JOURNAL OF GEOPHYSICAL RESEARCH, VOL. 106, NO.

D4, PAGES 3449-3474, FEBRUARY 27, 2001

A theoretical analysisof cloud condensationnucleus

(C CN) instruments
Athanasios

Nenes

California Instituteof Technology,Pasadena,California

Patrick Y. Chuang
National Center for AtmosphericResearch,Boulder,Colorado

Richard C. Flagan and JohnH. Seinfeld

California Instituteof Technology,Pasadena,California

Abstract. The behaviorand performanceof four cloudcondensationnucleusinstrumentsare

theoreticallyanalyzed.They includethe staticdiffusioncloudchamber(SDCC), the Fukuta
continuousflow spectrometer
(FCNS), the Hudsoncontinuousflow spectrometer
(HCNS),
andthe CaliforniaInstituteof Technologycontinuousflow spectrometer
(CCNS). A numerical model of eachinstrumentis constructedon the basisof a generalfluid dynamicscodecoupled to an aerosolgrowth/activationmodel.Instrumentperformanceis exploredby simulating
instrumentresponsewhen samplinga monodisperse
ammoniumsulfateaerosol.The uncertaintyin the wall temperatureboundaryconditionis estimatedfor all the instrumentsand is
foundto be appreciableonly for the CCNS. The CCNS andHCNS modelsreasonablyreproducedexperimentaldata,while reportedlimits were alsoverifiedby the FCNS model.Regardingthe performanceof eachinstrument,simulationsshowthatthe SDCC producesdropletsthat are monodisperse
to within 10% of the particlediameter(for particlesof a constant
critical supersaturation).
The FCNS can potentiallyactivateparticlesover a wide rangeof
critical supersaturations,
but the prevailingdesignexhibitslow sensitivityto particleswith
criticalsupersaturations
below 0.1% as a resultof the shorttime availablefor dropletgrowth
underlow supersaturations.
The resolutioncapabilityof bothHCNS andCCNS with respect
to critical supersaturation
is shownto be particularlysensitiveto operationalparameters.This
is a consequence
of the stronglynonlinearnatureof dropletgrowth;dropletsizecannotalways
be usedto distinguishparticleswith differentcritical supersaturation
becauseof the growing
droplets'trendtowardmonodispersity.
Of the two instruments,the HCNS generallydisplays
higherresolutioncapability.This is attributedto the smootherandmonotonicsupersaturation
profilesestablishedin the HCNS. While differentdesignparametersor operatingconditions
may leadto modestshiftsin the performancefrom thatpredictedherefor any of the four instruments,
the essentialfeaturesdescribedin thispaperare inherentto their designs.

This studyanalyzesthe performanceof four existingCCN

instrumentdesigns.The main focusof this work is to deterIn theory, the cloud droplet activationspectrumof atmos- minethe capabilityof eachinstrument
(or, moreprecisely,of
pheric aerosolscan be inferred on the basisof composition. the methodologyembodiedby eachinstrument)to resolvea
Measuringthe completechemicalcompositionof atmospheric CCN activationspectrum.
The resolutioncomputedis solelya
aerosolas a function of particle size in real time, however, is resultof the processof CCN activationand growthwithin
not yet possible.Thereforea directmeasurement
of the parti- eachinstrument;uncertaintyintroducedby the dropletdetecclesthat activateto form dropletsunder supersaturations
typi- tion systemis not considered.
Furthermore,
the modelsconcal of atmosphericcloudsis the acceptedway to experimen- structedhererepresent
idealizedinstruments.
This abstraction
tally measurecloud condensationnuclei (CCN). Existing in- allows one to calculatethe best possible(theoreticallimit)
1. Introduction

strumentsto determinethe CCN distributionexposean aero- resolutionfor an actualinstrument;secondaryeffectsnot consol sampleto a controlledenvironmentwith known water su- sideredin thesemodelswill furtherdegradethe resolution.
persaturation
profiles;the activationspectrumis thenobtained
In additionto assumingidealizedinstruments,it is also asby measuringthe number(or sizedistribution)of particlesthat sumedthat a perfectlymonodisperse
aerosolis introduced,
activate.

Papernumber2000JD900614.

composed
of pure(NH4)2SO4.
In reality,atmospheric
aerosol
is polydisperse
andwith a nonuniformcomposition.
As a consequence,
particleswiththesamepotentialfor activation
need
differenttimesfor growth;this shouldhavea deleteriouseffect on the instrumentperformance
but will not be addressed

0148-0227/01/2000JD900614509.00

in the current study.

Copyright2001 by theAmericanGeophysical
Union.

3449

3450

NENES

ET AL.'

ANALYSIS

OF CCN INSTRUMENTS

An important uncertaintyarisesfrom the water film temperaturesthat are used to generatesupersaturation

in each instrument. Typically, CCN instrumentsmeasureand control
temperaturesby using thermocouples(or thermistors)that are

t Cold
plate
-

--

273

- " 283

embedded
in thechamber
wallrather
thanatthegas-wet
sur-

-- 290

face interface.The actualtemperaturedifferencebetweenthe

_

coldandhotwaterfilmsis lowerthanthemeasured
value
owing
tothethermal
resistances
oftheplate
andfilms,
leading

to a lower supersaturation
than intended.As a result, the in-

ferred
activation
spectrum
isbiased
toward
smaller
sizes.

In the sections that follow, the CCN instruments are de-

scribed;
then
themathematical
models
used
tosimulate
them

arepresented.
An estimate
of uncertainty
in thewaterfilm

temperature
boundary
conditions
then
follows.
Theresponse

to a monodisperseaerosolinput is simulatedfor each instrument. Finally, the performanceof each (idealized)instrument

is assessed on the basis of these simulations.

0.01

2. Description of CCN Instruments

Of the CCN instrumentscurrentlyavailable, we will focus

upon four: (1) the staticdiffusion cloud chamber(SDCC); (2)
the continuousflow parallel plate chamber,specifically,the
designof Fukuta and Saxena [1979] (FCNS); (3) the CCN
spectrometerof Hudson [1989] (HCNS) and; (4) the California Institute of Technology (Caltech) CCN spectrometer
(CCNS) [Chuang et al., 2000]. Other instruments,for example, isothermalhaze chambers(IHC) [Laktionov,1972], have
been used to measure

CCN

but will

not be discussed

10

Temperaturedifferencebetweenplates(K)

Figure 2. Maximum supersaturation

(percent)in the SDCC
as a function of hot and cold plate temperatures.Linear
temperatureand water vapor concentrationprofiles are
assumed.
Watervaporsaturation
pressure
is calculated
from a
correlationgivenby Seinfeldand Pandis[1998].

here.

IHC instrumentsdo not actually activate the particlesinto

dropletsbut rather measurethe diametersof particlesin equilibrium with an ambient relative humidity of 100%, from
which the critical supersaturation,&, can be inferred. In the-

ory, this is not a limitationif the particlesare composedof inorganicsalts,but ambiguitycould arise if slightly soluble
compounds
or surfactants
are presentin the particles[Alofs,
1978; Shulman et al., 1996].

wall
2.1. Static Thermal

Cloud Chamber

Theseinstrumentsare amongthe oldestfor measuringCCN

concentrations.
The original staticthermaldiffusionchamber
design[Twomey,1963] consistsof two parallelmetalplates,
held at differenttemperatures,
with their facingsurfaceswetted (Figure1). Assumingquiescentconditionsthroughoutthe
chamber,lineartemperatureand nearlyparabolicsupersaturation profilesdevelopbetweenthe plates,with the maximum
supersaturation
locatedmidway.Figure2 showsthe maximum
supersaturation
generatedin the SDCC for a varietyof hot and
cold platetemperatures.
The CCN that are ableto activateat
the prescribedmaximum supersaturation
grow to become
large dropletsand in this way are distinguishedfrom those

gl
"' Coldwall
,

Diffusion

Hot wall

that do not activate. The concentration of CCN that activate at

,,"'*l viewVOlume_l

symmetry
axis
,
-

..........

side-wall

thisprescribed
supersaturation
is determinedby measuring
the
droplet number concentration.In order to obtain the CCN
spectrum,the numberof activateddropletsmustbe measured
at severalsupersaturations,
whichis achievedby changingthe
temperaturedifferencebetweenthe plates.This processtypi-

callyrequiresseveralminutesper.spectrum
[Lala and Jiusto,
1977]. The lowest critical supersaturation
that can be measured in the SDCC is around 0.2% [Sinnarwalla and Alofs,

1973].
................................................................................................................................................

origin

Cold wall

Figure 1. Staticdiffusioncloudchamber(SDCC).

One of the primary challengesregardingSDCC measurementsinvolvesthe methodusedfor countingthe particlesthat

activatewithin the regioncloseto the maximumsupersaturation. Initially, direct countingof the activateddropletswas
used but has been almost abandonedowing to the difficulty

NENES

ET AL.' ANALYSIS

OF CCN INSTRUMENTS

3451

Outlet

Metal
envelope
.....
::::
:::::::
....

Insulation
Inlet

Hott s
H

state, eliminating transientsthat complicatedata analysis.

Furthermore,usefuldatacan be obtainedcontinuously,
rather
............................................
than in the samplingintervalsof batchcycle operation.When
the sampleis confinedto the regioncloseto the centerlineof
the instrument,all CCN are exposedto essentiallythe same
supersaturation.
CFDC measurements
are limitedto supersaturationslargerthan about0.1%, owing to the long growthtime
requiredat low supersaturations.
When the two platesare oriented horizontally,gravitationalsedimentationlimits the time
during which dropletsexperiencea uniform supersaturation
and can causesignificantparticle loss within the instrument.
For verticallyorientedplates,the maximumtemperaturedifferencethat can be imposedis limited by buoyancy-induced
flows. Of the two configurations,however,the vertical seems
to be more effective and is normallyused.
An improvementof the CFDC was proposedby Fukuta
and Saxena [ 1979] (FCNS). In this design,a gradientin temperatureis imposed perpendicularto the flow direction, so
that particleswith the sameresidencetime experiencedifferent supersaturations
along different streamlines(Figure 3).
This instrumentthereforecan be regardedas a seriesof CFDC
origin
instrumentsoperatingsimultaneously
at differenttemperature
differences.Figure4 showsqualitativetemperature
andsupersaturationprofiles perpendicularto the flow for fully devel-

It__A_erosoj
r_egi_on_
_ _.1
,/

Cold tip

Figure 3. Fukutacontinuousflow spectrometer

(FCNS).
associated with such measurements. Photometric

wall

estimation is

now the method of choice; concentration is inferred from the

light scatteredoff the growing dropletscontainedwithin a

view volume in the proximityof the instrument'scenter.Regardlessof the scatteringmetricused(suchas peakintensity,
rate of signal growth, etc.), each introducesuncertaintiesthat
affect the resolution that can be obtained with SDCCs, be-

causelight scatteringis a strongfunctionof concentration

and
particle size (both of which vary considerablyduring the

wall

measurement).

