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Process-oriented observational constraints for the anthropogenic effective radiative forcing due to aerosol–cloud interactions (ERFaci) are highly desirable because the uncertainty associated with ERFaci poses a significant challenge to climate prediction. The contoured frequency by optical depth diagram (CFODD) analysis supports the evaluation of model representation of cloud liquid-to-rain conversion processes because the slope of a CFODD, generated from joint MODerate Resolution Imaging Spectroradiometer (MODIS)-CloudSat cloud retrievals, provides an estimate of cloud droplet collection efficiency in single-layer warm liquid clouds. Here, we present an updated CFODD analysis as an observational constraint on the ERFaci due to warm rain processes and apply it to the U.S. Department of Energy's Energy Exascale Earth System Model version 2 (E3SMv2). A series of sensitivity experiments shows that E3SMv2 droplet collection efficiencies and ERFaci are highly sensitive to autoconversion, i.e., the rate of mass transfer from cloud liquid to rain, yielding a strong correlation between the CFODD slope and the shortwave component of ERFaci (ERFaciSW; Pearson's R=-0.91). E3SMv2's CFODD slope (0.20 ± 0.04) is in agreement with observations (0.20 ± 0.03). The strong sensitivity of ERFaciSW to the CFODD slope provides a useful constraint on highly uncertain warm rain processes, whereby ERFaciSW, constrained by MODIS-CloudSat, is estimated by calculating the intercept of the linear association between the ERFaciSW and the CFODD slopes, using the MODIS-CloudSat CFODD slope as a reference.

Mineral dust and sea spray aerosol represent important sources of ice-nucleating particles (INPs), the minor fraction of aerosol particles able to trigger cloud ice crystal formation and, consequently, influence multiple climate-relevant cloud properties including lifetime, radiative properties and precipitation initiation efficiency. Mineral dust is considered the dominant INP source in many parts of the world due to its ice nucleation efficiency and its sheer abundance, with global emission rates of up to 4700 Tg a−1. However, INPs emitted from the ocean surface in sea spray aerosol frequently dominate INP populations in remote marine environments, including parts of the Southern Ocean where cloud-resolving model simulations have demonstrated that cloud radiative properties are likely strongly controlled by INPs. Here we report INP concentrations measured in aerosol and seawater samples during Air Quality and Climate Change in the Arabian Basin (AQABA), a shipborne campaign that spanned the Red Sea, Gulf of Aden, Arabian Sea, Arabian Gulf and part of the Mediterranean. In aerosol samples collected within a few hundred kilometers of the first and second ranked sources of dust globally, the Sahara and Arabian Peninsula, INP concentrations ranged from 0.2 to 11 L−1 at −20 ∘C with observed ice-active surface site densities (ns) 1–3 orders of magnitude below levels predicted by mineral dust INP parameterizations. Over half of the samples (at least 14 of 26) were collected during dust storms with average dust mass concentrations between 150 and 490 µg m−3 (PM10), as simulated by the Modern-Era Retrospective analysis for Research and Application, version 2 (MERRA-2). The impacts of heat and peroxide treatments indicate that organics dominated the observed ice nucleation (IN) activity at temperatures ≥ −15 ∘C with proteinaceous (heat-labile) INPs frequently observed at high freezing temperatures >−10 ∘C. INP concentrations in seawater samples ranged between 3 and 46 mL−1 at −19 ∘C, demonstrating the relatively low INP source potential of seawater in the region as compared to seawater from multiple other regions reported previously. Overall, our results demonstrate that despite proximity to the Sahara and the Arabian Peninsula and the dominance of mineral dust in the aerosol sampled, existing mineral dust parameterizations alone would not skillfully represent the near-surface ns in the observed temperature regime (−6 to −25 ∘C). Future efforts to develop or improve representations of dust INPs at modest supercooling (≥-15 ∘C) would benefit from a characterization of the specific organic species associated with dust INPs. More generally, an improved understanding of the organic species associated with increased IN activity and their variability across dust source regions would directly inform efforts to determine whether ns-based parameterizations are appropriate for faithful representation of dust INPs in this sensitive temperature regime, whether region-specific parameterizations are required, or whether an alternative to the ns approach is necessary.

