Aerosol Science and Technology

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Charging of Ultra-Fine Aerosol Particles by an

Ozone-Free Indirect UV Photo-Charger

B. Grob, H. Burtscher & R. Niessner

To cite this article: B. Grob, H. Burtscher & R. Niessner (2013) Charging of Ultra-Fine Aerosol
Particles by an Ozone-Free Indirect UV Photo-Charger, Aerosol Science and Technology, 47:12,
1325-1333, DOI: 10.1080/02786826.2013.840357

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 Aerosol Science and Technology, 47:1325–1333, 2013
Copyright C American Association for Aerosol Research
ISSN: 0278-6826 print / 1521-7388 online
DOI: 10.1080/02786826.2013.840357
Charging of Ultra-Fine Aerosol Particles by an Ozone-Free
Indirect UV Photo-Charger
B. Grob,1 H. Burtscher,1,2 and R. Niessner1
1
Department of Analytical Chemistry, Technische Universität München, Munich, Germany
2
Institute for Aerosol and Sensor Technology, University of Applied Sciences, Northwestern Switzerland,
Windisch, Switzerland
Particle charging by indirect photoemission may be an alterna-
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tive to charging methods based on corona discharge or on bipolar
charging by radioactive ion sources. An indirect charger using a
low energy UV radiation is introduced and characterized in de-
tail. Depending on the carrier gas, photoelectrons or ions formed
by electron-attachment charge the particles by diffusion charging.
The achieved charging efficiency is in the range of 20–70% for
particle sizes of 20 to 100 nm. It can easily be modulated by a
small voltage applied to the photoemitter. To achieve stable elec-
tron emission, glassy carbon with its very inert surface is used as
photoemitter. Particle losses are very small. The charge distribu-
tion has been measured by a tandem DMA setup. The experimental
results are compared with the theory of unipolar diffusion charg-
ing based on the Fuchs’ combination probability of ions with the
particles. The charger characterization has been performed by car-
bon particles in a size range of 20–100 nm, produced by a spark
discharge generator.
1. INTRODUCTION
For many techniques to measure size and concentration of
submicron particles, as for example mobility analysis, it is nec-
essary to charge the particles electrically. A number of ways
to charge particles have been developed including unipolar and
bipolar charging.
The most frequently used technique for bipolar charging is
producing gas ions by a radioactive source (Kr-85, Ni-63, Am-
241, Po-210). These ions then attach to the particles by diffu-
sion. The main advantage of bipolar charging is that a charge
equilibrium is established, which is independent of the ion con-
centration. This allows achieving a very well-defined charge
distribution. The charging efficiency is limited, which has the
Received 6 June 2013; accepted 27 August 2013.
Address correspondence to B. Grob, Department of Analytical
Chemistry, Technische Universität München, Marchioninistraße 17,
Munich 813777, Germany. E-mail: benedikt.grob@mytum.de
advantage that the number of multiply charged particles is mod-
erate and the disadvantage of reducing the detection limit. On
the other hand, dealing with radioactive sources causes more and
more problems, in particular for field measurements. Therefore,
alternatives are investigated since very long time. Meanwhile
X-ray ionizers are available (Han et al. 2003; Kaufman 2010)
which are easier to handle, but still are subject to restriction in
transport in some countries. Chargers based on bipolar electrical
discharges have also been investigated (bipolar corona, Stom-
mel and Riebel 2005, dielectric barrier discharge, Byeon et al.
2008) but so far with limited success. A comparison of different
bipolar chargers can be found in Kallinger et al. (2012). Bipolar
charging is applied for differential mobility analysis in scanning
devices (DMPS, SMPS).
Unipolar charging can be obtained on the one hand by di-
rectly ionizing the particles by irradiation with electromagnetic
radiation (UV light), leading to the emission of electrons. This
process (direct photoelectric charging) is strongly material de-
pendent and can be used to selectively charge certain particle
classes (Schmidt-Ott and Siegmann 1978; Burtscher et al. 1982).
If charging should be material-independent, unipolar ions
can be produced by a corona discharge (silent electrical dis-
charge). These ions attach to the particles by diffusion (unipolar
diffusion charging) or assisted by an electrical field (field charg-
ing). Field charging is used in electrostatic precipitators, where
charging and precipitation are achieved by the same field. For
measurement purposes, usually diffusion charging is used. The
charging occurs in a mainly field-free area.
Unipolar charging allows obtaining a higher efficiency than
bipolar charging, but as a consequence this also leads to more
multiply charged particles.
It is applied in the fast mobility analyzers (EEPS, FMPS,
DMS500), where the parallel measurement of many channels by
electrometers requires an efficient charging technique to achieve
a reasonable detection limit.
Also, a number of particle sensors (diffusion charging sen-
sors, EAD, NSAM, DiSC, etc.) make use of corona charging.
1325
 1326 B. GROB ET AL.

