Spatiotemporal changes in aerosol properties by hygroscopic growth and impacts on radiative forcing and heating rates during DISCOVER-AQ 2011

This research has been supported by the H2020 Marie Sklodowska-Curie Actions (grant no. 778349), the Spanish Ministry of Economy and Competitiveness (RTI2018101154.A.I00), and by the Russian Science Foundation (project 2117-00114, entitled Development of lidar retrieval algorithms).This work focuses on the characterization of vertically resolved aerosol hygroscopicity properties and their direct radiative effects through a unique combination of ground-based and airborne remote sensing measurements during the Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER-AQ) 2011 field campaign in the Baltimore-Washington DC metropolitan area. To that end, we combined aerosol measurements from a multiwavelength Raman lidar located at NASA Goddard Space Flight Center and the airborne NASA Langley High Spectral Resolution Lidar-1 (HSRL-1) lidar system. In situ measurements aboard the P-3B airplane and ground-based Aerosol Robotic Network - Distributed Regional Aerosol Gridded Observational Network (AERONET-DRAGON) served to validate and complement quantifications of aerosol hygroscopicity from lidar measurements and also to extend the study both temporally and spatially. The focus here is on 22 and 29 July 2011, which were very humid days and characterized by a stable atmosphere and increasing relative humidity with height in the planetary boundary layer (PBL). Combined lidar and radiosonde (temperature and water vapor mixing ratio) measurements allowed the retrieval of the Hanel hygroscopic growth factor which agreed with that obtained from airborne in situ measurements and also explained the significant increase of extinction and backscattering with height. Airborne measurements also confirmed aerosol hygroscopicity throughout the entire day in the PBL and identified sulfates and water-soluble organic carbon as the main species of aerosol particles. The combined Raman and HSRL-1 measurements permitted the inversion for aerosol microphysical properties revealing an increase of particle radius with altitude consistent with hygroscopic growth. Aerosol hygroscopicity pattern served as a possible explanation of aerosol optical depth increases during the day, particularly for fine-mode particles. Lidar measurements were used as input to the libRadtran radiative transfer code to obtain vertically resolved aerosol radiative effects and heating rates under dry and humid conditions, and the results reveal that aerosol hygroscopicity is responsible for larger cooling effects in the shortwave range (7-10 W m(-2) depending on aerosol load) near the ground, while heating rates produced a warming of 0.12 K d(-1) near the top of PBL where aerosol hygroscopic growth was highest.H2020 Marie Sklodowska-Curie Actions 778349Spanish Ministry of Economy and Competitiveness RTI2018101154.A.I00Russian Science Foundation (RSF) 2117-0011

Aerosol number fluxes and concentrations over a southern European urban area

Although cities are an important source of aerosol particles, aerosol number flux measurements over urban areas are scarce. These measurements are however important as they can allow us to identify the different sources/sinks of aerosol particles and quantify their emission contributions. Therefore, they can help us to understand the aerosol impacts on human health and climate, and to design effective mitigation strategies through the reduction of urban aerosol emissions. In this work we analyze the aerosol number concentrations and fluxes for particles with diameters larger than 2.5 nm measured by eddy covariance technique at an urban area (Granada city, Spain) from November 2016 to April 2018. This is the first study of particle number flux in an urban area in the Iberian Peninsula and is one of the few current studies that report long-term aerosol number flux measurements. The results suggest that, on average, Granada urban area acted as a net source for atmospheric aerosol particles with median particle number flux of 150 x 10(6) m(-2) s(-1). Downward negative fluxes were observed in only 12% of the analyzed data, and most of them were observed during high aerosol load conditions. Both aerosol number fluxes and concentrations were maximum in winter and 50% larger than those measured in summer due to the increased emissions from domestic heating, burning of residual agricultural waste in the agricultural area surrounding the site, as well as to the lower aerosol dilution effects during winter. The analysis of the seasonal diurnal variability of the aerosol number concentration revealed the significant impact of traffic emissions on aerosol population over Granada urban area in all seasons. It also shows the impact of domestic heating and agricultural waste burning emissions in winter as well as the influence of new particle formation processes in summer and spring seasons. Closer analysis by wind sector demonstrated that both aerosol concentrations and fluxes from urban sector (where high density of anthropogenic sources is located) were lower than those from rural sector (which includes agricultural area but also the main highway of the city). This evidences the strong impact of aerosol emissions from traffic circulating on the highway on aerosol population over our measurement site.Peer reviewe

