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Pollen grains emitted by urban vegetation are the main primary biological airborne particles (PBAPs) which alter the biological quality of urban air and have a significant impact on human health. This work analyses the interactions which exist between pollen-type PBAPs, meteorological variables, and air pollutants in the urban atmosphere so that the complex relationships and trends in future scenarios of changing environmental conditions can be assessed. For this study, the 1992-2018 pollen data series from the city of Granada (southeast Spain) was used, in which the dynamics of the total pollen as well as the 8 main pollen types (Cupressaceae, Olea, Pinus, Platanus, Poaceae, Populus, Quercus and Urticaceae) were analysed. The trend analysis showed that all except Urticaceae trended upward throughout the series. Spearman's correlations with meteorological variables showed that, in general, the most influential variables on the pollen concentrations were the daily maximum temperature, relative humidity, water vapor pressure, global radiation, and insolation, with different effects on different pollen types. Parallel analysis by neural networks (ANN) confirmed these variables as the predominant ones, especially global radiation. The correlation with atmospheric pollutants revealed that ozone was the pollutant with the highest influence, although some pollen types also showed correlation with NO2, SO2, CO and PM10. The Generalized Linear Models (GLM) between pollen and pollutants also indicated O3 as the most prominent variable. These results highlight the active role that pollen-type PBAPs have on urban air quality by establishing their interactions with meteorological variables and pollutants, thereby providing information on the behaviour of pollen emissions under changing environmental conditions.
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Contaminantes Atmosféricos , Contaminantes Ambientales , Contaminantes Atmosféricos/análisis , Alérgenos/análisis , Ciudades , Monitoreo del Ambiente , Humanos , Estaciones del Año , EspañaRESUMEN
Vibrational Raman effect is widely used in atmospheric lidar systems, but rotational Raman present several advantages. We have implemented a new setup in the ultraviolet branch of an existing multiwavelength lidar system to collect signal from rotational Raman lines of Oxygen and Nitrogen. We showed that, with an appropriate filter wavelength selection, the systematic error introduced in the particle optical properties due to temperature dependence was less than 4%. With this new setup, we have been able to retrieve aerosol extinction and backscatter coefficients profiles at 355 nm with 1-h time resolution during daytime and up to 1-min time resolution during nighttime.
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This work deals with the analysis of the electronic subsystem of a multiwavelength elastic scanning lidar. Several calibration tests are applied to the Cubatão scanning lidar placed at the industrial area of Cubatão in the State of São Paulo (Brazil), in order to improve the knowledge of its performing itself and to design protocols for correcting lidar signal for undesirable instrumental effects. In particular, the trigger delay is assessed by means of zero-bin and bin-shift tests for analog (AN) and photo-counting (PC) signals, respectively. Dark current test is also performed to detect potential range-dependency that could affect lidar products. All tests were performed at different spatial resolutions. These instrumental corrections were applied to a case study of data acquired for characterizing the optical and microphysical properties of particles in an industrial flare. To that aim, a graphical method based on the space defined by the extinction-related Angström exponent versus its spectral curvature is used to derive the contribution of fine aerosol to extinction and the size of the fine aerosols in the industrial flare, therefore revealing features of the processes occurring inside the flame. Our study demonstrates the potential of this new technique for the study and measurement of industrial emissions.
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A reliable determination of equivalent black carbon (eBC) mass concentrations derived from filter absorption photometers (FAPs) measurements depends on the appropriate quantification of the mass absorption cross-section (MAC) for converting the absorption coefficient (babs) to eBC. This study investigates the spatial-temporal variability of the MAC obtained from simultaneous elemental carbon (EC) and babs measurements performed at 22 sites. We compared different methodologies for retrieving eBC integrating different options for calculating MAC including: locally derived, median value calculated from 22 sites, and site-specific rolling MAC. The eBC concentrations that underwent correction using these methods were identified as LeBC (local MAC), MeBC (median MAC), and ReBC (Rolling MAC) respectively. Pronounced differences (up to more than 50 %) were observed between eBC as directly provided by FAPs (NeBC; Nominal instrumental MAC) and ReBC due to the differences observed between the experimental and nominal MAC values. The median MAC was 7.8 ± 3.4 m2 g-1 from 12 aethalometers at 880 nm, and 10.6 ± 4.7 m2 g-1 from 10 MAAPs at 637 nm. The experimental MAC showed significant site and seasonal dependencies, with heterogeneous patterns between summer and winter in different regions. In addition, long-term trend analysis revealed statistically significant (s.s.) decreasing trends in EC. Interestingly, we showed that the corresponding corrected eBC trends are not independent of the way eBC is calculated due to the variability of MAC. NeBC and EC decreasing trends were consistent at sites with no significant trend in experimental MAC. Conversely, where MAC showed s.s. trend, the NeBC and EC trends were not consistent while ReBC concentration followed the same pattern as EC. These results underscore the importance of accounting for MAC variations when deriving eBC measurements from FAPs and emphasize the necessity of incorporating EC observations to constrain the uncertainty associated with eBC.
