A new method to retrieve the real part of the equivalent refractive index of atmospheric aerosols

This document is the Accepted Manuscript version of the following article: S. Vratolis, et al, ‘A new method to retrieve the real part of the equivalent refractive index of atmospheric aerosols’, Journal of Aerosol Science, Vol. 117: 54-62, March 2018. Under embargo until 29 December 2019. The final, published version is available online at DOI: https://doi.org/10.1016/j.jaerosci.2017.12.013.In the context of the international experimental campaign Hygroscopic Aerosols to Cloud Droplets (HygrA-CD, 15 May to 22 June 2014), dry aerosol size distributions were measured at Demokritos station (DEM) using a Scanning Mobility Particle Sizer (SMPS) in the size range from 10 to 550 nm (electrical mobility diameter), and an Optical Particle Counter (OPC model Grimm 107 operating at the laser wavelength of 660 nm) to acquire the particle size distribution in the size range of 250 nm to 2.5 μm optical diameter. This work describes a method that was developed to align size distributions in the overlapping range of the SMPS and the OPC, thus allowing us to retrieve the real part of the aerosol equivalent refractive index (ERI). The objective is to show that size distribution data acquired at in situ measurement stations can provide an insight to the physical and chemical properties of aerosol particles, leading to better understanding of aerosol impact on human health and earth radiative balance. The resulting ERI could be used in radiative transfer models to assess aerosol forcing direct effect, as well as an index of aerosol chemical composition. To validate the method, a series of calibration experiments were performed using compounds with known refractive index (RI). This led to a corrected version of the ERI values, (ERICOR). The ERICOR values were subsequently compared to model estimates of RI values, based on measured PM2.5 chemical composition, and to aerosol RI retrieved values by inverted lidar measurements on selected days.Peer reviewe

A comparative analysis of the causes of air pollution in three cities of the Danube region: implications for the implementation of the air quality directives

The causes of air pollution in three cities of the Danube region (Budapest, Sofia and Zagreb) were studied using datasets of measurements and modelling tools. The contributions from different activity sectors, including natural sources and their geographical origin were quantified. It was observed that most of the pollutants are emitted locally. However, the medium to long range transport may be also considerable. On the basis of the output of the source identification, a series of measures were proposed to deal wtih the pollution problem at local, national and international levels.JRC.H.2-Air and Climat

Assessment of wood burning versus fossil fuel contribution to wintertime black carbon and carbon monoxide concentrations in Athens, Greece

The scope of this study was to estimate the contribution of fossil fuel and wood burning combustion to black carbon (BC) and carbon monoxide (CO) during wintertime, in Athens. For that purpose, in situ measurements of equivalent black carbon (eBC) and CO were simultaneously conducted in a suburban and an urban background monitoring site in Athens during the 3 months of winter 2014–2015. For the deconvolution of eBC into eBC emitted from fossil fuel (BCff) and wood burning (BCwb), a method based on the spectral dependency of the absorption of pure black carbon and brown carbon was used. Thereafter, BCwb and BCff estimated fractions were used along with measured CO concentrations in a multiple regression analysis, in order to quantify the contribution of each one of the combustion sources to the ambient CO levels. For a comparative analysis of the results, we additionally estimated the wood burning and fossil fuel contribution to CO, calculated on the basis of their CO&thinsp;∕&thinsp;NOx emission ratios. The results indicate that during wintertime BC and CO are mainly emitted by local sources within the Athens Metropolitan Area (AMA). Fossil fuel combustion, mainly from road traffic, is found to be the major contributor to both eBC in PM2.5 and CO ambient concentrations in AMA. However, wintertime wood burning makes a significant contribution to the observed eBC (of about 30&thinsp;%) and CO concentrations (on average, 11 and 16&thinsp;% of total CO in the suburban and urban background sites respectively). Both BC and CO from biomass burning (BCwb and COwb, respectively) present a clear diurnal pattern, with the highest concentrations during night-time, supporting the theory of local domestic heating being their main source.</p

