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High-altitude remote sites are unique places to study aerosol-cloud interactions since they are located at the altitude where clouds may form. At these remote sites, organic aerosols (OA) are the main constituents of the overall aerosol population, playing a crucial role in defining aerosol hygroscopicity (κ). To estimate the CCN budget at OA dominated sites, it is crucial to accurately characterize OA hygroscopicity (κOA) and how its temporal variability affects the CCN activity of the aerosol population since κOA is not well established due to complex nature of ambient OA. In this study, we performed CCN closures at a high-altitude remote site during summer season to investigate the role of κOA in predicting CCN concentrations under different atmospheric conditions. In addition, we performed an OA source apportionment using Positive Matrix Factorization (PMF). Three OA factors were identified from the PMF analysis: hydrocarbon-like OA (HOA), less-oxidized oxygenated OA (LO-OOA) and more-oxidized oxygenated OA (MO-OOA), with average contributions of 5 %, 36 % and 59 % of the total OA, respectively. This result highlights the predominance of secondary organic aerosol with high degree of oxidation at this high-altitude site. To understand the impact of each OA factor on the overall OA hygroscopicity we defined three κOA schemes that assume different hygroscopicity values for each OA factor. Our results show that the different κOA schemes lead to similar CCN closure results between observations and predictions (slope and correlation ranging between 1.08–1.40 and 0.89–0.94, respectively). However, the predictions were not equally accurate across the day. During nighttime, CCN predictions underestimated observations by 6–16 %, while during morning and midday hours, when the aerosol was influenced by vertical transport of particles and/or new particle formation events, CCN concentrations were overestimated by 0–20 %. To further evaluate the role of κOA in CCN predictions, we established a new OA scheme that uses the OA oxidation level (parameterized by the f44 factor) to calculate κOA and predict CCN. This method also shows a large bias, especially during midday hours (up to 40 %), indicating that diurnal information about the oxygenation degree does not improve CCN predictions. Finally, we used a neural network model with four inputs: N80 (number concentration of particles with diameter >80 nm), OA fraction, f44 and surface global radiation) to predict CCN. This model matched the observations better than the previous approaches, with a bias within ±10 % and with no daily variation, reproducing the CCN variability along the day. Therefore, neural network models seem to be an appropriate tool to estimate CCN concentrations using ancillary parameters accordingly. [ABSTRACT FROM AUTHOR]

Light-absorbing aerosols (LAAs) are short-lived climate forcers with a significant impact on Earth's radiative balance. LAAs include dust aerosols, black carbon (BC) and organic light-absorbing carbonaceous aerosol (collectively termed brown carbon, BrC), which have also been proven to be highly toxic. In this study, aerosol absorption at five wavelengths (ranging from ultraviolet to infrared) was monitored continuously using filter-based photometers during two winter seasons in 2020 and 2021 in the city of Modena (southern central Po Valley, northern Italy), at two regulatory air quality monitoring sites, along with other pollutants (coarse particulate matter, PM 10 ; fine particulate matter, PM 2.5 ; O 3 ; NO; NO 2 ; and C 6 H 6) and the vehicular traffic rate. The aerosol optical depth (AOD) and other column aerosol optical properties were concurrently monitored at four wavelengths by an AErosol RObotic NETwork (AERONET) sun photometer under urban background conditions within Modena. In situ absorption levels were apportioned to both sources (fossil fuel and biomass burning) and species (BC and BrC), while columnar absorption was apportioned to BC, BrC and mineral dust. The combined analysis of the atmospheric aerosol and gas measurements and of the meteorological conditions (in situ and from the ERA5 reanalysis) identified the location of potential urban sources of BC and BrC, most likely related to traffic and biomass burning. In situ data show different diurnal/weekly patterns for BrC from biomass burning and BC from traffic, with minor differences between the background and the urban traffic conditions. AERONET version 3 absorption aerosol optical depth (AAOD) retrievals at four wavelengths allowed the estimation of the absorptive direct radiative effect due to LAAs over the same period under the reasonable assumption that the AOD signal is concentrated within the mixing layer. AERONET retrievals showed a modest correlation of columnar absorption with planetary boundary layer (PBL)-scaled in situ observations, although the correlation improved significantly during a desert dust transport event that affected both in situ aerosol and columnar absorption, particularly in the blue spectrum range. A low correlation occurred between the contribution of BrC to aerosol absorption for the in situ and the columnar observations, with the BrC contribution being generally larger for in situ observations. Finally, evidence of a highly layered atmosphere during the study period, featuring significant spatial mixing and modest vertical mixing, was shown by ERA5-based atmospheric temperature profiles and by the large correlation of concurrent AERONET AOD retrievals in Modena and in Ispra (on the northwestern side of the Po Valley, ca. 225 km from Modena). [ABSTRACT FROM AUTHOR]

Between April 2002 and June 2017, the Global Monitoring Laboratory (GML) of the National Oceanic and Atmospheric Administration (NOAA) made continuous measurements of a suite of in situ aerosol optical properties at a long-term monitoring site near Trinidad Head (THD), California. In addition to aerosol optical properties, between 2002–2006 a scanning humidograph system was operated, and inorganic ion and total aerosol mass concentrations were obtained from filter measurements. A combined analysis of these datasets demonstrates consistent patterns in aerosol climatology and highlights changes in sources throughout the year. THD is predictably dominated by sea salt aerosols; however, marine biogenic aerosols are the largest contributor to PM 1 in the warmer months. Additionally, a persistent combustion source appears in the winter, likely a result of wintertime home heating. While the influences of local anthropogenic sources from vehicular and marine traffic are visible in the optical aerosol data, their influence is largely dictated by the wind direction at the site. Comparison of the THD aerosol climatology to that reported for other marine sites shows that the location is representative of clean marine measurements, even with the periodic influence of anthropogenic sources. [ABSTRACT FROM AUTHOR]

Between April 2002 and June 2017, the National Oceanic and Atmospheric Administration (NOAA) Earth System Research Laboratory (ESRL) made continuous measurements of a suite of in-situ aerosol optical properties at a long-term monitoring site near Trinidad Head (THD), California. In addition to aerosol optical properties, between 2002–2006 a scanning humidograph system was operated and inorganic ion and total aerosol mass concentrations were obtained from filter measurements. Combined analysis of these datasets demonstrates consistent patterns in aerosol climatology and highlights changes in sources throughout the year. THD is predictably dominated by sea salt aerosols, however, marine biogenic aerosols are the largest contributor to PM1 in the warmer months. Additionally, a persistent combustion source appears in the winter, likely a result of wintertime home heating. While the influences of local anthropogenic sources from vehicular and marine traffic are visible in the optical aerosol data, their influence is largely dictated by wind direction at the site. Comparison of the THD aerosol climatology to that reported for other marine sites shows that the location is representative of clean marine measurements, even with the periodic influence of anthropogenic sources. [ABSTRACT FROM AUTHOR]

Light Absorbing Aerosols (LAA) are short-lived climate forcers with a significant impact on Earth radiative balance and include dust aerosols, Black Carbon (BC) and organic light-absorbing carbonaceous aerosol (collectively termed as Brown Carbon, BrC), which have been also proven to be highly toxic. Aerosol absorption at 5 wavelengths (UV, B, G, R, IR) by filter photometer was monitored continuously during two winter seasons in 2020 and 2021 in the city of Modena (South-central Po valley, Northern Italy) at the two regulatory air quality monitoring sites, along with other pollutants (PM10, PM2.5, O3, NO, NO2, C6H6) and vehicular traffic rate. Columnar levels of AOD and of other aerosol optical properties were concurrently monitored at multiple wavelengths by a local sun-photometer at urban background conditions and within the AERONET network. In-situ absorption levels were apportioned both to sources (fossil fuel, biomass burning) and to species (BC, BrC), while columnar absorption was apportioned to BC, BrC and mineral dust. The combined analysis of the atmospheric aerosol and gas levels and of the meteorological conditions (in-situ and by ERA5 reanalysis) identified the location of potential urban sources for BC and BrC, most likely traffic and biomass burning. In-situ data shown different diurnal/weekly patterns for BrC by biomass burning and BC by traffic, with minor differences among the background and the traffic urban conditions. AERONET version 3 Absorption Aerosol Optical Depth (AAOD) retrievals at 4 wavelengths allowed the estimate of the Absorptive Direct Radiative Effect by LAA over the same period under the reasonable assumption that the AOD signal is built up within the mixing layer. AERONET retrievals showed a modest correlation of columnar absorption with PBL-scaled in-situ observations, although the correlation improves significantly during a desert dust transport event, affecting both in-situ aerosol and columnar absorption, particularly in the Blue spectrum range. Low correlation occurred between the contribution of BrC aerosol absorption for the in-situ and the columnar observations, with this contribution being generally larger at the former. Finally, evidences of a strongly layered atmosphere during the study period, featured by large spatial mixing and modest vertical mixing, were shown by ERA5-based atmospheric temperature profiles and by the large correlation of concurrent AERONET AOD retrievals in Modena and in Ispra (on the NW side of the Po valley, ca. 225 km distant from Modena). [ABSTRACT FROM AUTHOR]

