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We characterise the vertical distribution of biomass-burning emissions across the Amazon during the biomass-burning season (July–November) with an extensive climatology of smoke plumes derived from MISR and MODIS (2005–2012) and CALIOP (2006–2012) observations. Smoke plume heights exhibit substantial variability, spanning a few hundred metres up to 6 km above the terrain. However, the majority of the smoke is located at altitudes below 2.5 km. About 60 % of smoke plumes are observed in drought years, 40 %–50 % at the peak month of the burning season (September) and 94 % over tropical forest and savanna regions, with respect to the total number of smoke plume observations. At the time of the MISR observations (10:00–11:00 LT), the highest plumes are detected over grassland fires (with an averaged maximum plume height of ∼1100 m) and the lowest plumes occur over tropical forest fires (∼800 m). A similar pattern is found later in the day (14:00–15:00 LT) with CALIOP, although at higher altitudes (2300 m grassland vs. 2000 m tropical forest), as CALIOP typically detects smoke at higher altitudes due to its later overpass time, associated with a deeper planetary boundary layer, possibly more energetic fires, and greater sensitivity to thin aerosol layers. On average, 3 %–20 % of the fires inject smoke into the free troposphere; this percentage tends to increase toward the end of the burning season (November: 15 %–40 %). We find a well-defined seasonal cycle between MISR plume heights, MODIS fire radiative power and atmospheric stability across the main biomes of the Amazon, with higher smoke plumes, more intense fires and reduced atmospheric stability conditions toward the end of the burning season. Lower smoke plume heights are detected during drought (800 m) compared to non-drought (1100 m) conditions, in particular over tropical forest and savanna fires. Drought conditions favour understory fires over tropical forest, which tend to produce smouldering combustion and low smoke injection heights. Droughts also seem to favour deeper boundary layers and the percentage of smoke plumes that reach the free troposphere is lower during these dry conditions. Consistent with previous studies, the MISR mid-visible aerosol optical depth demonstrates that smoke makes a significant contribution to the total aerosol loading over the Amazon, which in combination with lower injection heights in drought periods has important implications for air quality. This work highlights the importance of biome type, fire properties and atmospheric and drought conditions for plume dynamics and smoke loading. In addition, our study demonstrates the value of combining observations of MISR and CALIOP constraints on the vertical distribution of smoke from biomass burning over the Amazon.

Biomass burning is a significant source of trace gases and aerosols to the atmosphere, and the evolution of these species depends acutely on where they are injected into the atmosphere. GEOS-Chem is a chemical transport model driven by assimilated meteorological data that is used to probe a variety of scientific questions related to atmospheric composition, including the role of biomass burning. This paper presents the development and implementation of a new global biomass burning emissions injection scheme in the GEOS-Chem model. The new injection scheme is based on monthly gridded Multi-angle Imaging SpectroRadiometer (MISR) global plume-height stereoscopic observations in 2008. To provide specific examples of the impact of the model updates, we compare the output from simulations with and without the new MISR-based injection height scheme to several sets of observations from regions with active fires. Our comparisons with Arctic Research on the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) aircraft observations show that the updated injection height scheme can improve the ability of the model to simulate the vertical distribution of peroxyacetyl nitrate (PAN) and carbon monoxide (CO) over North American boreal regions in summer. We also compare a simulation for October 2010 and 2011 to vertical profiles of CO over the Amazon Basin. When coupled with larger emission factors for CO, a simulation that includes the new injection scheme also better matches selected observations in this region. Finally, the improved injection height improves the simulation of monthly mean surface CO over California during July 2008, a period with large fires.

