Chapter 1 Final
Chapter 1 Final
Chapter 1 Final
CHAPTER 1
INTRODUCTION
Chapter 1: Introduction
Chapter 1: Introduction
Most recently the DBD technology opened possible emerging novel applications in biology and
medical field [16, 17]. Also, the ultraviolet (UV) and vacuum ultraviolet (VUV) sources based
on DBD emerged as a superior tool for many industrial applications [18]. The mercury based
UV/VUV sources have excellent efficiency but also have one major drawback. The
decomposition of mercury in air or water can cause serious health problems and also
environmental pollution. Efforts are going on worldwide to find the alternatives for the mercury
free light sources. Very recently, a new generation of lamps has been developed based on
excimer radiations that are capable of producing efficient UV to deep UV light radiations [19
22].
The DBD based excimers are the best alternative for the generation of UV/VUV radiation either
with rare gases or with rare gas mixture of halogens [23-25]. It is well known that the excimers,
which are unstable excited molecular complexes, are generated in a number of ways, e.g., by
dielectric barrier discharges, high-energy electron beams, x-rays, synchrotron radiations, protons,
heavy ions and microwave discharges [24,26]. The DBD plasmas are used as effective sources of
the excited dimmer which terminates to the unbound or weakly bound metastable states and
leads to generate VUV/UV or visible light radiations effectively [24-25]. This is one of the most
proficient ways to produce the necessary precursor for formation of excimers because DBDs
have ability of producing high energetic electrons and excited dimmers at high pressures [27].
Furthermore, the DBD plasmas have potential adoptability for industrial applications because of
their simplicity or the geometric freedom, high efficiency, low cost, etc. [28].
The UV/VUV radiation dynamics from DBD driven excilamp was experimentally studied for the
first time by Lomaev et al. [23]. In earlier days the disadvantage of DBDs was that the UV
radiation generation was characterized only by 10-15% electrical to optical convergence
efficiency. However, Vollkommer and Hitzhschke [29] solved certain basic hindrances and
improved the efficiency. The new configuration led to develop Xeradex source as shown in Fig.
1.1 with efficiency as maximum as 40% in converting electrical energy into ultraviolet radiation
at wavelength 172 nm during the glow discharge.
Chapter 1: Introduction
Fig. 1.1. Osram Xeradex 20 excimer light source emitting 172 nm of wavelength [30]
These new types of mercury free light sources are highly applicable for the medical applications.
Galina Matafonova and Valeriy Batoev published a review article on recent advances on
excilamps in 2012 [31] and described detail applications of excilamps in microbial inactivation
by direct UV treatment. There is existence of many applications related to the use of DBD in
medicines and biology [32-37]. Fridman et al. [34] demonstrated that without any visible or
microscopic damage to the skin tissues the blood-clot formation in seconds is possible by the
direct treatment using floating electrode DBD air plasma. This discharge configuration used in
the treatment of living tissues and is shown in Fig. 1.2.
(a)
(b)
4
Chapter 1: Introduction
Fig. 1.3. UVB treatment at wavelength 308 nm (a) Before, (b) After [38]
The effect of XeBr*, KrCl*, and KrClKrBr* excilamps on five microbiological cultures have
also been compared [39,40]. Matafonova et al. in 2008 have observed that rapid inactivation of
bacteria happens while KrCl* excilamp with 222 nm wavelength [41]. They further showed that
the Escherichia coli (E-coli) and Staphylococcus aureus (S-aureus) bacteria are the most
sensitive at this wavelength and 100% deactivation of these bacteria occurred in couple of tens of
seconds. Moreover, the XeBr* excilamp (289nm) provided the higher inactivation efficiency for
E. coli and Pseudomonas aeruginosa [42] as compared to the mercury-lamp. Fig. 1.4 illustrates
the flow chart for associated physical and chemical components of DBD along with most
prominent applications. The discharge physics and plasma chemistry play important role in
deciding the specific application that still requires many researches.