One could make the simplifyingassumptionthat all activating particles,regardlessof their critical supersaturation,
have approximatelythe samegrowthbehavior.This approximation is reasonablewhen the critical supersaturation,
Sc, is
much smaller than the maximum supersaturation,
Smax(becausethenthe drivingforcefor growthis approximately
equal
to the supersaturation).
For S,closeto Smax,
particleswith differentcriticalsupersaturations
needdifferenttimesto growup
to a given size. Furthermore,the parabolic supersaturation
profile within the instrumentexposesparticlesto differentsupersaturationswithin the view volume; so dropletswith the
samecritical supersaturation
do not grow unifo__rm_!y
throughout the view volume.The combinationof a nonuniformsupersaturationprofile and different growth rates amongthe activating particles generatesa droplet distribution within the

Hot

:::::::::;:::::::::;:;:;:;:;:;::;:;:;:;:::;:;:;:::;::;:::;:;:;:;:;:;:::::::::::::::::::::::::;:;:;::;:;:;::::;:;::::::;:;:;::;:;::;:;:;:::::::;:;::;:?:::;:;:;::::::::;:;:;:;:;::;::::::;:;:::::

s
x
IE::!:i::i:i:5:5:5::!::::!::::E:!:5:!:::!:::5::!:!:::i::!:!::i::!:::i:5::5:i:!:5:i:::i::i:i:i:i:!:i:i:i:i:i:i:i:i::i:i:i:::::::::::::::::::::::::i:i:i:
.......
z..l

Cold

wall

view volume that contributesto the uncertaintyin the aerosol

measurement. As was mentioned in the introduction, addi-

tional uncertaintycould arisefrom the differencebetweenthe

imposedand effectivetemperaturedifferences.

wall

2.2. Continuous Flow Parallel Plate Diffusion Chamber

Supersaturation
The continuousflow parallelplatethermaldiffusionchamber (CFDC) [Sinnarwalla
andAlofs,1973]wasdeveloped
to Figure 4. Typical temperatureand supersaturationprofiles
overcome some of the limitations of the SDCC. Because the

for the FCNS along a flow section, for developed inlet

sampleflow is continuous,
theinstrument
operates
at steady

conditions.

3452

NENES

ET AL.: ANALYSIS

OF CCN INSTRUMENTS

develops).If all streamlines

aresimultaneously
probed,a CCN
spectrumcanbe obtainedin realtime.

autlet

2.3. Dynamic CCN Spectrometers

Inlet

Non-heated

section

(top view)

Warm
side/ ThlTh2Th3Th4
........................................................................................................
:'"':'::'.'.'.'..'iii!

Cold side

Tc1

Tc1

Tc2

Tc3

Tc4

Figure 5. Hudsoncontinuous
flow spectrometer
(HCNS).

The underlyingidea behindtheseinstrumentsis to expose

an aerosolsampleto a variablesupersaturation
field and infer
the CCN spectrumfrom the outlet dropletsize distribution.
CCN with low Scare expectedto activatenearthe entranceof
the instrument,and so they have more time to grow than do
particleswith higherSc;the latteractivatefartherdowntheinstrument.Thereforethe outlet droplet size is expectedto decreasewith increasingcritical supersaturation.
Furthermore,
the initial size of the particlesenteringthe instrument(being
in equilibriumwith the inlet RH) decreaseswith increasing
critical supersaturation,thus enhancingthe size differences
betweenparticlesof different critical supersaturation,
Sc.The
sensitivityof the instrumentdependscritically on how the
outlet droplet size varies with particle dry size, and henceSc.
Becausethe rate of dropletgrowth variesinverselywith particle diameter, the droplet size distributionconsiderablynarrowsasparticlesgrow,implyingthat a veryprecisesizemeasurementmay be neededat the outlet of the instrument.Comparedwith SDCCs and CFDCs, dynamicspectrometers
utilize
a completelydifferentconceptin instrumentdesign,in both
the activation and size measurementcomponents.
Hudson [1989] developed a dynamic spectrometerby

modifying a continuousflow thermal diffusion chamber

(HCNS) (Figure5). This instrumentexposesthe sampleair to
a supersaturation
profile that increasesin the streamwisedirection,as shownin Plate 1. The flow field is preconditioned
ment. It should be noted that Smax
is attained toward the exit of
beforea supersaturation
is imposed,in a similarfashionto the
the instrument,after the concentrationand temperaturefields FCNS. Becausethe HCNS design measuresparticlesover a
develop. A significant portion of the instrumentis used to large rangeof S,.simultaneously,CCN spectracan potentially
"precondition"the aerosolflow, by developingthe velocity be determinedrapidly.The reportedrangeof measurablecritiand temperatureprofiles before exposingthe flow to the wet- cal supersaturations
in the HCNS is considerablylargerthan
ted hot wall. If this is not done, incomingair that mixes with that for thermal diffusion chambers,0.01 to 1%, covering
saturatedhot air in the entranceregion of the instrumentcan much of the rangeof interestfor climaticallyimportantwarm
generate much higher supersaturationsthan intended. This clouds.The supersaturation
rangeis extendedbecauselow Sc
may biasthe measurement
by activatingaerosolcorresponding particlesare exposedto very high supersaturations,
thusconto a different supersaturation
than prescribed.Strictly speak- siderablyacceleratingtheir growth.This instrumentalso uses
ing, the FCNS is a particle counter, since each streamlineis
white light sizedetection,eliminatingany sizeambiguityfrom
exposedto only one supersaturation
(after the flow completely Mie scatteringresonances
seenin lasersizedetection.Because
oped laminar flow (neglectingsidewalland buoyancyeffects).
The profiles for a given streamlineare similarto thoseattained
in the SDCC at steadystate;so diagramssuchas Figure2 can
be used for predictingSmax
at different positionsin the instru-

Iinlet
Warm

Cold

section section Insulation

Sheath
air
Aerosolair

Symmetryaxis
Figure 6. Caltechcontinuousflow spectrometer(CCNS).

NENES ET AL.' ANALYSIS

OF CCN INSUMENTS

3453

Non-heated
section

Warm
side
/
I

Th Th2

-1

Th3

Th4

Centerline -,- ................................

3.0

--'l
=.X
,

Tc Tc

Tc2

Tca Tc4

Coldside

2.0

(top
view)

1.0

0.0

mm

mm

mm

mmmmm

mmmmm

mmmmmmmmm

mmmmmmmmm

mm

mm
Nm
m
mm
m
i i

Max. AT (K)
4

-1.0

-2.0

.........10
-12

-3.0

0.0

0.1

0.2

0.3

Position (m)
Plate 1. Typicalsupersaturation
(percent)profilesfor the HCNS alonga flow section,for various
maximum
temperature
differences,
ATmax
(theAT at thelastsegment).
Thetemperature
difference
between
eachsegment
is assumed
to increase
witha constant
step("linearramp")onbothcoldandwarmsides.
The
profilesarecomputed
byusingtheHCNSnumerical
modelin thispaper.

of the speedand wide range of supersaturations

that can be
covered,this instrumenthas been used frequentlyon airborne
measurements[McMur, 2000].
The Caltech CCN spectrometer(CCNS) [Chuang et al.,
2000] (Figure6) implements Hudson's streamwisegradient
method in tube flow. A method originally developedby Hoppel et al. [ 1979] is employedto producesupersaturation
in the
flow in a wet-walledcylindricaltube;the tubeis dividedalong
its lengthinto sectionsthat are alternatelyheatedor cooled.As
the air flows throughthe tube, it is saturatedin the warm sections and then cooled to produce supersaturationnear the
center of the tube. The supersaturation
profile that develops
dependson the geometryof the segments,the flow rates,the
temperaturedifference,and the operatingpressure.The supersaturationis increasedalong the length of the tube by increasingthe temperaturedifferencebetweensuccessivetube
segments,leadingto a centerlinesupersaturation
profile such
as that shownin Figure7. The first sectioncan be usedto precondition the inlet flow.

Anotherimportantissueis to estimatethe uncertaintythat

would arise when calibration curvesproducedby using pure

salt aerosol are used to infer ambient CCN spectra. Both

spectrometers
operateon the assumption
that particleswith
the same S. (but different composition)will have the same

growthbehaviorwhenexposed
to anidenticalsupersaturation
field. In reality,an even stricterconstraint
mustbe satisfied:
the KOhler curves need to be similar, which is not the case for

aerosol-containing
surfactantand slightlysolublematerial.
Furthermore,the inlet air may also containcondensablegases
that can also have a large impacton the activationproperties
of the aerosol;this may not be correctlyaccountedfor in the
instrument. These issues are to be addressed in future studies.

3. Mathematical

Models of CCN Instruments

To evaluatethe performanceof the different CCN instruments, flow, heat, and mass transfer have been numerically
modeled within each instrumentto determinethe temperature,

watervapor,andsupersaturation
distributions
as a functionof
positionand,for unsteady
instrument
operation,
time.Particle
activationand growthare simultaneously
simulatedby tracking individualparticlesas they flow throughthe instrument.

3454

NENES ET AL.: ANALYSIS

OF CCN INSTRUMENTS

84 Warm
Cold

Centerline

0.0

0.1

0.2

0.3

0.4

0.5

0.6

0.7

Axial position (m)

Figure 7. Indicative supersaturation
(percent)profile for the CCNS along a flow section.The volumetric

flowrateis0.7L rain'.Theprofile
iscomputed
byusing
theCCNSnumerical
model
ofthispaper.
The equationsusedto describeaerosolparticlegrowthare first
given in the next section,followed by the generalform of the
gas phaseequationsused for all the instruments.
Finally, the
appropriate boundary conditions and specific relations for
eachinstrumentare given.
3.1.

Aerosol

2k,2zcM
RT

Growth

The rate of changeof dropletsize for eachof the particles

is calculatedfrom the diffusionalgrowth equation[Seinfeld
and Pandis, 1998]'

where Ma is the mean molar massof air, k,,is the thermal

of air, and ar is the thermalaccommodation
coefficient.The
equilibriumsupersaturation
of the droplet, S,.
q is givenby the
K6hler equation:

P
dt

S -Seq
P

Pw

arDppc
p

conductivity
of air, p is theair density,Cpis theheatcapacity

dD
P

where D,. is the diffusivity of water vapor in air, acis the

condensationcoefficient. The thermal conductivity of air
modifiedfor noncontinuum
effects,k, is givenby

'

(1)

+
w-1
RT
AHvapPwlAHvapM
)
S
eq
:exp[
4M.,o',,,
_6n.MwV.,
]_

4p*D'
pMw

4k'
aT

TR

'

RTp..D,,

1,

whereDpis theparticlediameter,p' is thesaturation

vapor

pressure
atthelocaltemperature
T, & = p,,/p*- 1 isthelocal
supersaturation,S,
qis the equilibrium supersaturation
of the

where o-wis watersurfacetension,nsis the numberof moles

droplet,p},is the waterdensity,AHvap

is the enthalpyof va-

of soluteperparticle,anddpis thedrydiameter
of theparticle.

porization of water, Mw is the molar massof water, and R is

the universalgasconstant.DT.is the diffusivityof watervapor 3.2. Gas PhaseEquations

in air modified for noncontinuum effects [Fukuta and Walter,
1970]:
mv

1+ 2D,, 2zcM
w
acDp

RT

Differential momentum, energy, and mass conservation

balances are written for the gas phase, assuming a twodimensional Cartesian or axisymmetric coordinate system.
This results in a system of differential equations,each of
which is of the generalform

NENES

ET AL.'

