Biomass Burning Season Research Articles

Data assimilation of satellite-retrieved ozone, carbon monoxide and nitrogen dioxide with ECMWF's Composition-IFS

Abstract. Daily global analyses and 5-day forecasts are generated in the context of the European Monitoring Atmospheric Composition and Climate (MACC) project using an extended version of the Integrated Forecasting System (IFS) of the European Centre for Medium-Range Weather Forecasts (ECMWF). The IFS now includes modules for chemistry, deposition and emission of reactive gases, aerosols, and greenhouse gases, and the 4-dimensional variational data assimilation scheme makes use of multiple satellite observations of atmospheric composition in addition to meteorological observations. This paper describes the data assimilation setup of the new Composition-IFS (C-IFS) with respect to reactive gases and validates analysis fields of ozone (O3), carbon monoxide (CO), and nitrogen dioxide (NO2) for the year 2008 against independent observations and a control run without data assimilation. The largest improvement in CO by assimilation of Measurements of Pollution in the Troposphere (MOPITT) CO columns is seen in the lower troposphere of the Northern Hemisphere (NH) extratropics during winter, and during the South African biomass-burning season. The assimilation of several O3 total column and stratospheric profile retrievals greatly improves the total column, stratospheric and upper tropospheric O3 analysis fields relative to the control run. The impact on lower tropospheric ozone, which comes from the residual of the total column and stratospheric profile O3 data, is smaller, but nevertheless there is some improvement particularly in the NH during winter and spring. The impact of the assimilation of tropospheric NO2 columns from the Ozone Monitoring Instrument (OMI) is small because of the short lifetime of NO2, suggesting that NO2 observations would be better used to adjust emissions instead of initial conditions. The results further indicate that the quality of the tropospheric analyses and of the stratospheric ozone analysis obtained with the C-IFS system has improved compared to the previous "coupled" model system of MACC.

Spatial and temporal variation in CO over Alberta using measurements from satellites, aircraft, and ground stations

Abstract. Alberta is Canada's largest oil producer, and its oil sands deposits comprise 30% of the world's oil reserves. The process of bitumen extraction and upgrading releases trace gases and aerosols to the atmosphere. In this study we present satellite-based analysis to explore, for the first time, various contributing factors that affect tropospheric carbon monoxide (CO) levels over Alberta. The multispectral product that uses both near-infrared (NIR) and the thermal-infrared (TIR) radiances for CO retrieval from the Measurements of Pollution in the Troposphere (MOPITT) is examined for the 12-year period from 2002 to 2013. The Moderate Resolution Imaging Spectroradiometer (MODIS) thermal anomaly product from 2001 to 2013 is employed to investigate the seasonal and temporal variations in forest fires. Additionally, in situ CO measurements at industrial and urban sites are compared to satellite data. Furthermore, the available MOZAIC/IAGOS (Measurement of Ozone, Water Vapor, Carbon Monoxide, Nitrogen Oxide by Airbus In-Service Aircraft/In service Aircraft for Global Observing System) aircraft CO profiles (April 2009–December 2011) are used to validate MOPITT CO data. The climatological time curtain plot and spatial maps for CO over northern Alberta indicate the signatures of transported CO for two distinct biomass burning seasons: summer and spring. Distinct seasonal patterns of CO at the urban sites (Edmonton and Calgary) point to the strong influence of traffic. Meteorological parameters play an important role in the CO spatial distribution at various pressure levels. Northern Alberta shows a stronger upward lifting motion which leads to larger CO total column values, while the poor dispersion in central and southern Alberta exacerbates the surface CO pollution. Interannual variations in satellite data depict a slightly decreasing trend for both regions, while the decline trend is more evident from ground observations, especially at the urban sites. MOPITT CO vertical averages and MOZAIC/IAGOS aircraft profiles were in good agreement within the standard deviations at all pressure levels. There is consistency between the time evolution of high-CO episodes monitored by satellite and ground measurements and the fire frequency peak time, which implies that biomass burning has affected the tropospheric CO distribution in northern Alberta. These findings have further demonstrated the potential use of the MOPITT V5 multispectral (NIR + TIR) product for assessing a complicated surface process.

