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Combined retrievals of boreal forest fire aerosol properties with a polarimeter and lidar
K. Knobelspiesse, B. Cairns, M. Ottaviani, R. Ferrare, J. Hair, C. Hostetler, M. Obland, R. Rogers, J. Redemann, Y. Shinozuka, A. Clarke, S. Freitag, S. Howell, V. Kapustin,C. McNaughton
Atmospheric Chemistry and Physics (ACP) & Discussions (ACPD) , 2011,
Abstract: Absorbing aerosols play an important, but uncertain, role in the global climate. Much of this uncertainty is due to a lack of adequate aerosol measurements. While great strides have been made in observational capability in the previous years and decades, it has become increasingly apparent that this development must continue. Scanning polarimeters have been designed to help resolve this issue by making accurate, multi-spectral, multi-angle polarized observations. This work involves the use of the Research Scanning Polarimeter (RSP). The RSP was designed as the airborne prototype for the Aerosol Polarimetery Sensor (APS), which was due to be launched as part of the (ultimately failed) NASA Glory mission. Field observations with the RSP, however, have established that simultaneous retrievals of aerosol absorption and vertical distribution over bright land surfaces are quite uncertain. We test a merger of RSP and High Spectral Resolution Lidar (HSRL) data with observations of boreal forest fire smoke, collected during the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS). During ARCTAS, the RSP and HSRL instruments were mounted on the same aircraft, and validation data were provided by instruments on an aircraft flying a coordinated flight pattern. We found that the lidar data did indeed improve aerosol retrievals using an optimal estimation method, although not primarily because of the contraints imposed on the aerosol vertical distribution. The more useful piece of information from the HSRL was the total column aerosol optical depth, which was used to select the initial value (optimization starting point) of the aerosol number concentration. When ground based sun photometer network climatologies of number concentration were used as an initial value, we found that roughly half of the retrievals had unrealistic sizes and imaginary indices, even though the retrieved spectral optical depths agreed within uncertainties to independent observations. The convergence to an unrealistic local minimum by the optimal estimator is related to the relatively low sensitivity to particles smaller than 0.1 (μm) at large optical thicknesses. Thus, optimization algorithms used for operational aerosol retrievals of the fine mode size distribution, when the total optical depth is large, will require initial values generated from table look-ups that exclude unrealistic size/complex index mixtures. External constraints from lidar on initial values used in the optimal estimation methods will also be valuable in reducing the likelihood of obtaining spurious retrievals.
Injection in the lower stratosphere of biomass fire emissions followed by long-range transport: a MOZAIC case study
J.-P. Cammas, J. Brioude, J.-P. Chaboureau, J. Duron, C. Mari, P. Mascart, P. Nédélec, H. Smit, H.-W. P tz, A. Volz-Thomas, A. Stohl,M. Fromm
Atmospheric Chemistry and Physics (ACP) & Discussions (ACPD) , 2009,
Abstract: This paper analyses a stratospheric injection by deep convection of biomass fire emissions over North America (Alaska, Yukon and Northwest Territories) on 24 June 2004 and its long-range transport over the eastern coast of the United States and the eastern Atlantic. The case study is based on airborne MOZAIC observations of ozone, carbon monoxide, nitrogen oxides and water vapour during the crossing of the southernmost tip of an upper level trough over the Eastern Atlantic on 30 June and on a vertical profile over Washington DC on 30 June, and on lidar observations of aerosol backscattering at Madison (University of Wisconsin) on 28 June. Attribution of the observed CO plumes to the boreal fires is achieved by backward simulations with a Lagrangian particle dispersion model (FLEXPART). A simulation with the Meso-NH model for the source region shows that a boundary layer tracer, mimicking the boreal forest fire smoke, is lofted into the lowermost stratosphere (2–5 pvu layer) during the diurnal convective cycle at isentropic levels (above 335 K) corresponding to those of the downstream MOZAIC observations. It is shown that the order of magnitude of the time needed by the parameterized convective detrainment flux to fill the volume of a model mesh (20 km horizontal, 500 m vertical) above the tropopause with pure boundary layer air would be about 7.5 h, i.e. a time period compatible with the convective diurnal cycle. Over the area of interest, the maximum instantaneous detrainment fluxes deposited about 15 to 20% of the initial boundary layer tracer concentration at 335 K. According to the 275-ppbv carbon monoxide maximum mixing ratio observed by MOZAIC over Eastern Atlantic, such detrainment fluxes would be associated with a 1.4–1.8 ppmv carbon monoxide mixing ratio in the boundary layer over the source region.