The Community Atmosphere Model (CAM), version 5, is now coupled to extensive tropospheric and stratospheric chemistry, called CAM5-chem, and is available in addition to CAM4-chem in the Community Earth System Model (CESM) version 1.2. The main focus of this paper is to compare the performance of configurations with internally derived "free running" (FR) meteorology and "specified dynamics" (SD) against observations from surface, aircraft, and satellite, as well as understand the origin of the identified differences. We focus on the representation of aerosols and chemistry. All model configurations reproduce tropospheric ozone for most regions based on in situ and satellite observations. However, shortcomings exist in the representation of ozone precursors and aerosols. Tropospheric ozone in all model configurations agrees for the most part with ozonesondes and satellite observations in the tropics and the Northern Hemisphere within the variability of the observations. Southern hemispheric tropospheric ozone is consistently underestimated by up to 25%. Differences in convection and stratosphere to troposphere exchange processes are mostly responsible for differences in ozone in the different model configurations. Carbon monoxide (CO) and other volatile organic compounds are largely underestimated in Northern Hemisphere mid-latitudes based on satellite and aircraft observations. Nitrogen oxides (NOx) are biased low in the free tropical troposphere, whereas peroxyacetyl nitrate (PAN) is overestimated in particular in high northern latitudes. The present-day methane lifetime estimates are compared among the different model configurations. These range between 7.8 years in the SD configuration of CAM5-chem and 8.8 years in the FR configuration of CAM4-chem and are therefore underestimated compared to observational estimations. We find that differences in tropospheric aerosol surface area between CAM4 and CAM5 play an important role in controlling the burden of the tropical tropospheric hydroxyl radical (OH), which causes differences in tropical methane lifetime of about half a year between CAM4-chem and CAM5-chem. In addition, different distributions of NOx from lightning explain about half of the difference between SD and FR model versions in both CAM4-chem and CAM5-chem. Remaining differences in the tropical OH burden are due to enhanced tropical ozone burden in SD configurations compared to the FR versions, which are not only caused by differences in chemical production or loss but also by transport and mixing. For future studies, we recommend the use of CAM5-chem configurations, due to improved aerosol description and inclusion of aerosol–cloud interactions. However, smaller tropospheric surface area density in the current version of CAM5-chem compared to CAM4-chem results in larger oxidizing capacity in the troposphere and therefore a shorter methane lifetime.

Ten-year observations of trace gases at Pico Mountain Observatory (PMO), a free troposphere site in the central North Atlantic, were classified by transport patterns using the Lagrangian particle dispersion model, FLEXPART. The classification enabled identifying trace gas mixing ratios associated with background air and long- range transport of continental emissions, which were defined as chemical signatures. Comparison between the chemical signatures revealed the impacts of natural and anthropogenic sources, as well as chemical and physical processes during long transport,on air composition in the remote North Atlantic. Transport of North American anthropogenic emissions(NA-Anthro) and summertime wildfire plumes (Fire) significantly enhanced CO and O3 at PMO. Summertime CO enhancements caused by NA-Anthro were found to have been decreasing by a rate of 0.67 ± 0.60 ppbv/year in the ten-year period, due possibly to reduction of emissions in North America. Downward mixing from the upper troposphere and stratosphere due to the persistent Azores-Bermuda anticyclone causes enhanced O3 and nitrogen oxides. The d[O3]/d [CO] value was used to investigate O3 sources and chemistry in different transport patterns. The transport pattern affected by Fire had the lowest d [O3]/d [CO], which was likely due to intense CO production and depressed O3 production in wildfire plumes. Slightly enhanced O3 and d [O3]/d [CO] were found in the background air, suggesting that weak downward mixing from the upper troposphere is common at PMO. Enhancements of both butane isomers were found during upslope flow periods, indicating contributions from local sources. The consistent ratio of butane isomers associated with the background air and NA-anthro implies no clear difference in the oxidation rates of the butane isomers during long transport. Based on observed relationships between non-methane hydrocarbons, the averaged photochemical age of the air masses at PMO was estimated to be 11 ± 4 days.

The Pico Mountain Observatory, located at 2225 m a.s.l. in the Azores Islands, was established in 2001 to observe long-range transport from North America to the central North Atlantic. In previous research conducted at the observatory, ozone enhancement (> 55 ppbv) in North American outflows was observed, and efficient ozone production in these outflows was postulated. This study is focused on determining the causes for high d[O3] / d[CO] values (~1 ppbv ppbv−1) observed in the summers of 2009 and 2010. The folded retroplume technique, developed by Owen and Honrath (2009), was applied to combine upwind FLEXPART transport pathways with GEOS-Chem chemical fields. The folded result provides a semi-Lagrangian view of polluted North American outflow in terms of physical properties and chemical processes, including production/loss rate of ozone and NOx produced by lightning and thermal decomposition of peroxy acetyl nitrate (PAN). Two transport events from North America were identified for detailed analysis. High d[O3] / d[CO] was observed in both events, but due to differing transport mechanisms, ozone production tendency differed between the two. A layer of net ozone production was found at 2 km a.s.l. over the Azores in the first event plume, apparently driven by PAN decomposition during subsidence of air mass in the Azores–Bermuda High. In the second event, net ozone loss occurred during transport in the lower free troposphere, yet observed d[O3] / d[CO] was high. We estimate that in both events, CO loss through oxidation contributed significantly to d[O3] / d[CO] enhancement. Thus, it is not appropriate to use CO as a passive tracer of pollution in these events. In general, use of d[O3] / d[CO] as an indicator of net ozone production/loss may be invalid for any situation in which oxidants are elevated. Based on our analysis, use of d[O3] / d[CO] to diagnose ozone enhancement without verifying the assumption of negligible CO loss is not advisable.