Where Aerosols Become Clouds—Potential for Global Analysis Based on CALIPSO Data

This study evaluates the potential to determine the global distribution of hydrated aerosols based on Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) data products. Knowledge of hydrated aerosol global distribution is of high relevance in the study of the radiative impact of aerosol-cloud interactions on Earth’s climate. The cloud-aerosol discrimination (CAD) score of the Cloud-Aerosol LIdar with Orthogonal Polarization (CALIOP) instrument on the CALIPSO satellite separates aerosols and clouds according to the probability density functions (PDFs) of attenuated backscatter, total color ratio, volume depolarization ratio, altitude and latitude. The pixels that CAD fails to identify as either cloud or aerosol are used here to pinpoint the occurrence of hydrated aerosols and to globally quantify their relative frequency using data of August from 2006 to 2013. Atmospheric features in this no-confidence range mostly match with aerosol PDFs and imply an early hydration state of aerosols. Their strong occurrence during August above the South-East Atlantic and below an altitude of 4 km coincides with the biomass burning season in southern Africa and South America.

Biomass burning related ozone damage on vegetation over the Amazon forest: a model sensitivity study

Abstract. The HadGEM2 earth system climate model was used to assess the impact of biomass burning on surface ozone concentrations over the Amazon forest and its impact on vegetation, under present-day climate conditions. Here we consider biomass burning emissions from wildfires, deforestation fires, agricultural forest burning, and residential and commercial combustion. Simulated surface ozone concentration is evaluated against observations taken at two sites in the Brazilian Amazon forest for years 2010 to 2012. The model is able to reproduce the observed diurnal cycle of surface ozone mixing ratio at the two sites, but overestimates the magnitude of the monthly averaged hourly measurements by 5–15 ppb for each available month at one of the sites. We vary biomass burning emissions over South America by ±20, 40, 60, 80 and 100% to quantify the modelled impact of biomass burning on surface ozone concentrations and ozone damage on vegetation productivity over the Amazon forest. We used the ozone damage scheme in the "high" sensitivity mode to give an upper limit for this effect. Decreasing South American biomass burning emissions by 100% (i.e. to zero) reduces surface ozone concentrations (by about 15 ppb during the biomass burning season) and suggests a 15% increase in monthly mean net primary productivity averaged over the Amazon forest, with local increases up to 60%. The simulated impact of ozone damage from present-day biomass burning on vegetation productivity is about 230 TgC yr−1. Taking into account that uncertainty in these estimates is substantial, this ozone damage impact over the Amazon forest is of the same order of magnitude as the release of carbon dioxide due to fire in South America; in effect it potentially doubles the impact of biomass burning on the carbon cycle.

Influence of biomass burning plumes on HONO chemistry in eastern China

Abstract. Nitrous acid (HONO) plays a key role in atmospheric chemistry by influencing the budget of hydroxyl radical (OH). In this study, a two-month measurement of HONO and related quantities were analyzed during a biomass burning season in 2012 at a suburban site in the western Yangtze River delta, eastern China. An overall high HONO concentration with the mean value of 0.76 ppbv (0.01 ppbv to 5.95 ppbv) was observed. During biomass burning (BB) periods, both HONO concentration and HONO/NO2 ratio were enhanced significantly (more than a factor of 2, p < 0.01) compared with non-biomass burning (non-BB) periods. A correlation analysis showed that the HONO in BB plumes was more correlated with nitrogen dioxide (NO2) than that with potassium (a tracer of BB). Estimation by the method of potassium tracing suggests a maximum contribution of 17 ± 12% from BB emission to the observed HONO concentrations, and the other over 80% of the observed nighttime HONO concentrations during BB periods were secondarily produced by the heterogeneous conversion of NO2. The NO2-to-HONO conversion rate (CHONO) in BB plumes was almost twice as that in non-BB plumes (0.0062 hr−1 vs. 0.0032 hr−1). Given that the residence time of the BB air masses was lower than that of non-BB air masses, these results suggest BB aerosols have higher NO2 conversion potentials to form HONO than non-BB aerosols. A further analysis based on comparing the surface area at similar particle mass levels and HONO/NO2 ratios at similar surface area levels suggested larger specific surface areas and higher NO2 conversion efficiencies of BB aerosols. A mixed plume of BB and anthropogenic fossil fuel (FF) emissions was observed on 10 June with even higher HONO concentrations and HONO/NO2 ratios. The strong HONO production potential (high HONO/NO2 to PM2.5 ratio) was accompanied with a high sulfate concentration in this plume, suggesting a promotion of mixed aerosols to the HONO formation. In summary, our study suggests an important role of BB in atmospheric chemistry by affecting the HONO budget. This can be especially important in eastern China, where agricultural burning plumes are inevitably mixed with urban and industrial pollution.

