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![Page 1: Formaldehyde from Space: Unexplored regions, New Data, New Challenges. Paul Palmer University of Edinburgh.](https://reader033.fdocuments.us/reader033/viewer/2022051115/56649ed35503460f94be3d4f/html5/thumbnails/1.jpg)
Formaldehyde from Space: Unexplored
regions, New Data, New Challenges.
Paul Palmer University of Edinburgh
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A modest beginning….
Thomas et al, GRL, 1998
NO2HCHO
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Vertical column retrievals
8 x 1016 molec cm-2T
ransm
issi
on
Chance et al, GRL, 2000
337-356 nm (O3, NO2, BrO, O2-O2)
1) Direct fit of observed radiances: slant columns
AMF = AMFG w() S() d1
0
Radiative transfer
Normalised HCHO profile
Palmer et al, JGR, 2001
2) Air-mass factor calculation: vertical columns
Estimated Error Budget
Slant column fitting: 4x1016 molec cm-2
AMF:
1) UV albedo (8%)
2) Model error (10%)
3) Clouds (20%)
4) Aerosols (20%)
Subtotal 30%
For a vertical column of 2x1016 molec cm-2 and AMF of 0.7
TOTAL = 9x1015 molec cm-2
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biogenic, pryogenic, anthropogenic
pryogenicanthropogenic
biogenicanthropogenic
pryogenicpyrogenicanthropogenic
biogenicanthropogenic
Th
om
as
Kuro
su,
Harv
ard
-Sm
ithso
nia
n
HCHO August 2006Ozone Monitoring Experiment
Global distribution of HCHO, OMI August 2006
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Continent 2
Direct intercontinental transport of pollutants O
3
NOx, RH, CO
Continent 1
O3
Ocean physics, chemistry, biology
Pyro-convection
HO2
O3
NO
OH
NO2
hv
Visibility
A simplistic view of tropospheric chemistry
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Environmental factors:• temperature• solar irradiance• leaf area index• leaf age
July2003
MEGAN Isoprene Emission Inventory
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North AmericaPalmer et al, JGR, [2001, 2003,
2006] Abbot et al, GRL, 2003 Chance et al, GRL, 2000
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Relating HCHO Columns to VOC Emissions
VOC HCHOhours
OH
hours
h, OH
Local linear relationship between HCHO and E
kHCHO
EVOC = (kVOCYVOCHCHO)HCHO
___________
VOC source
Distance downwind
HCHO Isoprene
-pinenepropane
100 km
EVOC: HCHO from GEOS-CHEM CTM and MEGAN isoprene emission model
Palmer et al, JGR, 2003.
Net
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May 2001
Jun 2001
Jul 2001
Aug 2001
Sep 2001[1012 C cm-2 s-1]
Isoprene Monoterpenes MBO
Isoprene largely from broadleaf (e.g., poplar, sweetgum, aspen and oak)
Monoterpenes primarily from coniferous tree (pine, cedar, redwood)
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Master Chemical Mechanism yield calculations
Cu
mu
lati
ve H
CH
O y
ield
[p
er
C]
0 2 4 6 8 10 12 14 16 18 20 220.00
0.05
0.10
0.15
0.20
0.25
0.30
0.35
0.40
HC
HO
YIE
LD
PE
R C
RE
AC
TE
D
DAYS
NOX= 1 PPB NOX= 100 PPT
pinene
( pinene similar)DAYS
0.4
0 20 40 60 80 100 120 1400.00
0.05
0.10
0.15
0.20
0.25
0.30
0.35
0.40
0.45
0.50
0.55C
umm
ula
tive
HC
HO
Yie
ld fr
om
iso
pren
e o
xid
atio
n (p
er C
)
TIME (HOURS)
NOX = 0.1 PPB
NOX =1 PPB
Figure 18. Formation of HCHO from isoprene. Vertical lines denote midnight of each day
Isoprene
HOURS
0.5NOx = 1 ppb
NOx = 0.1 ppb
Parameterization (1ST-order decay) of HCHO production from monoterpenes in global 3-D CTM
Higher CH3COCH3 yield from monoterpene oxidation delayed (and smeared) HCHO production
Palmer et al, JGR, 2006.