ter, but below the threshold for ozone formation and below
the threshold, where particles start to emit electrons. Usually
the latter restriction will be dominant for the upper limit. This
leaves only a narrow window of photon energies. No materials
exist that have a stable ionization threshold below about 4.5 eV,
when exposed to air. Above little more than 5 eV, ambient air
molecules start emitting electrons. As a result, the available
range of wavelength is ca. 275–240 nm.
At ambient pressure, most photoelectrons will diffuse back
FIG. 1. Particle charging by indirect photoemission. (Color figure available
online.)
to the emitter if the voltage U is zero or very small. The cor-
responding ion concentration will be low. The electron escape
probability increases with increasing U, until all electrons es-
More information can be found for example in Dhaniyala et al.
cape. On the other hand, a high U will lead to a rapid precip-
(2011) or Intra and Tippayawong (2011).
itation of the electrons or ions, respectively. This reduces the
Corona chargers are relatively simple, robust devices. Some
ion concentration again. Therefore, the ion concentration will
drawbacks are that the corona always produces some ozone. To
be low for very small and for high U, somewhere in between a
minimize ozone formation, carbon microfibers have been used
maximum exists, where the charging efficiency also will have
for ion generation (Han et al. 2008). Depending on the carrier
its maximum. A quantitative treatment will follow.
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gas of the particles, the plasma of the corona discharge may

In carrier gases without electronegative molecules electrons
act as a chemical reactor, producing undesired species, in some
remain free. Due to their very high mobility, their residence time
cases also additional particles. Many chargers need an electrical
is short, and the charge concentration will be low.
field to bring the ions into the charging zone that leads to losses
Once the electron/ion concentration is known, the product
for very small particles.
of concentration and residence time (N × t product) can be
Here, we use a different approach for unipolar diffusion
determined, which is directly related to the charging efficiency.
charging. A surface is irradiated with UV light of a photon
energy higher than the ionization threshold of the surface, but
below the threshold of the particles and that for ozone forma- 3. THEORETICAL CALCULATION
tion. Depending on the carrier gas the emitted photoelectrons OF PARTICLE CHARGING
remain free (in noble gases) or attach to gas molecules (if an The experimental results were compared with the theoreti-
electronegative gas like oxygen is available). In air, negative cal considerations for unipolar diffusion charging described by
ions are formed within microseconds. These ions then attach to Adachi et al. (1985) using Fuchs’ combination probability of
the particles by diffusion (Figure 1). A very small DC-voltage U ions with the particles and the basic differential equations from
is applied between the photoemitter and a grid to assist electron Boisdron and Brock (1970) in the case of unipolar diffusion
escape from the emitter. charging:
This technique (indirect photoelectric charging) allows a very
soft ion production mainly without inducing undesired chemi- dn0
= −β0 n0 N [1]
cal reactions. To our knowledge, Bucholski and Niessner (1991) dt
introduced indirect photoelectric charging first. Later Oh et al. dnp
= βp−1 np−1 N − βp np N. [2]
(2004) used an indirect photoemission charger to investigate dt
the effect of particle shape on the charging efficiency. Shimada
In these equations, n0 denotes the number concentration of
et al. (1997, 1999) used indirect photoemission to charge par-
the uncharged particles, np the number concentration of the
ticles for electrostatic precipitation. Even if some earlier work
particles carrying p elementary charges, and nT particle number
exists, where this technique has been applied, it never has been
concentration in total. N specifies the ion concentration and β p
investigated thoroughly. Here we will present a detailed charac-
the combination probability.
terization of an indirect photoemission charger with the purpose
Assuming that the initial particles are uncharged, the analyt-
to substitute radioactive bipolar charger or corona chargers, e.g.,
ical solution for the charged fraction of particles np /nT carrying
used for producing a monodisperse aerosol by electrostatic clas-
p elementary charges can be found:
sification.
n0
= exp(−β0 N t) [3]
nT
p−1  p
2. BASIC CONSIDERATIONS np   exp(−βj N t)
The photon energy of the UV light source has to be chosen = βk N p . [4]
nT j =0 l=0,l=j (βl − βj )N
such that it is above the ionization threshold of the photoemit- k=0
 A NEW UNIPOLAR CHARGER AS ALTERNATIVE TO KR-85 OR CORONA 1327