PurpleAir sensors (PASs) are low-cost tools to measure fine particulate matter (PM) concentrations and are now widely used, especially in regions with few regulatory monitors. However, the raw PAS data have significant biases, so the sensors must be calibrated to generate accurate data. The U.S. EPA recently developed a national correction equation and has integrated corrected PAS data onto its AirNow website. This integration results in much better spatial coverage for PM 2.5 (particulate matter with diameters less than 2.5 µ m) across the US. The goal of our study is to evaluate the EPA correction equation for three different types of aerosols: typical urban wintertime aerosol, smoke from biomass burning, and mineral dust. We identified 50 individual pollution events, each having a peak hourly PM 2.5 concentration of at least 47 µ g m -3 and a minimum of 3 h over 40 µ g m -3 and characterized the primary aerosol type as either typical urban, smoke, or long-range transported dust. For each event, we paired a PAS sampling outside air with a nearby regulatory PM 2.5 monitor to evaluate the agreement. All 50 events show statistically significant correlations (R values between 0.71–1.00) between the hourly PAS and regulatory data but with varying slopes. We then corrected the PAS data using either the correction equation from Barkjohn et al. (2021) or a new equation that is now being used by the U.S. EPA for the AirNow Fire and Smoke Map (U.S. EPA, 2022b). Both equations do a good job at correcting the data for smoke and typical pollution events but with some differences. Using the Barkjohn et al. (2021) equation, we find mean slopes of 1.00 and 0.99 for urban and smoke aerosol events, respectively, for the corrected data versus the regulatory data. For heavy smoke events, we find a small change in the slope at very high PM 2.5 concentrations (> 600 µ g m -3), suggesting a ∼ 20 % underestimate in the corrected PAS data at these extremely high concentrations. Using the new EPA equation, we find slopes of 0.95 and 0.88 for urban and smoke events, respectively, indicating a slight underestimate in PM 2.5 using this equation, especially for smoke events. For dust events, while the PAS and regulatory data still show significant correlations, the PAS data using either correction equation underestimate the true PM 2.5 by a factor of 5–6. We also examined several years of co-located regulatory and PAS data from a site near Owens Lake, California (CA), which experiences high concentrations of PM 2.5 due to both smoke and locally emitted dust. For this site, we find similar results as above; the corrected PAS data are accurate in smoke but are too low by a factor of 5–6 in dust. Using these data, we also find that the ratios of PAS-measured PM 10 / PM 1 mass and 0.3 µ m / 5 µ m particle counts are significantly different for dust compared to smoke. Using this difference, we propose a modified correction equation that improves the PAS data for some dust events, but further work is needed to improve this algorithm. [ABSTRACT FROM AUTHOR]

PurpleAir Sensors (PASs) are low-cost tools to measure fine particulate matter (PM) concentrations and are now widely used, especially in regions with few regulatory monitors. However, the raw PAS data have significant biases, so the sensors must be calibrated to generate accurate data. The U.S. EPA recently developed a national correction equation and have integrated corrected PAS data onto its AirNow website. This integration results in much better spatial coverage for PM2.5 across the U.S. The goal of our study is to evaluate the EPA correction equation for three different types of aerosols: typical urban wintertime aerosol, smoke from biomass burning, and mineral dust. We identified 50 individual pollution events, each having a peak hourly PM2.5 concentration of at least 47 µg m-3 and a minimum of 3 hours over 40 µg m-3 and characterize the primary aerosol type as either typical urban, smoke or dust. For each event, we paired an PAS sampling outside air with a nearby regulatory PM2.5 monitor to evaluate the agreement. All 50 events show statistically significant correlations (R values between 0.71-1.00) between the hourly PAS and regulatory data, but with varying slopes. Using the standard EPA correction for the typical urban and smoke aerosols, we find average slopes of 1.00 and 0.99, respectively. This means that the standard EPA correction is highly effective at generating accurate data for these aerosol types. For heavy smoke events, we find a small change in the slope at very high PM2.5 concentrations (>600µg m-3), suggesting a ~20% under-estimate in the corrected PAS data at these extremely high concentrations. For dust events, while the PAS and regulatory data still show significant correlations, the PAS data using the standard correction underestimates the true PM2.5 by a factor of 5-6. We also examined several years of co-located regulatory and PAS data from a site near Owens Lake, CA, which experiences high concentrations of PM2.5 due to both smoke and dust. For this site we find similar results as above; the PAS corrected data are accurate in smoke, but are too low by a factor of 5-6 in dust. Using these data we also find that the ratios of PAS measured PM10 to PM1 mass and 0.3 µm to 5 µm particle counts are significantly different for dust compared to smoke. Given the ability of the PAS data to identify dust aerosols, we propose a modified correction algorithm that significantly improves the PAS data for dust events. [ABSTRACT FROM AUTHOR]

Optical properties of surface aerosols at Dome C, Antarctica, in 2007–2013 and their potential source areas are presented. Scattering coefficients (σsp) were calculated from measured particle number size distributions with a Mie code and from filter samples using mass scattering efficiencies. Absorption coefficients (σap) were determined with a three-wavelength Particle Soot Absorption Photometer (PSAP) and corrected for scattering by using two different algorithms. The scattering coefficients were also compared with σsp measured with a nephelometer at the South Pole Station (SPO). The minimum σap was observed in the austral autumn and the maximum in the austral spring, similar to other Antarctic sites. The darkest aerosol, i.e., the lowest single-scattering albedo ωo≈0.91 , was observed in September and October and the highest ωo≈0.99 in February and March. The uncertainty of the absorption Ångström exponent αap is high. The lowest αap monthly medians were observed in March and the highest in August–October. The equivalent black carbon (eBC) mass concentrations were compared with eBC measured at three other Antarctic sites: the SPO and two coastal sites, Neumayer and Syowa. The maximum monthly median eBC concentrations are almost the same (∼3±1 ng m -3) at all these sites in October–November. This suggests that there is no significant difference in eBC concentrations between the coastal and plateau sites. The seasonal cycle of the eBC mass fraction exhibits a minimum f (eBC) ≈0.1 % in February–March and a maximum ∼4 %–5 % in August–October. Source areas were calculated using 50 d FLEXPART footprints. The highest eBC concentrations and the lowest ωo were associated with air masses coming from South America, Australia and Africa. Vertical simulations that take BC particle removal processes into account show that there would be essentially no BC particles arriving at Dome C from north of latitude 10 ∘ S at altitudes <1600 m. The main biomass-burning regions Africa, Australia and Brazil are more to the south, and their smoke plumes have been observed at higher altitudes than that, so they can get transported to Antarctica. The seasonal cycle of BC emissions from wildfires and agricultural burning and other fires in South America, Africa and Australia was calculated from data downloaded from the Global Fire Emissions Database (GFED). The maximum total emissions were in August–September, but the peak of monthly average eBC concentrations is observed 2–3 months later in November, not only at Dome C, but also at the SPO and the coastal stations. The air-mass residence-time-weighted BC emissions from South America are approximately an order of magnitude larger than from Africa and Oceania, suggesting that South American BC emissions are the largest contributors to eBC at Dome C. At Dome C the maximum and minimum scattering coefficients were observed in austral summer and winter, respectively. At the SPO σsp was similar to that observed at Dome C in the austral summer, but there was a large difference in winter, suggesting that in winter the SPO is more influenced by sea-spray emissions than Dome C. The seasonal cycles of σsp at Dome C and at the SPO were compared with the seasonal cycles of secondary and primary marine aerosol emissions. The σsp measured at the SPO correlated much better with the sea-spray aerosol emission fluxes in the Southern Ocean than σsp at Dome C. The seasonal cycles of biogenic secondary aerosols were estimated from monthly average phytoplankton biomass concentrations obtained from the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) satellite sensor data. The analysis suggests that a large fraction of the biogenic scattering aerosol observed at Dome C has been formed in the polar zone, but it may take a month for the aerosol to be formed, be grown and get transported from the sea level to Dome C. [ABSTRACT FROM AUTHOR]

Even though the Arctic is remote, aerosol properties observed there are strongly influenced by anthropogenic emissions from outside the Arctic. This is particularly true for the so-called Arctic haze season (January through April). In summer (June through September), when atmospheric transport patterns change, and precipitation is more frequent, local Arctic sources, i.e., natural sources of aerosols and precursors, play an important role. Over the last few decades, significant reductions in anthropogenic emissions have taken place. At the same time a large body of literature shows evidence that the Arctic is undergoing fundamental environmental changes due to climate forcing, leading to enhanced emissions by natural processes that may impact aerosol properties. In this study, we analyze 9 aerosol chemical species and 4 particle optical properties from 10 Arctic observatories (Alert, Kevo, Pallas, Summit, Thule, Tiksi, Barrow/Utqiaġvik, Villum, and Gruvebadet and Zeppelin Observatory – both at Ny-Ålesund Research Station) to understand changes in anthropogenic and natural aerosol contributions. Variables include equivalent black carbon, particulate sulfate, nitrate, ammonium, methanesulfonic acid, sodium, iron, calcium and potassium, as well as scattering and absorption coefficients, single scattering albedo and scattering Ångström exponent. First, annual cycles are investigated, which despite anthropogenic emission reductions still show the Arctic haze phenomenon. Second, long-term trends are studied using the Mann–Kendall Theil–Sen slope method. We find in total 41 significant trends over full station records, i.e., spanning more than a decade, compared to 26 significant decadal trends. The majority of significantly declining trends is from anthropogenic tracers and occurred during the haze period, driven by emission changes between 1990 and 2000. For the summer period, no uniform picture of trends has emerged. Twenty-six percent of trends, i.e., 19 out of 73, are significant, and of those 5 are positive and 14 are negative. Negative trends include not only anthropogenic tracers such as equivalent black carbon at Kevo, but also natural indicators such as methanesulfonic acid and non-sea-salt calcium at Alert. Positive trends are observed for sulfate at Gruvebadet. No clear evidence of a significant change in the natural aerosol contribution can be observed yet. However, testing the sensitivity of the Mann–Kendall Theil–Sen method, we find that monotonic changes of around 5 % yr -1 in an aerosol property are needed to detect a significant trend within one decade. This highlights that long-term efforts well beyond a decade are needed to capture smaller changes. It is particularly important to understand the ongoing natural changes in the Arctic, where interannual variability can be high, such as with forest fire emissions and their influence on the aerosol population. To investigate the climate-change-induced influence on the aerosol population and the resulting climate feedback, long-term observations of tracers more specific to natural sources are needed, as well as of particle microphysical properties such as size distributions, which can be used to identify changes in particle populations which are not well captured by mass-oriented methods such as bulk chemical composition. [ABSTRACT FROM AUTHOR]

