In recent years, marine, freshwater and terrestrial pollution with microplastics has been discussed extensively, whereas atmospheric microplastic transport has been largely overlooked. Here, we present global simulations of atmospheric transport of microplastic particles produced by road traffic (TWPs – tire wear particles and BWPs – brake wear particles), a major source that can be quantified relatively well. We find a high transport efficiencies of these particles to remote regions. About 34% of the emitted coarse TWPs and 30% of the emitted coarse BWPs (100 kt yr⁻¹ and 40 kt yr⁻¹ respectively) were deposited in the World Ocean. These amounts are of similar magnitude as the total estimated direct and riverine transport of TWPs and fibres to the ocean (64 kt yr⁻¹). We suggest that the Arctic may be a particularly sensitive receptor region, where the light-absorbing properties of TWPs and BWPs may also cause accelerated warming and melting of the cryosphere.

Sea-spray aerosols (SSA) are an important part of the climate system because of their effects on the global radiative budget – both directly as scatterers and absorbers of solar and terrestrial radiation, and indirectly as cloud condensation nuclei (CCN) influencing cloud formation, lifetime, and precipitation. In terms of their global mass, SSA have the largest uncertainty of all aerosols. In this study we review 21 SSA source functions from the literature, several of which are used in current climate models. In addition, we propose a~new function. Even excluding outliers, the global annual SSA mass produced spans roughly 3–70 Pg yr⁻¹ for the different source functions, for particles with dry diameter D_p < 10 μm, with relatively little interannual variability for a given function. The FLEXPART Lagrangian particle dispersion model was run in backward mode for a large global set of observed SSA concentrations, comprised of several station networks and ship cruise measurement campaigns. FLEXPART backward calculations produce gridded emission sensitivity fields, which can subsequently be multiplied with gridded SSA production fluxes in order to obtain modeled SSA concentrations. This allowed us to efficiently and simultaneously evaluate all 21 source functions against the measurements. Another advantage of this method is that source-region information on wind speed and sea surface temperatures (SSTs) could be stored and used for improving the SSA source function parameterizations. The best source functions reproduced as much as 70% of the observed SSA concentration variability at several stations, which is comparable with "state of the art" aerosol models. The main driver of SSA production is wind, and we found that the best fit to the observation data could be obtained when the SSA production is proportional to U₁₀^3.5, where U₁₀ is the source region averaged 10 m wind speed. A strong influence of SST on SSA production, with higher temperatures leading to higher production, could be detected as well, although the underlying physical mechanisms of the SST influence remains unclear. Our new source function with wind speed and temperature dependence gives a global SSA production for particles smaller than D_p < 10 μm of 9 Pg yr⁻¹, and is the best fit to the observed concentrations.

In the Arctic, impurities in the atmosphere and cryosphere can strongly affect the atmospheric radiation and surface energy balance. While black carbon has hence received much attention, mineral dust has been in the background. Mineral dust is not only transported into the Arctic from remote regions but also, possibly increasingly, generated in the region itself. Here we study mineral dust in the Arctic based on global transport model simulations. For this, we have developed a dust mobilization scheme in combination with the Lagrangian particle dispersion model FLEXPART. A model evaluation, based on measurements of surface concentrations and annual deposition at a number of stations and aircraft vertical profiles, shows the suitability of this model to study global dust transport. Simulations indicate that about 3% of global dust emission originates from high‐latitude dust sources in the Arctic. Due to limited convection and enhanced efficiency of removal, dust emitted in these source regions is mostly deposited closer to the source than dust from for instance Asia or Africa. This leads to dominant contributions of local dust sources to total surface dust concentrations (~85%) and dust deposition (~90%) in the Arctic region. Dust deposition from local sources peaks in autumn, while dust deposition from remote sources occurs mainly in spring in the Arctic. With increasing altitude, remote sources become more important for dust concentrations as well as deposition. Therefore, total atmospheric dust loads in the Arctic are strongly influenced by Asian (~38%) and African (~32%) dust, whereas local dust contributes only 27%. Dust loads are thus largest in spring when remote dust is efficiently transported into the Arctic. Overall, our study shows that contributions of local dust sources are more important in the Arctic than previously thought, particularly with respect to surface concentrations and dust deposition.