ANALYSIS

OF CCN

INSUMENTS

3455

Furthermore, a source term in the momentum equations,

Jbuoy,
represents
themomentum
generated
fromthermalbuoyancyeffects.For ideal gasesit is givenby

ox
x2F-

(2)

x2F
x---
o

wherex,,x2arethespatial
coordinates
and is thedependent
variable(e.g.,T). SOis a source
term,andF0is a transport
coefficient,both of which dependon the form of . Table 1

Jbuoy T.u,k
(x2),

(5)

whereT is the temperature

and g,: is the component
of
gravity in the x2 direction.Tbuk
(X2)is the x averagetemperatureat position x2 and is computeddifferentlyfor each
instrument.Finally, ,o is gasphasedensity,calculatedat Tbuk

liststheexpressions
of So,F0 for eachtypeof . ForCartesiangeometry,
theexponenta = 0 andthecoordinates
x,x2
can be replacedwith the moreconventional
x, y. For axisymmetric
geometry,
a = 1 andthecoordinates
x,x2 canbe

(x2).

replacedwith themoreconventional
z, r.
The rateof condensation
of liquidwater(in molesper vol-

3.3. Static Diffusion

umeof airpersecond)
ontheaerosol
particles,
Jcond,
is needed
in the watervaporandenergyconservation
equations.
This

Cloud Chamber

The geometryand characteristic

parameters
of the SDCC
are shownin Figure 1. The followingassumptions
are madeto
simulate the instrument: (1) there is a two-dimensionalaxisymmetricchambergeometry;(2) the air is quiescent;(3) particles fall by gravitationalsedimentationand attain terminal
velocity instantaneously
as they grow; (4) coagulationand
Brownian diffusion of particles are neglected;and (5) wet
wallsact as a perfectsink/source
of watervapor,i.e., the air is
saturatedwith watervaporat the walls.
At the top and bottomwalls, a constanttemperature
bound-

quantityis givenby
1 d%
M,. dt

where
wLis thelocalliquidwater
content
(kgm3air).Fora
population
of waterdroplets
consisting
of Ni droplets
of diameter
Dpipervolume
of air,

arycondition
is imposed,
whileat thesymmetry
axis,3T/Or=
0. At the sidewall, a compositeheat conduction-naturalconvectionheat flux boundaryconditionis used,

w--p.6,=, ' "

= u (Ln.- Tr),

wheren is the numberof dropletsizesfoundin the distribu-

(6)

tionandp,.isthedensity
of water.Onthebasis
of thisdefinibis the ambienttemtionof wL,therateof change
of liquidwatercontent
of the where is the heatflux per unit area,Tam
peratureoutsideof the cell, Tf is the air temperature
at the

particlesis

computationalcell adjacentto the sidewall,and U is the appropriateheattransfercoefficientbetweentheoutsideambient

dwL
d N.D..
dt dt
;z ,.

and chamber fluid,

dD,,

(3)

1C,

In 1+

U h kwall T '

wheredDpi/dtis calculated
fromtheaerosolgrowthequations.
Substituting
equation(3) into the definitionfor Jcond
gives

J....
d: .7T
p..
i:NiD2
pidD,i
m,,,
dt

whereCpis thewallheatcapacity,
kw:,U
is thesidewall
thermal
(4)

conductivity,andh is the naturalconvectionheattransfercoefficient, calculatedby the following correlation[Incropera

and DeWitt, 1985]:

Table 1. TransferCoefficientsand SourceTermsfor the GasPhaseEquations

Conservation
Law

Continuity

x,momentumu

/1

x=momentum

Heat

Cp

Water vapor

pD,

(7a)

P)__.ll
8uh
(2 J
8vJuoy
-x-x_+x
''x._J
'-x2L
+

xy

_
x,

- 8x= 'PJco.d
Cp

--PJco.d

3456

NENES ET AL.: ANALYSIS

0.670Ra}/4

hL

= NuL = 0.68 +
k

(7b)

OF CCN INSTRUMENTS

r,(z)
=r,,-

1+(0.492/Pr)9"614/9
'

(W-z) . r,,(z)
= +

(W-z),

where s is a coordinatethat runs along the heatedwall, with

its origin locatedat the hot tip (Figure 3) and endsat the cold
tip;

where

CpP2gL
3V--Tanlb

Rs

ar

r,,-rc

ds

2W +H

is the Rayleigh number for an ideal gas, Pr =///pk(, is the

Prandtlnumber, is the averagetemperature

of the SDCC
Plexiglaswall, and Tam
b is the ambienttemperature.The first
term on the right-handside of equation(7a) is the heat conduction

resistance between

the outer sidewall

and the envi-

ronment, and the second term is the resistance within the

sidewall.At the sidewall and the symmetryaxis, OC/Or= O.

Particles are assumedinitially to occupy the entire chamber,
with a uniform concentrationand size distributionthroughout.
The droplet sedimentationvelocity is given by the Stokes
equation[Seinfeldand Pandis, 1998],

is the temperaturegradient along the s coordinate. At the

walls, the air is assumedto be saturatedwith water vapor at
the local temperature.At the outlet, 0C/Ox= 0. Basedon the
sheath/aerosol flow ratio, the section of the flow field occu-

pied by the aerosolis calculatedfrom a massbalance.Finally,

the meantemperature
H

IT(x,y)dx
Tbu,
(Y)=

0
2

DpPpgCc

18//

(8)

is used in calculatingthe buoyancyterm in the u momentum

equation.

where

3.5. Hudson Continuous Flow Spectrometer

In simulatingthe HCNS (Figure 5), the following assumptions are invoked:(1) conditionsare steadystate;(2) geometry
is two-dimensionalCartesian;(3) aerosolparticlesfollow the
is theslipcorrection
factor,pp is theparticledensity,//isthe air flow streamlineswith the samevelocityas the surrounding
air viscosity,g is the gravityconstant,and ,;[is the meanfree air; (4) sedimentation,coagulation,and Brownian diffusion of
path of air.
particlesare neglected;(5) walls act as a perfectsink/sourceof
water vapor, i.e., the air is saturatedwith water vapor right
3.4. Fukuta ContinuousFlow Spectrometer
adjacentto the walls; and (6) buoyancyis neglected.The twodimensional
assumptionneglectstop and bottomwall effects.
Using scalingarguments,it can be shownthat sidewalleffects in the velocity field become significant when the dis- This can be shown through scaling argumentsto be a good
tance from the sidewallsis of order H. The FCNS geometry approximationwhen the aspectratio H/W is largeandbreaks
examinedhasan aspectratio of W/H = 20; somorethan90% down only when the distancefrom the sidewallsis of order W.
of the total width of the instrumentremainsunaffectedby the In additionto the constanttemperatureconditionposedat the
presenceof walls. Thus the FCNS (Figure 3) can be reasona- controlledtemperaturesections,a zero-heatflux conditionis
bly simulatedby solving a seriesof two-dimensionalprob- assumed at the insulated areas.

Cc=1+(2/Dp
)[1.257
+0.4exp
(-1.1Dp
I/1,)1

lems, each of which is for a fixed value of the z coordinate. A

vertical flow configurationis assumed.In addition,the following assumptionsare made: (1) conditionsare steadystate;
(2) aerosol particles follow the air flow streamlines,at the
same velocity as the surroundingair; (3) coagulationand
Brownian diffusion of particlesare neglected;(4) walls act as
a perfect sink/sourceof water vapor; and (5) the temperature
profile alongthe wall (in the z direction)is linear.
Two typesof inlet velocityconditionsare considered,fully
developed(i.e., parabolic) or plug flow. The other variables
(T, C) are assumedto have a uniform profile at the inlet. At
the walls, a no-slip boundaryconditionis assumed,u = v = 0,
and for the outlet, 0u / 0x = 0; v = 0. At the outlet, 0T / 0x = 0.

3.6. Caltech Continuous Flow Spectrometer

In formulating the conservationequationsfor the CCNS,

the sameassumptionsas thosefor the HCNS are made,except
that an axisymmetriccoordinate system is used. Although
buoyancyis not expectedto be significant,it is includedin the
model for completeness.Tbun(Z)
in this case is the radialaveragetemperatureat axial positionz:

I 2IrrT(r,
z)dr
=

A constanttemperatureconditionis used for the walls; this is

2;rrdr
0
a function of the z position of the sectionexaminedand is
computedby using assumption(5). Given that the temperature
at the two tips Th (for any x, y = H and z = W) and Tc (for any Boundaryinlet conditionsusedare similarto thoseof section
x, y = 0 and z = W) are known, the temperatures
at the top 3.4. In addition to those, 0u / Or = Ov/ Or = 0C / Or = 0T / Or = 0
wall T, and the bottom wall Tbat a given coordinatez are
at the symmetryaxis.

NENES

ET AL.'

ANALYSIS

tions

The conservationequationsfor the four instrumentscannot

be solvedanalytically;so a numericalsolutionis obtainedby
the finite volume method [Patankar, 1980]. A hybrid upwindcentral differencing schemeis used for calculatingthe confluxes over the finite

control volumes.

The

schemeusedemploysa staggeredgrid, in which each velocity

grid node lies between two scalarvolumes,ensuringthat the
numericalsolutionis consistentwith respectto pressure.The
Semi-Implicit Method for Pressure-Linked Equations
(SIMPLE) iterative solution method [Patankar, 1980] is used
to solve the hydrodynamiccycle of the finite volume equations, while the particle growth equationsare solvednumerically integratedwith the LSODE solverof Hindmarsh[1983].
The computercode used for the numericalsimulationswas
based on the TEACH-2E

CFD code [Gosman and Ideriah,

1976] coupledtogetherwith an aerosolgrowth module. The

computationalgrid and time stepusedensurethat the numerical solutionis within a few percentof the asymptotic(with respectto grid density)limit. The numericalsolutionwas obtainedby using 100 cells for each spatialcoordinate.For the
unsteadystatesimulationsof the SDCC, a time stepof 0.025 s
is taken for the gas phase equations,for a total integration
time of 30 s. The aerosolgrowthequationsuse a variabletime
step, which is scaleddependingon the instrumentsimulated.
For the SDCC simulations,it is scaledon the gas phasetime
step,while the othersuse the transittime througha computa-

Tf,is estimated
fromtheheatflux throughthewalls.The temperaturedifferencebetweenTf and the controlledwall temperature,T,,.,is then computedand expressedas a fraction of
the "nominal" difference, Th -T,., for various values of water
film thickness,filter paper thickness,and flow rates.Realistic

values
forbothpaperandwaterfilmthickness
are10-3m;the
wall is assumedto be of order 10-2m.
5.1. SDCC Uncertainty Analysis

With respect to wall heat transfer in the SDCC, the following can be assumed:(1) steady state conditionsand (2)
one-dimensionalconductiveheat transfer(stagnantflow field)
along the axial direction of the instrument(see Figure 8a).
With theseassumptions,the heat flux betweenpoints 1 and 2,
Q,2,is equal to the heat flux betweenthe top and bottomwall,
Qt,;,.Expressingthesefluxes as a functionof the temperature
differences,T,-T,. and T-T2, we have Q,2 = Qt.b,which
leads to

wall

W!I
114-1
t----

(a)

tional cell.

