Aerosol Science & Technology

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Size Distributions of Motor Vehicle Exhaust

PM: A Comparison Between ELPI and SMPS
Measurements

M. Matti Maricq , Diane H. Podsiadlik & Richard E. Chase

To cite this article: M. Matti Maricq , Diane H. Podsiadlik & Richard E. Chase (2000)
Size Distributions of Motor Vehicle Exhaust PM: A Comparison Between ELPI and SMPS
Measurements, Aerosol Science & Technology, 33:3, 239-260, DOI: 10.1080/027868200416231

To link to this article: https://doi.org/10.1080/027868200416231

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 Aerosol Science and Technology 33:239–260 (2000)
° c 2000 American Association for Aerosol Research
Published by Taylor and Francis
0278-6826/ 00/ $12.00 + .00

Size Distributions of Motor Vehicle Exhaust PM:

A Comparison Between ELPI and
SMPS Measurements
M. Matti Maricq¤ , Diane H. Podsiadlik, and Richard E. Chase
FORD MOTOR COMPANY, RESEARCH LABORATORY, P.O. BOX 2053, MD 3083,
DEARBORN, MI 48121

ABSTRACT. Particle size measurements using the electrical low pressure impactor
(ELPI) and scanning mobility particle sizer (SMPS) are compared from the perspec-
tive of characterizing the particulate matter in motor vehicle exhaust. Both steady
state vehicle operation and transient drive cycles are considered, and both gasoline
and diesel fueled vehicle emissions are compared. Although the ELPI and SMPS
measure different physical properties, respectively, the aerodynamic diameter and
mobility diameter, the steady state particle size distributions are in close agreement,
except for the 37 nm impactor stage of the ELPI which may overestimate particle
number by up to a factor of two relative to the SMPS. This has little effect on the
volume, or mass, weighted distribution. These, too, are generally in good agreement,
though discrepancies appear at large particle size due to multiple charging effects
in the SMPS and to electrometer offsets and the small particle loss correction in
the ELPI. Selecting particles based on their electrical mobility with the SMPS,
and then measuring their aerodynamic diameter with the ELPI, reveals that diesel
particulate matter with well-speciŽ ed mobility diameter exhibits a wide range in
aerodynamic diameter and, therefore, also in effective density. Over transient drive
cycles, the ELPI provides second by second particle distributions, whereas the SMPS
must be run in a Ž xed particle size mode and size distributions constructed from
repeated tests. The ELPI registers higher instantaneous PM emission rates during
transients than the SMPS due to the faster time responses of the ELPI. The time in-
tegrated ELPI and SMPS size distributions, however, remain in good agreement. The
relative merits of the two instruments for steady state and transient tests are discussed.