PLAS
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Fig. 1.4. Flow chart involving DBD applications
This dissertation involves the augmentation of DBD discharge physics understanding and to
leverage it for the development of an efficient DBD based VUV/UV excimer light source with
practical applications. However, the performance of DBD plasma depends on the treatment time
for a definite applied voltage in a specific electrode geometry and discharge arrangement. A
homogeneous discharge is advantageous than a filamentary discharge in most DBD plasma
applications. The homogeneous or diffused discharge offers uniform radiations in indirect
5
Chapter 1: Introduction
treatment and also delivery of active species uniformly in direct treatment and have better control
over physical and chemical changes. There is the number of ways by which the discharge
parameters of a homogeneous discharge can be controlled [4346]. To have better understanding,
the classification of DBDs along with discharge mechanism understanding is most important.
(a)
Chapter 1: Introduction
(b)
Fig. 1.5. Image of discharge in parallel plate DBD (a) filamentary discharge (b) Diffused
discharge
The filamentary mode operation consists of thin plasma channels stochastically distributed in
the gas gap between the working electrodes. These microdischarges are several tens of microns
in diameter and last for several tens of nanoseconds. On the other hand homogeneous discharge
fills the entire gap with practically uniform plasma. Filamentary DBDs are less used in surface
and plasma radiation processing because of the non-uniform plasma interactions, so the real
challenge was to get diffused discharge at atmospheric/sub-atmospheric pressure operation of
DBDs. Diffused DBD under atmospheric pressure was first reported by Kanazawa et al. in 1988
[48]. They found that the discharge current waveform of the diffused DBD is one discharge pulse
(about 1 s) per half-cycle of the applied voltage, while the filamentary DBD consists of many
short-lived pulses (about 10 ns) per half-cycle [49,50].
It is reported that for the different gases and mixture of the gases, DBD is filamentary in
nature at atmospheric pressure discharge operations and diffusive at sub-atmospheric pressure
discharge operations [51]. The controlling of the mean energy of the electron with the variation
of the external parameters such as geometry and type of dielectric used also play an important
role in diffused discharge operation of the DBDs [27]. Accordingly, the operating pressure, the
inter-electrode gap (geometry) and the type of the dielectric play important role to influence the
spectral characteristics. Hence depending on the application, specific requirement for DBD have
led to use the different configurations.
The DBDs are mainly classified in three basic configurations: the volume discharge, (VD)
surface discharge (SD) and coplanar discharge (CD) arrangements [52]. Fig. 1.6 illustrates
the different configurations arrangement of DBDs. Fig. 1.6 (a-d) describe the volume discharge
arrangement, Fig. 1.6(e) shows the surface discharge and Fig. 1.6(f) depicts the coplanar
discharge which is the combination of surface discharge and the planer discharge arrangements.
Chapter 1: Introduction
The VD arrangement of the DBD consists of two parallel electrodes in which either one or
both electrodes are covered by the dielectric layer. The discharge is executed in a gas gap
between two parallel plates or concentric cylindrical electrodes covered by the dielectrics. The
discharge occurs in the form of mcirodischarges or filaments, which are distributed in the gas
gap between the electrodes. The SD arrangement consists of number of surface electrodes on the
dielectric layer and a counter electrode on its reverse side. It means one electrode is exposed to
the air and the other is covered by the dielectric material. There is no clearly defined discharge
gap in this case. The microdischarges are, in this case, rather individual discharge channels that
occur in a thin layer on the dielectric surface and can be considered homogenous over a definite
distance.
(b)
(a)
(d)
(c)
Chapter 1: Introduction
(e)
(f)
Fig. 1.6. Schematic view of different DBD configurations
The plasma actuator is the one of best example for SD arrangement of DBDs [52]. The CD
arrangement is characterized by pairs of long parallel electrodes with opposite polarity. The
discharge occurs in the gas gap and on the surface of the dielectric. Typical gas spaces vary from
several tens of micrometers to several centimeters. The CD arrangement is the combination of
two configurations. It is characterized by the pairs of electrodes of opposite polarity situated
within the bulk of the dielectric as shown in Fig. 1.6(f).
