Plasma Sources Science and Technology

Dielectric barrier discharges (DBDs) are plasmas generated in configurations with an insulating (dielectric) material between the electrodes which is responsible for a self-pulsing operation. DBDs are a typical example of nonthermal atmospheric or normal pressure gas discharges. Initially used for the generation of ozone, they have opened up many other fields of application. Therefore DBDs are a relevant tool in current plasma technology as well as an object for fundamental studies. Another motivation for further research is the fact that so-called partial discharges in insulated high voltage systems are special types of DBDs. The breakdown processes, the formation of structures, and the role of surface processes are currently under investigation. This review is intended to give an update to the already existing literature on DBDs considering the research and development within the last two decades. The main principles and different modes of discharge generation are summarized. A collection of known as well as special electrode configurations and reactor designs will be presented. This shall demonstrate the different and broad possibilities, but also the similarities and common aspects of devices for different fields of applications explored within the last years. The main part is devoted to the progress on the investigation of different aspects of breakdown and plasma formation with the focus on single filaments or microdischarges. This includes a summary of the current knowledge on the electrical characterization of filamentary DBDs. In particular, the recent new insights on the elementary volume and surface memory mechanisms in these discharges will be discussed. An outlook for the forthcoming challenges on research and development will be given.

Laser-produced transient tin plasmas are the sources of extreme ultraviolet (EUV) light at 13.5 nm wavelength for next-generation nanolithography, enabling the continued miniaturization of the features on chips. Generating the required EUV light at sufficient power, reliability, and stability presents a formidable multi-faceted task, combining industrial innovations with attractive scientific questions. This topical review presents a contemporary overview of the status of the field, discussing the key processes that govern the dynamics in each step in the process of generating EUV light. Relevant physical processes span over a challenging six orders of magnitude in time scale, ranging from the (sub-)ps and ns time scales of laser-driven atomic plasma processes to the several μs required for the fluid dynamic tin target deformation that is set in motion by them.

Magnetron sputtering deposition has become the most widely used technique for deposition of both metallic and compound thin films and is utilized in numerous industrial applications. There has been a continuous development of the magnetron sputtering technology to improve target utilization, increase ionization of the sputtered species, increase deposition rates, and to minimize electrical instabilities such as arcs, as well as to reduce operating cost. The development from the direct current (dc) diode sputter tool to the magnetron sputtering discharge is discussed as well as the various magnetron sputtering discharge configurations. The magnetron sputtering discharge is either operated as a dc or radio frequency discharge, or it is driven by some other periodic waveforms depending on the application. This includes reactive magnetron sputtering which exhibits hysteresis and is often operated with an asymmetric bipolar mid-frequency pulsed waveform. Due to target poisoning the reactive sputter process is inherently unstable and exhibits a strongly non-linear response to variations in operating parameters. Ionized physical vapor deposition was initially achieved by adding a secondary discharge between the cathode target and the substrate and later by applying high power pulses to the cathode target. An overview is given of the operating parameters, the discharge properties and the plasma parameters including particle densities, discharge current composition, electron and ion energy distributions, deposition rate, and ionized flux fraction. The discharge maintenance is discussed including the electron heating processes, the creation and role of secondary electrons and Ohmic heating, and the sputter processes. Furthermore, the role and appearance of instabilities in the discharge operation is discussed.

In this review we describe a transient type of gas discharge which is commonly called a streamer discharge, as well as a few related phenomena in pulsed discharges. Streamers are propagating ionization fronts with self-organized field enhancement at their tips that can appear in atmospheric air, or more generally in gases over distances larger than order 1 cm times N ₀/ N, where N is gas density and N ₀ is gas density under ambient conditions. Streamers are the precursors of other discharges like sparks and lightning, but they also occur in for example corona reactors or plasma jets which are used for a variety of plasma chemical purposes. When enough space is available, streamers can also form at much lower pressures, like in the case of sprite discharges high up in the atmosphere. We explain the structure and basic underlying physics of streamer discharges, and how they scale with gas density. We discuss the chemistry and applications of streamers, and describe their two main stages in detail: inception and propagation. We also look at some other topics, like interaction with flow and heat, related pulsed discharges, and electron runaway and high energy radiation. Finally, we discuss streamer simulations and diagnostics in quite some detail. This review is written with two purposes in mind: first, we describe recent results on the physics of streamer discharges, with a focus on the work performed in our groups. We also describe recent developments in diagnostics and simulations of streamers. Second, we provide background information on the above-mentioned aspects of streamers. This review can therefore be used as a tutorial by researchers starting to work in the field of streamer physics.