'

wall

Before proceedingwith the numericalsimulationof the instruments,it is instructiveto perform an analysisof the uncertaintyin one of the most critical parametersof CCN instruments,
namely,the temperature
boundaryconditionfor the
instrumentwall. When operatingthe instruments,
one controls
the temperatureof the metal supportingwall (or plates),
whereasthe boundaryconditionthat actuallygovernsthe performanceof the instrumentis the temperatureof the inner face

wall

T/,

Tt

-......
--m-.
....
:-.'ir.4-
T

__

(b)

water
film+filter
paper

..............

temperatures
would bias the predictions,sincethe supersaturation is a strong function of temperaturedifference. One
could include heat transferthroughthe walls and film in the
simulations,but the analysisof constantwall temperatureis
adequatefor the purposeof estimatingthe relativemagnitude
of the uncertaintyarisingfrom a temperaturedifference.Furthermore,suchan analysisis usefulin thatit is independentof
any specificgeometryor configuration.
When estimatingthe wall temperatureuncertainty,one
mustconsiderall the factorsthatcontributeto the temperature
drop between the controlledtemperatureside and the water

hotside

WlI

(c)

film. Apart from the metal walls and the water film, there is
also a material that helps keep the walls wet. The material
conventionallyused for the SDCC, FCNS, and CCNS is filter
paper, while the HCNS usesa steel matrix. The material will
certainty in the continuous flow instrumentsthan on the
SDCC. The resultsfor the SDCC may be consideredintuitive,
but the analysisis includedfor completeness.

! L

15+1

between these two

be shownto havea largerimpacton the wall temperature

un-

-- ---

water
filrn+
filter
paper

Instruments

of the water film on the wall. Differences

Tt

w2]

5. Uncertainty Analysisfor Wall Temperature

of CCN

3457

In orderto assessthe effect of wall temperatureuncertainty,

simpleheat transfermodelswill be constructedfor all of the
instruments.In thesemodels,the inner waterfilm temperature,

4. Numerical Solution of Conservation Equa-

vective-diffusive

OF CCN INSTRUMENTS

' ' "' .........

water
film
+filter
paperI

fl

1+2 .....

w:
cold
side

Figure 8. Geometriesused in the simple modelsdeveloped

for determiningthe uncertaintyin the temperatureboundary
conditions for (a) the SDCC; (b) the CCNS, and (c) the
HCNS.

3458

NENES ET AL.: ANALYSIS OF CCN INSTRUMENTS

Sl,2(rl - T2) '-St,b(rh-rc),

(9)

practically equal to the nominal. For example, for

where Ui,2 and Ut.bare the total heat transfercoefficientsbetweenpoints1, 2 andt, b, respectively.
Theseheattransferco-

film, T- is about 1.99 K, the uncertaintythus being at

most0.01 K. This resultis not surprising,sincethe gap be-

era and DeWitt, 1985] to lead to

thermal conductivity compared with conductivitiesof the

T,-T c = 2 K, then, dependingon the thicknessof the water

efficients
canbeevaluated
by theresistance
method
[Inctop- tween the plates is occupiedmostly by air, which has low

L-(ll+12)-(4+2)

UI,2

other materials. The resistance therefore to heat conduction is

(10)

ka

(Wl+ w2)

St,b

kst.steel
4

mainly owing to the air and is relatively insensitiveto the

presenceof water and filter paper. In addition, variationsin
water film or changesin wall thicknessdo not have a large
impact on the uncertainty.It can be concludedthat once the
steadystate temperatureprofile has been achieved,the temperatureuncertaintyin the instrumentis negligible.
5.2. CCNS Uncertainty Analysis

L-(1,+12)-(l+2)
k,

+ R, + R,2,

(11a)

In our presentationof the two spectrometers,

usuallythe
HCNS precedes the CCNS. For convenience,however, we
shall begin now with the CCNS, for which we assumethe

wherekst.s,eel
=15, kwater
=0.58 and :p.p,
=0.1 arethethermal following:(1) conditionsare steadystate;(2) thereis oneconductivities
(inW m-l K-l) of stainless
steel,water,andfil- dimensional
conductive
heattransferalongtheradialdirection
and convectiveheat transferalongthe axial directionof the
thewall,filterpaper,andwaterfilm, respectively
(i = 1 corre- instrument;
(3) ontheentryto eachhotandcoldsegment,
the
sponds
to thehotplate,whilei = 2 refersto thecoldplate).In temperature
profileis uniformandequalto thewalltemperasection;
(4) theflow fieldis fullydevelequation
(11a), theresistances
of thewall,soaked
filterpaper, tureof theprevious

ter paper,respectively.Also, wi, li, and . are the thicknessof

and air are assumed to be in series. The resistance of the

opedand laminar;and (5) the latentheat flux from water con-

soakedfilter paper,R,i, is

densation
throughthe wall is smallin comparison
with the
sensible heat transfer, which is reasonablefor near-atmos-

g$i=

phericpressures
andsmalltemperature
differences.
Theapkwater +

prophategeometryis definedin Figure8b. With theseas-

kpaper

min(Si,1,) min(8,,li)
8-min (8,li) /,-min (t,,1,)
kwater

kpaper

sumptions,
theproblemreduces
to a developing
temperature
profilein theentryregionof a pipe,witha fullydeveloped
(11b)

hydrodynamic
flow field. The heatflux throughthe wall for
thegivensegment
therefore
canbecalculated
by
O= hAaT ,

Thefirsttermin theaboveequation
assumes
thatanequal
segmentof waterand filter paperare combined
in parallel
area,AT is thetempera(whichcorresponds
to thewell-soaked
portionof thefilterpa- whereA is thetotalsurfaceexchange

per), andthe remainingpaper(or water)is connected

in series. ture changeof the bulk fluid betweenentry and exit of the
Allowing for the excessof filter paperand waterconsiders pipe segment,and h is the mean heat transfercoefficient,

by the followingcorrelation
[Incropera
situations
wherethe filter paperis partiallydry or whentoo whichis calculated
and DeWitt, 1985]:
muchwateris provided
on thefilterpaper.Thesensitivity
of
hD
0.0668Gz
theuncertainty
to theseconditions
is an important
operating

parameterof theseinstruments.

= NuD = 3.66q1+ O.04Gz2/ '

(14)

Substituting
equations
(11a),(l lb), and(10) into (9) and
solvingfor (r - T2)/(Th- Tc)yield
where
Gz = Re Pr (D / L)
is
the
Graetz
number,
Re= (4pVDrD/)is the Reynoldsnumber,Pr = lt/pk, is the

r-r2

ka

+ R,lk, + R,lko

(Wl
qw2)
kst
stee
I '

L-(1,+12)-((51+(52)

Prandtl number,L and D are the length and diameterof the

segment,
and1) isthevolumetric
flowratethrough
thepipe.

(12)

The uncertaintycouldthereforebe definedas

T-T2
/><
100%.

1-T,-T

Using assumption3, the bulk temperaturesin and out of the

sectionareequalto eitherThor T..The temperature
difference
AT thenin (13) is approximatedwith Th- T.
Furthermore,theheatflux canbe expressed
asa functionof

theinnerfilm Tf andtheouterwalltemperature
T,,as

whereU is the heattransfercoefficientthroughthe combined

metal wall, filter paper,andwaterfilm andis calculatedas'

Using equation(12), we calculatethat for caseswherethe

water and paperthicknesses

are equal,the ratio is at most

0.99. Thismeansthatthe effectivetemperature

difference
is

142

--=+R,,
U kq.stee
I

(16)

NENES

ET AL.'

ANALYSIS

where,as in equation(11b),

kwaer +

OF CCN

INSTRUMENTS

3459

can be seen,the uncertaintyis a somewhatstrongfunctionof

filter paper thicknessand has a weaker dependenceon water
film thickness.Everything else remaining constant,the minimum uncertaintyis encounteredwhen the water film and filter
paper have the same thickness;under this condition the uncertaintyrangesbetween 4 and 6%. However, when the water
thicknessbecomessmallerthan the filter paper(i.e., the paper
partially dries),the magnitudeof the uncertaintyincreasesand
can approach10%, or higher. The reasonfor this behavior,

kpaper

min(&/)
rain(&/)
- rain(&l) + I - rain
k,mer
kpaper

Equating
equations
(13)and(15)andsolving
for(T,.- Tf)/(Th
- Tc)yield

(17)

The uncertaintycould thereforebe definedas

which differs from the SDCC, lies in the fact that forced con-

vection in the CCNS increasesthe heat transfer efficiency

through the bulk of the fluid, and so the resistancesin the
water film and filter paper have a larger effect on the temperaturedrop acrossthe wall than in the SDCC. Furthermore,
the temperaturedifferencesbetweensegmentsneededto generate supersaturations
along the centerlineare increased,comparedwith the SDCC; so the absolutevalueof the uncertainty
increasesalong with it. For Xalllpl,
.......... for Th -T. = 10 K , UlU:11,

dependingon the thicknessof the waterfilm, T,.- T.rcan

>< 100%.

rangebetween0.5 and 1 K.
Given that heat transfer efficiency increaseswith the flow

Equation(17) dependson the thicknessof the materialsand

on the Reynoldsnumber.The validity of assumption3 decreasesas Re increasesbut can be usedin our analysis,since
the instrumentis operatedusuallyat low Re and providesan
upperlimit estimateof theuncertainty.
The appropriateness
of
assumption3 can be assessed
from the numericalsolutions.

rate,onewouldexpectthat (T.- Tf)/(Th - Tc)dependson the

flow rate. Indeed,this is the case,assumingthat wall and paper thicknessdo not change,a tenfold increasein flow rate
addsan additional 10% to the uncertainty;this would translate

to a T,.- T.rashighas2 K if Th- Tc= 10 K. As wasstatedbe-

fore, assumption3 is not as appropriateat high flow rates;so

the uncertaintymay not increaseby as much as 10%, but still
Figure9 showscontours
of (T.- T.r)/(Th-Tc) asa function one would expectan appreciablechangein film temperature.
of water film and paperthickness.The wall thicknessis asIn any case, especiallywhen condensationalheat flux is
sumed
tobe 1 cm,andtheflowrateisequalto 10L min-.As considered (which further increasesthe temperatureuncer-

20
18

16

12
10
"

6
4

10

12

14

16

18

20

Water film thickness(% of gap)

Figure9. Contours
of (T,.- T.r)/(Th- TOfortheCCNSasa function
of paperandwaterfilm thickness.
The
thickness of the metal wall is assumed to be 1 cm.

3460

NENES

ET AL.' ANALYSIS

tainty), one would expectthat the effective temperaturein the

instrumentwould be appreciablysmallerthan that posedon
the walls. Therefore any simulationsor experimentalcalibrationsshouldbe adjustedfor this difference.

OF CCN INSUMENTS

which meansthat the temperaturedrop acrossthe film is the

samemagnitudefor bothcold andhot walls.After furthermanipulationsof equation(21) we obtain

5.3. HCNS and FCNS Uncertainty Analysis

Both the HCNS and FCNS employ laminar flow between

parallelplates.The two systemsdiffer in the choiceof the porouswetted layer; the FCNS usesfilter paper(as in the SDCC
and CCNS) while the HCNS usesporousmetal. The thermal
conductivityof the latter materialis much higherthan that of
the paper, leading to much smaller temperaturedifferences
between the measuredand surfacetemperatures.A general
model that accountsfor the resistancein the porousmaterial
will enableevaluationof the uncertaintiesin both systems.
In the following analysis,we assumeas follows: (1) conditions are steady state; (2) one-dimensionalconductiveheat
transfer is perpendicularto the flow, and convectiveheat
transferis along the flow axis; (3) the fluid reachesthe developedlinear temperatureprofile at the exit of eachsegment;(4)
the sectionalaveragetemperaturedoesnot vary throughoutthe
instrument(which is true in the HCNS for a symmetrically
cold-hottemperatureprofile); (5) the flow field is fully developed and laminar;and (6) the latentheat flux owing to water
condensationis small in comparisonwith the sensibleheat
transfer,which is reasonablefor near-atmospheric
pressures
and small temperaturedifferences.The geometryis definedin
Figure 8c. Resistancethroughthe steel matrix of the HCNS is
neglected.With theseassumptions,the problemreducesto a
developingtemperatureprofile in the entry region of an enclosedplate geometry,with the hydrodynamicflow field fully
developed.Assumption4 ensuresthat the bulk enthalpyof the
fluid doesnot changeas it passesthroughthe instrument;thus
any heat exchangebetweenthe platesis perpendicularto the
flow. For a given segment,the heat flux throughthe hot wall,

The heat flux from the fluid to the cold film, 4c, can also
be expressedas

c=hAC(Tbu,k_T),

(23)

where Tbun
is the bulk temperatureof the fluid (which is the
samealonga segment)and h is the meanheattransfercoefficient.Sincethe systemis in steadystate,thisheatflux is equal
to the flux that passesthroughthe cold wall (equation(19)).

