Scott James Doyle

Tell el-Ḥesi, a well-known archaeological site located about 25 km east-northeast from Gaza (Figs. 1–2), contains stratified materials spanning the Chalcolithic through Hellenistic periods and an o...

Beryllium (Be), a soft alkaline earth metal, is used by the fusion community as a first wall material and within mixed-breeder blankets. During operation, Be is spread throughout the reactor and deposits on plasma-facing surfaces, including optical components. These Be coated surfaces readily oxidise forming BeO, degrading the optical properties and leading to Be and O being present in the plasmas formed near these surfaces. In this paper we present an Ar/O 2 /Be reaction mechanism for use in low-temperature plasma modelling, derived from calculated excitation, ionisation and momentum cross-sections for Be. Due to the similar properties of Be and aluminium (Al), Al is often used as a proxy in experiments; we compare plasma properties for Be containing plasmas with a well characterised Ar/O 2 /Al reaction mechanism. The two mechanisms produce similar plasma densities but dissimilar rates of diffusion, highlighting the limitations of using Al as a proxy. This work underlines that correct modelling of gas flow throughout the reactor is important in reliably predicting the re-deposition of eroded material such as BeO.

Enhancing reactive species transport at the plasma–liquid interface is important for scaling of atmospheric pressure plasmas studied in the laboratory to real-world applications. It is well-known that the introduction of turbulence at any interface will enhance mixing by enhancing species uptake from the gas phase to the liquid phase by surface renewal processes, entrainment, bubbles and surface area modification. The goal of this work is to isolate surface effects associated with turbulence from the multitude of turbulent transport enhanced processes by artificially introducing surface perturbations using Faraday waves. Experiments were conducted to determine decoloration rate constants of a model contaminant (methylene blue) as a function of both discharge features (including positive and negative streamers) and hydrodynamics (Faraday surface wavelengths). The local plasma ionization wave at the interfacial structure was modeled and compared to experiments. Interestingly, it was found in experiments that plasma in contact with the water also generated capillary waves thus modifying the surface as well. Plasma ionization waves in combination with acoustic driven Faraday waves adds to the complexity of interpreting the effects of, for example, surface area increases, due to these complex coupled phenomenon. Local plasma ionization wave structure appears to be modified (increased propagation distance) when the liquid is perturbed, leading to increased contact of the liquid water surface with reactive species. Along with interfacial surface area growth, nonlinear convective transport is also increased with perturbations, leading to the general realization that acoustic perturbations can improve transport and thus decoloration of the model contaminant dye.

Plasmas interacting with liquid surfaces produce a complex interfacial layer where the local chemistry in the liquid is driven by fluxes from the gas phase of electrons, ions, photons, and neutral radicals. Typically, the liquid surface has at best mild curvature with the fluxes of impinging plasma species and applied electric field being nominally normal to the surface. With liquids such as water having a high dielectric constant, structuring of the liquid surface by producing a wavy surface enables local electric field enhancement due to polarization of the liquid, as well as producing regions of higher and lower advective gas flow across the surface. This structuring (or waviness) can naturally occur or can be achieved by mechanical agitation such as with acoustic transducers. Electric field enhancement at the peaks of the waves of the liquid produces local increases in sources of reactive species and incident plasma fluxes which may be advantageous for plasma driven solution electrochemistry (PDSE) applications. In this paper, results are discussed from a computational investigation of pulsed atmospheric pressure plasma jets onto structured water solutions containing AgNO₃ as may be used in PDSE for silver nanoparticle (NP) formation. The solution surface consists of standing wave patterns having wavelength and wave depth of hundreds of microns to 1 mm. The potential for structured liquid surfaces to facilitate spatially differentiated chemical selectivity and enhance NP synthesis in the context of PDSE is discussed.

Energetic species produced by gas-phase plasmas that impinge on a liquid surface can initiate physicochemical processes at the gas/liquid interface and in the liquid phase. The interaction of these energetic species with the liquid phase can initiate chemical reaction pathways referred to as plasma-driven solution electrochemistry (PDSE). There are several processing opportunities and challenges presented by PDSE. These include the potential use of PDSE to activate chemical pathways that are difficult to activate with other approaches as well as the use of renewable electricity to generate plasmas that could make these liquid-phase chemical conversion processes more sustainable and environmentally friendly. In this review, we focus on PDSE as an approach for controlled and selective chemical conversion including the synthesis of nanoparticles and polymers with desired but currently uncontrollable or unattainable properties as the next step in the use of PDSE. The underpinning redox chemistry and transport processes of PDSE are reviewed as many PDSE-driven processes are transport-limited due to the many short-lived highly reactive species involved.

Electrodeless Low-Frequency (LF)/Radio-Frequency (RF) plasma sources often suffer from low power coupling efficiencies due to the lack of overlapping field with the dynamic plasma load. However, the power supplies for these plasma sources typically have very high power efficiencies (>90%) and are more cost-effective compared to microwave sources. If the coupling efficiency to the plasma can be increased, these plasma sources offer a competitive technology for the sustainable electrification of the chemical industry. This work experimentally investigates five power coupling methods, applied to toroidal CO₂ plasmas in a quartz vessel. The research was based on similar ferrite coupling as used in energy-efficient plasma lamps. The higher resistance of the CO₂ plasma decreased the power coupling from 90% (for mercury-vapor plasma) to 66% at 1 mbar. High coupling efficiencies in LF/RF powered discharges can be achieved in two manners: either the inductance of the transformer cores can be increased, or the electromagnetic wave frequency can be increased. Furthermore, additional ferrite cores in parallel with the primary coils can be used to increase the impedance transformation. An experiment with six ferrite cores with a single primary winding in parallel, at a frequency of about 10 MHz and a power of 1 kW, showed that this frequency has a detrimental effect on the magnetic permeability and the losses in the ferrite result in a decrease of coupling to 33% at 1.5 mbar. At a frequency of 66 kHz with a nanocrystalline soft magnetic material core, a coupling of 89% was achieved in 1.5 mbar plasma for a power of 3.1 kW. This configuration exhibits decreasing coupling efficiencies at higher pressures since the plasma impedance increases, which again limits the coupling of the transformer due to a lack of inductance. The investigation of alternative coreless coil plasma configurations resulted in coupling efficiencies up to 89% decreasing to 50% at 102 mbar for a toroidal plasma enclosed by toroidally spiraling coils.