There is no ideal atomic propellant for ion thrusters. Xenon commonly used as propellant becomes resource-critical in light of electric propulsion commercialization. Combining these considerations leads to seeking alternatives to xenon as propellant. In this review, we summarize the current literature on molecular propellants. We define two classes of molecules, group I and II, comprising diatomic molecules and more complex molecules, respectively. We identify basic properties which a candidate molecule belonging to either group, I or II, should possess in order to be suitable as molecular propellant. We discuss the pits and traps in testing such candidate molecules inside a thruster on the basis of our experiences with iodine (a member of group I) and adamantane (a member of group II). The thruster system needs to be individually adopted for each propellant candidate in order to enable a thorough testing inside the thruster. The same holds for optimizing the thruster’s performance when fed with a new propellant because the microscopic processes occurring inside the plasma will differ from molecule to molecule. These circumstances make such testing time-consuming and costly. To accelerate systematic screening of the vast number of molecular species in terms of suitability as propellant, we propose a screening and evolution procedure based on combining chemical engineering and fundamental physical measurements.

Plasma–liquid interactions represent a growing interdisciplinary area of research involving plasma science, fluid dynamics, heat and mass transfer, photolysis, multiphase chemistry and aerosol science. This review provides an assessment of the state-of-the-art of this multidisciplinary area and identifies the key research challenges. The developments in diagnostics, modeling and further extensions of cross section and reaction rate databases that are necessary to address these challenges are discussed. The review focusses on non-equilibrium plasmas.

When the working gas of a negative ion source is changed from hydrogen to its isotope, deuterium, an ‘isotope effect’ is observed; namely, several plasma characteristics such as the electron energy distribution, the atomic fraction and the spectra of rovibrationally excited molecules change. The understanding of the effect becomes more important, as research and development aiming at ITER power level operation is being challenged with feeding deuterium to the ion sources. As a historical review of the effort to develop hydrogen/deuterium negative ion sources, several types of negative ion sources designed for the neutral beam plasma heating are described: double charge exchange sources, volume sources and surface-plasma sources. The early results with volume sources operated with and without cesium are introduced. The characteristics of the source charged with deuterium are compared to those of the source charged with hydrogen. The isotope effect did not appear pronounced as the negative ion density was measured in a small source but became more pronounced when the plasma source size was enlarged and the discharge power density was increased to higher values. Surface plasma sources were optimized for deuterium operation but could not achieve the same performance as a source operated with hydrogen at the same power and pressure. The lower velocity of negative deuterium ions leaving the low work function surface seemed to limit the production efficiency. Fundamental processes causing these differences in negative ion source operation are summarized. After explaining the current status of negative ion source research and development, the acquired knowledge is utilized to the development of large negative ion sources for nuclear fusion research and to the development of compact negative ion sources for neutron source applications.

Streamer discharges generated by nanosecond high-voltage pulses have gained attraction for a variety of reasons, but mainly because they are very efficient for a number of plasma-processing applications. More specifically, researchers have noted that the pulse duration and the rise time of the applied high-voltage pulse have a significant influence on the radical yield of the transient plasmas generated with these pulses; shorter pulses result in higher yields. With the need to study transient plasmas generated by these short pulses comes the need to understand how to generate those pulses and to understand the interaction between the pulse source and the discharge. In this topical review, we will explore the different methods with which to generate nanosecond high-voltage pulses, how the interaction between the pulse source and the discharge may influence the source and the discharge and how to optimize the energy transfer from the pulse source to the discharge.

Over the past few decades many diagnostics have been developed to study the non-equilibrium nature of plasma. These developments have given experimentalists the possibility to measure in situ molecular and atomic densities, electron and ion densities, temperatures and velocities of species in the plasma, to just name a few. Many of the diagnostic techniques are based on the ‘photon-in, photon-out’ principle and were at first developed to perform spectroscopy on atoms and molecules. Much later they were introduced in the research of plasmas. In this foundation paper we will focus on optical-based diagnostics that are now for quite some time common use in the field of low-temperature plasma physics research. The basic principles of the diagnostics will be outlined and references will be given to papers where these techniques were successfully applied. For a more comprehensive understanding of the techniques the reader will be referred to textbooks.

Microwave plasmas are a promising technology for energy-efficient CO ₂ valorization via conversion of CO ₂ into CO and O ₂ using renewable energies. A 2.45 GHz microwave plasma torch with swirling CO ₂ gas flow is studied in a large pressure (20–1000 mbar) and flow (1–100 L min ⁻¹) range. Two different modes of the plasma torch, depending on the operating pressure and microwave input power, are described: at pressures below 120 mbar the plasma fills most of the plasma torch volume whereas at pressures of about 120 mbar an abrupt contraction of the plasma in the center of the resonator is observed along with an increase of the gas temperature from 3000 K to 6000 K. The CO outflow is generally found to be proportional to the plasma effective power and exhibits no significant dependence on the actual CO ₂ flow injected into the reactor but only on the input power at certain pressure. Thermal dissociation calculations show that, even at the lowest pressures of this study, the observed conversion and energy efficiency are compatible with a thermal dissociation mechanism.

