AN APPROACH TO ESTIMATE GLOBAL BIOMASS BURNING EMISSIONS OF ORGANIC AND BLACK CARBON FROM MODIS FIRE RADIATIVE POWER

Biomass burning is an important global phenomenon affecting atmospheric composition with significant implications for climatic forcing. Wildland fire is the main global source of fine primary carbonaceous aerosols in the form of organic carbon (OC) and black carbon (BC), but uncertainty in aerosol emission estimates from biomass burning is still rather large. Application of satellite based measures of fire radiative power (FRP) has been demonstrated to offer an alternative approach to estimate biomass consumed with the potential to estimate the associated emissions from fires. To date, though, no study has derived integrated FRP (referred to as fire radiative energy or FRE) at a global scale, in part due to limitations in temporal or spatial resolution of satellite sensors. The main objective of this research was to quantify global biomass burning emissions of organic and black carbon aerosols and the corresponding effect on planetary radiative forcing. The approach is based on the geophysical relationship between the flux of FRE emitted, biomass consumed, and aerosol emissions. Aqua and Terra MODIS observations were used to estimate FRE using a simple model to parameterize the fire diurnal cycle based on the long term ratio between Terra and Aqua MODIS FRP and cases of diurnal satellite measurements of FRP made by the geostationary sensor SEVIRI, precessing sensor VIRS, and high latitude (and thus high overpass frequency) observations by MODIS. Investigation of the atmospheric attenuation of MODIS channels using a parametric model based on the MODTRAN radiative transfer model indicates a small bias in FRE estimates which was accounted for. Accuracy assessment shows that the FRE estimates are precise (R2 = 0.85), but may be underestimated. Global estimates of FRE show that Africa and South America dominate biomass burning, accounting for nearly 70% of the annual FRE generated. The relationship between FRE and OCBC estimates made with a new MODIS-derived inversion product of daily integrated biomass burning aerosol emissions was explored. The slope of the relationship within each of several biomes yielded a FRE-based emission factor. The biome specific emission factors and FRE monthly data were used to estimate OCBC emissions from fires on a global basis for 2001 to 2007. The annual average was 17.23 Tg which was comparable to previously published values, but slightly lower. The result in terms of global radiative forcing suggests a cooling effect at both the top-of-atmosphere (TOA) and surface approaching almost -0.5 K which implies that biomass burning aerosols could dampen the warming effect of green house gas emissions. An error budget was developed to explore the sources and total uncertainty in the OCBC estimation. The results yielded an uncertainty value of 58% with specific components of the process warranting future consideration and improvement. The uncertainty estimate does not demonstrate a significant improvement over current methods to estimate biomass burning aerosols, but given the simplicity of the approach should allow for refinements to be made with relative ease

Aerosol Remote Sensing in Polar Regions

Multi-year sets of ground-based sun-photometer measurements conducted at 12 Arctic sites and 9 Antarctic sites were examined to determine daily mean values of aerosol optical thickness tau(lambda) at visible and near-infrared wavelengths, from which best-fit values of ngstrm's exponent alpha were calculated. Analyzing these data, the monthly mean values of tau(0.50 micrometers) and alpha and the relative frequency histograms of the daily mean values of both parameters were determined for winter-spring and summer-autumn in the Arctic and for austral summer in Antarctica. The Arctic and Antarctic covariance plots of the seasonal median values of alpha versus tau(0.50 micrometers) showed: (i) a considerable increase in tau(0.50 micrometers) for the Arctic aerosol from summer to winter-spring, without marked changes in alpha; and (ii) a marked increase in tau(0.50 micrometer) passing from the Antarctic Plateau to coastal sites, whereas alpha decreased considerably due to the larger fraction of sea-salt aerosol. Good agreement was found when comparing ground-based sun-photometer measurements of tau(lambda) and alpha at Arctic and Antarctic coastal sites with Microtops measurements conducted during numerous AERONET/MAN cruises from 2006 to 2013 in three Arctic Ocean sectors and in coastal and off-shore regions of the Southern Atlantic, Pacific, and Indian Oceans, and the Antarctic Peninsula. Lidar measurements were also examined to characterize vertical profiles of the aerosol backscattering coefficient measured throughout the year at Ny-lesund. Satellite-based MODIS, MISR, and AATSR retrievals of tau(lambda) over large parts of the oceanic polar regions during spring and summer were in close agreement with ship-borne and coastal ground-based sun-photometer measurements. An overview of the chemical composition of mode particles is also presented, based on in-situ measurements at Arctic and Antarctic sites. Fourteen log-normal aerosol number size-distributions were defined to represent the average features of nuclei, accumulation and coarse mode particles for Arctic haze, summer background aerosol, Asian dust and boreal forest fire smoke, and for various background austral summer aerosol types at coastal and high-altitude Antarctic sites. The main columnar aerosol optical characteristics were determined for all 14 particle modes, based on in-situ measurements of the scattering and absorption coefficients. Diurnally averaged direct aerosol-induced radiative forcing and efficiency were calculated for a set of multimodal aerosol extinction models, using various Bidirectional Reflectance Distribution Function models over vegetation-covered, oceanic and snow-covered surfaces. These gave a reliable measure of the pronounced effects of aerosols on the radiation balance of the surface-atmosphere system over polar regions

