Helmut Roth, Weimin Jiang, Dazhong Yin, and É ric Giroux
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Institute for Chemical Process and Environmental Technology
Helmut Roth, Weimin Jiang,
Dazhong Yin, and Éric Giroux
CMAQ Nucleation Algorithms and their impact on PM modeling results
in the Lower Fraser Valley
National Research Council of Canada
Ottawa, Canada
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Institute for Chemical Process and Environmental Technology
• Introduction
• Nucleation Rates
• Impact on PM
• Conclusions & future work
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Institute for Chemical Process and Environmental Technology
IntroductionIntroduction
• Episode: Pacific ’93 (1993 Jul 31 – Aug 07)
• Emissions: SMOKE, Giroux, É. et al
• Meteorology: MM5, Yin, D. et al
• Domain
• Nucleation Algorithms
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Institute for Chemical Process and Environmental Technology
Horizontal domainsHorizontal domains
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Institute for Chemical Process and Environmental Technology
Nucleation parameterizations & algorithmsNucleation parameterizations & algorithms
• HK98: Harrington and Kreidenweis (1998) Fully coupled equations of 2-mode 2-moment model implemented in aero2
• KLPx: Kulmala et al (1998) Equations of classical nucleation theory Implemented in aero2, aero3: KLP2, KLP3 Differences in number distribution, density
• sulphuric acid – water system
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Institute for Chemical Process and Environmental Technology
Nucleation rates: Nucleation rates: modeling modeling
C M A Qa ero_ noop
em is
m et
o ther
[S U L A E R ]C T M _ C O N C
dtd river
a ero2nu cl on ly
H K 9 8 | K L P 2 | K L P 3
nu clea tionra tes
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Institute for Chemical Process and Environmental Technology
11stst layer domain-average number rates layer domain-average number rates
Layer1 mean [number] production rate
1.0E+00
1.0E+03
1.0E+06
1.0E+09
0 12 0 12 0 12 0 12 0 12 0 12 0 12 0 12 0
Time of day, 1993 Jul 31 0:00 to Aug 08 0:00, PDT
nu
clea
tion
rat
e (#
/ m
3 / s)
1.0E-10
1.0E-07
1.0E-04
sula
er c
onc
(pp
mV
)
HK98 NUMi
KLP3 NUMi
meanL1 sulaer
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Institute for Chemical Process and Environmental Technology
11stst layer domain average ASO4I rates layer domain average ASO4I rates
Layer1 mean [ASO4i] production rate
1.0E-15
1.0E-12
1.0E-09
1.0E-06
1.0E-03
0 12 0 12 0 12 0 12 0 12 0 12 0 12 0 12 0
Time of day, 1993 Jul 31 0:00 to Aug 08 0:00, PDT
m g /
m3
/ s
HK98 ASO4i
KLP2 ASO4i
KLP3 ASO4i
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Institute for Chemical Process and Environmental Technology
11stst layer number rate statistics layer number rate statistics
peak cell
(Aug05 13:00) peak domain average
(Aug05 14:00) episode average
HK98 5.15e09 6.30e07 16.2e05 KLP2 10.95e09 2.82e07 2.12e05 KLP3 10.95e09 2.82e07 2.12e05
all maxima occur in cell (17,8)
Neptune Beach
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Institute for Chemical Process and Environmental Technology
Time-average, 1Time-average, 1stst layer number rate layer number rate
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Institute for Chemical Process and Environmental Technology
Correlation at time of peak nucleationCorrelation at time of peak nucleation
KLP3 vs HK98 #
1.00E+00
1.00E+02
1.00E+04
1.00E+06
1.00E+08
1.00E+10
1.00E+06 1.00E+07 1.00E+08 1.00E+09 1.00E+10
HK98
KL
P3
> m
in
KLP3 #
r2=0.9
Aug 05
13:00
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Institute for Chemical Process and Environmental Technology
Impact on PM concentrations: Impact on PM concentrations: model runsmodel runs
• Common inputs
• Full gas phase calculations
• All aerosol processes
• Different nucleation algorithms:NOOP HK98 KLP2 KLP3
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Institute for Chemical Process and Environmental Technology
Number concentrationNumber concentration
0.0E+00
2.0E+09
4.0E+09
6.0E+09
0 12 0 12 0 12 0 12 0 12 0 12 0 12 0 12 0
Time of day
[nu
mb
er]
(m
-3)
Noop
HK98
KLP2
KLP3
i-mode
PM2.5
First layer mean PM2.5 [number]
0.0E+00
2.0E+09
4.0E+09
6.0E+09
0 12 0 12 0 12 0 12 0 12 0 12 0 12 0 12 0
par
ticl
es /
m3
Noop # 25
HK98 # 25
KLP2 # 25KLP3 # 25
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Institute for Chemical Process and Environmental Technology
Time-average, 1Time-average, 1stst layer NUMATKN layer NUMATKN
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Institute for Chemical Process and Environmental Technology
Sulphate (ASO4) concentrationSulphate (ASO4) concentration
0.00
0.05
0.10
0.15
0.20
0.25
0 12 0 12 0 12 0 12 0 12 0 12 0 12 0 12 0
Time of day
[AS
O4
I] (
ug
m-3
)
Noop
HK98
KLP2
KLP3
0.4
0.8
1.2
1.6
2.0
0 12 0 12 0 12 0 12 0 12 0 12 0 12 0 12 0
NoopASO4
HK98ASO4
KLP2ASO4
KLP3ASO4
PM2.5
i-mode
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Institute for Chemical Process and Environmental Technology
Time-average, 1Time-average, 1stst layer ASO4I layer ASO4I
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Institute for Chemical Process and Environmental Technology
Main ConclusionsMain Conclusions
• KLP2 and KLP3 results very similar
• KLPx had greatest individual cell rate.
• HK98 had greatest average rates.
• HK98 more responsive to [SULAER] fluctuations.
• HK98 increases number concentration over NOOP; KLPx does not.
• No increase in PM2.5 SO4 mass over NOOP.
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Institute for Chemical Process and Environmental Technology
Future workFuture work
• Impact of nucleation algorithms on model performance using ambient number concentration data
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AcknowledgementsAcknowledgements
• U.S. EPA: CMAQ source code
• Environment Canada: emissions and met data, ambient PM mass data
• Program of Energy Research and Development (PERD) in Canada: funding support
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Thank you !Thank you !
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Institute for Chemical Process and Environmental Technology
Time-average, 1Time-average, 1stst layer mass rate layer mass rate
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n u cle a t io n _ K L P2 /n u cle a t io n _ K L P3 /n u cle a t io n _ H K 9 8 /n u cle a t io n _ n o o p
a e ro pro c
a e ro _ driv e r
a e ro s te p m o de _ m e rg in g /m o de _ m e rg in g _ n o o p
PM e m is /PM e m is _ n o o p
1
1
aer o _ d ata
1
c o n s t_ d ata
5
air _ d ata
4
aer o em is _ d a ta
3
p r ec u r s r _ d ata
2
in o re ql_ e ql3 /in o re ql_ e ql3 _ n o o p
co n d_ n u cl/co n d_ n u cl_ n o o p
S O A _ Pa n dis /S O A _ O du m /S O A _ S ch e ll/
S O A _ n o o p
co a g u la t io n /co a g u la t io n _ n o o p
o de _ s o lv e r s ize v a r
s ize v a r
1
1
1
1 1
1
1
1
1
2 3 4
5
2
2
2
5
3 5
2
4
4
44
4
5
5
5
5
5
5
5
2
5
5