In situ measurements of carbon monoxide (CO) and ozone (O3) at the Pico Mountain Observatory (PMO) located in the Azores, Portugal, are analyzed together with results from an atmospheric chemical transport model (GEOS-Chem) and satellite remote sensing data (AIRS (Atmospheric Infrared Sounder) for CO, and TES (Tropospheric Emission Spectrometer) for O3) to examine the evolution of free-troposphere CO and O3 over the North Atlantic for 2001–2011. GEOS-Chem captured the seasonal cycles for CO and O3 well but significantly underestimated the mixing ratios of CO, particularly in spring. Statistically significant (using a significance level of 0.05) decreasing trends were found for both CO and O3 based on harmonic regression analysis of the measurement data. The best estimates of the possible trends for CO and O3 measurements are −0.31 ± 0.30 (2-σ) ppbv yr−1 and −0.21 ± 0.11 (2-σ) ppbv yr−1, respectively. Similar decreasing trends for both species were obtained with GEOS-Chem simulation results. The most important factor contributing to the decreases in CO and O3 at PMO over the past decade is the decline in anthropogenic emissions from North America, which more than compensate for the impacts from increasing Asian emissions. It is likely that climate change in the past decade has also affected the intercontinental transport of O3.

We analyze an extensive record of aerosol smoke plume heights derived from observations over North America for the fire seasons of 2002 and 2004–2007 made by the Multi-angle Imaging SpectroRadiometer (MISR) instrument on board the NASA Earth Observing System Terra satellite. We characterize the magnitude and variability of smoke plume heights for various biomes, and assess the contribution of local atmospheric and fire conditions to this variability. Plume heights are highly variable, ranging from a few hundred meters up to 5000 m above the terrain at the Terra overpass time (11:00–14:00 local time). The largest plumes are found over the boreal region (median values of ~850 m height, 24 km length and 940 m thickness), whereas the smallest plumes are found over cropland and grassland fires in the contiguous US (median values of ~530 m height, 12 km length and 550–640 m thickness). The analysis of plume heights in combination with assimilated meteorological observations from the NASA Goddard Earth Observing System indicates that a significant fraction (4–12%) of plumes from fires are injected above the boundary layer (BL), consistent with earlier results for Alaska and the Yukon Territories during summer 2004. Most of the plumes located above the BL (>83%) are trapped within stable atmospheric layers. We find a correlation between plume height and the MODerate resolution Imaging Spectroradiometer (MODIS) fire radiative power (FRP) thermal anomalies associated with each plume. Smoke plumes located in the free troposphere (FT) exhibit larger FRP values (1620–1640 MW) than those remaining within the BL (174–465 MW). Plumes located in the FT without a stable layer reach higher altitudes and are more spread-out vertically than those associated with distinct stable layers (2490 m height and 2790 m thickness versus 1880 m height and 1800 m thickness). The MISR plume climatology exhibits a well-defined seasonal cycle of plume heights in boreal and temperate biomes, with greater heights during June–July. MODIS FRP measurements indicate that larger summertime heights are the result of higher fire intensity, likely due to more severe fire weather during these months. This work demonstrates the significant effect of fire intensity and atmospheric structure on the ultimate rise of fire emissions, and underlines the importance of considering such physical processes in modeling smoke dispersion.