The input power of a CO ₂ microwave plasma is modulated at kHz rate in scans of duty cycle at constant average power to investigate gas heating dynamics and its relation to dissociation efficiency. Rotational temperature profiles obtained from rotational Raman scattering reveal peak temperatures of up to 3000 , while the edge temperature remains cold (500 ). During the plasma ‘OFF’-period, the gas cools down convectively, but remains overall too hot to allow for strong overpopulation of vibrational modes (2200 in the core). Fast optical imaging monitors plasma volume variations and shows that power density scales with peak power. As dissociation scales with observed peak rotational temperature, it is concluded that thermal processes dominate. A simple 0D model is constructed which explains how higher power density favors dissociation over radial energy transport. Thermal decomposition is reviewed in relation to quenching oxygen radicals with vibrationally excited CO ₂, to reflect on earlier reported record efficiencies of 90%.

Laser ablation in liquid-phase (LAL) has been developed since the 1990s, but the interest in laser synthesis of colloids has emerged in the last decade due to a significant improvement in the production rate, proven comparative advantages in biomedical and catalysis applications, and recent commercialization. However, the method relies on highly transient phenomena, so that the fundamental understanding lacks behind the LAL synthesis refinement research. The complexity of the physics and chemistry involved has led to experimental and theoretical investigations that attempt to provide a basic description of the underlying processes but face the challenge of temporal and spatial resolution as well as non-equilibrium conditions. It appears that the processes occurring at the early time scales, ranging from femtoseconds to several microseconds are critical in the definition of the final product. The review is mainly dedicated to the comprehensive description of the processes occurring at early time scales, which include the description of laser-matter interaction for ultrashort and short laser pulses, plasma formation processes as well as comparison of the measured plasma parameters at these time scales, and subsequent description of the cavitation bubble dynamics. Furthermore, the plasma and cavitation bubble chemistry are addressed, and their impact on the nanoparticle formation is emphasized.

The LisbOn KInetics Boltzmann (LoKI-B) is an open-source simulation tool ( https://github.com/IST-Lisbon/LoKI) that solves a time and space independent form of the two-term electron Boltzmann equation, for non-magnetised non-equilibrium low-temperature plasmas excited by DC/HF electric fields from different gases or gas mixtures. LoKI-B was developed as a response to the need of having an electron Boltzmann solver easily addressing the simulation of the electron kinetics in any complex gas mixture (of atomic/molecular species), describing first and second-kind electron collisions with any target state (electronic, vibrational and rotational), characterized by any user-prescribed population. LoKI-B includes electron-electron collisions, it handles rotational collisions adopting either a discrete formulation or a more convenient continuous approximation, and it accounts for variations in the number of electrons due to non-conservative events by assuming growth models for the electron density. On input, LoKI-B defines the operating work conditions, the distribution of populations for the electronic, vibrational and rotational levels of the atomic/molecular gases considered, and the relevant sets of electron-scattering cross sections obtained from the open-access website LXCat ( http://lxcat.net/). On output, it yields the isotropic and the anisotropic parts of the electron distribution function (the former usually termed the electron energy distribution function), the electron swarm parameters, and the electron power absorbed from the electric field and transferred to the different collisional channels. LoKI-B is developed with flexible and upgradable object-oriented programming under MATLAB ^®, to benefit from its matrix-based architecture, adopting an ontology that privileges the separation between tool and data. This topical review presents LoKI-B and gives examples of results obtained for different model and real gases, verifying the tool against analytical solutions, benchmarking it against numerical calculations, and validating the output by comparison with available measurements of swarm parameters.

Plasma-enhanced atomic layer deposition (PEALD) has obtained a prominent position in the synthesis of nanoscale films with precise growth control. Apart from the well-established contribution of highly reactive neutral radicals towards film growth in PEALD, the ions generated by the plasma can also play a significant role. In this work, we report on the measurements of ion energy and flux characteristics on grounded and biased substrates during plasma exposure to investigate their role in tailoring material properties. Insights from such measurements are essential toward understanding how a given PEALD process at different operating conditions can be influenced by energetic ions. Ion flux-energy distribution functions (IFEDFs) of reactive plasmas typically used for PEALD (O ₂, H ₂, N ₂) were measured in a commercial 200 mm remote inductively coupled plasma ALD system equipped with RF substrate biasing. IFEDFs were obtained using a gridded retarding field energy analyzer and the effect of varying ICP power, pressure and bias conditions on the ion energy and flux characteristics of the three reactive plasmas were investigated. The properties of three material examples—TiO _x , HfN _x and SiN _x —deposited using these plasmas were investigated on the basis of the energy and flux parameters derived from IFEDFs. Material properties were analyzed in terms of the total ion energy dose delivered to a growing film in every ALD cycle, which is a product of the mean ion energy, total ion flux and plasma exposure time. The properties responded differently to the ion energy dose depending on whether it was controlled with RF substrate biasing where ion energy was enhanced, or without any biasing where plasma exposure time was increased. This indicated that material properties were influenced by whether or not ion energies exceeded energy barriers related to physical atom displacement or activation of ion-induced chemical reactions during PEALD. Furthermore, once ion energies were enhanced beyond these threshold barriers with RF substrate biasing, material properties became a function of both the enhanced ion energy and the duration for which the ion energy was enhanced during plasma exposure. These results have led to a better insight into the relation between energetic ions and the ensuing material properties, e.g. by providing energy maps of material properties in terms of the ion energy dose during PEALD. It serves to demonstrate how the measurement and control of ion energy and flux characteristics during PEALD can provide a platform for synthesizing nanoscale films with the desired material properties.