The Plantower PMS5003 sensors (PMS) used in the PurpleAir monitor PA-II-SD configuration (PA-PMS) are equivalent to cell-reciprocal nephelometers using a 657 nm perpendicularly polarized light source that integrates light scattering from 18 to 166 ∘. Yearlong field data at the National Oceanic and Atmospheric Administration's (NOAA) Mauna Loa Observatory (MLO) and Boulder Table Mountain (BOS) sites show that the 1 h average of the PA-PMS first size channel, labeled " > 0.3 µ m" ("CH1"), is highly correlated with submicrometer aerosol scattering coefficients at the 550 and 700 nm wavelengths measured by the TSI 3563 integrating nephelometer, from 0.4 to 500 Mm -1. This corresponds to an hourly average submicrometer aerosol mass concentration of approximately 0.2 to 200 µ g m -3. A physical–optical model of the PMS is developed to estimate light intensity on the photodiode, accounting for angular truncation of the volume scattering function as a function of particle size. The model predicts that the PMS response to particles > 0.3 µ m decreases relative to an ideal nephelometer by about 75 % for particle diameters ≥ 1.0 µ m. This is a result of using a laser that is polarized, the angular truncation of the scattered light, and particle losses (e.g., due to aspiration) before reaching the laser. It is shown that CH1 is linearly proportional to the model-predicted intensity of the light scattered by particles in the PMS laser to its photodiode over 4 orders of magnitude. This is consistent with CH1 being a measure of the scattering coefficient and not the particle number concentration or particulate matter concentration. The model predictions are consistent with data from published laboratory studies which evaluated the PMS against a variety of aerosols. Predictions are then compared with yearlong fine aerosol size distribution and scattering coefficient field data at the BOS site. Field data at BOS confirm the model prediction that the ratio of CH1 to the scattering coefficient would be highest for aerosols with median scattering diameters < 0.3 µ m. The PMS detects aerosols smaller than 0.3 µ m diameter in proportion to their contribution to the scattering coefficient. The results of this study indicate that the PMS is not an optical particle counter and that its six size fractions are not a meaningful representation of particle size distribution. The relationship between the PMS 1 h average CH1 and bsp1 , the scattering coefficient in Mm -1 due to particles below 1 µ m aerodynamic diameter, at wavelength 550 nm, is found to be bsp1 = 0.015 ± 2.07 × 10 -5 × CH1, for relative humidity below 40 %. The coefficient of determination r2 is 0.97. This suggests that the low-cost and widely used PA monitors can be used to measure and predict the submicron aerosol light scattering coefficient in the mid-visible nearly as well as integrating nephelometers. The effectiveness of the PA-PMS to serve as a PM 2.5 mass concentration monitor is due to both the sensor behaving like an imperfect integrating nephelometer and the mass scattering efficiency of ambient PM 2.5 aerosols being roughly constant. [ABSTRACT FROM AUTHOR]

Aerosol particles are a complex component of the atmospheric system which influence climate directly by interacting with solar radiation, and indirectly by contributing to cloud formation. The variety of their sources, as well as the multiple transformations they may undergo during their transport (including wet and dry deposition), result in significant spatial and temporal variability of their properties. Documenting this variability is essential to provide a proper representation of aerosols and cloud condensation nuclei (CCN) in climate models. Using measurements conducted in 2016 or 2017 at 62 ground-based stations around the world, this study provides the most up-to-date picture of the spatial distribution of particle number concentration (Ntot) and number size distribution (PNSD, from 39 sites). A sensitivity study was first performed to assess the impact of data availability on Ntot 's annual and seasonal statistics, as well as on the analysis of its diel cycle. Thresholds of 50 % and 60 % were set at the seasonal and annual scale, respectively, for the study of the corresponding statistics, and a slightly higher coverage (75 %) was required to document the diel cycle. Although some observations are common to a majority of sites, the variety of environments characterizing these stations made it possible to highlight contrasting findings, which, among other factors, seem to be significantly related to the level of anthropogenic influence. The concentrations measured at polar sites are the lowest (∼ 10 2 cm -3) and show a clear seasonality, which is also visible in the shape of the PNSD, while diel cycles are in general less evident, due notably to the absence of a regular day–night cycle in some seasons. In contrast, the concentrations characteristic of urban environments are the highest (∼ 10 3 –10 4 cm -3) and do not show pronounced seasonal variations, whereas diel cycles tend to be very regular over the year at these stations. The remaining sites, including mountain and non-urban continental and coastal stations, do not exhibit as obvious common behaviour as polar and urban sites and display, on average, intermediate Ntot (∼ 10 2 –10 3 cm -3). Particle concentrations measured at mountain sites, however, are generally lower compared to nearby lowland sites, and tend to exhibit somewhat more pronounced seasonal variations as a likely result of the strong impact of the atmospheric boundary layer (ABL) influence in connection with the topography of the sites. ABL dynamics also likely contribute to the diel cycle of Ntot observed at these stations. Based on available PNSD measurements, CCN-sized particles (considered here as either >50 nm or >100 nm) can represent from a few percent to almost all of Ntot , corresponding to seasonal medians on the order of ∼ 10 to 1000 cm -3 , with seasonal patterns and a hierarchy of the site types broadly similar to those observed for Ntot. Overall, this work illustrates the importance of in situ measurements, in particular for the study of aerosol physical properties, and thus strongly supports the development of a broad global network of near surface observatories to increase and homogenize the spatial coverage of the measurements, and guarantee as well data availability and quality. The results of this study also provide a valuable, freely available and easy to use support for model comparison and validation, with the ultimate goal of contributing to improvement of the representation of aerosol–cloud interactions in models, and, therefore, of the evaluation of the impact of aerosol particles on climate. [ABSTRACT FROM AUTHOR]

Long-term measurements of atmospheric mass concentrations of black carbon (BC) are needed to investigate changes in its emission, transport, and deposition. However, depending on instrumentation, parameters related to BC such as aerosol absorption coefficient (babs) have been measured instead. Most ground-based measurements of babs in the Arctic have been made by filter-based absorption photometers, including particle soot absorption photometers (PSAPs), continuous light absorption photometers (CLAPs), Aethalometers, and multi-angle absorption photometers (MAAPs). The measured babs can be converted to mass concentrations of BC (MBC) by assuming the value of the mass absorption cross section (MAC; MBC= babs/ MAC). However, the accuracy of conversion of babs to MBC has not been adequately assessed. Here, we introduce a systematic method for deriving MAC values from babs measured by these instruments and independently measured MBC. In this method, MBC was measured with a filter-based absorption photometer with a heated inlet (COSMOS). COSMOS-derived MBC (MBC (COSMOS)) is traceable to a rigorously calibrated single particle soot photometer (SP2), and the absolute accuracy of MBC (COSMOS) has been demonstrated previously to be about 15 % in Asia and the Arctic. The necessary conditions for application of this method are a high correlation of the measured babs with independently measured MBC and long-term stability of the regression slope, which is denoted as MAC cor (MAC derived from the correlation). In general, babs – MBC (COSMOS) correlations were high (r2= 0.76–0.95 for hourly data) at Alert in Canada, Ny-Ålesund in Svalbard, Barrow (NOAA Barrow Observatory) in Alaska, Pallastunturi in Finland, and Fukue in Japan and stable for up to 10 years. We successfully estimated MAC cor values (10.8–15.1 m 2 g -1 at a wavelength of 550 nm for hourly data) for these instruments, and these MAC cor values can be used to obtain error-constrained estimates of MBC from babs measured at these sites even in the past, when COSMOS measurements were not made. Because the absolute values of MBC at these Arctic sites estimated by this method are consistent with each other, they are applicable to the study of spatial and temporal variation in MBC in the Arctic and to evaluation of the performance of numerical model calculations. [ABSTRACT FROM AUTHOR]

Even though the Arctic is remote, aerosol properties observed there are strongly influenced by anthropogenic emissions from outside the Arctic. This is particularly true for the so-called Arctic haze season (January through April). In summer (June through September), when atmospheric transport patterns change, and precipitation is more frequent, local Arctic, i.e. natural sources of aerosols and precursors, play an important role. Over the last decades, significant reductions in anthropogenic emissions have taken place. At the same time a large body of literature shows evidence that the Arctic is undergoing fundamental environmental changes due to climate forcing, leading to enhanced emissions by natural processes that may impact aerosol properties. In this study, we analyze nine aerosol chemical species and four particle optical properties from ten Arctic observatories (Alert, Gruvebadet, Kevo, Pallas, Summit, Thule, Tiksi, Barrow, Villum, Zeppelin) to understand changes in anthropogenic and natural aerosol contributions. Variables include equivalent black carbon, particulate sulfate, nitrate, ammonium, methanesulfonic acid, sodium, iron, calcium and potassium, as well as scattering and absorption coefficients, single scattering albedo and scattering ngström exponent. First, annual cycles are investigated, which despite anthropogenic emission reductions still show the Arctic haze phenomenon. Second, long-term trends are studied using the Mann-Kendall Theil-Sen slope method. We find in total 28 significant trends over full station records, i.e. spanning more than a decade, compared to 17 significant decadal trends. The majority of significantly declining trends is from anthropogenic tracers and occurred during the haze period, driven by emission changes between 1990 and 2000. For the summer period, no uniform picture of trends has emerged. Twenty-one percent of trends, i.e. eleven out of 57, are significant, and of those five are positive and six are negative. Negative trends include not only anthropogenic tracers such as equivalent black carbon at Kevo, but also natural indicators such as methanesulfonic acid and non-sea salt calcium at Alert. Positive trends are observed for sulfate at Zeppelin and Gruvebadet. No clear evidence of a significant change in the natural aerosol contribution can be observed yet. However, testing the sensitivity of the Mann-Kendall Theil-Sen method, we find that monotonic changes of around 5 % per year in an aerosol property are needed to detect a significant trend within one decade. This highlights that long-term efforts well beyond a decade are needed to capture smaller changes. It is particularly important to understand the ongoing natural changes in the Arctic, where interannual variability can be high, such as with forest fire emissions and their influence on the aerosol population. To investigate the climate-change induced influence on the aerosol population and the resulting climate feedback, long-term observations of tracers more specific to natural sources are needed, as well as of particle microphysical properties such as size distributions, which can be used to identify changes in particle populations which are not well captured by mass-oriented methods such as bulk chemical composition. [ABSTRACT FROM AUTHOR]