Seasonal and interannual variations in HCN amounts in the upper troposphere and lower stratosphere observed by MIPAS

Abstract. We present a HCN climatology of the years 2002–2012, derived from FTIR limb emission spectra measured with the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) on the ENVISAT satellite, with the main focus on biomass burning signatures in the upper troposphere and lower stratosphere. HCN is an almost unambiguous tracer of biomass burning with a tropospheric lifetime of 5–6 months and a stratospheric lifetime of about 2 years. The MIPAS climatology is in good agreement with the HCN distribution obtained by the spaceborne ACE-FTS experiment and with airborne in situ measurements performed during the INTEX-B campaign. The HCN amounts observed by MIPAS in the southern tropical and subtropical upper troposphere have an annual cycle peaking in October–November, i.e. 1–2 months after the maximum of southern hemispheric fire emissions. The probable reason for the time shift is the delayed onset of deep convection towards austral summer. Because of overlap of varying biomass burning emissions from South America and southern Africa with sporadically strong contributions from Indonesia, the size and strength of the southern hemispheric plume have considerable interannual variations, with monthly mean maxima at, for example, 14 km between 400 and more than 700 pptv. Within 1–2 months after appearance of the plume, a considerable portion of the enhanced HCN is transported southward to as far as Antarctic latitudes. The fundamental period of HCN variability in the northern upper troposphere is also an annual cycle with varying amplitude, which in the tropics peaks in May after and during the biomass burning seasons in northern tropical Africa and southern Asia, and in the subtropics peaks in July due to trapping of pollutants in the Asian monsoon anticyclone (AMA). However, caused by extensive biomass burning in Indonesia and by northward transport of part of the southern hemispheric plume, northern HCN maxima also occur around October/November in several years, which leads to semi-annual cycles. There is also a temporal shift between enhanced HCN in northern low and mid- to high latitudes, indicating northward transport of pollutants. Due to additional biomass burning at mid- and high latitudes, this meridional transport pattern is not as clear as in the Southern Hemisphere. Upper tropospheric HCN volume mixing ratios (VMRs) above the tropical oceans decrease to below 200 pptv, presumably caused by ocean uptake, especially during boreal winter and spring. The tropical stratospheric tape recorder signal with an apparently biennial period, which was detected in MLS and ACE-FTS data from mid-2004 to mid-2007, is corroborated by MIPAS HCN data. The tape recorder signal in the whole MIPAS data set exhibits periodicities of 2 and 4 years, which are generated by interannual variations in biomass burning. The positive anomalies of the years 2003, 2007 and 2011 are caused by succession of strongly enhanced HCN from southern hemispheric and Indonesian biomass burning in boreal autumn and of elevated HCN from northern tropical Africa and the AMA in subsequent spring and summer. The anomaly of 2005 seems to be due to springtime emissions from tropical Africa followed by release from the summertime AMA. The vertical transport time of the anomalies is 1 month or less between 14 and 17 km in the upper troposphere and 8–11 months between 17 and 25 km in the lower stratosphere.

Seasonal and spatial variations of global aerosol optical depth: multi-year modelling with GEOS-Chem-APM and comparisons with multiple-platform observations

