Optical Emission Imaging Research Articles

Hydrogen peroxide production of underwater nanosecond-pulsed streamer discharges with respect to pulse parameters and associated discharge characteristics

Pulsed streamer discharges submerged in water have demonstrated potential in a number of applications. Especially the generation of discharges by short high-voltage pulses in the nanosecond range has been found to offer advantages with respect to efficacies and efficiencies. The exploited plasma chemistry generally relies on the initial production of short-lived species, e.g. hydroxyl radicals. Since the diagnostic of these transient species is not readily possible, a quantification of hydrogen peroxide provides an adequate assessment of underlying reactions. These conceivably depend on the characteristics of the high-voltage pulses, such as pulse duration, pulse amplitude, as well as pulse steepness.A novel electrochemical flow-injection system was used to relate these parameters to hydrogen peroxide concentrations. Accordingly, the accumulated hydrogen peroxide production for streamer discharges ignited in deionized water was investigated for pulse durations of 100 ns and 300 ns, pulse amplitudes between 54 kV and 64 kV, and pulse rise times from 16 ns to 31 ns. An independent control of the individual pulse parameters was enabled by providing the high-voltage pulses with a Blumlein line. Applied voltage, discharge current, optical light emission and time-integrated images were recorded for each individual discharge to determine dissipated energy, inception statistic, discharge expansion and the lifetime of a discharge.Pulse steepness did not affect the hydrogen peroxide production rate, but an increase in amplitude of 10 kV for 100 ns pulses nearly doubled the rate to (0.19 ± 0.01) mol l−1 s−1, which was overall the highest determined rate. The energy efficiency did not change with pulse amplitude, but was sensitive to pulse duration. Notably, production rate and efficiency doubled when the pulse duration decreased from 300 ns to 100 ns, resulting in the best peroxide production efficiency of (9.2 ± 0.9) g kWh−1. The detailed analysis revealed that the hydrogen peroxide production rate could be described by the energy dissipation in a representative single streamer. The production efficiency was affected by the corresponding discharge volume, which was comprised by the collective volume of all filaments. Hence, dissipating more energy in a filament resulted in an increased production rate, while increasing the relative volume of the discharge compared to its propagation time increased the energy efficiency.

Conventional and non-conventional diagnostics of a stable atmospheric pressure DC normal glow microplasma discharge intended for in situ TEM studies

A simple setup utilizing parallel flat electrodes with a 50–150 μm interelectrode distance divided by a Kapton spacer with a 1 mm diameter whole as discharge region intended for in situ transmission electron microscope studies is presented. The rather small setup operated in Ar or He results in an atmospheric pressure DC normal glow discharge and is investigated using various diagnostics. I–V characteristics show a glow-like behavior of the microplasma. Significant differences due to the working gas, electrode material and electrode distance have been observed. Currents in the range of 0.5–3 mA resulted in electrode potentials of 140–190 V for most experimental conditions. Optical emission spectroscopy and imaging revealed stable plasma operation and enabled the determination of current densities (approx. 16 mA mm−2 for He, or 28 mA mm−2 for Ar) independent of the input current as the discharge channel grows in diameter. Sheath thicknesses in the range of a few μm have been calculated by the collision-dominated Child–Langmuir law and trends are confirmed by the optical imaging. Energy flux measurements revealed a pronounced effect of ions on the measurement process and resulted in high energy fluxes locally up to 275 W cm−2. Effective secondary electron emission coefficients ranging from 1 to 1.6 depending on the discharge conditions have been determined based on the energy balance at the cathode.

Optical Diagnostics during Pulsed Laser Ablation in Liquid (PLAL) for the Production of Metallic Nanoparticles

Pulsed laser ablation in liquid (PLAL) is gaining an important role as a methodology for producing nanostructures without the use of chemicals and stabilizers. Several nanomaterials have been produced and the engineering of PLAL is becoming an important task for the dissemination of this approach for nanostructure production. Monitoring the processes involved in the PLAL during nanostructure production can be extremely useful for improving the experimental methods and for pushing PLAL to new material formation. In this paper, we discuss the use of optical techniques for investigating the specific stages involved in the production of nanomaterials with PLAL. In particular, the recent advancements of these optical techniques for each specific stage of the PLAL process will be discussed: optical emission spectroscopy and imaging for the investigation of the plasma phase, shadowgraph imaging for the investigation of the cavitation bubble dynamics and different scattering techniques for the visualization of the produced nanostructure.