A new method for the quantification of ambient particulate-matter emission fluxes

An inversion method has been developed in order to quantify the emission fluxes of certain aerosol pollution sources across a wide region in the Northern Hemisphere, mainly in Europe and western Asia. The data employed are the aerosol contribution factors deducted by positive matrix factorization (PMF) on a PM2.5 chemical composition dataset from 16 European and Asian cities for the period 2014 to 2016. The spatial resolution of the method corresponds to the geographic grid cell size of the Lagrangian particle dispersion model (Flexible Particle Dispersion Model, FLEXPART, 1∘ × 1∘) which was utilized for the air mass backward simulations. The area covered is also related to the location of the 16 cities under study. Species with an aerodynamic geometric mean diameter of 400 nm and 3.1 µm and a geometric standard deviation of 1.6 and 2.25, respectively, were used to model the secondary sulfate and dust aerosol transport. Potential source contribution function (PSCF) analysis and generalized Tikhonov regularization were applied so as to acquire potential source areas and quantify their emission fluxes. A significant source area for secondary sulfate on the east of the Caspian Sea is indicated, when data from all stations are used. The maximum emission flux in that area is as high as 10 × 10−12 kg m−2 s−1. When Vilnius, Dushanbe, and Kurchatov data were excluded, the areas with the highest emission fluxes were the western and central Balkans and southern Poland. The results display many similarities to the SO2 emission maps provided by the OMI-HTAP (Ozone Monitoring Instrument-Hemispheric Transport Air Pollution) and ECLIPSE (Evaluating the Climate and Air Quality Impacts of Short-Lived Pollutants) databases. For dust aerosol, measurements from Athens, Belgrade, Debrecen, Lisbon, Tirana, and Zagreb are utilized. The west Sahara region is indicated as the most important source area, and its contribution is quantified, with a maximum of 17.6 × 10−12 kg m−2 s−1. When we apply the emission fluxes from every geographic grid cell (1∘ × 1∘) for secondary sulfate aerosol deducted with the new method to air masses originating from Vilnius, a useful approximation to the measured values is achieved.</p

Comparison and complementary use of in situ and remote sensing aerosol measurements in the Athens Metropolitan Area

© 2020 Elsevier Ltd. All rights reserved. This manuscript is licensed under the Creative Commons Attribution-NonCommercial-NoDerivatives 4.0 International Licence http://creativecommons.org/licenses/by-nc-nd/4.0/.In the summer of 2014 in situ and remote sensing instruments were deployed in Athens, in order to study the concentration, physical properties, and chemical composition of aerosols. In this manuscript we aim to combine the measurements of collocated in situ and remote sensing instruments by comparison and complementary use, in order to increase the accuracy of predictions concerning climate change and human health. We also develop a new method in order to select days when a direct comparison on in situ and remote sensing instruments is possible. On selected days that displayed significant turbulence up to approximately 1000 m above ground level (agl), we acquired the aerosol extinction or scattering coefficient by in situ instruments using three approaches. In the first approach the aerosol extinction coefficient was acquired by adding a Nephelometer scattering coefficient in ambient conditions and an Aethalometer absorption coefficient. The correlation between the in situ and remote sensing instruments was good (coefficient of determination R2 equal to 0.69). In the second approach we acquired the aerosol refractive index by fitting dry Nephelometer and Aethalometer measurements with Mie algorithm calculations of the scattering and absorption coefficients for the size distribution up to a maximum diameter of 1000 nm obtained by in situ instruments. The correlation in this case was relatively good (R2 equal to 0.56). Our next step was to compare the extinction coefficient acquired by remote sensing instruments to the scattering coefficient calculated by Mie algorithm using the size distribution up to a maximum diameter of 1000 nm and the equivalent refractive index (ERICOR), which is acquired by the comparison of the size distributions obtained by a Scanning Mobility Particle Sizer (SMPS) and an Optical Particle Counter (OPC). The agreement between the in situ and remote sensing instruments in this case was not satisfactory (R2 equal to 0.35). The last comparison for the selected days was between the aerosol extinction Ångström exponent acquired by in situ and remote sensing instruments. The correlation was not satisfactory (R2 equal to 0.4), probably due to differences in the number size distributions present in the air volumes measured by in situ and remote sensing instruments. We also present a day that a Saharan dust event occurred in Athens in order to demonstrate the information we obtain through the synergy of in situ and remote sensing instruments on how regional aerosol is added to local aerosol, especially during pollution events due to long range transport.Peer reviewe