By equatingthetwo fluxesandsolvingfor Tf, we obtain

Tf- hTbuk
+UcT"'c
h+U c

(24)

By substituting
equation(24) into equation(22), we finally get

.r_ 1- 2

rd:- c,

h+ V

-E

(25)

The uncertaintycouldthereforebe definedas

1- .r-T x 100%.

Thc)

The heat transfercoefficient h is calculatedfrom equation

'", canbe expressed

asa functionof theinnerfilm Tf and (14) by using the hydraulic diameter. To incorporatethe
noncircular section effects, the heat transfer coefficient calcu-

theouterwall temperatureT' as

lated from (14) is then multipliedby a factorof 2, which is the

limiting factor for an aspectratio approachinginfinity [Incroperaand DeW#t, 1985]. This approximation
is reasonable,
giventhattheHCNS examinedherehasan aspectratio W/H =

whereUhistheheattransfer
coefficient
through
thecombined20.
Equation(25) dependson thethickness
of the materialsand
metalwall,filterpaper,
andwaterfilm(equation
(16)),andAh
is the exchangesurfaceon the hot wall side.A similarexpres- on the Reynoldsnumber.However, if Tburemainsthe same
between segments,then the uncertaintyremains the same
sioncan be writtenfor the cold plate side:
throughoutthe instrument.Given that heat transferefficiency
increases with the flow rate, one would expect that

=UA(T.,- Tf),

(19)

where Tfc and T,5 are the inner film and outer wall tempera-

turesat thecoldwall, respectively,

andAcis theexchange
surface on the cold wall side. Furthermore,becausethe systemis
in steadystateand the fluid doesnot experienceany overall
increasein enthalpy, 4,= 4c; so

UhA
h(T.j
_T,,)
h - UCA
c

c.

(2O)

(T -T/)/(T,'.'- T7) depends

ontheflow rate.Indeedthisis the
case,as shownby Figure 10. The wall thicknessis 1.0 cm, and
the paperthicknessin this plot is assumedto be zero (therefore thisplot showsthe uncertaintyfor the HCNS). As canbe
seen,for a film thicknessthat is 5% of the gap, a tenfold increasein the flow rate almostdoublesthe uncertainty,from 11
to 18% (or a ratio of 0.89 to 0.82). However, for film thicknessesaround1% of the gap (or around1 mm in our case),the
flow rate has little effect on the uncertainty and remains
around3-5% (or a ratio of 0.97 to 0.95). For example,for

T,'.'-T7= 5 K, dependingon the thicknessof the waterfilm,

4.85and4.75K, or theuncertainty
Assumingthat the surfaceareasand heat transfercoefficients T -T/ canrangebetween
is at most 0.25 K. Thus the temperatureuncertaintyis exare alsoequal, we get that
pectedto havea minoreffecton the instrument
performance

=r c

c,

and is thereforeneglected.

NENES

ET AL.: ANALYSIS

3461

OF CCN INSTRUMENTS
,

20
18

10

Water film thickness(% of gap)

Figure10. Contours
of (T,,- Tr)/(Th- Tc)fortheHCNSasa function
of flowrateandwaterfilmthickness.
The thicknessof the metalwall is assumedto be 1 cm, andno filter paperis used.

The presenceof the filter paperin the FCNS is expectedto

increasethe temperatureuncertainty,relative to the HCNS.
For a paperthicknessof 1 mm, which is well wetted,and wall
thicknessof I cm, the uncertaintyis around5%. A tenfold increasein the flow rate almostdoublesthe uncertainty,from 5
to 9% (or 0.95 to 0.91 ratio). For example,for T,"-T5= 5 K,
dependingon the thicknessof the water film, T]'-T; can
rangebetween4.75 and 4.55 K, or the uncertaintyrangesbetween 0.25 and 0.45 K. Thus althoughthe uncertaintyis increasedwith respectto the HCNS, it is still smallenoughto be

6. Operating Conditions
After assessingthe uncertaintyin the wall temperature
boundaryconditionfor each device, the geometricdimensions,operatingconditions,and aerosolusedfor simulating
the performance
of the instruments
needto be specified.The
dimensionsand operating conditions of each instrument,
which are summarizedin Tables 2 to 5, are thosereportedin
the literature. The SDCC dimensions were taken from an ex-

istinginstrument(P. Chuang,internalcommunication,
CaliforniaInstituteof Technology,1999). The FCNS, HCNS, and

considered minor.

Table 2. OperatingConditionsandParametersfor the SDCC (P. Chang,

internal communication, 1999)
Parameter
Distancebetweenplates,m
Radiusof plates,m
Thickness of view volume, m
Radius of view volume, m

Initial pressure,Pa
Initial relative humidity, %
Bottomplate temperature(constant),K
Top plate temperature(variable), K
Sidewall thickness, m

Thermal
conductivity
of sidewall,
W m'2K-1
Ambient temperature,K

Value/Range

lxlO -2
0.1

lxlO -3
lxlO -3
1.013 x 105
1 O0

290
292 to 297

2x 10-3
1.4 (Plexiglas)
290

3462

NENES

ET AL.: ANALYSIS

OF CCN INSUMENTS

Table 3. OperatingConditionsandParametersfor the FCNS [Fukutaand

Saxena, 1979]
Parameter

Value/Range
0.838, 0.191, 0.018

Length, width, and height,m

Orientation

Distance

vertical

from entrance where wall becomes

0.168, 0.168

wet on top and bottom plates, m

Inlet pressure,Pa
Inlet relative humidity, %

1.013x 105
100

1.6667x 10'4

Volumetric
flowrate,m s-

283

Inlet temperature(constant),K
Cold tip temperature(constant),K
Hot tip temperature(variable), K
Ambient temperature,K

CCNS dimensionswere on the basisof thosegiven in the literature [Fukuta and Saxena, 1979; Hudson et al., 1981; Hud-

son, 1989, Yumand Hudson,2000; Chuanget al., 2000]. The

dimensionsused for the HCNS simulations[Yum and Hudson,

283
284 to 293
290

7. Simulation

of Instrument

Performance

7.1. SDCC

First, it is useful to determine the extent of wall effects, the

2000] are different from thosereportedby [1989] and reflect

changesin the instrumentthat improveits resolution.Flow

time neededto attainthe steadystateprofiles,and the concentrationbelow which depletioneffects(in the water vapor and
fields)arenegligible.Simulationsrevealthatwall
ratesandwall temperatures
are allowedto varybut, again,re- temperature
flect reportedoperatingconditions.
effects extend inward of the order of the gap betweenthe
To determine the behavior of the instrument,we simulate plates,which coversroughly one seventhof the total radius.
theresponse
of eachinstrument
asa functionof initialparticle Thus wall effectsare not expectedto influencemeasurements

diameter;the inlet aerosolin all the simulations

presented
is made near the center of the instrument. The maximum conassumedto be monodisperseand composedof ammonium centrationof the aerosolwithin the instrument,beforedeplesulfate. The number concentration in each instrument is assumed to be low, in order to minimize their effect on the su-

tion effectsare seen,dependson both S,.and Smax;

simulations
indicatethatconcentrations
below 1000 cm-3insidethe SDCC
persaturation
andtemperature
fieldsfrom thedepletionof gas ensurethat the supersaturationfield is uninfluencedby the
phase water vapor. This is particularlyimportantfor the aerosol.When depletioneffects are not important,the time
SDCC, sincebiasesin the supersaturation
and temperature neededto achievesteadystaterangesbetween3 s (for 7-K diffields from the presenceof the aerosolcomplicategrowth ference)to 5 s (for 2-K difference).An interestingfeatureis
history.
that the supersaturation
profiles approachthe steadystatein a

Table 4. OperatingConditionsandParametersfor the HCNS [Hudsonet al.,

1981; Hudson, 1989; Yum and Hudson, 2000]
Pm'ameter

Value/Range

Length, width, height,m

Height of aerosolinjector
Length of wetted wall on hot and cold

0.38, 0.3, 0.015

0.0015

0.28, 0.38

side, m

Total numberof heatedsegments

Insulator length, m
Orientation

Sheath/aerosol

9
0.001
vertical

volumetric

flow ratio

Totalvolumetric
flowrate,m s-
Inlet pressure,Pa
Aerosol, sheathflow inlet temperature
(constant), K
Aerosol, sheath flow inlet relative

humidity, %
Minimum cold side temperature,K
Maximum hot side temperature,K

10 to 20

3.3 x 10-4to 5.0 x 10-5

3.09 x 104
295,295
100, 90
295-289
295-301

NENES

ET AL.: ANALYSIS

OF CCN INSTRUMENTS

3463

Table 5. OperatingConditionsandParameters
for theCCNS [Chuanget al., 2000]
Parameter

Value/Range

Length,radiusof tube,m
Radiusof aerosol
injector

0.7,9.27x 10
2.29x 10-3

Total numberof hot-coldpairs

Insulatorlength,m

7
0.01

Orientation of instrument

vertical

Sheath/aerosol volumetric flow ratio

0.7 to 20.0

Totalvolumetric
flowrate,mss-
Inletpressure,
Pa

1.166x 10-s
1.013x 10s

Inlet relative humidity, %

Aerosol, sheathflow inlet temperature

100
295, 295

(constant), K

Aerosol, sheathflow inlet relative

humidity, %
at,

100, 90
1.0, 1.0 (case 1)
0.98, 0.041(cases2-4)

ac

Wall segmenttemperatureprofiles, K

295,290, 295, 290, 295,290, 295, 285,295, 285, 295,283, 295,283 (case1)
295, 290, 295, 290, 295,290, 295,285,295, 285,295,283, 295,283 (case2)
294, 291,294, 291,294, 291,294, 287,294, 287,294, 285, 297,285 (case3)
294, 292, 294, 292, 294, 292, 294, 289,294, 289, 294, 287, 297,287 (case4)

