Time-resolved OES of nanosecond pulsed discharges in N$_{2}$ and N$_{2}$/H$_{2}$O mixtures]{Time-resolved optical emission spectroscopy of nanosecond pulsed discharges in atmospheric pressure N$_{2}$ and N$_{2}$/H$_{2}$O mixtures
R. M. van der Horst, T. Verreycken, E. M. van Veldhuizen, P. J. Bruggeman
In this contribution, nanosecond pulsed discharges in N$_{2}$ and N$_{2}$/0.9% H$_{2}$O at atmospheric pressure (at 300 K) are studied with time-resolved imaging, optical emission spectroscopy and Rayleigh scattering. A 170 ns high voltage pulse is applied across two pin-shaped electrodes at a frequency of 1 kHz. The discharge consists of three phases: an ignition phase, a spark phase and a recombination phase. During the ignition phase the emission is mainly caused by molecular nitrogen (N$_{2}$(C-B)). In the spark and recombination phase mainly atomic nitrogen emission is observed. The emission when H$_{2}$O is added is very similar, except the small contribution of H$_α$ and the intensity of the molecular N$_{2}$(C-B) emission is less.
The plasma parameters such as electron distribution function and electron density of three atmospheric-pressure transient discharges namely filamentary and homogeneous dielectric barrier discharges in air, and the spark discharge of argon plasma coagulation (APC) system are determined. A combination of numerical simulation as well as diagnostic methods including current measurement and optical emission spectroscopy (OES) based on nitrogen emissions is used. The applied methods supplement each other and resolve problems, which arise when these methods are used individually. Nitrogen is used as …
In this work, evolution of parameters of nanosecond repetitively pulsed (NRP) discharges in pin-to-pin configuration in air was studied during transient stage of initial twenty discharge pulses. Gas and plasma parameters in the discharge gap were measured using coherent microwave scattering (CMS), optical emission spectroscopy (OES) and laser Rayleigh scattering (LRS) for NRP discharges at repetition frequencies of 1, 10 and 100 kHz. Memory effects (when perturbations induced by the previous discharge pulse would not decay fully till the subsequent pulse) were detected for the repetition frequ…
This work investigates the development of nanosecond pulsed discharges in water ignited with the application of both positive and negative polarity pulses to submerged pin to plane electrodes. Optical diagnostics are used to study two main aspects of these discharges: the initiation phase, and the development phase. Nanosecond pulses up to 24 kV with 4 ns rise time, 10 ns duration and 5 ns fall time are used to ignite discharges in a 1.5 mm gap between a copper plate and a tungsten needle with radius of curvature of 25 um. Fast ICCD imaging is used to trace the discharge development over varyi…
Dielectric barrier discharge (DBD) in air is characterized applying current measurement, numerical simulation and optical emission spectroscopy (OES). For OES, a non-calibrated spectrometer is used. This diagnostic method is applicable when cross-sectional area of the active plasma volume and current density can be determined. The nitrogen emission in the spectral range of 380 nm- 406 nm is used for OES diagnostics. Electric field in the active plasma volume is determined applying the measured spectrum, well-known Frank-Condon factors for nitrogen transitions and numerically- simulated electro…
In this work, we present an experimental study of nanosecond high-voltage discharges in a pin-to-pin electrode configuration at atmospheric conditions operating in single-pulse mode (no memory effects). Various discharge parameters, including voltage, current, gas density, rotational/vibrational/gas temperature, and electron number density, were measured. Several different measurement techniques were used, including microwave Rayleigh scattering, laser Rayleigh scattering, optical emission spectroscopy enhanced with a nanosecond probing pulse, fast photography, and electrical parameter measure…
In this work, the temporal decay of electrons produced by an atmospheric pin-to-pin nanosecond discharge operating in the spark regime was measured via a combination of microwave Rayleigh scattering (MRS) and laser Rayleigh scattering (LRS). Due to the initial energy deposition of the nanosecond pulse, a variance in local gas density occurs on the timescale of electron decay. Thus, the assumption of a constant collisional frequency is no longer applicable when electron number data is extracted from the MRS measurements. To recalibrate the MRS measurements throughout the electron decay period, …
This work presents an experimental study of a nanosecond repetitively pulsed dielectric barrier discharge interacting with a transient laminar flame propagating in a channel of height near the quenching distance of the flame. The discharge and the flame are of comparable size, and the discharge is favoured at a location where it is coupled with the reaction zone and burned gas. The primary goal is to determine how the discharge evolves on the time scale of the flame passage, with the evolution driven by the changing gas state produced by the moving flame front. This work complements the large …