Recent AeroCom phase II experiments showed a large diversity in aerosol optical depth (AOD) among 16 detailed global aerosol models, which contributes to the large uncertainty in the predicted aerosol radiative forcing. The GEOS-Chem-APM, a global size-resolved aerosol model, can be considered as a representative AeroCom II model. In this study, multi-year AOD data (2004–2012) from ground-based Aerosol Robotic Network (AERONET) measurements and Moderate Resolution Imaging Spectroradiometer (MODIS), Multi-angle Imaging SpectroRadiometer (MISR) and Sea-viewing Wide Field-of-view Sensor (SeaWiFS) satellite retrievals are used to evaluate the performance of GEOS-Chem-APM in capturing observed seasonal and spatial AOD variations. Compared to the observations, the modelled AOD is overall good over land, but quite low over ocean possibly due to low sea salt emission in the model and/or higher AOD in satellite retrievals, specifically MODIS and MISR. We chose 72 AERONET sites having at least 36 months data available and representative of high spatial domain to compare with the model and satellite data. Comparisons in various representative regions show that the model overall agrees well in the major anthropogenic emission regions, such as Europe, East Asia and North America. Relative to the observations, the modelled AOD is systematically lower in biomass burning regions such as South Africa and South America possibly due to uncertainties in emission inventory, but slightly higher in North Africa likely associated with stronger dust emissions in the model. The model is able to capture the realistic seasonal cycle in all regions, including the peak of AOD in major dust events months and biomass burning seasons. The simulated inter-annual variability is overall consistent with the observations, which is distinctly shown in South Africa and South America with strong inter-annual variability compared to other regions.

Airborne verification of CALIPSO products over the Amazon: a case study of daytime observations in a complex atmospheric scene

Abstract. A daytime underflight of CALIPSO with the Facility for Airborne Atmospheric Measurements was performed on 20 September 2012 in the Amazon region of Brazil, during the biomass burning season. The scene is dominated by a thin elevated layer (aerosol optical depth (AOD) 0.03 at 532 nm) and a moderately turbid boundary layer (AOD ~ 0.2 at 532 nm). The boundary layer is topped with small broken stratocumulus clouds. In this complex scene, a comparison of observations from the airborne and spaceborne lidars reveals a few discrepancies. The CALIPSO detection scheme tends to miss the elevated thin layer, and also shows several gaps (~ 30%) in the boundary layer. The small clouds are not correctly removed from the signals; this can cause the CALIPSO aerosol subtype to oscillate between smoke and polluted dust and may introduce distortion in the aerosol retrieval scheme. The magnitude of the average extinction coefficient estimated from CALIPSO Level 2 data in the boundary layer is as expected, when compared to the aircraft lidar and accounting for wavelength scaling. However, when the gaps in aerosol detection mentioned above are accounted for, we are left with an overall estimate of AOD for this particular scene that is of the order of two thirds of that determined with the airborne lidar.

A 2-year record of atmospheric mercury species at a background Southern Hemisphere station on Amsterdam Island

Abstract. Although essential to fully understand the cycling of mercury at the global scale, mercury species records in the Southern Hemisphere are scarce. Under the framework of the Global Mercury Observation System (GMOS) project, a monitoring station has been set up on Amsterdam Island (37°48´ S, 77°34´ E) in the remote southern Indian Ocean. For the first time in the Southern Hemisphere, a 2-year record of gaseous elemental mercury (GEM), reactive gaseous mercury (RGM) and particle-bound mercury (PBM) is presented. GEM concentrations were remarkably steady (1.03 ± 0.08 ng m−3) while RGM and PBM concentrations were very low and exhibited a strong variability (mean: 0.34 pg m−3, range: < detection limit–4.07 pg m−3; and mean: 0.67 pg m−3, range: < detection limit–12.67 pg m−3, respectively). Despite the remoteness of the island, wind sector analysis, air mass back trajectories and the observation of radonic storms highlighted a long-range contribution from the southern African continent to the GEM and PBM budgets from July to September during the biomass burning season. Low concentrations of GEM were associated with southerly polar and marine air masses from the remote southern Indian Ocean. This unique data set provides new baseline GEM concentrations in the Southern Hemisphere midlatitudes while mercury speciation along with upcoming wet deposition data will help to improve our understanding of the mercury cycle in the marine boundary layer.

Variability in aerosol optical properties and radiative forcing over Gorongosa (18.97oS, 34.35oE) in Mozambique