The electric field in an ionization wave discharge in nitrogen at 20–100 mbar, initiated by positive polarity, high-voltage, ns duration pulses, is measured by ps second harmonic generation. The axial electric field component is determined both during the propagation of the ionization wave along the discharge tube, and after the wave reaches the grounded electrode, spanning the entire discharge gap. The temporal resolution of the present measurements is 200 ps, with the spatial resolution in the axial direction of approximately 0.5 mm. The second harmonic signal exhibits a quadratic dependence on the Laplacian electric field but indicates that in this pressure range most of the signal is generated within the wall of the tube. Absolute calibration of the signal is obtained from the current shunt data, after the ionization wave has reached the grounded electrode. Comparison of the data taken at different pressures shows that the peak value of the axial electric field in the wave front, 8–11 kV cm ⁻¹, has a fairly weak dependence on pressure, with the peak reduced electric field reaching ≈2000 Td at 20 mbar. Reducing the pressure from 100 to 20 mbar, while keeping the discharge pulse voltage waveform the same, steepens the ionization wave front considerably, from 3.0 to 1.0 ns full width at half maximum. The results demonstrate that ps second harmonic generation may be employed for electric field measurements in low-pressure discharges, discharges sustained in small diameter capillary tubes, and discharges sustained in gas mixtures with low nonlinear susceptibility, at the conditions when the detection of the signal generated directly in the plasma is challenging. High temporal resolution of the present measurements indicates a possibility of detection of non-local electron kinetics effects induced by a rapidly varying, high peak value electric field in low and moderate pressure ionization wave discharges.

Emission characteristics of a directly heated, rod-shaped LaB₆ hot cathode has been studied in a multi-dipole confinement device. It is found that contrary to predictions from the conventional space-charge limited emission theory, emission current is not simply limited to a maximum value but eventually extinguished by space-charge related effects. In addition, directional preference of electron emission towards the positive lead of the applied heating voltage can be visibly observed. Results suggest that thermionically emitted electrons trapped in the virtual cathode are pumped towards the high voltage lead of the applied heating, and that the magnetic effects for filament heating currents exceeding 50 A may be the underlying mechanism of extinguishment; that is, the gyromotion of surface emitted electrons for sufficiently great heating currents may prevent electrons from escaping the virtual cathode. Geometrical effects are also briefly discussed.

Oxygen molecules in the lowest metastable state, O₂(a¹Δ_g), play an important role in oxygen plasmas due to their high reactivity and significant concentrations. The accumulation of high densities of O₂(a¹Δ_g) occurs due to its low quenching rate. This paper demonstrates the existence, at high gas temperatures (700–1700 K), of fast quenching of O₂(a¹Δ_g) by O(³P) atoms, a process that has not been considered in previous models. Experiments were carried out at oxygen pressures of 10–100 Torr in an 81 MHz CCP discharge in a quartz tube with external electrodes. This setup provides high absorbed power density, leading to both high gas temperatures and significant O(³P) densities. We observe that the O₂(a¹Δ_g) density is significantly limited at high gas temperatures by rapid quenching by atomic oxygen. The results were interpreted using a self-consistent 1D discharge model. The observations can only be explained by the inclusion of a rapid quenching reaction: O₂(a¹Δ_g) + O(³P) → O₂(X³Σ_g⁻) + O(³P), with an activation energy in the range of 0.54–0.69 eV. The rate constant was determined over a wide range of discharge conditions (P = 20–100 Torr and T_g = 800–1700 K), giving values between 3 × 10⁻¹¹ exp(−8000/T) cm³ s⁻¹ to 1.5 × 10⁻¹¹ exp(−6300/T) cm³ s⁻¹. A possible mechanism for this process is discussed. Measurements of the density of metastable O₂(b¹Σ_g⁺) molecules also indicated the existence of quenching by atomic oxygen, with a somewhat lower activation energy of ~0.32 eV. The variations of the measured [O₂(b¹Σ_g⁺)]/N mole-fraction could be fitted by the model using a rate constant 2 × 10⁻¹¹ × exp(−3700/T) cm³ s⁻¹ for this process. These quenching processes of metastable O₂(a¹Δ_g) and O₂(b¹Σ_g⁺) molecules by oxygen atoms are important for oxygen plasmas and could have a significant impact on the kinetics of oxygen-containing mixtures at higher gas temperatures, for example in plasma-assisted combustion or in high-pressure plasma processing reactors.

