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Abstract. Even though the Arctic is remote, aerosol properties observed there arestrongly influenced by anthropogenic emissions from outside the Arctic. Thisis particularly true for the so-called Arctic haze season (January throughApril). In summer (June through September), when atmospheric transportpatterns 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 emissionshave taken place. At the same time a large body of literature shows evidencethat the Arctic is undergoing fundamental environmental changes due toclimate forcing, leading to enhanced emissions by natural processes that mayimpact aerosol properties. In this study, we analyze 9 aerosol chemical species and 4 particleoptical properties from 10 Arctic observatories (Alert, Kevo, Pallas,Summit, Thule, Tiksi, Barrow/Utqiaġvik, Villum, and Gruvebadet and ZeppelinObservatory – both at Ny-Ålesund Research Station) to understand changesin anthropogenic and natural aerosol contributions. Variables includeequivalent black carbon, particulate sulfate, nitrate, ammonium,methanesulfonic acid, sodium, iron, calcium and potassium, as well asscattering and absorption coefficients, single scattering albedo andscattering Ångström exponent. First, annual cycles are investigated, which despite anthropogenic emissionreductions still show the Arctic haze phenomenon. Second, long-term trendsare studied using the Mann–Kendall Theil–Sen slope method. We find in total41 significant trends over full station records, i.e., spanning more than adecade, compared to 26 significant decadal trends. The majority ofsignificantly declining trends is from anthropogenic tracers and occurredduring the haze period, driven by emission changes between 1990 and 2000.For the summer period, no uniform picture of trends has emerged. Twenty-sixpercent of trends, i.e., 19 out of 73, are significant, and of those 5 arepositive and 14 are negative. Negative trends include not only anthropogenictracers such as equivalent black carbon at Kevo, but also natural indicatorssuch as methanesulfonic acid and non-sea-salt calcium at Alert. Positivetrends are observed for sulfate at Gruvebadet. No clear evidence of a significant change in the natural aerosolcontribution can be observed yet. However, testing the sensitivity of theMann–Kendall Theil–Sen method, we find that monotonic changes of around 5 % yr−1 in an aerosol property are needed to detect a significanttrend within one decade. This highlights that long-term efforts well beyonda decade are needed to capture smaller changes. It is particularly importantto understand the ongoing natural changes in the Arctic, where interannualvariability can be high, such as with forest fire emissions and theirinfluence on the aerosol population. To investigate the climate-change-induced influence on the aerosolpopulation and the resulting climate feedback, long-term observations oftracers more specific to natural sources are needed, as well as of particlemicrophysical properties such as size distributions, which can be used toidentify changes in particle populations which are not well captured bymass-oriented methods such as bulk chemical composition. 

Soot particles form during combustion of carbonaceous materials and impact climate and air quality. When freshly emitted, they are typically fractal-like aggregates. After atmospheric aging, they can act as cloud condensation nuclei, and water condensation or evaporation restructure them to more compact aggregates, affecting their optical, aerodynamic, and surface properties. Here we survey the morphology of ambient soot particles from various locations and different environmental and aging conditions. We used electron microscopy and show extensive soot compaction after cloud processing. We further performed laboratory experiments to simulate atmospheric cloud processing under controlled conditions. We find that soot particles sampled after evaporating the cloud droplets, are significantly more compact than freshly emitted and interstitial soot, confirming that cloud processing, not just exposure to high humidity, compacts soot. Our findings have implications for how the radiative, surface, and aerodynamic properties, and the fate of soot particles are represented in numerical models.

 

Sulfur compounds are an important constituent of particulate matter, with impacts on climate and public health. While most sulfur observed in particulate matter has been assumed to be sulfate, laboratory experiments reveal that hydroxymethanesulfonate (HMS), an adduct formed by aqueous phase chemical reaction of dissolved HCHO and SO₂, may be easily misinterpreted in measurements as sulfate. Here we present observational and modeling evidence for a ubiquitous global presence of HMS. We find that filter samples collected in Shijiazhuang, China, and examined with ion chromatography within 9 days show as much as 7.6 μg m⁻³of HMS, while samples from Singapore examined 9–18 months after collection reveal ~0.6 μg m⁻³of HMS. The Shijiazhuang samples show only minor traces of HMS 4 months later, suggesting that HMS had decomposed over time during sample storage. In contrast, the Singapore samples do not clearly show a decline in HMS concentration over 2 months of monitoring. Measurements from over 150 sites, primarily derived from the IMPROVE network across the United States, suggest the ubiquitous presence of HMS in at least trace amounts as much as 60 days after collection. The degree of possible HMS decomposition in the IMPROVE observations is unknown. Using the GEOS‐Chem chemical transport model, we estimate that HMS may account for 10% of global particulate sulfur in continental surface air and over 25% in many polluted regions. Our results suggest that reducing emissions of HCHO and other volatile organic compounds may have a co‐benefit of decreasing particulate sulfur.