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To cite this article: Seong-Ho Yoo , Seung-Ki Chae & Benjamin Y. H. Liu (1996) Influence
of Particle Refractive Index on the Lower Detection Limit of Light Scattering Aerosol
Counters, Aerosol Science and Technology, 25:1, 1-10, DOI: 10.1080/02786829608965374
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ELSEVIER
ABSTRACT. Light scattering particle counters are widely used for aerosol re-
search. They are also important tools for monitoring airborne particles in the
semiconductor and pharmaceutical industries. For the latter application, it is
important to know the influence of particle material properties on the counter
response, particularly the effect of particle refractive index on the lower detection
limit of the counter. In this paper, the effect of particle refractive index on the lower
detection limit of aerosol particle counters has been studied using the Mie theory.
Counting efficiencies have also been measured to verify the theoretical results. The
measurements were made with PSL (polystyrene latex), silicon, silicon nitride, and
silicon dioxide particles. Two commercially available aerosol counters and a con-
densation nucleus counter were used in the study. The theoretical study show that
both the real and the imaginary parts of the particle refractive index affectthe lower
detection limit of a light scattering particle counter. For transparent particles, an
increase in the particle refractive index causes a decrease in the lower detection
limit. And the absorptive component in the refractive index of the particle causes a
further drop in the lower detection limit for the specific counters studied. Experi-
mental measurements show good agreement with the theoretical results. Among the
test particles used, silicon had the largest refractive index, followed by silicon
nitride, PSL, and silicon dioxide. The lower detection limit of the counters studied
also shows a corresponding decreasing trend with silicon dioxide giving the highest
lower detection limit, followed by PSL, silicon nitride, and silicon as the refractive
index of the particle is increased and the lower detection limit of the counter is
decreased. The difference between the theoretical and experimental lower detection
limits was found to be less than 10% in most cases. AEROSOL SCIENCE AND
TECHNOLOGY 25:l-10 (1996)
refractive index, and shape, as well as the influence of particle refractive index on the
wavelength of the light and the collec- lower detection limit of particle counters
tion geometry of the counter. Hodkinson can help to better understand the source of
and Greenfield (19651, Cooke and Kerker measurement errors caused by particle re-
(19751, and Heyder and Gebhart (1979) fractive index.
studied the effect of these parameters on In a typical facility used for semiconduc-
aerosol particle counter response by theo- tor device fabrication, various types of air-
retical methods. Whitby and Vomela (1967) borne contaminant particles can be en-
and Quenzel (1969) investigated the effect countered. An important source is the pro-
of particle properties on the sizing accuracy cess equipment itself and particles such as
experimentally. Wen and Kasper (1986) and silicon dioxide and silicon nitride are gen-
Liu and Szymanski (1987) experimentally erated during the oxide and nitride film
studied the counting efficiency and the deposition process used in semiconductor
lower detection limit of some commercially device fabrication. In this study, we have
available particle counters. focused our attention on such process gen-
Light scattering counters are usually cali- erated particles. Table 1 lists some of the
brated by means of polystyrene latex (PSL) particles included in the present study along
spheres. Since the optical properties of the with their refractive indices at the He-Ne
PSL sphere generally differ from the prop- laser light wavelength of h = 0.633 p m and
erties of the actual particles being mea- the solid state laser wavelength at h = 0.780
sured, errors may arise as a result of the Pm.
different optical properties of the calibra- Present knowledge about the lower de-
tion and the actual particles. For this rea- tection limit of the available aerosol counter
son, it is important to understand the dif- is rather limited. Most previous studies were
ference in counter response due to material empirically based. In this study, the lower
property differences and how this differ- detection limit of the counter is studied
ence may cause measurement errors. both theoretically and by experiments. The
Makynen et al. (1982) have pointed out the effect of the particle refractive index on the
importance of the need to perform calibra- lower detection limit is then presented.
tion studies using particles of different re-
fractive indices.
Among the response characteristics of a THEORETICAL STUDY OF THE
light scattering counter, one of the most LOWER DETECTION LIMIT
important is the lower detection limit, i.e., Theoretical Response of Aerosol Particle
the smallest particle that can be detected Counters
by the counter. In the semiconductor indus- The amount of light scattering by a particle
try the operational class of a cleanroom is as it passes through the viewing volume of
Aerosol Science and Technology Refractive Index and Light Scattering Detection Limits 3
25:l July 1996
Calibration
Polystyrene Latex (PSL) 1.59-i0.0 1.58-i0.0
Semiconductor
Silicon (Si) 3.88-i0.02 3.71-i0.007
Silicon Dioxide (SiO,) 1.46-iO.O 1.45-iO.O
Silicon Nitride (Si,N,) 2.02-iO.O 2.00-i0.0
Metal
Aluminum (Al) 1.30-i7.48 2.63-i8.59
Chromium (Cr) 3.48-i4.36 4.08-i4.35
Iron (Fe) 235.i3.36 3.00-i3.60
Nickel (Ni) 1.92-i3.65 2.43-i4.31
Special Metal
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j
u
.
d
,y.