Monumental heritage exposure to urban black carbon pollution

In this study, aerosol light-absorption measurements obtained at three sites during a winter campaign were used to analyse and identify the major sources of Black Carbon (BC) particles in and around the Alhambra monument, a UNESCO World Heritage Site that receives over 2 million visitors per year. The Conditional Bivariate Probability Function and the Aethalometer model were employed to identify the main sources of BC particles and to estimate the contributions of biomass burning and fossil fuel emissions to the total Equivalent Black Carbon (EBC) concentrations over the monumental complex. Unexpected high levels of EBC were found at the Alhambra, comparable to those measured in relatively polluted European urban areas during winter. EBC concentrations above 3.0 μg/m3, which are associated with unacceptable levels of soiling and negative public reactions, were observed at Alhambra monument on 13 days from 12 October 2015 to 29 February 2016, which can pose a risk to its long-term conservation and may cause negative social and economic impacts. It was found that road traffic emissions from the nearby urban area and access road to the Alhambra were the main sources of BC particles over the monument. However, biomass burning emissions were found to have very small impact on EBC concentrations at the Alhambra. The highest EBC concentrations were observed during an extended stagnant episode associated with persistent high-pressure systems, reflecting the large impact that can have these synoptic conditions on BC over the Alhambra.European Union's Horizon 2020 Research and Innovation Programme under grant agreement No. 654109, ACTRIS-2.Spanish Ministry of Economy and Competitiveness and FEDER through project CGL2013-45410-R, CGL2016-81092-R 598 and CGL2012-30729.Andalusia Regional Government through project P12- RNM-2409 and P12-FQM-1889

Quantifying traffic, biomass burning and secondary source contributions to atmospheric particle number concentrations at urban and suburban sites

In this study, we propose a new approach to determine the contributions of primary vehicle exhaust (N-1(ff)), primary biomass burning (N-1(bb)) and secondary (N-2) particles to mode segregated particle number concentrations. We used simultaneous measurements of aerosol size distribution in the 12-600 nm size range and black carbon (BC) concentration obtained during winter period at urban and suburban sites influenced by biomass burning (BB) emissions. As expected, larger aerosol number concentrations in the 12-25 and 25-100 nm size ranges are observed at the urban site compared to the suburban site. However, similar concentrations of BC are observed at both sites due to the larger contribution of BB particles to the observed BC at suburban (34%) in comparison to urban site (23%). Due to this influence of BB emissions in our study area, the application of the Rodriguez and Cuevas (2007) method, which was developed for areas mainly influenced by traffic emissions, leads to an overestimation of the primary vehicle exhaust particles concentrations by 18% and 26% in urban and suburban sites, respectively, as compared to our new proposed approach. The results show that (1) N-2 is the main contributor in all size ranges at both sites, (2) N-1(ff) is the main contributor to primary particles (>70%) in all size ranges at both sites and (3) N-1(bb) contributes significantly to the primary particles in the 25-100 and 100-600 nm size ranges at the suburban (24% and 28%, respectively) and urban (13% and 20%, respectively) sites. At urban site, the N-1(ff) contribution shows a slight increase with the increase of total particle concentration, reaching a contribution of up to 65% at high ambient aerosol concentrations. New particle loination events are an important aerosol source during summer noon hours but, on average, these events do not implicate a considerable contribution to urban particles. (C) 2021 Elsevier B.V. All rights reserved.Peer reviewe

ParaDIME: Parallel Distributed Infrastructure for Minimization of Energy for data centers

Dramatic environmental and economic impact of the ever increasing power and energy consumption of modern computing devices in data centers is now a critical challenge. On the one hand, designers use technology scaling as one of the methods to face the phenomenon called dark silicon (only segments of a chip function concurrently due to power restrictions). On the other hand, designers use extreme-scale systems such as teradevices to meet the performance needs of their applications which in turn increases the power consumption of the platform. In order to overcome these challenges, we need novel computing paradigms that address energy efficiency. One of the promising solutions is to incorporate parallel distributed methodologies at different abstraction levels. The FP7 project ParaDIME focuses on this objective to provide different distributed methodologies (software-hardware techniques) at different abstraction levels to attack the power-wall problem. In particular, the ParaDIME framework will utilize: circuit and architecture operation below safe voltage limits for drastic energy savings, specialized energy-aware computing accelerators, heterogeneous computing, energy-aware runtime, approximate computing and power-aware message passing. The major outcome of the project will be a noval processor architecture for a heterogeneous distributed system that utilizes future device characteristics, runtime and programming model for drastic energy savings of data centers. Wherever possible, ParaDIME will adopt multidisciplinary techniques, such as hardware support for message passing, runtime energy optimization utilizing new hardware energy performance counters, use of accelerators for error recovery from sub-safe voltage operation, and approximate computing through annotated code. Furthermore, we will establish and investigate the theoretical limits of energy savings at the device, circuit, architecture, runtime and programming model levels of the computing stack, as well as quantify the actual energy savings achieved by the ParaDIME approach for the complete computing stack with the real environment