The scattering and backscattering enhancement factors (f (RH) and fb (RH)) describe how aerosol particle light scattering and backscattering, respectively, change with relative humidity (RH). They are important parameters in estimating direct aerosol radiative forcing (DARF). In this study we use the dataset presented in that compiles f (RH) and fb (RH) measurements at three wavelengths (i.e., 450, 550 and 700 nm) performed with tandem nephelometer systems at multiple sites around the world. We present an overview of f (RH) and fb (RH) based on both long-term and campaign observations from 23 sites representing a range of aerosol types. The scattering enhancement shows a strong variability from site to site, with no clear pattern with respect to the total scattering coefficient. In general, higher f (RH) is observed at Arctic and marine sites, while lower values are found at urban and desert sites, although a consistent pattern as a function of site type is not observed. The backscattering enhancement fb (RH) is consistently lower than f (RH) at all sites, with the difference between f (RH) and fb (RH) increasing for aerosol with higher f (RH). This is consistent with Mie theory, which predicts higher enhancement of the light scattering in the forward than in the backward direction as the particle takes up water. Our results show that the scattering enhancement is higher for PM 1 than PM 10 at most sites, which is also supported by theory due to the change in scattering efficiency with the size parameter that relates particle size and the wavelength of incident light. At marine-influenced sites this difference is enhanced when coarse particles (likely sea salt) predominate. For most sites, f (RH) is observed to increase with increasing wavelength, except at sites with a known dust influence where the spectral dependence of f (RH) is found to be low or even exhibit the opposite pattern. The impact of RH on aerosol properties used to calculate radiative forcing (e.g., single-scattering albedo, ω0 , and backscattered fraction, b) is evaluated. The single-scattering albedo generally increases with RH, while b decreases. The net effect of aerosol hygroscopicity on radiative forcing efficiency (RFE) is an increase in the absolute forcing effect (negative sign) by a factor of up to 4 at RH = 90 % compared to dry conditions (RH < 40 %). Because of the scarcity of scattering enhancement measurements, an attempt was made to use other more commonly available aerosol parameters (i.e., ω0 and scattering Ångström exponent, αsp) to parameterize f (RH). The majority of sites (75 %) showed a consistent trend with ω0 (higher f (RH = 85 %) for higher ω0), while no clear pattern was observed between f (RH = 85 %) and αsp. This suggests that aerosol ω0 is more promising than αsp as a surrogate for the scattering enhancement factor, although neither parameter is ideal. Nonetheless, the qualitative relationship observed between ω0 and f (RH) could serve as a constraint on global model simulations. [ABSTRACT FROM AUTHOR]

Optical properties of surface aerosols at Dome C, Antarctica in 2007-2013 and their potential source areas are presented. Scattering coefficients (ssp) were calculated from measured particle number size distributions with a Mie code and from filter samples using mass scattering efficiencies. Absorption coefficients (sap) were determined with a 3-wavelength Particle Soot Absorption Photometer (PSAP) and corrected for scattering by using two different algorithms. The scattering coefficients were also compared with ssp measured with a nephelometer at the South Pole Station (SPO). The minimum sap was observed in the austral autumn and the maximum in the austral spring, similar to other Antarctic sites. The darkest aerosol, i.e., the lowest single scattering albedo ?o ˜ 0.91 was observed in September and October and the highest ?o ˜ 0.99 in February and March. The uncertainty of the absorption Ångström exponent aap is high. The lowest aap monthly medians were observed in March and the highest in August – October. The equivalent black carbon (eBC) mass concentrations were compared with eBC measured at three other Antarctic sites: the SPO and two coastal sites, Neumayer and Syowa. The maximum monthly median eBC concentrations are almost the same (~3 ± 1 ng m-3 ) at all these sites in October-November. This suggests that there is no significant difference in eBC between the coastal and plateau sites. The seasonal cycle of the eBC mass fraction exhibits a minimum f(eBC) ˜ 0.1% in February-March and a maximum ~4-5% in August-October. Source areas were calculated using 50-day FLEXPART footprints. The highest eBC concentrations and the lowest ?o were associated with air masses coming from South America, Australia and Africa. Vertical simulations that take BC particle removal processes into account show that there would be essentially no BC particles arriving at Dome C from north of latitude 10°S at altitudes < 1600 m. The main biomass-burning regions Africa, Australia and Brazil are more to the south and their smoke plumes have been observed at higher altitudes than that so they can get transported to Antarctica. The seasonal cycle of BC emissions from wildfires and agricultural burning and other fires in South America, Africa and Australia were calculated from data downloaded from the Global Fire Emissions Database (GFED). The maximum total emissions were in August-September but the peak of monthly average eBC concentrations is observed 2 – 3 months later in November not only at Dome C but also at SPO and the coastal stations. The air mass residence-time-weighted BC emissions from South America are approximately an order of magnitude larger than from Africa and Oceania suggesting that South American BC emissions are the largest contributors to eBC at Dome C. At Dome C the maximum and minimum scattering coefficients were observed in austral summer and winter, respectively. At SPO ssp was similar to that observed at Dome C in the austral summer but there was a large difference in winter, suggesting that in winter SPO is more influenced by sea spray emissions than Dome C. The seasonal cycles of ssp at Dome C and at the SPO were compared with the seasonal cycles of secondary and primary marine aerosol emissions. The ssp measured at SPO correlated much better with the sea-spray aerosol emission fluxes in the Southern Ocean than ssp at Dome C. The seasonal cycles of biogenic secondary aerosols were estimated from monthly average phytoplankton biomass concentrations obtained from the CALIOP satellite sensor data. The analysis suggests that a large fraction of the biogenic scattering aerosol observed at Dome C has been formed in the polar zone but it may take a month for the aerosol to be formed, grown and get transported from the sea level to Dome C. [ABSTRACT FROM AUTHOR]

The Plantower PMS5003 sensors (PA-PMS) used in the PurpleAir (PA) monitor PA-II-SD configuration are equivalent to cell-reciprocal nephelometers using a 657 nm perpendicularly polarized light source that integrates light scattering from 18 to 166 degrees. Yearlong field data at the National Oceanic and Atmospheric Administration's (NOAA) Mauna Loa Observatory (MLO) and Boulder Table Mountain (BOS) sites show that the 1 h average of the PA-PMS first size channel, labeled ">0.3 µm" ("CH1") is highly correlated with submicrometer aerosol scattering coefficients at the 550 nm and 700 nm wavelengths measured by the TSI 3563 integrating nephelometer, from 0.4 Mm-1 to 500 Mm-1. This corresponds to an hourly average submicrometer aerosol mass concentration of approximately 0.2 to 200 µg m-3. A physical-optical model of the PA-PMS is developed to estimate light intensity on the photodiode, accounting for angular truncation as a function of particle size. Predictions are then compared with yearlong fine aerosol size distribution and scattering coefficient field data at the BOS site. It is shown that CH1 is linearly proportional to the model-predicted intensity of the light scattered by particles in the PA-PMS laser to its photodiode over 4 orders of magnitude. This is consistent with CH1 being a measure of the scattering coefficient and not the particle number concentration or particulate matter concentration. Field data at BOS confirm the model prediction that the ratio of CH1 to the scattering coefficient would be highest for aerosols with median scattering diameters <0.3 µm. The PA-PMS detects aerosols smaller than 0.3 µm diameter in proportion to their contribution to the scattering coefficient. The model predicts that the PA-PMS response to particles >0.3 µm decreases relative to an ideal nephelometer by about 75% for particle diameters =1.0 µm. This is a result of using a laser that is polarized, the angular truncation of the scattered light, and particle loss in the instrument before reaching the laser. The results of this study indicate that the PA-PMS is not an optical particle counter and that its six size fractions are not an accurate representation of particle size distribution. The relationship between the PA-PMS 1 h average CH1 and bsp1, the scattering coefficient in Mm-1 due to particles below 1 µm aerodynamic diameter, at wavelength 550 nanometers, is found to be bsp1 = 0.015 ± 2.07 × 10-5 × CH1, for relative humidity below 40%. The coefficient of determination R² is 0.97. This suggests that the low-cost and widely used PA monitors can be used to measure and predict the aerosol light scattering coefficient in the mid-visible nearly as well as integrating nephelometers. [ABSTRACT FROM AUTHOR]

