Time-dependent source apportionment of submicron organic aerosol for a rural site in an alpine valley using a rolling positive matrix factorisation (PMF) window

We collected 1 year of aerosol chemical speciation monitor (ACSM) data in Magadino, a village located in the south of the Swiss Alpine region, one of Switzerland's most polluted areas. We analysed the mass spectra of organic aerosol (OA) by positive matrix factorisation (PMF) using Source Finder Professional (SoFi Pro) to retrieve the origins of OA. Therein, we deployed a rolling algorithm, which is closer to the measurement, to account for the temporal changes in the source profiles. As the first-ever application of rolling PMF with multilinear engine (ME-2) analysis on a yearlong dataset that was collected from a rural site, we resolved two primary OA factors (traffic-related hydrocarbon-like OA (HOA) and biomass burning OA (BBOA)), one mass-to-charge ratio ( m/z) 58-related OA (58-OA) factor, a less oxidised oxygenated OA (LO-OOA) factor, and a more oxidised oxygenated OA (MO-OOA) factor. HOA showed stable contributions to the total OA through the whole year ranging from 8.1 % to 10.1 %, while the contribution of BBOA showed an apparent seasonal variation with a range of 8.3 %–27.4 % (highest during winter, lowest during summer) and a yearly average of 17.1 %. OOA (sum of LO-OOA and MO-OOA) contributed 71.6 % of the OA mass, varying from 62.5 % (in winter) to 78 % (in spring and summer). The 58-OA factor mainly contained nitrogen-related variables which appeared to be pronounced only after the filament switched. However, since the contribution of this factor was insignificant (2.1 %), we did not attempt to interpolate its potential source in this work. The uncertainties (σ) for the modelled OA factors (i.e. rotational uncertainty and statistical variability in the sources) varied from ±4 % (58-OA) to a maximum of ±40 % (LO-OOA). Considering that BBOA and LO-OOA (showing influences of biomass burning in winter) had significant contributions to the total OA mass, we suggest reducing and controlling biomass-burning-related residential heating as a mitigation strategy for better air quality and lower PM levels in this region or similar locations. In Appendix A, we conduct a head-to-head comparison between the conventional seasonal PMF analysis and the rolling mechanism. We find similar or slightly improved results in terms of mass concentrations, correlations with external tracers, and factor profiles of the constrained POA factors. The rolling results show smaller scaled residuals and enhanced correlations between OOA factors and corresponding inorganic salts compared to those of the seasonal solutions, which was most likely because the rolling PMF analysis can capture the temporal variations in the oxidation processes for OOA components. Specifically, the time-dependent factor profiles of MO-OOA and LO-OOA can well explain the temporal viabilities of two main ions for OOA factors, m/z 44 (CO⁺₂) and m/z 43 (mostly C2H3O+). Therefore, this rolling PMF analysis provides a more realistic source apportionment (SA) solution with time-dependent OA sources. The rolling results also show good agreement with offline Aerodyne aerosol mass spectrometer (AMS) SA results from filter samples, except for in winter. The latter discrepancy is likely because the online measurement can capture the fast oxidation processes of biomass burning sources, in contrast to the 24 h filter samples. This study demonstrates the strengths of the rolling mechanism, provides a comprehensive criterion list for ACSM users to obtain reproducible SA results, and is a role model for similar analyses of such worldwide available data

A European aerosol phenomenology - 7: High-time resolution chemical characteristics of submicron particulate matter across Europe