INTRODUCTION lation between ambient PM concentrations and

Particulate matter (PM) size has become a topic
of considerable current interest. Epidemiolog-
ical studies have uncovered a statistical corre-
¤
Correspondin g author.
hospital admissions and death rates (Dockery
and Pope 1994; Pope et al. 1995). At least partly
on this account, the Environmental Protection
Agency (EPA) has promulgated a new PM2.5
ambient standard for particles with aerodynamic
240 M. M. Maricq et al.
diameter · 2.5 l m.1 In turn, this has spurred in-
terest in particle size and especially in ultraŽ ne
and nano-particles. These have been speculated
as being responsible for the adverse health ef-
fects (Donaldson et al. 1998), though the actual
mechanism remains unknown. UltraŽ ne parti-
cles have been found in urban areas before day-
break; however, their source has thus far been in-
ferred, but not identiŽ ed (Booker and Earnshaw
1998). They have been reported in motor ve-
hicle exhaust (Greenwood et al. 1996), though
recent work has shown that dilution tunnel ar-
tifacts can produce high ultraŽ ne particle con-
centrations that appear to originate from the test
vehicle, but do not (Maricq et al. 1999a).
From a regulatory standpoint, the emissions
standards are written in terms of PM mass. The
conventional measurement method consists of
transporting the vehicle exhaust to a dilution
tunnel, sampling a portion of the diluted ex-
haust onto Ž lter media, and recording the mass
gained on the Ž lters over set phases of a drive
cycle, such as the Federal Test Procedure (FTP).
Though convenient for regulatory purposes, the
mass over a drive cycle provides but one, rather
crude, measure of PM emissions. For a number
of reasons a more complete characterization of
motor vehicle PM is desirable. Particle composi-
tion has been used to ascertain source apportion-
ment of PM emissions in the Los Angeles Basin
(Schauer et al. 1996; Cass 1997). Although at
the present time the mechanism by which par-
ticles adversely affect health remains unknown,
one supposes that it depends on the size and
composition of the particles. From an engineer-
ing standpoint, changes in engine design, or
fuel composition, may affect not only particle
mass emissions, but their size and composition
as well. As one example, a modern heavy duty
diesel engine has been cited to give lower PM
mass emissions, yet with particle numbers equal
to or exceeding those from an older technol-
ogy engine (Baumgard and Johnson 1996). In
another study, dimethoxy methane additive to
diesel fuel was found to reduce PM mass in
1National Ambient Air Quality Standard for Particulate
Matter: Final Rule, Federal Register, 1997, 62, 38652.
Aerosol Science and Technology
33:3 September 2000
the exhaust by reducing particle size, but not
their number (Maricq et al. 1998). Thus a more
complete picture of the nature of particles and
their formation may lead to engine and fuel im-
provements that lower both the mass and number
emissions.
The present paper compares two instruments
that allow the scope of vehicle PM emissions to
be extended in two directions: 1) the determina-
tion of particle size and 2) the second by second
measurement of particle emission rate over a
transient drive cycle. The SMPS is well known
in the aerosol community, but its application to
automobile exhaust, especially transient tests, is
quite recent. The ELPI is a new innovation that
has only been available over the past few years
(Keskinen et al. 1992). Cascade impactors, such
as the MOUDI, have been used to determine
size dependent mass emissions, but these cannot
provide information on transients. Devices such
as the smoke meter and tapered element oscil-
lating mass balance (TEOM) provide transient
data on exhaust opacity and mass, respectively,
but lack particle sizing capability. The electri-
cal low pressure impactor (ELPI) and scanning
mobility particle sizer (SMPS) provide both siz-
ing and transient measurement capability and,
as such, have elicited considerable interest with
respect to motor vehicle PM. A third instru-
ment, the quartz-crystal microbalance (Chuan
1976; Rickeard et al. 1996), measures transient
changes in size selected PM mass emissions,
but it is not considered here. Though the em-
phasis of this paper is on particle size measure-
ment technology, it must be kept in mind that
reliable and accurate vehicle PM emissions data
arguably depend more on proper sampling and
transport of the particle laden vehicle exhaust
than on the instruments themselves (Maricq
et al. 1999a; Kittelson and Abdul-Khalek 1998;
Kittelson et al. 1999).
EXPERIMENTAL METHOD
Vehicle Emissions
The motor vehicle particulate measurements
presented herein are obtained from chassis
Aerosol Science and Technology
33:3 September 2000
TABLE 1. Test vehicles.
Fuel
Vehicle Year # Cyl Inject.a
Diesel
D1 1995 4 IDI
D2 1998 4 DI
D3 1998 4 DI
Gasoline
G1 1997 6 PFI
G2 1997 6 PFI
G3 1996 6 PFI
a DI = direct injection, IDI = indirect injection, PFI = port fuel injection.
dynamometer tests that have been previously de-
scribed (Maricq et al. 1999b). The test vehicles,
described in Table 1, are run on a 122 cm sin-
gle roll, AC electric dynamometer. The exhaust
is transported from the tailpipe through a cor-
rugated stainless steel hose to a dilution tunnel
(particle losses during trasport have been dis-
cussed by Kittelson et al. 1999). Separate trans-
fer hoses and dilution tunnels are used for diesel
and gasoline fueled vehicles. The transfer hose
measures 9.1 cm in diameter and 5.8 m in length
for gasoline vehicles and 10.4 cm in diameter
and 7.6 m in length for diesel vehicles. The res-
idence time of the exhaust in the transfer hose
depends on the exhaust volume, which in turn is
a function of vehicle speed and load. Over the
FTP cycle, the exhaust volume typically varies
between 0.1 m3 /min at idle to 2.5 m3 /min dur-
ing the stronger accelerations. Consequently the
residence time ranges from about 1 to 20 s. At
a steady 50 mph cruise, the exhaust volume is
about 0.63 m3 /min for 4 cylinder engines and
about 0.85 m3 /min for 8 cylinder and light duty
diesel engines; thus the transit time through the
transfer hose is 3 –4 s.
Normally the transfer hose is insulated and
heated (only during the cold start portion of a
test) to prevent water condensation. However,
recent experiments (Maricq et al. 1999a) have
shown that excessive heating of the transfer
hose by vehicle exhaust, which can occur below
150 ±C, can produce large numbers of nanoparti-
cles, on the order of 108 cm ¡ 3 , that are typically
Comparison of ELPI and SMPS 241
Odometer
Test Fuel Miles Transmission Catalyst
Euro. cert. 12,200 5 spd manual Oxidation
Euro. cert. 4,500 5 spd manual Oxidation
Euro. cert. 1,200 5 spd manual Oxidation
EPA cert. 35,500 Automatic Three way
Cal ph 2 refrm 4,200 Automatic Three way
Cal ph 2 refrm 2,900 Automatic Three way
< 30 nm in diameter. This artifact arises from
desorption, and potentially pyrolysis, by the hot
vehicle exhaust of hydrocarbons that have been
deposited on the inner transfer hose surfaces dur-
ing previous vehicle tests. These released hydro-
carbons subsequently nucleate during dilution.
The data presented here has been collected under
conditions for which this transfer hose “artifact”
has been veriŽ ed to be negligible by sampling
PM directly from the tailpipe using an ejector
pump diluter (a high velocity stream of air or
nitrogen past a small oriŽ ce is used to pump
exhaust via the Bernoulli effect and simultane-
ously dilute it).
Upon entering the 30.4 cm diameter stainless
steel dilution tunnel, the vehicle exhaust (typi-
cally containing 13% water vapor for gasoline
engines and < 8% for diesel engines) is turbu-
lently mixed with heated (38±C), Ž ltered, low
humidity air. The total tunnel  ow is held con-
stant at a value between 10 and 30 m3 /min; thus
the dilution ratio depends on exhaust  ow. It
varies between about 3 and 120 over the FTP cy-
cle. For a 70 mph steady state cruise it is roughly
a factor of 8. At a point more than 10 tunnel
diameters downstream, a portion of the diluted
exhaust is sampled through a 0.9 cm diameter
j-shaped probe pointing upstream into the  ow.
For gasoline vehicle tests, the sample is split into
a 0.4 L/min  ow for the SMPS and a 10 L/min
 ow for the ELPI. In the case of diesel vehicles,
an ejector pump provides secondary dilution by
a factor of 8, before introducing the sample into
242 M. M. Maricq et al.
the particle sizing instruments. Though the sam-
pling is not isokinetic, this has relatively little
impact on particles in the 10 –500 nm range that
are typical of motor vehicle exhaust.
PSL Tests
While the emphasis of this paper is particle size
measurements of vehicle exhaust, it is instruc-
tive to examine the response of the ELPI and
SMPS to aerosols of polystyrene latex (PSL)
spheres. Unlike exhaust PM, PSLs have very
narrow size distributions, with widths of only
a few nanometers, which makes them useful
for size calibration. The aerosols are generated
by diluting the PSLs (Duke ScientiŽ c) into dis-
tilled water and atomizing the resulting suspen-
sion (model 9302a atomizer, TSI) with a 5 std
L/min  ow of particle-free nitrogen. The aerosol
is dried (model 3062 diffusion drier, TSI) and di-
luted with nitrogen to bring the total  ow up to
>10 std L/min. It is then sampled simultane-
ously by the ELPI and SMPS.
INSTRUMENT DESCRIPTION
SMPS
To make the comparison of particle size mea-
surements more meaningful, we present a brief
overview of the operating principles of the two
instruments. The SMPS (TSI model 3934L)
consists of a 85 Kr bipolar charger, an elec-
trostatic classiŽ er, and a condensation nuclei
counter (CNC). The sample aerosol is Ž rst
brought to a Boltzmann charge distribution by
beta emission from the 85 Kr source (Liu and Pui
1974; Wiedensohler 1988). The probability of
Ž nding a particle with + 1 (or ¡ 1) charge in-
creases with its diameter from a probability of
0.09 at 20 nm to 0.23 at 130 nm. After this,
the fraction of + 1 (and ¡ 1) charged particles
decreases owing to increasingly facile multiple
charging (§2, §3, etc.) of the larger particles.
This complication limits SMPS measurements
to particles below » 1000 nm in diameter.
The electrostatic classiŽ er consists of a
43.6 cm annular cavity formed by two concen-
Aerosol Science and Technology
33:3 September 2000
tric cylinders (0.937 cm o.d. and 1.958 cm i.d.),
across which an electric potential is placed. Be-
tween the cylinders  ows a sheath gas of Ž l-
tered air (at 2.0 –20 std L/min) and the poly-
disperse aerosol (at 0.2 –2.0 std L/min). The
charged sample aerosol is introduced along the
inner wall of the outer electrode. As the posi-
tively charged particles are accelerated toward
the inner electrode by the electric Ž eld, they
experience drag due to the sheath gas. Conse-
quently, they quickly reach a terminal radial ve-
locity that depends on the particle’s electrical
mobility (Willeke and Baron 1993). Depend-
ing on the voltage applied across the cylinders,
only particles within a narrow range of electri-
cal mobility, and therefore diameter, will follow
the required trajectory to pass through the exit
aperture of the classiŽ er (Knutson and Whitby
1975). For slowly changing aerosols, such as
motor vehicle exhaust during steady state op-
eration, Wang and Flagan (1990) have shown
how particle size distributions can be obtained
by scanning the voltage across the classiŽ er.