A phenomenology of new particle formation (NPF) at 13 European sites

New particle formation (NPF) events occur almost everywhere in the world and can play an important role as a particle source. The frequency and characteristics of NPF events vary spatially, and this variability is yet to be fully understood. In the present study, long-term particle size distribution datasets (minimum of 3 years) from 13 sites of various land uses and climates from across Europe were studied, and NPF events, deriving from secondary formation and not traffic-related nucleation, were extracted and analysed. The frequency of NPF events was consistently found to be higher at rural background sites, while the growth and formation rates of newly formed particles were higher at roadsides (though in many cases differences between the sites were small), underlining the importance of the abundance of condensable compounds of anthropogenic origin found there. The growth rate was higher in summer at all rural background sites studied. The urban background sites presented the highest uncertainty due to greater variability compared to the other two types of site. The origin of incoming air masses and the specific conditions associated with them greatly affect the characteristics of NPF events. In general, cleaner air masses present higher probability for NPF events, while the more polluted ones show higher growth rates. However, different patterns of NPF events were found, even at sites in close proximity (<ĝ€¯200ĝ€¯km), due to the different local conditions at each site. Region-wide events were also studied and were found to be associated with the same conditions as local events, although some variability was found which was associated with the different seasonality of the events at two neighbouring sites. NPF events were responsible for an increase in the number concentration of ultrafine particles of more than 400ĝ€¯% at rural background sites on the day of their occurrence. The degree of enhancement was less at urban sites due to the increased contribution of other sources within the urban environment. It is evident that, while some variables (such as solar radiation intensity, relative humidity, or the concentrations of specific pollutants) appear to have a similar influence on NPF events across all sites, it is impossible to predict the characteristics of NPF events at a site using just these variables, due to the crucial role of local conditions. © Author(s) 2021

A phenomenology of new particle formation (NPF) at 13 European sites

New particle formation (NPF) events occur almost everywhere in the world and can play an important role as a particle source. The frequency and characteristics of NPF events vary spatially, and this variability is yet to be fully understood. In the present study, long-term particle size distribution datasets (minimum of 3 years) from 13 sites of various land uses and climates from across Europe were studied, and NPF events, deriving from secondary formation and not traffic-related nucleation, were extracted and analysed. The frequency of NPF events was consistently found to be higher at rural background sites, while the growth and formation rates of newly formed particles were higher at roadsides (though in many cases differences between the sites were small), underlining the importance of the abundance of condensable compounds of anthropogenic origin found there. The growth rate was higher in summer at all rural background sites studied. The urban background sites presented the highest uncertainty due to greater variability compared to the other two types of site. The origin of incoming air masses and the specific conditions associated with them greatly affect the characteristics of NPF events. In general, cleaner air masses present higher probability for NPF events, while the more polluted ones show higher growth rates. However, different patterns of NPF events were found, even at sites in close proximity (< 200 km), due to the different local conditions at each site. Region-wide events were also studied and were found to be associated with the same conditions as local events, although some variability was found which was associated with the different seasonality of the events at two neighbouring sites. NPF events were responsible for an increase in the number concentration of ultrafine particles of more than 400% at rural background sites on the day of their occurrence. The degree of enhancement was less at urban sites due to the increased contribution of other sources within the urban environment. It is evident that, while some variables (such as solar radiation intensity, relative humidity, or the concentrations of specific pollutants) appear to have a similar influence on NPF events across all sites, it is impossible to predict the characteristics of NPF events at a site using just these variables, due to the crucial role of local conditions.Peer reviewe