A new approach to the development of extraction systems capable of forming ion beams with previously inaccessible intensity is proposed. The use of inhomogeneous accelerating field allows to improve the ion beam formation efficiency significantly. The increase of electric field magnitude is achieved by changing the shape of the electrodes only, without increasing the accelerating voltage and decreasing the interelectrode distance. The comparison is made between a new extraction system and a flat traditional one, which is the most common. The use of a new electrode geometry allows to increase the lifetime of the electrodes in sources of intense beams operating in a continuous wave mode. For electron cyclotron resonance ion sources, results demonstrate the possibility to form high-quality ion beams with a current density of more than 1A cm⁻².

A voltage and power controlled surface dielectric barrier discharge for the removal of volatile organic compounds (VOCs) from gas streams is studied by means of current–voltage measurements, flame ionization detectors, and gas chromatography–mass spectrometry (GC–MS). The discharge is generated in a defined synthetic air gas stream at atmospheric pressure by application of a damped sinusoidal voltage waveform resulting from a resonant circuit. Multiple organic compounds, namely n-butane, butanol, isobutanol, ethyl acetate, diethyl ether, and butoxyethanol, are tested at concentrations of 50, 100, 200, and 400 ppm (parts per million), as well as peak-to-peak voltages of 8 to 13 kV_pp and pulse repetition frequencies of 250 to 4000 Hz. The dissipated power within the system is calculated utilizing the measured voltage and current waveforms. The conversion and absolute degradation of the VOCs are determined by flame ionization detectors. An increasing concentration of VOCs is found to increase the dissipated power marginally, suggesting a higher conductivity and higher electron densities in the plasma. Of the applied VOCs, n-butane is found to be the most resistant to the plasma treatment, while higher concentrations consistently result in a lower conversion and a higher absolute degradation across all tested compounds. Corresponding amounts of converted molecules per expended joule are given as a comparable parameter by weighting the absolute degradation with the dissipated power. Finally, specific reaction products are determined by online GC–MS, further confirming carbon dioxide (CO₂) as a major reaction product, alongside a variety of less prevalent side products, depending on the structure of the original compound. The findings of this study are intended to promote the development of energy efficient processes for the purification of gas streams in both, industry and consumer market. Potential applications of the presented technique could be found in car paint shops, chemical plants, hospital ventilation systems, or air purifiers for living space.

We investigated CO₂ splitting in recombining H₂ and He plasmas with ultralow electron temperatures between 0.1 and 0.4 eV. The conversion from CO₂ to CO and O₂ was observed in the ultralow-temperature plasmas. Since the rate coefficients of dissociation of CO₂ via electronic excited states are negligible at the ultralow electron temperature, the present experimental result gives us corroborative evidence of the CO₂ splitting via vibrational excited states. The rate coefficient of the CO₂ splitting, which was evaluated from the temporal variation of the CO₂ density, decreased clearly with the electron temperature. In addition, the rate coefficient observed in the ionizing H₂ plasma with an electron temperature of 4 eV was one order of magnitude smaller than that observed in the recombining plasmas. It has been shown that the CO₂ splitting via vibrational excited states has a larger rate coefficient than that via electronic excited states.

Magnetron sputtering deposition has become the most widely used technique for deposition of both metallic and compound thin films and is utilized in numerous industrial applications. There has been a continuous development of the magnetron sputtering technology to improve target utilization, increase ionization of the sputtered species, increase deposition rates, and to minimize electrical instabilities such as arcs, as well as to reduce operating cost. The development from the direct current (dc) diode sputter tool to the magnetron sputtering discharge is discussed as well as the various magnetron sputtering discharge configurations. The magnetron sputtering discharge is either operated as a dc or radio frequency discharge, or it is driven by some other periodic waveforms depending on the application. This includes reactive magnetron sputtering which exhibits hysteresis and is often operated with an asymmetric bipolar mid-frequency pulsed waveform. Due to target poisoning the reactive sputter process is inherently unstable and exhibits a strongly non-linear response to variations in operating parameters. Ionized physical vapor deposition was initially achieved by adding a secondary discharge between the cathode target and the substrate and later by applying high power pulses to the cathode target. An overview is given of the operating parameters, the discharge properties and the plasma parameters including particle densities, discharge current composition, electron and ion energy distributions, deposition rate, and ionized flux fraction. The discharge maintenance is discussed including the electron heating processes, the creation and role of secondary electrons and Ohmic heating, and the sputter processes. Furthermore, the role and appearance of instabilities in the discharge operation is discussed.