During transient operation, motor vehicle par-
ticle emission rates vary too rapidly to permit
size distribution measurement by scanning the
SMPS. Instead, the voltage on the classiŽ er is
Ž xed to transmit a narrow distribution of particle
sizes throughout the entire drive cycle. Distribu-
tions of particle number versus size and time are
subsequently constructed from 4–8 time traces
at Ž xed sizes in the 20 nm to 500 nm diame-
ter range. For each such trace, the raw particle
count rate, C(t, D p ), is recorded at 2 s intervals
and converted to a differential tailpipe emission
rate via
dN(t ) C(t, D p )T (D p )q T a C ( 1)
= e ,
d log(D p ) qa f ( + 1)e i e c
where N (t ) represents the tailpipe particles
per second, T (D p ) is the transmission function
of the classiŽ er (approximated as a triangle,
2/D (logD p )), qT is the tunnel  ow, qa is the
aerosol sample  ow, f ( + 1) is the size depen-
dent fraction of particles with a single positive
charge, and e c and e i are, respectively, the efŽ -
ciencies of the condensation nuclei counter and
Aerosol Science and Technology
33:3 September 2000
the impactor at the entrance of the classiŽ er. The
factor ea C provides a coincidence correction for
high particle count rates (a = 4 £ 10 ¡ 7 s).
The SMPS used in the present study em-
ploys the model 3010 CNC to count the parti-
cles size selected by the classiŽ er. The counting
efŽ ciency of this model drops below 50% for
particles smaller than about 12 nm. It is pos-
sible, as discussed by Mertes et al. (1995), to
reduce the lower limit to about 6 nm by increas-
ing the temperature difference between saturator
and condenser from 17±C to 25±C. The 1/e time
response of the 3010 CNC is approximately 2 s,
after subtracting the delay associated with the
aerosol  ow through the counter.
ELPI
The electrical low pressure impactor (Dekati,
Tampere, Finland) is based on a design by
Keskinen et al. (1992) (Kymäläinen et al. 1996).
The principal components include a corona dis-
charge, Berner low pressure impactor, and a
series of electrometers. The diode type corona
discharge provides unipolar charging of the par-
ticles in the sample aerosol. It is coupled with
a trap which removes ions and small (< 20 nm)
particles that can otherwise produce extraneous
currents at the electrometers. The amount of
charge accepted by the particle increases with
its mobility diameter. For particles < » 200 nm
diameter, the principal mechanism is diffusion
charging, which is independent of material prop-
erties (Hinds 1982). The charging efŽ ciency is
given empirically by the segmented power law
X(D p ) = a D bp , (2 )
where a = 277.52 and b = 3.178 for D p <
0.048 l m, a = 3.557 and b = 1.741 for 0.048
< D p < 0.15 l m, and a = 1.335 and b =
1.241 for D p > 0.15 l m. Recently, Marjamäki
et al. (1999) have determined a somewhat differ-
ent set of parameters a and b, which they found
to be the same for NaCl and dioctyl sebacate
aerosols.
After charging, the aerosol proceeds through
a thirteen stage Berner cascade impactor oper-
Comparison of ELPI and SMPS 243
ating at 100 mTorr and a nominal  ow rate of
10 std L/min, where particles are separated ac-
cording to aerodynamic diameter. The impactors
cover the size range of 37 nm to 10.5 l m, with
D50% cut points of 37 nm, 63 nm, 119 nm,
187 nm, 283 nm, 433 nm, 698 nm, 1.08 l m,
1.75 l m, 2.67 l m, 4.33 l m, 6.94 l m, and
10.54 l m, respectively, for stages 1 –13 (in the
text, stages are referred to by their D50% cut
points). Calibration of the impactor stage cut-
off curves has been discussed by Marjamäki
et al. (1999). These authors also measure the ef-
Ž ciency of the diode charger trap and Ž nd it to be
lower than speciŽ ed by the manufacturer for par-
ticles larger than 2 l m in diameter; however, this
is of little consequence for vehicle tailpipe PM.
Each of the twelve lower stages is connected
to an electrometer that measures the current de-
posited from particle impaction. In principle,
knowing the charging efŽ ciency, Equation (2),
one can deduce the size dependent rate of parti-
cle emissions from the impactor stage currents.
In practice, there are a some subtle issues to
be considered. The Ž rst involves the distinc-
tion between aerodynamic diameter and mobil-
ity diameter. The currents on the impactor stages
depend on the distribution of aerodynamic di-
ameters in the aerosol sample. However, the
charging efŽ ciency depends on the mobility dia-
meter.
Reconciliation of this difference in particle
properties requires knowing the effective par-
ticle density, which in the case of vehicle ex-
haust is itself likely dependent on particle di-
ameter (one can imagine that the small primary
particles composing soot have higher effective
density than larger particles formed by their ag-
glomeration). In principle, one can determine
the density by combined inertial and mobility
measurements on the sample aerosol (Kelly and
McMurry 1992). Following this idea, Ahlvik
et al. (1998) measured the effective density of
diesel PM using a tandem combination of SMPS
and ELPI. This approach is used in the present
work to show that mobility selected particles
have a distribution of effective densities. How-
ever, we Ž rst present a direct comparison of
244 M. M. Maricq et al.
the ELPI aerodynamic size distributions to the
SMPS mobility size distributions and then ad-
dress the issue of mobility versus aerodynamic
size measurement.
The second complication concerns the need
to correct the currents on the upper, large par-
ticle, impactor stages for small particle losses
that occur as the aerosol passes through. The
losses occur both because of diffusion and elec-
trostatic forces experienced by the particles. An
empirical correction algorithm is employed by
the ELPI software to account for the stage by
stage losses. The corrections can be signiŽ cant
for the Ž rst few stages in the original impactor
design, due to charging of the te on used to insu-
late between stages. The newer, metal shielded,
te on insulators require smaller corrections for
small particle loss, as discussed below.
Particle bounce presents a third difŽ culty,
since it transfers charge from one stage to an-
other stage that is meant for smaller particles.
The present study utilizes the greased aluminum
foil substrates recommended by the manufac-
turer, in which an Apiezon grease/CCl 4 slurry
is painted onto the foils (about 0.2 –0.4 mg of
grease). This method may not be equally effec-
tive in preventing bounce for all types of par-
ticles. It should be relatively good for diesel
exhaust PM, which because of its organic con-
tent is inherently somewhat sticky. This is cor-
roborated by transient FTP cycle gasoline vehi-
cle PM measurements compared using the bare
impactors, greased foils, and Ž lter paper sub-
strates that showed consistent results within the
expected test to test variability. The greased foils
may be less effective for harder, drier aerosols
such as minerals or PSLs.
A fourth consideration concerns transient PM
emissions measurements. In this case, the ELPI
can show both positive and negative apparent
aerosol concentrations. There is also a time
alignment issue arising from the successive
traversal of the impactor stages by the sample
aerosol and the effect that this has on the con-
version of impactor current to particle concen-
tration.
Aerosol Science and Technology
33:3 September 2000
STEADY STATE MEASUREMENTS
PSLs
Figure 1 illustrates number and volume we-
ighted size distributions for 240 nm and 503 nm
PSLs as recorded by the ELPI and SMPS. It
is immediately obvious, particularly in the case
of the 240 nm PSLs, that the number weighted
size distributions recorded by the two instru-
ments differ signiŽ cantly. In large part, this is an
overly severe test of the ELPI. The PSL spheres
comprise the minority of the atomized particles.
The majority background particles are presum-
ably formed from residual salts that remain dis-
solved in the distilled water used to suspend the
PSLs and/or from chemicals used to stabilize
the concentrated PSLs. By virtue of the very
narrow distribution in PSL particle size, they
fall into 1 –2 bins of the high resolution SMPS
distribution (D logD p = 0.031) and are readily
visible against the relatively small fraction of
background particles also falling into this nar-
row size range. In contrast, the ELPI has nearly a
factor of 10 lower resolution (D logD p = » 0.2);
thus, the contribution of the PSLs to an im-
pactor stage is a factor of 10 smaller relative
to the background PM impacting that stage.
Also, possibly due to particle bounce, the 240
nm PSLs are split between the 187 nm and
283 nm stages of the ELPI, further diluting
their impact on the appearance of the size dis-
tribution.
Despite the disparity in distributions, the
PSL particle numbers registered by the ELPI
(corrected for small particle loss, as discussed
below) and SMPS (corrected for multiple charg-
ing) are in reasonable accord, especially in the
503 nm PSL case. The average number of par-
ticles on the 187 nm and 283 nm stages is about
20% lower than the area under the 240 nm SMPS
peak, whereas the number of particles on the
433 nm stage is about equal to the area under
the 503 nm SMPS peak. Why the background
particles appear 3–5 times more prevalent in the
ELPI measurements is unclear. One factor that
may be relevant, particularly at the low particle
Aerosol Science and Technology
33:3 September 2000
FIGURE 1. Comparison of SMPS and ELPI measurements of PSL size distributions.
concentrations in Figure 1, is that the effects of
electrical noise and electrometer offsets become
progressively larger as particle size decreases.
Random  uctuations from noise and slow drifts
in the electrometer zero points are presumably of
the same magnitude for each impactor stage, i.e.,
the current on the nth stage is I n § D I . Accord-
ing to Equation (2) this translates into an uncer-
tainty in particle number of D Nn = D I / X(D p ).
Inserting the expressions for X (D p ) given the
above reveals that D N 1 /D N6 = 35 for the un-
certainty in ELPI particle number at 48 nm rel-
ative to the uncertainty at 550 nm.
Particle bounce may also play a role. PSLs
that don’t stick to the impactor stage for which
they are meant, transfer charge to the smaller
particle stages. The increase is more than pro-
portional to the number of particles that bounce,
since these carry more charge than those par-
ticles intended to impact on a particular stage.
Comparison of ELPI and SMPS 245
The bounce problem is expected to worsen to-
wards the smaller particle stages owing to the
increasing impactor jet velocities (Marjamäki
et al. 1999). This, too, is consistent with the ob-
servation in Figure 1 that the discrepancy be-
tween ELPI and SMPS measurements of the
PSLs is greater (smaller PSL peak and higher
small particle background) for the 240 nm PSLs
as compared to the 503 nm size.
The ELPI and SMPS volume distributions il-
lustrated in Figure 1 (B & D) appear in better
accord because the D 3p weighting reduces the
importance of the smaller size background par-
ticles relative to the PSLs. Actually, the ELPI
overestimates by 35% the 240 nm PSL volume,
and by about 50% the 503 nm PSL volume,
relative to the corresponding peak areas in the
SMPS volume distributions. Also, the 240 nm
PSL peak in the SMPS spectrum appears shifted
relative to its ELPI counterpart. The 1.05 g/cm3
246 M. M. Maricq et al. Aerosol Science and Technology
33:3 September 2000