FIG. 2. Configuration of the indirect photoelectric charger. (Color figure available online.)
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The combination probability β p has been determined using spark discharge generator; for some experiments, NaCl particles
Fuchs’ limiting sphere theory (1963) whereupon the diffusion have been used.
coefficient Dion , mean thermal velocity cion , and the mean free
path of the ions λion in dry air have been calculated by following
equations (Adachi et al. 1985). 4.1. Setup of the Indirect Photoemission Charger (IPC)
Figure 2 shows the indirect photoelectric charger, used for our
Dion = kTZion /e [5] experiments. A pen ray Hg low-pressure mercury lamp, emitting

cion = 8kT /π (Mion /Na ) [6] at 254 nm (ozone-free version, suppressing the 185-nm line) is
 applied. It has a lighted length of 45 mm. A glassy carbon rod
Zion kTMion Mair with a diameter of 6 mm is used as electron emitter. Glassy
λion = 1.329 , [7]
e (Mion + Mair )Na carbon is used because it combines an ionization threshold in
the desired window with a very inert surface. This is essential to
where k is the Boltzmann factor, Na the Avogadro number, T achieve a stable electron emission. To keep the surface clean, the
the temperature that was considered to be 300 K, and e the rod can be heated to a temperature of about 80◦ C by an electrical
elementary charge. As we have been using dried air as carrier current through the rod. Lamp and emitter are placed in the
gas in our study, we assumed the formation of O− 2 ions by focuses of an elliptical mirror. Thereby the light is focused onto
electron attachment in a three-body reaction with oxygen or the rod. The rod is placed in the axis of a quartz tube. A metal grid
nitrogen molecules as third body (Davies 1983): at the inner wall of the tube allows to apply an electrical voltage
between the rod and the screen. The particle charging time is
e− + O2 + M → O−
2 + M. [8] 0.45 s considering a flux of 0.3 lmin−1 and an inner diameter of
the grid of 10 mm. We assume that charging takes only place
In the presence of CO2 , further reactions can form heavier along the illuminated length. The current of ions, arriving at
CO− 4 ions as considered by Davies (1983). Therefore, we set the screen is measured by a current–voltage converter, having
the molecular weight for the ions M ion = 76 g/mol and the a sensitivity of 0.4 V/nA (400 M feedback resistor). This
ion mobility Z ion = 2.3 × 10−4 m2/Vs (Davies 1983). In the amplifier keeps the grid virtually at ground potential.
experimental results, we used mainly the average number of We determined the ion concentration from the measured
elementary charges per particle, η, defined as follows: current by following consideration. The measured ion current
through the grid is defined as follows:
∞
np
η= p . [9]
n
p=0 T
I = eN 2π r2 Lv. [10]

4. EXPERIMENTAL SETUP The length L is the length of the UV irradiation, which is

A prototype of an indirect charger has been built. Extended equal to the length of the lamp. The inner radius of the grid
tests have been performed with carbon particles produced by a is substituted by r2 . The drift velocity of the ions v can be
 1328 B. GROB ET AL.

