Boreal Biomass Burning Plumes Research Articles

Impact of biomass burning emission on total peroxy nitrates: fire plume identification during the BORTAS campaign

Abstract. Total peroxy nitrate ( ∑ PN) concentrations have been measured using a thermal dissociation laser-induced fluorescence (TD-LIF) instrument during the BORTAS campaign, which focused on the impact of boreal biomass burning (BB) emissions on air quality in the Northern Hemisphere. The strong correlation observed between the ∑ PN concentrations and those of carbon monoxide (CO), a well-known pyrogenic tracer, suggests the possible use of the ∑ PN concentrations as marker of the BB plumes. Two methods for the identification of BB plumes have been applied: (1) ∑ PN concentrations higher than 6 times the standard deviation above the background and (2) ∑ PN concentrations higher than the 99th percentile of the ∑ PNs measured during a background flight (B625); then we compared the percentage of BB plume selected using these methods with the percentage evaluated, applying the approaches usually used in literature. Moreover, adding the pressure threshold ( ∼ 750 hPa) as ancillary parameter to ∑ PNs, hydrogen cyanide (HCN) and CO, the BB plume identification is improved. A recurrent artificial neural network (ANN) model was adapted to simulate the concentrations of ∑ PNs and HCN, including nitrogen oxide (NO), acetonitrile (CH3CN), CO, ozone (O3) and atmospheric pressure as input parameters, to verify the specific role of these input data to better identify BB plumes.

Size-dependent wet removal of black carbon in Canadian biomass burning plumes

Abstract. Wet deposition is the dominant mechanism for removing black carbon (BC) from the atmosphere and is key in determining its atmospheric lifetime, vertical gradient and global transport. Despite the importance of BC in the climate system, especially in terms of its ability to modulate the radiative energy budget, there are few quantitative case studies of wet removal in ambient environments. We present a case study of BC wet removal by examining aerosol size distributions and BC coating properties sampled in three Canadian boreal biomass burning plumes, one of which passed through a precipitating cloud. This depleted the majority of the plume's BC mass, and the largest and most coated BC-containing particles were found to be preferentially removed, suggesting that nucleation scavenging was likely the dominant mechanism. Calculated single-scattering albedo (SSA) showed little variation, as a large number of non-BC particles were also present in the precipitation-affected plume. The remaining BC cores were smaller than those observed in previous studies of BC in post-precipitation outflow over Asia, possibly due to the thick coating by hydrophilic compounds associated with the Canadian biomass burning particles. This study provides measurements of BC size, mixing state and removal efficiency to constrain model parameterisations of BC wet removal in biomass burning regions, which will help to reduce uncertainty in radiative forcing calculations.

Ozone photochemistry in boreal biomass burning plumes

Abstract. We present an analysis of ozone (O3) photochemistry observed by aircraft measurements of boreal biomass burning plumes over eastern Canada in the summer of 2011. Measurements of O3 and a number of key chemical species associated with O3 photochemistry, including non-methane hydrocarbons (NMHCs), nitrogen oxides (NOx) and total nitrogen containing species (NOy), were made from the UK FAAM BAe-146 research aircraft as part of the "quantifying the impact of BOReal forest fires on Tropospheric oxidants over the Atlantic using Aircraft and Satellites" (BORTAS) experiment between 12 July and 3 August 2011. The location and timing of the aircraft measurements put BORTAS into a unique position to sample biomass burning plumes from the same source region in Northwestern Ontario with a range of ages. We found that O3 mixing ratios measured in biomass burning plumes were indistinguishable from non-plume measurements, but evaluating them in relationship to measurements of carbon monoxide (CO), total alkyl nitrates (ΣAN) and the surrogate species NOz (= NOy-NOx) revealed that the potential for O3 production increased with plume age. We used NMHC ratios to estimate photochemical ages of the observed biomass burning plumes between 0 and 10 days. The BORTAS measurements provided a wide dynamic range of O3 production in the sampled biomass burning plumes with ΔO3/ΔCO enhancement ratios increasing from 0.020 ± 0.008 ppbv ppbv−1 in plumes with photochemical ages less than 2 days to 0.55 ± 0.29 ppbv ppbv−1 in plumes with photochemical ages greater than 5 days. We found that the main contributing factor to the variability in the ΔO3/ΔCO enhancement ratio was ΔCO in plumes with photochemical ages less than 4 days, and that was a transition to ΔO3 becoming the main contributing factor in plumes with ages greater than 4 days. In comparing O3 mixing ratios with components of the NOy budget, we observed that plumes with ages between 2 and 4 days were characterised by high aerosol loading, relative humidity greater than 40%, and low ozone production efficiency (OPE) of 7.7 ± 3.5 ppbv ppbv−1 relative to ΣAN and 1.6 ± 0.9 ppbv ppbv−1 relative to NOz. In plumes with ages greater than 4 days, OPE increased to 472 ± 28 ppbv ppbv−1 relative to ΣAN and 155 ± 5 ppbv ppbv−1 relative to NOz. From the BORTAS measurements we estimated that aged plumes with low aerosol loading were close to being in photostationary steady state and O3 production in younger plumes was inhibited by high aerosol loading and greater production of ΣAN relative to O3. The BORTAS measurements of O3 photochemistry in boreal biomass burning plumes were found to be consistent with previous summertime aircraft measurements made over the same region during the Arctic Research of the Composition of the Troposphere (ARCTAS-B) in 2008 and Atmospheric Boundary Layer Experiment (ABLE 3B) in 1990.