density of the PSLs leads to a mobility diameter
that is 8 nm smaller than the aerodynamic di-
ameter at 250 nm. This only slightly improves
the shift between SMPS and ELPI peaks. An-
other factor that may in uence both the shift
and relative intensities is the small particle loss
correction made by the ELPI, which is discussed
further below.
Vehicle Exhaust PM Emissions
Because engine development is usually con-
ducted at Ž xed speed and load, whereas emis-
sions regulations are based on transient drive cy-
cles, both types of PM measurements are
discussed in this paper: steady state tests here
and transient tests in a separate section below.
Steady state light duty diesel exhaust PM size
distributions recorded by the ELPI and SMPS
are compared in Figure 2 (A & C) and Fig-
ure 3. Six distributions, taken from tests sepa-
rated by two weeks, are overlayed in each panel
of Figure 2 to illustrate experimental variabil-
ity. The tests employed a European diesel fuel
(65.9% saturates, 5.5% oleŽ ns, 28.6% aromat-
ics, with a sulfur content of 0.034 wt%). Figure 3
contrasts the particle emissions for this base fuel
versus a 30% dimethoxy methane (DMM)/base
fuel blend (Maricq et al. 1998).
The number (volume) distributions are given
in terms of the rate of particles (particle volume)
exiting the tailpipe. These units are natural for