This paper reports the observational results of aerosol optical, microphysical and radiative characteristics for the time measured over Gorongosa (18.97oS, 34.35oE, 30 m asl) in Mozambique using a ground-based AERONET sun-sky radiometer. In the present study, the data recorded during the period July–December, 2012 have been used and particular attention was paid to show how aerosol loading evolves during the biomass burning season (spring) including pre- and post-months. The results reveal that the monthly mean aerosol optical depth (AOD) at 500 nm was high (low) with 0.64 ± 0.34 (0.20 ± 0.06) in September (November), while the Angstrom Exponent (AE) (α 440–870) decreased, except September (1.56 ± 0.26) due to increase in the fine-mode aerosol concentration produced from biomass burning. The volume size distribution (VSD) has bimodal lognormal structure and has fine-mode (coarse) maximum at a radius of 0.15 µm (3.0 µm) in September (December). The single scattering albedo (SSA) decreases with wavelength from July to October and almost stable in November and December. The imaginary (Im) refractive index (RI) showed a strong evidence of black carbon aerosol origin during the biomass burning months. Aerosol radiative forcing (ARF) computed from SBDART model shows large negative values at the surface (−89.22 W m−2) and at the top (−22.36 W m−2), with a higher value of atmospheric forcing (+66.87 W m−2) resulting in average tropospheric heating rate of 1.88 K day−1 for the study period. Further, the comparison shows good agreement between the ARFs at the top and bottom of the atmosphere derived from AERONET to SBDART.

Boundary layer regulation in the southeast Atlantic cloud microphysics during the biomass burning season as seen by the A‐train satellite constellation

AbstractSolar radiation absorption by biomass burning aerosols has a strong warming effect over the southeast Atlantic. Interactions between the overlying smoke aerosols and low‐level cloud microphysics and the subsequent albedo perturbation are, however, generally ignored in biomass burning radiative assessments. In this study, Cloud‐Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) are combined with Aqua satellite observations from Moderate Resolution Imaging Spectroradiometer (MODIS), Advanced Microwave Scanning Radiometer–EOS (AMSR‐E), and Clouds and the Earth's Radiant Energy System (CERES) to assess the effect of variations in the boundary layer height and the separation distance between the cloud and aerosol layers on the cloud microphysics. The merged data analyzed at a daily temporal resolution suggest that overlying smoke aerosols modify cloud properties by decreasing cloud droplet size despite an increase in the cloud liquid water as boundary layer deepens, north of 5°S. These changes are controlled by the proximity of the aerosol layer to the cloud top rather than increases in the column aerosol load. The correlations are unlikely driven by meteorological factors, as three predictors of cloud variability, lower tropospheric stability, surface winds, and mixing ratio suggest that cloud effective radius, cloud top height, and liquid water path should correlate positively. Because cloud effective radius anticorrelates with cloud liquid water over the region with large microphysical changes—north of 5°S—the overall radiative consequence at the top of the atmosphere is a strong albedo susceptibility, equivalent to a 3% albedo increase due to a 10% decrease in cloud effective radius. This albedo enhancement partially offsets the aerosol solar absorption. Our analysis emphasizes the importance of accounting for the indirect effect of smoke aerosols in the cloud microphysics when estimating the radiative impact of the biomass burning at the top of the atmosphere.

EOF와 SVD을 이용한 아프리카 지역에서 관측된 OMI HCHO 자료의 검증

We have found an error in the operational OMI HCHO columns, and corrected it by applying a background parameterization derived on a 4th order polynomial fit to the time series of monthly average OMI HCHO data. The corrected OMI HCHO agrees with this understanding as well as with the other sensors measurements and has no unrealistic trends. A new scientific approach, statistical analyses with EOF and SVD, was adapted to reanalyze the consistency of the corrected OMI HCHO with other satellite measurements of HCHO, CO, NO 2 , and fire counts over Africa. The EOF and SVD analyses with MOPITT CO, OMI NO 2 , SCIAMAHCY, and OMI HCHO show the overall spatial and temporal pattern consistent with those of biomass burning over these regions. However, some discrepancies were observed from OMI HCHO over northern equatorial Africa during the northern biomass burning seasons: The maximum HCHO was found further downwind from where maximum fire counts occur and the minimum was found in January when biomass burning is strongest. The statistical analysis revealed that the influence of biogenic activity on HCHO wasn’t strong enough to cause the discrepancies, but it is caused by the error in OMI HCHO from using the wrong Air Mass Factor (AMF) associated with biomass burning aerosol. If the error is properly taken into consideration, the biomass burning is the strongest source of HCHO seasonality over the regions. This study suggested that the statistical tools are a very efficient method for evaluating satellite data.