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Contaminantes Atmosféricos , Contaminantes Atmosféricos/análisis , Monitoreo del Ambiente/métodos , Aerosoles/análisis , Estaciones del Año , Hollín/análisis , Carbono/análisis , Material Particulado/análisisRESUMEN
The indirect effect of aerosols on climate through aerosol-cloud-interactions is still highly uncertain and limits our ability to assess anthropogenic climate change. The foundation of this uncertainty is in the number of cloud condensation nuclei (CCN), which itself mainly stems from uncertainty in aerosol sources and how particles evolve to become effective CCN. We analyze particle number size distribution (PNSD) and CCN measurements from an urban site in a two-step method: (1) we use an unsupervised clustering model to classify the main aerosol categories and processes occurring in the urban atmosphere and (2) we explore the influence of the identified aerosol populations on the CCN properties. According to the physical properties of each cluster, its diurnal timing, and additional air quality parameters, the clusters are grouped into five main aerosol categories: nucleation, growth, traffic, aged traffic, and urban background. The results show that, despite aged traffic and urban background categories are those with lower total particle number concentrations (Ntot) these categories are the most efficient sources in terms of contribution to the overall CCN budget with activation fractions (AF) around 0.5 at 0.75 % supersaturation (SS). By contrast, road traffic is an important aerosol source with the highest frequency of occurrence (32 %) and relatively high Ntot, however, its impact in the CCN activity is very limited likely due to lower particle mean diameter and hydrophobic chemical composition. Similarly, nucleation and growth categories, associated to new particle formation (NPF) events, present large Ntot with large frequency of occurrence (22 % and 28 %, respectively) but the CCN concentration for these categories is about half of the CCN concentration observed for the aged traffic category, which is associated with their small size. Overall, our results show that direct influence of traffic emissions on the CCN budget is limited, however, when these particles undergo ageing processes, they have a significant influence on the CCN concentrations and may be an important CCN source. Thus, aged traffic particles could be transported to other environments where clouds form, triggering a plausible indirect effect of traffic emissions on aerosol-cloud interactions and consequently contributing to climate change.
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Contaminación del Aire , Material Particulado , Material Particulado/análisis , Aerosoles/análisis , Atmósfera/química , Análisis por ConglomeradosRESUMEN
High-altitude mountain areas are sentinel ecosystems for global environmental changes such as anthropogenic pollution. In this study, we report a source apportionment of particulate material with an aerodynamic diameter smaller than 10 µm (PM10) in a high-altitude site in southern Europe (Sierra Nevada Station; SNS (2500 m a.s.l.)) during summer 2021. The emission sources and atmospheric secondary processes that determine the composition of aerosol particles in Sierra Nevada National Park (Spain) are identified from the concentrations of organic carbon (OC), elemental carbon (EC), 12 major inorganic compounds, 18 trace elements and 44 organic molecular tracer compounds in PM10 filter samples collected during day- and nighttime. The multivariate analysis of the joint dataset resolved five main PM10 sources: 1) Saharan dust, 2) advection from the urbanized valley, 3) local combustion, 4) smoke from a fire-event, and 5) aerosol from regional recirculation with high contribution of particles from secondary inorganic and organic aerosol formation processes. PM sources were clearly associated with synoptic meteorological conditions, and day- and nighttime circulation patterns typical of mountainous areas. Although a local pollution source was identified, the contribution of this source to PM10, OC and EC was small. Our results evidence the strong influence of middle- and long-range transport of aerosols, mainly from anthropogenic origin, on the aerosol chemical composition at this remote site.
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This study analyzed the variability of equivalent black carbon (eBC) mass concentrations and their sources in urban Europe to provide insights into the use of eBC as an advanced air quality (AQ) parameter for AQ standards. This study compiled eBC mass concentration datasets covering the period between 2006 and 2022 from 50 measurement stations, including 23 urban background (UB), 18 traffic (TR), 7 suburban (SUB), and 2 regional background (RB) sites. The results highlighted the need for the harmonization of eBC measurements to allow for direct comparisons between eBC mass concentrations measured across urban Europe. The eBC mass concentrations exhibited a decreasing trend as follows: TR > UB > SUB > RB. Furthermore, a clear decreasing trend in eBC concentrations was observed in the UB sites moving from Southern to Northern Europe. The eBC mass concentrations exhibited significant spatiotemporal heterogeneity, including marked differences in eBC mass concentration and variable contributions of pollution sources to bulk eBC between different cities. Seasonal patterns in eBC concentrations were also evident, with higher winter concentrations observed in a large proportion of cities, especially at UB and SUB sites. The contribution of eBC from fossil fuel combustion, mostly traffic (eBCT) was higher than that of residential and commercial sources (eBCRC) in all European sites studied. Nevertheless, eBCRC still had a substantial contribution to total eBC mass concentrations at a majority of the sites. eBC trend analysis revealed decreasing trends for eBCT over the last decade, while eBCRC remained relatively constant or even increased slightly in some cities.