I.,1
'
- - - - .
Si3N4
- - - PSL s*
FIGURE 1. Theoretical response of the PMS LAS-X FIGURE 3. Theoretical response of the TSI LPC 3753
counter to PSL, silicon, and silicon compound parti- counter to PSL, silicon, and silicon compound parti-
cles. cles.
Aerosol Science and Technology Refractive Index and Light Scattering Detection Limits 5
0 1 2 3 4
0.1 1.o 10.0
Particle Diameter (pm) Real Part of Refractive Index (n)
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FIGURE 4. Theoretical response of the TSI LPC 3753 FIGURE 5. The lower detection limit of the PMS
counter to PSL and metal particles. LAS-X counter as a function of the real part of the
refractive index.
0 1 2 3 4 5 6
cle refractive index approaches the medium
refractive index. Scattering intensity calcu- Imagmary Part of Refractive Index (k)
lations do not converge if the refractive FIGURE 6. The lower detection limit of the PMS
indices of the particle and medium are too LAS-X counter as a function of the imaginary part of
close to each other. For transparent parti- the refractive index.
6 S.-H. Yoo et al. Aerosol Science and Technology
25:l July 1996
LPC 3753
g 1.0
a 3 oo
.. 4 00
a
- -3--===
1
FIGURE 7. The lower detection limit of the TSI LPC FIGURE 8. The lower detection limit of the TSI LPC
3753 counter as a function of the real part of the 3753 counter as a function of the imaginary part of the
refractive index. refractive index.
Tables 2 and 3 summarize the calculation of the Si particle. On the other hand, the
results for various real and imaginary parts lower detection limit of the counter for
of the refractive index. For the PMS LAS-X silicon dioxide particles is only 0.13 p m due
counter, the lower detection limit is as small to the smaller real refractive index of SiO,
as 0.087 p m for silicon particle whose real in comparison with that of PSL. For the
refractive index is considerably higher than TSI 3753 counter with a nominal lower
that of PSL. The ability of the counter to detection limit of 0.3 pm, the theoretical
detect particles as small as 0.087 p m can be lower detection limit of the counter for Si
attributed to the large real refractive index and SiO, particles are 0.18 and 0.33 pm,
TABLE 2. Lower Detection Limit of PMS LAS-X Counter in wm for Various Particle Refractive Indices
Real Imaginary ( k )
(n) 0.0 0.05 0.1 0.5 1.O 5.0 7.0
Aerosol Science and Technology Refractive Index and Light Scattering Detection Limits 7
25:l July 1996
TABLE 3. Lower Detection Limit of TSI LPC 3753 Counter in p m for Various Particle Refractive Indices
Real Imaginary ( k )
n 0.0 0.05 0.1 0.5 1.O 5.0 7.0
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Excess
Air t Sheath Air
Diffusion
Dryer
Po-210
Neutralizer
-1
H.V. Power
Supply
Necleus
Aerosol
Particle
Counter Counter
Differential
Absolute Mobility
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Filter Analyzer
Clean
Air
Atomizer
Po-210
Neutralizer Computers
Air
FlGURE 9. Schematic diagram of the experimental setup for lower detection limit measurement.
terial and sizes is shown in Fig. 9. The same Results of Counting EfJiciency Measurements
counters used in the theoretical studies are Experimental result for the LAS-X counter
also used in the experiments. Aerosol of a is shown in Fig. 10. All particle materials
known size and material is first generated used in the experiments showed about
by the particle generation system consisting 100% counting efficiency at a particle size
of an atomizer, a neutralizer, and a differ- 2 0.2 pm. However, different counting
ential mobility analyzer (DMA). Monodis-
perse particles generated by the DMA are
introduced to both the particle counters
and the condensation nucleus counter
(CNC). Among the particle materials listed
in Table 1, PSL, silicon, silicon nitride and
silicon dioxide particle are used in the ex-
perimental study.
