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Anthropogenic ammonia (NH₃) emissions have significantly increased in recent decades due to enhanced agricultural activities, contributing to global air pollution. While the effects of NH₃on surface air quality are well documented, its influence on particle dynamics in the upper troposphere-lower stratosphere (UTLS) and related aerosol impacts remain unquantified. NH₃reaches the UTLS through convective transport and can enhance new particle formation (NPF). This modeling study evaluates the global impact of anthropogenic NH₃on UTLS particle formation and quantifies its effects on aerosol loading and cloud condensation nuclei (CCN) abundance. We use the EMAC Earth system model, incorporating multicomponent NPF parameterizations from the CERN CLOUD experiment. Our simulations reveal that convective transport increases NH₃-driven NPF in the UTLS by one to three orders of magnitude compared to a baseline scenario without anthropogenic NH₃, causing a doubling of aerosol numbers over high-emission regions. These aerosol changes induce a 2.5-fold increase in upper tropospheric CCN concentrations. Anthropogenic NH₃emissions increase the relative contribution of water-soluble inorganic ions to the UTLS aerosol optical depth (AOD) by 20% and increase total column AOD by up to 80%. In simulations without anthropogenic NH₃, UTLS aerosol composition is dominated by sulfate and organic species, with a marked reduction in ammonium nitrate and aerosol water content. This results in a decline of aerosol mass concentration by up to 50%. These findings underscore the profound global influence of anthropogenic NH₃emissions on UTLS particle formation, AOD, and CCN production, with important implications for cloud formation and climate. 

Abstract Isoprene (C₅H₈) is the non-methane hydrocarbon with the highest emissions to the atmosphere. It is mainly produced by vegetation, especially broad-leaved trees, and efficiently transported to the upper troposphere in deep convective clouds, where it is mixed with lightning NO_x. Isoprene oxidation products drive rapid formation and growth of new particles in the tropical upper troposphere. However, isoprene oxidation pathways at low temperatures are not well understood. Here, in experiments at the CERN CLOUD chamber at 223 K and 243 K, we find that isoprene oxygenated organic molecules (IP-OOM) all involve two successive$${{{\rm{OH}}}}^{\bullet}$$ ${\mathrm{OH}}^{\bullet }$oxidations. However, depending on the ambient concentrations of the termination radicals ($${{{{\rm{HO}}}}_{2}}^{\bullet},\,{{{\rm{NO}}}}^{\bullet}$$ ${{\mathrm{HO}}_2}^{\bullet },{\mathrm{NO}}^{\bullet }$, and$${{{\rm{NO}}}}_{2}^{\bullet}$$ ${\mathrm{NO}}_2^{\bullet }$), vastly-different IP-OOM emerge, comprising compounds with zero, one or two nitrogen atoms. Our findings indicate high IP-OOM production rates for the tropical upper troposphere, mainly resulting in nitrate IP-OOM but with an increasing non-nitrate fraction around midday, in close agreement with aircraft observations. 

Abstract During summer, ammonia emissions in Southeast Asia influence air pollution and cloud formation. Convective transport by the South Asian monsoon carries these pollutant air masses into the upper troposphere and lower stratosphere (UTLS), where they accumulate under anticyclonic flow conditions. This air mass accumulation is thought to contribute to particle formation and the development of the Asian Tropopause Aerosol Layer (ATAL). Despite the known influence of ammonia and particulate ammonium on air pollution, a comprehensive understanding of the ATAL is lacking. In this modelling study, the influence of ammonia on particle formation is assessed with emphasis on the ATAL. We use the EMAC chemistry-climate model, incorporating new particle formation parameterisations derived from experiments at the CERN CLOUD chamber. Our diurnal cycle analysis confirms that new particle formation mainly occurs during daylight, with a 10-fold enhancement in rate. This increase is prominent in the South Asian monsoon UTLS, where deep convection introduces high ammonia levels from the boundary layer, compared to a baseline scenario without ammonia. Our model simulations reveal that this ammonia-driven particle formation and growth contributes to an increase of up to 80% in cloud condensation nuclei (CCN) concentrations at cloud-forming heights in the South Asian monsoon region. We find that ammonia profoundly influences the aerosol mass and composition in the ATAL through particle growth, as indicated by an order of magnitude increase in nitrate levels linked to ammonia emissions. However, the effect of ammonia-driven new particle formation on aerosol mass in the ATAL is relatively small. Ammonia emissions enhance the regional aerosol optical depth (AOD) for shortwave solar radiation by up to 70%. We conclude that ammonia has a pronounced effect on the ATAL development, composition, the regional AOD, and CCN concentrations. 