FIGURE 2. Comparison of ELPI and SMPS measurements of particles in diesel exhaust under steady state vehicle
operation. Panels A and B show number weighted distributions. Panels C and D give the corresponding volume
weighted distributions. All of the SMPS data is plotted versus mobility diameter; however, the ELPI data is presented
as a function of aerodynamic diameter in Panels A and C. These data are corrected to mobility diameter in Panels B
and D.
Aerosol Science and Technology
33:3 September 2000
FIGURE 3. ELPI and SMPS examination of the effect of dimethoxy methane fuel additive on diesel PM emissions.
a dilution tunnel operating at a constant total
(exhaust + diluent)  ow rate. At 60 mph, the ve-
hicle exhaust  ow is » 1.3 m3 /min; thus the ex-
haust particle number concentration in Figure 2
is » 0.9 £ 108 particles/cm 3 at 60 mph.
Although the ELPI and SMPS size distri-
butions are superimposed on the same plots,
the size axis has a different meaning for the
two instruments. For the ELPI, where particles
are separated by impaction, the distributions
are a function of aerodynamic diameter. For
the SMPS, where particles are segregated
in an electrical Ž eld, they are a function of
mobility diameter. Ignoring this distinction for
Comparison of ELPI and SMPS 247
the moment, the ELPI and SMPS distributions
appear generally in good agreement. The ELPI
tends to overestimate the number of particles
on the 37 nm and, sometimes, the 63 nm stages
(e.g., Figure 3A). Volume weighting accen-
tuates differences at larger particle diameters
(e.g., Figures 2C and 3B). However, both
instruments reveal in Figure 3 that the addition
of DMM to the diesel fuel only slightly reduces
particle number emissions and that the major
effect is a » 30 nm reduction in particle size.
Both instruments indicate that DMM causes
particle volume emissions to decrease to about
1/3 of the base fuel value.
248 M. M. Maricq et al.
The origins of the discrepancies between
ELPI and SMPS size distributions arise from
a number of contributing factors. One difŽ -
culty is that the instruments measure two dif-
ferent aspects of particle size. Another is the
small particle loss correction that the ELPI
makes. These are discussed in detail below and
IVD. Particle bounce poses a third factor that
may be suspected in the higher than expected
particle concentrations recorded by the 37 nm
stage.
A fourth factor is that both instruments rely on
charging the particles to measure their number
(or volume), and this depends on particle size.
The charging efŽ ciency for the ELPI has a power
law dependence on size given by Equation (2).
For the SMPS, the fraction of + 1 charged
particles obeys a Boltzmann distribution. In
either case, charging efŽ ciency decreases in a
nonlinear fashion with decreasing particle size,
but the effect is more dramatic for the ELPI.
Relative to the peak in the diesel PM size dis-
tributions at about 100 nm, the charging efŽ -
ciency at 50 nm is 3 times lower for the ELPI,
but only 30% lower for the SMPS. Thus elec-
trometer noise in the ELPI will have a relatively
larger impact on the accuracy of measuring the
numbers of small particles than a deterioration
in counting statistics will have for the SMPS.
The ELPI is also susceptible to slow drifts in
the electrometer zero values, which lead to suc-
cessively larger systematic uncertainties for the
smaller particle impactor stages. This can be al-
leviated by frequent checks of the electrometer
zero points by momentarily replacing the test
aerosol with particle free air.
Mobility Versus Aerodynamic Diameter
A true comparison between ELPI and SMPS
size distributions requires knowledge of parti-
cle density as a function of its diameter. This is
accomplished by assuming that the particle den-
sity reported in the study of Ahlvik et al. (1998),
which decreases from about 1.5 g/cm3 at a mo-
bility diameter of 30 nm to 0.5 g/cm3 at Dmob =
300 nm, applies to the diesel PM measured in
Aerosol Science and Technology
33:3 September 2000
the present work. The density affects the con-
version from aerodynamic to mobility diameter
in two ways: First, the diameter axis scales as
³ ´
q 0 Cc (Daero ) 1/ 2
Dmob = Daero , ( 3)
q e C c (Dmob )
where C c = 1 + 2.284 k / D p + 1.116 k / D p
exp(¡ 0.500 D p /k ) is the Cunningham slip
correction (Willeke and Baron 1993), q e is the
effective particle density, q 0 = 1 g/cm3 repre-
sents unit density, and k is the mean free path
(6.65 £ 10 ¡ 6 cm for air at 1 atm). Because C c
depends on particle size, this conversion must be
done iteratively. Qualitatively, if q e > 1, the mo-
bility diameter is smaller than the aerodynamic
diameter and vice versa for q e < 1. Second,
the density affects the charging efŽ ciencies as-
signed by the ELPI software to various particle
sizes. Thus when q e > 1, the mobility size is
smaller and, hence, the charging efŽ ciency is
lower than anticipated by the ELPI. Again, the
reverse is true for particles with q e < 1.
The net effect on the ELPI data of the trans-
formation to mobility diameter is evident upon
contrasting the data in Figures 2A and C with
the corresponding data in Figures 2B and D. In
Figures 2B and D, Equation (3) has been used
to replot the ELPI size distributions as a func-
tion of mobility diameter, and corrected parti-
cle number and volume values have been de-
termined using a charger efŽ ciency based on
Dmob and not Daero . The outcome is an increased
discrepancy between SMPS and ELPI distri-
butions, both for particle number and volume.
For the particles impacting on the 37 nm and
63 nm stages q e > 1; thus for the D50% = 37 nm
stage, the transformation to mobility diameter
decreases the midpoint diameter from 48 nm to
34 nm and increases particle number by a factor
of X(48 nm)/X(34 nm) = 3. For the D50% =
63 nm stage, the midpoint diameter decreases
from 87 nm to 66 nm and particle number in-
creases by the ratio X(87 nm)/X(66 nm) = 1.6.
For particles larger than » 300 nm, q e < 1; thus
the data corresponding to the D50% = 283 nm
impactor stages and above shift to larger diame-
ter, from 350 nm to 475 nm for the 283 nm stage,
Aerosol Science and Technology
33:3 September 2000
and the particle numbers decrease by a factor of
X(350 nm)/X(475 nm) = 0.7. This shift to larger
particles combined with a decrease in number
mimics the approximately log-normal shape of
the size distributions; thus the converted ELPI
data on the large diameter side of the distribu-
tions remain in good agreement with the SMPS
data.
Placing the ELPI and SMPS distributions on
the equal footing of mobility diameter increases
the disparity between the two sets of measure-
ments. This is true of the diesel vehicle PM emis-
sions presented in Figure 2, as well as gasoline
vehicle particle emissions. The present conclu-
sion is in contrast with the results of Ahlvik et al.
(1998), where the ELPI distributions plotted as
a function of aerodynamic diameter underesti-
mated the SMPS measurements at small particle
diameter and for which the transformation of the
ELPI data to a mobility diameter improved the
agreement. The reasons for this are uncertain.
One possibility, considered below, is that parti-
cles impacting on a particular stage do not all
have the same density.
ELPI Distributions of Mobility Selected
Diesel PM
One way to investigate the issue of aerodynamic
versus mobility diameter is via a combined
SMPS/ELPI measurement of diesel particulate
matter (Ahlvik et al. 1998). The SMPS samples
the diesel exhaust and generates a monodisperse
aerosol having a well-deŽ ned mobility diameter.
The monodisperse aerosol is then sized aero-
dynamically using the ELPI. For these experi-
ments, the SMPS sheath and aerosol  ow rates
are set to 10 L/min and 1 L/min, respectively,
which provides a sufŽ cient total  ow to fulŽ ll
the 9.5 L/min requirement of the ELPI. The re-
sults are displayed in Figure 4.
The solid curve in each panel depicts the
mobility size distribution of the test diesel ex-
haust PM. The individual panels illustrate aero-
dynamic size distributions (bar graphs) recorded
with mobility diameter set to near the impactor
midpoints of the four lowest ELPI stages, which
Comparison of ELPI and SMPS 249
range from 48 nm to 240 nm. The conversion
of the electrical currents registered on the im-
pactor stages to particle number does not use
the conventional algorithm employed by the
ELPI, which bases particle charging efŽ ciency
on aerodynamic diameter. Instead, the mobil-
ity diameter selected by the SMPS determines
the charging efŽ ciency; thus at a given mobility
diameter the efŽ ciency is the same for all im-
pactor stages. It varies from X(Dmob ) = 0.018
at Dmob = 48 nm (top left panel) to X(Dmob ) =
0.216 at Dmob = 240 nm (lower right panel).
The ELPI number distributions have been scaled
to account for the 8.5:1 dilution of the monodis-
perse aerosol and for the SMPS transmission
function, assumed to be triangular with a full
width at half height of dlog(D p ) » = 0.05.
If diesel soot were spherical with a density
of 1 g/cm3 , and if the impactor cutoff curves
were ideal, each of the mobility selected aerosols
would register on a single ELPI impactor stage,
but Figure 4 shows that this is not so. Though
steep, the impactor efŽ ciency curves are not in-
Ž nite. Measurements by Marjamäki et al. (1999)
show that for the lower stages, if 90% of the par-
ticles impact on stage i, approximately 15% will
impact on stage i + 1. For this reason, and be-
cause of small particle losses and bounce, some
current will appear on neighboring stages; still,
the assumption of unit density spheres would
imply a narrow ELPI distribution.
Instead, at Dmob = 48 nm, particles range in
aerodynamic size from 48 nm to 149 nm, al-
though owing to the low charging efŽ ciency of
48 nm particles the aerodynamic distribution at
this mobility is rather susceptible to electrometer
noise and offsets. At Dmob = 48 nm, the calcu-
lated arithmetic mean aerodynamic diameter is
61 nm (93 nm if the negative particle numbers
recorded by the 187 nm and 283 nm stages are
omitted), but this is likely an overestimate since
particles smaller than 30 nm are not recorded
by the ELPI. Particles with Dmob = 87 nm range
from 48 nm to > 350 nm in aerodynamic size, but
the upper stage currents may arise from losses
of small particles. The mean aerodynamic di-
ameter of h Daero i = 116 nm is about 30% larger
250 M. M. Maricq et al. Aerosol Science and Technology
33:3 September 2000

