Abstract. Following the emergence of the severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) responsible for COVID-19 in December 2019 in Wuhan (China) and its spread to the rest of the world, the World Health Organization declared a global pandemic in March 2020. Without effective treatment in the initial pandemic phase, social distancing and mandatory quarantines were introduced as the only available preventative measure. In contrast to the detrimental societal impacts, air quality improved in all countries in which strict lockdowns were applied, due to lower pollutant emissions. Here we investigate the effects of the COVID-19 lockdowns in Europe on ambient black carbon (BC), which affects climate and damages health, using in situ observations from 17 European stations in a Bayesian inversion framework. BC emissions declined by 23 kt in Europe (20 % in Italy, 40 % in Germany, 34 % in Spain, 22 % in France) during lockdowns compared to the same period in the previous 5 years, which is partially attributed to COVID-19 measures. BC temporal variation in the countries enduring the most drastic restrictions showed the most distinct lockdown impacts. Increased particle light absorption in the beginning of the lockdown, confirmed by assimilated satellite and remote sensing data, suggests residential combustion was the dominant BC source. Accordingly, in central and Eastern Europe, which experienced lower than average temperatures, BC was elevated compared to the previous 5 years. Nevertheless, an average decrease of 11 % was seen for the whole of Europe compared to the start of the lockdown period, with the highest peaks in France (42 %), Germany (21 %), UK (13 %), Spain (11 %) and Italy (8 %). Such a decrease was not seen in the previous years, which also confirms the impact of COVID-19 on the European emissions of BC.
Carbonaceous soot particles are formed during incomplete combustion of fossil fuels, biofuels or biomass and are considered to be a significant proportion of aerosol emission, especially in polluted areas, and to contain light-absorbing carbon fractions. The light-absorbing carbon components make these particles exhibit positive radiative forcing and thus they contribute to atmospheric warming processes. The exact contribution to this process however still has significant uncertainties. One of the sources of uncertainty is related to the capacity to accurately describe soot spectral optical properties (MAC/MSC/MEC - mass absorption/scattering/extinction cross-sections in m2g-1; CRI - complex refractive index), due to significant uncertainties for key measurements like the absorption coefficient or absorbing mass fraction. A second source is considered to be the change of the optical properties with the variable physico-chemical state of soot (e.g. chemical composition, morphology, primary particle size, aggregate size distribution, coating and mixing state) which depends on (i) the combustion conditions/sources  and is (ii) known to change during atmospheric lifetime due to ageing and mixing processes.The present work aims at providing new measurements of soot spectral optical properties and investigating their dependence on particles’ physico-chemical state and the role of measurement uncertainties. For this, a set of original experiments was performed in the 4.3m3 CESAM atmospheric simulation chamber (https://cesam.cnrs.fr/) on soot aerosols generated by a commercial propane diffusion flame soot generator (miniCAST model 6204 TYPE C, JING). In these experiments, the variability of soot properties due to (i) generation and (ii) atmospheric ageing was explored. Different combustion conditions going from fuel–leaner to fuel-richer were set to produce soot aerosol with different effective densities, EC/TC-ratios ranging from 0.8 ± 0.1 to 0.0 ± 0.1 and size distributions with median diameters between 30 and 120 nm. Selected aerosols were subjected to ageing in a N2/O2 atmosphere under simulated atmospheric conditions (humid, with/without illumination, up to 26 hours lifetime). In these conditions, physical and chemical ageing, under the presence of different gaseous phases (O3, SO2) and addition of a second aerosol phase produced by photo-oxidation of SO2 or the ozonolysis of α-pinene, led to changes in the physico-chemical properties of the soot.State-of-the-art techniques were used to generate an extensive dataset of physico-chemical parameters (mass concentration, morphology, effective density, composition, size distribution) and spectral optical properties (absorption, scattering, extinction coefficients) for different soot aerosols and different ageing states of these. The absorption coefficient in particular was measured by both filter-based (AE - Aethalometer, MAAP - Multi-Angle Absorption Photometer, MWAA – Multi-Wavelength Absorbance Analyzer, PP_UniMI - Polar Photometer by University of Milano) and extinction minus scattering techniques. The MAC, MSC and MEC datasets, retrieved by combining these measurements, will be presented for the ensemble of chamber experiments and the variability of these parameters in link with variations in the particles’ physico-chemical properties will be discussed together with key relevant uncertainties.