Within the framework of the AeroCom (Aerosol Comparisons between Observations and Models) initiative, the state-of-the-art modelling of aerosol optical properties is assessed from 14 global models participating in the phase III control experiment (AP3). The models are similar to CMIP6/AerChemMIP Earth System Models (ESMs) and provide a robust multi-model ensemble. Inter-model spread of aerosol species lifetimes and emissions appears to be similar to that of mass extinction coefficients (MECs), suggesting that aerosol optical depth (AOD) uncertainties are associated with a broad spectrum of parameterised aerosol processes. Total AOD is approximately the same as in AeroCom phase I (AP1) simulations. However, we find a 50 % decrease in the optical depth (OD) of black carbon (BC), attributable to a combination of decreased emissions and lifetimes. Relative contributions from sea salt (SS) and dust (DU) have shifted from being approximately equal in AP1 to SS contributing about 2/3 of the natural AOD in AP3. This shift is linked with a decrease in DU mass burden, a lower DU MEC, and a slight decrease in DU lifetime, suggesting coarser DU particle sizes in AP3 compared to AP1. Relative to observations, the AP3 ensemble median and most of the participating models underestimate all aerosol optical properties investigated, that is, total AOD as well as fine and coarse AOD (AOD f , AOD c), Ångström exponent (AE), dry surface scattering (SC dry), and absorption (AC dry) coefficients. Compared to AERONET, the models underestimate total AOD by ca. 21 % ± 20 % (as inferred from the ensemble median and interquartile range). Against satellite data, the ensemble AOD biases range from - 37 % (MODIS-Terra) to - 16 % (MERGED-FMI, a multi-satellite AOD product), which we explain by differences between individual satellites and AERONET measurements themselves. Correlation coefficients (R) between model and observation AOD records are generally high (R>0.75), suggesting that the models are capable of capturing spatio-temporal variations in AOD. We find a much larger underestimate in coarse AOD c (∼ - 45 % ± 25 %) than in fine AOD f (∼ - 15 % ± 25 %) with slightly increased inter-model spread compared to total AOD. These results indicate problems in the modelling of DU and SS. The AOD c bias is likely due to missing DU over continental land masses (particularly over the United States, SE Asia, and S. America), while marine AERONET sites and the AATSR SU satellite data suggest more moderate oceanic biases in AOD c. Column AEs are underestimated by about 10 % ± 16 %. For situations in which measurements show AE > 2, models underestimate AERONET AE by ca. 35 %. In contrast, all models (but one) exhibit large overestimates in AE when coarse aerosol dominates (bias ca. + 140 % if observed AE < 0.5). Simulated AE does not span the observed AE variability. These results indicate that models overestimate particle size (or underestimate the fine-mode fraction) for fine-dominated aerosol and underestimate size (or overestimate the fine-mode fraction) for coarse-dominated aerosol. This must have implications for lifetime, water uptake, scattering enhancement, and the aerosol radiative effect, which we can not quantify at this moment. Comparison against Global Atmosphere Watch (GAW) in situ data results in mean bias and inter-model variations of - 35 % ± 25 % and - 20 % ± 18 % for SC dry and AC dry , respectively. The larger underestimate of SC dry than AC dry suggests the models will simulate an aerosol single scattering albedo that is too low. The larger underestimate of SC dry than ambient air AOD is consistent with recent findings that models overestimate scattering enhancement due to hygroscopic growth. The broadly consistent negative bias in AOD and surface scattering suggests an underestimate of aerosol radiative effects in current global aerosol models. Considerable inter-model diversity in the simulated optical properties is often found in regions that are, unfortunately, not or only sparsely covered by ground-based observations. This includes, for instance, the Sahara, Amazonia, central Australia, and the South Pacific. This highlights the need for a better site coverage in the observations, which would enable us to better assess the models, but also the performance of satellite products in these regions. Using fine-mode AOD as a proxy for present-day aerosol forcing estimates, our results suggest that models underestimate aerosol forcing by ca. - 15 %, however, with a considerably large interquartile range, suggesting a spread between - 35 % and + 10 %. [ABSTRACT FROM AUTHOR]

The scattering and backscattering enhancement factors (f(RH) and fb(RH)) describe how aerosol particle light scattering and backscattering, respectively, change with relative humidity (RH). They are important parameters in estimating direct aerosol radiative forcing (DARF). In this study we use a dataset presented in Burgos et al. (2019) that compiles f(RH) and fb(RH) measurements at three wavelengths (i.e. 450, 550 and 700 nm) performed with tandem nephelometer systems at multiple sites around the world. We present an overview of f(RH) and fb(RH) based on both long-term and campaign observations from 23 sites representing a range of aerosol types. The scattering enhancement shows a strong variability from site to site, with no clear pattern with respect to total scattering coefficient. In general, higher f(RH) is observed at Arctic and marine sites while lower values are found at urban and desert sites, although a consistent pattern as a function of site type is not observed. The backscattering enhancement fb(RH) is consistently lower tan f(RH) at all sites, with the difference between f(RH) and fb(RH) increasing for aerosol with higher f(RH). This is consistent with Mie theory which predicts higher enhancement of the light-scattering in the forward than in the backward direction as the particle takes up water. Our results show that the scattering enhancement is higher for PM1 than PM10 at most sites, which is also supported by theory due to the change in scattering efficiency with the size parameter that relates particle size and wavelength of incident light. At marine-influenced sites this difference is enhanced when coarse particles (likely sea salt) predominate. For most sites, f(RH) is observed to increase with increasing wavelength, except at sites with a known dust influence where the spectral dependence of f(RH) is found to be low or even exhibit the opposite pattern. The impact of RH on aerosol properties used to calculate radiative forcing (e.g., single scattering albedo, ω0, and backscattered fraction, b) is evaluated. The single scattering albedo generally increases with RH while b decreases. The net effect of aerosol hygroscopicity on radiative forcing efficiency (RFE) is an increase in the absolute forcing effect (negative sign) by a factor of up to 4 at RH = 90 % compared to dry conditions (RH < 40 %). Because of the scarcity of scattering enhancement measurements, an attempt was made to use other, more commonly available aerosol parameters (i.e., ω0 and scattering Angström exponent, αsp) to parameterize f(RH). The majority of sites (75 %) showed a consistent trend with ω0 (higher f (RH = 85 %) for higher ω0), while no clear pattern was observed between f (RH = 85 %) and αsp. This suggests that aerosol ω0 is more promising tan αsp as a surrogate for the scattering enhancement factor, although neither parameter is ideal. Nonetheless, the qualitative relationship observed between ω0 and f(RH) could serve as a constraint on global model simulations. [ABSTRACT FROM AUTHOR]

Long-term measurements of black carbon (BC) are warranted for investigating changes in its emission, transport, and deposition. However, depending on instrumentation, parameters related to BC such as aerosol absorption coefficient (babs) have been measured instead. Most ground-based measurements of babs in the Arctic have been made by filter-based absorption photometers, including multi-angle absorption photometers (MAAP), particle soot absorption photometers (PSAP), continuous light absorption photometer (CLAP), and Aethalometers. The measured babs can be converted to atmospheric mass concentrations of BC (MBC) by assuming the value of the mass absorption cross section (MAC = babs/MBC). However, the accuracy of conversion of babs to MBC has not been adequately assessed. Here, we introduce a systematic method for deriving MAC values from babs measured by these instruments and independently measured MBC. In this method, MBC was measured with a filter-based absorption photometer with a heated inlet (COSMOS). COSMOS- derived MBC (MBC (COSMOS)) is traceable to a rigorously calibrated single particle soot photometer (SP2) and the absolute accuracy of MBC (COSMOS) has been demonstrated previously to be about 15 % in Asia and the Arctic. The necessary conditions for application of this method are a high correlation of the measured babs with independently measured MBC, and long-term stability of the correlation slope, which represents the MAC. In general, babs - MBC (COSMOS) correlations were high (r² = 0.84-0.96 for hourly data) at Fukue in Japan, Barrow in Alaska, Ny-Ålesund in Svalbard, Pallastunturi in Finland, and Alert in Canada, and stable up to for 10 years. We successfully estimated MAC values (11.0-15.2 m² g-1 at a wavelength of 550 nm) for these instruments and these MAC values can be used to obtain error-constrained estimates of MBC from babs measured at these sites even in the past, when COSMOS measurements were not made. Because the absolute values of MBC in these Arctic sites estimated by this method are consistent with each other, they are applicable to study spatial and temporal variation of MBC and to evaluate performance of numerical model calculations. [ABSTRACT FROM AUTHOR]

The Mann–Kendall test associated with the Sen's slope is a very widely used non-parametric method for trend analysis. It requires serially uncorrelated time series, yet most of the atmospheric processes exhibit positive autocorrelation. Several prewhitening methods have therefore been designed to overcome the presence of lag-1 autocorrelation. These include a prewhitening, a detrending and/or a correction of the detrended slope and the original variance of the time series. The choice of which prewhitening method and temporal segmentation to apply has consequences for the statistical significance, the value of the slope and of the confidence limits. Here, the effects of various prewhitening methods are analyzed for seven time series comprising in situ aerosol measurements (scattering coefficient, absorption coefficient, number concentration and aerosol optical depth), Raman lidar water vapor mixing ratio, as well as tropopause and zero-degree temperature levels measured by radio-sounding. These time series are characterized by a broad variety of distributions, ranges and lag-1 autocorrelation values and vary in length between 10 and 60 years. A common way to work around the autocorrelation problem is to decrease it by averaging the data over longer time intervals than in the original time series. Thus, the second focus of this study evaluates the effect of time granularity on long-term trend analysis. Finally, a new algorithm involving three prewhitening methods is proposed in order to maximize the power of the test, to minimize the number of erroneous detected trends in the absence of a real trend and to ensure the best slope estimate for the considered length of the time series. [ABSTRACT FROM AUTHOR]

This study presents a multiparameter analysis of aerosol trends over the last 2 decades at regional and global scales. Regional time series have been computed for a set of nine optical, chemical-composition and mass aerosol properties by using the observations from several ground-based networks. From these regional time series the aerosol trends have been derived for the different regions of the world. Most of the properties related to aerosol loading exhibit negative trends, both at the surface and in the total atmospheric column. Significant decreases in aerosol optical depth (AOD) are found in Europe, North America, South America, North Africa and Asia, ranging from -1.2 % yr -1 to -3.1 % yr -1. An error and representativity analysis of the spatially and temporally limited observational data has been performed using model data subsets in order to investigate how much the observed trends represent the actual trends happening in the regions over the full study period from 2000 to 2014. This analysis reveals that significant uncertainty is associated with some of the regional trends due to time and space sampling deficiencies. The set of observed regional trends has then been used for the evaluation of 10 models (6 AeroCom phase III models and 4 CMIP6 models) and the CAMS reanalysis dataset and of their skills in reproducing the aerosol trends. Model performance is found to vary depending on the parameters and the regions of the world. The models tend to capture trends in AOD, the column Ångström exponent, sulfate and particulate matter well (except in North Africa), but they show larger discrepancies for coarse-mode AOD. The rather good agreement of the trends, across different aerosol parameters between models and observations, when co-locating them in time and space, implies that global model trends, including those in poorly monitored regions, are likely correct. The models can help to provide a global picture of the aerosol trends by filling the gaps in regions not covered by observations. The calculation of aerosol trends at a global scale reveals a different picture from that depicted by solely relying on ground-based observations. Using a model with complete diagnostics (NorESM2), we find a global increase in AOD of about 0.2 % yr -1 between 2000 and 2014, primarily caused by an increase in the loads of organic aerosols, sulfate and black carbon. [ABSTRACT FROM AUTHOR]

