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Cloud field Dobson O 3. Gaseous Reactions SAPRC-99. Gas-phase absorption Tropospheric O 3. Gaseous Loss. Photolysis Rates. On-line TUV. Heterogeneous Reactions (Dust). Gas-Aerosol Equilibrium interaction. Dust surface saturation. Aerosol Production. Aerosol Optical Properties. - PowerPoint PPT Presentation
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Dust, Aerosol Ions and Their Interactions with Gaseous Species in East Asia during Springtime 2001: Three-Dimensional Model Study Combining Observations
Youhua Tang1, Gregory R. Carmichael1, John H. Seinfeld2, Donald Dabdub3, Rodney J. Weber4, Barry Huebert5, Antony D. Clarke5, Gakuji Kurata6, Sergio A. Guazzotti7, David A. Sodeman7,
Kimberly A. Prather7, Itsushi Uno8, Jung-Hun Woo1, David G. Streets9, Chul-Han Song4, Adrian Sandu10, Theodore L. Anderson11, Robert W. Talbot12 and Jack E. Dibb12
1. Center for Global and Regional Environmental Research, University of Iowa2. Dept. of Chemical Engineering and Environmental Science Engineering,
California Institute of Technology
3. Dept. of Mechanical and Aerospace Engineering, U. of California at Irvine4. School of Earth and Atmospheric Sciences, Georgia Institute of Technology5. School of Ocean and Earth Science and Technology, University of Hawaii6. Dept. of Ecological Engineering, Toyohashi University of Technology, Japan
7. Dept. of Chemistry and Biochemistry, University of California at San Diego 8. Research Institute for Applied Mechanics, Kyushu University, Japan9. Decision and Information Sciences Division, Argonne National Laboratory10. Dept. of Computer Science, Virginia Technical University11. Dept. of Atmospheric Science, University of Washington at Seattle12. Dept. of Earth Sciences, University of New Hampshire
Framework of Chemical Interactions
3332
24223
NODust
HNO NODust
NO
SODust
SO 1.5ODust
O
To represent the involvement of dust in heterogeneous chemistry we define the dust surface fresh ratio as
active
activefresh Ca
NOCaCaSOCaD 234 )(
where Caactive is the amount of dust active calcium that is
available for heterogeneous reactions:
Cloud fieldDobson O3
On-line TUV
Aerosol Optical
Properties
Gas-phase absorptio
n
Tropospheric O 3
Photolysis Rates
AerosolEquilibrium Module
SCAPE
Gaseous ReactionsSAPRC-99
HeterogeneousReactions (Dust)
Gas-A
erosol E
quilib
rium
interaction
Gaseous Loss
Dust su
rface
satu
ratio
n
Aeroso
l Pro
duction
Four aerosol size bins are used: 0.1µm-0.3µm, 0.3µm-1.0µm, 1.0µm-2.5µm, and 2.5µm-10µm (referred to as bins 1 to 4, respectively).
TA
S T
otal Ca (µ
g/std m
3)
Ca Increase
Sim
ulated
Total C
a (µg/std
m3
)
Ca Increase
Irregular Points
Re-Colored by Coarse Dust Fresh RatioThe C-130 measurements of sulfate and nitrate coarse ratios show different correlations under different dust loading, represented by the Ca concentrations. When dust loading increased, the correlations show less variation and converge to a certain point related to dust coarse ratio. Both model and measurements show similar trends. The simulations also show some points that do not follow this trend. For these points, nitrate and sulfate coarse ratios are linearly related. Re-colored by the coarse dust fresh ratio, these points were identified as fresh (un-aged) dust. When dust was very fresh, both nitrate and sulfate increase their coarse ratios since they follow similar uptake mechanisms.