In this review we describe a transient type of gas discharge which is commonly called a streamer discharge, as well as a few related phenomena in pulsed discharges. Streamers are propagating ionization fronts with self-organized field enhancement at their tips that can appear in atmospheric air, or more generally in gases over distances larger than order 1 cm times N ₀/ N, where N is gas density and N ₀ is gas density under ambient conditions. Streamers are the precursors of other discharges like sparks and lightning, but they also occur in for example corona reactors or plasma jets which are used for a variety of plasma chemical purposes. When enough space is available, streamers can also form at much lower pressures, like in the case of sprite discharges high up in the atmosphere. We explain the structure and basic underlying physics of streamer discharges, and how they scale with gas density. We discuss the chemistry and applications of streamers, and describe their two main stages in detail: inception and propagation. We also look at some other topics, like interaction with flow and heat, related pulsed discharges, and electron runaway and high energy radiation. Finally, we discuss streamer simulations and diagnostics in quite some detail. This review is written with two purposes in mind: first, we describe recent results on the physics of streamer discharges, with a focus on the work performed in our groups. We also describe recent developments in diagnostics and simulations of streamers. Second, we provide background information on the above-mentioned aspects of streamers. This review can therefore be used as a tutorial by researchers starting to work in the field of streamer physics.

Over the past few decades many diagnostics have been developed to study the non-equilibrium nature of plasma. These developments have given experimentalists the possibility to measure in situ molecular and atomic densities, electron and ion densities, temperatures and velocities of species in the plasma, to just name a few. Many of the diagnostic techniques are based on the ‘photon-in, photon-out’ principle and were at first developed to perform spectroscopy on atoms and molecules. Much later they were introduced in the research of plasmas. In this foundation paper we will focus on optical-based diagnostics that are now for quite some time common use in the field of low-temperature plasma physics research. The basic principles of the diagnostics will be outlined and references will be given to papers where these techniques were successfully applied. For a more comprehensive understanding of the techniques the reader will be referred to textbooks.

Biased electrodes are common components of plasma sources and diagnostics. The plasma–electrode interaction is mediated by an intervening sheath structure that influences properties of the electrons and ions contacting the electrode surface, as well as properties of the bulk plasma. A rich variety of sheath structures have been observed, including ion sheaths, electron sheaths, double sheaths, double layers, anode glow, and fireballs. These represent complex self-organized responses of the plasma that depend not only on the local influence of the electrode, but also on the global properties of the plasma and the other boundaries that it is in contact with. This review summarizes recent advances in understanding the conditions under which each type of sheath forms, what the basic stability criteria and steady-state properties of each are, and the ways in which each can influence plasma–boundary interactions and bulk plasma properties. These results may be of interest to a number of application areas where biased electrodes are used, including diagnostics, plasma modification of materials, plasma sources, electric propulsion, and the interaction of plasmas with objects in space.

When the working gas of a negative ion source is changed from hydrogen to its isotope, deuterium, an ‘isotope effect’ is observed; namely, several plasma characteristics such as the electron energy distribution, the atomic fraction and the spectra of rovibrationally excited molecules change. The understanding of the effect becomes more important, as research and development aiming at ITER power level operation is being challenged with feeding deuterium to the ion sources. As a historical review of the effort to develop hydrogen/deuterium negative ion sources, several types of negative ion sources designed for the neutral beam plasma heating are described: double charge exchange sources, volume sources and surface-plasma sources. The early results with volume sources operated with and without cesium are introduced. The characteristics of the source charged with deuterium are compared to those of the source charged with hydrogen. The isotope effect did not appear pronounced as the negative ion density was measured in a small source but became more pronounced when the plasma source size was enlarged and the discharge power density was increased to higher values. Surface plasma sources were optimized for deuterium operation but could not achieve the same performance as a source operated with hydrogen at the same power and pressure. The lower velocity of negative deuterium ions leaving the low work function surface seemed to limit the production efficiency. Fundamental processes causing these differences in negative ion source operation are summarized. After explaining the current status of negative ion source research and development, the acquired knowledge is utilized to the development of large negative ion sources for nuclear fusion research and to the development of compact negative ion sources for neutron source applications.

Knowing which processes and species are responsible for discharge inception is important for being able to speed up, delay, or completely avoid it. We study discharge inception in 500 mbar synthetic air by applying 10 ms long 17 kV pulses with a repetition frequency of 2 Hz to a pin-to-plate electrode geometry with a gap length of 6 cm. We record inception times for hundreds of pulses by measuring the time delay between the rising edge of the high-voltage (HV) pulse and the signal from a photo-multiplier tube. Three characteristic time scales for inception are observed: (1) 20 ns, (2) 25 μs, and (3) 125 μs. To investigate the underlying processes, we apply a low-voltage (LV) pulse in between the HV pulses. These LV pulses can speed up or delay discharge inception, and our results suggest that the three time scales correspond to: (1) free electrons or electron detachment from negative ions close to the electrode, (2) a process that liberates electrons from (quasi)-neutrals, and (3) the drift of an elevated density of negative ions to the ionization zone. However, each of these explanations has its caveats, which we discuss. We present a theoretical analysis of the distribution of inception times, and perform particle simulations in the experimental discharge geometry. Some of the observed phenomena can be explained by these approaches, but a surprizing number of open questions remain.