The Great Atlantic Sargassum Belt (GASB) first appeared in 2011 and quickly became the largest interconnected floating biome globally. Sargassum spp. requires both phosphorus (P) and nitrogen (N) for growth, yet the sources fueling the GASB are unclear. Here, we use coral–bound nitrogen isotopes from six coral cores to reconstruct N2 fixation, the primary source of bioavailable N to the surface ocean across the wider Caribbean over the past 120 years. Our data indicate that changes in N2 fixation were controlled by multidecadal and interannual changes in the supply of excess P from equatorial upwelling in the Atlantic. We show that the supply of P from equatorial upwelling and N from the N2 fixation response can explain the extent of the GASB since 2011. # Equatorial upwelling of phosphorus drives Atlantic N~2~ fixation and *Sargassum* blooms This Excel file contains time series data combining coral geochemical records (δ¹⁵N and δ¹⁸O), climate indices, Sargassum biomass, and major riverine outflows. The dataset integrates multiple spatially distributed records to examine long-term variability in nutrient dynamics, climate forcing, and ecological responses in the Caribbean and tropical Atlantic. Values that were not available or are missing are indicated as N/A. ## Column Reference Table File: Caribbean_data_for_DRYAD.xlsx | Column Name | Description | | :----------------------------------- | :------------------------------------------------------------------------------------------------- | | **Year\_CR\_Turneffe** | Calendar year of sampling for coral records from Turneffe Atoll (Belize) and Cahuita (Costa Rica). | | **Cahuita Costa Rica\_d18O\_ts** | Coral δ¹⁸O time series from Cahuita, Costa Rica (proxy for SST and freshwater input). | | **d15N\_CR** | Coral-bound δ¹⁵N from Cahuita, Costa Rica (proxy for nitrogen source/processing). | | **Turneffe Atoll\_d18O\_ts** | Coral δ¹⁸O time series from Turneffe Atoll, Belize. | | **d15N\_Turneffe** | Coral-bound δ¹⁵N from Turneffe Atoll. | | **Date\_MQ** | Sampling date for Martinique (MQ) site. | | **d18O\_MQ** | Coral δ¹⁸O from Martinique. | | **d15N\_MQ** | Coral δ¹⁵N from Martinique. | | **Year Bermuda** | Calendar year for Bermuda coral samples. | | **d15N Bermuda** | Coral δ¹⁵N from Bermuda. | | **Year\_CUBA** | Calendar year for Cuban coral records. | | **d15N\_CUBA** | Coral δ¹⁵N from Cuba. | | **d15N\_Mexico** | Coral δ¹⁵N from Mexico. | | **Year\_Tobago** | Calendar year for Tobago coral samples. | | **d15N\_Tobago** | Coral δ¹⁵N from Tobago. | | **Year AMM** | Year corresponding to Atlantic Meridional Mode (AMM) values. | | **AMM\_SST** | Sea Surface Temperature anomalies associated with the AMM. | | **AMM\_Wind** | Wind anomalies associated with the AMM. | | **AMO** | Atlantic Multidecadal Oscillation index value. | | **average\_year** | Averaged year across all coral records included. | | **AVERAGE\_rescaled** | Composite δ¹⁵N record rescaled across sites. | | **error\_propagated** | Propagated error estimate for the rescaled average. | | **AVERAGE\_rescaled\_noCR\_BM\_TB** | Rescaled δ¹⁵N average excluding Costa Rica, Bermuda, and Tobago. | | **error\_propagated2** | Propagated error for the reduced-site average. | | **Months Sargassum** | Month of Sargassum observation. | | **Monthly Sargassum biomass (tons)** | Monthly biomass estimates of pelagic Sargassum (tons). | | **Year\_SST\_SSS** | Year corresponding to SST/SSS data. | | **SST\_10-20N\_20-60W** | Sea Surface Temperature average over 10–20°N, 20–60°W. | | **SSS\_10-20N\_20-60W** | Sea Surface Salinity average over the same region. | | **U\_windstress\_10\_20N\_58\_62W** | Zonal wind stress (10–20°N, 58–62°W). | | **windspeed\_0\_20N\_20\_50W** | Mean wind speed (0–20°N, 20–50°W). | | **Geo\_u\_12\_18N\_60\_80W (CC)** | Geostrophic zonal velocity (12–18°N, 60–80°W), Caribbean Current proxy. | | **DU\_scav\_areaweight** | Dust deposition (scavenging flux, area-weighted). | | **DU\_ddep\_areaweight** | Dust dry deposition (area-weighted). | | **BC\_scav\_areaweight** | Black carbon scavenging flux (area-weighted). | | **Bc\_ddep\_areaweight** | Black carbon dry deposition (area-weighted). | | **BC\_total\_areaweight** | Total black carbon deposition (area-weighted). | | **DU\_total\_areaweight** | Total dust deposition (area-weighted). | | **Obidos\_Amazon\_m3\_s** | Amazon River discharge at Óbidos station (m³/s). | | **Ciudad Bolivar\_Orinoco\_m3\_s** | Orinoco River discharge at Ciudad Bolívar (m³/s). | | **Year Pstar** | Year corresponding to P\* (phosphorus excess) record. | | **Pstar** | Phosphorus excess (indicator of nutrient balance, micro Molar). | | **Amazon\_outflow\_date** | Date of Amazon outflow measurement. | | **Amazon\_outflow\_km3** | Amazon River outflow volume (km³). | | **Orinoco\_outflow\_date** | Date of Orinoco outflow measurement. | | **Orinoco\_outflow\_km3** | Orinoco River outflow volume (km³). | Links to other publicly accessible locations of the data: * [https://climexp.knmi.nl](http://...) Data was derived from the following sources: * Climate Explorer was used for gridded satellite-derived products (SST, SSS, windspeed, windstress) by using the geographical extent as indicated in the manuscript ## Code/Software No software was used for data analysis, and the codes used for figures and data analyses are available on GitHub ([https://github.com/marinejon/](https://github.com/marinejon/)) 