Characterizing North American biomass burning layers in the free troposphere with a single particle soot photometer

Waldbrände sind eine Hauptquelle von Ruß, der schwarzen Kohlenstoff enthält, den am stärksten absorbierendem Partikeltyp in der Atmosphäre. Durch Vertikaltransport können Waldbrandaerosolschichten die obere Troposphäre erreichen, was ihre Klimawirkung noch verstärken kann, da die Lebenszeit von Aerosolpartikeln in der Atmosphäre mit der Höhe zunimmt. Diese Arbeit befasst sich mit der Charakterisierung von schwarzem Ruß in Waldbrandaerosolschichten in der freien und oberen Troposphäre anhand von Messdaten, die 2012 bei der Deep Convective Clouds and Chemistry (DC3) Flugzeugmesskampagne mit einem SP2 gewonnen wurden. Die Rußpartikel, die in diesen in Waldbrandaerosolschichten gemessen wurden, unterscheiden sich zwischen Schichten in unterschiedlichen Höhen. Anhand einer Fallstudie vom 11. Juni 2012, bei der Rußmassenkonzentrationen von bis zu 2 µg /m³ gemessen wurden, werden Waldbrandaerosolschichten in der freien Troposphäre unterhalb von etwa 8 km Höhe exemplarisch dargestellt. Diese Schichten enthalten Rußpartikel mit einem Massenmediandurchmesser von 160-200 nm, etwa 60-80% dieser Rußpartikel weisen dicke Ummantelungen aus anderem Material auf. In den meisten dieser Schichten war die Konzentration von Partikeln größer 2 µm, wie Staub, erhöht, auf Werte bis zu 1 cm3. Die Waldbrandaerosolschichten, die in der oberen Troposphäre gemessen wurden, unterschieden sich in den Rußpartikeleigenschaften von den schichten unterhalb von 8 km Höhe. Am 17. Juni wurde eine Waldbrandaerosolschicht in der oberen Troposphäre, auf 11 km Höhe, vermessen, die durch ein Gewitter nach oben transportiert wurde. Das Verhältnis von CO und Rußmassenkonzentration in der Schicht weist auf eine geringere Auswaschung hin, als sie im Ausfluss von Gewitterambossen beobachtet wurde. Auch erhöhte Ozonkonzentrationen deuten darauf hin, dass die Waldbrandaerosolschicht nicht im Hauptaufwindbereich sondern in schwächeren Aufwinden unterhalb des Ambosses transportiert wurde und sich mit stratosphärischer Luft vermischte. Waldbrandaerosolschichten in der oberen Troposphäre enthielten Rußpartikel, deren Massenmediandurchmessern mit 145 nm etwas kleiner waren als in Waldbrandaerosolschichten der mittleren Troposphäre. Etwa 50% der Rußpartikel waren intern gemischt. Diese Massengrößenverteilung von Rußpartikeln war nicht nur in allen bei DC3 beobachteten Waldbrandaerosolschichten nahezu identisch, sondern gleicht auch anderen Beobachtungsdaten von Rußpartikeln in Waldbrandaerosolschichten in der oberen Troposphäre, was auf eine stabile Gleichgewichtsverteilung hindeutet. Das Verhältnis von Rußmassenkonzentration und CO, 4.05 (ng/m³)/ppb in der freien Troposphäre und 1.43 (ng/m³)/ppb in der oberen Troposphäre, zeigt, dass bis zu zwei Drittel der Rußmasse beim Transport ausgewaschen wurden. Durch die große horizontale Ausdehnung der Schichten konnte eine dieser nur wenige hundert Meter dicken Schicht immer noch Ruß in Größenordnung von 2 Mg enthalten, was etwa einem Achtel der täglichen Flugzeugemissionen in der oberen Troposphäre entspricht.Biomass burning is the largest natural source of black carbon, the most absorbing particle type in the atmosphere. Layers containing biomass burning aerosol that are lifted into the upper troposphere have an increased atmospheric lifetime which can enhance their effect on climate. Biomass burning layers were measured during the Deep Convective Clouds and Chemistry (DC3) campaign with an airborne SP2 in the free and upper troposphere. Two case studies show the properties of black carbon particles in biomass burning layers at different altitudes. On June 11, 2012, biomass burning layers in Oklahoma and Missouri at 3-8 km altitude contained high concentrations, up to 2 µg/m³, of large, thickly coated black carbon particles. Biomass burning layers measured on June 17, 2012, over Kansas and Arkansas were located in the upper troposphere, at about 11 km altitude. The mass size distribution of black carbon particles and the rBC/CO ratio indicate that the biomass burning layers underwent cloud processing by a large thunderstorm on the previous day. Washout was less strong than for anvil outflow, leading to the conclusion that the layer was not transported in the main updrafts but in weaker updrafts that mixed with stratospheric air in the anvil region. Black carbon in layers up to 9 km altitude contain large particles with a mass median diameter of about 160-200 nm with 60-80% of the particles being thickly coated. Concentrations of large particles, possibly dust, were elevated above background in biomass burning layers up to 1 cm-3. Biomass burning layers in the upper troposphere (UT-BB) are vertically often only thin, several hundred meters thick, but can horizontally stretch over about thousand kilometers. The estimated total amount of black carbon in one biomass burning layer is about 2 Mg, which corresponds to roughly one eighth of daily global aviation emissions. Black carbon particles in upper tropospheric biomass burning layers showed a nearly constant, probably steady-state, mass size distribution with mass median diameters of 145 nm, (160-200 nm in the middle troposphere). The O3 concentrations in the UT-BB layers were elevated, with values above 200 ppb. The lower rBC/CO ratio of the UT-BB layers, 1.43 (ng/m³)/ppb in contrast to 4.05 (ng/m³)/ppb in the middle troposphere, indicates that up to two thirds of black carbon particles were removed during transport