Abstract. It is important to understand the relative contribution of primary and secondary particles to regional and global aerosol so that models can attribute aerosol radiative forcing to different sources. In large-scale models, there is considerable uncertainty associated with treatments of particle formation (nucleation) in the boundary layer (BL) and in the size distribution of emitted primary particles, leading to uncertainties in predicted cloud condensation nuclei (CCN) concentrations. Here we quantify how primary particle emissions and secondary particle formation influence size-resolved particle number concentrations in the BL using a global aerosol microphysics model and aircraft and ground site observations made during the May 2008 campaign of the European Integrated Project on Aerosol Cloud Climate Air Quality Interactions (EUCAARI). We tested four different parameterisations for BL nucleation and two assumptions for the emission size distribution of anthropogenic and wildfire carbonaceous particles. When we emit carbonaceous particles at small sizes (as recommended by the Aerosol Intercomparison project, AEROCOM), the spatial distributions of campaign-mean number concentrations of particles with diameter >50 nm (N50) and >100 nm (N100) were well captured by the model (R2≥0.8) and the normalised mean bias (NMB) was also small (−18% for N50 and −1% for N100). Emission of carbonaceous particles at larger sizes, which we consider to be more realistic for low spatial resolution global models, results in equally good correlation but larger bias (R2≥0.8, NMB = −52% and −29%), which could be partly but not entirely compensated by BL nucleation. Within the uncertainty of the observations and accounting for the uncertainty in the size of emitted primary particles, BL nucleation makes a statistically significant contribution to CCN-sized particles at less than a quarter of the ground sites. Our results show that a major source of uncertainty in CCN-sized particles in polluted European air is the emitted size of primary carbonaceous particles. New information is required not just from direct observations, but also to determine the "effective emission size" and composition of primary particles appropriate for different resolution models.
The size‐segregated chemical composition of aerosols was investigated during winters 2000 and 2001 at Puy de Dôme (1465 m above sea level, France), a site most of the time located in the free troposphere. Aerosols have been sampled using low‐pressure cascade impactors (Electrical Low Pressure Impactor (ELPI) and Small Deposition Impactor (SDI) 13 and 12 stages) and analyzed for inorganic (Na + , NH 4 + , K + , Mg 2+ , Ca 2+ , Cl − , NO 3 − , and SO 4 2− ) and organic (HCOO − , CH 3 COO − , and C 2 O 4 2− ) ions, organic and elemental carbon (OC and EC), insoluble dust, and total mass. Under cloudy conditions, the sampling includes interstitial aerosol as well as the residue of evaporated cloud droplets. Aerosols (and residues of cloud droplets) were sampled in different air masses, which can be classified into three different categories according to their aerosol load and composition: background (BG), anthropogenic (ANT), and specific events (EV) that include advection of Saharan dust and upward transport from the polluted boundary layer to the site. On the basis of the presence or absence of coarse sea‐salt particles, a further classification permits us to distinguish air masses that have or have not been exposed to the ocean. A closed mass balance is achieved on submicron ranges (mean departure of 18.5%) for the three main air mass categories, providing a reliable description of main aerosol types in the west European free troposphere. The total aerosol mass at 50% relative humidity is close to 2.7 ± 0.6 μg m −3 in BG, 5.3 ± 1.0 μg m −3 in ANT, and 15 to 22 μg m −3 in EV air masses. The aerosol mass distribution generally exhibits two submicron modes (Acc1 at 0.2 ± 0.1 μm and Acc2 at 0.5 ± 0.2 μm geometric mean diameter (calculated for every impactor stage) and a supermicron mode (2 ± 1 μm). Aerosols exhibit a high degree of external mixing with carbonaceous (EC and OC) and ionic species associated with Acc1 and Acc2. Concentrations of light carboxylates and mineral dust never exceed 4% of the total content of analyzed compounds, except for a Saharan dust event during which the contribution of insoluble dust reaches 26% of the total aerosol mass. Depending on the sampled air mass, bulk water‐soluble inorganic species and carbonaceous material account for 25–70% and 15–60% of the total mass, respectively. The OC fraction is higher in air masses with low aerosol load (53%, 32%, and 22% for BG, ANT, and EV, respectively). Conversely, the EC fraction is enhanced from 4% in BG to 10% in ANT and 14% in EV. The inorganic fraction is more abundant in EV (55%) and ANT (60%) than in BG (40%) air masses as a result of enhanced nit .
