ALBERT

Description: Anthropogenic nitrogen (N) emissions to the atmosphere have increased significantly the deposition of nitrate (NO3−) and ammonium (NH4+) to the surface waters of the open ocean, with potential impacts on marine productivity and the global carbon cycle. Global-scale understanding of the impacts of N deposition to the oceans is reliant on our ability to produce and validate models of nitrogen emission, atmospheric chemistry, transport and deposition. In this work,  ∼  2900 observations of aerosol NO3− and NH4+ concentrations, acquired from sampling aboard ships in the period 1995–2012, are used to assess the performance of modelled N concentration and deposition fields over the remote ocean. Three ocean regions (the eastern tropical North Atlantic, the northern Indian Ocean and northwest Pacific) were selected, in which the density and distribution of observational data were considered sufficient to provide effective comparison to model products. All of these study regions are affected by transport and deposition of mineral dust, which alters the deposition of N, due to uptake of nitrogen oxides (NOx) on mineral surfaces. Assessment of the impacts of atmospheric N deposition on the ocean requires atmospheric chemical transport models to report deposition fluxes; however, these fluxes cannot be measured over the ocean. Modelling studies such as the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP), which only report deposition flux, are therefore very difficult to validate for dry deposition. Here, the available observational data were averaged over a 5° × 5° grid and compared to ACCMIP dry deposition fluxes (ModDep) of oxidised N (NOy) and reduced N (NHx) and to the following parameters from the Tracer Model 4 of the Environmental Chemical Processes Laboratory (TM4): ModDep for NOy, NHx and particulate NO3− and NH4+, and surface-level particulate NO3− and NH4+ concentrations. As a model ensemble, ACCMIP can be expected to be more robust than TM4, while TM4 gives access to speciated parameters (NO3− and NH4+) that are more relevant to the observed parameters and which are not available in ACCMIP. Dry deposition fluxes (CalDep) were calculated from the observed concentrations using estimates of dry deposition velocities. Model–observation ratios (RA, n), weighted by grid-cell area and number of observations, were used to assess the performance of the models. Comparison in the three study regions suggests that TM4 overestimates NO3− concentrations (RA, n =  1.4–2.9) and underestimates NH4+ concentrations (RA, n =  0.5–0.7), with spatial distributions in the tropical Atlantic and northern Indian Ocean not being reproduced by the model. In the case of NH4+ in the Indian Ocean, this discrepancy was probably due to seasonal biases in the sampling. Similar patterns were observed in the various comparisons of CalDep to ModDep (RA, n =  0.6–2.6 for NO3−, 0.6–3.1 for NH4+). Values of RA, n for NHx CalDep–ModDep comparisons were approximately double the corresponding values for NH4+ CalDep–ModDep comparisons due to the significant fraction of gas-phase NH3 deposition incorporated in the TM4 and ACCMIP NHx model products. All of the comparisons suffered due to the scarcity of observational data and the large uncertainty in dry deposition velocities used to derive deposition fluxes from concentrations. These uncertainties have been a major limitation on estimates of the flux of material to the oceans for several decades. Recommendations are made for improvements in N deposition estimation through changes in observations, modelling and model–observation comparison procedures. Validation of modelled dry deposition requires effective comparisons to observable aerosol-phase species' concentrations, and this cannot be achieved if model products only report dry deposition flux over the ocean.

Description: Arid regions are a major source of mineral dust aerosol. Transport from these sources can have a great impact on aerosol climatology in distant regions. In order to assess the impact of dust on climate we must understand how dust properties change after long distance transport from sources. This study addresses the changes in columnar aerosol properties when mineral dust outbreaks from western Africa arrive over the eastern Caribbean after transport across the Atlantic Ocean, a transit of 5–7 days. We use data from the NASA Aerosol Robotic Network (AERONET) located at five Caribbean and two western Africa sites to characterize changes in columnar aerosol properties: aerosol optical depth (AOD), size distribution, single scattering albedo, and refractive indexes. We first characterized the local aerosol climatology at each site and then using air mass back trajectories we identified those days when trajectories over Caribbean sites back-tracked to western Africa. Over the period 1996–2014 we identify 3174 days, an average of 167 days per year, when the air mass over the Caribbean sites could be linked to at least one of the two western Africa sites. For 1162 of these days, AOD data are available for the Caribbean sites as well as for the corresponding western Africa sites about 5–7 days earlier, when the air mass passed over these sites. We identified dust outbreaks as those air masses yielding AOD  ≥  0.2 and an Ångström exponent below 0.6. On this basis of the total 1162 days, 484 meet the criteria for mineral dust outbreaks. We observe that the AOD at 440 nm decreases by about 0.16 or 30 % during transport. The volume particle size distribution shows a similar decrease in the volume concentration, mainly in the coarse mode. The single scattering albedo, refractive indexes, and asymmetry factor remain unchanged. The difference in the effective radius over western Africa sites with respect to Caribbean sites ranges between 0 and −0.3 µm. Finally we conclude that in about half of the cases only non-spherical dust particles are present in the atmosphere over the western Africa and Caribbean sites, while in the other cases dust particles were mixed with other types of aerosol particles.