nonsymmetric
fashion,from the bottomplate to the top. AlThe behaviorof the SDCC dependson the supersaturation
thoughthe direction(from bottomto top or vice versa)could profile, which can be characterized
by the maximumsuperchange(dependingon the initial conditionsin the instrument), saturation,Sin:x,and the critical supersaturation
of the obthe asymmetricapproachto a steadystateprofile would tend servedparticles.Particleswith S,--Stoa
x activateonlymidway
to bias the particles on one side of the view volume toward betweenthe platesand are observedas they grow and sedilarger sizes.The strengthof this bias dependson the duration ment out of that small region.Their growthrate is initially
of the transientsrelativeto the total growthtime.
slow' so concentration
peakslate. On the otherhand,particles
Plate 2a presentsthe simulatedeffective radius (defined as with S.<< Stoa
x grow throughoutmuch of the volume of the
the third momentover the secondmomentof the dropletsize SDCC and relativelyrapidly. Particlesthat activatewell above
distribution) within the view volume as a function of time for the view volumegrow and reachlargersizesas they sediment
differentdry aerosolsizes.Plate3a represents
the normalized towardthat level. The peak in ten
for 0.05-gm particlesoccurs
aerosol concentration in the view volume as a function of
as muchas 5 s later (not shown)thanthat for 0.5-gm particles.
time. In both plots, the initial aerosol concentrationis uni- This large variation may accountfor the multiple peaks in
form, and the temperaturedifferencebetweenthe plates is scatteredlight intensityprofilesseenwhen polydisperse
aerokept at 2 K. This temperaturedifferencegeneratesa maximum solsare sampled.
supersaturation
of about0.15%. Undertheseconditions,partiIncreasingthe temperaturedifference between the plates
cleswith dry diameterlargerthan 0.1 gm shouldactivate.In- increasesStarx.A larger range of particle sizes satisfiesthe
deed,this is what is seen.Simulationsfor 0.05- and 0.09-gm conditionS.<< Smax,
and the particle size dependenceof the
particles yield constant effective radius and concentration, effective radius decreases as illustrated in Plates 2b and 3b,
meaning that the particlesgrow to their equilibrium size, which are the sameas Plates2a and 3a, but for AT = 7 K (Smax
which is not large enoughto experiencesignificantsedimen- = 1.81%). All of the particle sizes considered activate
tationon the timescaleof the simulations.
Largerparticlesdo throughouthalf of the SDCC volume. Both the effective rashow variability, and they are the ones that activate.The be- dius and droplet concentrationin the view volume display
haviorof particleswith a dry diameterof 0.50 gm differsfrom similartime dependenceover the 0.05- to 0.5-gm sizerange.
those of the other sizes examined, because sedimentation veIn determining the precision of the droplet diameter atlocity of such particlesis appreciableeven for subsaturated tained in the view volume, we define the "dropletdiameter
conditions. As a result, the concentration in the view volume

resolution,"
Ro,,
= Dp/ADp,as the ratioof the meandiameter

increasesbecauseaerosolfrom above falls throughit more overitsvariation.

A valueof Ro.= 10 meansthatthedroplet
rapidly than the aerosolwithin the view volume falls out. The diameterrangesaround 10% of its mean value. A high value
concentration
of particlesof smallerinitial sizestaysrelatively of this resolutionthroughoutthe durationof the measurement
constant,as particles that fall out of the view volume are re- ensuresthat particles with the same critical supersaturation
placed by those from above. This behavior lasts roughly producedropletsthat are closeto being monodisperse
within
around 7 s, during which the slope of the effective radius theviewvolume.Plate4 displaysR,,,,asa function
of time,
curve is approximatelythe samefor all particle sizes.After for variousparticle sizes.Plate 4a assumesa temperaturedifmost of the aerosol above the view volume has passed ference between plates of 2 K, while Plate 4b is for a differthrough,the aerosolconcentration
startsdropping.
enceof 7 K. Becauseinitially the aerosolin the SDCC is per-

3464

NENES ET AL.' ANALYSIS OF CCN INSTRUMENTS

1.25

3.0

2.5

0.09

0.12

0.20

0.25

0.30

0.50

(a)

2.0

(a)

1.00

1.0

0.09

0.12

0.20

'

0.25

0.5
0.75

0.0

''1

0.300.50

10

10

Time

TllTI e

5.0

'

1.25

(b)

(b)

0.09

0.12

''

0.20

'

0.25

1.00

t'q

0.30

0.09

"0.12

0.20

0.25

0.50
0

Time

Plate2. Simulated
effective
radius
in theSDCC
view

0.75

.......

Time

window
asafunction
oftimeforvarious
initial
particles
sizes Plate3. Simulated
particle
concentration
intheSDCCview
(drydiameter,
micrometers).
Thetemperature
differencewindow
asafunction
oftimeforvarious
initial
particles
sizes
between
thetwoplates
is assumed
tobe(a)2 K (Srnax
= (drydiameter,
micrometers).
Thetemperature
difference

0.15%)
and(b)7
K(Srn,,x
= 1.81%).

between
thetwoplates
is assumed
tobe(a)2 K (Srn,,x
-0.15%) and(b) 7 K (Srn,,
= 1.81%).

NENES

ET AL.: ANALYSIS

OF CCN INSTRUMENTS

3465

urements. However, buoyancy forces develop that limit the

maximum temperaturedifference that can be imposed at a
given flow rate. Simulations indicate that the maximum temperaturedifferencethat can be imposedfor the reportedflow
rate is about 6 K, a value that agreeswith the experimentally
reported difference [Fukuta and Saxena, 1979]. Larger temperaturedifferenceslead to flow reversal.The simulationsare
relatively insensitiveto the specifictype of inlet velocity profile; so the resultspresentedapply to both inlet velocitytypes.
The supersaturationfields that develop within the instrument control the growth of aerosol particles.Although the
maximum value of the supersaturationcan be estimatedfrom
the local temperature difference between the hot and cold
walls and Figure 2, the supersaturation
profile has to develop

1000

first before this maximum

10

Time

100
0.09

'

0.20

' 0.12

0.25

& 10

value is attained. Plate 5 shows su-

persaturationprofiles for different streamlinesalong the centerline of the FCNS. As can be seen, half (or more) of the flow
path is subsaturated,exposing particlesto the maximum supersaturationfor only a fraction of their residencetime in the
instrument.Moreover, the time in the supersaturated
region
decreaseswith decreasingS...... Therefore particles with low
S,. may not have sufficient time to activate by the time they
reach the outlet. This difficulty is compounded by slow
growth once activatedat low S.....
Buoyancy effects on the velocity field tend to distort the
supersaturationprofiles from being symmetric around the
centerline;this deviation becomesstrongeras the temperature
difference between the plates increases.The position of the
maximum supersaturation
is also shiftedslightly.Furtheraway
from the tips, the temperaturegradient between the walls decreases,buoyancyeffects becomelessimportant,and symmetric supersaturation(and temperature)profiles are attained.The
centerlineregion, however, particularlyfor the low S,.streamlines, is relatively unaffectedby buoyancy.
Plate 6 showsthe simulatedresponsecurvesfor the FCNS.
The horizontal axis representsthe critical supersaturationof
the inlet aerosol, and the vertical axis is the outlet wet diame-

ter of the aerosol.Each curve representsa different centerline

streamlinewith its own supersaturation.The particleoutlet diameter is relatively insensitiveto the inlet aerosol size, for
particlesfor which Sc< Stoa,.Particlesof S.> Smax
do not acti-

(b)

vate: so there is a dramatic

decrease in outlet size. The result-

10; this meansthat the dropletsizesrangewithin 10% of their

mean diameter,regardlessof temperaturedifferenceor initial
particle size (Table 6).

ing "elbow" in the curve enablesdetectionof particleswith S

< Smxof the specific streamline,sincethere is a clear distinction between particlesthat activate and those that do not. The
sharperthis "elbow" is, the better resolvedthe CCN concentration is at the given supersaturation.Farther away from the
heated tips, the maximum supersaturationdecreases,and the
positionof the "elbow" shifts toward lower critical supersaturations. However, becausegrowth at lower supersaturationsis
slower and becausethe particle exposureto the maximum supersaturationis briefer, droplets do not grow as much (in
comparison with larger supersaturationstreamlines). As a
consequence,the elbow becomesless pronounced,eventually
vanishingcompletely.The elbow more or lessdisappearsat Sc
= 0.1%, in agreementwith the value reportedby Fukuta and
Saxena [1979]. In its CUlTentconfiguration, the FCNS can
probeeffectivelyCCN with S,.between0.1 and 1.0%.

7.2.

7.3.

Time

Plate 4. Simulated particle size resolutionin the SDCC view

window as a functionof time for variousinitial particlessizes
(dry diameter, micrometers). The temperature difference

betweenthe two platesis assumedto be (a) 2 K (Sm,,x

=

0.15%)and(b) 7 K (Sm,,x
= 1.81%).
fectly monodisperse,
the resolutionin both plots startsoff
from infinity.As the supersaturation
profilesdevelopandthe

particlesgrow, R,. dropsandfluctuates

aroundthe valueof

FCNS

The continuous flow in the FCNS eliminates some of the

limitations that arise from the transient nature of SDCC meas-

CCNS

At first glance, this instrumentseemsto avoid many of the

problemsencounteredin the FCNS. Buoyancyeffects are not

3466

NENES

ET AL.: ANALYSIS

OF CCN INSTRUMENTS

1.5
Acresolre;ion Z.,z

[ ..........

1.0

Cold

O.S
o.o
/

--0:140

--0.065
--- 0.015

0.0

0.1

0.2

0.3

0.4

0.5

0.6

0.7

y-position(m)
Plate 5. Supersaturation
(percent)profilesfor differentstreamlines
alongthe centerlineof theFCNS

lOO

Critical curve

lO

--0.190

--0.140
--0.115

0.090

--

0.065

Hot

I Aerosolregioni z

--0.040

--0.015
o.1

0.001

Cold

i i I l i iI

0.01

i i I ill I

0.1

Criticalsupersaturation
(%)
Plate 6. Simulatedgrowthcurvesfor selectedstreamlines
of theFCNS.The temperature
differencebetween

thetipsis5 K, andthevolumetric
flowrateis20L min-.

NENES ET AL.: ANALYSIS

OF CCN INSTRUMENTS

3467

Table 6. Summaryof SDCC Simulations

AT, K

Smax,%

D,/AD
sinViewVolume

Dry Diameter of Smallest

(NH4)2SO4 Particle
Activated, gm

Mean

Minimum

Maximum

0.15

0.101

14.8

12.6

0.34

0.059

10.0

8.3

13.7

0.60

0.040

10.2

5.0

12.7

0.93

0.030

8.9

4.0

11.4

1.34

0.024

9.3

0.2

13.4

1.81

0.019

10.5

8.7

13.0

21.0

significant,and most of the instrumentis utilized for exposing boundaryconditions.The predictedsize is larger(by abouta
the particlesto supersaturations
(Figure7). The supersatura- factor of 2) than the measureddata. When loweringthe temtion profile is, however,considerablymore complex, making peratureboundaryconditionby around2-3 K (which,acit more difficult

to assess instrument

behavior

on the basis of

the temperatureand supersaturation

profilesalone.It is, therefore importantto evaluatethe sensitivityof the predictedoutlet droplet distributionto the parametersthat affect particle
growth. Two very important parametersaffecting the simulations are the film temperatureat the wall (which determines
the supersaturation)and the mass accommodationcoefficient
(which affectsthe particle growth).
Figure 11 showspredictedand measuredcalibrationcurves
for the CCNS. Details about the experimental data can be
found in the work of Chuang et al. [2000]. Curves correspondingto cases1 to 4 in Figure 11 representthe temperature
boundaryconditionsand accommodationcoefficientsspecified in Table 5. Case 1 representsan accommodationcoefficient of unity and the nominal wall temperaturesas the wall

cordingto section5.2, is a reasonable

drop,especiallysince
latent heat flux throughthe film can furtherincreasethe uncertainty),the predictedcurves(case3, case4) lie closeto the

experimental
data.Changingthe accommodation
coefficient
from 1.0 to 0.041 further improvesthe predictions.In all
cases,though,the qualitativebehaviorof the curvedoesnot
change:the outletdiameterof dropletsis relativelyinsensitive
to critical supersaturation
(particularlywhen the dropletsare
activated).Thus the model capturesthe essentialfeaturesof
the instrumentdespitethe complexgrowthbehaviorimposed
by the supersaturation
profilethatdevelopsin the instrument.
For subsequent
simulations,
case3 conditions
areused.
From both simulationsand experimentaldata, it is clear
thatthe dropletsize at the outletof the CCNS is relativelyinsensitiveto the initial particlesize. For a rangeof critical su-

100

Experiment
---

Case 1

Case 2

........................................
Case 3
.................
Case 4

0.01

0.1

Critical supersaturation
(%)
Figure 11. Experimentaland simulatedcalibrationcurvesfor the CCNS. The differentsimulationcases
correspondto differentvaluesof effectivewall temperatureand accommodation
coefficients,the valuesof
which are given in Table 5.