Analysis of Discharge Characteristics of Cold Atmospheric Pressure Plasma Jet

In this article, the investigation has been carried out for the characterization of the proposed tapered geometry of dielectric barrier discharge (DBD)-based cold atmospheric pressure plasma jet (C-APPJ) on the basis of optical emission spectroscopy (OES) and imaging for different operating parameters, such as argon gas flow rates, applied voltages, and frequencies. The detailed characteristics for the formation of the plasma plume using argon as a working gas have been presented for a wide range of flow rates [1–3 standard liter per minute (SLM)] and frequencies (15–25 kHz). Increasing the pulse frequency, the length and the diameter of the plasma plume increase, while the length of the plasma plume increases when increasing the gas flow rate up to 2 SLM. Time-integrated images have been captured using the intensified charge couple device (ICCD) camera, which illustrates that the plasma plume comprises different emission layers of definite patterns. The propagation dynamics and formation of different emission layers of the plasma plume have also been investigated using the COMSOL Multiphysics simulation. It has been observed that the local electric field of 6 kV/cm is responsible for the propagation of the plasma bullet and the generation of the electron with an average energy of ~9 eV. OES has also been performed to understand the plasma chemistry and identify the reactive species in the C-APPJ. The discharge analysis and characteristics performed through experiment and simulation would certainly be helpful for the design and development of C-APPJ sources.

Shock front behavior during pulsed laser ablation of graphite

Pulsed laser ablation of pyrolytic graphite with a 4-J / cm2 KrF laser in backgrounds of air, argon, nitrogen, and helium at pressures up to 10 Torr was performed to study the plume dynamics. Optical emission imaging with a 2-ns gated intensified charged-coupled device camera was used to determine shock front positions and plume trajectories for characterization by free expansion, Sedov–Taylor (ST) blast, and drag models. The plume expands with initial Mach numbers of M = 55, decreasing to M ∼ 20 as the emission becomes too weak to detect. The plumes begin with a planar shock front and thickness of a few mean free paths, but evolve to higher dimensionality, n, depending on pressure and mass of the background gas. The ST energy released in the sudden ablation is typically 33% the laser pulse energy. Blast energy and plume dimensionality are correlated with stopping distances, which are typically greater than 103 mean free paths. Upper bounds for the mass ablated (1 to 2 μg / pulse) and hole depth (∼88 to 183 nm) are inferred from the shock kinetic energy relative to laser pulse energy. The inferred hole depth ranges from 0.32 to 0.67 percent of the thermal diffusion length as the pressure increases from 1 to 10 Torr for these conditions where the fluence is just above twice the ablation threshold.

Dynamics of plasma streamers in a helium surface micro-discharge array at atmospheric pressure

The dynamic evolution of plasma optical emission from an array of surface micro-discharges has been investigated by optical emission imaging. The array was operated in helium at atmospheric pressure and driven at 2.0 W at a frequency of 30 kHz. The findings indicate that surface charges and external voltage have a significant contribution to the splitting of the plasma streamer, with luminous fronts moving at velocities of 8.3–22.4 km s−1. The split plasmas induce new discharge events within a single hexagonal cell. Furthemore, we present the case of two co- and counter-propagating streamers generated within one hexagon mesh element. Experimental evidence reveals that the co-propagating streamers merge and produce a new streamer front with enhanced intensity under the combined effects of electrostatic repulsion, gas dynamic interaction and a photolytic process. As the spacing between the counter-propagating streamers decreases, the streamers interact electrically, resulting in a modification of the shape of these streamers as well as a decrease in their velocities and emission intensities. The emergence of secondary streamers is also observed. This behavior is related to surface charges accumulated during a previous half cycle and their redistribution due to the turbulence fluctuations dominated by electrohydrodynamic force. From the propagation of an individual streamer, it is shown that surface charges accumulated in a previous negative half cycle can determine the plasma path to some extent. The ionization wave propagates over the rim electrode with a velocity of about 20 km s−1, resulting in a distinct discharge channel and a strong interaction between neighboring hexagonal units in an array. The ionization wave leads to the propagation of plasma across the dielectric surface of the array.