C5H8+OH(i) RO2+NOHCHO, MVK, MACR
(ii) RO2+HO2ROOH
ROOH recycle RO and RO2
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Monthly mean AVHRR LAI
MEGAN (isoprene)Canopy model; Leaf age;
LAI; Temperature; Fixed Base factors
GEIAMonoterpenes; MBO;Acetone; Methanol
MODEL BIOSPHERE
GEOS-CHEM Modeling Overview
GEOS-CHEM global 3Dchemistry transport model
PAR, T
Emissions
MCM: parameterized HCHO source from monoterpenes and MBO
model without isoprene
Isoprene emission [1013 atomC cm-2 s-1]
Mod
el H
CH
O
colu
mn
[1
01
6
mole
c cm
-2]
SE USA
ΩHCHO= S EISOP+B
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Seasonal Variation of Y2001 Isoprene Emissions
•Good accord for seasonal variation, regional distribution of emissions (differences in hot spot locations – implications for O3 prod/loss).
•Other biogenic VOCs play a small role in GOME interpretation
May
Jun
Aug
Sep
Jul
0 3.5
7
1012 atom C cm-2s-
1
GOME MEGAN MEGAN GOME
Palmer et al, JGR, 2006.
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Isop
ren
e fl
ux [
10
12 C
cm
-2 s
-1]
Julian Day, 2001
MEGANObsGOME
Sparse ground-truthing of GOME HCHO columns and derived isoprene flux estimates
Seasonal Variation: Comparison with eddy correlation isoprene flux measurements (B. Lamb) is encouraging
Atlanta, GA
May Jun July Aug Sep
PAMS Isoprene, 10-12LT [ppbC]
GO
ME H
CH
O [
10
16 m
ole
c c
m-2]
1996 1997 1998 1999 2000 2001Interannual Variation:
Correlate with EPA isoprene surface concentration data. Outliers due to local emissions.
Atlanta, GA
PROPHET Forest Site, MI
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GOME Isoprene Emissions: 1996-2001May Jun Jul Aug Sep
1996
1997
1998
1999
2000
2001
[1012 molecules cm-2s-1]0 5 10
Palm
er
et
al, JG
R,
2006.
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Surface temperature explains 80% of GOME-observed variation in HCHO
NCEP Surface Temperature [K]
GO
ME Iso
pre
ne E
mis
sions
[1
012 a
tom
s C
cm
-2s-
1] G98 fitted to
GOME data
G98 Modeled curves
Time to revise model parameterizations of isoprene emissions?
Palm
er
et
al, JG
R,
2006.
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EuropeCurci et al, in prep, 2007
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Correlation of high ozone with temperature is driven by:1) Stagnation, 2) Biogenic hydrocarbon emissions, 3) Chemistry
Ozone exceedances of 90 ppbv,summer 2003 (#days)
0-1; 1-5; 5-10; >10 40
45
50
55
60
65
70
- 60 - 50 - 40 - 30 - 20 - 10 0 10
“Normal” airmass flow
44
46
48
50
52
54
56
- 20 - 15 - 10 - 5 0 5 10
Stagnant airmass flow
0
200
400
600
800
1000
1200
1400
27-Jul
29-Jul
31-Jul
2-Aug
4-Aug
6-Aug
8-Aug
10-Aug
12-Aug
14-Aug
16-Aug
18-Aug
20-Aug
22-Aug
24-Aug
26-Aug
28-Aug
30-Aug
0
5
10
15
20
25
30
35
40
Tem
pera
ture
(C
)
Isop
ren
e (
pp
t)
Isoprene c/o Ally Lewis
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Only continent where ANTHRO > BIO emissions
[Simpson et al., JGR 1999]
A = hot; B = warm temperate; C = cool temperate
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What Controls HCHO Columns Over Europe?
