion of the source where the NFx density has been lowered by this dissociation. -
Abstract The electric field distribution in the ionization waves propagating over a microchannel array dielectric surface, with the channels either empty or filled with distilled water, is measured by ps Electric Field Induced Second Harmonic (EFISH) generation. The surface ionization wave is initiated by the atmospheric pressure N2-Ar plasma jet impinging on the surface vertically and powered by ns pulse discharge bursts. The results show that the electric field inside the microchannels, specifically its horizontal component, is enhanced by up to a factor of 2. The field enhancement region is localized within the channels. The vertical electric field inside the channels lags in time compared to the field measured at the ridges, indicating the transient reversal of the ionization wave propagation direction across the channels (toward the jet). This is consistent with the phase-locked plasma emission images and confirmed by the kinetic modeling predictions, which show that the ionization wave “jumps” over the empty channels and propagates into the channels only after the jump between the adjacent ridges. When the channels are filled with water, the wave speed increases by up to 50%, due to the higher effective dielectric constant of the surface. No evidence of a significant electric field enhancement near the dielectric surface (ceramic or water) has been detected, within the spatial resolution of the present diagnostic, ~100 μm.
Free, publicly-accessible full text available January 22, 2025 -
Abstract Atmospheric pressure plasma jets (APPJs) are increasingly being used to functionalize polymers and dielectric materials for biomedical and biotechnology applications. Once such application is microfluidic labs-on-a-chip consisting of dielectric slabs with microchannel grooves hundreds of microns in width and depth. The periodic channels, an example of a complex surface, present challenges in terms of directly and uniformly exposing the surface to the plasma. In this paper, we discuss results from computational and experimental investigations of negative APPJs sustained in Ar/N2mixtures flowing into ambient air and incident onto a series of microchannels. Results from two-dimensional plasma hydrodynamics modeling are compared to experimental measurements of electric field and fast-camera imaging. The propagation of the plasma across dry microchannels largely consists of a sequence of surface ionization waves (SIWs) on the top ridges of the channels and bulk ionization waves (IWs) crossing over the channels. The IWs are directed into electric field enhanced vertices of the next ridge. The charging of these ridges produce reverse IWs responsible for the majority of the ionization. The propagation of the plasma across water filled microchannels evolve into hopping SIWs between the leading edges of the water channels, regions of electric enhancement due to polarization of the water. Positive, reverse IWs follow the pre-ionized path of the initial negative waves.
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Abstract Sterilization of skin prior to surgery is challenged by the reservoir of bacteria that resides in hair follicles. Atmospheric pressure plasma jets (APPJs) have been proposed as a method to treat and deactivate these bacteria as atmospheric plasmas are able to penetrate into structures and crevices with dimensions similar to those found in hair follicles. In this paper, we discuss results from a computational investigation of an APPJ sustained in helium flowing into ambient air, and incident onto a layered dielectric similar to human skin in which there are idealized hair follicles. We found that, depending on the location of the follicle, the bulk ionization wave (IW) incident onto the skin, or the surface IW on the skin, are able to launch IWs into the follicle. The uniformity of treatment of the follicle depends on the location of the
first entry of the plasma into the follicle on the top of the skin. Typically, only one side of the follicle is treated on for a given plasma pulse, with uniform treatment resulting from rastering the plasma jet across the follicle over many pulses. Plasma treatment of the follicle is sensitive to the angle of the follicle with respect to the skin, width of the follicle pocket, conductivity of the dermis and thickness of the underlying subcutaneous fat layer, the latter due to the change in capacitance of the tissue. -
Abstract Mechanisms for the cold atmospheric plasma (CAP) treatment of cells in solution are needed for more optimum design of plasma devices for wound healing, cancer treatment, and bacterial inactivation. However, the complexity of organic molecules on cell membranes makes understanding mechanisms that result in modifications (i.e. oxidation) of such compounds difficult. As a surrogate to these systems, a reaction mechanism for the oxidation of cysteine in CAP activated water was developed and implemented in a 0-dimensional (plug-flow) global plasma chemistry model with the capability of addressing plasma-liquid interactions. Reaction rate coefficients for organic reactions in water were estimated based on available data in the literature or by analogy to gas-phase reactions. The mechanism was validated by comparison to experimental mass-spectrometry data for COST-jets sustained in He/O2, He/H2O and He/N2/O2mixtures treating cysteine in water. Results from the model were used to determine the consequences of changing COST-jet operating parameters, such as distance from the substrate and inlet gas composition, on cysteine oxidation product formation. Results indicate that operating parameters can be adjusted to select for desired cysteine oxidation products, including nitrosylated products.