The VD arrangement of DBD has been investigated by several researchers whereas the
investigations of SDs are rare [54, 55]. The efficiency of SDs is lower than that of VDs and
perhaps this is the reason. So, the volume discharge configuration in the DBDs is the appropriate
choice to study the discharge behavior of the DBDs. Hence VD configuration of the DBD has
been considered in the present research work.
It is to be mentioned that the most influencing factors to the efficiency of the DBDs is
dielectric material [56]. The choice of the dielectric material is based on the good insulating
material properties so as to sustain the high voltage stresses and also have small loss angle. The
most preferred dielectric materials are glass, quartz and alumina (ceramics) albeit the choice of
dielectric material depends on the specific application. Shape of electrodes is also useful
parameters in term of efficiency enhancement. The most used forms are planar or cylindrical but
metal plate, metal grid, or narrow metal strips can also be used.
Chapter 1: Introduction
A basic VD configuration of DBD as shown in Fig. 1.6(c) has been considered to understand the
discharge phenomena of the DBDs. At initial stage many microdischarges occurs in the discharge
region. In fact, when a dielectric barrier layer is placed in front of the electrodes [57] and high
voltage is applied between the two electrodes, it limits the discharge current but streamers are
formed. To understand it more clearly, when the applied high voltage kept remains constant, the
charges from plasma accumulates on the dielectric surface which are basically wall charges (Fig.
1.7) and these reduce the effective electric field inside the discharge gap leading to quench the
discharge in short time [58]. To illustrate it more clearly, the induced field due to accumulated
charges localizes the net field and discharge is extinguished when the net field is lower than the
breakdown field. The charge accumulation on the surface of the dielectric barrier reduces the
electric field at the location of microdischarges which results in the current termination within
nanoseconds. These short duration current discharges are clearly known as the microdischarges
and lead to lower the heat dissipation and the DBD plasma remains firmly non-thermal and nonequilibrium.
Fig. 1.7 Schematic view of the DBD discharge: the charge density on the dielectric barriers
generates a field that opposes the applied field (s= Surface charge density, Es=Electric field
generated due to charge deposition at the dielectric layers).
In order to sustain the sub-atmospheric/ atmospheric pressure glow discharge in the used VD
configuration of the DBD, the applied voltage needs to transform over time, which is essential
condition for such discharges [59]. The applied frequency, pulse width, pulse rise and pulse
shape are the parameters, which controls the discharge dynamics [27]. The applied pulses
basically controls the charges accumulated on the insulator surfaces and also accordingly
removed. This is called memory effect which is the most dominant feature of the barrier
10
Chapter 1: Introduction
discharges [60]. In fact, when we apply the external pulse/sinusoidal voltage to the DBD and the
external voltage increases continuously, the microdischarges are initiated randomly at new
locations because of the presence of residual charges on the dielectric surfaces. These residual
charges reduce the electric field at the positions where microdischarges have already appeared.
When the voltage reversal occurs, new microdischarges are generated at the previous
microdischarges locations and due to the residual charges on the dielectric surface it will take
less external voltage for the breakdown in the subsequent half cycle. If the applied voltage is
adequately enough, the accumulated charges are sufficient to initiate the discharge at next half
cycle of the applied voltage. The basic phenomenon is first the accumulated charge store energy
before the discharge initiation and then release the energy in subsequent discharge. The more
stored energy of these charges results the discharge power increasing.
For the low applied voltage discharges, the discharge is always in Townsend phase and current
density is less than 1mA cm-2 [61]. In this type of discharge, the influence of accumulated charge
can be neglected. In general, the charge accumulation on the dielectric layer increases very fast
with the increase in applied voltage and accordingly the memory effect increases. This increased
memory effect further leads to form more microdischarges. Naude and his co-workers have
shown the transition of Townsend-like to filamentary discharge clearly [62]. They further showed
that the bunch of filamentary streamers or microdischarges can be transformed to the diffuse
discharge, which depends on the driving frequency, operating pressure, and detailed chemistry
coupled through the surrounding gases.