Diamond chemical vapor deposition using a zero-total gas flow environment

We demonstrate diamond growth through microwave plasma-enhanced chemical vapor deposition using a sealed (static-mode) CH4/H2 process gas mixture. The growth experiments were complemented by spatially and spectrally resolved optical emission imaging measurements of electronically excited C2 and CH radicals in the hot plasma core. The as-grown material was characterized by Raman Spectroscopy and Scanning Electron Microscopy and shown to be typical of polycrystalline diamond grown using traditional methods. Moreover, this material was essentially indistinguishable from material grown using a tracked flow-mode of operation in which the input methane flow rate was progressively reduced to mimic the time evolving C2 emission intensities in the static-mode experiments. These proving static-mode studies demonstrate a ~30-fold improvement (cf. that achieved using standard flow-mode conditions) in the conversion efficiency of carbon in the input source gas into diamond, and we argue that further gains should be possible with appropriate reactor and process optimization. Static-flow growth could be particularly advantageous in the case of depositions using limited, expensive, hazardous, or environmentally damaging feedstock gases.

How the Ligand Field in Lanthanide Coordination Complexes Determines Magnetic Susceptibility Anisotropy, Paramagnetic NMR Shift, and Relaxation Behavior.

ConspectusComplexes of lanthanide(III) ions are being actively studied because of their unique ground and excited state properties and the associated optical and magnetic behavior. In particular, they are used as emissive probes in optical spectroscopy and microscopy and as contrast agents in magnetic resonance imaging (MRI). However, the design of new complexes with specific optical and magnetic properties requires a thorough understanding of the correlation between molecular structure and electric and magnetic susceptibilities, as well as their anisotropies. The traditional Judd–Ofelt–Mason theory has failed to offer useful guidelines for systematic design of emissive lanthanide optical probes. Similarly, Bleaney’s theory of magnetic anisotropy and its modifications fail to provide accurate detail that permits new paramagnetic shift reagents to be designed rather than discovered.A key determinant of optical and magnetic behavior in f-element compounds is the ligand field, often considered as an electrostatic field at the lanthanide created by the ligands. The resulting energy level splitting is a sensitive function of several factors: the nature and polarizability of the whole ligand and its donor atoms; the geometric details of the coordination polyhedron; the presence and extent of solvent interactions; specific hydrogen bonding effects on donor atoms and the degree of supramolecular order in the system. The relative importance of these factors can vary widely for different lanthanide ions and ligands. For nuclear magnetic properties, it is both the ligand field splitting and the magnetic susceptibility tensor, notably its anisotropy, that determine paramagnetic shifts and nuclear relaxation enhancement.We review the factors that control the ligand field in lanthanide complexes and link these to aspects of their utility in magnetic resonance and optical emission spectroscopy and imaging. We examine recent progress in this area particularly in the theory of paramagnetic chemical shift and relaxation enhancement, where some long-neglected effects of zero-field splitting, magnetic susceptibility anisotropy, and spatial distribution of lanthanide tags have been accommodated in an elegant way.

Optical Emission Imaging and Modeling Investigations of Microwave-Activated SiH4/H2 and SiH4/CH4/H2 Plasmas

Silicon is a known trace contaminant in diamond grown by chemical vapor deposition (CVD) methods. Deliberately Si-doped diamond is currently attracting great interest because of the attractive optical properties of the negatively charged silicon-vacancy (SiV-) defect. This work reports in-depth studies of microwave activated H2 plasmas containing trace (10-100 ppm) amounts of SiH4, with and without a few % of CH4, operating at pressures and powers relevant for contemporary diamond CVD, using a combination of experiment (spatially resolved optical emission (OE) imaging) and two-dimensional plasma chemical modelling. Key features identified from analysis and modelling of the OE from electronically excited H, H2, Si, and SiH species in the dilute Si/H plasmas include (i) fast H-shifting reactions ensure that Si atoms are the most abundant silicon-containing species throughout the entire reactor volume, (ii) the low ionization potentials of all SiHx (x ≤ 4) species and efficient ion conversion reactions ensure that even trace SiH4 additions cause a change in the dominant ions in the plasma volume (from H3+ to SiHx+), with consequences for electron-ion recombination rates and ambipolar diffusion coefficients and (iii) the total silicon content in the reactor volume can be substantially perturbed by silicon deposition and H atom etching reactions at the reactor walls. The effects of adding trace amounts of SiH4 to a pre-existing C/H plasma are shown to be much less dramatic, but include (i) a Si substrate or fused silica components within the reactor is a ready (unintended) source of gas phase Si-containing species, (ii) OE from electronically excited Si atoms should provide a reliable measure of the Si content in the hot plasma region and (iii) Si atoms and/or SiC2 species are the most abundant gas phase Si-containing species just above the growing diamond surface and thus the most likely carriers of the silicon incorporated into CVD diamond.