The uptake of water by atmospheric aerosols has a pronounced effect on particle light scattering properties, which in turn are strongly dependent on the ambient relative humidity (RH). Earth system models need to account for the aerosol water uptake and its influence on light scattering in order to properly capture the overall radiative effects of aerosols. Here we present a comprehensive model–measurement evaluation of the particle light scattering enhancement factor f (RH), defined as the particle light scattering coefficient at elevated RH (here set to 85 %) divided by its dry value. The comparison uses simulations from 10 Earth system models and a global dataset of surface-based in situ measurements. In general, we find a large diversity in the magnitude of predicted f (RH) amongst the different models, which can not be explained by the site types. Based on our evaluation of sea salt scattering enhancement and simulated organic mass fraction, there is a strong indication that differences in the model parameterizations of hygroscopicity and model chemistry are driving at least some of the observed diversity in simulated f (RH). Additionally, a key point is that defining dry conditions is difficult from an observational point of view and, depending on the aerosol, may influence the measured f (RH). The definition of dry also impacts our model evaluation, because several models exhibit significant water uptake between RH = 0 % and 40 %. The multisite average ratio between model outputs and measurements is 1.64 when RH = 0 % is assumed as the model dry RH and 1.16 when RH = 40 % is the model dry RH value. The overestimation by the models is believed to originate from the hygroscopicity parameterizations at the lower RH range which may not implement all phenomena taking place (i.e., not fully dried particles and hysteresis effects). This will be particularly relevant when a location is dominated by a deliquescent aerosol such as sea salt. Our results emphasize the need to consider the measurement conditions in such comparisons and recognize that measurements referred to as dry may not be dry in model terms. Recommendations for future model–measurement evaluation and model improvements are provided. [ABSTRACT FROM AUTHOR]

Aerosol particles are essential constituents of the Earth's atmosphere, impacting the earth radiation balance directly by scattering and absorbing solar radiation, and indirectly by acting as cloud condensation nuclei. In contrast to most greenhouse gases, aerosol particles have short atmospheric residence times, resulting in a highly heterogeneous distribution in space and time. There is a clear need to document this variability at regional scale through observations involving, in particular, the in situ near-surface segment of the atmospheric observation system. This paper will provide the widest effort so far to document variability of climate-relevant in situ aerosol properties (namely wavelength dependent particle light scattering and absorption coefficients, particle number concentration and particle number size distribution) from all sites connected to the Global Atmosphere Watch network. High-quality data from almost 90 stations worldwide have been collected and controlled for quality and are reported for a reference year in 2017, providing a very extended and robust view of the variability of these variables worldwide. The range of variability observed worldwide for light scattering and absorption coefficients, single-scattering albedo, and particle number concentration are presented together with preliminary information on their long-term trends and comparison with model simulation for the different stations. The scope of the present paper is also to provide the necessary suite of information, including data provision procedures, quality control and analysis, data policy, and usage of the ground-based aerosol measurement network. It delivers to users of the World Data Centre on Aerosol, the required confidence in data products in the form of a fully characterized value chain, including uncertainty estimation and requirements for contributing to the global climate monitoring system. [ABSTRACT FROM AUTHOR]

In order to assess the evolution of aerosol parameters affecting climate change, a long-term trend analysis of aerosol optical properties was performed on time series from 52 stations situated across five continents. The time series of measured scattering, backscattering and absorption coefficients as well as the derived single scattering albedo, backscattering fraction, scattering and absorption Ångström exponents covered at least 10 years and up to 40 years for some stations. The non-parametric seasonal Mann–Kendall (MK) statistical test associated with several pre-whitening methods and with Sen's slope was used as the main trend analysis method. Comparisons with general least mean square associated with autoregressive bootstrap (GLS/ARB) and with standard least mean square analysis (LMS) enabled confirmation of the detected MK statistically significant trends and the assessment of advantages and limitations of each method. Currently, scattering and backscattering coefficient trends are mostly decreasing in Europe and North America and are not statistically significant in Asia, while polar stations exhibit a mix of increasing and decreasing trends. A few increasing trends are also found at some stations in North America and Australia. Absorption coefficient time series also exhibit primarily decreasing trends. For single scattering albedo, 52 % of the sites exhibit statistically significant positive trends, mostly in Asia, eastern/northern Europe and the Arctic, 22 % of sites exhibit statistically significant negative trends, mostly in central Europe and central North America, while the remaining 26 % of sites have trends which are not statistically significant. In addition to evaluating trends for the overall time series, the evolution of the trends in sequential 10-year segments was also analyzed. For scattering and backscattering, statistically significant increasing 10-year trends are primarily found for earlier periods (10-year trends ending in 2010–2015) for polar stations and Mauna Loa. For most of the stations, the present-day statistically significant decreasing 10-year trends of the single scattering albedo were preceded by not statistically significant and statistically significant increasing 10-year trends. The effect of air pollution abatement policies in continental North America is very obvious in the 10-year trends of the scattering coefficient – there is a shift to statistically significant negative trends in 2009–2012 for all stations in the eastern and central USA. This long-term trend analysis of aerosol radiative properties with a broad spatial coverage provides insight into potential aerosol effects on climate changes. [ABSTRACT FROM AUTHOR]

The most widely used non-parametric method for trend analysis is the Mann-Kendall test associated with the Sen's slope. The Mann-Kendall test requires serially uncorrelated time series, whereas most of the atmospheric processes exhibit positive autocorrelation. Several prewhitening methods have been designed to overcome the presence of lag-1 autocorrelation. These include a prewhitening, a detrending and/or a correction for the detrended slope and the original variance of the time series. The choice of which prewhitening method and temporal segmentation to apply has consequences for the statistical significance, the value of the slope and of the confidence limits. Here, the effects of various prewhitening methods are analyzed for seven time series comprising in-situ aerosol measurements (scattering coefficient, absorption coefficient, number concentration and aerosol optical depth), Raman Lidar water vapor mixing ratio and the tropopause and zero degree levels measured by radio-sounding. These time series are characterized by a broad variety of distributions, ranges and lag-1 autocorrelation values and vary in length between 10 and 60 years. A common way to work around the autocorrelation problem is to decrease it by averaging the data over longer time intervals than in the original time series. Thus, the second focus of this study is evaluation of the effect of time granularity on long-term trend analysis. Finally, a new algorithm involving three prewhitening methods is proposed in order to maximize the power of the test, to minimize the amount of erroneous detected trends in the absence of a real trend and to ensure the best slope estimate for the considered length of the time series. [ABSTRACT FROM AUTHOR]

Within the framework of the AeroCom (Aerosol Comparisons between Observations and Models) initiative, the present day modelling of aerosol optical properties has been assessed using simulated data representative for the year 2010, from 14 global aerosol models participating in the Phase III Control experiment. The model versions are close or equal to those used for CMIP6 and AerChemMIP and inform also on bias in state of the art ESMs. Modelled column optical depths (total, fine and coarse mode AOD) and Ångström Exponents (AE) were compared both with ground based observations from the Aerosol Robotic Network (AERONET, version 3) as well as space based observations from AATSR-SU instruments. In addition, the modelled AODs were compared with MODIS (Aqua and Terra) data and a satellite AOD data-set (MERGED-FMI) merged from 12 different individual AOD products. Furthermore, for the first time, the modelled near surface scattering (under dry conditions) and absorption coefficients were evaluated against measurements made at low relative humidity at surface in-situ GAW sites. [ABSTRACT FROM AUTHOR]

Aerosol particles are essential constituents of the Earth’s atmosphere, impacting the earth radiation balance directly by scattering and absorbing solar radiation, and indirectly by acting as cloud condensation nuclei. In contrast to most greenhouse gases, aerosol particles have short atmospheric residence time resulting in a highly heterogeneous distribution in space and time. There is a clear need to document this variability at regional scale through observations involving, in particular, the in-situ near-surface segment of the atmospheric observations system. This paper will provide the widest effort so far to document variability of climate-relevant in-situ aerosol properties (namely wavelength dependent particle light scattering and absorption coefficients, particle number concentration and particle number size distribution) from all sites connected to the Global Atmosphere Watch network. High quality data from more than 90 stations worldwide have been collected and controlled for quality and are reported for a reference year in 2017, providing a very extended and robust view of the variability of these variables worldwide. The range of variability observed worldwide for light scattering and absorption coefficients, single scattering albedo and particle number concentration are presented together with preliminary information on their long-term trends and comparison with model simulation for the different stations. The scope of the present paper is also to provide the necessary suite of information including data provision procedures, quality control and analysis, data policy and usage of the ground-based aerosol measurements network. It delivers to users of the World Data Centre on Aerosol, the required confidence in data products in the form of a fully-characterized value chain, including uncertainty estimation and requirements for contributing to the global climate monitoring system. [ABSTRACT FROM AUTHOR]

This study presents a multi-parameter analysis of aerosol trends over the last two decades at regional and global scales. Regional time series have been computed for a set of nine optical, chemical composition and mass aerosol properties by using the observations of several ground-based networks. From these regional time series the aerosol trends have been derived for different regions of the world. Most of the properties related to aerosol loading exhibit negative trends, both at the surface and in the total atmospheric column. Significant decreases of aerosol optical depth (AOD) are found in Europe, North America, South America and North Africa, ranging from -1.3 %/yr to -3.1 %/yr. An error and representativity analysis of the incomplete observational data has been performed using model data subsets in order to investigate how likely the observed trends represent the actual trends happening in the regions over the full study period from 2000 to 2014. This analysis reveals that significant uncertainty is associated with some of the regional trends due to time and space sampling deficiencies. The set of observed regional trends has then been used for the evaluation of the climate models and their skills in reproducing the aerosol trends. Model performance is found to vary depending on the parameters and the regions of the world. The models tend to capture trends in AOD, column Angstrom exponent, sulfate and particulate matter well (except in North Africa), but show larger discrepancies for coarse mode AOD. The rather good agreement of the trends, across different aerosol parameters between models and observations, when co-locating them in time and space, implies that global model trends, including those in poorly monitored regions, are likely correct. The models can help to provide a global picture of the aerosol trends by filling the gaps in regions not covered by observations. The calculation of aerosol trends at a global scale reveals a different picture from the one depicted by solely relying on ground based observations. Using a model with complete diagnostics (NorESM2) we find a global increase of AOD of about 0.2 %/yr between 2000 and 2014, primarily caused by an increase of the loads of organic aerosol, sulfate and black carbon. [ABSTRACT FROM AUTHOR]