The PK-4 system is a micro-gravity dusty plasma experiment currently in operation on-board the International Space Station. The experiment utilizes a long DC discharge in neon or argon gases. We apply our 2D particle-in-cell with Monte Carlo collisions discharge simulation to compute local plasma parameters that serve as input data for future dust dynamics models. The simulation includes electrons, Ne ⁺ ions, and Ne ^m metastable atoms in neon gas and their collisions at solid surfaces including secondary electron emission and glass wall charging. On the time scale of the on-board optical imaging, the positive column appears stable and homogeneous. On the other hand, our simulations show that on microsecond time scales the positive column is highly inhomogeneous: ionization waves with phase velocities in the range between 500 m s ⁻¹ and 1200 m s ⁻¹ dominate the structure. In these waves, the electric field and charged particle densities can reach amplitudes up to 10 times of their average value. Our experiments on ground-based PK-4 replica systems fully support the numerical findings. In the experiment, the direction of the DC current can be alternated, which has been found to favor dust particle chain formation. We discuss possible mechanisms for how the highly oscillatory plasma environment contributes to the dust particle chain formation.

We investigate the propagation of positive streamers along a profiled dielectric surface in air at atmospheric pressure. Results from experiments and two-dimensional planar low-temperature plasma fluid simulations are presented and analysed. The test object consists of a disk-shaped high voltage electrode and a dielectric slab with 0.5 mm deep corrugations. The corrugated surface has a 47% larger surface area than the smooth reference surface. The experiments and simulations are performed at voltage levels that lead to either gap-bridging or arrested streamers. In both experiments and simulations, the streamers take a longer time to reach the ground electrode when propagating along the profiled surface than along the smooth reference surface. Also, arrested streamers stop closer to the high voltage electrode when a profiled surface is used. Streamers propagate closely along the surface profile in the simulations, which suggests that the observed surface profile effect is mainly a result of elongated streamer channels. Compared to the streamers propagating along the smooth surface, the elongated streamers on the profiled surface have less residual voltage at the streamer front to drive the streamer advancement.

Magnetron sputtering deposition has become the most widely used technique for deposition of both metallic and compound thin films and is utilized in numerous industrial applications. There has been a continuous development of the magnetron sputtering technology to improve target utilization, increase ionization of the sputtered species, increase deposition rates, and to minimize electrical instabilities such as arcs, as well as to reduce operating cost. The development from the direct current (dc) diode sputter tool to the magnetron sputtering discharge is discussed as well as the various magnetron sputtering discharge configurations. The magnetron sputtering discharge is either operated as a dc or radio frequency discharge, or it is driven by some other periodic waveforms depending on the application. This includes reactive magnetron sputtering which exhibits hysteresis and is often operated with an asymmetric bipolar mid-frequency pulsed waveform. Due to target poisoning the reactive sputter process is inherently unstable and exhibits a strongly non-linear response to variations in operating parameters. Ionized physical vapor deposition was initially achieved by adding a secondary discharge between the cathode target and the substrate and later by applying high power pulses to the cathode target. An overview is given of the operating parameters, the discharge properties and the plasma parameters including particle densities, discharge current composition, electron and ion energy distributions, deposition rate, and ionized flux fraction. The discharge maintenance is discussed including the electron heating processes, the creation and role of secondary electrons and Ohmic heating, and the sputter processes. Furthermore, the role and appearance of instabilities in the discharge operation is discussed.

In this review we describe a transient type of gas discharge which is commonly called a streamer discharge, as well as a few related phenomena in pulsed discharges. Streamers are propagating ionization fronts with self-organized field enhancement at their tips that can appear in atmospheric air, or more generally in gases over distances larger than order 1 cm times N ₀/ N, where N is gas density and N ₀ is gas density under ambient conditions. Streamers are the precursors of other discharges like sparks and lightning, but they also occur in for example corona reactors or plasma jets which are used for a variety of plasma chemical purposes. When enough space is available, streamers can also form at much lower pressures, like in the case of sprite discharges high up in the atmosphere. We explain the structure and basic underlying physics of streamer discharges, and how they scale with gas density. We discuss the chemistry and applications of streamers, and describe their two main stages in detail: inception and propagation. We also look at some other topics, like interaction with flow and heat, related pulsed discharges, and electron runaway and high energy radiation. Finally, we discuss streamer simulations and diagnostics in quite some detail. This review is written with two purposes in mind: first, we describe recent results on the physics of streamer discharges, with a focus on the work performed in our groups. We also describe recent developments in diagnostics and simulations of streamers. Second, we provide background information on the above-mentioned aspects of streamers. This review can therefore be used as a tutorial by researchers starting to work in the field of streamer physics.