Determination and analysis of in situ spectral aerosol optical properties by a multi-instrumental approach

Continuous in situ measurements of aerosol optical properties were conducted from 29 June to 29 July 2012 in Granada (Spain) with a seven-wavelength Aethalometer, a Multi-Angle Absorption Photometer, and a three-wavelength integrating nephelometer. The aim of this work is to describe a methodology to obtain the absorption coefficients (babs) for the different Aethalometer wavelengths. In this way, data have been compensated using algorithms which best estimate the compensation factors needed. Two empirical factors are used to infer the absorption coefficients from the Aethalometer measurements: C – the parameter describing the enhancement of absorption by particles in the filter matrix due to multiple scattering of light in the filter matrix – and f, the parameter compensating for non-linear loading effects in the filter matrix. Spectral dependence of f found in this study is not very strong. Values for the campaign lie in the range from 1.15 at 370 nm to 1.11 at 950 nm. Wavelength dependence in C proves to be more important, and also more difficult to calculate. The values obtained span from 3.42 at 370 nm to 4.59 at 950 nm. Furthermore, the temporal evolution of the Ångström exponent of absorption (αabs) and the single-scattering albedo (ω0) is presented. On average αabs is around 1.1 ± 0.3, and ω0 is 0.78 ± 0.08 and 0.74 ± 0.09 at 370 and 950 nm, respectively. These are typical values for sites with a predominance of absorbing particles, and the urban measurement site in this study is such. The babs average values are of 16 ± 10 Mm−1 (at 370 nm) and 5 ± 3 Mm−1 (at 950 nm), respectively. Finally, differences between workdays and Sundays have been further analysed, obtaining higher babs and lower ω0 during the workdays than on Sundays as a consequence of the diesel traffic influence.This work was financed jointly by the Spanish Ministry of Economy and Competitiveness and the European Regional Development Fund through projects CGL2011-24290, CGL2010-18782, CSD2007-00067, and CGL2012-33294; by the Valencia Autonomous Government through project PROMETEO/2010/064; the Andalusia Regional Government through projects P08-RNM-3568 and P10-RNM-6299; and by the Slovenian Ministry of Economic Development and Technology JR-KROP grant 3211-11-000519. The research leading to these results has received funding from the European Union Seventh Framework Programme (FP7/2007-2013) under grant agreement no. 262254 (ACTRIS). The collaboration of S. Segura in this work was possible thanks to fellowship BES-2010-031626

Spatial and temporal variability of carbonaceous aerosols: assessing the impact of biomass burning in the urban environment

Biomass burning (BB) is a significant source of atmospheric particles in many parts of the world. Whereas many studies have demonstrated the importance of BB emissions in central and northern Europe, especially in rural areas, its impact in urban air quality of southern European countries has been sparsely investigated. In this study, highly time resolved multi-wavelength absorption coefficients together with levoglucosan (BB tracer) mass concentrations were combined to apportion carbonaceous aerosol sources. The Aethalometer model takes advantage of the different spectral behaviour of BB and fossil fuel (FF) combustion aerosols. The model was found to be more sensitive to the assumed value of the aerosol Ångström exponent (AAE) for FF (AAEff) than to the AAE for BB (AAEbb). As result of various sensitivity tests the model was optimized with AAEff = 1.1 and AAEbb = 2. The Aethalometer model and levoglucosan tracer estimates were in good agreement. The Aethalometer model was further applied to data from three sites in Granada urban area to evaluate the spatial variation of CMff and CMbb (carbonaceous matter from FF or BB origin, respectively) concentrations within the city. The results showed that CMbb was lower in the city centre while it has an unexpected profound impact on the CM levels measured in the suburbs (about 40%). Analysis of BB tracers with respect to wind speed suggested that BB was dominated by sources outside the city, to the west in a rural area. Distinguishing whether it corresponds to agricultural waste burning or with biomass burning for domestic heating was not possible. This study also shows that although traffic restrictions measures contribute to reduce carbonaceous concentrations, the extent of the reduction is very local. Other sources such as BB, which can contribute to CM as much as traffic emissions, should be targeted to reduce air pollution.This research was partially supported by the Andalusia Regional Government through projects P10-RNM-6299 and P12-RNM-2409, by the Spanish Ministry of Economy and Competitiveness and FEDER through project CGL2013_45410-R; by EUREKA and the Slovenian Ministry of Economic Development and Technology grants (Eurostars grant E!4825 FC Aeth, JR-KROP grant 3211-11-000519); and by European Union's Horizon 2020 Research and Innovation Programme under grant agreement No. 654109, ACTRIS-2. The authors would like to thank Air Quality Service from Junta de Andalucía (Consejería de Medio Ambiente y Ordenación del Territorio) and Vicerrectorado de Política Científica e Investigación from the University of Granada for their support in the installation of the Aethalometer at PC and GV, respectively.G. Titos was partially funded by Programa del Plan Propio de Investigación “Contrato Puente” of the University of Granada and by the Spanish Ministry of Economy and Competitiveness under postdoctoral program Juan de la Cierva – Formación (FJCI-2014-20819)