[1] Measurements of NO, NO2, and NOy (total reactive nitrogen oxides) made at the Pico Mountain station, 38.47°N, 28.40°W, 2.2 km above sea level, from July 2002 to August 2005 are used to characterize the seasonal and diurnal variations of nitrogen oxides in the background lower free troposphere (FT) over the central North Atlantic Ocean. These observations reveal a well-defined seasonal cycle of nitrogen oxides (NOx = NO + NO2 and NOy), with higher mixing ratios during the summertime. Observed NOx and NOy levels are consistent with long-range transport of emissions, with significant removal en route to the measurement site. Larger summertime nitrogen oxides levels are attributed to boreal wildfire emissions and more efficient export and transport of NOy from eastern North America during that season. In addition, measurements of NOx and NOy obtained during in-cloud and cloud-free conditions are used to estimate PAN and HNO3 mixing ratios and examine the partitioning of the reactive nitrogen species. These estimates indicate that reactive nitrogen over the central North Atlantic lower FT largely exists in the form of PAN and HNO3 (∼80–90% of NOy) year-round. The composition of NOy shifts from dominance of PAN in winter-spring to dominance of HNO3 in summer-fall, as a result of changes in temperature and photochemistry over the region. A further comparison of the nitrogen oxides measurements with results from the global chemical transport model GEOS-Chem finds that simulated nitrogen oxides are significantly larger than the observations.

[1] Transport of North American anthropogenic and boreal wildfire emissions is a large source of nitrogen oxides over the North Atlantic region. To characterize the influence of transport of these emissions on nitrogen oxides levels over the central North Atlantic lower free troposphere (FT) and their further implications for hemispheric O3, we analyze measurements of NOx (NO + NO2), total reactive nitrogen oxides (NOy), CO, and O3 made at the Pico Mountain station (38.47°N 28.40°W, 2.2 km above sea level) in the Azores archipelago from July 2002 to August 2005. Transport of pollution from North America causes significant enhancements of nitrogen oxides year-round. An analysis of the export of United States NOx emissions to the FT based on observed ΔNOy/ΔCO in the anthropogenic plumes indicates that more than 94% of the NOx emitted over the United States is lost within the continent and/or during export out of the United States boundary layer and to the Azores, consistent with previous studies. However, our observations indicate that about 30% of the NOy initially exported out of the United States boundary layer reach the Azores lower FT. NOx was also significantly enhanced in these plumes. Since the lifetime of NOx is shorter than the transport timescale of most events, PAN decomposition and potentially photolysis of HNO3 provide a supply of NOx over the central North Atlantic lower FT. Observed ΔO3/ΔNOy ratios and significant NOy levels remaining in the North American plumes suggest a potential for O3 formation well downwind from North America. Summertime boreal wildfires in North America are responsible for important shifts in the nitrogen oxides distributions toward higher levels, with medians of NOy (117–175 pptv) and NOx (9–30 pptv) greater in boreal wildfire plumes. These findings demonstrate the potential hemispheric scale impact that boreal wildfire and North American anthropogenic events have on background NOx and NOy levels and on the tropospheric O3 budget.

task with significant uncertainties in the methods used. In this work, we assess the impact of seasonal trends in fuel consumption and flaming/smoldering ratios on emissions of species dominated by flaming combustion (e.g., NOx) and species dominated by smoldering combustion (e.g., CO). This is accomplished using measurements of CO and NOy at the free tropospheric Pico Mountain observatory in the central North Atlantic during the active boreal fire seasons of 2004 and 2005. DNOy/DCO enhancement ratios in aged fire plumes had higher values in June-July (7.3 � 10 �3 mol mol �1 ) relative to the values in August-September (2.8 � 10 �3 mol mol � 1 ), indicating that NOx/CO emission ratios declined significantly as the fire season progressed. This is consistent with our understanding that an increased amount of fuel is consumed via smoldering combustion during late summer, as deeper burning of the drying organic soil layer occurs. A major growth in fuel consumption per unit area is also expected, due to deeper burning. Emissions of CO and NOx from North American boreal fires were estimated using the Boreal Wildland Fire Emissions Model, and their long-range transport to the sampling site was modeled using FLEXPART. These simulations were generally consistent with the observations, but the modeled seasonal decline in the DNOy/DCO enhancement ratio was less than observed. Comparisons using alternative fire emission injection height scenarios suggest that plumes with the highest CO levels at the observatory were lofted well above the boundary layer, likely as a result of intense crown fires.