0 2 4 6 8 10T IM E (G M T )
0
2
4
6
Fin
e A
mm
oniu
m (
ug/
std
m3 )
0
2000
4000
6000
8000
Alt
itu
de
(m)
PILS ObservedSim ulated with DustSim ulated without DustFlight Altitude
0 2 4 6 8 10T IM E (G M T )
0
0.2
0.4
0.6
Du
sr F
resh
Rat
ios
0
2000
4000
6000
8000
Alt
itu
de
(m)
Fine Dust Fresh RatioCoarse Dust Fresh RatioFlight Altitude
0 0.2 0.4 0.6 0.8 1M o d e le d R a tio s
0
1000
2000
3000
4000
5000
6000
7000
Alt
itud
e (m
)
Fine Dust Fresh RatioCoarse Dust Fresh RatioSulfate Fine RatioNitrate Fine RatioAmmonia Aerosol Ratio
0 4 8 12Io n C o nc e n tr a tio n s (u g /s td m 3)
0
1000
2000
3000
4000
5000
6000
7000
Alt
itud
e (m
)
Simulated Fine CaSimulated Coarse CaPILS Fine CaMOI Coarse CaSimulated Fine CO3Simulated Coarse CO3
C-130 Flight 8 encountered aged dust Dust did not influence the sub-micron sulfate, but significantly increased the super-micron sulfate concentration. Sub-micron dust ages faster than the super-micron dust.
9 9 1 0 0 1 0 1 1 0 2 1 0 3 1 0 4J u lian D a y (G M T )
0
0.2
0.4
0.6
0.8
1
Ion
Fin
e R
atio
s an
d T
otal
Dus
t F
resh
Rat
io0
1000
2000
3000
4000
AG
L (
m)
Sulfate Fine RatioNitrate Fine RatioDust Fresh RatioAltitude (AGL)Longitude
9 0
1 0 0
1 1 0
1 2 0
1 3 0
Lon
gitu
de
9 9 1 0 0 1 0 1 1 0 2 1 0 3 1 0 4J u lia n D a y (G M T )
0
4
8
12
16
20
Fin
e Io
ns
(ug/
std
m3 )
CalciumAmmoniumNitrateSulfate
9 9 1 0 0 1 0 1 1 0 2 1 0 3 1 0 4J u lia n D a y (G M T )
0
2
4
6
8
Coa
rse
Ion
s (u
g/st
d m
3 )
CalciumAmmoniumNitrateSulfate
Extracted model results along trajectory C (shown left) illustrating the dust aging process and composition variation.
0 2 4 6 8T IM E (G M T )
0
2
4
6
8
Fin
e C
alci
um (
ug/s
td m
3 )
0
2000
4000
6000
8000
Alt
itu
de
(m)
PILS ObservedSimulated with DustSimulated without DustFlight Altitude
0 2 4 6 8T IM E (G M T )
0
5
10
15
20
25
Tot
al C
alci
um (
ug/s
td m
3 )
0
2000
4000
6000
8000
Alt
itu
de
(m)
TAS ObservedSimulated with DustSimulated without DustFlight Altitude
0 2 4 6 8T IM E (G M T )
0
0.2
0.4
0.6
0.8
Fin
e M
agn
esiu
m (
ug/
std
m3 )
0
2000
4000
6000
8000
Alt
itu
de
(m)
PILS ObservedSimulated with DustSimulated without DustFlight Altitude
0 2 4 6 8T IM E (G M T )
0
1
2
3
Tot
al M
agne
sium
(u
g/st
d m
3 )
0
2000
4000
6000
8000
Alt
itu
de (
m)
TAS ObservedSimulated with DustSimulated without DustFlight Altitude
0 2 4 6 8T IM E (G M T )
0
4
8
12
16
Fin
e S
ulf
ate
(ug/
std
m3 )
0
2000
4000
6000
8000
Alt
itu
de
(m)
PILS ObservedSim ulated with DustSim ulated without DustFlight Altitude
0 2 4 6 8T IM E (G M T )
0
4
8
12
16
Tot
al S
ulfa
te (
ug/s
td m
3 )
0
2000
4000
6000
8000
Alt
itud
e (m
)
TAS ObservedSimulated with DustSimulated without DustFlight Altitude
0 2 4 6 8T IM E (G M T )
0
1
2
3
4
5
6
7
Fin
e N
itra
te (
ug/s
td m
3 )
0
2000
4000
6000
8000
Alt
itud
e (m
)
PILS ObservedSimulated with DustSimulated without DustFlight Altitude
0 2 4 6 8T IM E (G M T )
0
2
4
6
8
10
Tot
al N
itra
te (
ug/
std
