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Abstract. Sulfate and nitrate aerosols degrade air quality, modulate radiative forcing and the hydrological cycle, and affect biogeochemical cycles, yet their global cycles are poorly understood. Here, we examined trends in 21 years of aerosol measurements made at Ragged Point, Barbados, the easternmost promontory on the island located in the eastern Caribbean Basin. Though the site has historically been used to characterize African dust transport, here we focused on changes in nitrate and non-sea-salt (nss) sulfate aerosols from 1990–2011. Nitrate aerosol concentrations averaged over the entire period were stable at 0.59 µg m−3 ± 0.04 µg m−3, except for elevated nitrate concentrations in the spring of 2010 and during the summer and fall of 2008 due to the transport of biomass burning emissions from both northern and southern Africa to our site. In contrast, from 1990 to 2000, nss-sulfate decreased 30 % at a rate of 0.023 µg m−3 yr−1, a trend which we attribute to air quality policies enacted in the United States (US) and Europe. From 2000–2011, sulfate gradually increased at a rate of 0.021 µg m−3 yr−1 to pre-1990s levels of 0.90 µg m−3. We used the Community Multiscale Air Quality (CMAQ) model simulations from the EPA's Air QUAlity TimE Series (EQUATES) to better understand the changes in nss-sulfate after 2000. The model simulations estimate that increases in anthropogenic emissions from Africa explain the increase in nss-sulfate observed in Barbados. Our results highlight the need to better constrain emissions from developing countries and to assess their impact on aerosol burdens in remote source regions. 

The number concentration and properties of aerosol particles serving as cloud condensation nuclei (CCN) are important for understanding cloud properties, including in the tropical Atlantic marine boundary layer (MBL), where marine cumulus clouds reflect incoming solar radiation and obscure the low-albedo ocean surface. Studies linking aerosol source, composition, and water uptake properties in this region have been conducted primarily during the summertime dust transport season, despite the region receiving a variety of aerosol particle types throughout the year. In this study, we compare size-resolved aerosol chemical composition data to the hygrocopicity parameter κ derived from size-resolved CCN measurements made during the Elucidating the Role of Clouds-Circulation Coupling in Climate (EUREC4A) and Atlantic Tradewind Ocean-Atmosphere Mesoscale Interaction Campaign (ATOMIC) campaigns from January to February 2020. We observed unexpected periods of wintertime long-range transport of African smoke and dust to Barbados. During these periods, the accumulation-mode aerosol particle and CCN Number concentrations as well as the proportions of dust and smoke particles increased, whereas average κ slightly decreased (κ = 0.46 +/- 0.10) from marine background conditions (κ = 0.52 +/- 0.09) when the particles were mostly composed of marine organics and sulfate. Size-resolved chemical analysis shows that smoke particles were the major contributor to the accumulation mode during long-range transport events, indicating that smoke is mainly responsible for the observed increase in CCN number concentrations. Earlier studies conducted at Barbados have mostly focused on the role of dust in CCN, but our results show that aerosol hygroscopicity and CCN number concentrations during wintertime long-range transport events over the tropical North Atlantic are also affected by African smoke. Our findings highlight the importance of African smoke for atmospheric processes and cloud formation over the Caribbean. In the file “Dust_Mass_Conc_Royer2022” dust mass concentrations in grams per meter^3 are provided for each day of sampling. These data were used to generate Figure 2a in the manuscript. The file “Particle_Type_#fract_Royer2022” contains data obtained through CCSEM/EDX analysis and used to generate the temporal chemistry plot (Figure 4) provided in the manuscript. The data contains particle numbers for each particle type identified on stage 3 of the sampler, total particle numbers analyzed for the entire stage 3 sample, as well as particle number fractions in % values. In the file “Size-resolved_chem_Royer2022” we provide particle # and number fraction (%) values used to generate size-resolved chemistry plots in the manuscript (Figures 5a and 5b). The file includes all particle numbers and number fractions for sea salt, aged sea salt, dust+sea salt, dust, dust+smoke, smoke, sulfate, and organic particles in each size bin from 0.1 through 8.058 um during cumulative clean marine periods and CAT Event 1 as described in the manuscript. The file “K_at_0.16S_Royer2022” contains κ values calculated at 0.16% supersaturation (S) throughout the entire sampling period. These data were specifically used to generate the plot in Figure 7a. The file “CCN#_at_0.16S_Royer2022” contains cloud condensation nuclei (CCN) values calculated at 0.16% supersaturation (S) throughout the entire sampling period. These data were used to create the CCN portion of the plot in Figure 7b. 

Abstract. The number concentration and properties of aerosol particles serving ascloud condensation nuclei (CCN) are important for understanding cloudproperties, including in the tropical Atlantic marine boundary layer (MBL), where marine cumulus clouds reflect incoming solar radiation and obscure thelow-albedo ocean surface. Studies linking aerosol source, composition, andwater uptake properties in this region have been conducted primarily duringthe summertime dust transport season, despite the region receiving a varietyof aerosol particle types throughout the year. In this study, we comparesize-resolved aerosol chemical composition data to the hygroscopicityparameter κ derived from size-resolved CCN measurements made duringthe Elucidating the Role of Clouds–Circulation Coupling in Climate (EUREC4A) and Atlantic Tradewind Ocean-Atmosphere Mesoscale Interaction Campaign (ATOMIC) campaigns from January to February 2020. Weobserved unexpected periods of wintertime long-range transport of Africansmoke and dust to Barbados. During these periods, the accumulation-mode aerosol particle and CCN number concentrations as well as the proportions ofdust and smoke particles increased, whereas the average κ slightlydecreased (κ=0.46±0.10) from marine backgroundconditions (κ=0.52±0.09) when the submicron particles were mostly composed of marine organics and sulfate. Size-resolved chemicalanalysis shows that smoke particles were the major contributor to theaccumulation mode during long-range transport events, indicating that smokeis mainly responsible for the observed increase in CCN numberconcentrations. Earlier studies conducted at Barbados have mostly focused onthe role of dust on CCN, but our results show that aerosol hygroscopicity and CCN number concentrations during wintertime long-range transport events over the tropical North Atlantic are also affected by African smoke. Ourfindings highlight the importance of African smoke for atmospheric processesand cloud formation over the Caribbean.