FIGURE 4. Aerodynamic size distributions of mobility size selected diesel exhaust particles. The solid lines represent
the SMPS measurement of mobility diameter. Arrows indicate the mobility size and approximate SMPS transmission
window selected in each panel. Histograms depict ELPI measurements of aerodynamic diameter. The impactor currents
are converted to particle number by dividing by the charger efŽ ciency based on the mobility diameter and not, as done
by the ELPI, based on the impactor midpoint diameter. The horizontal axis label Dp represents mobility diameter
for the SMPS measurement and aerodynamic diameter for the ELPI distributions. Uncertainties in h Daero i represent
measurement variations during the same vehicle test. Test to test variations could easily double this.

than the mobility size. At Dmob = 155 nm, a sim-
ilarly broad aerodynamic distribution is found,
but it is shifted to somewhat larger particles. The
mean aerodynamic diameter of 130 nm is now
slightly smaller than the corresponding mobil-
ity diameter. For mobility diameters larger than
about 150 nm, the aerodynamic diameter falls
progressively further behind; thus at Dmob = 240
nm, h D aero i = 133 nm and at Dmob = 325 nm,
h Daero i = 106 nm, though the last value has sig-
niŽ cant uncertainty owing to the very small frac-
tion of diesel exhaust particles at 325 nm. The
above averages are given as arithmetic means.
The geometric means are not much different;
about 11% higher than the arithmetic mean for
Dmob = 48 nm and 8% lower for Dmob ¸ 87 nm.
As a matter of consistency, note that integrat-
ing each of the aerodynamic distributions over
size approximately reproduces, to within 10%
to 30%, the number of particles at the indicated
mobility diameter displayed by the SMPS dis-
tribution.
Selecting the mobility diameter and measur-
ing the distribution of aerodynamic diameters
Aerosol Science and Technology
33:3 September 2000
FIGURE 5. Diesel exhaust particle density as a function
of mobility diameter. Vertical bars represent § 1 stan-
dard deviation of the density distribution as determined
by the mobility selected aerodynamic size distributions
in Figure 5. The open symbol represents the effect of
omitting the negative particle concentrations recorded
by the 187 nm and 283 nm ELPI stages for the 48 nm
mobility selected particles. The arrow indicates the den-
sity of graphite.
permits the distribution of effective particle den-
sities to be calculated using Equation (3). The
arithmetic average densities are plotted versus
mobility diameter in Figure 5. The densities are
somewhat sensitive (§20%) to whether one at-
tributes the particles registered on the 283 nm
stage and higher to truly aerodynamically large
particles or to small particles lost on these stages
due to electrostatic forces and diffusion. The
density of Dmob = 48 nm particles exhibits a
large variation depending on whether (Ž lled cir-
cles) or not (open circle) the 187 nm and 283 nm
stage data in Figure 4 are included. Further-
more, the density at this mobility could fall
lower than indicated depending on how many
have aerodynamic diameters below 30 nm. As
shown by Figure 5, the decrease in particle den-
sity with increasing mobility diameter observed
in this work is in good agreement with the re-
Comparison of ELPI and SMPS 251
sults of Ahlvik et al. (1998). But the present
work shows that the trend applies only to the
average particle density. Actually, at each mo-
bility diameter there is a wide range of parti-
cle densities, as indicated by the vertical bars,
that spans a major portion of the spectrum of
diesel exhaust particle size. This is consistent
with the fractal morphology attributed to diesel
exhaust PM.
ELPI Small Particle Loss
Diffusion and electrostatic forces cause losses
of small particles as they pass through the upper
stages of the cascade impactor. This distorts the
size distribution from its true form, shifting it
to larger size. An empirical algorithm subtracts
the unwarranted impactor currents that occur
from the loss of 37–63 nm particles as they pass
through the 63 nm and higher stages, for the loss
of 63–119 nm particles as they pass through the
119 nm and higher stages, etc., and augments the
less than expected currents on the lower stages
that arise because of these losses. The extent of
the required corrections depends on whether the
original te on or the new metal shielded insula-
tors are used to electrically isolate the impactor
stages.
Figure 6 portrays the effect of the small par-
ticle loss correction on diesel exhaust PM size
distributions for both sets of insulators. Note that
two different diesel vehicles, each run at a steady
state 60 mph, were employed for tests of the old
and new insulators. Though the overall emis-
sion levels are roughly a factor of two differ-
ent, the relative effects of the loss correction re-
main well illustrated. For the old insulators, the
correction increases the particle numbers reg-
istered by the 37 nm and 63 nm ELPI stages
by 36% and 24%, respectively. Because the
metal shielding reduces the electrostatic losses
that arise from charging of the te on insulators,
the corrections to particle number for these two
stages fall to 13% and 5% when using the new
insulators.
In contrast to the moderate effect on particle
number, the correction can have a substantial
252 M. M. Maricq et al. Aerosol Science and Technology
33:3 September 2000

FIGURE 6. Effect of the ELPI small particle loss correction on diesel vehicle exhaust PM. Tests were conducted at a
steady state 60 mph using different vehicles for the two sets of insulators. Raw and corrected number (panels A and
B) and volume (panels C and D) distributions are compared using the old te on insulators (panels A and C) versus
the new metal shielded insulators (panels B and D).

effect on particle volume at large particle diame-
ters. The example in Figure 6 represents a “worst
case” scenario in which essentially no particles
above 1 l m are present in the aerosol, but large
numbers of small particles exist. With the old in-
sulators, the apparently large “negative” particle
volumes arise either from an over-correction of
the small particle loss, or from small electrom-
eter zero offset errors, that are exacerbated by
weighting for particle volume. As with parti-
cle number, the correction to particle volume
is smaller when using the new insulators. In
this example, either the electrometer zero off-
sets happen to be positive or there is an under-
correction of the losses.
While the new insulators are desirable from
the point of view that they reduce the errors as-
sociated with losing particles in the upper stages
and then having to correct for this, it is clear that
they cannot overcome the problem that volume
weighting greatly ampliŽ es the effects of noise
and electrometer zeroing on the concentrations
of large particles. The effect of the electrometer
offsets on the volume distribution needs to be
kept in mind when measuring vehicle exhaust,
since it contains high numbers of Ž ne and very
few coarse particles. It becomes less of an issue
as the fraction of large particles in the sample
aerosol increases.
TRANSIENT PM EMISSIONS
MEASUREMENTS
PM emissions regulations are typically based on
transient drive cycles, such as the FTP, US06,
Aerosol Science and Technology
33:3 September 2000
and ECE. To monitor particle emissions under
such circumstances requires a time response of a
few seconds or less. As explained above, the 30 s
minimum scan time of the SMPS necessitates
that size distributions be constructed from repeat
tests at Ž xed particle size. In contrast, the ELPI
provides second by second size distributions,
thereby signiŽ cantly reducing test time require-
ments. Transient operation, however, introduces
a number of new issues to the measurement
process.
The Ž rst is that the time response of the ELPI
depends on the sensitivity range of the instru-
ment, as illustrated by Figure 7 for the D50% =
Comparison of ELPI and SMPS 253
FIGURE 7. ELPI transient response at
the various input sensitivity settings.
This example is of gasoline vehicle PM
emissions over the Ž rst 100 s of the FTP
drive cycle.
63 nm stage. Choosing progressively higher sen-
sitivity results in a loss of time response, which
decreases from approximately 1 s for the 400 pA
range to about 20 s at the 10 pA range. Whereas
both the inherent time duration of the PM emis-
sions and the response function of the ELPI com-
bine to determine the peak widths, the instru-
ment response clearly dominates for the 40 pA
and 10 pA scales. To minimize the instrumental
contribution to the peak widths, the remainder
of the transient work discussed below utilizes
the 400 pA sensitivity range.
Though it is useful to think of the current
recorded on an ELPI stage as arising from the
254 M. M. Maricq et al. Aerosol Science and Technology
33:3 September 2000