m3 )
0
2000
4000
6000
8000
Alt
itud
e (m
)
TAS ObservedSimulated with DustSimulated without DustFlight Altitude
0 2 4 6 8T IM E (G M T )
0
2
4
6
Fin
e A
mm
oniu
m (
ug/
std
m3 )
0
2000
4000
6000
8000
Alt
itud
e (m
)
PILS ObservedSimulated with DustSimulated without DustFlight Altitude
0 2 4 6 8T IM E (G M T )
0
1
2
3
4
5
Tot
al A
mm
oniu
m (
ug/
std
m3 )
0
2000
4000
6000
8000
Alt
itu
de
(m)
TAS ObservedSimulated with DustSimulated without DustFlight Altitude
0 2 4 6 8T IM E (G M T )
0
500
1000
1500
2000
2500
Coa
rse
Du
st (
ug/
std
m3 )
0
2000
4000
6000
8000
Fli
ght
Alt
itud
e (m
)
O b serv ed C oa rse P a rtic leS im u la ted C oa rse D u stF lig h t A ltitu d e
O b served an d S im u la ted D u st in C -130 F lig h t #6 (04 /11 /2001 )
0 2 4 6 8T IM E (G M T )
0
0.0002
0.0004
0.0006
0.0008
AO
E @
550
nm
(/m
)
0
2000
4000
6000
8000
Fli
ght
Alt
itud
e (m
)
O b serv ed A O ES im u la ted A O E w ith D u stS im u la ted A O E w ith o u t D u stF lig h t A ltitu d e
O b serv ed a n d S im u la ted A O E in C -13 0 F lig h t # 6 (0 4 /1 1 /2 00 1 )
Measurements Compared to the Simulations with and without Dust along C-130 Flight 6
Simulations with and without dust clearly show the dust influence on secondary aerosols. Dust increased total sulfate and nitrate concentrations, especially their coarse portions, but the high Ca loading repelled ammonia uptake. The dust storms also significantly increased aerosol extinction.
Averaged Dust Concentration (µg/m3) Averaged in the layers below 3km
GMS-5 Dust-Enhanced Image
Simulated Total Dust below 3 km with Weather Stations where Dust Were Reported
Simulated Dust Fresh Ratio in the 400m level Simulated Sulfate Coarse Ratio in the 400m level
C-130 Flight 6 & 7
Trajectory C
Simulated Dust Fresh Ratio DfreshSimulated Sulfate (contour, µg/m3) and its Coarse Ratio (color-coded)
Apr 7
Apr 9
Apr 11
Apr 13
The dust storms that occurred from April 4-14, 2001 in East Asia were named “perfect storm”by some ACE-Asia investigators. These dust storms accompanied with cold-air outbreak and were transported eastward. Dusts became aged (shown by dust fresh ratio) when passing over polluted areas and sulfate in the coarse fraction increased (i.e., coarse ratio). The interaction of dust, secondary aerosols and gaseous species through equilibria and heterogeneous processes significantly affected related species and aerosol size distributions, which was verified by aircrafts (C-130 and Twin Otter), NOAA ship (Ronald H. Brown), and ground measurements. The C-130 flight 6 encountered the strongest dust events.
C-130 Flight 8
Thank you for your attention
For further information, please contact us:
Youhua Tang [email protected] Carmichael [email protected]
C-130 flight 6 encountered the strongest dust storm during ACE-Asia campaign, which strongly affected both aerosol (left) and gaseous species via equalibria, heterogeneous and radiative processes.