Description: Icelandic dust sources are known to be highly active, yet there exist few model simulations of Icelandic dust that could be used to assess its impacts on the environment. We here present estimates of dust emission and transport in Iceland over 27 years (1990–2016) based on FLEXDUST and FLEXPART simulations and meteorological re-analysis data. Simulations for the year 2012 based on high-resolution operational meteorological analyses are used for model evaluation based on PM2. 5 and PM10 observations in Iceland. For stations in Reykjavik, we find that the spring period is well predicted by the model, while dust events in late fall and early winter are overpredicted. Six years of dust concentrations observed at Stórhöfði (Heimaey) show that the model predicts concentrations of the same order of magnitude as observations and timing of modelled and observed dust peaks agrees well. Average annual dust emission is 4.3 ± 0.8 Tg during the 27 years of simulation. Fifty percent of all dust from Iceland is on average emitted in just 25 days of the year, demonstrating the importance of a few strong events for annual total dust emissions. Annual dust emission as well as transport patterns correlate only weakly to the North Atlantic Oscillation. Deposition amounts in remote regions (Svalbard and Greenland) vary from year to year. Only limited dust amounts reach the upper Greenland Ice Sheet, but considerable dust amounts are deposited on Icelandic glaciers and can impact melt rates there. Approximately 34 % of the annual dust emission is deposited in Iceland itself. Most dust (58 %), however, is deposited in the ocean and may strongly influence marine ecosystems.

Description: Dust emission is initiated when surface wind velocities exceed the threshold of wind erosion. Many dust models used constant threshold values globally. Here we use satellite products to characterize the frequency of dust events and land surface properties. By matching this frequency derived from Moderate Resolution Imaging Spectroradiometer (MODIS) Deep Blue aerosol products with surface winds, we are able to retrieve a climatological monthly global distribution of the wind erosion threshold (Vthreshold) over dry and sparsely vegetated surfaces. This monthly two-dimensional threshold velocity is then implemented into the Geophysical Fluid Dynamics Laboratory coupled land–atmosphere model (AM4.0/LM4.0). It is found that the climatology of dust optical depth (DOD) and total aerosol optical depth, surface PM10 dust concentrations, and the seasonal cycle of DOD are better captured over the “dust belt” (i.e., northern Africa and the Middle East) by simulations with the new wind erosion threshold than those using the default globally constant threshold. The most significant improvement is the frequency distribution of dust events, which is generally ignored in model evaluation. By using monthly rather than annual mean Vthreshold, all comparisons with observations are further improved. The monthly global threshold of wind erosion can be retrieved under different spatial resolutions to match the resolution of dust models and thus can help improve the simulations of dust climatology and seasonal cycles as well as dust forecasting.

Description: Mineral dust aerosol can be a major driver of aerosol climatology in regions distant from the sources. This study addresses the change of columnar aerosol properties when mineral dust arrives to the Caribbean Basin after transport from Africa over the Atlantic Ocean. We use data from NASA Aerosol Robotic Network (AERONET) sites in five Caribbean and two West African sites to characterize changes in aerosol properties: aerosol optical depth, size distribution, single scattering albedo, and refractive indexes. After obtaining local aerosol climatology in each area, the air mass connections between West Africa and Caribbean Basin have been investigated by means of air mass back trajectories. Over the period 1996–2014 we identify 3174 connection days, on average, 167 connection days per year. Among these, 1162 pairs of data present aerosol data in Caribbean sites with corresponding aerosol observations in Western Africa sites ~5–7 days before. Of these 1162 days, 484 meet the criteria to be characterized as mineral dust outbreaks. Based on these days we observe the following changes in aerosol-related properties in transiting the Atlantic: AOD decreases about 0.16 or −30 %; the volume particle size distribution shape shows no changes; single scattering albedo, refractive indexes, and asymmetry factor remain unchanged; the difference in the effective radius in West African area with respect to Caribbean Basin is between 0 and +0.3 µm; and half of the analyzed cases present predominance of non-spherical particles in both areas.

Description: Dust emission is initiated when surface wind velocities exceed the threshold of wind erosion. Most dust models used constant threshold values globally. Here we use satellite products to characterize the frequency of dust events and surface properties. By matching this frequency derived from Moderate Resolution Imaging Spectroradiometer (MODIS) Deep Blue aerosol products with surface winds, we are able to retrieve a climatological monthly global distribution of wind erosion threshold (Vthreshold) over dry and sparsely-vegetated surface. This monthly two-dimensional threshold velocity is then implemented into the Geophysical Fluid Dynamics Laboratory coupled land-atmosphere model (AM4.0/LM4.0). It is found that the climatology of dust optical depth (DOD) and total aerosol optical depth, surface PM10 dust concentrations, and seasonal cycle of DOD are better captured over the dust belt (i.e. North Africa and the Middle East) by simulations with the new wind erosion threshold than those using the default globally constant threshold. The most significant improvement is the frequency distribution of dust events, which is generally ignored in model evaluation. By using monthly rather than annual mean Vthreshold, all comparisons with observations are further improved. The monthly global threshold of wind erosion can be retrieved under different spatial resolutions to match the resolution of dust models and thus can help improve the simulations of dust climatology and seasonal cycle as well as dust forecasting.