calculated by the ion mobility Zion and the electrical field E. particles then pass through a Kr-85 charger. A plate condenser
removes all remaining charged particles. The number concentra-
v = Zion E. [11] tion of the monodisperse, neutral particles nT , entering the IPC,
is measured by a CPC. The charged particles npT downstream the
The electrical field at r2 can be obtained by knowing the IPC are measured by an aerosol electrometer (TSI3068). It was
potential applied to the rod U and the radius of the rod r1 . evaluated from the electrometer current IAEM and the aerosol
flux q by the assumption of single charged particles (p = 1).
U
E=
. [12]
r2 log rr21 IAEM
npT = . [14]
eq
Therefore, the ion concentration can be calculated by the
following equation: The average number of elementary charges per particle η can
r2
be calculated as follows:
I log r1
N= . [13]
2π eLZion U npT
η= . [15]
nT
4.2. Setup to Determine the Average Number
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of Elementary Charges Per Particle
The experimental setup to determine the average number of
elementary charges per particle is shown in Figure 3. Particles
are produced by a Palas GFG1000 spark generator, equipped
with carbon electrodes. The generator is followed by a differ-
ential mobility analyzer to select one particle size class. These
To determine losses, the CPC may be connected also down-
stream the IPC. Loss measurements are performed with carbon
particles from the spark generator and with NaCl particles pro-
duced by an atomizer. Losses are determined by comparing
the concentration, measured with the CPC upstream and down-
stream the IPC.

FIG. 3. Setup to measure the average number of elementary charges per particle.
 A NEW UNIPOLAR CHARGER AS ALTERNATIVE TO KR-85 OR CORONA 1329
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FIG. 4. Setup to measure multiple charges.

4.3. Setup to Determine Multiple Charging 5. RESULTS

To determine the fraction of multiply charged particles, a Experiments have been made with different carrier gas for
tandem DMA setup is used (Figure 4). As before monodisperse, the particles by mixing the argon stream of the spark discharge
neutral particles enter the IPC. At the outlet, a second DMA is generator with the sheath gas of the DMA using dry air, nitrogen,
placed that classifies the particles according to the number of and argon. As for most applications the carrier gas will be air,
charges they carry. results with air are shown in detail, then a brief section for the
The shown setup delivers only the fraction of charged other gases follows.
particles:
5.1. Dry Air
np 5.1.1. Average Number of Elementary Charges Per Particle
θp =  . [16]
p=1 np In Figure 5, the ion current and the average number of el-
ementary charges per particle are plotted versus the voltage,
To consider also the fraction of uncharged particles nnT0 fol- applied at the rod. For low voltages the ion current is small, be-
lowing method was used for the calculation. The concentration cause most of the emitted electrons diffuse back to the rod. With
measured by the aerosol electrometer npT with the setup de- increasing voltage the escape probability also increases, which
scribed in Section 4.2 is defined as: leads to an increasing ion current (for more information on
back diffusion probability of photoelectrons, see for example

npT = pnp . [17] Radmilović-Radjenović et al. 2009). However, the increasing
p=1 voltage also leads to a higher drift velocity of the ions, reducing
the ion concentration and thus the N × t product, which is re-
Knowing also the total number concentration nT , the con- sponsible for the average charge. For very low voltages the ion
centration of the neutral particles can be calculated: current is very small, for high voltage the ion residence time.
As a result, the ion concentration and the average charge have
 npT a maximum occurring at ca. 1.4 V. For all following measure-
n0 = nT − np = nT −  . [18] ments, the rod voltage has been set to 1.4 V. The experiment and
p=1 p=1 pθp
the theoretical calculation show the same trend. The theoretical
 1330 B. GROB ET AL.
FIG. 5. Ion current and average number of elementary charges per particle
for 40-nm particles versus voltage, applied at the rod. The error bars show the
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single standard deviation of the averaged measured values in consideration of
Gaussian error propagation.
average charge is about 4% larger than measured for 1.4 V. The
difference between theory and experiment can be explained that
the Fuchs’ model does not consider the particle losses. For in-
creasing voltage the differentiation is increasing, which can be
due to the effect of higher particle losses with increasing field
strength.
The average number of elementary charges as function of
particle size is shown in Figure 6. It is comparable to typical
efficiencies obtained with corona chargers. Experimental and
theoretical results fit very well considering again possible par-
ticle losses.
FIG. 6. Average number of elementary charges per particle as function of
particle size. Rod voltage: 1.4 V. The error bars show the single standard de-
viation of the averaged measured values in consideration of Gaussian error
propagation.
Figure 7 shows the current of charged particles versus their
number concentration. The perfect linearity up to particle con-
centrations of 5 × 105 cm−3 shows that no saturation occurs up
to high concentrations.
5.1.2. Losses
Particle penetration through the charger has been determined
for NaCl particles (mainly spherical) and particles produced by
the spark discharge generator (agglomerates). Results are plot-
ted in Figure 8. The difference observed, when UV lamp or rod
voltage is turned on and off, is very small. This indicates that
mainly diffusion losses are relevant, not electrostatic precipita-
tion. For larger particles, losses are slightly higher in the case
of agglomerates.
5.1.3. Multiple Charges
Multiple charges have been measured with a tandem DMA
setup. Figure 9 shows the mobility spectrum measured with
the second DMA, when 40-nm particles are selected with the
first. The modes for singly (main peak) and doubly charged
particles (mode on the right) are well visible. An additional
mode on the left of the main peak is due to larger particles,
leaving the first DMA doubly charged. No higher charges occur
for this particle size. The experimental result has been fitted
with a lognormal distribution for each mode to evaluate the
contribution of each mode. The fraction of charged particles was
calculated from the relative peak heights. The total contribution
of charged and uncharged particles is plotted in Figure 10. The
results for particle sizes from 20 nm to 100 nm are summarized
in Figure 11.
The results demonstrate for a particle size smaller than 40 nm
the fraction of double charged particles is smaller than 8%.
FIG. 7. Aerosol electrometer current versus CPC number concentration for 80-
nm particles. The error bars show the single standard deviation of the averaged
measured values. The fit includes n = 16 data points from a single measurement
(m = 1).
 A NEW UNIPOLAR CHARGER AS ALTERNATIVE TO KR-85 OR CORONA 1331