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Contaminantes Atmosféricos , Contaminación del Aire , Contaminantes Atmosféricos/análisis , Monitoreo del Ambiente/métodos , Aerosoles/análisis , Contaminación del Aire/análisis , Europa (Continente) , Estaciones del Año , Hollín/análisis , Carbono/análisis , Material Particulado/análisisRESUMEN
PM10 was collected during an EMEP winter campaign of 2017-2018 in two urban background sites in Barcelona (BCN) and Granada (GRA), two Mediterranean cities in the coast and inland, respectively. The concentrations of PM10, organic carbon (OC), elemental carbon (EC), and organic molecular tracer compounds such as hopanes, anhydro-saccharides, polycyclic aromatic hydrocarbon, and several biogenic and anthropogenic markers of secondary organic aerosols (SOA) were two times higher in GRA compared to BCN and related to the atmospheric mixing heights in the areas. Multivariate curve resolution (MCR-ALS) source apportionment analysis identified primary emissions sources (traffic + biomass burning) that were responsible for the 50% and 20% of the organic aerosol contributions in Granada and Barcelona, respectively. The contribution of biomass burning was higher in the holidays than in the working days in GRA while all primary combustion emissions decreased in holidays in BCN. The MCR-ALS identified that oxidative species and SOA formation processes contributed to 40% and 80% in Granada and Barcelona, respectively. Aged SOA was dominant in Granada and Barcelona under stagnant atmospheric conditions and in presence of air pollution. On the other hand, fresh SOA contributions from α-pinene oxidation (cis-pinonic acid) were three times higher in Barcelona than Granada and could be related to new particle formation, essentially due to overall cleaner air conditions and elevated air temperatures.
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Contaminantes Atmosféricos , Material Particulado , Aerosoles/análisis , Contaminantes Atmosféricos/análisis , Carbono/análisis , Ciudades , Monitoreo del Ambiente , Compuestos Orgánicos/análisis , Material Particulado/análisis , Estaciones del AñoRESUMEN
Understanding the activation properties of aerosol particles as cloud condensation nuclei (CCN) is important for the climate and hydrological cycle, but their properties are not fully understood. In this study, the CCN activation properties of aerosols are investigated at two different sites in southern Spain: an urban background station in Granada and a high altitude mountain station in the Sierra Nevada National Park, with a horizontal separation of 21 km and vertical separation of 1820 m. CCN activity at the urban environment is driven by primary sources, mainly road traffic. Maximum CCN concentrations occurred during traffic rush hours, although this is also when the activation fraction is lowest. This is due to the characteristics of the rush hour aerosol consisting of ultrafine and less hygroscopic particles. In contrast, the mountain site exhibited larger and more hygroscopic particles, with CCN activity driven by the joint effect of new particle formation (NPF) and vertical transport of anthropogenic particles from Granada urban area by orographic buoyant upward flow. This led to the maximum concentrations of CCN and aerosol particles occurring at midday at the mountain site. Clear differences in the diurnal evolution of CCN between NPF events and non-event days were observed at the Sierra Nevada station, demonstrating the large contribution of NPF to CCN concentrations, especially at high supersaturations. The isolated contribution of NPF to CCN concentration has been estimated to be 175% higher at SS = 0.5% relative to what it would be without NPF. We conclude that NPF could be the major source of CCN at this mountain site. Finally, two empirical models were used to parameterize CCN concentration in terms of aerosol optical or physical parameters. The models can explain measurements satisfactorily at the urban station. At the mountain site both models cannot reproduce satisfactorily the observations at low SS.
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The most recent works demonstrate that the lidar overlap function, which describes the overlap between the laser beam and the receiver field of view, can be determined experimentally for the 355 and 532 nm channels using Raman signals. Nevertheless, the Raman channels cannot be used to determine the lidar overlap for the infrared channel (1064 nm) because of their low intensity. In addition, many Raman lidar systems only provide inelastic signals with reasonable signal-to-noise ratio at nighttime. In view of this fact, this work presents a modification of that method, based on the comparison of attenuated backscatter profiles derived from lidar and ceilometer, to retrieve the overlap function for the lidar infrared channel. Similarly to the Raman overlap method, the approach presented here allows to derive the overlap correction without an explicit knowledge of all system parameters. The application of the proposed methodology will improve the potential of Raman lidars to investigate the aerosol microphysical properties in the planetary boundary layer, extending the information of 1064 nm backscatter profiles to the ground and allowing the retrieval of microphysical properties practically close to the surface.