Effects of mixing state on optical and radiative properties of black carbon in the European Arctic

Atmospheric aging promotes internal mixing of black carbon (BC), leading to an enhancement of light absorption and radiative forcing. The relationship between BC mixing state and consequent absorption enhancement was never estimated for BC found in the Arctic region. In the present work, we aim to quantify the absorption enhancement and its impact on radiative forcing as a function of microphysical properties and mixing state of BC observed in situ at the Zeppelin Arctic station (78°&thinsp;N) in the spring of 2012 during the CLIMSLIP (Climate impacts of short-lived pollutants in the polar region) project.Single-particle soot photometer (SP2) measurements showed a mean mass concentration of refractory black carbon (rBC) of 39&thinsp;ng&thinsp;m−3, while the rBC mass size distribution was of lognormal shape, peaking at an rBC mass-equivalent diameter (DrBC) of around 240&thinsp;nm. On average, the number fraction of particles containing a BC core with DrBC&gt;80&thinsp;nm was less than 5&thinsp;% in the size range (overall optical particle diameter) from 150 to 500&thinsp;nm. The BC cores were internally mixed with other particulate matter. The median coating thickness of BC cores with 220&thinsp;nm&thinsp;&lt;&thinsp;DrBC&lt; 260&thinsp;nm was 52&thinsp;nm, resulting in a core–shell diameter ratio of 1.4, assuming a coated sphere morphology. Combining the aerosol absorption coefficient observed with an Aethalometer and the rBC mass concentration from the SP2, a mass absorption cross section (MAC) of 9.8&thinsp;m2&thinsp;g−1 was inferred at a wavelength of 550 nm. Consistent with direct observation, a similar MAC value (8.4&thinsp;m2&thinsp;g−1 at 550&thinsp;nm) was obtained indirectly by using Mie theory and assuming a coated-sphere morphology with the BC mixing state constrained from the SP2 measurements. According to these calculations, the lensing effect is estimated to cause a 54&thinsp;% enhancement of the MAC compared to that of bare BC particles with equal BC core size distribution. Finally, the ARTDECO radiative transfer model was used to estimate the sensitivity of the radiative balance to changes in light absorption by BC as a result of a varying degree of internal mixing at constant total BC mass. The clear-sky noontime aerosol radiative forcing over a surface with an assumed wavelength-dependent albedo of 0.76–0.89 decreased, when ignoring the absorption enhancement, by −0.12&thinsp;W&thinsp;m−2 compared to the base case scenario, which was constrained with mean observed aerosol properties for the Zeppelin site in Arctic spring. The exact magnitude of this forcing difference scales with environmental conditions such as the aerosol optical depth, solar zenith angle and surface albedo. Nevertheless, our investigation suggests that the absorption enhancement due to internal mixing of BC, which is a systematic effect, should be considered for quantifying the aerosol radiative forcing in the Arctic region.</p