FIG. 8. Penetration through the charger as function of particle size for NaCl
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particles, produced by a nebulizer, and carbon particles, produced by the GfG FIG. 10. Fraction of neutral, singly, and doubly charged 40-nm particles.
1000 spark discharge generator. The error bars show the single standard de-
viation of the averaged measured values in consideration of Gaussian error
propagation. From Figure 11, it can be estimated an extrinsic charging
efficiency of the charger between 20% and 70%.

For 80–100 nm, the distribution gets very broad with particles
carrying up to four elementary charges. In this range of particle
size, one has to mention that the modes of the electrical mobility
spectrum of multiple-charged particles appear only in a single
peak. This makes it delicate for the fitting procedure to find the
right solution.
5.1.4. Particle Material
Experiments with particles from the spark generator and also
with NaCl particles show a stable, reproducible performance
of the charger. We also did some experiments with combustion
aerosols, produced by a flame soot generator (AVL Particle Gen-
erator, AVL LIST GMBH, Austria). If the volatile fraction of
these particles is removed by an evaporation tube or a thermode-
nuder, positively charged particles leave the charger. Obviously
direct photoelectron emission from the particles dominates the
charging process in this case.

FIG. 9. Mobility distribution obtained with the second DMA, starting with 40-
nm particles. The solid lines are fit to a lognormal distribution for each mode (1
to 4 charges per particle of the unipolar charger and the larger multiply charged
particles from the Kr-85 bipolar charger passing the first DMA are considered).
The error bars show the single standard deviation of the averaged measured
values. The fit includes n = 51 data points that are the mean value of m = 3
measurements. FIG. 11. Fraction of multiply charged particles from 20 to 100 nm.
 1332 B. GROB ET AL.

lyzer (O341 M, environment s. a., France). The measurement

has been performed with a flux of 2 lmin−1 of particle and ozone-
free air for turning on and off the UV light. For comparison, it
is also shown the ozone concentration for ambient air in the lab.
The results demonstrate no significant ozone production by the
UV lamp. Moreover, we did not observe any undesired particles
produced by the UV light in our experiments.

5.2. Argon and Nitrogen as Carrier Gas

Whereas emitted electrons immediately form ions in air, elec-
trons remain free in pure noble gases and also in N2 . This has
a strong influence on particle charging. The very much higher
mobility of free electrons leads to a short residence time. As
a consequence, the same current leads to a much lower elec-
tron concentration, and the N × t product is much smaller. In
addition, attachment coefficients are significantly different.
In contrast to ions, the electron mobility depends on the
FIG. 12. Ozone concentration measured after the charger with the condition of energy or the drift velocity of the electrons, respectively.
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UV lamp on and off for ozone-free air. For comparison the ozone concentration
of the ambient air in the lab is plotted additional.
5.1.5. Ozone Formation
It was proved that the used pen ray Hg low-pressure mer-
cury lamp is prohibiting the ozone formation by eliminating the
185-nm line with a quartz jacket. Figure 12 shows the ozone
concentration after the charger measured with an ozone ana-
Figure 13 shows the measured grid current and the average
number of elementary charges per particle as function of the rod
voltage. The shape of the current–voltage relation is similar to
the one obtained for air; it is mainly determined by the back-
diffusion probability of electrons to the rod.
However, the average charge versus rod voltage is very
different. The charging efficiency reaches a maximum already
at a low voltage, even if the current still is low. With increasing