Injection in the lower stratosphere of biomass fire emissions followed by long-range transport: a MOZAIC case study  [PDF]
J.-P. Cammas,J. Brioude,J.-P. Chaboureau,J. Duron
Atmospheric Chemistry and Physics Discussions , 2008,
Abstract: This paper analyses a stratospheric injection by deep convection of biomass fire emissions over North America (Alaska, Yukon and Northwest Territories) on 24 June 2004 and its long-range transport over the eastern coast of the United States and the eastern Atlantic. The case study is done using MOZAIC observations of ozone, carbon monoxide, nitrogen oxides (NOx+PAN) and water vapour during the crossing of the southernmost tip of an upper level trough over the Eastern Atlantic on 30 June 03:00 UTC and 10:00 UTC and in a vertical profile over Washington DC on 30 June 17:00 UTC, and by lidar observations of aerosol backscattering at Madison (University of Wisconsin) on 28 June. Attribution of the plumes to the boreal fires is achieved by backward simulations with a Lagrangian particle dispersion model (FLEXPART). A simulation with the Meso-NH model for the source region shows that a boundary layer tracer, mimicking the boreal forest fire smoke, is lofted into the lowermost stratosphere (2–5 pvu layer) during the diurnal convective cycle. The isentropic levels (above 335 K) correspond to those of the downstream MOZAIC observations. The parameterized convective detrainment flux is intense enough to fill the volume of a model mesh (20 km horizontal, 500 m vertical) above the tropopause with pure boundary layer air in a time period compatible with the convective diurnal cycle, i.e. about 5 h. The maximum instantaneous detrainment fluxes deposited about 15–20% of the initial boundary layer tracer concentration at 335 K, which according to the 275-ppbv carbon monoxide maximum mixing ratio observed by MOZAIC over eastern Atlantic, would be associated with a 1.4–1.8 ppmv carbon monoxide mixing ratio in the boundary layer over the source region.
Injection in the lower stratosphere of biomass fire emissions followed by long-range transport: a MOZAIC case study  [PDF]
J.-P. Cammas,J. Brioude,J.-P. Chaboureau,J. Duron
Atmospheric Chemistry and Physics (ACP) & Discussions (ACPD) , 2009,
Abstract: This paper analyses a stratospheric injection by deep convection of biomass fire emissions over North America (Alaska, Yukon and Northwest Territories) on 24 June 2004 and its long-range transport over the eastern coast of the United States and the eastern Atlantic. The case study is based on airborne MOZAIC observations of ozone, carbon monoxide, nitrogen oxides and water vapour during the crossing of the southernmost tip of an upper level trough over the Eastern Atlantic on 30 June and on a vertical profile over Washington DC on 30 June, and on lidar observations of aerosol backscattering at Madison (University of Wisconsin) on 28 June. Attribution of the observed CO plumes to the boreal fires is achieved by backward simulations with a Lagrangian particle dispersion model (FLEXPART). A simulation with the Meso-NH model for the source region shows that a boundary layer tracer, mimicking the boreal forest fire smoke, is lofted into the lowermost stratosphere (2–5 pvu layer) during the diurnal convective cycle at isentropic levels (above 335 K) corresponding to those of the downstream MOZAIC observations. It is shown that the order of magnitude of the time needed by the parameterized convective detrainment flux to fill the volume of a model mesh (20 km horizontal, 500 m vertical) above the tropopause with pure boundary layer air would be about 7.5 h, i.e. a time period compatible with the convective diurnal cycle. Over the area of interest, the maximum instantaneous detrainment fluxes deposited about 15 to 20% of the initial boundary layer tracer concentration at 335 K. According to the 275-ppbv carbon monoxide maximum mixing ratio observed by MOZAIC over Eastern Atlantic, such detrainment fluxes would be associated with a 1.4–1.8 ppmv carbon monoxide mixing ratio in the boundary layer over the source region.