GEOS-CHEM HCHO Column in
Summer
BIOGENIC CONTROL
NO ISOP/NO ANTHRO
Biogenic control of HCHO column:
• Eastern Europe
• Northern Europe
• Iberian Peninsula
• Turkey(GEIA Emissions)
0.4
1.2
1
ANTHROPOGENIC CONTROL
v7-01-02
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EMEP DataGEIA
MEGAN
EMEP stations, Aug 2000
Comparison between GEOS-CHEM and EMEP data
Isop
ren
e
(pp
b)
HC
HO
(p
pb
)
Day, Aug 2000
Donon
•Some (limited) evidence that HCHO signal is biogenic
•MEGAN consistently too low
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Aug 1996 1996-2000 Aug Mean
GOME HCHO Columns Over Europe
2.52.01.51.00.5[1016 molec cm-
2]
Data on a regular 0.5 x 0.5 degree grid
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Isop
ren
e
em
issi
on
GEIA = Guenther et al, JGR (1995)
Spatial separation method used for North America was not clean over Europe
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Work in progress: inverting as a function of NOx rather than
geographyGEOS-CHEM NO2 Columns, Aug 2000 [1015 molec cm-
2]GEOS-CHEM: Isoprene vs
HCHO columns over Europe
L, M and H NOx a bit arbitrary
Resulting inversion does not distinguish properly biogenic vs anthropogenic HCHO
ΩHCHO= S EISOP+B
EISOP [1012 molec cm-2s-1]
Ω H
CH
O [
10
16 m
ole
c cm
-2]
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GOME isoprene flux have an uncertainty < 200%, comparable, if not less, that bottom-up inventories
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Tropical Ecosystems Barkley and Palmer, WIP
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Tropical ecosystems represent 75% of biogenic NMVOC emissions
What drives observed variability of tropical BVOC emissions?
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Sla
nt
Colu
mn H
CH
O [
10
16 m
ole
c cm
-2]
Sep 1997
Nov 1997
19971998199920002001
X = Active Fire (ATSR)
Mon
thly
ATS
R F
irecou
nts
Day of Year
Significant pyrogenic HCHO source over tropicsGood: Additional trace gas measurement of biomass burning; effect can be identified largely by firecounts (see below)
Bad: Observed HCHO a mixture of biogenic and pyrogenic – difficult to separate without better temporal and spatial resolution
GOME
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HCHO and Isoprene over the Amazon
In situ isoprene 2002
Tro
stdorf e
t al,
200
4
19971998199920002001
GOME
ATSR Firecounts used to remove HCHO from fires
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em
issio
n r
ate
(C
)(µ
g g
-1 h
-1)
PA
R(µ
mol m
-2 s
-1)
assim
ilati
on
(C
)(m
g g
-1 h
-1)
0
1
2
3
4
5
6
limonene myrcene b-pinene a-pinene sabinene
500
1000
1500
00:0006:00
12:0018:00
00:0006:00
12:0018:00
00:00
0
2
4
local time [hh:mm]
10
20
30
40
tem
pera
ture
[°C
]
0
2
4 G
93
for
isop
.[s
um
of
mon
ote
rpen
es]
tran
sp
irati
on
(mm
ol m
-2 s
-1)
monoterpene emission of Apeiba tibourbou
0
0.1
0.2
0.3
0.4
0.5
0.6
0.7
0.8
0.9
00:00 02:24 04:48 07:12 09:36 12:00 14:24 16:48 19:12 21:36 00:00
Time bin midpoint
Co
nce
ntr
atio
n (
pp
b)
0
1
2
3
4
5
6
00:00 02:24 04:48 07:12 09:36 12:00 14:24 16:48 19:12 21:36 00:00
Time bin midpoint
Co
nce
ntr
atio
n (
pp
b)
0
0.5
1
1.5
2
2.5
3
3.5
00:00 02:24 04:48 07:12 09:36 12:00 14:24 16:48 19:12 21:36 00:00
Time bin midpoint
Co
nce
ntr
atio
n (
pp
b)
Isoprene
Limonene
Beta-pinene
[pp
b]
Time of DayC/o J. Kesselmeier
C/o J. Saxton A. Lewis
Amazon
AfricaCan isoprene explain the observed magnitude and variance of HCHO columns over the tropics?
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The future?Newer orbits….better spatial and temporal resolution…
Bu
rrow
s et
al,
20
04
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Biomass Burning: emissions and injection heights
OMI HCHO c/o T. Kurosu
ATSR Firecounts
October 2006ACE HCHO c/o P. Bernath
•Pyro-convective transport is difficult to model accurately.
•Two (or more) pieces of independent information allows a simultaneous inversion of surface emission and injection height.
Schoeberl et al, 2006