Observations of surface radiation and stratospheric processes at Thule Air Base, Greenland, during the IPY

Ground-based measurements of atmospheric parameters have been carried out for more than 20 years at the Network for the Detection of Atmospheric Composition Change (NDACC) station at Thule Air Base (76.5°N, 68.8°W), on the north-western coast of Greenland. Various instruments dedicated to the study of the lower and middle polar atmosphere are installed at Thule in the framework of a long standing collaboration among Danish, Italian, and US research institutes and universities. This effort aims at monitoring the composition, structure and dynamics of the polar stratosphere, and at studying the Arctic energy budget and the role played by different factors, such as aerosols, water vapour, and surface albedo. During the International Polar Year (IPY), in winter 2008-2009, an intensive measurement campaign was conducted at Thule within the framework of the IPY project “Ozone layer and UV radiation in a changing climate evaluated during IPY” (ORACLE-O3) which sought to improve our understanding of the complex mechanisms that lead to the Arctic stratospheric O3 depletion. The campaign involved a lidar system, measuring aerosol backscatter and depolarization ratios up to 35 km and atmospheric temperature profiles from 25 to 70 km altitude, a ground-based millimeter-wave spectrometer (GBMS) used to derive stratospheric mixing ratio profiles of different chemical species involved in the stratospheric ozone depletion cycle, and then ground-based radiometers and a Cimel sunphotometer to study the Arctic radiative budget at the surface. The observations show that the surface radiation budget is mainly regulated by the longwave component throughout most of the year. Clouds have a significant impact contributing to enhance the role of longwave radiation. Besides clouds, water vapour seasonal changes produce the largest modification in the shortwave component at the surface, followed by changes in surface albedo and in aerosol amounts. For what concerns the middle atmosphere, during the first part of winter 2008-2009 the cold polar vortex allowed for the formation of polar stratospheric clouds (PSCs) which were observed above Thule by means of the lidar. This period was also characterized by GBMS measurements of low values of O3 due to the catalytic reactions prompted by the PSCs. In mid- January, as the most intense Sudden Stratospheric Warming event ever observed in the Arctic occurred, GBMS and lidar measurements of O3, N2O, CO and temperature described its evolution as it propagated from the upper atmosphere to the lower stratosphere