An investigation of methods for injecting emissions from boreal wildfires using WRF-Chem during ARCTAS
W. R. Sessions, H. E. Fuelberg, R. A. Kahn,D. M. Winker
Atmospheric Chemistry and Physics (ACP) & Discussions (ACPD) , 2011,
Abstract: The Weather Research and Forecasting Model (WRF) is considered a "next generation" mesoscale meteorology model. The inclusion of a chemistry module (WRF-Chem) allows transport simulations of chemical and aerosol species such as those observed during NASA's Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) in 2008. The ARCTAS summer deployment phase during June and July coincided with large boreal wildfires in Saskatchewan and Eastern Russia. One of the most important aspects of simulating wildfire plume transport is the height at which emissions are injected. WRF-Chem contains an integrated one-dimensional plume rise model to determine the appropriate injection layer. The plume rise model accounts for thermal buoyancy associated with fires and local atmospheric stability. This paper describes a case study of a 10 day period during the Spring phase of ARCTAS. It compares results from the plume model against those of two more traditional injection methods: Injecting within the planetary boundary layer, and in a layer 3–5 km above ground level. Fire locations are satellite derived from the GOES Wildfire Automated Biomass Burning Algorithm (WF_ABBA) and the MODIS thermal hotspot detection. Two methods for preprocessing these fire data are compared: The prep_chem_sources method included with WRF-Chem, and the Naval Research Laboratory's Fire Locating and Monitoring of Burning Emissions (FLAMBE). Results from the simulations are compared with satellite-derived products from the AIRS, MISR and CALIOP sensors. When FLAMBE provides input to the 1-D plume rise model, the resulting injection heights exhibit the best agreement with satellite-observed injection heights. The FLAMBE-derived heights are more realistic than those utilizing prep_chem_sources. Conversely, when the planetary boundary layer or the 3–5 km a.g.l. layer were filled with emissions, the resulting injection heights exhibit less agreement with observed plume heights. Results indicate that differences in injection heights produce different transport pathways. These differences are especially pronounced in area of strong vertical wind shear and when the integration period is long.
Boreal forest fire emissions in fresh Canadian smoke plumes: C1-C10 volatile organic compounds (VOCs), CO2, CO, NO2, NO, HCN and CH3CN
I. J. Simpson, S. K. Akagi, B. Barletta, N. J. Blake, Y. Choi, G. S. Diskin, A. Fried, H. E. Fuelberg, S. Meinardi, F. S. Rowland, S. A. Vay, A. J. Weinheimer, P. O. Wennberg, P. Wiebring, A. Wisthaler, M. Yang, R. J. Yokelson,D. R. Blake
Atmospheric Chemistry and Physics (ACP) & Discussions (ACPD) , 2011,
Abstract: Boreal regions comprise about 17 % of the global land area, and they both affect and are influenced by climate change. To better understand boreal forest fire emissions and plume evolution, 947 whole air samples were collected aboard the NASA DC-8 research aircraft in summer 2008 as part of the ARCTAS-B field mission, and analyzed for 79 non-methane volatile organic compounds (NMVOCs) using gas chromatography. Together with simultaneous measurements of CO2, CO, CH4, CH2O, NO2, NO, HCN and CH3CN, these measurements represent the most comprehensive assessment of trace gas emissions from boreal forest fires to date. Based on 105 air samples collected in fresh Canadian smoke plumes, 57 of the 80 measured NMVOCs (including CH2O) were emitted from the fires, including 45 species that were quantified from boreal forest fires for the first time. After CO2, CO and CH4, the largest emission factors (EFs) for individual species were formaldehyde (2.1 ± 0.2 g kg 1), followed by methanol, NO2, HCN, ethene, α-pinene, β-pinene, ethane, benzene, propene, acetone and CH3CN. Globally, we estimate that boreal forest fires release 2.4 ± 0.6 Tg C yr 1 in the form of NMVOCs, with approximately 41 % of the carbon released as C1-C2 NMVOCs and 21 % as pinenes. These are the first reported field measurements of monoterpene emissions from boreal forest fires, and we speculate that the pinenes, which are relatively heavy molecules, were detected in the fire plumes as the result of distillation of stored terpenes as the vegetation is heated. Their inclusion in smoke chemistry models is expected to improve model predictions of secondary organic aerosol (SOA) formation. The fire-averaged EF of dichloromethane or CH2Cl2, (6.9 ± 8.6) × 10 4 g kg 1, was not significantly different from zero and supports recent findings that its global biomass burning source appears to have been overestimated. Similarly, we found no evidence for emissions of chloroform (CHCl3) or methyl chloroform (CH3CCl3) from boreal forest fires. The speciated hydrocarbon measurements presented here show the importance of carbon released by short-chain NMVOCs, the strong contribution of pinene emissions from boreal forest fires, and the wide range of compound classes in the most abundantly emitted NMVOCs, all of which can be used to improve biomass burning inventories in local/global models and reduce uncertainties in model estimates of trace gas emissions and their impact on the atmosphere.