P-3 #9
DC-8 #7
A
A
BB
Total Sulfate (g/std m3) in 400m level Total Nitrate (g/std m3) in 400m level
Simulated total sulfate, nitrate at 6GMT, March 7, 2001 at 400m layer. The left plot shows trajectories that arrived at the DC-8 flight 7 at 8:45GMT (A), and the P-3 flight 9 at 6:55GMT(B).
0 2 4 6 8 10 12T IM E (G M T )
0
4
8
12
Tot
al S
ulf
ate
(ug/
std
m3 )
0
4000
8000
12000
Alt
itu
de
(m)
ObservedSimulatedFlight Altitude
0 2 4 6 8 10 12T IM E (G M T )
0
4
8
12
Su
lfat
e (u
g/st
d m
3 )
1st bin2nd bin3nd bin4th bin
0 2 4 6 8 10 12T IM E (G M T )
0
1
2
3
Tot
al N
itra
te (
ug/
std
m3 )
0
100
200
300
400
CO
(p
pb
v)
Observed NitrateSimulated NitrateObserved COSimulated CO
0 2 4 6 8 10 12T IM E (G M T )
0
1
2
3
Nit
rate
(u
g/st
d m
3 )
1st bin2nd bin3nd bin4th bin
0 2 4 6 8 10 12T IM E (G M T )
0
1
2
3
4
Tot
al A
mm
oniu
m (
ug/
std
m3 )
0
1
2
3
Eth
ane
(pp
bv)
Observed AmmoniumSimulated AmmoniumObserved EthaneSimulated Ethane
0 2 4 6 8 10 12T IM E (G M T )
0
1
2
3
4
Am
mon
ium
(u
g/st
d m
3 )
1st bin2nd bin3nd bin4th bin
6 1 6 1 . 5 6 2 6 2 . 5 6 3 6 3 . 5 6 4 6 4 . 5 6 5 6 5 . 5 6 6 6 6 . 5Ju lia n D a y (G M T )
0
0.2
0.4
0.6
0.8
1
Ion
Fin
e R
atio
0
1000
2000
3000
4000
AG
L (
m)
SulfateNitrateAltitude (AGL)Longitude
9 0
1 0 0
1 1 0
1 2 0
1 3 0
1 4 0
Lon
gitu
de
6 1 6 2 6 3 6 4 6 5 6 6 6 7Ju lian D ay (G M T )
0
2
4
6
8
Sulf
ate
(ug/
std
m3 )
1st bin2nd bin3nd bin4th bin
6 1 6 2 6 3 6 4 6 5 6 6 6 7J u lia n D a y (G M T )
0
1
2
3
4
5
Nit
rate
(u
g/st
d m
3 )
1st bin2nd bin3nd bin4th bin
6 1 6 1 . 5 6 2 6 2 . 5 6 3 6 3 . 5 6 4 6 4 . 5 6 5 6 5 . 5 6 6 6 6 . 5J u lian D ay (G M T )
0
0.4
0.8
1.2
1.6
2
NO
x, H
NO
3, S
O2,
Tot
al N
itra
te (
pp
bv)
0
1
2
3
4
5
NO
y, N
H3 (
pp
bv)
NOxHNO3SO2Total Aerosol NitrateNOyNH3Observed HNO3
Simulated ions and their size distributions compared to filter measurements along on the DC-8 flight 7 (left), and simulated variations (down) along the trajectory A. Along this trajectory, SO2 condensation and sulfate uptake on fine mode repel nitrate to coarse mode. Aerosol consideration in the 3-D also corrected the overestimation of HNO3 by adding its aerosol uptake.
