Atmospheric Chemistry Experiment (ACE): Recent Results Peter Bernath (and ACE team) Department of...
-
Upload
alina-nichol -
Category
Documents
-
view
217 -
download
0
Transcript of Atmospheric Chemistry Experiment (ACE): Recent Results Peter Bernath (and ACE team) Department of...
![Page 1: Atmospheric Chemistry Experiment (ACE): Recent Results Peter Bernath (and ACE team) Department of Chemistry, University of York Heslington, York, UK and.](https://reader036.fdocuments.us/reader036/viewer/2022062518/56649c7c5503460f949311ea/html5/thumbnails/1.jpg)
Atmospheric Chemistry Experiment (ACE):
Recent ResultsPeter Bernath (and ACE team)
Department of Chemistry, University of York
Heslington, York, UK
and
Department of Chemistry, University of Waterloo, Waterloo, ON, Canada
![Page 2: Atmospheric Chemistry Experiment (ACE): Recent Results Peter Bernath (and ACE team) Department of Chemistry, University of York Heslington, York, UK and.](https://reader036.fdocuments.us/reader036/viewer/2022062518/56649c7c5503460f949311ea/html5/thumbnails/2.jpg)
ACE Satellite
See http://www.ace.uwaterloo.ca
![Page 3: Atmospheric Chemistry Experiment (ACE): Recent Results Peter Bernath (and ACE team) Department of Chemistry, University of York Heslington, York, UK and.](https://reader036.fdocuments.us/reader036/viewer/2022062518/56649c7c5503460f949311ea/html5/thumbnails/3.jpg)
Solar Occultation
Advantages: Radiance of sun gives higher S/N than emissionLimb view gives longer path length ~500 km (lower detection limits) than nadir“Self-calibrating” so excellent long-term accuracy and precisionDisadvantages: Modest global coverageSamples only free troposphere
![Page 4: Atmospheric Chemistry Experiment (ACE): Recent Results Peter Bernath (and ACE team) Department of Chemistry, University of York Heslington, York, UK and.](https://reader036.fdocuments.us/reader036/viewer/2022062518/56649c7c5503460f949311ea/html5/thumbnails/4.jpg)
Timeline Jan. 1998 Proposal to CSA Feb. 2001 FTS and Imager CDR Mar. 2001 MAESTRO CDR Jun. 2001 Bus CDR Sept. 2002 S/C integration & test Mar. 2003 Instrument test (Toronto) May 2003 Final integration (DFL) Aug. 2003 Launch Sept. 2003 Commissioning Feb. 2004 Routine operations Mar. 2004 Arctic campaign Feb. 2005 Arctic campaign Feb. 2006 Arctic campaign Feb. 2007 Arctic campaign Feb. 2008 Arctic campaign
First ACE data Feb. 2004, mission currently approved to March 2010. Mission had a 2-year lifetime – fifth anniversary Aug. 2008.
![Page 5: Atmospheric Chemistry Experiment (ACE): Recent Results Peter Bernath (and ACE team) Department of Chemistry, University of York Heslington, York, UK and.](https://reader036.fdocuments.us/reader036/viewer/2022062518/56649c7c5503460f949311ea/html5/thumbnails/5.jpg)
Instruments
Infrared Fourier Transform Spectrometer operating between 2 and 13 microns with a resolution of 0.02 cm-1
2-channel visible/near infrared Imagers, operating at 0.525 and 1.02 microns (cf., SAGE II)
Suntracker keeps the instruments pointed at the sun’s radiometric center.