Seasonality of aerosol optical properties in the Arctic

Given the sensitivity of the Arctic climate to short-lived climate forcers, long-term in situ surface measurements of aerosol parameters are useful in gaining insight into the magnitude and variability of these climate forcings. Seasonality of aerosol optical properties – including the aerosol light-scattering coefficient, absorption coefficient, single-scattering albedo, scattering Ångström exponent, and asymmetry parameter – are presented for six monitoring sites throughout the Arctic: Alert, Canada; Barrow, USA; Pallas, Finland; Summit, Greenland; Tiksi, Russia; and Zeppelin Mountain, Ny-Ålesund, Svalbard, Norway. Results show annual variability in all parameters, though the seasonality of each aerosol optical property varies from site to site. There is a large diversity in magnitude and variability of scattering coefficient at all sites, reflecting differences in aerosol source, transport, and removal at different locations throughout the Arctic. Of the Arctic sites, the highest annual mean scattering coefficient is measured at Tiksi (12.47&thinsp;Mm−1), and the lowest annual mean scattering coefficient is measured at Summit (1.74&thinsp;Mm−1). At most sites, aerosol absorption peaks in the winter and spring, and has a minimum throughout the Arctic in the summer, indicative of the Arctic haze phenomenon; however, nuanced variations in seasonalities suggest that this phenomenon is not identically observed in all regions of the Arctic. The highest annual mean absorption coefficient is measured at Pallas (0.48&thinsp;Mm−1), and Summit has the lowest annual mean absorption coefficient (0.12&thinsp;Mm−1). At the Arctic monitoring stations analyzed here, mean annual single-scattering albedo ranges from 0.909 (at Pallas) to 0.960 (at Barrow), the mean annual scattering Ångström exponent ranges from 1.04 (at Barrow) to 1.80 (at Summit), and the mean asymmetry parameter ranges from 0.57 (at Alert) to 0.75 (at Summit). Systematic variability of aerosol optical properties in the Arctic supports the notion that the sites presented here measure a variety of aerosol populations, which also experience different removal mechanisms. A robust conclusion from the seasonal cycles presented is that the Arctic cannot be treated as one common and uniform environment but rather is a region with ample spatiotemporal variability in aerosols. This notion is important in considering the design or aerosol monitoring networks in the region and is important for informing climate models to better represent short-lived aerosol climate forcers in order to yield more accurate climate predictions for the Arctic.</p

Differentiation of coarse-mode anthropogenic, marine and dust particles in the High Arctic islands of Svalbard

19 pages, 8 figures,1 table, 1 appendix.-- Data availability: The APS data can be accessed from https://doi.org/10.5281/zenodo.3961473 (Traversi et al., 2020). The absorption coefficient data are available upon request from Gilardoni et al. (2020). Data supporting this publication can be accessed upon request from the corresponding authorsUnderstanding aerosol–cloud–climate interactions in the Arctic is key to predicting the climate in this rapidly changing region. Whilst many studies have focused on submicrometer aerosol (diameter less than 1 µm), relatively little is known about the supermicrometer aerosol (diameter above 1 µm). Here, we present a cluster analysis of multiyear (2015–2019) aerodynamic volume size distributions, with diameter ranging from 0.5 to 20 µm, measured continuously at the Gruvebadet Observatory in the Svalbard archipelago. Together with aerosol chemical composition data from several online and offline measurements, we apportioned the occurrence of the coarse-mode aerosols during the study period (mainly from March to October) to anthropogenic (two sources, 27 %) and natural (three sources, 73 %) origins. Specifically, two clusters are related to Arctic haze with high levels of black carbon, sulfate and accumulation mode (0.1–1 µm) aerosol. The first cluster (9 %) is attributed to ammonium sulfate-rich Arctic haze particles, whereas the second one (18 %) is attributed to larger-mode aerosol mixed with sea salt. The three natural aerosol clusters were open-ocean sea spray aerosol (34 %), mineral dust (7 %) and an unidentified source of sea spray-related aerosol (32 %). The results suggest that sea-spray-related aerosol in polar regions may be more complex than previously thought due to short- and long-distance origins and mixtures with Arctic haze, biogenic and likely blowing snow aerosols. Studying supermicrometer natural aerosol in the Arctic is imperative for understanding the impacts of changing natural processes on Arctic aerosoThis research has been supported by the Natural Environment Research Council (grant no. NE/S00579X/1). We acknowledge support of the publication fee by the CSIC Open Access Publication Support Initiative through its Unit of Information Resources for Research (URICI)With the institutional support of the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2019-000928-S)Peer reviewe