Spectral measurements of inductively coupled and m = +1, −1 helicon discharge modes of the constructed plasma source

In the present context, the industrial type of Amirkabir helicon plasma source has been introduced that was designed and constructed at the Helicon Plasma Laboratory of Amirkabir University of Technology with the aim of using it in material processing applications. Helicon plasma in two m = +1 and m = −1 modes of operation was studied, and also its application was compared with the inductively coupled plasma (ICP) mode in this experimental work. This study was performed by employing two techniques including optical emission spectroscopy and imaging using a camera with polarizing filters, in which the images and spectra of ICP and m = +1, −1 helicon plasma modes were recorded under the experimental conditions. The effects of the device operational parameters on the argon plasma emission spectra were investigated in the wavelength range of 350–950 nm. It was observed from the comparison of the plasma spectra that the ionization rate increases significantly for the plasma helicon mode than ICP and also for m = +1 helicon mode of operation than m = −1. In this work, the values of device operational parameters such as the RF power delivered to the half-helix antenna, external magnetic field intensity, and the injected gas flow rate were varied in the range of 400–900 W, 100–300 mT, and 1–10 SCCM in the experiment, respectively. In addition, the optimum values of RF power, magnetic field intensity, and the injected gas flow rate for achieving the maximum ionization rate were, respectively, obtained as 900 W, 300 mT, and 3 SCCM.

The Structure of the Orion Nebula in the Direction of θ1 Ori C

Abstract We have used existing optical emission and absorption lines, [C ii] emission lines, and H i absorption lines to create a new model for a central column of material near the Trapezium region of the Orion Nebula. This was necessary because recent high spectral resolution spectra of optical emission lines and imaging spectra in the [C ii] 158 μm line have shown that there are new velocity systems associated with the foreground Veil and the material lying between θ 1 Ori C and the main ionization front of the nebula. When a family of models generated with the spectral synthesis code Cloudy were compared with the surface brightness of the emission lines and strengths of the Veil absorption lines seen in the Trapezium stars, distances from θ 1 Ori C were derived, with the closest, highest ionization layer being 1.3 pc. The line-of-sight distance of this layer is comparable with the size of the inner Huygens region in the plane of the sky. These layers are all blueshifted with respect to the Orion Nebula Cluster of stars, probably because of the pressure of a hot central bubble created by θ 1 Ori C's stellar wind. We find velocity components that are ascribed to both sides of this bubble. Our analysis shows that the foreground [C ii] 158 μm emission is part of a previously identified layer that forms a portion of a recently discovered expanding shell of material covering most of the larger Extended Orion Nebula.

Combined Spatially Resolved Optical Emission Imaging and Modeling Studies of Microwave-Activated H2/Ar and H2/Kr Plasmas Operating at Powers and Pressures Relevant for Diamond Chemical Vapor Deposition.

Microwave (MW) activated H2/Ar (and H2/Kr) plasmas operating under powers and pressures relevant to diamond chemical vapor deposition have been investigated experimentally and by 2-D modeling. The experiments return spatially and wavelength resolved optical emission spectra of electronically excited H2 molecules and H and Ar(/Kr) atoms for a range of H2/noble gas mixing ratios. The self-consistent 2-D( r, z) modeling of different H2/Ar gas mixtures includes calculations of the MW electromagnetic fields, the plasma chemistry and electron kinetics, heat and species transfer and gas-surface interactions. Comparison with the trends revealed by the spatially resolved optical emission measurements and their variations with changes in process conditions help guide identification and refinement of the dominant plasma (and plasma emission) generation mechanisms and the more important Ar-H, Ar-H2, and H-H2 coupling reactions. Noble gas addition is shown to encourage radial expansion of the plasma, and thus to improve the uniformity of the H atom concentration and the gas temperature just above the substrate. Noble gas addition in the current experiments is also found to enhance (unwanted) sputtering of the copper base plate of the reactor; the experimentally observed increase in gas phase Cu* emission is shown to correlate with the near substrate ArH+ (and KrH+) ion concentrations returned by the modeling, rather than with the relatively more abundant H3+ (and H3O+) ions.