Similarities and differences in the submicron atmospheric aerosol chemical composition are analyzed from a unique set of measurements performed at 21 sites across Europe for at least one year. These sites are located between 35 and 62°N and 10° W – 26°E, and represent various types of settings (remote, coastal, rural, industrial, urban). Measurements were all carried out on-line with a 30-min time resolution using mass spectroscopy based instruments known as Aerosol Chemical Speciation Monitors (ACSM) and Aerosol Mass Spectrometers (AMS) and following common measurement guidelines. Data regarding organics, sulfate, nitrate and ammonium concentrations, as well as the sum of them called non-refractory submicron aerosol mass concentration ([NR-PM1]) are discussed. NR-PM1 concentrations generally increase from remote to urban sites. They are mostly larger in the mid-latitude band than in southern and northern Europe. On average, organics account for the major part (36–64%) of NR-PM1 followed by sulfate (12–44%) and nitrate (6–35%). The annual mean chemical composition of NR-PM1 at rural (or regional background) sites and urban background sites are very similar. Considering rural and regional background sites only, nitrate contribution is higher and sulfate contribution is lower in mid-latitude Europe compared to northern and southern Europe. Large seasonal variations in concentrations (μg/m³) of one or more components of NR-PM1 can be observed at all sites, as well as in the chemical composition of NR-PM1 (%) at most sites. Significant diel cycles in the contribution to [NR-PM1] of organics, sulfate, and nitrate can be observed at a majority of sites both in winter and summer. Early morning minima in organics in concomitance with maxima in nitrate are common features at regional and urban background sites. Daily variations are much smaller at a number of coastal and rural sites. Looking at NR-PM1 chemical composition as a function of NR-PM1 mass concentration reveals that although organics account for the major fraction of NR-PM1 at all concentration levels at most sites, nitrate contribution generally increases with NR-PM1 mass concentration and predominates when NR-PM1 mass concentrations exceed 40 μg/m³ at half of the sites. © 2021 The Author

A European aerosol phenomenology - 7 : High-time resolution chemical characteristics of submicron particulate matter across Europe

Similarities and differences in the submicron atmospheric aerosol chemical composition are analyzed from a unique set of measurements performed at 21 sites across Europe for at least one year. These sites are located between 35 and 62 degrees N and 10 degrees W - 26 degrees E, and represent various types of settings (remote, coastal, rural, industrial, urban). Measurements were all carried out on-line with a 30-min time resolution using mass spectroscopy based instruments known as Aerosol Chemical Speciation Monitors (ACSM) and Aerosol Mass Spectrometers (AMS) and following common measurement guidelines. Data regarding organics, sulfate, nitrate and ammonium concentrations, as well as the sum of them called non-refractory submicron aerosol mass concentration ([NR-PM1]) are discussed. NR-PM1 concentrations generally increase from remote to urban sites. They are mostly larger in the mid-latitude band than in southern and northern Europe. On average, organics account for the major part (36-64%) of NR-PM1 followed by sulfate (12-44%) and nitrate (6-35%). The annual mean chemical composition of NR-PM1 at rural (or regional background) sites and urban background sites are very similar. Considering rural and regional background sites only, nitrate contribution is higher and sulfate contribution is lower in midlatitude Europe compared to northern and southern Europe. Large seasonal variations in concentrations (mu g/m(3)) of one or more components of NR-PM1 can be observed at all sites, as well as in the chemical composition of NR-PM1 (%) at most sites. Significant diel cycles in the contribution to [NR-PM1] of organics, sulfate, and nitrate can be observed at a majority of sites both in winter and summer. Early morning minima in organics in concomitance with maxima in nitrate are common features at regional and urban background sites. Daily variations are much smaller at a number of coastal and rural sites. Looking at NR-PM1 chemical composition as a function of NR-PM1 mass concentration reveals that although organics account for the major fraction of NR-PM1 at all concentration levels at most sites, nitrate contribution generally increases with NR-PM1 mass concentration and predominates when NR-PM1 mass concentrations exceed 40 mu g/m(3) at half of the sites.Peer reviewe

A European aerosol phenomenology - 7: High-time resolution chemical characteristics of submicron particulate matter across Europe

