Plastic pollution is one of the most pressing environmental and social issues of the 21st century. Recent work has highlighted the atmosphere’s role in transporting microplastics to remote locations [S. Allen et al., Nat. Geosci. 12, 339 (2019) and J. Brahney, M. Hallerud, E. Heim, M. Hahnenberger, S. Sukumaran, Science 368, 1257–1260 (2020)]. Here, we use in situ observations of microplastic deposition combined with an atmospheric transport model and optimal estimation techniques to test hypotheses of the most likely sources of atmospheric plastic. Results suggest that atmospheric microplastics in the western United States are primarily derived from secondary re-emission sources including roads (84%), the ocean (11%), and agricultural soil dust (5%). Using our best estimate of plastic sources and modeled transport pathways, most continents were net importers of plastics from the marine environment, underscoring the cumulative role of legacy pollution in the atmospheric burden of plastic. This effort uses high-resolution spatial and temporal deposition data along with several hypothesized emission sources to constrain atmospheric plastic. Akin to global biogeochemical cycles, plastics now spiral around the globe with distinct atmospheric, oceanic, cryospheric, and terrestrial residence times. Though advancements have been made in the manufacture of biodegradable polymers, our data suggest that extant nonbiodegradable polymers will continue to cycle through the earth’s systems. Due to limited observations and understanding of the source processes, there remain large uncertainties in the transport, deposition, and source attribution of microplastics. Thus, we prioritize future research directions for understanding the plastic cycle. Significance Microplastic particles and fibers generated from the breakdown of mismanaged waste are now so prevalent that they cycle through the earth in a manner akin to global biogeochemical cycles. In modeling the atmospheric limb of the plastic cycle, we show that most atmospheric plastics are derived from the legacy production of plastics from waste that has continued to build up in the environment. Roads dominated the sources of microplastics to the western United States, followed by marine, agriculture, and dust emissions generated downwind of population centers. At the current rate of increase of plastic production (∼4% per year), understanding the sources and consequences of microplastics in the atmosphere should be a priority.

Atmospheric ice‐nucleating particles (INPs) play a critical role in cloud freezing processes, with important implications for precipitation formation and cloud radiative properties, and thus for weather and climate. Additionally, INP emissions respond to changes in the Earth System and climate, for example, desertification, agricultural practices, and fires, and therefore may introduce climate feedbacks that are still poorly understood. As knowledge of the nature and origins of INPs has advanced, regional and global weather, climate, and Earth system models have increasingly begun to link cloud ice processes to model‐simulated aerosol abundance and types. While these recent advances are exciting, coupling cloud processes to simulated aerosol also makes cloud physics simulations increasingly susceptible to uncertainties in simulation of INPs, which are still poorly constrained by observations. Advancing the predictability of INP abundance with reasonable spatiotemporal resolution will require an increased focus on research that bridges the measurement and modeling communities. This review summarizes the current state of knowledge and identifies critical knowledge gaps from both observational and modeling perspectives. In particular, we emphasize needs in two key areas: (a) observational closure between aerosol and INP quantities and (b) skillful simulation of INPs within existing weather and climate models. We discuss the state of knowledge on various INP particle types and briefly discuss the challenges faced in understanding the cloud impacts of INPs with present‐day models. Finally, we identify priority research directions for both observations and models to improve understanding of INPs and their interactions with the Earth System.

Emission rates and properties of ice nucleating particles (INPs) are required for proper representation of aerosol–cloud interactions in atmospheric models. Few investigations have quantified marine INP emissions, a potentially important INP source for remote oceanic regions. Previous studies have suggested INPs in sea spray aerosol (SSA) are linked to oceanic biological activity. This proposed link was explored in this study by measuring INP emissions from nascent SSA during phytoplankton blooms during two mesocosm experiments. In a Marine Aerosol Reference Tank (MART) experiment, a phytoplankton bloom was produced with chlorophyll-a (Chl a) concentrations reaching 39 μg L−1, while Chl a concentrations more representative of natural ocean conditions were obtained during the Investigation into Marine Particle Chemistry and Transfer Science (IMPACTS; peak Chl a of 5 μg L−1) campaign, conducted in the University of California, San Diego, wave flume. Dynamic trends in INP emissions occurred for INPs active at temperatures > −30°C. Increases in INPs active between −25° and −15°C lagged the peak in Chl a in both studies, suggesting a consistent population of INPs associated with the collapse of phytoplankton blooms. Trends in INP emissions were also compared to aerosol composition, abundances of microbes, and enzyme activity. In general, increases in INP concentrations corresponded to increases in organic species in SSA and the emissions of heterotrophic bacteria, suggesting that both microbes and biomolecules contribute to marine INP populations. INP trends were not directly correlated with a single biological marker in either study. Direct measurements of INP chemistry are needed to accurately identify particles types contributing to marine INP populations.