Sensitivity of mesoscale modeling of smoke direct radiative effect to the emission inventory: a case study in northern sub-Saharan African region

An ensemble approach is used to examine the sensitivity of smoke loading and smoke direct radiative effect in the atmosphere to uncertainties in smoke emission estimates. Seven different fire emission inventories are applied independently to WRF-Chem model (v3.5) with the same model configuration (excluding dust and other emission sources) over the northern sub-Saharan African (NSSA) biomass-burning region. Results for November and February 2010 are analyzed, respectively representing the start and end of the biomass burning season in the study region. For February 2010, estimates of total smoke emission vary by a factor of 12, but only differences by factors of 7 or less are found in the simulated regional (15°W–42°E, 13°S–17°N) and monthly averages of column PM2.5 loading, surface PM2.5 concentration, aerosol optical depth (AOD), smoke radiative forcing at the top-of-atmosphere and at the surface, and air temperature at 2 m and at 700 hPa. The smaller differences in these simulated variables may reflect the atmospheric diffusion and deposition effects to dampen the large difference in smoke emissions that are highly concentrated in areas much smaller than the regional domain of the study. Indeed, at the local scale, large differences (up to a factor of 33) persist in simulated smoke-related variables and radiative effects including semi-direct effect. Similar results are also found for November 2010, despite differences in meteorology and fire activity. Hence, biomass burning emission uncertainties have a large influence on the reliability of model simulations of atmospheric aerosol loading, transport, and radiative impacts, and this influence is largest at local and hourly-to-daily scales. Accurate quantification of smoke effects on regional climate and air quality requires further reduction of emission uncertainties, particularly for regions of high fire concentrations such as NSSA.

Impacts of fire emissions and transport pathways on the interannual variation of CO in the tropical upper troposphere

Abstract. This study investigates the impacts of fire emission, convection, various climate conditions and transport pathways on the interannual variation of carbon monoxide (CO) in the tropical upper troposphere (UT), by evaluating the field correlation between these fields using multi-satellite observations and principle component analysis, and the transport pathway auto-identification method developed in our previous study. The rotated empirical orthogonal function (REOF) and singular value decomposition (SVD) methods are used to identify the dominant modes of CO interannual variation in the tropical UT and to study the coupled relationship between UT CO and its governing factors. Both REOF and SVD results confirm that Indonesia is the most significant land region that affects the interannual variation of CO in the tropical UT, and El Niño–Southern Oscillation (ENSO) is the dominant climate condition that affects the relationships between surface CO emission, convection and UT CO. In addition, our results also show that the impact of El Niño on the anomalous CO pattern in the tropical UT varies strongly, primarily due to different anomalous emission and convection patterns associated with different El Niño events. In contrast, the anomalous CO pattern in the tropical UT during La Niña period appears to be less variable among different events. Transport pathway analysis suggests that the average CO transported by the "local convection" pathway (ΔCOlocal) accounts for the differences of UT CO between different ENSO phases over the tropical continents during biomass burning season. ΔCOlocal is generally higher over Indonesia–Australia and lower over South America during El Niño years than during La Niña years. The other pathway ("advection within the lower troposphere followed by convective vertical transport") occurs more frequently over the west-central Pacific during El Niño years than during La Niña years, which may account for the UT CO differences over this region between different ENSO phases.

Long-term in situ observations of biomass burning aerosol at a high altitude station in Venezuela – sources, impacts and interannual variability

Abstract. First long-term observations of South American biomass burning aerosol within the tropical lower free troposphere are presented. The observations were conducted between 2007 and 2009 at a high altitude station (4765 m a.s.l.) on the Pico Espejo, Venezuela. Sub-micron particle volume, number concentrations of primary particles and particle absorption were observed. Orographic lifting and shallow convection leads to a distinct diurnal cycle at the station. It enables measurements within the lower free troposphere during night-time and observations of boundary layer air masses during daytime and at their transitional regions. The seasonal cycle is defined by a wet rainy season and a dry biomass burning season. The particle load of biomass burning aerosol is dominated by fires in the Venezuelan savannah. Increases of aerosol concentrations could not be linked to long-range transport of biomass burning plumes from the Amazon basin or Africa due to effective wet scavenging of particles. Highest particle concentrations were observed within boundary layer air masses during the dry season. Ambient sub-micron particle volume reached 1.4±1.3 μm3 cm−3, refractory particle number concentrations (at 300 °C) 510±420 cm−3 and the absorption coefficient 0.91±1.2 Mm−1. The respective concentrations were lowest within the lower free troposphere during the wet season and averaged at 0.19±0.25 μm3 cm−3, 150±94 cm−3 and 0.15±0.26 Mm−1. A decrease of particle concentrations during the dry seasons from 2007–2009 could be connected to a decrease in fire activity in the wider region of Venezuela using MODIS satellite observations. The variability of biomass burning is most likely linked to the El Niño–Southern Oscillation (ENSO). Low biomass burning activity in the Venezuelan savannah was observed to follow La Niña conditions, high biomass burning activity followed El Niño conditions.