Similarities and differences in the submicron atmospheric aerosol chemical composition are analyzed from a unique set of measurements performed at 21 sites across Europe for at least one year. These sites are located between 35 and 62°N and 10° W – 26°E, and represent various types of settings (remote, coastal, rural, industrial, urban). Measurements were all carried out on-line with a 30-min time resolution using mass spectroscopy based instruments known as Aerosol Chemical Speciation Monitors (ACSM) and Aerosol Mass Spectrometers (AMS) and following common measurement guidelines. Data regarding organics, sulfate, nitrate and ammonium concentrations, as well as the sum of them called non-refractory submicron aerosol mass concentration ([NR-PM1]) are discussed. NR-PM1 concentrations generally increase from remote to urban sites. They are mostly larger in the mid-latitude band than in southern and northern Europe. On average, organics account for the major part (36–64%) of NR-PM1 followed by sulfate (12–44%) and nitrate (6–35%). The annual mean chemical composition of NR-PM1 at rural (or regional background) sites and urban background sites are very similar. Considering rural and regional background sites only, nitrate contribution is higher and sulfate contribution is lower in mid-latitude Europe compared to northern and southern Europe. Large seasonal variations in concentrations (μg/m³) of one or more components of NR-PM1 can be observed at all sites, as well as in the chemical composition of NR-PM1 (%) at most sites. Significant diel cycles in the contribution to [NR-PM1] of organics, sulfate, and nitrate can be observed at a majority of sites both in winter and summer. Early morning minima in organics in concomitance with maxima in nitrate are common features at regional and urban background sites. Daily variations are much smaller at a number of coastal and rural sites. Looking at NR-PM1 chemical composition as a function of NR-PM1 mass concentration reveals that although organics account for the major fraction of NR-PM1 at all concentration levels at most sites, nitrate contribution generally increases with NR-PM1 mass concentration and predominates when NR-PM1 mass concentrations exceed 40 μg/m³ at half of the sites

The evolving SARS-CoV-2 epidemic in Africa: Insights from rapidly expanding genomic surveillance

INTRODUCTION Investment in Africa over the past year with regard to severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) sequencing has led to a massive increase in the number of sequences, which, to date, exceeds 100,000 sequences generated to track the pandemic on the continent. These sequences have profoundly affected how public health officials in Africa have navigated the COVID-19 pandemic. RATIONALE We demonstrate how the first 100,000 SARS-CoV-2 sequences from Africa have helped monitor the epidemic on the continent, how genomic surveillance expanded over the course of the pandemic, and how we adapted our sequencing methods to deal with an evolving virus. Finally, we also examine how viral lineages have spread across the continent in a phylogeographic framework to gain insights into the underlying temporal and spatial transmission dynamics for several variants of concern (VOCs). RESULTS Our results indicate that the number of countries in Africa that can sequence the virus within their own borders is growing and that this is coupled with a shorter turnaround time from the time of sampling to sequence submission. Ongoing evolution necessitated the continual updating of primer sets, and, as a result, eight primer sets were designed in tandem with viral evolution and used to ensure effective sequencing of the virus. The pandemic unfolded through multiple waves of infection that were each driven by distinct genetic lineages, with B.1-like ancestral strains associated with the first pandemic wave of infections in 2020. Successive waves on the continent were fueled by different VOCs, with Alpha and Beta cocirculating in distinct spatial patterns during the second wave and Delta and Omicron affecting the whole continent during the third and fourth waves, respectively. Phylogeographic reconstruction points toward distinct differences in viral importation and exportation patterns associated with the Alpha, Beta, Delta, and Omicron variants and subvariants, when considering both Africa versus the rest of the world and viral dissemination within the continent. Our epidemiological and phylogenetic inferences therefore underscore the heterogeneous nature of the pandemic on the continent and highlight key insights and challenges, for instance, recognizing the limitations of low testing proportions. We also highlight the early warning capacity that genomic surveillance in Africa has had for the rest of the world with the detection of new lineages and variants, the most recent being the characterization of various Omicron subvariants. CONCLUSION Sustained investment for diagnostics and genomic surveillance in Africa is needed as the virus continues to evolve. This is important not only to help combat SARS-CoV-2 on the continent but also because it can be used as a platform to help address the many emerging and reemerging infectious disease threats in Africa. In particular, capacity building for local sequencing within countries or within the continent should be prioritized because this is generally associated with shorter turnaround times, providing the most benefit to local public health authorities tasked with pandemic response and mitigation and allowing for the fastest reaction to localized outbreaks. These investments are crucial for pandemic preparedness and response and will serve the health of the continent well into the 21st century

Long-term real-time chemical characterization of submicron aerosols at Montsec (southern Pyrenees, 1570 m a.s.l.)

