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Ice-nucleating proteins (INPs) catalyze ice formation at high subzero temperatures, with major biological and environmental implications. While bacterial INPs have been structurally characterized, their counterparts in other organisms remain unknown. Here, we identify a new class of efficient INPs in fungi. These proteins are membrane-free, adopt β-solenoid folds, and multimerize to form large ice-binding surfaces, showing mechanistic parallels with bacterial INPs. Structural modeling, sequence analysis, and functional assays show they are encoded by orthologs of the bacterial InaZ gene, likely acquired via horizontal gene transfer. Our results demonstrate that distinct lineages have independently converged on a common molecular strategy to overcome the energetic barriers of ice formation. The discovery of cell-free INPs provides tools for freezing applications and reveals biophysical constraints on nucleation across life. 

Various aerosols, including mineral dust, soot, and biological particles, can act as ice nuclei, initiating the freezing of supercooled cloud droplets. Cloud droplet freezing significantly impacts cloud properties and, consequently, weather and climate. Some biological ice nuclei exhibit exceptionally high nucleation temperatures close to 0 °C. Ice-nucleating macromolecules (INMs) found on pollen are typically not considered among the most active ice nuclei. Still, they can be highly abundant, especially for species such as Betula pendula, a widespread birch tree species in the boreal forest. Recent studies have shown that certain tree-derived INMs exhibit ice nucleation activity above −10 °C, suggesting they could play a more significant role in atmospheric processes than previously understood. Our study reveals that three distinct INM classes active at −8.7, −15.7, and −17.4 °C are present in B. pendula. Freeze drying and freeze–thaw cycles noticeably alter their ice nucleation capability, and the results of heat treatment, size, and chemical analysis indicate that INM classes correspond to size-varying aggregates, with larger aggregates nucleating ice at higher temperatures, in agreement with previous studies on fungal and bacterial ice nucleators. Our findings suggest that B. pendula INMs are potentially important for atmospheric ice nucleation because of their high prevalence and nucleation temperatures. 

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/)) 

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. 

Abstract. Mass accommodation is an essential process for gas–particle partitioning oforganic compounds in secondary organic aerosols (SOA). The massaccommodation coefficient is commonly described as the probability of a gasmolecule colliding with the surface to enter the particle phase. It is oftenapplied, however, without specifying if and how deep a molecule has topenetrate beneath the surface to be regarded as being incorporated into thecondensed phase (adsorption vs. absorption). While this aspect is usuallynot critical for liquid particles with rapid surface–bulk exchange, it canbe important for viscous semi-solid or glassy solid particles to distinguishand resolve the kinetics of accommodation at the surface, transfer acrossthe gas–particle interface, and further transport into the particle bulk. For this purpose, we introduce a novel parameter: an effective massaccommodation coefficient αeff that depends on penetrationdepth and is a function of surface accommodation coefficient, volatility,bulk diffusivity, and particle-phase reaction rate coefficient. Applicationof αeff in the traditional Fuchs–Sutugin approximation ofmass-transport kinetics at the gas–particle interface yields SOApartitioning results that are consistent with a detailed kinetic multilayermodel (kinetic multilayer model of gas–particle interactions in aerosols and clouds, KM-GAP; Shiraiwa et al., 2012) and two-film model solutions (Modelfor Simulating Aerosol Interactions and Chemistry, MOSAIC;Zaveri et al., 2014) but deviate substantially from earlier modelingapproaches not considering the influence of penetration depth and relatedparameters. For highly viscous or semi-solid particles, we show that the effective massaccommodation coefficient remains similar to the surface accommodationcoefficient in the case of low-volatility compounds, whereas it can decrease byseveral orders of magnitude in the case of semi-volatile compounds. Such effectscan explain apparent inconsistencies between earlier studies deriving massaccommodation coefficients from experimental data or from molecular dynamicssimulations. Our findings challenge the approach of traditional SOA models using theFuchs–Sutugin approximation of mass transfer kinetics with a fixed massaccommodation coefficient, regardless of particle phase state and penetrationdepth. The effective mass accommodation coefficient introduced in this studyprovides an efficient new way of accounting for the influence of volatility,diffusivity, and particle-phase reactions on SOA partitioning in processmodels as well as in regional and global air quality models. While kineticlimitations may not be critical for partitioning into liquid SOA particlesin the planetary boundary layer (PBL), the effects are likely important foramorphous semi-solid or glassy SOA in the free and upper troposphere (FT–UT)as well as in the PBL at low relative humidity and low temperature. 