The applied power is also most influencing parameter and it has been found that for increased
applied power the patterned discharge becomes homogeneous gradually [44,63-65]. Somekawa
and his group (2005) explained the theoretical analysis of transition between filamentary to
diffuse mode and also explained the concept of self erasing effect for the succeeding discharge
cycle [66]. For efficient electrical to radiative energy conversion in the plasma, the homogeneity
in the plasma play an important role [67-69] though there are aforementioned large number of
influencing parameters, which need to be understood before arriving to a final conclusion on the
discharge parameter dependency. Hence in the presented VD configuration of the DBDs, an
effort has been made to understand the dielectric barrier discharge in filamentary and diffused
11
Chapter 1: Introduction
mode of operation at different discharge operating conditions for optimum VUV/UV efficiency
so as to develop a practical device for water purification application.
To identify the discharge operating parameters, appropriate diagnostics of DBDs are needed.
However, in very thin geometries of DBDs in-situ diagnostics are not possible [70] but passive
diagnostics, such as, Electrical Analysis [71], Image Intensified Charge Couple Device (ICCD)
imaging [72], Optical Emission Spectroscopy (OES) [73] and particle-in-cell (PIC) simulations
[70] can provide appropriate information about the discharges, and such diagnostics studies are
necessary for the characterization of plasma devices. As the discharge is triggered from the
applied voltage waveform, a non negligible capacitive current component is added to the real
current of the DBD plasma [74]. Moreover, due to the accumulated charges on the dielectric
barrier, there is an induced voltage in the plasma which is quite different from the applied
voltage. Hence a specific data processing through an electrical analysis can compute the whole
measurements. This calculation requires an equivalent circuit model [71] analysis, which
includes all capacitors under consideration. The capacitive and discharge current separation from
the total current has not been clearly worked out so far and this can further help in diagnosing the
electron plasma density through discharge resistivity method [75].
The ICCD camera imaging can investigate the space and time resolved characteristics of the
plasma discharge within discharge region [76] and can easily determine the discharge structures
of the gas gap so as to compare with the PIC simulations [60]. Based on such comparison one
can obtained certain useful parameters and a comparison of the discharge appearance under
sinusoidal and pulse excitation through ICCD showed that under unipolar pulse excitation more
diffuse discharge is observed.
In recent years, the optical emission spectroscopy (OES) has proven to be very versatile
technique for passive plasma diagnostic especially in low and atmospheric pressure discharges
[77]. In fact, there are many atomic and physical processes involved in the DBDs which mainly
depends on the electron energy, electron plasma temperature and electron plasma density. Using
OES technique one can easily determine the electron plasma densities (Ne) and electron plasma
temperatures (Te) and many other parameters of interest [78]. Techniques based on OES are noninvasive and require only moderate spectroscopic equipment, easy to implement and
measurements are usually fast. The OES technique combines measurements of certain line12
Chapter 1: Introduction
intensities that can be compared with the collisional-radiative (CR) model analysis of a plasma
discharge depending on the discharge equilibrium under consideration [79].
This analysis
provides the relative intensities of spectral lines emitted from different upper levels which are
proportional to the relative populations of the excited states and consequently depend on the
plasma parameters. Such analyses have been rarely practiced in the DBDs and hence focused
efforts are needed in this direction.
To compliment the passive plasma diagnostics, computational modeling can successfully be
applied for studying physical phenomena that cannot be effectively investigated experimentally [80].
Using simulations a small change in the operating parameters of the discharge system can be easily
studied. Some preliminary efforts have been made using PIC simulations to interpret DBDs and a
few codes have been developed [81]. The Oopic-Pro is an object oriented particle-in-cell 2-D
simulation code. It solves for the fields on the grid and calculates the particle trajectories including
self-consistently the effects of charged particles on the fields with respect to the space and time
variations. This also treats collision and ionization processes of a background neutral gas with Monte
Carlo collisions method and able to find the electrical as well as the plasma parameters throughout
the gas gap which cannot be calculated through the experiments. To measure the plasma parameters
through the experiments using OES the line-of-sight measurements of the DBD gives average output
but using the PIC simulation a distributive and clear output from every point of the gas gap can be
taken out.