Observations of peroxyacetyl nitrate (PAN) in the upper troposphere by the Atmospheric Chemistry Experiment-Fourier Transform Spectrometer (ACE-FTS)

Abstract. Peroxyacetyl nitrate (CH3CO·O2NO2, abbreviated as PAN) is a trace molecular species present in the troposphere and lower stratosphere due primarily to pollution from fuel combustion and the pyrogenic outflows from biomass burning. In the lower troposphere, PAN has a relatively short lifetime and is principally destroyed within a few hours through thermolysis, but it can act as a reservoir and carrier of NOx in the colder temperatures of the upper troposphere, where UV photolysis becomes the dominant loss mechanism. Pyroconvective updrafts from large biomass burning events can inject PAN into the upper troposphere and lower stratosphere (UTLS), providing a means for the long-range transport of NOx. Given the extended lifetimes at these higher altitudes, PAN is readily detectable via satellite remote sensing. A new PAN data product is now available for the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) version 3.0 data set. We report observations of PAN in boreal biomass burning plumes recorded during the BORTAS (quantifying the impact of BOReal forest fires on Tropospheric oxidants over the Atlantic using Aircraft and Satellites) campaign (12 July to 3 August 2011). The retrieval method employed by incorporating laboratory-recorded absorption cross sections into version 3.0 of the ACE-FTS forward model and retrieval software is described in full detail. The estimated detection limit for ACE-FTS PAN is 5 pptv, and the total systematic error contribution to the ACE-FTS PAN retrieval is ~ 16%. The retrieved volume mixing ratio (VMR) profiles are compared to coincident measurements made by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) instrument on the European Space Agency (ESA) Environmental Satellite (ENVISAT). The MIPAS measurements demonstrated good agreement with the ACE-FTS VMR profiles for PAN, where the measured VMR values are well within the associated measurement errors for both instruments and comparative measurements differ no more than 70 pptv. The ACE-FTS PAN data set is used to obtain zonal mean distributions of seasonal averages from ~ 5–20 km. A strong seasonality is clearly observed for PAN concentrations in the global UTLS. Since the principal source of PAN in the UTLS is due to lofted biomass burning emissions from the pyroconvective updrafts created by large fires, the observed seasonality in enhanced PAN coincides with fire activity in different geographical regions throughout the year.

ACE-FTS observations of pyrogenic trace species in boreal biomass burning plumes during BORTAS