[1] Upslope flows caused by mechanical forcing in strong synoptic winds or by buoyant forcing driven by solar heating under weak synoptic winds can influence the air composition at mountaintop observatories. Using meteorological and trace gas measurements at the PICO-NARE observatory on Pico mountain (Azores Islands, North Atlantic Ocean), the frequency and impact of such orographic flows on a small, volcanic, subtropical island was examined. To determine the origin of mechanically lifted air, upstream kinetic energy was balanced against potential energy gained during uplift (Sheppard's model). Mechanically forced upslope flow is most important during October through April, when the calculated probability of observing marine boundary layer (MBL) air at the observatory near the summit ranges from 35 to 60% per month. In contrast, lower synoptic wind speeds and a more stable lower free troposphere during May–September result in a reduced frequency of MBL impacts (

enhancements of CO, BC, NOy and NOx, with levels up to 250 ppbv, 665 ng m 3 , 1100 pptv and 135 pptv, respectively. Enhancement ratios relative to CO were variable in the plumes sampled, most likely because of variations in wildfire emissions and removalprocessesduringtransport.AnalysesofDBC/DCO,DNOy/DCOandDNOx/DCO ratios indicate that NOy and BC were on average efficiently exported in these plumes and suggest that decomposition of PAN to NOx was a significant source of NOx. High levels of NOx suggest continuing formation of O3 in these well-aged plumes. O3 levels were also significantly enhanced in the plumes, reaching up to 75 ppbv. Analysis of DO3/DCO ratios showed distinct behaviors of O3 in the plumes, which varied from significant to lower O3 production. We identify several potential reasons for the complex effects of boreal wildfire emissions on O3 and conclude that this behavior needs to be explored further in the future. These observations demonstrate that boreal wildfire emissions significantly contributed to the NOx and O3 budgets in the central North Atlantic lower free troposphere during summer 2004 and imply large-scale impacts on direct radiative forcing of the atmosphere and on tropospheric NOx and O3.

Summertime observations of O 3 and CO made at the PICO-NARE station during 2001, 2003, and 2004 are used to assess the impact of boreal forest fires on the distribution of O 3 mixing ratios in the midlatitude Northern Hemisphere (NH) lower free troposphere (FT). Backward trajectories were used to select measurements impacted by outflow from high-latitude regions. Measurements during these periods were segregated into two subsets: those obtained during periods with and without apparent significant upwind fire emissions. Periods affected by fire emissions were identified based on enhanced CO levels confirmed by global simulations of fire emissions transport. During fireimpacted periods, O 3 was shifted toward higher mixing ratios, with medians significantly higher than in periods without detectable upwind fire impacts. This implies a significant impact of boreal wildfires on midlatitude lower FT background O 3 during summer. Predicted future increases in boreal wildfires may therefore affect summertime O 3 levels over large regions.

[1] We report summertime measurements of CO and O3 obtained during 2001–2003 at the PICO-NARE mountaintop station in the Azores. Frequent events of elevated CO mixing ratios were observed. On the basis of backward trajectories arriving in the free troposphere and global simulations of biomass burning plumes, we attribute nearly all these events to North American pollution outflow and long-range transport of biomass burning emissions. There was a high degree of interannual variability in CO levels: median [CO] ranged from 65 ppbv in 2001 to 104 ppbv in 2003. The highest concentrations were associated with transport of Siberian fire emissions during summer 2003, when Siberian fire activity was unusually high. Ozone mixing ratios also increased (by up to ∼30 ppbv) during the fire events. These findings demonstrate the significant hemispheric scale impact that biomass burning events have on background CO and O3 levels. O3 enhancements of similar magnitude were also observed in North American pollution outflow. O3 and CO were correlated during North American outflow events, with a slope averaging 1.0 (d[O3]/d[CO], ppbv/ppbv) when no fire impact was present. This slope is more than 80% larger than early 1990s observations made in the eastern United States and nearshore outflow region, even after accounting for declining U.S. CO emissions and for CO loss during transport to the Azores, and is not consistent with simple dilution of U.S. outflow with marine background air. We conclude that a significantly larger amount of O3 production occurred in the air sampled during this study, and we suggest several potential reasons for this, each of which could imply potentially significant shortcomings in current estimates of the hemispheric impact of North American emissions on tropospheric ozone and should be evaluated in future studies.