Ice-nucleating particles (INPs) are rare atmospheric aerosols that initiate primary ice formation, but accurately simulating their concentrations and variability in large-scale climate models remains a challenge. Doing so requires both simulating major particle sources and parameterizing their ice nucleation (IN) efficiency. Validating and improving model predictions of INP concentrations requires measuring their concentrations delineated by particle type. We present a method to speciate INP concentrations into contributions from dust, sea spray aerosol (SSA), and bioaerosol. Field campaign data from Bodega Bay, California, showed that bioaerosols were the primary source of INPs between −12° and −20°C, while dust was a minor source and SSA had little impact. We found that recent parameterizations for dust and SSA accurately predicted ambient INP concentrations. However, the model did not skillfully simulate bioaerosol INPs, suggesting a need for further research to identify major factors controlling their emissions and INP efficiency for improved representation in models.

The formation of ice in clouds can strongly impact cloud properties and precipitation processes during storms, including atmospheric rivers. Sea spray aerosol (SSA) particles are relatively inefficient as ice nucleating particles (INPs) compared to mineral dust. However, due to the vast coverage of the Earth's surface by the oceans, a number of recent studies have focused on identifying sources of marine INPs, particularly in regions lacking a strong influence from dust. This study describes the integration, validation, and application of a system coupling a continuous flow diffusion chamber with a single particle mass spectrometer using a pumped counterflow virtual impactor to remove nonnucleated particles and selectively measure the composition of INPs with a detection efficiency of 3.10 × 10⁻⁴. In situ measurements of immersion freezing INP composition were made at a coastal site in California using the integrated system. Mineral dust particles were the most abundant ice crystal residual type during the sampling period and found to be ice active despite having undergone atmospheric processing. SSA were more abundant in ambient measurements but represented only a minor fraction of the ice crystal residual population at −31 °C. Notably, the SSA particles that activated were enriched with organic nitrogen species that were likely transferred from the ocean. Calculations of ice nucleation active site densities were within good agreement with previous studies of mineral dust and SSA.

A major component of California's yearly precipitation comes from wintertime atmospheric river events which bring large amounts of moisture from the tropics up to the midlatitudes. Understanding these systems, specifically the effects of aerosol particles on precipitation associated with these storms, was a major focus of the 2015 Atmospheric Radiation Measurement Cloud Aerosol Precipitation Experiment, which was part of the wintertime California Water 2015 campaign. The measurement campaign provided sampling platforms on four aircraft, including the Atmospheric Radiation Measurement Aerial Facility G‐1, as well as the National Oceanic and Atmospheric Administration Ronald H. Brown research vessel and at a ground station in Bodega Bay, CA. Measurements of ice nucleating particles (INPs) were made with the Colorado State University Continuous Flow Diffusion Chamber aboard the G‐1, and aerosol filters were collected on the G‐1, at the Bodega Bay site and on the Ronald H. Brown for postprocessing via immersion freezing in the Colorado State University Ice Spectrometer. Aerosol composition was measured aboard the G‐1 with the Aerosol Time‐of‐Flight Mass Spectrometer. Here we present INP concentrations and aerosol chemical compositions during the course of the aircraft campaign. During the atmospheric river event, we found that marine aerosol was the main aerosol type and that marine INPs were dominant at cloud activation temperatures, which is in stark contrast to the dominance of dust INPs during the atmospheric river events in the California Water 2011 campaign.