Motivated by the huge need for data for non-equilibrium plasma modeling, a theoretical investigation of dissociative electron attachment to the NO molecule is performed. The calculations presented here are based on the local-complex-potential approach, taking into account five NO ⁻ resonances. Three specific channels of the process are studied, including the production of excited nitrogen atoms N( ²D) and of its anions N ⁻. Interpretation of the existing experimental data and their comparison with our theoretical result are given. A full set of ro-vibrationally-resolved cross sections and the corresponding rate coefficients are reported. In particular, a relatively large cross sections for N ⁻ ion formation at low energy of the incident electron and for vibrationally excited NO target are predicted. Finally, molecular rotation effects are discussed.

Atmospheric pressure plasmas are effective sources for reactive species, making them applicable for industrial and biomedical applications. We quantify ground-state densities of key species, atomic oxygen (O) and hydrogen (H), produced from admixtures of water vapour (up to 0.5%) to the helium feed gas in a radio-frequency-driven plasma at atmospheric pressure. Absolute density measurements, using two-photon absorption laser induced fluorescence, require accurate effective excited state lifetimes. For atmospheric pressure plasmas, picosecond resolution is needed due to the rapid collisional de-excitation of excited states. These absolute O and H density measurements, at the nozzle of the plasma jet, are used to benchmark a plug-flow, 0D chemical kinetics model, for varying humidity content, to further investigate the main formation pathways of O and H. It is found that impurities can play a crucial role for the production of O at small molecular admixtures. Hence, for controllable reactive species production, purposely admixed molecules to the feed gas is recommended, as opposed to relying on ambient molecules. The controlled humidity content was also identified as an effective tailoring mechanism for the O/H ratio.

We present a set of self-consistent cross sections for electron transport in gaseous tetrahydrofuran (THF), that refines the set published in our previous study [1] by proposing modifications to the quasielastic momentum transfer, neutral dissociation, ionisation and electron attachment cross sections. These adjustments are made through the analysis of pulsed-Townsend swarm transport coefficients, for electron transport in pure THF and in mixtures of THF with argon. To automate this analysis, we employ a neural network model that is trained to solve this inverse swarm problem for realistic cross sections from the LXCat project. The accuracy, completeness and self-consistency of the proposed refined THF cross section set is assessed by comparing the analyzed swarm transport coefficient measurements to those simulated via the numerical solution of Boltzmann’s equation.

Microwave plasmas are a promising technology for energy-efficient CO ₂ valorization via conversion of CO ₂ into CO and O ₂ using renewable energies. A 2.45 GHz microwave plasma torch with swirling CO ₂ gas flow is studied in a large pressure (20–1000 mbar) and flow (1–100 L min ⁻¹) range. Two different modes of the plasma torch, depending on the operating pressure and microwave input power, are described: at pressures below 120 mbar the plasma fills most of the plasma torch volume whereas at pressures of about 120 mbar an abrupt contraction of the plasma in the center of the resonator is observed along with an increase of the gas temperature from 3000 K to 6000 K. The CO outflow is generally found to be proportional to the plasma effective power and exhibits no significant dependence on the actual CO ₂ flow injected into the reactor but only on the input power at certain pressure. Thermal dissociation calculations show that, even at the lowest pressures of this study, the observed conversion and energy efficiency are compatible with a thermal dissociation mechanism.

Plasma treatment and plasma polymerization processes aiming to form amine groups on polystyrene surfaces were studied in-silico with molecular dynamics simulations. The simulations were compared with two experiments, (i) plasma treatment in N ₂/H ₂ bipolar pulsed discharge and (ii) plasma polymerization in cyclopropylamine/Ar radio frequency (RF) capacitively coupled discharge. To model favorable conditions for the incorporation of primary amine groups, we assumed the plasma treatment as the flux of NH ₂ radicals and energetic NH ₃ ions, and the plasma polymerization as the flux of cyclopropylamine molecules and energetic argon ions. It is shown in both the simulation and the experiment that the polystyrene treatment by the bipolar pulsed N ₂/H ₂ plasmas with an applied voltage of about ±1 kV formed a nitrogen-rich layer of a thickness of only a few nm. The simulations also showed that, as the NH ₃ incident energy increases, the ratio of primary amines to the total number of N atoms on the surface decreases. It is because the energetic ion bombardment brakes up N–H bonds of primary amines, which are mostly brought to the surface by NH ₂ radical adsorption. Our previous experimental work on the CPA plasma polymerization showed that increased RF power invested in the plasma leads to the deposition of films with lower nitrogen content. The MD simulations showed an increase of the nitrogen content with the Ar energy and a limited impact of the energetic bombardment on the retention of primary amines. Thus, the results highlighted the importance of the gas-phase processes on the nitrogen incorporation and primary amines retention in the plasma polymers. However, the higher energy flux towards the growing film clearly decreases amount of hydrogen and increases the polymer cross-linking.