A new, more physically based wet removal scheme for aerosols has been implemented in the Lagrangian particle dispersion model FLEXPART. It uses three-dimensional cloud water fields from the European Centre for Medium-Range Weather Forecasts (ECMWF) to determine cloud extent and distinguishes between in-cloud and below-cloud scavenging. The new in-cloud nucleation scavenging depends on cloud water phase (liquid, ice or mixed-phase), based on the aerosol's prescribed efficiency to serve as ice crystal nuclei and liquid water nuclei, respectively. The impaction scavenging scheme now parameterizes below-cloud removal as a function of aerosol particle size and precipitation type (snow or rain) and intensity. Sensitivity tests with the new scavenging scheme and comparisons with observational data were conducted for three distinct types of primary aerosols, which pose different challenges for modeling wet scavenging due to their differences in solubility, volatility and size distribution: (1) ¹³⁷Cs released during the Fukushima nuclear accident attached mainly to highly soluble sulphate aerosol particles, (2) black carbon (BC) aerosol particles, and (3) mineral dust. Calculated e-folding lifetimes of accumulation mode aerosols for these three aerosol types were 11.7, 16.0, and 31.6 days respectively, when well mixed in the atmosphere. These are longer lifetimes than those obtained by the previous removal schem, and, for mineral dust in particular, primarily result from very slow in-cloud removal, which globally is the primary removal mechanism for these accumulation mode particles. Calculated e-folding lifetimes in FLEXPART also have a strong size dependence, with the longest lifetimes found for the accumulation-mode aerosols. For example, for dust particles emitted at the surface the lifetimes were 13.8 days for particles with 1 µm diameter and a few hours for 10 µm particles. A strong size dependence in below-cloud scavenging, combined with increased dry removal, is the primary reason for the shorter lifetimes of the larger particles. The most frequent removal is in-cloud scavenging (85 % of all scavenging events) but it occurs primarily in the free troposphere, while below-cloud removal is more frequent below 1000 m (52 % of all events) and can be important for the initial fate of species emitted at the surface, such as those examined here. For assumed realistic in-cloud removal efficiencies, both BC and sulphate have a slight overestimation of observed atmospheric concentrations (a factor of 1.6 and 1.2 respectively). However, this overestimation is largest close to the sources and thus appears more related to overestimated emissions rather than underestimated removal. The new aerosol wet removal scheme of FLEXPART incorporates more realistic information about clouds and aerosol properties and it compares better with both observed lifetimes and concentration than the old scheme.

In this study we have analyzed whether tourist cruise ships have an influence on measured sulfur dioxide (SO₂), ozone (O₃), Aitken mode particle and equivalent black carbon (EBC) concentrations at Ny Ålesund and Zeppelin Mountain on Svalbard in the Norwegian Arctic during summer. We separated the measurement data set into periods when ships were present and periods when ships were not present in the Kongsfjord area, according to a long-term record of the number of passengers visiting Ny Ålesund. We show that when ships with more than 50 passengers cruise in the Kongsfjord, measured daytime mean concentrations of 60 nm particles and EBC in summer show enhancements of 72 and 45%, respectively, relative to values when ships are not present. Even larger enhancements of 81 and 72% were found for stagnant conditions. In contrast, O₃ concentrations were 5% lower on average and 7% lower under stagnant conditions, due to titration of O₃ with the emitted nitric oxide (NO). The differences between the two data subsets are largest for the highest measured percentiles, while relatively small differences were found for the median concentrations, indicating that ship plumes are sampled relatively infrequently even when ships are present although they carry high pollutant concentrations. We estimate that the ships increased the total summer mean concentrations of SO₂, 60 nm particles and EBC by 15, 18 and 11%, respectively. Our findings have two important implications. Firstly, even at such a remote Arctic observatory as Zeppelin, the measurements can be influenced by tourist ship emissions. Careful data screening is recommended before summertime Zeppelin data is used for data analysis or for comparison with global chemistry transport models. However, Zeppelin remains as one of the most valuable Arctic observatories, as most other Arctic observatories face even larger local pollution problems. Secondly, given landing statistics of tourist ships on Svalbard, it is suspected that large parts of the Svalbard archipelago are affected by cruise ship emissions. Thus, our results may be taken as a warning signal of future pan-Arctic conditions if Arctic shipping becomes more frequent and emission regulations are not strict enough.

We present here emissions estimated from a newly developed emission model for residential wood combustion (RWC) at high spatial and temporal resolution, which we name the MetVed model. The model estimates hourly emissions resolved on a 250 m grid resolution for several compounds, including particulate matter (PM), black carbon (BC) and polycyclic aromatic hydrocarbons (PAHs) in Norway for a 12-year period. The model uses novel input data and calculation methods that combine databases built with an unprecedented high level of detail and near-national coverage. The model establishes wood burning potential at the grid based on the dependencies between variables that influence emissions: i.e. outdoor temperature, number of and type and size of dwellings, type of available heating technologies, distribution of wood-based heating installations and their associated emission factors. RWC activity with a 1 h temporal profile was produced by combining heating degree day and hourly and weekday activity profiles reported by wood consumers in official statistics. This approach results in an improved characterisation of the spatio-temporal distribution of wood use, and subsequently of emissions, required for urban air quality assessments. Whereas most variables are calculated based on bottom-up approaches on a 250 m spatial grid, the MetVed model is set up to use official wood consumption at the county level and then distributes consumption to individual grids proportional to the physical traits of the residences within it. MetVed combines consumption with official emission factors that makes the emissions also upward scalable from the 250 m grid to the national level. The MetVed spatial distribution obtained was compared at the urban scale to other existing emissions at the same scale. The annual urban emissions, developed according to different spatial proxies, were found to have differences up to an order of magnitude. The MetVed total annual PM_2.5 emissions in the urban domains compare well to emissions adjusted based on concentration measurements. In addition, hourly PM_2.5 concentrations estimated by an Eulerian dispersion model using MetVed emissions were compared to measurements at air quality stations. Both hourly daily profiles and the seasonality of PM_2.5 show a slight overestimation of PM_2.5 levels. However, a comparison with black carbon from biomass burning and benzo(a)pyrene measurements indicates higher emissions during winter than that obtained by MetVed. The accuracy of urban emissions from RWC relies on the accuracy of the wood consumption (activity data), emission factors and the spatio-temporal distribution. While there are still knowledge gaps regarding emissions, MetVed represents a vast improvement in the spatial and temporal distribution of RWC.