In order to assess the global evolution of aerosol parameters affecting climate change, a long-term trend analyses of aerosol optical properties were performed on time series from 52 stations situated across five continents. The time series of measured scattering, backscattering and absorption coefficients as well as the derived single scattering albedo, backscattering fraction, scattering and absorption Ångström exponents covered at least 10 years and up to 40 years for some stations. The non-parametric seasonal Mann-Kendall (MK) statistical test associated with several prewhitening methods and with the Sen's slope were used as main trend analysis methods. Comparisons with General Least Mean Square associated with Autoregressive Bootstrap (GLS/ARB) and with standard Least Mean Square analysis (LMS) enabled confirmation of the detected MK statistically significant trends and the assessment of advantages and limitations of each method. Currently, scattering and backscattering coefficients trends are mostly decreasing in Europe and North America and are not statistically significant in Asia, while polar stations exhibit a mix of increasing and decreasing trends. A few increasing trends are also found at some stations in North America and Australia. Absorption coefficients time series also exhibit primarily decreasing trends. For single scattering albedo, 52 % of the sites exhibit statistically significant positive trends, mostly in Asia, Eastern/Northern Europe and Arctic, 18 % of sites exhibit statistically significant negative trends, mostly in central Europe and central North America, while the remaining 30 % of sites have trends, which are not statistically significant. In addition to evaluating trends for the overall time series, the evolution of the trends in sequential 10 year segments was also analyzed. For scattering and backscattering, statistically significant increasing 10 year trends are primarily found for earlier periods (10 year trends ending in 2010-2015) for polar stations and Mauna Loa. For most of the stations, the present-day statistically significant decreasing 10 year trends of the single scattering albedo were preceded by not statistically significant and statistically significant increasing 10 year trends. The effect of air pollution abatement policies in continental North America is very obvious in the 10 year trends of the scattering coefficient - there is a shift to statistically significant negative trends in 2010-2011 for all stations in the eastern and central US. This long-term trend analysis of aerosol radiative properties with a broad spatial coverage enables a better global view of potential aerosol effects on climate changes. [ABSTRACT FROM AUTHOR]

The Chilean Coastal Orographic Precipitation Experiment (CCOPE) was a 3-month field campaign (June, July and August 2015) that investigated wintertime coastal rain events. Reported here are analyses of aerosol measurements made at a coastal site during CCOPE. The aerosol monitoring site was located near Arauco, Chile. Aerosol number concentrations and aerosol size distributions were acquired with a condensation particle counter (CPC) and an ultra high sensitivity aerosol spectrometer (UHSAS). Arauco CPC data were compared to values measured at the NOAA observatory Trinidad Head (THD) on the northern Pacific coast of California. The winter-averaged CPC concentration at Arauco is 2971 ± 1802 cm -3 ; at THD the average is 1059 ± 855 cm -3. Despite the typically more pristine South Pacific region, the Arauco average is larger than at THD (p<0.01). Aerosol size distributions acquired during episodes of onshore flow were analyzed with Köhler theory and used to parameterize cloud condensation nuclei activation spectra. In addition, sea salt aerosol (SSA) concentration was parameterized as a function of sea surface wind speed. It is anticipated these parameterizations will be applied in modeling of wintertime Chilean coastal precipitation. [ABSTRACT FROM AUTHOR]

Despite the potential importance of black carbon (BC) to radiative forcing of the Arctic atmosphere, vertically-resolved measurements of the particle light scattering coefficient (Bsp) and light absorption coefficient (Bap) in the springtime Arctic atmosphere are infrequent, especially measurements at latitudes at or above 80oN. Here, relationships among vertically-distributed aerosol optical properties Bap, Bsp, and single scattering albedo or SSA), particle microphysics and particle chemistry are examined for a region of the Canadian archipelago between 79.9oN and 83.4oN from near the surface to 500 hPa. Airborne data collected during April, 2015, are combined with ground-based observations from the observatory at Alert, Nunavut and simulations from the GEOS-Chem-TOMAS model (Kodros et al., 2018) to increase our knowledge of the effects of BC on light absorption in the Arctic troposphere. The results are constrained for Bsp less than 15 Mm-1, which represent 98% of the observed Bsp, because the single scattering albedo (SSA) has a tendency to be lower at lower Bsp, resulting in a larger relative contribution to Arctic warming. At 18.4 m2 g-1, the average BC mass absorption coefficient (MAC) from the combined airborne and Alert observations is substantially higher than the two averaged modelled MAC values (9.5 m2 g-1 and 7.0 m2 g-1) for two different internal mixing assumptions, the latter of which is based on previous observations. The higher observed MAC value may be explained by an underestimation of BC and possible differences in BC microphysics and morphologies between the observations and model. We present Bap and SSA based on the assumption that Bap is overestimated in the observations in addition to the assumption that the higher MAC is explained. Median values of the measured Bap, rBC and organic component of particles all increase by a factor of 1.8±0.1 going from near-surface to 750 hPa, and values higher than the surface persist to 600 hPa. Modelled BC, organics, and Bap agree with the near-surface measurements, but do not reproduce the higher values observed between 900 hPa and 600 hPa. The differences between modelled and observed optical properties follow the same trend as the differences between the modelled and observed concentrations of the carbonaceous components (black and organic). Some discrepancies in the model may be due to the use of a relatively low imaginary refractive index of BC as well as by the ejection of biomass burning particles only into the boundary layer at sources. For the assumption of the higher observed MAC value, the SSA range between 0.88 and 0.94, which is significantly lower than other recent estimates for the Arctic, in part reflecting the constraint of Bsp <15 Mm-1. The large uncertainties in measuring optical properties and BC as well as the large differences between measured and modelled values, here and in the literature, argue for improved measurements of BC and light absorption by BC as well as more vertical profiles of aerosol chemistry, microphysics, and other optical properties in the Arctic. [ABSTRACT FROM AUTHOR]

High altitude stations are often emphasized as free tropospheric measuring sites but they remain influenced by atmospheric boundary layer (ABL) air masses due to convective transport processes. The local and meso-scale topographical features around the station are involved in the convective boundary layer development and in the formation of thermally induced winds leading to ABL air lifting. The station altitude alone is not a sufficient parameter to characterize the ABL influence. In this study, a topography analysis is performed allowing calculation of a newly defined index called ABL-TopoIndex. The ABL-TopoIndex is constructed in order to correlate with the ABL influence at the high altitude stations and long-term aerosol time series are used to assess its validity. Topography data from the global digital elevation model GTopo30 were used to calculate five parameters for 43 high and 3 middle altitude stations situated on five continents. The geometric mean of these five parameters determines a topography based index called ABL-TopoIndex, which can be used to rank the high altitude stations as a function of the ABL influence. To construct the ABL-TopoIndex, we rely on the criteria that the ABL influence will be low if the station is one of the highest points in the mountainous massif, if there is a large altitude difference between the station and the valleys or high plains, if the slopes around the station are steep, and finally if the inverse drainage basin potentially reflecting the source area for thermally lifted pollutants to reach the site is small. All stations on volcanic islands exhibit a low ABL-TopoIndex, whereas stations in the Himalayas and the Tibetan Plateau have high ABL-TopoIndex values. Spearman's rank correlation between aerosol optical properties and number concentration from 28 stations and the ABL-TopoIndex, the altitude and the latitude are used to validate this topographical approach. Statistically significant (SS) correlations are found between the 5th and 50th percentiles of all aerosol parameters and the ABL-TopoIndex, whereas no SS correlation is found with the station altitude. The diurnal cycles of aerosol parameters seem to be best explained by the station latitude although a SS correlation is found between the amplitude of the diurnal cycles of the absorption coefficient and the ABL-TopoIndex. [ABSTRACT FROM AUTHOR]

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 (12.47Mm-1), and the lowest annual mean scattering coefficient is measured at Summit (1.74Mm-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 (0.48Mm-1), and Summit has the lowest annual mean absorption coefficient (0.12Mm-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. [ABSTRACT FROM AUTHOR]

Since 2005, we have monitored the physicochemical and optical properties of aerosols at the Cape San Juan Atmospheric Observatory, Puerto Rico. Based on the Hybrid Single-Particle Lagrangian Integrated trajectories (HYSPLIT) and satellite imagery from the Volcanic Ash Advisory Center (VAAC) in Washington D.C., Moderate Resolution Imaging Spectroradiometer (MODIS), and Saharan air layer (SAL) images, we grouped natural aerosols in three categories: marine, African dust and volcanic ash. A sun-sky radiometer from the NASA's AErosol RObotic NETwork (AERONET) assessed the total aerosol optical depth and its fine fraction. A 3-wavelength nephelometer and particle soot absorption photometer assessed the scattering and absorption coefficients. Two impactors segregated the submicron (Dp < 1 μm) particles from the total (Dp < 10 μm) enabling us to calculate the sub-micron scattering and absorption fractions. The measured variables served to calculate the single scattering albedo and radiative forcing efficiency. All variables except the single scattering albedo making up the aerosol climatology for Puerto Rico had different means as function of the aerosol category at p < 0.05. For the period 2005-2010, the largest means ±95% confidence interval of the scattering coefficient (53 ± 4 Mm-1), absorption coefficient (1.8 ± 0.16 Mm-1), and optical depth (0.29 ± 0.03), suggested African dust is the main contributor to the columnar and surface aerosol loading in summer. About two thirds (63%) of the absorption in African dust was due to the coarse mode and about one third due to the fine mode. In volcanic ash, fine aerosols contributed 60% of the absorption while coarse contributed 40%. Overall, the coarse and fine modes accounted for ~ 80% and 20% of the total scattering. The African dust load was 3.5 times the load of clean marine, 1.9 times greater than the clean marine with higher sea salt content, and 1.7 times greater than volcanic ash. African dust caused 50% more cooling than that volcanic ash at the top of the atmosphere and 50% more heating than that of volcanic ash within the marine boundary layer (MBL). [ABSTRACT FROM AUTHOR]