Description: Icelandic dust sources are known to be highly active, yet there exist few model simulations of Icelandic dust that could be used to assess its impacts on the environment. We here present estimates of dust emission and transport in Iceland over 27 years (1990–2016) based on FLEXDUST & FLEXPART simulations and meteorological re-analysis data. Simulations for the year 2012 based on high-resolution operational meteorological analyses are used for model evaluation based on PM2.5 and PM10 observations in Iceland. For stations in Reykjavik, we find that the spring period is well predicted by the model, while dust events in late fall and early winter are overpredicted. Six years of dust concentrations observed at Stórhöfði (Heimaey) show that the model predicts concentrations in the same order of magnitude as observations and timing of modelled and observed dust peaks agrees well. Annual dust emission amounts to 4.3±0.8 Tg during the 27 years of simulation. Fifty percent of all dust from Iceland is on average emitted in just 25 days of the year, demonstrating the importance of a few strong events for annual total dust emissions. Annual dust emission as well as transport patterns correlate only weakly to the North Atlantic Oscillation. Deposition amounts in remote regions (Svalbard and Greenland) vary from year to year. Only limited dust amounts reach the upper Greenland Ice Sheet, but much dust is deposited on Icelandic glaciers and can impact melt rates there. Approximately 34 % of the annual dust emission is deposited in Iceland itself. Most dust (58 %) however, is deposited in the ocean and may strongly influence marine ecosystems.

Description: Nitrogen (N) emissions to the atmosphere have increased by a factor of 3–4 through anthropogenic activity since the Industrial Revolution. This has led to large increases in the deposition of nitrate (NO3−) and ammonium (NH4+) to the surface waters of the open ocean, with potential impacts on marine productivity and the global carbon cycle. Global-scale understanding of N deposition to the oceans is reliant on our ability to produce and validate models of nitrogen emission, atmospheric chemistry, transport and deposition. In this work, ~ 2900 observations of aerosol NO3− and NH4+ concentrations, acquired from sampling aboard ships in the period 1995–2012, are used to assess the performance of modelled N concentration and deposition fields over the remote ocean. Three ocean regions (the eastern tropical North Atlantic, the northern Indian Ocean and northwest Pacific) were selected in which the density and distribution of observational data were considered sufficient to provide effective comparison to model products. All of these study regions are affected by transport and deposition of mineral dust, which alters the deposition of N. Surface particulate NO3− and NH4+ concentrations simulated by the TM4-ECPL (TM4) model were compared to observed aerosol concentrations. Dry deposition fluxes of these species predicted by TM4 (ModDep) were compared with equivalent fluxes calculated from the observed concentrations (CalDep) using two commonly applied methods for the determination of CalDep. CalDep was also compared to total dry deposition fluxes of oxidised N (NOy) and reduced N (NHx) from TM4 and the ACCMIP multi-model mean product. Comparison in the three study regions suggests that TM4 over-estimates NO3− concentrations and under-estimates NH4+ concentrations, with spatial distributions in the tropical Atlantic and northern Indian Ocean not being reproduced by the model. In the case of NH4+ in the Indian Ocean, this discrepancy was probably due to seasonal biases in the sampling. Similar patterns were observed in the various comparisons of CalDep to ModDep and it was not possible to assess objectively the relative merits of the two methods for estimating CalDep. Comparisons of NH4+ CalDep to NHx ModDep were impaired by the significant fraction of gas-phase NH3 deposition incorporated in the TM4 and ACCMIP model products. All of the comparisons (of concentration and deposition) suffered due to the large uncertainty in dry deposition velocities used in the models and in the calculation of CalDep. These uncertainties have been a major limitation on estimates of the flux of material to the oceans for several decades.

Description: Cloud optical properties in the trade winds over the eastern Caribbean Sea have been shown to be sensitive to cloud condensation nuclei (CCN) concentrations. The objective of the current study was to investigate the CCN properties in the marine boundary layer (MBL) in the tropical western North Atlantic, in order to assess the respective roles of inorganic sulfate, organic species, long-range transported mineral dust and sea-salt particles. Measurements were carried out in June–July 2013, on the east coast of Barbados, and included CCN number concentrations, particle number size distributions and offline analysis of sampled particulate matter (PM) and sampled accumulation mode particles for an investigation of composition and mixing state with transmission electron microscopy (TEM) in combination with energy-dispersive X-ray spectroscopy (EDX). During most of the campaign, significant mass concentrations of long-range transported mineral dust was present in the PM, and influence from local island sources can be ruled out. The CCN and particle number concentrations were similar to what can be expected in pristine marine environments. The hygroscopicity parameter κ was inferred, and values in the range 0.2–0.5 were found during most of the campaign, with similar values for the Aitken and the accumulation mode. The accumulation mode particles studied with TEM were dominated by non-refractory material, and concentrations of mineral dust, sea salt and soot were too small to influence the CCN properties. It is highly likely that the CCN were dominated by a mixture of sulfate species and organic compounds.