UV / Visible spectrometer (MAESTRO) 0.4 to 1.03 microns, resolution ~1-2 nm
StartrackerBernath et al. GRL, 32, L15S01 (2005)
![Page 6: Atmospheric Chemistry Experiment (ACE): Recent Results Peter Bernath (and ACE team) Department of Chemistry, University of York Heslington, York, UK and.](https://reader036.fdocuments.us/reader036/viewer/2022062518/56649c7c5503460f949311ea/html5/thumbnails/6.jpg)
SCISAT-1 Spacecraft (Bristol)
![Page 7: Atmospheric Chemistry Experiment (ACE): Recent Results Peter Bernath (and ACE team) Department of Chemistry, University of York Heslington, York, UK and.](https://reader036.fdocuments.us/reader036/viewer/2022062518/56649c7c5503460f949311ea/html5/thumbnails/7.jpg)
Optical Layout (ABB-Bomem)
Secondaymirror (6)
Field stop (5)
IR Filter(7)
Suntrackermirror (1)
Aperturestop (4)
PV MCTDetector
(18)
Glare stop(16)
Coolerwindow (17)
Outputcondenser
(14)
INTcorner-cubemirror (10)
End mirror(13)
INTcorner-cubemirror (11)
(12)
(9)
(12): Reflective coating(9): B/S coating
Beamsplit ter/compensatorassembly (8)
Primary mirror (3)
Fold mirror(22)
Lenses(23)
0.525 mimager (28)
1.02 mimager (26)
Dichroic(24)
Solarinput
Compensator
VIS/NIR-Quad CellDichroic
Quad Cell(21)
Lenses(20)
LaserMetrologyDetection
1.02 mfilter (25)
0.525 mfilter (27)
Beam splitter
Foldmirror(15) Laser Metrology Insertion
MAESTROInterface (2)
PV InSbDetector
Lens
Lens Glare stop
Dichroic
1.55 mfilter (19)
![Page 8: Atmospheric Chemistry Experiment (ACE): Recent Results Peter Bernath (and ACE team) Department of Chemistry, University of York Heslington, York, UK and.](https://reader036.fdocuments.us/reader036/viewer/2022062518/56649c7c5503460f949311ea/html5/thumbnails/8.jpg)
MAESTRO
Dual concave grating spectrograph, 1-2 nm resolution
MAESTRO PI:T. McElroy, MSC
![Page 9: Atmospheric Chemistry Experiment (ACE): Recent Results Peter Bernath (and ACE team) Department of Chemistry, University of York Heslington, York, UK and.](https://reader036.fdocuments.us/reader036/viewer/2022062518/56649c7c5503460f949311ea/html5/thumbnails/9.jpg)
Global Occultation Distribution
![Page 10: Atmospheric Chemistry Experiment (ACE): Recent Results Peter Bernath (and ACE team) Department of Chemistry, University of York Heslington, York, UK and.](https://reader036.fdocuments.us/reader036/viewer/2022062518/56649c7c5503460f949311ea/html5/thumbnails/10.jpg)
FTS – Decontamination Results
After 6 months operationAfter decontamination
Ryan Hughes
![Page 11: Atmospheric Chemistry Experiment (ACE): Recent Results Peter Bernath (and ACE team) Department of Chemistry, University of York Heslington, York, UK and.](https://reader036.fdocuments.us/reader036/viewer/2022062518/56649c7c5503460f949311ea/html5/thumbnails/11.jpg)
Occultation sequence
![Page 12: Atmospheric Chemistry Experiment (ACE): Recent Results Peter Bernath (and ACE team) Department of Chemistry, University of York Heslington, York, UK and.](https://reader036.fdocuments.us/reader036/viewer/2022062518/56649c7c5503460f949311ea/html5/thumbnails/12.jpg)
ACE-FTS Species Measured
Baseline species (version 2.2):
H2O, O3, N2O, CO, CH4, NO, NO2, HNO3, HF, HCl, N2O5, ClONO2, CCl2F2, CCl3F, as well as pressure and temperature from CO2 lines
Other routine species:
COF2, CHF2Cl, CF4, CH3Cl, C2H6, SF6, OCS, HCN
Research species:
CCl4, HOCl, H2O2, HO2NO2, CCl2FCClF2, CH3CClF2, ClO, C2H2, C2H6, COFCl, COCl2, CH3OH, HCOOH, H2CO, N2 and additional isotopologues
![Page 13: Atmospheric Chemistry Experiment (ACE): Recent Results Peter Bernath (and ACE team) Department of Chemistry, University of York Heslington, York, UK and.](https://reader036.fdocuments.us/reader036/viewer/2022062518/56649c7c5503460f949311ea/html5/thumbnails/13.jpg)
CO2 line near 61 km
Typical ACE-FTS fitting results
Note: results are plotted on the raw measurement grid
Boone et al. Appl. Opt. 44, 7218 (2005)
![Page 14: Atmospheric Chemistry Experiment (ACE): Recent Results Peter Bernath (and ACE team) Department of Chemistry, University of York Heslington, York, UK and.](https://reader036.fdocuments.us/reader036/viewer/2022062518/56649c7c5503460f949311ea/html5/thumbnails/14.jpg)
Temperature Retrievals-CO2
90 km
15 km
Schwartz et al. JGR, 113, D15S11 (2008)
![Page 15: Atmospheric Chemistry Experiment (ACE): Recent Results Peter Bernath (and ACE team) Department of Chemistry, University of York Heslington, York, UK and.](https://reader036.fdocuments.us/reader036/viewer/2022062518/56649c7c5503460f949311ea/html5/thumbnails/15.jpg)
Stratospheric Chlorine Budget
Mean ClTOT (ppbv) slope (ppbv/km) Northern high latitudes 3.74 ± 0.12 0.010 ± 0.001 Northern midlatitudes 3.65 ± 0.09 0.007 ± 0.001 Tropics 3.62 ± 0.11 0.009 ± 0.001 Southern midlatitudes 3.65 ± 0.09 0.007 ± 0.001 Southern high latitudes 3.71 ± 0.16 0.014 ± 0.001
Northern Midlatitudes
Southern Midlatitudes
Current HALOE value 3.3 ppb
Nassar et al.
WMO Ozone Report 2006
JGR, 111, D22312 (2006)
CFC-11, CFC-12 , HCFC-22, CCl4, CH3Cl, CF4, CFC-113, HCFC-142b, HFC134a, F2CO, ClFCO,
Cl2CO
![Page 16: Atmospheric Chemistry Experiment (ACE): Recent Results Peter Bernath (and ACE team) Department of Chemistry, University of York Heslington, York, UK and.](https://reader036.fdocuments.us/reader036/viewer/2022062518/56649c7c5503460f949311ea/html5/thumbnails/16.jpg)
Asian Monsoon Anticyclone
Park et al., ACP, 8, 757 (2008)
![Page 17: Atmospheric Chemistry Experiment (ACE): Recent Results Peter Bernath (and ACE team) Department of Chemistry, University of York Heslington, York, UK and.](https://reader036.fdocuments.us/reader036/viewer/2022062518/56649c7c5503460f949311ea/html5/thumbnails/17.jpg)
Global Distribution of Phosgene, Cl2CO
Latitude (in Degrees)
Alt
itu
de
(in
Km
)
2004-2005-2006 COCl2 Volume Mixing Ratio (in pptv)
-80 -60 -40 -20 0 20 40 60 800
5
10
15
20
25
30
35
40
0
10
20
30
40
50
60
Fu et al. GRL, 34, L17815 (2007) (Toon et al.’s calculated linelist for ν5 near 850 cm-1)
-10 0 10 20 30 400
5
10
15
20
25
30
Volume Mixing Ratio (in pptv)
Alt
itu
de
(in
km
)
85oS-60oS
60oS-30oS
30oS-30oN
30oN-60oN
60oN-90oNWilson et al. 1988Kindler et al. 1995
50oN-80oN
0o-90oN
0o-85oS
Cl ClC
Oװ
![Page 18: Atmospheric Chemistry Experiment (ACE): Recent Results Peter Bernath (and ACE team) Department of Chemistry, University of York Heslington, York, UK and.](https://reader036.fdocuments.us/reader036/viewer/2022062518/56649c7c5503460f949311ea/html5/thumbnails/18.jpg)
Distribution of COClF
•Carbonyl chlorofluoride is a product of chlorofluorocarbon (CFC-11 mainly) decomposition
•Previously studied by aircraft (5 - 12 km)
•First global picture obtained from ACE-FTS
•Spectroscopy based on Brown’s ATMOS linelist created from Kitt Peak spectra, with rough intensities.