A new photometer is described for continuous determination of the aerosol light absorption coefficient, optimized for long-term studies of the climate-forcing properties of aerosols. Measurements of the light attenuation coefficient are made at blue, green, and red wavelengths, with a detection limit of 0.02Mm-1 and a precision of 4% for hourly averages. The uncertainty of the light absorption coefficient is primarily determined by the uncertainty of the correction scheme commonly used to convert the measured light attenuation to light absorption coefficient and ranges from about 20% at sites with high loadings of strongly absorbing aerosols up to 100% or more at sites with low loadings of weakly absorbing aerosols. Much lower uncertainties (ca. 40 %) for the latter case can be achieved with an advanced correction scheme. [ABSTRACT FROM AUTHOR]

Knowledge of aerosol size and composition is important for determining radiative forcing effects of aerosols, identifying aerosol sources and improving aerosol satellite retrieval algorithms. The ability to extrapolate aerosol size and composition, or type, from intensive aerosol optical properties can help expand the current knowledge of spatiotemporal variability in aerosol type globally, particularly where chemical composition measurements do not exist concurrently with optical property measurements. This study uses medians of the scattering Ångström exponent (SAE), absorption Ångström exponent (AAE) and single scattering albedo (SSA) from 24 stations within the NOAA/ESRL Federated Aerosol Monitoring Network to infer aerosol type using previously published aerosol classification schemes. Three methods are implemented to obtain a best estimate of dominant aerosol type at each station using aerosol optical properties. The first method plots station medians into an AAE vs. SAE plot space, so that a unique combination of intensive properties corresponds with an aerosol type. The second typing method expands on the first by introducing a multivariate cluster analysis, which aims to group stations with similar optical characteristics and thus similar dominant aerosol type. The third and final classification method pairs 3-day backward air mass trajectories with median aerosol optical properties to explore the relationship between trajectory origin (proxy for likely aerosol type) and aerosol intensive parameters, while allowing for multiple dominant aerosol types at each station. The three aerosol classification methods have some common, and thus robust, results. In general, estimating dominant aerosol type using optical properties is best suited for site locations with a stable and homogenous aerosol population, particularly continental polluted (carbonaceous aerosol), marine polluted (carbonaceous aerosol mixed with sea salt) and continental dust/biomass sites (dust and carbonaceous aerosol); however, current classification schemes perform poorly when predicting dominant aerosol type at remote marine and Arctic sites and at stations with more complex locations and topography where variable aerosol populations are not well represented by median optical properties. Although the aerosol classification methods presented here provide new ways to reduce ambiguity in typing schemes, there is more work needed to find aerosol typing methods that are useful for a larger range of geographic locations and aerosol populations. [ABSTRACT FROM AUTHOR]

High altitude stations are often emphasized as free tropospheric measuring sites but they remain influenced by atmospheric boundary layer (ABL) air masses due to convective transport processes. The local and meso-scale topographical features around the station are involved in the convective boundary layer development and in the formation of thermally induced winds leading to ABL air lifting. The station altitude is not a sufficient parameter to characterize the ABL influence. Topography data from the global digital elevation model GTopo30 were used to calculate 5 parameters for 46 high altitude stations situated in five continents. The geometric mean of these 5 parameters determines a topography based index called ABL-TopoIndex which can be used to rank the high altitude stations as a function of the ABL influence. To construct the ABL-TopoIndex, we rely on the criteria that the ABL influence will be low if the station is one of the highest points in the mountainous massif, if there is a large altitude difference between the station and the valleys or plateaus, if the slopes around the station are steep, and finally if the drainage basin for air convection is small. All stations on volcanic islands exhibit a low ABL-TopoIndex whereas stations in the Himalaya and the Tibetan Plateau have high ABL-TopoIndex values. Spearman's rank correlation between aerosol optical properties and number concentration from 28 stations and the ABL-TopoIndex, the altitude and the latitude are used to validate this topographical approach. Statistically significant (s.s.) correlations are found between the 5 and 50 percentiles of all aerosol parameters and the ABL-TopoIndex whereas no s.s. correlation is found with the station altitude. The diurnal cycles of aerosol parameters seem to be best explained by the station latitude although a s.s. correlation is found between the amplitude of the diurnal cycles of the absorption coefficient and the ABL-TopoIndex. Finally, the main flow paths for air convection were calculated for various ABL heights. [ABSTRACT FROM AUTHOR]

Atmospheric aerosols stay a major cause of uncertainty in climate prediction. Hundreds of teragrams and the absorbing properties of aerosols such as African dust and volcanic ash affect radiative balance changing atmospheric temperature and thus, climate. Since 2005, we began to check the physicochemical and optical properties of aerosols at the Cape San Juan Atmospheric Observatory, Puerto Rico. Based on the Hybrid Single-Particle Lagrangian Integrated Trajectory backward trajectories and satellite imagery from the Volcanic Ash Advisory Center in Washington D.C., Moderate Resolution Imaging Spectroradiometer, and Saharan air layer images, we grouped natural aerosols in three air masses: marine, African dust and volcanic ash. A sun-sky radiometer from the NASA's AErosol RObotic NETwork assessed total aerosol optical depth and its fine fraction. A 3-wavelength nephelometer and particle soot absorption photometer assessed the scattering and absorption coefficients. Two impactors segregated the submicron (Dp < 1 μm) particles from the total (Dp < 10 μm) enabling us to calculate the sub-micron scattering and absorption fractions. The measured variables served to calculate the single scattering albedo and radiative forcing efficiency. All variables but the single scattering albedo making up the aerosol climatology for Puerto Rico had different means as function of the air mass category at p < 0.05. For the period 2005-2010, the largest means ± 95 % confidence interval of the scattering coefficient (53 ± 4 Mm-1), absorption coefficient (1.8 ± 0.16 Mm-1), and optical depth (0.29 ± 0.03), suggested African dust is the main contributor to the columnar and surface aerosol loading in summer. About two thirds (63 %) of the absorption in African dust was due to the coarse mode and about one third due to the fine mode. In volcanic ash, fine aerosols contributed 60 % of the absorption while coarse contributed 40 %. Overall, the coarse and fine modes accounted for ~ 80 % and 20 % of the total scattering. The African dust load was 3.5 times the load of clean marine, 1.9 times greater than clean with higher sea salt content and 1.7 times greater than volcanic ash. African dust caused 50 % more cooling that volcanic ash at the top of the atmosphere and 50 % more heating than that of volcanic ash within the marine boundary layer. [ABSTRACT FROM AUTHOR]

Here we present new results comparing aerosol optical depth (AOD), aerosol absorption optical depth (AAOD) and column single scattering albedo (SSA) obtained from in situ vertical profile measurements with AERONET ground-based remote sensing from two rural, continental sites in the US. The profiles are closely matched in time (within 3 h) and space (within 15 km) with the AERONET retrievals. We have used Level 1.5 inversion retrievals when there was a valid Level 2 almucantar retrieval in order to be able to compare AAOD and column SSA below AERONET's recommended loading constraint (AOD> 0.4 at 440 nm). While there is reasonable agreement for the AOD comparisons, the direct comparisons of in situ-derived to AERONET-retrieved AAOD (or SSA) reveal that AERONET retrievals yield higher aerosol absorption than obtained from the in situ profiles for the low aerosol optical depth conditions prevalent at the two study sites. However, it should be noted that the majority of SSA comparisons for AOD440 > 0.2 are, nonetheless, within the reported SSA uncertainty bounds. The observation that, relative to in situ measurements, AERONET inversions exhibit increased absorption potential at low AOD values is generally consistent with other published AERONET-in situ comparisons across a range of locations, atmospheric conditions and AOD values. This systematic difference in the comparisons suggests a bias in one or both of the methods, but we cannot assess whether the AERONET retrievals are biased towards high absorption or the in situ measurements are biased low. Based on the discrepancy between the AERONET and in situ values, we conclude that scaling modeled black carbon concentrations upwards to match AERONET retrievals of AAOD should be approached with caution as it may lead to aerosol absorption overestimates in regions of low AOD. Both AERONET retrievals and in situ measurements suggest there is a systematic relationship between SSA and aerosol amount (AOD or aerosol light scattering) - specifically that SSA decreases at lower aerosol loading. This implies that the fairly common assumption that AERONET SSA values retrieved at high-AOD conditions can be used to obtain AAOD at low-AOD conditions may not be valid. [ABSTRACT FROM AUTHOR]

Here we present new results comparing aerosol absorption optical depth (AAOD) and column single scattering albedo (SSA) obtained from in-situ vertical profile measurements with AERONET ground-based remote sensing from two rural continental sites in the US. The profiles are closely matched in time (within +/-3 h) and space (within 15 km) with the AERONET retrievals. These direct comparisons of in-situ-derived to AERONET-retrieved AAOD (or SSA) reveal that AERONET retrievals yield higher aerosol absorption for the low aerosol optical depth (AOD) conditions prevalent at the two study sites. The tendency of AERONET inversions to overestimate absorption at low AOD values is generally consistent with other published comparisons. We conclude that scaling modelled black carbon concentrations upwards to match AERONET retrievals of AAOD may lead to aerosol absorption overestimates in regions of low AOD. [ABSTRACT FROM AUTHOR]