Wavelength-dependent variations of the electron characteristics in laser-induced plasmas: A combined hydrodynamic and adiabatic expansion modelling and time-gated, optical emission imaging study

The spatial and temporal evolution of the absolute electron densities and temperatures in plasmas formed by nanosecond pulsed laser ablation of silicon in vacuum at two wavelengths (1064 and 532 nm), at similar irradiances, have been explored by complementary simulation (using combined hydrodynamic and adiabatic models) and experiment. Modelling the laser-target and laser-plume interactions with the POLLUX code reveals the evolving composition and dynamics of the laser induced plasma (LIP) during the incident laser pulse: 532 nm irradiation causes more ablation, but the LIP formed by 1064 nm excitation has a higher average charge state and expands faster. The experimental data, from the analysis of Stark broadened line shapes of SiIII and SiIV cations in time-gated, position- and wavelength-resolved images of the plume emission, allow characterisation of the plume dynamics at later times. These dynamics are compared with predictions from two forms of adiabatic expansion model. Both take as input parameters the plume properties returned by the POLLUX simulations for the end of the laser pulse, but differ according to whether the initial plasma is assumed isothermal or isentropic. The study illustrates the important λ-dependences of the target absorption coefficient (in establishing the ablated material density) and of electron–ion inverse bremsstrahlung absorption (in coupling laser radiation into the emergent plasma); the extents to which these interactions, the relative ablation yields, and the plume expansion dynamics depend on λ; and the importance of identifying appropriate initial conditions for adiabatic expansion modelling of LIP in vacuum.

Propeller arc: design and basic characteristics

A new atmospheric pressure non-equilibrium plasma source named the ‘Propeller Arc’ (PA) is developed using the concept of rotating electrodes. The PA device consists of a rotating cathode, driven by a motor, with one or more fixed anodes. Plasma is ignited at or near the narrowest gap as the rotating cathode passes by the anode and then it is extended up to a length of ∼66 mm or longer depending on the supplied power. This allows for efficient ignition, followed by a quick increase in plasma volume. The PA is similar to the widely used gliding arc (GA); however, unlike the GA, PA does not require imposed gas flow, and the PA discharge frequency can be easily controlled by the motor angular velocity. In this paper, the basic characteristics of PA are investigated using two different operation modes: pulse modulation and DC power. Discharge properties including electrical characteristics, time-resolved optical emission images, plasma electrical properties such as resistance and average electric field (discharge voltage divided by gap distance) and plasma power consumption are reported. Use of multiple anodes to increase the plasma volume is also demonstrated. As the PA has a compact design and is relatively easy to stabilize and control without the need for applied gas flow, it has potential to be adapted for many different applications such as nitrogen fixation, fuel and carbon dioxide conversion, waste, odor and hydrogen sulfide treatment, etc.

Phase-resolved optical emission spectroscopy of a transient plasma created by a low-pressure dielectric barrier discharge jet

A transient plasma created by a low-pressure dielectric-barrier discharge operated with argon was investigated by means of optical emission spectroscopy and imaging. Images of the discharge and emission spectra were recorded with sub-phase resolution and relative densities of excited argon states were obtained. Profiles of densities and electron temperatures were evaluated for the discharge cycle by comparison with results of a collisional-radiative model (CRM). To overcome difficulties in sub-cycle modelling of the important argon 1s states, a combination of the CRM with a density estimation based on radiation-trapping is proposed. Absolute densities of all four 1s states were measured and additionally verified by tunable laser absorption spectroscopy. The presented combination may help to improve optical diagnostics of rare gas plasmas in cases were the dominating processes for the 1s states are not known with sufficient accuracy.

Study of the Effect of Water Pressure on Plasma and Cavitation Bubble Induced by Pulsed Laser Ablation in Liquid of Silver and Missed Variations of Observable Nanoparticle Features.