Assessment of smoke shortwave radiative forcing using empirical angular distribution models

The Clouds and the Earth's Radiant Energy System (CERES) data has been used by several studies to calculate the top of atmosphere (TOA) shortwave aerosol radiative forcing (SWARF) of biomass burning aerosols over land. However, the current CERES angular distribution models that are used to convert measured TOA radiances to fluxes are not characterized by aerosols. Using our newly developed empirical angular models for smoke aerosols we calculate the SWARF over South America for eight years (2000–2008) during the biomass burning season. Our results indicate that when compared to our new angular distribution model-derived values, the instantaneous SWARF is underestimated by the CERES data by nearly 3.3Wm−2. Our studies indicate that it is feasible to develop angular models using empirical methods that can then be used to reduce uncertainties in aerosol radiative forcing calculations. More importantly, empirically-based methods for calculating radiative forcing can serve as a benchmark for modeling studies.

Long-term analysis of NO2, CO, and AOD seasonal variability using satellite observations over Asia and intercomparison with emission inventories and model

Long-term analysis of tropospheric nitrogen dioxide (NO2) columns retrieved from GOME, SCIAMACHY, OMI and GOME-2 satellites, carbon monoxide (CO) columns from MOPITT satellite, and aerosol optical depths (AODs) from MODIS satellite was performed for Southeast Asian countries including Japan and China during 1996–2012. The results show that significant increasing levels of tropospheric NO2 columns can be clearly observed during the study period, especially above the eastern regions of China. The cities located in different latitude zones present the seasonal cycle of NO2 columns, CO columns, and AODs differently. For the cities located around mid-latitude zone, the maximum levels of NO2 and CO columns can be observed in the winter (November–March) and the minimum in the summer (June–September). On the contrary, the maximum levels for the cities near Equator zone are revealed in dry season (June–October). In the case of AODs, the maximum peaks normally occur during biomass burning season. Ground monitoring concentrations of NO2, CO, and PM10 were also comparably analyzed with satellite NO2 columns, CO columns, and AODs, respectively. Anthropogenic and biomass burning emissions were derived to investigate the consistency with satellite retrievals. The results show that satellite observations are able to capture the trend and seasonal variability of the emissions and ground concentrations. The model simulations were conducted using CMAQ model. Generally, simulated model results agree well with those retrieved from satellite measurements for spatial distribution and seasonal pattern. However, the modeled results underestimate satellite data probably due to the inaccuracy in emission inventories, the inaccuracy of spatial and temporal allocations, and the uncertainties in the satellite retrievals.

Free troposphere as a major source of CCN for the equatorial pacific boundary layer: long-range transport and teleconnections

