Reconstructing ozone chemistry from Asian fires using satellite and aircraft

measurements (Spring ARCTAS 2008)

Richard Dupont 1, John Worden 1, Brad Pierce 2, Johnathan Hair 3, Marta Fenn 3, Paul Hamer 1, Murali Natarajan 3, Todd Schaack 4, Allen Lenzen 4, Eric Apel 5, Jack Dibb 6, Glenn Diskin 3 and Andrew Weinheimer 5

1. Jet Propulsion Laboratory/Caltech, Pasadena, CA, USA2. NOAA/NESDIS/STAR, Madison, WI, USA3. NASA Langley Research Center, Hampton, VI, USA4. Space Science and Engineering Center, University of Wisconsin, Madison, WI, USA 5. National Center for Atmospheric Research, Boulder, CO, USA 6. University of New Hampshire - EOS, Durham, NH, USA

Ozone (O3)

O3 + hv O1D

CO/CH4/VOC

O2

H2OOH HO2/RO2

NO

NO2hv

O(3P)

O2

HOx

HONO

HONO2

HO2NO2

H2O2

ROOH

The third most important greenhouse gas in the atmosphere (IPCC, 2007).

An important source of hydroxyl radicals (HOx), the “detergent” of the atmosphere;

Wildfire emissions affect atmospheric composition at a global scale (Andreae, 1983; Reichle et al, 1986, Fishman et al., 1990, Soja et al., 2006);

Biomass burning emissions appear to be comparable to fossil fuel emissions (Seiler and Crutzen, 1980; Crutzen and Andreae, 1990);

Global biomass burning emissions

Asian biomass burning emissions

Asian fires = 10% of global bb C emissions (Van der Werf et al., 2006);Important role in tropospheric CO variability and magnitude in the Northern Hemisphere (Novelli et al., 2003; Edwards et al., 2004; Kasischke et al., 2005; Pfister et al., 2005; Nedelec et al., 2005);Influence tropospheric O3 concentrations over North America (Jaffe et al., 2004;

Bertschi and Jaffe, 2005; Morris et al., 2006), the Arctic (Warnecke et al., 2008) and even Europe (Simmonds et al., 2005).

Fires impact on tropospheric O3 concentrations is challenging to estimate. O3 production depends on aerosols (photochemical production) as well as highly variable PAN and NOx emissions and the cycling between these species (Mauzerall et al., 1996; Lapina et al., 2006; Val Martin et al., 2006; Real et al., 2007; Verma et al., 2009).

Quantifying the impact of Asian fires on O3 concentrations over North America during the Spring ARCTAS 2008 campaign;

Identifying the chemical and dynamical processes involved during the transport of biomass burning plumes over the Pacific ocean.

Goals

MODIS fire count

Spring ARCTAS: April 2008

High fire activity over Asian boreal region in April 2008 (Fisher et al., 2010)

3 regions of major fire activity in the mid-northern latitudes:- Kazakhstan- Siberia- South East Asia (Thailand)

ARCTASARCTAS

Warm conveyor belt

Multiple types of measurement platforms:- Aircraft (NASA DC8, …)- Satellites (TES, OMI, MODIS, …- Ground-based measurements- Sondes (ARCIONS)

CO2H2O, N2O O3

TES

TES = infrared Fourier Transform SpectrometerSpectral range = 650-2250 cm-1

Nadir footprint = 5.3 km (across-track) × 8.5 km (along track) (Beer et al., 2001)O3 vertical resolution = about 6 kmMain sensitivity = middle troposphere

NASA/DC8 aircraft data

Ozone (O3) and Aerosol Scattering Ratio (ASR) = Differential Absorption LidarCarbon monoxide (CO) = Spectrometer and photometerSulfur dioxide (SO2) = Chemical Ionization Mass Spectrometer Black Carbon (BC) = Particle photometerNitrogen Oxides (NOx) + PeroxyAcetyl Nitrate (PAN) = NCAR NOxyO3Hydrogen CyaNide (HCN) = Chemical Ionization Mass Spectrometer

RAQMS (Pierce et al., JGR, 2007)

Developed by UW-Madison and NASA LangleyGlobal 3D modelAssimilation and forecast of chemistry and aerosols including STESpatial resolution : 2°×2°35 vertical levels (max 60km)Temporal resolution : 6h

Long range transport

Kazakhstan/Siberianplume

Thailandplume

ASR O3

Chemistry

The lower/middle tropospheric plume has a biomass burning origin;

Kazakhstan/Siberian plume trajectory (RAQMS)

Kazakhstan/Siberian plume trajectory (RAQMS)

Kazakhstan/Siberian plume trajectory (RAQMS)

Kazakhstan and Siberian fires increase background concentrations of CC, CO and O3 respectively by 4 ppbv, 50 ppbv and nearly 9 ppbv in the lower troposphere;

Thailand fires increase background concentrations of CC, CO and O3 respectively by 2 ppbv, 70 ppbv and nearly 10 ppbv in the upper troposphere;

Fires impact over Northwestern America

Conclusion

The stratosphere appears to be the main contributor of O3 concentrations in Asian biomass burning plumes during spring. However, photochemistry also plays an important role;

After transport over the Pacific, Thailand and Kazakhstan fires increase tropospheric O3 concentrations of about 10 ppbv relative to background levels;

The Asian fires can contribute to about 10-15% of the tropospheric O3 concentrations measured over the west coast of North America.