FIGURE 8. Responses of the 4.3 ¹ m and 63 nm ELPI stages to bursts of particles emitted by a light duty diesel vehicle
driven over the ECE cycle. Panels A and B: old insulators. Panels C and D: metal shielded insulators. Panels E and F:
vehicle speed.

charge that is deposited by the impacting parti-
cles, this is an oversimpliŽ cation. Figure 8 con-
trasts the responses of the 4.3 l m and 63 nm
stages to diesel exhaust PM measured over the
ECE drive cycle. While the lineshapes regis-
tered by these two stages are very different, both
traces correlate with vehicle acceleration. As can
be anticipated from Figures 2, 3, and 6, diesel
exhaust contains virtually no » 5 l m particles.
The response of the 4.3 l m stage arises not from
charged particles impacting on it, but rather from
their passage through the impactor, which acts as
a Faraday cage. Acceleration of the vehicle gen-
erates narrow pulses of particulate emissions,
which are sampled and charged by the ELPI.The
passage of these pulses of 20 –300 nm charged
particles through the 4.3 l m stage appears to the
electrometer as an alternating current (AC) and
gives rise to the characteristic “derivative” line-
shape. In contrast, the 63 nm stage lies near the
peak in the diesel PM size distribution. The cur-
rent on this stage does arise from the impacting
charged aerosol particles and, therefore, yields
a series of strictly positive peaks proportional
Aerosol Science and Technology
33:3 September 2000
to the particle emission rate during the drive
cycle.
The AC response of the 4.3 l m stage ap-
pears smaller when using the metal shielded as
opposed to the original te on insulators. Since
this response arises from passage through the
impactor stage, one would expect it to be the
same for both sets of insulators. Partly the AC
response is smaller because the particle emis-
sions were smaller during the test with the metal
shielded insulators, as evident by the smaller
peaks recorded by the 63 nm stage for the new
versus old insulators. Whether the redesigned
insulators themselves reduce the AC response
remains unclear.
FIGURE 9. Expanded view of ELPI response to transient particulate emissions.
Comparison of ELPI and SMPS 255
During passage of Ž ne particle pulses through
the upper ELPI stages, a fraction is lost by dif-
fusion and electrostatic forces. The result is an
asymmetry in the “derivative” lineshape, with
the negative branch smaller than the positive
branch owing to the deposition of some small
particles. As evident from Figure 8, the extent
of asymmetry is quite small; yet it is this differ-
ence, the net current, that must be corrected by
the small particle loss correction. A complica-
tion arises, as shown by the expanded view in
Figure 9, from the time required by the parti-
cle pulse to traverse the cascade impactor. The
“derivative peak” registered by the 6.9 l m stage
occurs almost 4 s earlier than the current peak
256 M. M. Maricq et al.
arising from impaction of particles on the 37 nm
stage; thus corrections for small particle loss
must account for the time delay between the cur-
rents registered on succeeding impactor stages.
There are in general two types of corrections:
reductions to the currents registered by the upper
stages that compensate for diffusional and elec-
trostatic losses of small particles not intended to
impact on these stages, and increases to the cur-
rents recorded by the lower stages that account
for the particles that do not reach these stages.
In the former case, one must estimate the re-
duction to the current on stage m, D I m (t ), from
the current on stage n at a future delayed time,
i.e., from I n (t + (m ¡ n)/ 3) assuming a constant
aerosol  ow rate through the cascade impactor
( » 1/3 s per stage). However, the increase to I n (t )
due to losses from the particle burst during pas-
sage through the preceding stages is based on
the number of particles in the burst; the delay is
not relevant.
This has the following implications for ELPI
measurements of transient motor vehicle ex-
haust PM emissions. The number weighted size
distributions are dominated by particles less
than about 300 nm, i.e., those impacting the
lowest 5 stages. The principal corrections to
these stages are from particles lost on the upper
states. These corrections are small, comparable
to those for the steady state measurements in
Figure 6 (< » 36% for the te on insulators and
< » 13% for the metal shielded insulators), and
they are largely unaffected by the time delay
through the impactors. In contrast, the correc-
tions to the large particle volumes, already sub-
stantial as illustrated in Figure 6, are exacerbated
by the requirement for time alignment of the
corrections.
A transient number weighted distribution of
gasoline vehicle PM emissions recorded by the
ELPI is compared in Figure 10, for phase 1 of the
FTP cycle, to a SMPS distribution constructed
from seven such tests. As already illustrated by
Figure 8, the narrow peaks in PM number emis-
sions over time occur during vehicle accelera-
tion. These peaks appear nearly twice as intense
in the ELPI size distribution as compared to the
Aerosol Science and Technology
33:3 September 2000
peaks in the SMPS distribution. Three factors
contribute to this. First, in this example the ELPI
size distribution peaks at the 37 nm stage, which
typically overestimates the particle number rel-
ative to the SMPS measurement.
A second factor concerns the effect that par-
ticles smaller than the 37 nm lower limit of the
ELPI, but larger than the 20 nm particles re-
moved by the trap, have on the lowest few stages
as they pass through. Judging from Figures 2, 3,
and 11 (below), particles smaller than 37 nm in
diameter constitute 10 –20% of the total particle
number. These contribute a “derivative” shaped
transient superimposed on the positive going
peaks generated by the particles impacting on
these stages. This composite would contribute
to higher than expected peak heights.
The instrument time response of the ELPI rel-
ative to the SMPS is a third, and perhaps the
most important, factor in uencing the relative
peak heights in the three-dimensional distribu-
tions of Figure 10. As illustrated by Figure 10C,
the peaks in particle emissions that occur during
the transient drive cycle are about 50% wider in
time for the SMPS as compared to the ELPI. The
rise and fall times for the ELPI, a convolution of
the instrument response and the temporal pro-
Ž le of the PM emissions, are both about 2 –3 s.
The SMPS exhibits an asymmetric peak shape
with a rise time of about 5 s and a decay of
nearly 10 s. Since the particulate measurement
for the SMPS is spread out more in time than for
the ELPI, the peaks in the distributions appear
smaller.
That the ELPI and SMPS data in Figure 10
are consistent is evidenced by the agreement be-
tween the time integrated size distributions dis-
played in Figure 11. The top two panels compare
ELPI and SMPS data for phase 1 (cold start)
and phase 3 (hot start) of the FTP drive cycle;
the lower two panels compare PM size distribu-
tions integrated over the US06 cycle. The SMPS
data appear here as discrete points because they
are collected from 6 –8 transient tests, each con-
ducted at a Ž xed particle size. The time inte-
grated size distributions compared in Figure 11,
which no longer depend on instrument time
Aerosol Science and Technology
33:3 September 2000
response, exhibit good agreement, within the
scatter of the data points, between the ELPI and
SMPS measurements. As with the steady state
measurements plotted in Figures 2 and 3, the
37 nm stage of the ELPI overestimates the SMPS
measurement of 37 –63 nm particles.
DISCUSSION
The near quantitative agreement (except for the
37 nm ELPI stage) between particle size mea-
surements made by the ELPI and SMPS is
remarkable on two counts: the dissimilar mea-
surement methodologies and the fact that the
Comparison of ELPI and SMPS 257
FIGURE 10. Comparison of ELPI and
SMPS distributions of gasoline vehicle
PM emissions versus particle diameter
and time. Panel A: ELPI data. Panel B:
SMPS data constructed from 7 vehicle
tests, each at Ž xed particle size. Panel
C: Transient response of ELPI versus
SMPS.
instruments measure distinct physical particle
properties. Moreover, a comparable level of con-
sistency between the two instruments is obtained
for steady state as well as transient PM emissions
measurements. The consistency between ELPI
and SMPS particle size distributions observed
in the present study differs from the results of
comparisons made by Dickens et al. (1997) and
Moon and Donald (1997), who found the ELPI
measurements to be signiŽ cantly lower, by a fac-
tor of 2–4, in concentration and shifted to larger
particle size, by a factor of 1.2–2, as compared
to the SMPS. However, measurements at the
University of Minnesota (Kittelson, private
258 M. M. Maricq et al. Aerosol Science and Technology
33:3 September 2000