The characteristics of atmospheric-pressure microdischarges excited by nanosecond high-voltage pulses are investigated in helium-nitrogen mixtures, as a function of the parameters of the excitation voltage pulses. In particular, cases of single-pulse excitation, unipolar and bipolar double-pulse excitation are studied, at different pulse durations, voltage amplitudes, and delay times (for the case of double-pulse excitation). Our investigations are carried out with a particle-simulation code that also comprises the treatment of the VUV resonance radiation in the plasma. The simulations allow g…
An influence of a high-voltage (3-17 kV) 20 ns pulse on a weakly-ionized low-pressure (0.1-10 Pa) capacitively-coupled radiofrequency (RF) argon plasma is studied experimentally. The plasma evolution after pulse exhibits two characteristic regimes: a bright flash, occurring within 100 ns after the pulse (when the discharge emission increases by 2-3 orders of magnitude over the steady-state level), and a dark phase, lasting a few hundreds μs (when the intensity of the discharge emission drops significantly below the steady-state level). The electron density increases during the flash and remain…
The focusing of a secondary shock wave was experimentally recorded during the implementation of an extended nanosecond high-current discharge of a cylindrical configuration in air. Using high-speed shadowgraph recording (up to 300 000 frames/s) of the emerging unsteady flow, cylindrically symmetric gas-dynamic discontinuities were visualized: a diverging shock wave moving from the discharge plasma boundary, a diverging contact discontinuity separating the shock-heated gas from the nonequilibrium region excited by the discharge plasma, and also a converging compression wave (secondary shock wav…
CO$_2$ dissociation stimulated by vibrational excitation in non-equilibrium discharges has drawn lots of attention. Ns-discharges are known for their highly non-equilibrium conditions. It is therefore of interest to investigate the CO$_2$ excitation in such discharges. In this paper, we demonstrate the ability for monitoring the time evolution of CO$_2$ ro-vibrational excitation with a well-selected wavelength window around 2289.0 cm$^{-1}$ and a single CW quantum cascade laser (QCL) with both high accuracy and temporal resolution. The rotational and vibrational temperatures for both the symme…
The plasma dry reforming reaction of methane with carbon dioxide is investigated in a nanosecond repetitively pulsed discharge, a type of plasma that offers one of the highest non-equilibrium and performance characteristics. The experiment's purpose was to examine the effect of varying the sequence of high-voltage pulses for the same plasma energy. We find that when successive pulses are closer than 500 $\rm μ$s, a memory-dominated regime gradually develops, which influences subsequent breakdown events. As a result, both a higher reactant conversion and more efficient use of the energy injecte…
The process of electron multiplication through the bouncing-like accelerated motion of electrons inside nanovoids formed owing to external electric fields in bulk liquid water is investigated using Monte Carlo simulations in Geant4-DNA. Our results show that the initial charge developed at the metal/liquid interface can be multiplied and expanded along the direction of the external electric field on a picosecond timescale, owing to collision-free interiors of the nanoruptures. Characteristic features of two different electron multiplication mechanisms are revealed and characterized. We find th…
The efficiency of the conversion of CO$_2$ into CO with nanosecond repetitively pulsed discharges (NRP) is investigated in a high pressure batch reactor. Stable discharges are obtained at up to 12~bar. By-products of CO$_2$ splitting are measured with gas chromatography. The energy efficiency is determined for a range of processing times, pulse energy, and fill pressures. The energy efficiency is found to be approximately 20% and is only weakly sensitive to the plasma operating parameters, i.e., the extent of CO$_2$ conversion is almost linearly-dependent on the specific energy input. A conver…
Electron temperature for inductively RF post-discharge of pure neon (Ne) with a newly reactor design was presented in comparison for two different methods. Optical emission spectroscopy (OES) was applied for characterizations of inductively RF Ne plasma at pressures between 0.17mbar and 1.4mbar for newly reactor type. Discharge and post-discharge were generated with an RF power supply at a frequency of 13.56MHz and output powers of 100, 160 and 200W. Spectra were evaluated in the range 200-1200nm by an optical spectrometer. At low pressure, the main spectral features reported were the waveleng…
Spatiotemporal dynamics of nanosecond pulsed discharge in the form of a fast ionization wave: self-consistent two-dimensional modeling and comparison with experiments under negative and positive polarity
Laboratory of Plasma Physics (CNRS, Ecole Polytechnique, Univ. Paris-Sud, Observatoire de Paris, Sorbonne Université, l’Institut Polytechnique de Paris), Ecole Polytechnique（等离子体物理实验室（法国国家科学研究中心、巴黎综合理工学院、巴黎南大学、巴黎天文台、索邦大学、巴黎理工学院），巴黎综合理工学院）
We report first ns-resolved absorption measurements of the ro-vibrational excitation of CO$_2$. The high temporal resolution of 8 ns is made possible by a fast detector (rise-time 5 ns), sensitive in the mid-infrared region. The resolution is achieved by a slow temperature scan of a quantum cascade laser and a segmented data capturing scheme. A repetitively pulsed ns discharge in 10% CO$_2$ + 90% He at 150 mbar and a repetition rate of 2 kHz is investigated. The evolution of the population densities of the different vibration modes as well as the associated vibrational and rotational temperatu…