Abstract. To further our understanding of the effects of biomass burning emissions on atmospheric composition, the BORTAS campaign (BOReal forest fires on Tropospheric oxidants over the Atlantic using Aircraft and Satellites) was conducted on 12 July to 3 August 2011 during the boreal forest fire season in Canada. The simultaneous aerial, ground and satellite measurement campaign sought to record instances of boreal biomass burning to measure the tropospheric volume mixing ratios (VMRs) of short- and long-lived trace molecular species from biomass burning emissions. The goal was to investigate the connection between the composition and the distribution of these pyrogenic outflows and their resulting perturbation to atmospheric chemistry, with particular focus on oxidant species to determine the overall impact on the oxidizing capacity of the free troposphere. Measurements of pyrogenic trace species in boreal biomass burning plumes were made by the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) onboard the Canadian Space Agency (CSA) SCISAT-1 satellite during the BORTAS campaign. Even though biomass burning emissions are typically confined to the boundary layer, outflows are often injected into the upper troposphere by isolated convection and fire-related convective processes, thus allowing space-borne instruments to measure these pyrogenic outflows. An extensive set of 14 molecules – CH3OH, C2H2, C2H6, C3H6O, CO, HCN, HCOOH, HNO3, H2CO, NO, NO2, OCS, O3, and PAN – have been analysed. Included in this analysis is the calculation of age-dependent sets of enhancement ratios for each of the species originating from fires in North America (Canada, Alaska) and Siberia for a period of up to 7 days. Ratio values for the shorter lived primary pyrogenic species decrease over time primarily due to oxidation by the OH radical as the plume ages and values for longer lived species such as HCN and C2H6 remain relatively unchanged. Increasing negative values are observed for the oxidant species, including O3, indicating a destruction process in the plume as it ages such that concentrations of the oxidant species have dropped below their off-plume values. Results from previous campaigns have indicated that values for the molar ratios of ΔO3 /ΔO obtained from the measurements of the pyrogenic outflow from boreal fires are highly variable and range from negative to positive, irrespective of plume age. This variability has been attributed to pollution effects where the pyrogenic outflows have mixed with either local urban NOx emissions or pyrogenic emissions from the long-range transport of older plumes, thus affecting the production of O3 within the plumes. The results from this study have identified another potential cause of the variability in O3 concentrations observed in the measurements of biomass burning emissions, where evidence of stratosphere–troposphere exchange due to the pyroconvective updrafts from fires has been identified. Perturbations caused by the lofted emissions in these fire-aided convective processes may result in the intrusion of stratospheric air masses into the free troposphere and subsequent mixing of stratospheric O3 into the pyrogenic outflows causing fluctuations in observed ΔO3/ΔCO molar ratios.

The influence of biomass burning on the global distribution of selected non-methane organic compounds

Abstract. Forests fires are a significant source of chemicals to the atmosphere including numerous non-methane organic compounds (NMOCs). We report airborne measurement of hydrocarbons, acetone and methanol from >500 whole air samples collected over Eastern Canada, including interceptions of several different boreal biomass burning plumes. From these and concurrent measurements of carbon monoxide (CO) we derive fire emission ratios for 29 different organic species relative to the emission of CO. These range from 8.9 ± 3.2 ppt ppb−1 CO for methanol to 0.007 ± 0.004 ppt ppb−1 CO for cyclopentane. The ratios are in good to excellent agreement with literature values. Using the GEOS-Chem global 3-D chemical transport model (CTM) we show the influence of biomass burning on the global distributions of benzene, toluene, ethene and propene (species which are controlled for air quality purposes and sometimes used as indicative tracers of anthropogenic activity). Using our observationally derived emission ratios and the GEOS-Chem CTM, we show that biomass burning can be the largest fractional contributor to observed benzene, toluene, ethene and propene levels in many global locations. The widespread biomass burning contribution to atmospheric benzene, a heavily regulated air pollutant, suggests that pragmatic approaches are needed when setting air quality targets as tailpipe and solvent emissions decline in developed countries. We subsequently determine the extent to which the 28 global-status World Meteorological Organisation – Global Atmosphere Watch stations worldwide are influenced by biomass burning sourced benzene, toluene, ethene and propene as compared to their exposure to anthropogenic emissions.

Emission Ratios for Ammonia and Formic Acid and Observations of Peroxy Acetyl Nitrate (PAN) and Ethylene in Biomass Burning Smoke as Seen by the Tropospheric Emission Spectrometer (TES).

We use the Tropospheric Emission Spectrometer (TES) aboard the NASA Aura satellite to determine the concentrations of the trace gases ammonia (NH3) and formic acid (HCOOH) within boreal biomass burning plumes, and present the first detection of peroxy acetyl nitrate (PAN) and ethylene (C2H4) by TES. We focus on two fresh Canadian plumes observed by TES in the summer of 2008 as part of the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS-B) campaign. We use TES retrievals of NH3 and HCOOH within the smoke plumes to calculate their emission ratios (1.0% ± 0.5% and 0.31% ± 0.21%, respectively) relative to CO for these Canadian fires. The TES derived emission ratios for these gases agree well with previous aircraft and satellite estimates, and can complement ground-based studies that have greater surface sensitivity. We find that TES observes PAN mixing ratios of ~2 ppb within these mid-tropospheric boreal biomass burning plumes when the average cloud optical depth is low (<0.1) and that TES can detect C2H4 mixing ratios of ~2 ppb in fresh biomass burning smoke plumes.