Laboratory for Atmospheres 2009 Technical Highlights

The 2009 Technical Highlights describes the efforts of all members of the Laboratory for Atmospheres. Their dedication to advancing Earth Science through conducting research, developing and running models, designing instruments, managing projects, running field campaigns, and numerous other activities, is highlighted in this report

Atmospheric water vapor and the aerosol direct radiative effect : Remote sensing and global model studies

Aerosols affect the climate both directly and indirectly. The direct effect comes from their influence on the radiation balance by scattering and absorption of solar radiation, while the indirect effect is based on the ways in which aerosols interact via clouds. Currently the total anthropogenic aerosol forcing includes one of the main uncertainties in the assessment of human induced climate change. The aerosol direct radiative effect (ADRE) can be simulated with either the radiative transfer modelling or estimated with solar radiation and aerosol amount measurements. Both approaches include significant uncertainties and this thesis focuses on the uncertainties on the measurement based estimation of ADRE and the uncertainties therein. The main scientific objectives of this thesis are to seek answers to the following four questions: 1) are the machine learning algorithms better than the a traditional lookup table (LUT) approach in estimating aerosol load (aerosol optical depth, AOD)?; 2) what is the role of water vapor (WVC) variability in the measurementbased regression method used to estimate the surface ADRE?; 3) how well do the radiative transfer codes, typically used in global aerosol models, agree?; 4) what is the impact of typically neglected diurnal aerosol variability in ADRE estimation? The results show that: 1) the machine learning algorithms are able to provide AOD more accurately than the LUT approach for conditions of varying aerosol optical properties, since in the LUT approach the aerosol model (e.g. single scattering albedo, asymmetry factor) needs to be fixed in advance. 2) It was found that covariability of AOD and WVC can have an influence in ADRE estimates, when using groundbased measurements of surface solar radiation and AOD. This has not been taken into account previously, but needs to be considered when these methods are applied. 3) The model intercomparison study, in which the models estimated the radiative fluxes for the same atmospheric states, revealed that there is relatively large diversity between models regarding the results from their radiative transfer modelling. 4) The main conclusion from the study focusing on the impact of systematic diurnal AOD cycles in aerosol direct radiative effect, was that even a notable diurnal change in AOD does not typically affect the 24h-average ADRE significantly

Lidar remote sensing and co-operative observations: Processing methods and aerosol radiative transfer