Abstract. Polycyclic aromatic hydrocarbons (PAHs) are carcinogenic air pollutants. The dispersion of PAHs in the atmosphere is influenced by gas–particle partitioning and chemical loss. These processes are closely interlinked and may occur at vastly differing timescales, which complicates their mathematical description in chemical transport models. Here, we use a kinetic model that explicitly resolves mass transport and chemical reactions in the gas and particle phases to describe and explore the dynamic and non-equilibrium interplay of gas–particle partitioning and chemical losses of PAHs on soot particles. We define the equilibration timescale τeq of gas–particle partitioning as the e-folding time for relaxation of the system to the partitioning equilibrium. We find this metric to span from seconds to hours depending on temperature, particle surface area, and the type of PAH. The equilibration time can be approximated using a time-independent equation, τeq≈1kdes+kads, which depends on the desorption rate coefficient kdes and adsorption rate coefficient kads, both of which can be calculated from experimentally accessible parameters. The model reveals two regimes in which different physical processes control the equilibration timescale: a desorption-controlled and an adsorption-controlled regime. In a case study with the PAH pyrene, we illustrate how chemical loss can perturb the equilibrium particulate fraction at typical atmospheric concentrations of O3 and OH. For the surface reaction with O3, the perturbation is significant and increases with the gas-phase concentration of O3. Conversely, perturbations are smaller for reaction with the OH radical, which reacts with pyrene on both the surface of particles and in the gas phase. Global and regional chemical transport models typically approximate gas–particle partitioning with instantaneous-equilibration approaches. We highlight scenarios in which these approximations deviate from the explicitly coupled treatment of gas–particle partitioning and chemistry presented in this study. We find that the discrepancy between solutions depends on the operator-splitting time step and the choice of time step can help to minimize the discrepancy. The findings and techniques presented in this work not only are relevant for PAHs but can also be applied to other semi-volatile substances that undergo chemical reactions and mass transport between the gas and particle phase. 

Thirdhand smoke (THS) persists in locations where smoking previously occurred and can be transported into non-smoking environments, leading to non-smoker exposure. Laboratory experiments using high-resolution mass spectrometry demonstrate that deposited particulate matter (PM) and smoke-exposed surrogate lung lining fluid (LLF) are substantial, chemically-complex reservoirs of gas-phase THS emissions, including hazardous air pollutants, polycyclic aromatic compounds, and nitrogen/oxygen-containing species. Both PM and LLF are persistent real-world THS reservoirs that chemically evolve over time, and can act as vehicles for the transport and emission of reactive pollutants and their reaction byproducts (e.g., acrolein). Deposited PM on clothes, furnishings, bodies, and/or airways will emit volatile to semi-volatile gases over long lifetimes, which can re-partition to other indoor materials and increase their overall persistence. On the other hand, LLF off-gassing consists predominantly of volatile organic compounds in amounts influenced by their aqueous solubilities, and their persistence in breath will be prolonged by re-distribution across internal aqueous reservoirs, as corroborated by multicompartment modeling in this study. 

Abstract. In the aqueous phase, fine particulate matter can form reactive species (RS)that influence the aging, properties, and health effects of atmosphericaerosols. In this study, we explore the RS yields of aerosol samples froma remote forest (Hyytiälä, Finland) and polluted urban locations(Mainz, Germany; Beijing, China), and we relate the RS yields to differentchemical constituents and reaction mechanisms. Ultra-high-resolution massspectrometry was used to characterize organic aerosol composition, electronparamagnetic resonance (EPR) spectroscopy with a spin-trapping technique wasapplied to determine the concentrations of ⚫OH,O2⚫-, and carbon- or oxygen-centered organic radicals, anda fluorometric assay was used to quantify H2O2. The aqueousH2O2-forming potential per mass unit of ambient PM2.5(particle diameter < 2.5 µm) was roughly the same for allinvestigated samples, whereas the mass-specific yields of radicals werelower for sampling sites with higher concentrations of PM2.5. Theabundances of water-soluble transition metals and aromatics in ambientPM2.5 were positively correlated with the relative fraction of⚫OH and negatively correlated with the relative fraction ofcarbon-centered radicals. In contrast, highly oxygenated organic molecules(HOM) were positively correlated with the relative fraction ofcarbon-centered radicals and negatively correlated with the relativefraction of ⚫OH. Moreover, we found that the relative fractionsof different types of radicals formed by ambient PM2.5 were comparableto surrogate mixtures comprising transition metal ions, organichydroperoxide, H2O2, and humic or fulvic acids. The interplay oftransition metal ions (e.g., iron and copper ions), highly oxidized organicmolecules (e.g., hydroperoxides), and complexing or scavenging agents (e.g.,humic or fulvic acids) leads to nonlinear concentration dependencies inaqueous-phase RS production. A strong dependence on chemical compositionwas also observed for the aqueous-phase radical yields oflaboratory-generated secondary organic aerosols (SOA) from precursormixtures of naphthalene and β-pinene. Our findings show how thecomposition of PM2.5 can influence the amount and nature ofaqueous-phase RS, which may explain differences in the chemical reactivityand health effects of particulate matter in clean and polluted air.