We investigate the development of meter long negative discharges and focus on their X-ray emissions. We describe appearance, timing and spatial distribution of the X-rays. They appear in bursts of nanosecond duration mostly in the cathode area. The spectrum can be characterized by an exponential function with 200 keV characteristic photon energy. With nanosecond-fast photography we took detailed images of the pre-breakdown phenomena during the time when X-rays were registered. We found bipolar discharge structures, also called "pilot systems", in the vicinity of the cathode. As in our previous…
We present a novel microplasma flow reactor using a dielectric barrier discharge (DBD) driven by repetitively nanosecond high-voltage pulses. Our DBD-based geometry can generate a non-thermal plasma discharge at atmospheric pressure and below in a regular pattern of micro-channels. This reactor can work continuously up to about 100 minutes in air, depending on pulse repetition rate and operating pressure. We here present the geometry and the main characteristics of the reactor. Pulse energies of 1.9 $μ$J and 2.7 $μ$J per channel at atmospheric pressure and 50 mbar, respectively, have been dete…
To optimize the adhesion of layers presenting strong barrier properties on low-density polyethylene (LDPE) surfaces, we investigated the influence of argon and argon-oxygen atmospheric pressure post-discharges. This study was performed using x-ray photoelectron spectroscopy, atomic force microscopy, optical emission spectroscopy (OES) and dynamic water contact angle (WCA) measurements. After the plasma treatment, a slight increase in the roughness was emphasized, more particularly for the samples treated in a post-discharge supplied in oxygen. Measurements of the surface roughness and of the o…
Nanosecond plasmas in liquids are being used for water treatment, electrolysis or biomedical applications. The exact nature of these very dynamic plasmas and most important their ignition physics are strongly debated. The ignition itself may be explained by two competing hypothesis: (i) ignition via field effects or (ii) via electron multiplication in nanovoids. Both hypothesis are supported by theory, but experimental data are very sparse due to the difficulty to monitor the very fast processes in space and time. In this paper, we are using fast camera measurements and fast emission spectrosc…
The formation of the electron energy distribution function in nanosecond atmospheric nitrogen discharges is investigated by means of self-consistent solution of the chemical kinetics and the Boltzmann equation for free electrons. The post-discharge phase is followed to few microseconds. The model is formulated in order to investigate the role of the cross section set, focusing on the vibrational-excitation by electron-impact through resonant channel. Four different cross section sets are considered, one based on internally consistent vibrational-excitation calculations which extend to the whol…
Paper presents a review of modern works on the gasdynamic flow control using a heat release in highly nonequilibrium pulsed plasma. The major attention is paid to the effects based on ultrafast (on nanosecond time scale at atmospheric pressure) local heating of the gas, since at present the main successes in high-speed flow control using gas discharges are associated with namely this thermal effect. The physical mechanisms that control the interaction of the discharges with gas flows are considered in detail. The first part of the review briefly describes the most popular approaches in plasma …
Experimental characterization and comparison of the temporal features of plasma produced by ultrafast (100 fs, 800 nm) and short-pulse (7ns, 1064 nm) laser pulses from a high purity nickel and zinc targets, expanding into a nitrogen background, are presented. The experiment is carried out under a wide pressure range of 10^-6 to 10^2 Torr, where the plume intensity is found to increase rapidly when the pressure approaches 1 Torr. Electron temperature (Te) is calculated from OES and is found to be independent of pressure for ultrafast excitation, whereas an enhancement in Te is observed around m…
The Maxwell time is a typical time scale for the screening of an electric field in a medium with a given conductivity. We introduce a generalization of the Maxwell time that is valid for gas discharges: the \emph{ionization screening time}, that takes the growth of the conductivity due to impact ionization into account. We present an analytic estimate for this time scale, assuming a planar geometry, and evaluate its accuracy by comparing with numerical simulations in 1D and 3D. We investigate the minimum plasma density required to prevent the growth of streamers with local field enhancement, a…
Nanosecond Surface Dielectric Barrier Discharge (ns-SDBDs) are a class of plasma actuators that utilize a high-voltage pulse of nanosecond duration between two surface-mounted electrodes to create an electrical breakdown of air, along with rapid heating. These actuators usually produce multiple filaments when operated at high pulse frequencies, and the rapid heating leads to the formation of shock waves and complex flow fields. In this work we replicate a single filament of the ns-SDBDs and characterize the induced flow using velocity measurements from particle image velocimetry and density me…