Chapter 1: Introduction
consumed power (Pdis) and some of the basic plasma parameters, such as, electron plasma density
and temperature with the variation of external operating conditions. The electrical parameters on
one hand can provide the selectivity of the power sources for optimum use while the basic
plasma parameters can help in understanding the optimum use of the plasma radiations during
the efficiency analysis of the DBD based VUV/UV light sources.
The single shot images of the DBD in VUV and visible region were also of some interest [82]
which showed the filamentary and diffused structures in the gap but the validation of these
discharge structures is also required. In terms of discharge structure, many researchers are trying
to get the discharge appearance during the process. However, it is necessary to record the short
microdischarge plasmas in the thin geometries of the DBDs using high speed camera, such as,
ICCD in order to get the space and time resolved discharge analysis of very short lived DBD
filaments. This can help to conclude whether the DBD discharge is filamentary or diffused in
nature.
Simultaneously, the simulation also deserves a high degree of credibility when plasma
discharges are transient [83]. So, to compare with the experimental results, a 2-dmensional time
dynamic code like Oopic-Pro can be used [84]. This can help in understanding the discharge
patterns and also can help in the measurements of the basic plasma parameters to compare with
the experimental results. There are some reports of the single microdischarge simulations [85]
but only measurements for a single microdischarge cannot provide the requisite information. In
fact, it just reduces the complexity during the simulation but a single microdischarge cannot
completely describe the array of the filaments which usually occurs in the DBD based excimer
sources. The large area simulation can allow getting the information on the elementary processes
in entire DBD discharge and can give complete description of the plasma during the discharge.
Therefore, there is a requirement for self-consistent simulation by considering all the parameters
simultaneously including, discharge geometry, gas type and pressure, type of dielectric, gas
kinematics, surface chemistry, atomic processes, etc. To do this a packaged code is a better
option and hence the Oopic-Pro code has been used. The theoretical calculations and simulation
model results compared with the experimental results can provide better insight to describe the
discharges in thin DBD geometries. The significant information obtained through the
14
Chapter 1: Introduction
simulations, electrical and spectroscopic diagnostics can further help to make an efficient
VUV/UV excimer source for their immediate use to society.
an efficient
VUV/UV DBD plasma discharge source for societal application. The following are the key
objective of this research work;
1. Design and development of different dielectric barrier discharge sources of volume
discharge configurations working at sub-atmospheric pressures.
2. Electrical characterization of these DBD sources for alternating and unipolar pulsed
voltage excitation mechanisms so as the power source is optimally used.
3. Optical emission spectroscopic characterization of these DBD sources for the
measurements of plasma parameters to help in understanding the optimum use of the
plasma radiations during the efficiency analysis of these DBD based VUV/UV light
sources.
4. Carrying out the particle-in-cell simulation of the designed and developed DBD sources
using electromagnetic simulation software OOPIC-Pro to understand the discharge
patterns and also to help in the measurement of the basic plasma parameters to compare
with the experimental results.
5. Development of an optimized DBD VUV/UV excimer source for the water treatment
application.
The essentials for the experiments and simulations including set-up, results, significance, and
discussion along with an extensive summary are included in the subsequent chapters of this
dissertation.
Chapter 1: Introduction
The scope of proposed research work is well focused to develop the DBD based VUV/UV light
sources and a primarily put forward an understanding to improve the efficiency of the DBD
based excimer light sources for some immediate VUV/UV excimer application. The introduction
to the DBDs and the broad literature review is presented in this chapter that covers a detailed
discussion to the different types of DBD discharges and the physics behind the discharges under
different geometries of DBDs. This chapter also gives a brief review of the useful applications
related to the research work undertaken.