In this work the effects of the pressure between 1-150 Bar on pulsed laser ablation in liquids (PLAL) during the production of silver nanoparticles (AgNPs) in water was investigated. The produced NPs are the results of two different well-known stages which are the plasma and the bubble evolution occurring until the generated material is released into the solution. The main aim of this work is to show which roles is played by the variation of water pressure on the laser induced plasma and the cavitation bubble dynamics during the NPs formation. Their implication on the comprehension of the as-produced NPs formation mechanisms is treated. The typical timescales of the different stages occurring in water at different pressures have been studied by optical emission spectroscopy (OES), imaging and shadowgraph experiments. Finally surface plasmon resonance (SPR) spectroscopy, transmission electron microscopy (TEM), dynamic light scattering (DLS) and scanning electron microscopy (SEM) for characterization of the material released in solution, have been used.

Time- and space-resolved spectroscopic characterization of laser-induced swine muscle tissue plasma

The spatial-temporal evolution of muscle tissue sample plasma induced by a high-power transversely excited atmospheric (TEA) CO2 pulsed laser at vacuum conditions (0.1–0.01Pa) has been investigated using high-resolution optical emission spectroscopy (OES) and imaging methods. The induced plasma shows mainly electronically excited neutral Na, K, C, Mg, H, Ca, N and O atoms, ionized C+, C2+, C3+, Mg+, Mg2+, N+, N2+, Ca+, O+ and O2+ species and molecular band systems of CN(B2Σ+–X2Σ+), C2(d3Πg–a3Πu), CH(B2Σ−–X2Π; A2Δ–X2Π), NH(A3Π–X3Σ−), OH(A2Σ+–X2 Σ+), and CaOH(B2Σ+–X2Σ+; A2Π–X2Σ+). Time-resolved two-dimensional emission spectroscopy is used to study the expanded distribution of different species ejected during ablation. Spatial and temporal variations of different atoms and ionic excited species are reported. Plasma parameters such as electron density and temperature were measured from the spatio-temporal analysis of different species. Average velocities of some plasma species were estimated.

Time-resolved optical emission imaging of an atmospheric plasma jet for different electrode positions with a constant electrode gap

The aim of this paper is to determine the influence of the position of the electrodes on the range of a plasma jet, for specific experimental conditions, by using time-resolved optical emission spectroscopy. The optimal position of the electrodes is determined for a fixed gas flow rate and applied excitation voltage. We characterize the helium plasma jet for different distances from the end of the glass tube, showing detailed results for four different electrode positions from the jet nozzle (7, 15, 30 and 50 mm). It was found that at the distance of 15 mm, the length of the plasma jet is at its maximum. The highest speeds of the plasma package travelling outside the glass tube of the atmospheric plasma jet are obtained for the same electrode configuration (15 mm from the jet nozzle). With the electrodes positioned at smaller distances from the nozzle, the plasma plume was much shorter, and at the larger distances the plasma did not even leave the glass tube.

Atmospheric Pressure Plasma Penetration inside Flexible Polymeric Tubes

An atmospheric argon plasma jet has been used to explore the plasma penetration inside tubes of small diameter and the plasma treatment effect on the inner tube surface. The goal of this paper is to show how the tube size can influence the plasma jet penetration and the resulting surface effects on polyethylene tubes with diameters varying between 0.28 mm and 3.00 mm. Optical emission spectroscopy and light emission images have been used to investigate the distribution of active species along the tube length. To examine the plasma treatment effect on the inner tube surface, capillary action, water contact angle measurements and XPS analysis have been used. The results presented in this paper will clearly demonstrate the great potential of atmospheric pressure plasma jets for inner tube surface modification.

Spectroscopic characterization and imaging of laser- and unipolar arc-induced plasmas

Tungsten plasmas induced by unipolar arcs were investigated using optical emission spectroscopy and imaging, and compared with laser-induced tungsten plasmas. The unipolar arcs were initiated in the linear-plasma simulator PISCES-A at UCSD under fusion relevant conditions. The electron temperature and density of the unipolar arc plasmas were in the range 0.5–0.7 eV and 0.7–2.0 × 1020 m−3, respectively, and increased with increasing negative bias voltage, but did not correlate with the surface temperature. In comparison, the electron temperature and density of the laser-induced plasmas were in the range 0.6–1.4 eV and 7 × 1019–1 × 1022 m−3, respectively.