Sulfate55.31
Nitrate25.86
Am m onium18.83
Sulfate27.77
Nitrate54.08
Amm onium18.15
Sulfate63.68
Nitrate17.02
Am m onium19.3
Sulfate51.89
Nitrate25.96
Am monium22.15
Sulfate58.62
Nitrate13.7
Ammonium27.68
Fine Ions Coarse Ions
When The trajectory B passed over
Shanghai
When The trajectory B arrived at the P-3 flight 9
Observed fine mass percentages on P-3 flight 9
The P-3 flight 9 encountered fresh city plumes and the simulation showed the composition evolution in fine and coarse modes along the trajectory B. As the air mass moved away from the city the sulfate portion increased in both the fine and coarse modes, as the result of SO2 condensation
Ship Ron-Brown Cruise
Trajectory Date Difference from the Arrival Point
9 4 9 6 9 8 1 0 0 1 0 2 1 0 4 1 0 6J u lia n D a y (G M T )
0
10
20
30
40
Obs
erve
d F
ine
Ions
(ug
/std
m3 ) Sodium
SulfateNitrateAmmoniumCa
0
0.1
0.2
0.3
0.4
0.5
Obs
erve
d F
ine
Cal
cium
(ug
/std
m3 )
9 4 9 6 9 8 1 0 0 1 0 2 1 0 4 1 0 6J u lia n D a y (G M T )
0
10
20
30
40
Sim
ulat
ed F
ine
Ions
(ug
/std
m3 ) Sodium
SulfateNitrateAmmoniumDust
0
200
400
600
Sim
ulat
ed F
ine
Dus
t (u
g/st
d m
3 )
9 4 9 6 9 8 1 0 0 1 0 2 1 0 4 1 0 6Ju lian D a y (G M T )
0
4
8
12
16
Obs
erve
d C
oars
e Io
ns (
ug/s
td m
3 )
SodiumSulfateNitrateAmmoniumCa
0
0.1
0.2
0.3
0.4
0.5
Obs
erve
d C
oars
e C
alci
um (
ug/s
td m
3 )
9 4 9 6 9 8 1 0 0 1 0 2 1 0 4 1 0 6J u lia n D a y (G M T )
0
2
4
6
8
10
Sim
ulat
ed C
oars
e Io
ns (
ug/s
td m
3 )
SodiumSulfateNitrateAmmoniumDust
0
400
800
1200
Sim
ulat
ed C
oars
e D
ust
(ug/
std
m3 )
9 4 9 6 9 8 1 0 0 1 0 2 1 0 4 1 0 6J u lian D a y
0
1 0 0
2 0 0
3 0 0
4 0 0
AT
OF
MS
Are
a R
atio
sfo
r C
oars
e S
ea S
alt
Par
ticl
es
ATOFMS Coarse Area Ratio 81/108ATOFMS Coarse Area Ratio 81/165Simulated Processed Coarse Cl
0
1
2
3
Sim
ulat
ed P
roce
ssed
Cl (
ug/s
td m
3 ) on
C
oars
e Se
a sa
lt
9 4 9 6 9 8 1 0 0 1 0 2 1 0 4 1 0 6J u lia n D a y (G M T )
0
1
2
3
4
5
Sim
ulat
ed C
oars
e N
O3- (u
g/st
d m
3 ) w
itho
ut
Du
stan
d th
e D
iffe
ren
ce b
etw
een
wit
h an
d w
ith
out
Dus
t
Simulated Coarse NO3 without DustSimulated Coarse NO3 DifferenceATOFMS Sea Salt PercentageATOFMS Dust Percentage
0
20
40
60
80
100
AT
OF
MS
Mea
sure
d P
erce
nta
ges
of C
oars
e N
itra
te C
onta
ined
in S
ea S
alt
and
Du
st
NOAA research vessel Ron Brown performed extensive measurements during the ACE-Asia experiment. The following plots show the simulations compared to observations along the ship track (marked in Julian day). During the dust
events (Julian day 101-103), both observation and simulation show ion enhancement in the coarse mode. The single particle measurements with ATOFMS of sulfate (m/z 165 corresponding to Na3SO4
+), and nitrate (m/z 108
corresponding to Na2NO3+) in the
super-micron sea salt particles indicating chemical processed sea salt, which is consistent with the simulation.