Real-time measurements of inorganic (sulfate, nitrate, ammonium, chloride and black carbon (BC)) and organic submicron aerosols (particles with an aerodynamic diameter of less than 1 μm) from a continental background site (Montsec, MSC, 1570 m a.s.l.) in the western Mediterranean Basin (WMB) were conducted for 10 months (July 2011–April 2012). An aerosol chemical speciation monitor (ACSM) was co-located with other online and offline PM₁ measurements. Analyses of the hourly, diurnal, and seasonal variations are presented here, for the first time, for this region. <br><br> Seasonal trends in PM₁ components are attributed to variations in evolution of the planetary boundary layer (PBL) height, air mass origin, and meteorological conditions. In summer, the higher temperature and solar radiation increases convection, enhancing the growth of the PBL and the transport of anthropogenic pollutants towards high altitude sites. Furthermore, the regional recirculation of air masses over the WMB creates a continuous increase in the background concentrations of PM₁ components and causes the formation of reservoir layers at relatively high altitudes. The combination of all these atmospheric processes results in a high variability of PM₁ components, with poorly defined daily patterns, except for the organic aerosols (OA). OA was mostly composed (up to 90%) of oxygenated organic aerosol (OOA), split in two types: semivolatile (SV-OOA) and low-volatility (LV-OOA), the rest being hydrocarbon-like OA (HOA). The marked diurnal cycles of OA components regardless of the air mass origin indicates that they are not only associated with anthropogenic and long-range-transported secondary OA (SOA) but also with recently produced biogenic SOA. <br><br> Very different conditions drive the aerosol phenomenology in winter at MSC. The thermal inversions and the lower vertical development of the PBL leave MSC in the free troposphere most of the day, being affected by PBL air masses only after midday, when the mountain breezes transport emissions from the adjacent valleys and plains to the top of the mountain. This results in clear diurnal patterns of both organic and inorganic concentrations. OA was also mainly composed (71%) of OOA, with contributions from HOA (5%) and biomass burning OA (BBOA; 24%). Moreover, in winter sporadic long-range transport from mainland Europe is observed. <br><br> The results obtained in the present study highlight the importance of SOA formation processes at a remote site such as MSC, especially in summer. Additional research is needed to characterize the sources and processes of SOA formation at remote sites

A new method for long-term source apportionment with time-dependent factor profiles and uncertainty assessment using SoFi Pro: application to 1 year of organic aerosol data