Abstract. Airborne aerosol measurements in the central equatorial Pacific during PASE (Pacific Atmospheric Sulfur Experiment) revealed that cloud condensation nuclei (CCN) activated in marine boundary layer (MBL) clouds were strongly influenced by entrainment from the free troposphere (FT). About 65% entered at sizes effective as CCN in MBL clouds, while ~25% entered the MBL too small to activate but subsequently grew via gas to particle conversion. The remaining ~10% were inferred to be sea salt aerosol. FT aerosols at low carbon monoxide (CO) mixing ratios (< 63 ppbv) were mostly volatile at 360 °C with a number mode peak of around 30–40 nm dry diameter and tended to be associated with cloud outflow from distant (3000 km or more) deep convection. Higher CO concentrations were commonly associated with trajectories from South America and the Amazon region (ca. ~10 000 km away) and occurred in layers indicative of combustion sources (biomass burning season) partially scavenged by precipitation. These had number modes near 60–80 nm dry diameter with a large fraction of CCN.2 (those activated at 0.2% supersaturation and representative of MBL clouds) prior to entrainment into the MBL. Flight averaged concentrations of CCN.2 were similar for measurements near the surface, below the inversion and in the FT just above the inversion, confirming that subsidence and entrainment of FT aerosol strongly influenced MBL CCN.2. Concurrent flight-to-flight variations of CCN.2 at all altitudes below 3 km also imply MBL CCN.2 concentrations were in quasi-equilibrium with the FT over a 2–3 day timescale. The observed FT transport over thousands of kilometers indicates teleconnections between MBL CCN and cloud-scavenged sources of both natural and/or residual combustion origin. Nonetheless, in spite of its importance, this source of CCN number is not well represented in most current models and is generally not detectable by satellite because of the low aerosol scattering in such layers as a result of cloud scavenging. In addition, our measurements confirm nucleation in the MBL was not evident during PASE and argue against a localized linear relation in the MBL between dimethyl sulfide (DMS) and CCN suggested by the CLAW hypothesis. However, when the FT is not impacted by long-range transport, sulfate aerosol derived from DMS pumped aloft in the ITCZ (Inter-Tropical Convergence Zone) can provide a source of CCN to the boundary layer via FT teleconnections involving more complex non-linear processes.

Short term variability of aerosol optical thickness at Belsk for the period 2002–2010

In this work variability of aerosol optical thickness (AOT) measured at Belsk, Poland is studied as well as modification of AOT during airmass advection towards Belsk. AOT measurements taken at Belsk and at AERONET stations located in eastern Germany, Belarus and Scandinavia are used as well as satellite measurements of AOT taken by MODIS instrument onboard Terra and Aqua satellites. Directions of airmass advection are determined by means of cluster analysis of airmass backward-trajectories.Changes of AOT at Belsk from day to day varies around zero regardless of time lag between measurements. The standard deviation of these measurements increases with increasing time lag. In case of advection from west and north direction such standard deviation is reduced. It gives good perspective for a persistent forecast of next day AOT.Analysis of AOT changes during airmass advection toward Belsk reveals two modes of AOT changes distributions. One of them with small increase of AOT and second one with larger increase of AOT, so-called loading mode. Loading mode dominates in case of advection from south direction whilst the first mode of AOT changes dominates in case of advection from other directions. Mean increase of AOT associated with the first mode is 0.034 ± 0.003. Analysis of backward-trajectories shows that aerosol loading occurs over urban/industrial regions located south and south-west of Belsk. Substantial aerosol loading is found during seasonal biomass burning episodes in Eastern Europe.

Aerosol particle vertical distributions and optical properties over Singapore

As part of the Seven Southeast Asian Studies (7SEAS) program, an Aerosol Robotic Network (AERONET) sun photometer and a Micro-Pulse Lidar Network (MPLNET) instrument have been deployed at Singapore to study the regional aerosol environment of the Maritime Continent (MC). Using coincident AERONET Level 2.0 and MPLNET Level 2.0a data from 24 September 2009 to 31 March 2011, the seasonal variability of aerosol particle vertical distributions and optical properties is examined. On average, the bulk (∼65%) of aerosol extinction is found below 1.5 km with substantial aerosol loading (∼35%) above. Possibly due to the transition from El Niño to La Niña conditions and subsequent reduction in fire events, the MPLNET mean integrated aerosol extinction is observed to be the lowest for July–September 2010, which coincides with the typical MC biomass burning season. On the other hand, the highest mean integrated extinctions are derived for January–March 2010 and 2011, which can be attributed to off-season MC biomass burning smoke and anthropogenic pollution. The seasonal lidar ratios also show higher occurrences ≥60 sr, which are indicative of biomass burning smoke, for October 2009–June 2010, but such occurrences decrease from July 2010 to March 2011 when La Niña conditions prevail. In addition, principal component analysis (PCA) identifies five primary aerosol vertical profile types over Singapore, i.e. strongly-capped/deep near-surface layer (SCD; 0–1.35 km), enhanced mid-level layer (EML; 1.35–2.4 km), enhanced upper-level layer (EUL; 2.4–3.525 km), deep contiguous layer (DCL; 3.525–4.95 km) and deep multi-layer (DML; >4.95 km). PCA also identifies an off-season MC biomass burning smoke event from 22 February to 8 March 2010, which is subsequently examined in detail.