FIGURE 11. ELPI and SMPS size distributions of particles in gasoline vehicle exhaust. Filled symbols show SMPS
data and open symbols represent ELPI data. Panels A and B show PM emissions integrated in time over phases 1 (cold
start) and 3 (hot start) of the FTP drive cycle. The smooth lines represent Ž ts of the data to log-normal distributions.
Panels C and D show PM emissions over the US06 portion of the SFTP drive cycle. The lines connect the data points.

communication) Ž nd, as we do, that the ELPI
and SMPS size distributions are in reasonable
accord.
In our conclusions about the consistency be-
tween ELPI and SMPS particle number and size
determinations, some caveats should be kept in
mind. By the nature of motor vehicle exhaust
PM, only the lower half of the ELPI size range
is tested. Exhaust PM largely does not extend
into the micron size range, nor does the SMPS
operate in this range. The agreement between
ELPI and SMPS measurements found herein ap-
plies to exhaust PM, which is characterized gen-
erally as fractal aggregates of » 20 nm carbon
spheroids coated to a smaller or larger degree
by semivolatile organic matter and sulfates. It is
not immediately obvious that similar measure-
ment consistency would necessarily be observed
for liquid aerosols or high density metallic or ce-
ramic nanoparticles, for example.
That the ELPI and SMPS record particle num-
bers and sizes in good agreement with each
other lends conŽ dence that the measurements
re ect the nature of the vehicle exhaust aerosol.
That this agreement occurs between an effec-
tive diameter based on electrical mobility and
one based on aerodynamic drag is curious. It
is not a consequence of diesel PM having unit
density; in contrast ELPI measurements of mo-
bility selected particles reveal particle densities
to range from about 0.2 to 1.5 g/cm3 . While
the average effective particle density declines
with increasing mobility diameter, particles of a
given diameter exhibit a wide range of density.
Aerosol Science and Technology
33:3 September 2000
It is possible that the agreement observed be-
tween ELPI and SMPS size distributions is a
con uence of a number of factors. Except for
the 37 nm stage, which gives erratic results ow-
ing to the low charging efŽ ciency of the very
small particles, the ELPI covers essentially the
upper half of the diesel PM size distribution.
The diameter for which the average particle den-
sity is unity lies near 150 nm, about half way
along the upper part of the size distribution. For
the 63 nm stage the average density is greater
than unity, implying that to make a consistent
comparison to the SMPS, the ELPI size needs
to be shifted toward smaller diameter, and the
particle concentration increased to account for
the consequently less efŽ cient charging, in or-
der to place it on a mobility diameter scale;
but this just follows along the SMPS distribu-
tion. Conversely, for the 119 nm, 187 nm, and
283 nm stages, the density falls below unity,
whereby the ELPI numbers are decreased and
sizes increased, again following the slope of the
distribution. Since each impactor stage actually
records particles having a wide range of mobil-
ity diameters, there is in actuality a range of size
shifts and particle number adjustments that are
required to place the ELPI results on a mobil-
ity scale; but such “averaging” would just bene-
Ž t the similarity in appearance of the ELPI and
SMPS size distributions.
The ELPI and SMPS each have their advan-
tages and disadvantages. In making steady state
measurements, the SMPS has the superior size
resolution by an order of magnitude and extends
down to 12 nm, even 3 nm with the model 3025
CNC. But the ELPI has the larger overall size
range, capable of measuring particles from 37
nm to 10 l m in diameter. The SMPS must cor-
rect for multiply charged particles, which appear
in the size distribution at fractions of the mobil-
ity diameter of singly charged particles. While
this problem is nearly inconsequential below
about 200 nm, distortions of the size distribution
become more pronounced as particle size ap-
proaches 1000 nm. The ELPI must deal with the
electrostatic and diffusional losses of particles
as they traverse the upper stages en route to the
Comparison of ELPI and SMPS 259
stage they are destined to impact. Augmenting
the number of particles registered by the lower
states because of these losses presents a mi-
nor problem, especially with the metal shielded
insulators, for which the corrections increase
particle numbers only by about 10% or less.
Subtracting the currents attributable to small
particle loss from the upper stages poses a more
serious difŽ culty. The losses, and requisite cor-
rections, are reduced by the metal shielded insu-
lators but remain signiŽ cant, giving essentially
meaningless values for the volume of motor ve-
hicle exhaust PM if extended to the 10 l m upper
end of the ELPI range.
For transient tests, the ELPI has a signiŽ cant
advantage over the SMPS, namely, the ability
to measure second by second size distributions
as opposed to a single size per test. Although
the SMPS can still be used to advantage in tran-
sient applications, its resolution is no longer a
beneŽ t as separate tests are required for each
size bin. Its primary beneŽ t is the ability to mea-
sure PM emissions smaller than the 37 nm lower
limit of the ELPI, which is important since a
substantial fraction of vehicle exhaust PM can
lie in this range. The possible development of a
“bucket” to catch particles below the 37 nm cut-
off would obviate this to some degree; however,
the discrepancy between the 37 nm stage of the
ELPI and the SMPS would Ž rst have to be re-
solved. The measurement of rapidly varying par-
ticle emission rates incurs additional problems.
For the ELPI, it exacerbates the small particle
loss correction, which requires time alignment
of the impaction events between different stages
of the cascade impactor. Both instruments are
adequate, but neither has quite the time response
to follow the PM emissions over drive cycles
such as the FTP, ECE, and US06. This leads to
apparent discrepancies between the intensities
of particle emissions recorded by the ELPI ver-
sus SMPS that largely disappear for the time in-
tegrated PM size distributions. In the near term,
it appears that both instruments will be required
if a complete characterization of particle num-
ber and size is contemplated for both steady state
and transient vehicle emissions measurements.
260 M. M. Maricq et al.
We thank Mike Loos, Jim Weir, and Gary Duszkiewicz for
their expert technical help with the chassis dynamomete r
and vehicle emissions testing. We also appreciate the helpful
discussions we have had with Jorma Keskinen.
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Received June 14, 1999; accepted November 1, 1999.