A new methodology for performing long-term source apportionment (SA) using positive matrix factorization (PMF) is presented. The method is implemented within the SoFi Pro software package and uses the multilinear engine (ME-2) as a PMF solver. The technique is applied to a 1-year aerosol chemical speciation monitor (ACSM) dataset from downtown Zurich, Switzerland. The measured organic aerosol mass spectra were analyzed by PMF using a small (14 d) and rolling PMF window to account for the temporal evolution of the sources. The rotational ambiguity is explored and the uncertainties of the PMF solutions were estimated. Factor–tracer correlations for averaged seasonal results from the rolling window analysis are higher than those retrieved from conventional PMF analyses of individual seasons, highlighting the improved performance of the rolling window algorithm for long-term data. In this study four to five factors were tested for every PMF window. Factor profiles for primary organic aerosol from traffic (HOA), cooking (COA) and biomass burning (BBOA) were constrained. Secondary organic aerosol was represented by either the combination of semi-volatile and low-volatility organic aerosol (SV-OOA and LV-OOA, respectively) or by a single OOA when this separation was not robust. This scheme led to roughly 40 000 PMF runs. Full visual inspection of all these PMF runs is unrealistic and is replaced by predefined user-selected criteria, which allow factor sorting and PMF run acceptance/rejection. The selected criteria for traffic (HOA) and BBOA were the correlation with equivalent black carbon from traffic (eBCtr) and the explained variation of 60, respectively. COA was assessed by the prominence of a lunchtime concentration peak within the diurnal cycle. SV-OOA and LV-OOA were evaluated based on the fractions of 43 and 44 in their respective factor profiles. Seasonal pre-tests revealed a non-continuous separation of OOA into SV-OOA and LV-OOA, in particular during the warm seasons. Therefore, a differentiation between four-factor solutions (HOA, COA, BBOA and OOA) and five-factor solutions (HOA, COA, BBOA, SV-OOA and LV-OOA) was also conducted based on the criterion for SV-OOA. HOA and COA contribute between 0.4–0.7 µg m−3 (7.8 %–9.0 %) and 0.7–1.2 µg m−3 (12.2 %–15.7 %) on average throughout the year, respectively. BBOA shows a strong yearly cycle with the lowest mean concentrations in summer (0.6 µg m−3, 12.0 %), slightly higher mean concentrations during spring and fall (1.0 and 1.5 µg m−3, or 15.6 % and 18.6 %, respectively), and the highest mean concentrations during winter (1.9 µg m−3, 25.0 %). In summer, OOA is separated into SV-OOA and LV-OOA, with mean concentrations of 1.4 µg m−3 (26.5 %) and 2.2 µg m−3 (40.3 %), respectively. For the remaining seasons the seasonal concentrations of SV-OOA, LV-OOA and OOA range from 0.3 to 1.1 µg m−3 (3.4 %–15.9 %), from 0.6 to 2.2 µg m−3 (7.7 %–33.7 %) and from 0.9 to 3.1 µg m−3 (13.7 %–39.9 %), respectively. The relative PMF errors modeled for this study for HOA, COA, BBOA, LV-OOA, SV-OOA and OOA are on average ±34 %, ±27 %, ±30 %, ±11 %, ±25 % and ±12 %, respectively

Characterization and source apportionment of organic aerosol using offline aerosol mass spectrometry

Field deployments of the Aerodyne Aerosol Mass Spectrometer (AMS) have significantly advanced real-time measurements and source apportionment of non-refractory particulate matter. However, the cost and complex maintenance requirements of the AMS make its deployment at sufficient sites to determine regional characteristics impractical. Furthermore, the negligible transmission efficiency of the AMS inlet for supermicron particles significantly limits the characterization of their chemical nature and contributing sources. In this study, we utilize the AMS to characterize the water-soluble organic fingerprint of ambient particles collected onto conventional quartz filters, which are routinely sampled at many air quality sites. The method was applied to 256 particulate matter (PM) filter samples (PM1, PM2:5, and PM10, i.e., PM with aerodynamic diameters smaller than 1, 2.5, and 10 μm, respectively), collected at 16 urban and rural sites during summer and winter. We show that the results obtained by the present technique compare well with those from co-located online measurements, e.g., AMS or Aerosol Chemical Speciation Monitor (ACSM). The bulk recoveries of organic aerosol (60–91 %) achieved using this technique, together with low detection limits (0.8 μg of organic aerosol on the analyzed filter fraction) allow its application to environmental samples. We will discuss the recovery variability of individual hydrocarbon ions, ions containing oxygen, and other ions. The performance of such data in source apportionment is assessed in comparison to ACSM data. Recoveries of organic components related to different sources as traffic, wood burning, and secondary organic aerosol are presented. This technique, while subjected to the limitations inherent to filter-based measurements (e.g., filter artifacts and limited time resolution) may be used to enhance the AMS capabilities in measuring size-fractionated, spatially resolved longterm data sets