D. Fu et al., to be submitted
![Page 19: Atmospheric Chemistry Experiment (ACE): Recent Results Peter Bernath (and ACE team) Department of Chemistry, University of York Heslington, York, UK and.](https://reader036.fdocuments.us/reader036/viewer/2022062518/56649c7c5503460f949311ea/html5/thumbnails/19.jpg)
Effect of Lightning (HNO3)
Lightning produces NO, which is oxidized to HNO3.
Need to have 6 Tg N/yr from lightning to match ACE observations of tropospheric HNO3 (Martin et al. JGR, 112, D09309 (2007))
![Page 20: Atmospheric Chemistry Experiment (ACE): Recent Results Peter Bernath (and ACE team) Department of Chemistry, University of York Heslington, York, UK and.](https://reader036.fdocuments.us/reader036/viewer/2022062518/56649c7c5503460f949311ea/html5/thumbnails/20.jpg)
ACE solar spectrum (F. Hase): 224782 spectra added, improvement over ATMOS, no telluric lines, but 0.02 cm-1 vs 0.01 cm-1 resolution (resolution largely determined by width of solar lines) and 750-4400 cm-1 vs 600-4800 cm-1.
CO, Δv=1
OH
CO Δv=2
CH, NH, OHACE Solar Spectrum
![Page 21: Atmospheric Chemistry Experiment (ACE): Recent Results Peter Bernath (and ACE team) Department of Chemistry, University of York Heslington, York, UK and.](https://reader036.fdocuments.us/reader036/viewer/2022062518/56649c7c5503460f949311ea/html5/thumbnails/21.jpg)
ATMOS Spacelab-3, 1985
ATMOS ATLAS-3, 1994
ACE, 2008
New atomic and molecular assignments (ACE linelist) by L. Wallace (NOAO); improved spectroscopic data for CH, NH and OH.
For OH, Reg Colin (ULB) finds v=4 can be improved.
![Page 22: Atmospheric Chemistry Experiment (ACE): Recent Results Peter Bernath (and ACE team) Department of Chemistry, University of York Heslington, York, UK and.](https://reader036.fdocuments.us/reader036/viewer/2022062518/56649c7c5503460f949311ea/html5/thumbnails/22.jpg)
Air Quality and Biomass Burning
![Page 23: Atmospheric Chemistry Experiment (ACE): Recent Results Peter Bernath (and ACE team) Department of Chemistry, University of York Heslington, York, UK and.](https://reader036.fdocuments.us/reader036/viewer/2022062518/56649c7c5503460f949311ea/html5/thumbnails/23.jpg)
Biomass Burning in Brazil
MODIS Fire Counts26 Sept. 200427 Sept. 200428 Sept. 2004
5
6
7
8
9
10
11
12
13
14
15
16
17
0.0 0.5 1.0 1.5 2.0 2.5 3.0 3.5
ss6139 - v2.1 CO*0.01 O
3*0.01
HCN C
2H
6
vmr (ppbv)
altit
ude
(km
)
![Page 24: Atmospheric Chemistry Experiment (ACE): Recent Results Peter Bernath (and ACE team) Department of Chemistry, University of York Heslington, York, UK and.](https://reader036.fdocuments.us/reader036/viewer/2022062518/56649c7c5503460f949311ea/html5/thumbnails/24.jpg)
CH3OH contribution to the spectrum
Dufour et al. ACP, 6, 3463 (2006); data from Xu et al. 2004
![Page 25: Atmospheric Chemistry Experiment (ACE): Recent Results Peter Bernath (and ACE team) Department of Chemistry, University of York Heslington, York, UK and.](https://reader036.fdocuments.us/reader036/viewer/2022062518/56649c7c5503460f949311ea/html5/thumbnails/25.jpg)
Global Methanol
Dufour et al. ACP, 7, 6119, 2007
LDMz-INCA model
(D. Hauglustaine)
ACE is an upper tropospheric “air quality” mission measuring global CH4, CH3OH, HCN, C2H2, C2H6, H2O2, HCOOH, H2CO, plus likely PAN and acetone.