In this study we have studied the initial stage of the nanosecond-pulsed discharge development in liquid phase. Modeling predicts that in the case of fast rising strong nonhomogeneous electric fields in the vicinity of high voltage pin electrode a region saturated with nanoscale non-uniformities may be developed. This phenomenon is attributed to the electrostriction mechanisms and may be used to explain development of breakdown in liquid phase. In this work, schlieren method was used in order to demonstrate formation of negative pressure region in liquids with different dielectric permittivity…
Atmospheric-pressure microdischarges excited by nanosecond high-voltage pulses are investigated in helium-nitrogen mixtures by first-principles particle-based simulations that include VUV resonance radiation transport via tracing photon trajectories. The VUV photons, of which the frequency redistribution in emission processes is included in some detail, are found to modify remarkably the computed discharge characteristics due to their ability to induce electron emission from the cathode surface. The electrons created this way enhance the plasma density and a significant increase of the transie…
We report on time-resolved measurements of electron number density by continuous-wave laser absorption in a low-energy nanosecond-scale laser-produced spark in atmospheric pressure air. Laser absorption is a result of free-free and bound-free electron excitation, with the absorption coefficient modeled and evaluated using estimates of the time-variation in electron temperature and probe laser absorption path length. Plasma electron number densities are determined to be as high as $n_\text{e}=7\times10^{19}$ cm$^{-3}$, and decay to $1/e$ of their peak values over a period of about 50 ns followi…
The effects of nanosecond pulsed non-equilibrium plasma discharges on ignition characteristics and low-temperature chemistry or LTC of DME/O2/Ar mixtures are numerically investigated in a plane-to-plane geometry at a reduced pressure of 76 Torr. Detailed numerical investigations of the two-stage ignition process in different temperature regimes of DME have been created through a high-fidelity one-dimensional, multi-timescale plasma-discharge model. Two different initial temperatures are set for comparison: 550K, the negative temperature coefficient regime, where LTC plays a dominate role; 800K…
In a DC point-to-plane corona discharge reactor, the mono filamentary streamers cross the inter electrode gap with a natural repetition frequency of some tens of kHz. The discharge phase (including the primary and the secondary streamers development) lasts only some hundred of nanoseconds while the post-discharge phases occurring between two successive discharge phases last some tens of microseconds. From the point of view of chemical activation, the discharge phases create radical and excited species located inside the very thin discharge filaments while during the post-discharge phases these…
Electron dynamics in planar radio frequency magnetron plasmas: III. Comparison of experimental investigations of power absorption dynamics to simulation results
In order to optimize the parameters of the plasma plume for atmospheric pressure plasma applications such as biological and industrial applications, it is highly necessary to thoroughly understand its characteristics. In this paper, various diagnostic techniques are discussed to characterize the atmospheric pressure plasma plume. The major emphasis of this work is to utilize possibly simple methods, low complexity in post data analysis and obtain in-situ information. The parameters of the plasma plume such as spatial variation of gas temperature, electron excitation temperature, plume velocity…
The understanding of the ro-vibrational dynamics in molecular (near)-atmospheric pressure plasmas is essential to investigate the influence of vibrational excited molecules on the discharge properties. In a companion paper, results of ro-vibrational coherent anti-Stokes Raman scattering (CARS) measurements for a nanosecond pulsed plasma jet consisting of two conducting molybdenum electrodes with a gap of 1 mm in nitrogen at 200 mbar are presented. Here, those results are discussed and compared to theoretical predictions based on rate coefficients for the relevant processes found in the literat…
Proof of operation of a micro-hollow cathode discharge driven by a true ns-pulsed high voltage: emission properties and atomic nitrogen production
Laboratoire des Sciences des Procédés et des Matériaux (LSPM), CNRS, Université Sorbonne Paris Nord（材料过程与科学实验室，法国国家科学研究中心，索邦巴黎北大学）；Laboratoire Energétique Moléculaire et Macroscopique, Combustion (EM2C), CNRS, Université Paris Saclay（分子与宏观能量、燃烧实验室，法国国家科学研究中心，巴黎萨克雷大学）
In this work, solid targets made from boron and boron nitride (BN) materials are ablated by a nanosecond pulsed laser at sub-atmospheric pressures of nitrogen and helium gases. Excited species in the ablation plume from the target are probed with spatiotemporally resolved optical emission spectroscopy (OES). Evaluation of chemical composition in the plasma plume revealed that for both boron-rich targets, emission from BN molecules is always observed in nitrogen-rich environments. In addition, BN molecules also present when ablating a boron nitride target in helium gas -- an indication that BN …