Boreal snow cover variations induced by aerosol emissions in the middle of the 21st century  [PDF]
M. Ménégoz,G. Krinner,Y. Balkanski,A. Cozic
The Cryosphere Discussions , 2012, DOI: 10.5194/tcd-6-4733-2012
Abstract: We used a coupled climate-chemistry model to quantify the impacts of aerosols on snow cover both for the present-day and for the middle of the 21st century. Black carbon (BC) deposition over continents induces a reduction in the Mean Number of Days With Snow at the Surface (MNDWS) that ranges from 0 to 10 days over large areas of Eurasia and Northern America for the present-day relative to the pre-industrial period. This is mainly due to BC deposition during the spring, a period of the year when the remaining of snow accumulated during the winter is exposed to both strong solar radiation and large amount of aerosol deposition induced themselves by a high level of transport of particles from polluted areas. North of 30° N, this deposition flux represents 222 Gg BC month 1 on average from April to June in our simulation. A large reduction in BC emissions is expected in the future in the Radiative Concentration Pathway (RCP) scenarios. Considering this scenario in our simulation leads to a decrease in the spring BC deposition down to 110 Gg month 1 in the 2050s in the RCP8.5 scenario. However, despite the reduction of the aerosol impact on snow, the MNDWS is strongly reduced by 2050, with a decrease ranging from 10 to 100 days from pre-industrial values over large parts of the Northern Hemisphere. This reduction is essentially due to temperature increase, which is quite strong in the RCP8.5 scenario in the absence of climate mitigation policies. Moreover, the projected sea-ice retreat in the next decades will open new routes for shipping in the Arctic. However, a large increase in shipping emissions in the Arctic by the mid 21st century does not lead to significant changes of BC deposition over snow-covered areas in our simulation. Therefore, the MNDWS is clearly not affected through snow darkening effects associated to these Arctic ship emissions. In an experiment without nudging toward atmospheric reanalyses, we simulated however some changes of the MNDWS considering such aerosol ship emissions. These changes are generally not statistically significant in boreal continents, except in the Quebec and in the West Siberian plains, where they range between 5 and 10 days. They are induced both by radiative forcings of the aerosols when they are in the atmosphere, and by all the atmospheric feedbacks. Climate change by the mid 21st century could also cause biomass burning activity (forest fires) to become more intense and occur earlier in the season. In an idealized scenario in which forest fires are 50% stronger and occur 2 weeks earlier than at present, we
Mega fire emissions in Siberia: potential supply of soluble iron from forests to the ocean  [PDF]
A. Ito
Biogeosciences Discussions , 2011, DOI: 10.5194/bgd-8-1483-2011
Abstract: Significant amounts of carbon and nutrients are released to the atmosphere due to large fires in forests. Characterization of the spatial distribution and temporal variation of the intense fire emissions is crucial for assessing the atmospheric loadings of aerosols and trace gases. This paper discusses issues of the representation of forest fires in the estimation of emissions and the application to an atmospheric chemistry transport model (CTM). The potential contribution of forest fires to the deposition of soluble iron (Fe) into the ocean is highlighted, with a focus on mega fires in eastern Siberia. Satellite products of burned area, active fire, and land cover are used to estimate biomass burning emissions in conjunction with a biogeochemical model. Satellite-derived plume height from MISR is used for the injection height of boreal forest fire emissions. This methodology is applied to quantify fire emission rates in each three-dimensional grid location in the high latitude Northern Hemisphere (> 30° N latitude) over a 5-year period from 2001 to 2005. There is large interannual variation in forest burned area during 2001–2005 (13–51 × 103 km2 yr 1) which results in a corresponding variation in the annual emissions of carbon monoxide (CO) (12–78 Tg CO yr 1). Satellite observations of CO from MOPITT are used to evaluate the model performance in simulating the spatial distribution and temporal variation of the fire emissions. During the major Siberian fire seasons in the summer of 2002 and in the spring of 2003, the model results for CO enhancements due to intense fires are in good agreement with MOPITT observations. These fire emission rates are applied to the aerosol chemistry transport model to examine the relative importance of biomass burning sources of soluble iron compared to those from dust sources. Compared to the dust sources without the atmospheric processing by acidic species, extreme fire events contribute to a significant deposition of soluble iron (10–60%) to downwind regions over the western North Pacific Ocean. It may imply that the supply of nutrients from large forest fires plays a role as a negative biosphere-climate feedback with regards to the ocean fertilization.