To determine the counting efficiency, the
TSI 3760 CNC was used as the reference
counter. Previous studies of CNC by Wen
and Kasper (1986) show that the absolute
counting efficiency of a CNC is nearly
0.08 0.1 0.2 0.3
100%. The counting efficiency of the parti-
cle counter, therefore, can be determined Particle Diameter (pm)
by comparing the aerosol concentration FIGURE 10. Experimental counting efficiency of the
measured by the counter and that by the PMS LAS-X counter for PSL, silicon, and silicon com-
rcference CNC. pound particles.
Aerosol Science and Technology Refractive Index and Light Scattering Detection Limits 9
25:l July 1996
dioxide with the smallest refractive index, FIGURE 11. Experimental counting efficiency of the
TSI LPC 3753 counter for PSL, silicon, and silicon
to PSL, silicon nitride, and silicon with in- compound particles.
creasing particle refractive index.
Figure 11 shows the results for the TSI
3753 counter. This result also shows a simi-
lar trend as that shown by the LAS-X equal to one half of the nominal maximum
counter. It should be noted, however, that counting efficiency of 120%.
the nominal counting efficiency of this The nominal lower detection limit pro-
counter as determined by the method de- vided by the manufacturer was verified with
scribed above was found to approach 120% PSL spheres and it turned out that the
rather than the theoretical limit of 100% at nominal and the actual lower sizing limit
large particle sizes. The cause of the greater are quite close. The comparisons between
number of particles counted by the TSI the theoretical and experimental results are
3753 laser particle counter is thought to be given in Table 4. The difference between
caused by the fact that there is no sheath the two values is generally much less than
air protection around the aerosol stream. 10%. The data thus support both the valid-
The lack of a sheath air around the aerosol ity of the theoretical and the experimental
stream can cause particle circulation within lower detection limit values obtained here.
the sensing volume of the counter, leading From this comparison, it seems reasonable
to a higher particle count for large particle to conclude that the lower detection limit
sizes. For this reason, we have determined obtained by the theoretical study such as
the lower detection limit of the TSI 3753 the results shown in Tables 2 and 3 can be
counter by determine the particle size at used to make a reasonably accurate esti-
which the measured counting efficiency is mate of the actual lower detection limit
detection limit of the counters increases as Hodkinson, J. R., and Greenfield, J. R. (1965).
the real part of the particle refractive index Appl. Opt. 4:1463-1474.
approaches that of the medium and de- Knollenberg, R. G., and Veal, D. L. (1992).
creases as the real part of the particle J. Inst. Enuiron, Sci. March/April, pp. 64-81.
refractive index deviates from that of the Liu, B. Y. H., Berglund, R. N., and Aganval,
medium in both directions. For both coun- J. K. (1974). Atmos. Enuiron. 8:717-732.
ters, a transparent particle will need an Liu, B. Y. H., and Szymanski, W. W. (1987). In
infinite particle size for the counter to de- Proceedings of the 33rd Annual Technical Meet-
tect as the real part of the particle refrac- ing, Institute of Environmental Sciences, San
tive index approaches that of the medium, Jose, CA, May 4-8, pp. 461-465.
as the particle becomes essentially invisible Liu, B. Y. H., W. W. Szymanski, W. W., and Pui,
as the particle and medium refractive index D. Y. H. (1986). ASHRAE Trans., Vol. 92,
becomes equal. Generally, a high imaginary Part lA, No. 2971, pp. 518-538.
part of the refractive index will cause the Makynen, J., Hakulinen, J., Kivisto, T., and
lower detection limit to decrease. The Lehtimaki, M. (1982). J. Aerosol Sci.
smallest lower detection limit calculated 13529-535.
was less than 50% of the nominal lower Martens, A. E., and Doonan, D. D. (1970). Appl.
detection limit. Opt. 9:1930-1931.
The result of the theoretical studv was Palik, Edward D. (1 985). Ed., Handbook of Opti-
verified by experiments with several parti- cal Constants of Solids, Academic, 1985.
cle materials. The lower detection limit Quenzel, H. (1969). Appl. Opt. 8:165-169.
measured with PSL aerees " well with the Wen, H. Y., and Kasper, G. (1986). J. Aerosol
nominal lower detection limit given by the Sci. 17:947-961.
manufacturer. The experimental results fol- Whitby, K. T., and Vornela, R. A. (1967). Enui-
low the general trend of the theoretical ron. Sci. Technol. 1:801-814.
results. The difference between the theo-
retical and experimental results is less than Reccivcd June 5, 1995; revised December 8,
10% in most cases. 1995.