Nitrogen
0.06 0.8
Average Charge
Average Charge

Ion Current [nA]

0.04 0.6
Ion Current

0.02 0.4

0 0.2

−0.02 0

Argon
0.4 1.6
0.35 1.4
Average Charge

Ion Current [nA]

0.3 1.2
0.25 1
0.2 0.8
0.15 0.6
0.1 0.4
0.05 0.2
0 0
Negative Voltage at Rod [V]

FIG. 13. Average number of elementary charges per particle and current-voltage relation for nitrogen (upper graph) and Ar (lower graph) for 40-nm particles (not
considering different particle mobilities for nitrogen and Ar in the DMA compared to air). A negative charging efficiency (defined as average number of negative
elementary charges) means that the particles carry a positive charge.
 A NEW UNIPOLAR CHARGER AS ALTERNATIVE TO KR-85 OR CORONA
voltage and increasing drift velocity the charging efficiency
strongly decreases, as this was also the case for air. But now,
after a minimum, the charging efficiency or the average charge
per particle starts increasing again. This can be explained by a
decrease in electron mobility with increasing drift velocity. The
effect of the increasing current now is dominant, the charge
concentration increases again. For both gases, the charging
efficiency is very low compared to the result for air. Using
data for the electron mobility versus drift velocity from Dutton
(1975) and electron attachment coefficients given by Romay
and Pui (1992), the shape of the efficiency-voltage curve can
be explained.
The “negative” average charge, observed for nitrogen at volt-
ages in the range of 5–12 V most probably is due to photoe-
mission directly from particles, leading to positively charged
particles. The indirect charging is very inefficient in this range,
thus already a very small probability of electron emission from
particles may be dominant.
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6. CONCLUSIONS
Indirect photoemission allows a stable and well-defined ma-
terial independent charging of ultrafine particles as long as the
work function is higher than the photon energy of the light
source. It can be an alternative to corona charging, having the
advantage of low losses and no ozone formation. The charging
efficiency is comparable to corona chargers. It can be varied
by changing the lamp intensity or the voltage, applied to the
photoemitter. This allows a very simple and effective control of
the charging efficiency.
For particles from the spark discharge generator, and also for
NaCl particles, no direct photoelectron emission is observed.
However, for particles from a flame soot generator direct pho-
toemission may be dominant. These particles either have a low
enough ionization threshold to be ionized by the 254-nm light of
the Hg lamp or are ionized by small amounts of light with higher
photon energy, which is not completely absorbed by the bulb of
the lamp. Similar effects have to be expected for other combus-
tion aerosols, but also for metal aerosols. This is a restriction of
the present setup, which has to be kept in mind.
It could be overcome by separating ion production and ion
attachment. Ions could be produced in a particle-free gas flow,
which is then mixed with the aerosol, as done already for other
reasons for corona chargers. This would also allow using slightly
higher photon energies and thus increase the charging efficiency.
Experiments with such a setup are in progress. The configura-
tion used by Shimada et al. (1997), where a thin gold film is
irradiated with UV light from one side and electrons are emitted
to the other side, also could at least significantly reduce direct
photoemission.
To run the charger with higher flow rates, the geometry could
be changed to use quartz tubes with larger diameters and longer
lamps to increase the residence time of the particles as well as
the ion concentration in the charger.
1333
The low pressure Hg lamp, used here has a limited live time
and needs several minutes to warm up. Alternative light sources
could be dielectric barrier discharge excimer lamps, which can
be produced with a variety of wavelengths, have a very long
lifetime and almost immediately reach their full intensity. In the
near future UV LED’s might be available, which would allow
to build a significantly smaller charger.
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