Abstract Aircraft observations have revealed ubiquitous new particle formation in the tropical upper troposphere over the Amazon^1,2and the Atlantic and Pacific oceans^3,4. Although the vapours involved remain unknown, recent satellite observations have revealed surprisingly high night-time isoprene mixing ratios of up to 1 part per billion by volume (ppbv) in the tropical upper troposphere⁵. Here, in experiments performed with the CERN CLOUD (Cosmics Leaving Outdoor Droplets) chamber, we report new particle formation initiated by the reaction of hydroxyl radicals with isoprene at upper-tropospheric temperatures of −30 °C and −50 °C. We find that isoprene-oxygenated organic molecules (IP-OOM) nucleate at concentrations found in the upper troposphere, without requiring any more vapours. Moreover, the nucleation rates are enhanced 100-fold by extremely low concentrations of sulfuric acid or iodine oxoacids above 10⁵ cm⁻³, reaching rates around 30 cm⁻³ s⁻¹at acid concentrations of 10⁶ cm⁻³. Our measurements show that nucleation involves sequential addition of IP-OOM, together with zero or one acid molecule in the embryonic molecular clusters. IP-OOM also drive rapid particle growth at 3–60 nm h⁻¹. We find that rapid nucleation and growth rates persist in the presence of NO_xat upper-tropospheric concentrations from lightning. Our laboratory measurements show that isoprene emitted by rainforests may drive rapid new particle formation in extensive regions of the tropical upper troposphere^1,2, resulting in tens of thousands of particles per cubic centimetre. 

Abstract. Information on the rate of diffusion of organic moleculeswithin secondary organic aerosol (SOA) is needed to accurately predict theeffects of SOA on climate and air quality. Diffusion can be important forpredicting the growth, evaporation, and reaction rates of SOA under certainatmospheric conditions. Often, researchers have predicted diffusion rates oforganic molecules within SOA using measurements of viscosity and theStokes–Einstein relation (D∝1/η, where D is the diffusioncoefficient and η is viscosity). However, the accuracy of thisrelation for predicting diffusion in SOA remains uncertain. Usingrectangular area fluorescence recovery after photobleaching (rFRAP), wedetermined diffusion coefficients of fluorescent organic molecules over8 orders in magnitude in proxies of SOA including citric acid, sorbitol,and a sucrose–citric acid mixture. These results were combined withliterature data to evaluate the Stokes–Einstein relation for predictingthe diffusion of organic molecules in SOA. Although almost all the data agreewith the Stokes–Einstein relation within a factor of 10, a fractionalStokes–Einstein relation (D∝1/ηξ) with ξ=0.93is a better model for predicting the diffusion of organic molecules in the SOAproxies studied. In addition, based on the output from a chemical transportmodel, the Stokes–Einstein relation can overpredict mixing times of organicmolecules within SOA by as much as 1 order of magnitude at an altitudeof ∼3 km compared to the fractional Stokes–Einstein relation with ξ=0.93. These results also have implications for other areas such as infood sciences and the preservation of biomolecules. 

Abstract New particle formation in the upper free troposphere is a major global source of cloud condensation nuclei (CCN) 1–4 . However, the precursor vapours that drive the process are not well understood. With experiments performed under upper tropospheric conditions in the CERN CLOUD chamber, we show that nitric acid, sulfuric acid and ammonia form particles synergistically, at rates that are orders of magnitude faster than those from any two of the three components. The importance of this mechanism depends on the availability of ammonia, which was previously thought to be efficiently scavenged by cloud droplets during convection. However, surprisingly high concentrations of ammonia and ammonium nitrate have recently been observed in the upper troposphere over the Asian monsoon region 5,6 . Once particles have formed, co-condensation of ammonia and abundant nitric acid alone is sufficient to drive rapid growth to CCN sizes with only trace sulfate. Moreover, our measurements show that these CCN are also highly efficient ice nucleating particles—comparable to desert dust. Our model simulations confirm that ammonia is efficiently convected aloft during the Asian monsoon, driving rapid, multi-acid HNO 3 –H 2 SO 4 –NH 3 nucleation in the upper troposphere and producing ice nucleating particles that spread across the mid-latitude Northern Hemisphere.