3468

NENES

ET AL.' ANALYSIS

persaturationspanning2 ordersof magnitude,the outlet diameterchangesat most by a factor of 2. This low sensitivity
arisesfrom the particlegrowth kinetics.At the late stagesof
growth, when the particle is in the continuumsize regionand
soluteand surfacetensioneffects are minor, equation(1) can
be integratedto yield

OF CCN INSTRUMENTS

resolvingthe CCN spectrum.Sincethe aerosoloccupiesa finite regionof the flow field, not all particlesare exposedto
the samesupersaturation
or havethe sameresidence
time.As
a consequence,
a monodisperse
inlet aerosolwill producea
dropletdistribution
withfinitespread;
thiseffectmayinterfere
with theabilityto resolvea CCN spectrum,
sincedropletsof a

givensizeat theoutletarenotunambiguously
relatedto critical supersaturation.
This spreadat the outletis a functionof

D,2=D2 po

the sheathto aerosolflow rate ratio (becausethat determines

the uniformityof the supersaturation

field andresidence
time
to whichthe particlesare exposed)andwill decrease
with in-

I S,,dt
tact

(26)

AHvpPw
IAHvpM
'')
-1

4k,T

TR

creasingratio.
In determiningthe precisionof the dropletdiametermeas-

urementneeded,we usethedropletdiameter
resolution,
R,,,
and the criticalsupersaturation
resolution,Rsc
=S,./AS,.DiThe particlesize at activation,Dpo,is relativelysmall;so at viding thesetwo quantities,we get the "resolutionratio,"
sufficientlylong growthtime,

R,c/R,,,.,
whichcanthenberelated
totheinstrument
response:

Rs S,.Zp S,.
[dD.
l

- 0,,

ISdt
v

D2=

t't

--

(27)

4-

"-1

4p'D,M,

4k,,T

(28)

where[dDp/dS.].,.
is the slopeof the calibration
curveat the

TR

i.e., all particlesapproachthe samesize, regardlessof initial

size (or &). This asymptoticapproachof all particlesto the
samesize also explainsthe uniform responseof the SDCC for
S,<< Smxand the consistentfinal particlesize of the FCNS
over a wide rangeof supersaturations.
Despite the weak dependenceof outlet diameteron particle
critical supersaturation,
the simulationscan be used to computethe resolutionin measureddropletdiameternecessary
for

....................
0.7
-'-10

20

given&. Figure 12 displaysthe resolutionratio computedfor

the CCNS for different sheathto aerosolflow rate ratios.Figure 12 illustratesthat the resolutionin critical supersaturation
is between 10 and 100 times smallerthan the dropletdiameter
resolution for the volumetric flow rate ratio used in the cali-

brationexperiment.This meansthat if the diametermeasure-

menthasan uncertainty
of 1% (or Ro,,
= 100),theuncertainty
in critical supersaturation
will range between 10 and 100%.
Increasingthe flow rate ratio increasesthe resolutionnotably,
but only up to a certainextent;the differencein resolution
between ratios of 10 and 20 is quite minimal. This is understandablebecausethe aerosol at such a high flow rate ratio
occupiesa volumeverycloseto the centerline;sothe particles
are exposedessentiallyto a uniform supersaturation
profile.
The resolutionratio is also a strongfunction of St.:it varies
almostby a factor of 10 for St.,rangingbetween0.01 and 1%.
This is a result of the changein the calibrationcurve slope,
which approacheszero as St. increases;this meansthat for
particlesof high St, dropletsize is moreor lessinsensitiveto
St or that the asymptoticlimit of equation(27) haspractically
been reached.This is not true for activatedparticleswith low

S,; theDpotermin equation(26) is notnegligible,

andoutlet

0.1

particlesizestill varieswith &.

To estimatethe uncertaintyin critical supersaturation
from
the spreadinducedby the instrument,we use equation(28),
and obtain that

lAD,,
inst
IdDp
1-1
d..'
0.0!

0.01

0. I

(29)

whereAS,/S,is the supersaturation

uncertainty
andIADplinst
is

the variationin droplet diameter,calculatedfrom the instrument model.Figure 13 displaysAS,/S,.as a functionof superCriticalsupersaturation
(%)
saturation,for the CCNS. The uncertaintywas predictedby
using
the curvesof Figure12 andthe variabilityof the calcuFigure12. Predicted
resolution
ratioRs,/RI,,fortheCCNS,
for different values of l)he..tdl)..e,.oso,.
The case 3 (Table 5) latedoutletdropletdiameter.As can be seen,the resultingunvalues of effective wall temperature and accommodation certaintyis large, rangingfrom 100 to over 1000%. This is
coefficients are used.
expected,sincetherelativevariationin dropletdiameterat the

NENES

ET AL.' ANALYSIS

1ooo

OF CCN INSTRUMENTS

3469

reveal that the droplet growth kinetics, like those for the
CCNS, lead to a restrictedrangeof final dropletsize for particles with a wide range of critical supersaturations.
For example, when the maximumplate temperatureis set to more than
6 K, the outlet droplet diameterchangesby a factor of 2 for
critical supersaturations
that span 2 ordersof magnitude(between 0.01 and 1%). This variation does not seem to be
stronglyinfluenced by the volumetric flow rate (althoughthe
outlet droplet diameter is) but dependsstronglyon the temperatureprofile in the instrument.Improvementis seen only
when the maximum temperaturedifference drops to 4 K; in
this case, the variation in droplet diameter increasesconsiderably but has the drawbackthat particleswith St.> 0.4% do

lOO

not activate. As can be seen, the resolution of the instrument

increasesas the outlet droplet size gets closer to the critical

curve;the drawbackto this is that the S.rangefor which particles are activated becomes more restricted.

Calibration data available in the literature [Yum and Hud-

son, 2000] do not preciselyspecifythe maximum temperature

difference (or the total volumetric flow rate) used in the
lO
HCNS, making it difficult to preciselyassessthe performance
O.Ol
o. 1
1
of the HCNS model. In addition, the data provide the mean
Critical supersaturation
(%)
channel number (as opposedto particle diameter) as a function of critical supersaturation.However, since mean channel
Figure 13. Relative critical supersaturation
uncertaintyas a numberscaleslinearly with particle size, the nondimensionalfunction of critical supersaturation,
for the CCNS. Each curve ized mean channel number and mean particle diameter are
represents
differentvaluesof Phe,h/l
......,. The uncertainty equivalentquantities:
was predicted by using the curves of Figure 12, and the
variability of the outlet droplet diameter (calculatedby the

F(S,)-F(S,hlgh) mp(s)-mp(S,
hlgh)
F(Xrlou,)--F(Xrhtgh
)

model results).

CCNS outlet is, on average,between15 and 20% (Table 7).

Thereforethe aerosol/sheath
flow rate ratio usedfor the operationof this instrumentis very influentialfor obtaininga

where F is the mean channel correspondingto critical supersaturationS,..Using these non-dimensionalizedquantities,we

comparemeasurementsto the model predictions(Plate 8). As
CCN spectrum.While increasingthis ratio to 10 or 20 consid- can be seen,the measurementsare very closeto model predicerably reduces the uncertainty,the uncertainty still exceeds tionsfor a volumetricflow rate of 20 L min- and a maximum
50% for S,. > 0.04%. Further increasingthe flow ratio might temperaturedifference of 6 K. Given that thesevaluesof flow
decreasethe uncertainty,but obtaininggood dropletcounting ratesand maximumtemperaturedifferenceare within reported
statisticsthen becomesa problem.
operatingconditions,we can assumethat the model captures
the behavior
7.4.

HCNS

of the HCNS.

Plate9 displaysthe predictedresolutionratio, R&/Rn,,,

for

The HCNS exposesparticlesto supersaturation

profilesthat the HCNS, for different temperatureprofiles and total voluvary smoothlyand monotonicallyin the streamwisedirection. metricflowratesof: (Plate9a)6 L min', and(Plate9b)20 L
Simulationswere performedfor severaldifferent temperature min-. The sheathto aerosolflow ratio was assumedto be 10.

profiles
atlow(6 L min-)andhigh(20L min-)totalvolumet- Here the instrument sensitivityis increasedin relation to that
ric flow rates (Plates7a and 7b, respectively).The sheathto
aerosol flow ratio was assumed to be 10. These simulations

of the CCNS, particularlyfor low temperaturedifferencesand

critical supersaturations
between0.1 and 1%. For a maximum

Table 7. PredictedOutletDropletDiameterVariabilityandResultingCriticalSupersaturation
............

.y................

Psheath

q.... ret,,,-tirnRanger,txx,,,mfi fil and 1 n)

ZDp,
%

Q......1

AS
c,%

Dp

Mean

Minimum

S,

Maximum

Mean

Minimum

Maximum

0.7

28.9

9.7

57.4

303.0

25.1

1326.2

10.0

5.5

1.1

36.5

53.7

2.7

755.3

20.0

4.0

0.6

19.3

38.6

1.5

388.3

3470

NENES

ET AL.: ANALYSIS

OF CCN INSTRUMENTS

variabilityof the outlet dropletdiameter.Plate 10a refersto a

lOO

(a)

volumetric
flow rateof 6 L min-I, andPlate10bhasa flow
rateof 20 L min-l (sheath
to aerosol
ratiois 10) For these
conditions, the relative variation in droplet diameter at the
HCNS outlet is on averageonly between2 and 3% (Table 8).

However,this is enoughto generatesubstantialuncertaintyin

S,..Minor fluctuationsin this variabilityaccountfor the large
fluctuationsseen in the computeduncertainty.For example,
for a maximumtemperaturedifferenceof 8 K (whichis an operationalvalue reportedby Hudson[ 1989]), the Scuncertainty
rangesbetween30 and 100% andcan reachas high as 390%.
When the maximumtemperaturedifferenceis around4 K, the
resolutionimprovesby an order of magnitudeand averages

lO

around 10%. The simulationsindicate that a spectrumcan be

obtainedfor critical supersaturations

between0.08 and 0.8%.
Particlesoutsideof this range do not activate,either because
the supersaturation
is lower than the criticalvalueor simply

6
Critical

curve

....... 10

because

12

Ol
0.1

O.Ol

there

are

kinetic

limitations

that

inhibit

low-

supersaturation
particlesfrom activating.
Comparedwith the CCNS, the HCNS seemsto exhibitless
uncertainty;this is attributedto the smootherand monotonic
supersaturation
profilesgeneratedin the HCNS. The oscilla-

Criticalsupersaturation
(%)

tions in the flow direction seen for CCNS slow down (or even

lOO

(b)

reverse)particlegrowth;so lessof the instrumentis utilized

for particlegrowth.Becauseof this,particlesof differentcritical supersaturations
essentiallygrow to the samesize by the
time theyreachthe outletof the instrument.