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/NF₃ mixtures. 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 NF₃ for the same conditions produces essentially complete NF₃ dissociation. Electron depletion as a result of dissociative attachment of NF₃ and NF _x fragments significantly alters the discharge topology, confining the electron density to the downstream portion of the source where the NF _x density has been lowered by this dissociation.

The development of real-time control strategies for key discharge parameters, such as densities, fluxes, and energy distributions, is of fundamental interest to many plasma sources. Over the last decade, multi-harmonic ‘tailored’ voltage waveforms have been successfully employed to achieve enhanced control of key parameters in a wide range of radio-frequency (RF) plasma sources through application of the electrical asymmetry effect (EAE). More recently, the analogous magnetic asymmetry effect (MAE) has been numerically and experimentally demonstrated to achieve a notable degree of control in parallel plate RF plasma sources. The MAE is achieved via selectively magnetising the charged species adjacent to one electrode, altering the charge flux to the surface and enforcing a DC self-bias to maintain quasineutrality. This study addresses the degree of control achieved by the MAE in a non-planar geometry via 2D fluid/kinetic simulations of a magnetised RF capacitively coupled plasma source employing two different magnetic topologies. The simultaneous application of the EAE and MAE is then presented for the same geometry, demonstrating a degree of non-linear behaviour dependant upon the applied magnetic topology. Control of the DC self-bias voltage η dc is demonstrated for a single 600   V pp , 13.56 MHz discharge in both ‘convergent’ (maximum on-axis field strength) and ‘divergent’ (minimum on-axis field strength) magnetic topolgies. MAE induced modulations of η dc   =   0.13   V pp and η dc   =   0.03   V pp are achieved for each magnetic topology, respectively, for magnetic field strengths between 50 and 1000 G. Simultaneous application of an EAE and MAE is achieved through a multi-harmonic ‘peak’-type tailored voltage waveform employing varying harmonic phase offsets between 0 ∘   ⩽   θ   ⩽   360 ∘ . The degree to which the DC self-bias voltage is modulated by the applied EAE is mediated by the orientation and magnitude of the applied magnetic field. The EAE induced DC self-bias modulations exhibit non-linear behaviour in response to a superimposed MAE, such that the resulting DC self-bias differs from an additive combination of the two effects alone Simultaneous application of the electrical and MAEs offers the possibility of further decoupling ion and electron dynamics in RF plasma sources, and represents an improvement over each approach in isolation.

The development of compact, low power, charge–neutral propulsion sources is of significant recent interest due to the rising application of micro-scale satellite platforms. Among such sources, radio frequency (rf) electrothermal microthrusters present an attractive option due to their scalability, reliability, and tunable control of power coupling to the propellant. For micropropulsion applications, where available power is limited, it is of particular importance to understand how electrical power can be transferred to the propellant efficiently, a process that is underpinned by the plasma sheath dynamics. In this work, two-dimensional fluid/Monte Carlo simulations are employed to investigate the effects of applied voltage frequency on the electron, ion, and neutral heating in an rf capacitively coupled plasma microthruster operating in argon. Variations in the electron and argon ion densities and power deposition, and their consequent effect on neutral-gas heating, are investigated with relation to the phase-averaged and phase-resolved sheath dynamics for rf voltage frequencies of 6–108 MHz at 450 V. Driving voltage frequencies above 40.68 MHz exhibit enhanced volumetric ionization from bulk electrons at the expense of the ion heating efficiency. Lower driving voltage frequencies below 13.56 MHz exhibit more efficient ionization due to secondary electrons and an increasing fraction of rf power deposition into ions. Thermal efficiencies are improved by a factor of 2.5 at 6 MHz as compared to the more traditional 13.56 MHz, indicating a favorable operating regime for low power satellite applications.

Non-equilibrium inductively coupled plasmas (ICPs) operating in hydrogen are of significant interest for applications including large-area materials processing. Increasing control of spatial gas heating, which drives the formation of neutral species density gradients and the rate of gas-temperature-dependent reactions, is critical. In this study, we use 2D fluid-kinetic simulations with the Hybrid Plasma Equipment Model to investigate the spatially resolved production of atomic hydrogen in a low-pressure planar ICP operating in pure hydrogen (10–20 Pa or 0.075–0.15 Torr, 300 W). The reaction set incorporates self-consistent calculation of the spatially resolved gas temperature and 14 vibrationally excited states. We find that the formation of neutral-gas density gradients, which result from spatially non-uniform electrical power deposition at constant pressure, can drive significant variations in the vibrational distribution function and density of atomic hydrogen when gas heating is spatially resolved. This highlights the significance of spatial gas heating on the production of reactive species in relatively high-power-density plasma processing sources.