Mega fire emissions in Siberia: potential supply of bioavailable iron from forests to the ocean
A. Ito
Biogeosciences (BG) & Discussions (BGD) , 2011,
Abstract: Significant amounts of carbon and nutrients are released to the atmosphere due to large fires in forests. Characterization of the spatial distribution and temporal variation of the intense fire emissions is crucial for assessing the atmospheric loadings of trace gases and aerosols. This paper discusses issues of the representation of forest fires in the estimation of emissions and the application to an atmospheric chemistry transport model (CTM). The potential contribution of forest fires to the deposition of bioavailable iron (Fe) into the ocean is highlighted, with a focus on mega fires in eastern Siberia. Satellite products of burned area, active fire, and land cover are used to estimate biomass burning emissions in conjunction with a biogeochemical model. Satellite-derived plume height from MISR is used for the injection height of boreal forest fire emissions. This methodology is applied to quantify fire emission rates in each three-dimensional grid location in the high latitude Northern Hemisphere (>30° N latitude) over a 5-yr period from 2001 to 2005. There is large interannual variation in forest burned area during 2001–2005 (13–49 × 103 km2 yr 1) which results in a corresponding variation in the annual emissions of carbon monoxide (CO) (14–81 Tg CO y 1). Satellite observations of CO column from MOPITT are used to evaluate the model performance in simulating the spatial distribution and temporal variation of the fire emissions. The model results for CO enhancements due to eastern Siberian fires are in good agreement with MOPITT observations. These validation results suggest that the model using emission rates estimated in this work is able to describe the interannual changes in CO due to intense forest fires. Bioavailable iron is derived from atmospheric processing of relatively insoluble iron from desert sources by anthropogenic pollutants (mainly sulfuric acid formed from oxidation of SO2) and from direct emissions of soluble iron from combustion sources. Emission scenarios for IPCC AR5 report (Intergovernmental Panel on Climate Change; Fifth Assessment Report) suggest that anthropogenic SO2 emissions are suppressed in the future to improve air quality. In future warmer and drier climate, severe fire years such as 2003 may become more frequent in boreal regions. The fire emission rates estimated in this study are applied to the aerosol chemistry transport model to examine the relative importance of biomass burning sources of soluble iron compared to those from dust sources. The model reveals that extreme fire events contribute to a significant deposition of soluble iron (20–40 %) to downwind regions over the western North Pacific Ocean, compared to the dust sources with no atmospheric processing by acidic species. These results suggest that the supply of nutrients from large forest fires plays a role as a negative biosphere-climate feedback with regards to the ocean fertilization.
Boreal forest fires in 1997 and 1998: a seasonal comparison using transport model simulations and measurement data  [PDF]
N. Spichtinger,R. Damoah,S. Eckhardt,C. Forster
Atmospheric Chemistry and Physics Discussions , 2004,
Abstract: Forest fire emissions have a strong impact on the concentrations of trace gases and aerosols in the atmosphere. In order to quantify the influence of boreal forest fire emissions on the atmospheric composition, the fire seasons of 1997 and 1998 are compared in this paper. Fire activity in 1998 was very strong, especially over Canada and Eastern Siberia, whereas it was much weaker in 1997. According to burned area estimates the burning in 1998 was more than six times as intense as in 1997. Based on hot spot locations derived from ATSR (Along Track Scanning Radiometer) data and official burned area data, fire emissions were estimated and their transport was simulated with a Lagrangian tracer transport model. Siberian and Canadian forest fire tracers were distinguished to investigate the transport of both separately. The fire emissions were transported even over intercontinental distances. Due to the El Ni o induced meteorological situation, transport from Siberia to Canada was enhanced in 1998. Siberian fire emissions were transported towards Canada and contributed concentrations more than twice as high as those due to Canada's own CO emissions by fires. In 1998 both tracers arrive at higher latitudes over Europe, which is due to a higher North Atlantic Oscillation (NAO) index in 1998. The simulated emission plumes are compared to CMDL (Climate Monitoring and Diagnostics Laboratory) CO2 and CO data, Total Ozone Mapping Spectrometer (TOMS) aerosol index (AI) data and Global Ozone Monitoring Experiment (GOME) tropospheric NO2 columns. All the data show clearly enhanced signals during the burning season of 1998 compared to 1997. The results of the model simulation are in good agreement with ground-based as well as satellite-based measurements.
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