Inter-relations of precipitation, aerosols, and clouds over Andalusia, southern Spain, revealed by the Andalusian Global ObseRvatory of the Atmosphere (AGORA)

The south-central interior of Andalusia experiences intricate precipitation patterns as a result of its semi-arid Mediterranean climate and the impact of Saharan dust and human-made pollutants. The primary aim of this study is to monitor the inter-relations between various factors, such as aerosols, clouds, and meteorological variables, and precipitation systems in Granada using ground-based remote sensing and in situ instruments including a microwave radiometer, ceilometer, cloud radar, nephelometer, and weather station. Over an 11-year period, we detected rain events using a physical retrieval method that employed microwave radiometer measurements. A composite analysis was applied to them to construct a climatology of the temporal evolution of precipitation. It was found that convective rain is the dominant precipitation type in Granada, accounting for 68 % of the rain events. The height of the cloud base is mainly distributed at an altitude of 2 to 7 km. Integrated water vapor (IWV) and integrated cloud liquid water (ILW) increase rapidly before the onset of rain. Aerosol scattering at the surface level and hence the aerosol concentration are reduced during rain, and the predominant mean size distribution of aerosol particles before, during, and after rain is almost the same. A meteorological environment favorable for virga formation is observed in Granada. The surface weather station detected rainfall later than the microwave radiometer, indicating virga according to ceilometer and cloud radar data. We used 889 rain-day events identified by weather station data to determine precipitation intensity classes and found that light rain is the main precipitation intensity class in Granada, accounting for 72 % of the rain-day events. This can be a result of the high tropospheric temperature induced by the Andalusian climate and the reduction of cloud droplet size by the high availability of aerosol particles in the urban atmosphere. This study provides evidence that aerosols, clouds, and meteorological variables have a combined impact on precipitation which can be considered for water resource management and improving rain forecasting accuracy.</p

Study of the relative humidity dependence of aerosol light-scattering in southern Spain

This investigation focuses on the characterisation of the aerosol particle hygroscopicity. Aerosol particle optical properties were measured at Granada, Spain, during winter and spring seasons in 2013. Measured optical properties included particle light-absorption coefficient (sap) and particle light-scattering coefficient (ssp) at dry conditions and at relative humidity (RH) of 85 +/- 10%. The scattering enhancement factor, f(RH=85%), had a mean value of 1.5 +/- 0.2 and 1.6 +/- 0.3 for winter and spring campaigns, respectively. Cases of high scattering enhancement were more frequent during the spring campaign with 27% of the f(RH=85%) values above 1.8, while during the winter campaign only 8% of the data were above 1.8. A Saharan dust event (SDE), which occurred during the spring campaign, was characterised by a predominance of large particles with low hygroscopicity. For the day when the SDE was more intense, a mean daily value of f(RH=85%)=1.3 +/- 0.2 was calculated. f(RH=85%) diurnal cycle showed two minima during the morning and afternoon traffic rush hours due to the increase in non-hygroscopic particles such as black carbon and road dust. This was confirmed by small values of the single-scattering albedo and the scattering Angstrom exponent. A significant correlation between f(RH=85%) and the fraction of particulate organic matter and sulphate was obtained. Finally, the impact of ambient RH in the aerosol radiative forcing was found to be very small due to the low ambient RH. For high RH values, the hygroscopic effect should be taken into account since the aerosol forcing efficiency changed from -13W/m2 at dry conditions to -17W/m2 at RH=85%.This work was supported by the Andalusia Regional Government through projects P10-RNM-6299 and P12-RNM-2409; by the Spanish Ministry of Economy and Competitiveness through projects CGL2010-18782, CSD2007-00067, CGL2011-13580-E/CLI and CGL2011-16124-E; and by EU through ACTRIS project (EU INFRA-2010-1.1.16-262254).G. Titos was funded by the program FPI of the Spanish Ministry of Economy and Competitiveness – Secretariat of Science, Innovation and Development under grant BES-2011-043721