![Page 26: Atmospheric Chemistry Experiment (ACE): Recent Results Peter Bernath (and ACE team) Department of Chemistry, University of York Heslington, York, UK and.](https://reader036.fdocuments.us/reader036/viewer/2022062518/56649c7c5503460f949311ea/html5/thumbnails/26.jpg)
Young Biomass Burning Plume
Coheur et al. ACP, 7, 547, 2007
![Page 27: Atmospheric Chemistry Experiment (ACE): Recent Results Peter Bernath (and ACE team) Department of Chemistry, University of York Heslington, York, UK and.](https://reader036.fdocuments.us/reader036/viewer/2022062518/56649c7c5503460f949311ea/html5/thumbnails/27.jpg)
PAN, Peroxyacetyl nitrate, etc.
Coheur et al. (Brussels), PAN from a biomass plume near East Africa
![Page 28: Atmospheric Chemistry Experiment (ACE): Recent Results Peter Bernath (and ACE team) Department of Chemistry, University of York Heslington, York, UK and.](https://reader036.fdocuments.us/reader036/viewer/2022062518/56649c7c5503460f949311ea/html5/thumbnails/28.jpg)
HCHO spectroscopy: new linelist
Use of HCHO line intensities calculated by A. Perrin
2831,6 2831,7 2831,8 2831,9 2832,0 2832,1 2832,2
0,0
0,2
0,4
0,6
0,8
1,0
Perrin, Jacquemart, Kwabia-Tchana & Lacome
1 22
1 22-21
1 21
1 21
3 18-20
3 175 8
0 8-8
1 7
Obs-Calc New Calc
Calc with HITRAN*1.28
Calc New calc
Obs
Tra
nsm
itta
nce
Wavenumber in cm-1
Missing lines
Error with multiplets
Dufour et al.
![Page 29: Atmospheric Chemistry Experiment (ACE): Recent Results Peter Bernath (and ACE team) Department of Chemistry, University of York Heslington, York, UK and.](https://reader036.fdocuments.us/reader036/viewer/2022062518/56649c7c5503460f949311ea/html5/thumbnails/29.jpg)
HCHO contribution to the spectrum
0,0
0,2
0,4
0,6
0,8
-0,05
0,00
0,05
2778,0 2778,2 2778,4 2778,6 2778,8
-0,05
0,00
0,05
Observed spectrum
without HCHO HCHO contribution
HCHO contributionwith HCHO
0,0
0,2
0,4
0,6
0,8
-0,10-0,050,000,050,10
2780,8 2780,9 2781,0 2781,1 2781,2 2781,3 2781,4 2781,5 2781,6-0,10-0,050,000,050,10
Observed spectrum
HCHO contributionwithout HCHO
HCHO contributionwith HCHO
6 spectral windows selected in 6 spectral windows selected in the range 2735 - 2830 cmthe range 2735 - 2830 cm-1-1 ::
2739.85 ; 2765.65 ; 2778.4 ; 2739.85 ; 2765.65 ; 2778.4 ; 2781.2 ; 2812.25 ; 2826.672781.2 ; 2812.25 ; 2826.67
0,2
0,4
0,6
0,8
-0,05
0,00
0,05
2826,2 2826,4 2826,6 2826,8 2827,0-0,05
0,00
0,05
Observed spectrum
HCHO contributionwithout HCHO
HCHO contributionwith HCHO