8. Summary and Conclusions

10

The behavior and performanceof four cloud condensation

nucleus instrumentsare theoretically analyzed.These include
the static diffusion cloud chamber (SDCC), the Fukuta continuous flow spectrometer(FCNS), the Hudson continuous
flow spectrometer(HCNS), and the Caltech continuousflow
spectrometer(CCNS). A numericalmodel of each instrument
on the basisof reportedinstrumentdimensionsand operating
conditionsis constructedon the basis of a general fluid dynamics code coupled to a description of aerosol
growth/activationmicrophysics.Instrument performanceis

12

exploredby simulatinginstrumentresponseto a monodisperse

6
8

Critical curve

ammonium

0.1
O.Ol

0.1

Criticalsupersaturation
(%)
Plate 7.

Simulated calibration curves for the HCNS, for

various maximum temperaturedifferences,ATmax(the AT at

thelastsegment),
anda volumetric
flowrateof (a)6 L min-
and(b) 20 L min-.Thetemperature
difference
between
each
segmentis assumedto increasewith a constantstep ("linear
ramp") on both cold and warm sides.

temperaturedifference of 4 and 6 K, the resolutionincreases

dramaticallyfor Sc> 0.1%. This happensbecausethe supersaturationgeneratedin thesecasesis not sufficient to activate
particleswith Sccloseto 1%; so an "elbow" similar to thosein

Plate 6 develops.Consequently,
the calibrationcurve slope
becomesmuch steeperaroundthe region of this elbow. Becauseof this, it is expectedthat the uncertaintyin the critical
supersaturation
is considerablylower than that for the CCNS.
Indeed, this is the case,as is shownby Plate 10. The uncertainty wascomputedby usingequation(28) and the calculated

sulfate

aerosol.

The

CCNS

and HCNS

models

were comparedwith experimentalmeasurements

and foundto
be in good agreement.The FCNS model predictionsagreed
with instrumentlimitationsreportedin the literature.
Uncertainties in the wall temperatureboundary condition
vary with instrumentconstructionand arise mainly from the
presenceof filter paper (used for wetting instrumentwalls).
Using a simpleheat transfermodel for each instrument,this
uncertaintyis found to be negligible for the SDCC (of the order of 0.01 K) and very small for the HCNS and FCNS (ranging between0.25 and 0.45 K). It can be appreciablefor the
CCNS (rangingbetween0.5 and 2 K); so the wall boundary
condition in the instrument simulations must be adjusted to
account for this. The numerical model for the CCNS reproducesexperimentalmeasurements,
when the wall temperature
boundary conditions is adjusted by a factor slightly higher
thanthat predictedby this simpleuncertaintyanalysis.
SDCC exhibit the least uncertaintyin the wall temperature
boundaryconditionsand producedropletsthat are (for a given
critical supersaturation)monodisperseto within 10% of the
dropletdiameter,throughoutthe durationof the measurement.
The FCNS is an instrumentthat can be used as a CCN spec-

NENES

ET AL.'

ANALYSIS

OF CCN

INSTRUMENTS

3471

1.0

Experiment

0.9

V=6,
--V=6

AT=4
AT=6

V=20

AT=4

V=20

AT=6

0.6

0.7

0.2

0.1

0.0

0.1

0.2

0.3

0.4

0.5

0.8

Critical supersaturation
(%)
Plate8. Experimental
andsimulated
calibration
curvesfor theHCNS.Non-dimensionalized
dropletdiameter
is plottedas a functionof critical supersaturation.
V is the total volumetricflow rate, and AT is the maximum
temperature
differencebetweentheplates. p.,he.,,hlpc,.
....,= 10 in thesimulations.

Table 8. PredictedOutlet Droplet DiameterVariability andResultingCritical Supersaturation

Uncertainty

fortheHCNS(P,he.,t/P,.o,o,
= 10,Critical
Supersaturation
Range
Between
0.01and1.0%)

Maximum
I?,
AT,K

ADp
%

Lmin
q

ASc,
%

Dp'

Mean

Minimum

S,.

Maximum

Mean

Minimum

Maximum

2.6

0.5

9.0

14.1

1.2

30.9

2.7

0.6

8.6

35.5

7.5

67.2

3.2

0.5

9.2

102.5

15.8

393.2

10

3.6

0.6

12.8

163.2

16.0

670.2
723.8

12

3.0

0.4

10.1

203.8

20.2

20

2.4

0.6

10.0

11.4

0.9

26.3

20

2.8

0.4

8.8

22.4

7.3

47.9

20

3.1

0.4

7.4

31.5

5.6

61.6

10

20

2.6

0.5

7.2

76.7

14.2

259.6

12

20

3.2

0.3

11.6

108.3

7.8

423.4

3472

NENES

ET AL.' ANALYSIS

OF CCN INSTRUMENTS

1000

4
10

....... 10

....... 8
12

0.1

VV/, , .vl ....

113
0.01

0.1

0.01
0.01

Criticalsupersaturation
(%)

0.1

Critical Supersaturation
(%)
1000
10.

4
4

6
8

>,

10
12

.... 10

'

'

12

01

0.01
0.01

CriticalSupersaturation
(%)

0.01

0.1

Criticalsupersaturation
(%)

Plate9. Predicted
resolution
ratioRs,./R,,,,
fortheHCNS,for
differentATm:,x,
anda volumetric
flow rateof (a) 6 L min-

and(b)20L min-. pshc,/p:e,.oso,=

10inthese
simulations.

Plate 10. Relativecritical supersaturation

uncertaintyas a
function of critical supersaturation,for the HCNS. The
uncertaintywas predictedby usingthe curvesof Plate 9 and

thevariabilityof theoutletdropletdiameter(calculated
by the

modelresults).
Volumetric
flowratesof (a)6 L min-[ and(b)

20L min-l. shealh/Pae,.osol

= 10inthese
simulations.

NENES

ET AL.: ANALYSIS

OF CCN INSTRUMENTS

trometer,sincedifferentstreamlines
attaindifferentsupersatu- kw,,
rations,allowingparticlesto activateover a rangeof critical kwa
t
supersaturations.
The range of critical supersaturations
that 1
can be measuredis limited because(1) the temperaturediffer- L
encemustbe kept smallenoughto avoidbuoyancy-inducedM,,
flow reversalor secondary
flows and (2) the instrumentloses
its sensitivityfor particlesof critical supersaturation
lower n
than0.1% becausethe particlesdo not haveenoughtime for
growth.The first issueis not a seriouslimitation, sincethe su- N
persaturationon the high temperaturedifference side is suffi- P
ciently high to includeall the climaticallyimportantaerosol. Pr
The secondlimitation,however,constrains
the abilityto probe p,
the climaticallycriticallow supersaturation
CCN. Both HCNS p,
and CCNS have inherentlimitationsin the ability to resolve
the distributionof particleswith respectto critical supersatu- r
ration. The most importantparametersaffectingthe perform- R
ance of dynamicspectrometers
are the maximum temperature Ra

difference
between
thewalls,thetotalvolumetric
flowrate,
and the sheathto aerosolvolumetric flow ratio. For the mono-

3473

thermal conductivity of wall.

thermalconductivityof liquid water.
paperthickness.
instrumentlength.
molecular weight of dry air.
molecular weight of water.
number of size sections in aerosol distribution.

numberof molesof soluteper particle.

aerosol number concentration.

air pressure.
Prandtl

number.

water vapor pressure.

saturationvapor pressureof water.

heat flux.

radial coordinate.

universal gas constant.

Rayleigh number.

dropletdiameter
resolution,
Dp/AD.
Re

disperse
ammonium
sulfate
aerosol
considered
here,condi-

Reynoldsnumber.

tionscan be foundfor the HCNS for whichan activation R,

criticalsupersaturation
resolution,&IASc.
thermalresistancethroughthe soakedfilter paper.

spectrumcan be resolvedfor critical supersaturations

between

wall coordinate

0.08 and0.8%. Simulations

for the HCNS indicatethatthe
calculated uncertainty in critical supersaturationexceeds
100% when the maximumtemperaturedifferenceexceeds6 K
for 20 L min- total flow rate or 8 K for 6 L min- total flow.
The sameuncertaintycan decreaseto 10% (on average)when
the temperaturedifferenceis reducedto 4 K. The uncertainty,
however, is not uniform and dependsstronglyon the initial
size of the particle. The predicteduncertaintyin the critical
supersaturation
for the CCNS is on averageabove50%.
While different designparametersor operatingconditions
may lead to modestshifts in the performancefrom that predicted for any of the four instruments,the essentialfeatures
describedin this paperare inherentto their designs.

of FCNS

instrument.

critical supersaturation
for activation,accordingto
KOhlerequilibriumtheory.
max maximum supersaturation.
supersaturation.
supersaturation
in equilibrium with particlesize.
time.

averagetemperatureof SDCC wall.

temperature.

bulk sectionaverage(bulk) temperature.

v

volumetric

flow rate.

terminal velocity.
velocity component.
u

heat transfer coefficient.

velocity component.
Notation
A

heat exchangearea.
condensation

coefficient.

thermal accommodation

coefficient.

water vapor concentration,molesper cubic meter.

specificheatof controlled-temperature
wall.
specificheat of dry air at constantpressure.
slip correctionfactor.

wall thickness.

instrument

WL

liquid watercontent(kilogramof liquid waterper vol-

ume of air).
x,, x2 generalizedspatialcoordinates.
x, y
Cartesiancoordinates.
z

water
vapor
diffusivity
inair,corrected
fornoncon-

Dp

water film thickness.

mean free path of air.

air viscosity.

Vs

particle
wetdiameter.
P
mean
channel
number
inparticle
sizemeasurement
of

HCNS.
g

acceleration
ofgravity.

heat transfer coefficient.

instrumentheight.
Jbuoy momentumgeneratedby thermalbuoyancy.
Jco.d rate of liquid watercondensation
on aerosolparticles.
k
thermal conductivityof air.
thermalconductivityof air, correctedfor noncontinuum
effects.

kpapethermal conductivityof filter paper.

kststeelthermalconductivityof stainlesssteel.

axial coordinate.

L/va
p enthalpyof evaporation
of water.

particle
drydiameter.
water
vapor
diffusivity
inair.
tinuumeffects.

width.

number of ions the solute dissociates into in solution.

densityof air.
densityof particle.
densityof water.
water surface tension.

Subscripts-superscripts
amb
f
c
h

ambient.

film.
cold wall.
hot wall.

wall.

t
b

top wall.
bottom

wall.

3474

NENES ET AL.: ANALYSIS

OF CCN INSTRUMENTS

Acknowledgments.This work was supported

by Office of Naval Laktionov,A. G., A constant-temperature
methodof determining
the
Research
grantN00014-91-0119.
We wouldalsoliketo acknowledge concentrationsof cloud condensationnuclei, Izv. Acadsci. USSR
Timothy VanRekenfor performingpart of the CCNS calibration
Annos.OceanicPhys.,Engl. Transl., 8, 672-677, 1972.

curve experiments.

Lala, G. G., and J. E. Jiusto,An automaticlight scatteringCCN

counter,J. AppI. Meteorol., 16, 413--418, 1977.
McMurry, P. H., A review of atmosphericaerosolmeasurements,At-

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