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Algoritmos , Atmósfera/análisis , Monitoreo del Ambiente/métodos , Rayos Láser , Radar , Refractometría/métodos , Rayos InfrarrojosRESUMEN
A reference dataset of multi-wavelength particle light scattering and hemispheric backscattering coefficients for different relative humidities (RH) between RH = 30 and 95% and wavelengths between λ = 450 nm and 700 nm is described in this work. Tandem-humidified nephelometer measurements from 26 ground-based sites around the globe, covering multiple aerosol types, have been re-analysed and harmonized into a single dataset. The dataset includes multi-annual measurements from long-term monitoring sites as well as short-term field campaign data. The result is a unique collection of RH-dependent aerosol light scattering properties, presented as a function of size cut. This dataset is important for climate and atmospheric model-measurement inter-comparisons, as a means to improve model performance, and may be useful for satellite and remote sensing evaluation using surface-based, in-situ measurements.
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A new method is presented for retrieval of the aerosol and cloud optical depth using a CCD camera equipped with a fish-eye lens (all-sky imager system). In a first step, the proposed method retrieves the spectral radiance from sky images acquired by the all-sky imager system using a linear pseudoinverse algorithm. Then, the aerosol or cloud optical depth at 500 nm is obtained as that which minimizes the residuals between the zenith spectral radiance retrieved from the sky images and that estimated by the radiative transfer code. The method is tested under extreme situations including the presence of nonspherical aerosol particles. The comparison of optical depths derived from the all-sky imager with those retrieved with a sunphotometer operated side by side shows differences similar to the nominal error claimed in the aerosol optical depth retrievals from sunphotometer networks.
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This study focuses on the analysis of the sensitivity of UV erythemal radiation (UVER) to variations in the total ozone column (TOC) under different sky conditions at Granada (southeastern Spain). The sensitivity is studied both in relative terms by means of the Radiation Amplification Factor (RAF) and in absolute terms using the Ozone Efficiency (OE). These two variables are determined for diverse sky conditions characterized by the cloud cover information given by a sky camera (in oktas) and the cloud optical depth (COD) estimated from global solar radiation measurements. As expected, in absolute terms, the TOC variations cause substantially smaller UVER changes during completely overcast situations than during cloud-free cases. For instance, the OE (SZA = 30°, TOC = 290 DU) decreases from 0.68 mW m(-2) per unit of TOC (0 oktas) to 0.50 mW m(-2) per unit of TOC (8 oktas). However, the opposite is observed when the analysis is performed in relative terms. Thus, the RAF (determined for SZA cases below 80°) increases from 1.1 for cloud-free cases (0 oktas) to 1.4 for completely overcast situations (8 oktas). This opposite behavior is also found when both RAF and OE are analyzed as functions of COD. Thus, while the OE strongly decreases with increasing COD, the RAF increases as COD increases.
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In recent years, there has been a substantial increase in attempts to model the flux of ultraviolet radiation (UV). UV irradiance at surface level is a result of the combined effects of solar zenith angle, surface elevation, cloud cover, aerosol load and optical properties, surface albedo and the vertical profile of ozone. In this study, we present the development of an artificial neural network (ANN) model that can be used to estimate solar UV irradiance on the basis of optical air mass, ozone columnar content, latitude, horizontal visibility data and cloud information such as type, coverage and height. ANN are widely accepted as a technology offering an alternative way to tackle complex and ill-defined problems. They can learn from examples, are fault tolerant in the sense that they are able to handle noisy and incomplete data, are able to deal with nonlinear problems and, once trained, can perform prediction and generalization at high speed. In this study, a multilayer perceptron network (MLP) consisting of an input layer, an output layer and one hidden layer was used. Training of the neural network was done using the Bayesian regulation back propagation algorithm. The study was developed using data from three stations on the Iberian Peninsula: Madrid and Murcia during the period 2000-2001 and Zaragoza in 2001. To train and validate the MPL neural networks, independent subsets of data were extracted from the complete database at each station. The results suggest that a MLP neural network using optical air mass, ozone columnar content, latitude and total cloud coverage provides the best estimates, with mean bias deviation and root mean square deviation of -0.1% and 18.0%, 1.6% and 19.6%, 0.1% and 14.6% at Madrid, Murcia and Zaragoza, respectively. Despite the dependence of the cloud radiative effect on cloud type, the use of additional information such as cloud type or cloud elevation did not improve these results. The performance of the developed ANN has been checked regarding its ability to estimate the UV index (UVI); results indicate that in more than 95% of the cases, the difference between estimated and measured values does not exceed one unit of UVI.