![Page 30: Atmospheric Chemistry Experiment (ACE): Recent Results Peter Bernath (and ACE team) Department of Chemistry, University of York Heslington, York, UK and.](https://reader036.fdocuments.us/reader036/viewer/2022062518/56649c7c5503460f949311ea/html5/thumbnails/30.jpg)
3 years of HCHO measurements with ACE-FTS
![Page 31: Atmospheric Chemistry Experiment (ACE): Recent Results Peter Bernath (and ACE team) Department of Chemistry, University of York Heslington, York, UK and.](https://reader036.fdocuments.us/reader036/viewer/2022062518/56649c7c5503460f949311ea/html5/thumbnails/31.jpg)
Preliminary comparisons with CTMs
MAM04 JJA04 SON04 DJF05 MAM05 JJA05 SON05 DJF06 MAM06 JJA06 SON06
10
20
30
40
50
60
70
80
90
100
110
120
MAM04 JJA04 SON04 DJF05 MAM05 JJA05 SON05 DJF06 MAM06 JJA06 SON06
102030405060708090
100110120130140150
MAM04 JJA04 SON04 DJF05 MAM05 JJA05 SON05 DJF06 MAM06 JJA06 SON06
30
40
50
60
70
80
90
100
HC
HO
vm
r (p
ptv)
LMDz-INCA ACE-FTS GEOS-CHEM
North Americar = 0.96r = 0.93
HC
HO
vm
r (p
ptv)
Europe-Russiar = 0.98r = 0.93
HC
HO
vm
r (p
ptv)
South Tropicsr = 0.0r = 0.38
8.5 kmComparison with 2 state-of-the-art models (LMDz-INCA and GEOS-Chem) that use different emissions inventories.North Hemisphere: seasonality of UT HCHO well reproduced intensity of the maximum not always reproduced
South Hemisphere: LMDz-INCA systematically smaller
South Tropics: small impact of biomass burning larger variability in the models
![Page 32: Atmospheric Chemistry Experiment (ACE): Recent Results Peter Bernath (and ACE team) Department of Chemistry, University of York Heslington, York, UK and.](https://reader036.fdocuments.us/reader036/viewer/2022062518/56649c7c5503460f949311ea/html5/thumbnails/32.jpg)
ACE Partners (Selected)
Canada- K. Walker, J. Drummond, K. Strong, J. McConnell, W. Evans, T. McElroy, I. Folkins, R. Martin, J. Sloan, T. Shepherd, etc.
USA- NASA launched ACE: C. Rinsland, L. Thomason (NASA-Langley), C. Randall (U. Colorado), B. Bojkov (NASA-Goddard), M. Santee, L. Froidevaux, G. Manney (JPL), etc.
Belgium- supplied CMOS imager chips: R. Colin, P.-F. Coheur, M. Carleer (ULB), D. Fussen, M. DeMaziere (IASB), M. Mahieu, R. Zander (Liege), etc.
UK- J. Remedios (Leicester), P. Palmer (Edinburgh), M. Chipperfield (Leeds)
France- C. Camy-Peyret, C. Clerbaux, C. Brogniez, G. Dufour, D. Hauglustaine (Paris)
Japan- M. Suzuki, Y. Kasai (JAXA) Sweden- G. Witt (Stockholm)
![Page 33: Atmospheric Chemistry Experiment (ACE): Recent Results Peter Bernath (and ACE team) Department of Chemistry, University of York Heslington, York, UK and.](https://reader036.fdocuments.us/reader036/viewer/2022062518/56649c7c5503460f949311ea/html5/thumbnails/33.jpg)
Sunset over Kitt Peak, AZ