This Ph.D. thesis focuses on: (i) the design and integration of a polarimetric channel for the multi-spectral Raman lidar station of the Universitat Politècnica de Catalunya (UPC), Remote Sensing, Antennas, Microwaves and Superconductivity Group (CommSensLab), (ii) the study of the temporal and spatial evolution of atmospheric aerosol optical, microphysical and radiative properties by means of active and passive remote sensing in the context of ACTRIS and Spanish National projects, and (iii) rainfall rate retrieval by means of a vertically-pointed ceilometer in the context of the Verification of the Origins of Rotation in Tornadoes Experiment Southeast (VORTEX-SE). The first goal of this Ph.D., tested on the UPC multi-spectral Raman lidar station, consists of developing a secondary optical receiving chain, installed next to the laser source. The secondary telescope, mounted in the optical chain, allows retrieving the cross-polarized return signal separately from the total-power signal, avoiding the need of a very precise characterization of the crosstalk parameters of the beam-splitters. The first experimental results, corresponding to a collection of atmospheric conditions over the city of Barcelona, are also presented. The second goal of this Ph.D. deals first with the GAME (Global Atmospheric Model) code, necessary to retrieve the aerosol radiative properties. The radiative fluxes estimated in the short-wave and long-wave spectral ranges at the bottom and the top of the atmosphere by GAME are compared to the ones retrieved by a different radiative transfer model, namely Two-Stream, in order to know the importance of the spectral parameterization of a radiative transfer code. Then, GAME code, in both configurations, is fed by means of three different datasets to evaluate the parameterization of the vertically-resolved properties and to assess the uncertainty of GAME when is tuned with input parameters from different sources. Afterwards, an evaluation of the seasonal variability of the aerosol background optical and radiative properties in the Western Mediterranean Basin (WMB) is performed by means of AERONET (Aerosol Robotic Network) sun-photometers data from two background sites, Ersa (Corsica Island, France) and Palma de Mallorca (Mallorca Island, Spain). In addition, in order to detect possible northeast-southwest gradients in the aerosol properties, a third site located at Abolrán (Alborán Island, Spain) is considered. Finally, during 15-24 June 2013 a moderate Saharan dust multi-intrusion was detected by some EARLINET/ACTRIS (Granada, Barcelona, Naples, Potenza and Serra la Nave (Italy)) and ADRIMED/ChArMEx (Cap d’en Font, (Minorca Island, Spain) and Ersa) stations. This Ph.D. uses this event to study the spatio-temporal evolution of the mineral dust properties, since the lidar stations were supported during the multi-intrusion by collocated AERONET sun-photometers and the Falcon 20 aircraft. Also the GAME code is used to estimate the aerosol radiaite effect during the Saharan dust event. Besides, air- and space-borne lidar measurements, satellite images and back-trajectories are used to confirm the multi-intrusion aspect of the event. The last goal of this Ph.D. pursues estimation of the rain rate (RR) from ceilometer measurements. In VORTEX-SE, a Vaisala CL-31 ceilometer, a S-band radar, and a disdrometer were deployed in Alabama during March-April 2016. First, rain-extinction coefficients from ceilometer attenuated backscatter measurements are derived by means of a modified form of the well-known slope-method. These coefficients are compared with the RRs measured by a collocated S-band radar and a disdrometer in order to get the RR-to-extinction models. Advanced covariance-weighted techniques are used to best assess and validate the estimated models. These models can be used to estimate the RR from the ceilometer in similar situations without need to have a collocated cooperative instrument permanently deployed.Este Ph.D. se centra en: (i) en el diseño e integración de un canal polarimétrico para la estación lidar multi espectral del grupo de teledetección, antenas, microondas y superconductividad (CommSensLab) de la Universitat Politècnica de Catalunya (UPC), (ii) en el estudio de la evolución temporal y espacial de las propiedades ópticas, microfísicas y radiativas de los aerosoles por medio de teledetección activa y pasiva en el contexto de ACTRIS y proyectos estatales, y (iii) en la recuperación de intensidad de lluvia por medio de un ceilómetro en configuración vertical en el contexto del proyecto Verification of the Origins of Rotation in Tornadoes Experiment Southeast (VORTEX-SE). El primer objetivo, realizado en la estación lidar de UPC, consiste en el desarrollo de una cadena óptica secundaria instalada junto al láser. El telescopio secundario, montado en la cadena óptica, permite recuperar la componente cross-polarized de la señal total por separado, evitando la necesidad de conocer con precisión los parámetros de los beam-splitters. Se presentan también los primeros resultados obtenidos en Barcelona durante diferentes situaciones atmosféricas. El segundo objetivo de este Ph.D. se centra en el código GAME (Global Atmospheric Model), necesario para recuperar las propiedades radiativas de los aerosoles. Los flujos radiativos estimados tanto en onda larga como en onda corta en la base y en la parte superior de la atmósfera son comparados con los estimados por otro código de transferencia radiativa, Two-Stream, para conocer la importancia de la parametrización espectral. Después, el código GAME es alimentado con 3 bases de datos diferentes para evaluar la parametrización de las propiedades resueltas en altura y conocer la incertidumbre de GAME cuando es alimentado con parámetros con diferentes orígenes. Por otro lado, se presenta una evaluación de la variabilidad estacional de las propiedades ópticas y radiativas del aerosol de fondo en la cuenca oeste mediterránea (WMB) realizada con datos de fotómetros solares de la red AERONET (Aerosol Robotic Network) situados en dos puntos considerados libres de contaminación: Ersa (isla de Córcega, Francia) y Palma de Mallorca. Además, para detectar posibles gradientes noreste-suroeste en las propiedades delos aerosoles, se considera un tercer punto ubicado en la isla de Alborán. Por último, en este Ph.D. se aprovecha una multi intrusión moderada de polvo sahariano, detectada entre los días 15 y 24 de junio de 2013 por algunas estaciones EARLINET/ACTRIS (Granada, Barcelona, Nápoles, Potenza y Serra la Nave (Italia)) y ADRIMED/ChArMEx (Cap d'en Font (Menorca) y Ersa), para estudiar la evolución espacio-temporal de las propiedades del polvo mineral, ya que las estaciones lidar estaban apoyadas durante el evento por fotómetros solares pertenecientes a la red AERONET, situados junto a las estaciones lidar, y por vuelos del Falcon 20. GAME es usado para obtener también el efecto radiativo de los aerosoles durante el evento de polvo sahariano. Para confirmar el aspecto de multi intrusión se utilizan medidas lidar tomadas a bordo de aviones y satélites, imágenes satelitales y retro trayectorias. El último objetivo del Ph.D. persigue la estimación de la RR utilizando medidas de un ceilómetro. En VORTEX-SE, se desplegaron (Alabama, marzo-abril 2016) un ceilómetro Vaisala CL-31, un radar de banda S y un disdrómetro. Se han estimado los coeficientes de extinción debida a la lluvia a partir del retorno atenuado medido por el ceilómetro, utilizando una versión modificada del método de la pendiente. Estos coeficientes se comparan con las intensidades de lluvia (RR) estimadas con el radar y el disdrómetro para obtener modelos de RR-extinción. Para validarlos se utilizan técnicas avanzadas de covarianza ponderada. Dichos modelos pueden usarse para estimar la RR con un ceilómetro, en situaciones similares, sin necesidad de tener desplegado permanentemente un instrumento cooperativo.Postprint (published version