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Abstract Ozone, O3, is a strong oxidizing agent often used for water purification. O3is typically produced in dielectric barrier discharges (DBDs) by electron-impact dissociation of O2, followed by three-body association reactions between O and O2. Previous studies on O3formation in low-temperature plasma DBDs have shown that O3concentrations can drop to nearly zero after continued operation, termed the ozone-zero phenomenon (OZP). Including small (<4%) admixtures of N2can suppress this phenomenon and increase the O3production relative to using pure O2in spite of power deposition being diverted from O2to N2and the production of nitrogen oxides, N
x Oy . The OZP is hypothesized to occur because O3is destroyed on the surfaces in contact with the plasma. Including N2in the gas mixture enables N atoms to occupy surface sites that would otherwise participate in O3destruction. The effect of N2in ozone-producing DBDs was computationally investigated using a global plasma chemistry model. A general surface reaction mechanism is proposed to explain the increase in O3production with N2admixtures. The mechanism includes O3formation and destruction on the surfaces, adsorption and recombination of O and N, desorption of O2and N2, and NOx reactions. Without these reactions on the surface, the density of O3monotonically decreases with increasing N2admixture due to power absorption by N2leading to the formation of nitrogen oxides. With N-based surface chemistry, the concentrations of O3are maximum with a few tenths of percent of N2depending on the O3destruction probability on the surface. The consequences of the surface chemistry on ozone production are less than the effect of gas temperature without surface processes. An increase in the O3density with N-based surface chemistry occurs when the surface destruction probability of O3or the surface roughness was decreased. -
Abstract Plasmas in contact with liquids can degrade organic molecules in a solution, as reactive oxygen and nitrogen species produced in the plasma solvate into the liquid. Immersing small droplets (tens of microns in diameter) in the plasma can more rapidly activate the liquid compared to treating a large volume of liquid with a smaller surface-to-volume ratio. The interactions between a radio frequency glow discharge sustained in He/H2O and a water droplet containing formate (HCOO−aq) immersed in and flowing through the plasma were modeled using a zero-dimensional global plasma chemistry model to investigate these activation processes. HCOO
− aqinteracts with OHaq, which is produced from the solvation of OH from the gas phase. The resulting HCOO− aqconcentrations were benchmarked with previously reported experimental measurements. The diameter of the droplet, initial HCOO− aqconcentration, and gas flow rate affect only the HCOO− aqconcentration and OHaqdensity, leaving the OH density in the gas phase unaffected. Power deposition and gas mixture (e.g. percentage of H2O) change both the gas and liquid phase chemistry. A general trend was observed: during the first portion of droplet exposure to the plasma, OHaqprimarily consumes HCOO− aq. However, O2−aq, a byproduct of HCOO− aqconsumption, consumes OHaqonce O2−aqreaches a critically large density. Using HCOO− aqas a surrogate for OHaq-sensitive contaminants, combinations of residence time, droplet diameter, water vapor density, and power will determine the optimum remediation strategy. -
Miniaturized photoionization detectors (PIDs) are used in conjunction with gas chromatography systems to detect volatile compounds in gases by collecting the current from the photoionized gas analytes. PIDs should be inexpensive and compatible with a wide range of analyte species. One such PID is based on the formation of a He plasma in a dielectric barrier discharge (DBD), which generates vacuum UV (VUV) photons from excited states of He to photoionize gas analytes. There are several design parameters that can be leveraged to increase the ionizing photon flux to gas analytes to increase the sensitivity of the PID. To that end, the methods to maximize the photon flux from a pulsed He plasma in a DBD-PID were investigated using a two-dimensional plasma hydrodynamics model. The ionizing photon flux originated from the resonance states of helium, He(3P) and He(21P), and from the dimer excimer He2*. While the photon flux from the resonant states was modulated over the voltage pulse, the photon flux from He2* persisted long after the voltage pulse passed. Several geometrical optimizations were investigated, such as using an array of pointed electrodes. However, increasing the capacitance of the dielectric enclosing the plasma chamber had the largest effect on increasing the VUV photon fluence to gas analytes.
Free, publicly-accessible full text available April 14, 2025 -
The conversion of methane, CH4, into higher value chemicals using low temperature plasmas is challenged by both improving efficiency and selectivity. One path towards selectivity is capturing plasma produced methyl radicals, CH3, in a solvent for aqueous processing. Due to the rapid reactions of methyl radicals in the gas phase, the transport distance from production of the CH3 to its solvation should be short, which then motivates the use of microplasmas. The generation of CH3 in Ar/CH4/H2O plasmas produced in nanosecond pulsed dielectric barrier discharge microplasmas is discussed using results from a computational investigation. The microplasma is sustained in the channel of a microfluidic chip in which the solvent flows along one wall or in droplets. CH3 is primarily produced by electron-impact of and dissociative excitation transfer to CH4, as well as CH2 reacting with CH4. CH3 is rapidly consumed to form C2H6 which, in spite of being subject to these same dissociative processes, accumulates over time, as do other stable products including C3H8 and CH¬3OH. The gas mixture and electrical properties were varied to assess their effects on CH3 production. CH3 production is largest with 5% CH4 in the Ar/CH4/H2O mixture due to an optimal balance of electron-impact dissociation, which increases with CH4 percentage, and dissociative excitation transfer and CH2 reacting with CH4, which decrease with CH4 percentage. Design parameters of the microchannels were also investigated. Increasing the permittivity of the dielectrics in contact with the plasma increased the ionization wave intensity which increased CH3 production. Increased energy deposition per pulse generally increased CH3 production as does lengthening pulse length up to a certain point. The arrangement of the solvent flow in the microchannel can also affect the CH3 density and fluence to the solvent. The fluence of CH3 to the liquid solvent is increased if the liquid is immersed in the plasma as a droplet or is a layer on the wall where the ionization wave terminates. The solvation dynamics of CH3 with varying numbers of droplets was also examined. The maximum density of solvated methyl radicals CH3aq occurs with a large number of droplets in the plasma. However, the solvated CH3aq density can rapidly decrease due to desolvation, emphasizing the need to quickly react the solvated species in the solvent.more » « lessFree, publicly-accessible full text available April 4, 2025