Abstract. Detailed investigations of the chemical and microphysical properties of atmospheric aerosol particles were performed at the puy-de-Dôme (pdD) research station (1465 m) in autumn (September and October 2008), winter (February and March 2009), and summer (June 2010) using a Time-of-Flight Aerosol Mass Spectrometer. Over the three campaigns, the average mass concentrations of the non-refractory submicron particles ranged from 10 μg m−3 up to 27 μg m−3. Highest nitrate and ammonium mass concentrations were measured during the winter and during periods when marine modified airmasses were arriving at the site, whereas highest concentrations of organic particles were measured during the summer and during periods when continental airmasses arrived at the site. The measurements reported in this paper show that atmospheric particle composition is strongly influenced by both the season and the origin of the airmass. The total organic mass spectra were analysed using positive matrix factorisation to separate individual organic components contributing to the overall organic particle mass concentrations. These organic components include a low volatility oxygenated organic aerosol particle (LV-OOA) and a semi-volatile organic aerosol particle (SV-OOA). Correlations of the LV-OOA components with fragments of m/z 60 and m/z 73 (mass spectral markers of wood burning) during the winter campaign suggest that wintertime LV-OOA are related to aged biomass burning emissions, whereas organic aerosol particles measured during the summer are likely linked to biogenic sources. Equivalent potential temperature calculations, gas-phase, and LIDAR measurements define whether the research site is in the planetary boundary layer (PBL) or in the free troposphere (FT)/residual layer (RL). We observe that SV-OOA and nitrate particles are associated with air masses arriving from the PBL where as particle composition measured from RL/FT airmasses contain high mass fractions of sulphate and LV-OOA. This study provides unique insights into the effects of season and airmass variability on regional aerosol particles measured at an elevated site.
Abstract. The present paper investigates the diurnal and seasonal variability of the aerosol total number concentration, number and volume size distribution between 10 nm and 10 μm, from a combination of a scanning mobility particle sizer (SMPS) and an optical counter (OPC), performed over a two-year period (January 2006–February 2008) at the Nepal Climate Observatory-Pyramid (NCO-P) research station, (5079 m a.s.l.). The annual average number concentration measured over the two-year period at the NCO-P is 860 cm−3. Total concentrations show a strong seasonality with maxima during pre-monsoon and post-monsoon seasons and minima during the dry and monsoon seasons. A diurnal variation is also clearly observed, with maxima between 09:00 and 12:00 UTC. The aerosol concentration maxima are mainly due to nucleation processes during the post-monsoon season, as witnessed by high nucleation mode integrated number concentrations, and to transport of high levels of pollution from the plains by valley breezes during the pre-monsoon season, as demonstrated by high accumulation mode integrated number concentrations. Night-time number concentration of particles (from 03:00 to 08:00 NST) are relatively low throughout the year (from 450 cm−3 during the monsoon season to 675 cm−3 during the pre-monsoon season), indicating the of high altitudes background level, as a result of downslope winds during this part of the day. However, it was found that these background concentrations are strongly influenced by the daytime concentrations, as they show the same seasonal variability. If nighttime concentrations were presumed to be representative of free troposphere (FT)/residual layer concentrations, they would be found to be two times higher than at other lower altitudes European sites, such as the Jungfraujoch. However, BL intrusions might contaminate the free troposphere/residual layer even at this altitude, especially during regional air masses influence. Night-time measurements were subsequently selected to study the FT composition according to different air masses, and the effect of long range transport to the station.