Aerosol-Cloud-Radiation Interactions in Regimes of Liquid Water Clouds

Despite large efforts and decades of research, the scientific understanding of how aerosols impact climate by modulating microphysical cloud properties is still low and associated radiative forcing estimates (RFaci ) vary with a wide spread. But since anthropogenically forced aerosol-cloud interactions (ACI) are considered to oppose parts of the global warming, it is crucial to know their contribution to the total radiative forcing in order to improve climate predictions. To obtain a better understanding and quantification of ACI and the associated radiative effect it as been suggested to use concurrent measurements and observationally constrained model simulations. In this dissertation a joint satellite-reanalysis approach is introduced, bridging the gap between climate models and satellite observations in a bottom-up approach. This methodology involves an observationally constrained aerosol model, refined and concurrent multi-component satellite retrievals, a state-of-the-art aerosol activation parameteriza- tion as well as radiative transfer model. This methodology is shown here to be useful for a quantitative as well as qualitative analysis of ACI and for estimating RFaci . As a result, a 10-year long climatology of cloud condensation nuclei (CCN) (particles from which cloud droplets form) is produced and evaluated. It is the first of its kind providing 3-D CCN concentrations of global coverage for various supersaturations and aerosol species and offering the opportunity to be used for evaluation in models and ACI studies. Further, the distribution and variability of the resulting cloud droplet numbers and their susceptibility to changes in aerosols is explored and compared to previous estimates. In this context, an analysis by cloud regime has been proven useful. Last but not least, the computation and analysis of the present-day regime-based RFaci represents the final conclusion of the bottom-up methodology. Overall, this thesis provides a comprehensive assessment of interactions and uncertainties related to aerosols, clouds and radiation in regimes of liquid water clouds and helps to improve the level of scientific understanding

Laboratory for Atmospheres: 2006 Technical Highlights

The 2006 Technical Highlights describes the efforts of all members of the Laboratory for Atmospheres. Their dedication to advancing Earth science through conducting research, developing and running models, designing instruments, managing projects, running field campaigns, and numerous other activities, are highlighted in this report

Laboratory for Atmospheres 2010 Technical Highlights

The 2010 Technical Highlights describes the efforts of all members of the Laboratory for Atmospheres. Their dedication to advancing Earth Science through conducting research, developing and running models, designing instruments, managing projects, running field campaigns, and numerous other activities, is highlighted in this report