The detailed description of equipments which are used for the experiments have been described
in chapter 2. This includes, description of the different designs of the DBD geometries including
parallel plate geometry, capillary source and a single barrier source. The experimental setup,
details about the electrical measurement equipments, brief discussion about the used optical
diagnostic tools and some details about the diagnostics tool limitations are also considered in this
chapter.
The discharge excitation results of three different geometries for sinusoidal and pulse
excitation are presented in chapter 3. This chapter emphasizes the electrical characterization of
developed sources to derive important electrical parameters using an equivalent electrical circuit
model. The information derived for the electrical parameters includes, the discharge current (Idis),
displacement current through the gap (Idg), gas gap voltage (Vg), dielectric voltage (Vd), memory
voltage (Vmo), supplied power (Psup) and consumed power (Pdis), which are measured for different
operating experimental conditions and in different gas pressures. This exercise has led to
understand the temporal evolution processes of all the internal electrical quantities and
quantitative estimations of the essential electrical parameters.
A parametric study of the DBD is presented and dependency of the different operating
parameters has been discussed which gives the insight of the discharge characteristics in both
excitation cases. The two excitation methods are evaluated on one basic VD configuration
(parallel plate configuration) and results showed that the pulse excitation is much efficient than
the sinusoidal excitation and are explained based on the memory charges.
Moreover the estimated values of the electrical parameters, such as, discharge current (Idis) and
gas gap voltage (Vg) are used to measure the internal dynamic resistance of the gas gap which in
turn is responsible for the measurement of the electron plasma density using discharge resistivity
16
Chapter 1: Introduction
method. The estimated electron plasma density for the parallel plate DBD and capillary DBD is
found to be in the range of 1010 -1011 cm-3 whereas in case of the single barrier DBD it is ~10 12
cm-3.
Chapter 4 contains detail about the DBD characterization using optical emission spectroscopy
(OES) to measure the basic plasma parameters, such as, the electron plasma density (Ne) and
electron plasma temperature (Te). The OES is a non-perturbing passive method for measuring the
plasma parameters and has been best exploited in the thin DBD geometries. For electron plasma
density and temperature estimations, the CR-model based line-ratio technique has been used and
theoretically predicted ratios are compared with ratios of the spectral lines measured
experimentally. The electron plasma density ~1010-1012 cm-3 and electron plasma temperature ~56 eV in the parallel plate and capillary DBD sources are reported, which has been verified using
a 2-D PIC simulation code also.
The kinetic simulations of the DBD sources are carried out for a symmetrical 2-D geometries of
the DBDs using OOPIC-Pro code. The simulations are carried out for both geometries i.e.,
parallel plate and capillary DBD sources. The peak electron plasma densities are obtained from
the simulations code at different radial distances of the discharge geometries for different
simulations times and operating pressures. Since the discharges are filamentary in nature, at the
initial operation of the simulations, the statistical analysis allowed us to measure the electron
plasma density and temperature in the simulations to compare with the spectroscopic average
measurements, which are found to be in close agreement.
Chapter 5 demonstrates the optimization of the single barrier DBD source filled with xenon
and chlorine for efficient use in the water purification application. The generation of excimer
radiation from the mixtures of the rare-gas Xe2 together with halide gas Cl2 and air admixture has
been investigated. The source has been optimized for maximum radiations of this UV-B (308
nm) light which occurs at ~ 2% Cl2 admixture in the xenon and at 25 kHz operating frequency.
Furthermore, to make the source more cost effective in the admixture of Xe 2 and Cl2, the air has
been introduced.
The application of this optimized single barrier DBD source using unipolar excitation is also
discussed in this chapter. The optimized source has been pinched-off at the condition of
maximum radiation efficiency and has been used for water purification study in particular for E17
Chapter 1: Introduction
coli bacteria deactivation. The complete procedure to stop the DNA growth of the bacteria using
direct plasma exposure to the bacteria has also been discussed in this chapter.
The conclusion with overall discussion is presented in Chapter 6, which has been arrived from
the characterization of the DBDs for measuring electrical and plasma parameters and
optimization of the DBD for societal applications. The future scope of the thesis is also presented
in this concluding chapter.
18