Ice-nucleating particles (INPs) represent a rare subset of aerosol particles that initiate cloud droplet freezing at temperatures above the homogenous freezing point of water (−38 ∘C). Considering that the ocean covers 71 % of the Earth's surface and represents a large potential source of INPs, it is imperative that the identities, properties and relative emissions of ocean INPs become better understood. However, the specific underlying drivers of marine INP emissions remain largely unknown due to limited observations and the challenges associated with isolating rare INPs. By generating isolated nascent sea spray aerosol (SSA) over a range of biological conditions, mesocosm studies have shown that marine microbes can contribute to INPs. Here, we identify 14 (30 %) cultivable halotolerant ice-nucleating microbes and fungi among 47 total isolates recovered from precipitation and aerosol samples collected in coastal air in southern California. Ice-nucleating (IN) isolates collected in coastal air were nucleated ice from extremely warm to moderate freezing temperatures (−2.3 to −18 ∘C). While some Gammaproteobacteria and fungi are known to nucleate ice at temperatures as high as −2 ∘C, Brevibacterium sp. is the first Actinobacteria found to be capable of ice nucleation at a relatively high freezing temperature (−2.3 ∘C). Air mass trajectory analysis demonstrates that marine aerosol sources were dominant during all sampling periods, and phylogenetic analysis indicates that at least 2 of the 14 IN isolates are closely related to marine taxa. Moreover, results from cell-washing experiments demonstrate that most IN isolates maintained freezing activity in the absence of nutrients and cell growth media. This study supports previous studies that implicated microbes as a potential source of marine INPs, and it additionally demonstrates links between precipitation, marine aerosol and IN microbes.

Ice-nucleating particles (INPs) are efficiently removed from clouds through precipitation, a convenience of nature for the study of these very rare particles that influence multiple climate-relevant cloud properties including ice crystal concentrations, size distributions and phase-partitioning processes. INPs suspended in precipitation can be used to estimate in-cloud INP concentrations and to infer their original composition. Offline droplet assays are commonly used to measure INP concentrations in precipitation samples. Heat and filtration treatments are also used to probe INP composition and size ranges. Many previous studies report storing samples prior to INP analyses, but little is known about the effects of storage on INP concentration or their sensitivity to treatments. Here, through a study of 15 precipitation samples collected at a coastal location in La Jolla, CA, USA, we found INP concentration changes up to > 1 order of magnitude caused by storage to concentrations of INPs with warm to moderate freezing temperatures (−7 to −19 ∘C). We compared four conditions: (1) storage at room temperature (+21–23 ∘C), (2) storage at +4 ∘C, (3) storage at −20 ∘C and (4) flash-freezing samples with liquid nitrogen prior to storage at −20 ∘C. Results demonstrate that storage can lead to both enhancements and losses of greater than 1 order of magnitude, with non-heat-labile INPs being generally less sensitive to storage regime, but significant losses of INPs smaller than 0.45 µm in all tested storage protocols. Correlations between total storage time (1–166 d) and changes in INP concentrations were weak across sampling protocols, with the exception of INPs with freezing temperatures ≥ −9 ∘C in samples stored at room temperature. We provide the following recommendations for preservation of precipitation samples from coastal or marine environments intended for INP analysis: that samples be stored at −20 ∘C to minimize storage artifacts, that changes due to storage are likely an additional uncertainty in INP concentrations, and that filtration treatments be applied only to fresh samples. At the freezing temperature −11 ∘C, average INP concentration losses of 51 %, 74 %, 16 % and 41 % were observed for untreated samples stored using the room temperature, +4, −20 ∘C, and flash-frozen protocols, respectively. Finally, the estimated uncertainties associated with the four storage protocols are provided for untreated, heat-treated and filtered samples for INPs between −9 and −17 ∘C.

Ice-nucleating particles (INPs) have been found to influence the amount, phase and efficiency of precipitation from winter storms, including atmospheric rivers. Warm INPs, those that initiate freezing at temperatures warmer than −10 ∘C, are thought to be particularly impactful because they can create primary ice in mixed-phase clouds, enhancing precipitation efficiency. The dominant sources of warm INPs during atmospheric rivers, the role of meteorology in modulating transport and injection of warm INPs into atmospheric river clouds, and the impact of warm INPs on mixed-phase cloud properties are not well-understood. In this case study, time-resolved precipitation samples were collected during an atmospheric river in northern California, USA, during winter 2016. Precipitation samples were collected at two sites, one coastal and one inland, which are separated by about 35 km. The sites are sufficiently close that air mass sources during this storm were almost identical, but the inland site was exposed to terrestrial sources of warm INPs while the coastal site was not. Warm INPs were more numerous in precipitation at the inland site by an order of magnitude. Using FLEXPART (FLEXible PARTicle dispersion model) dispersion modeling and radar-derived cloud vertical structure, we detected influence from terrestrial INP sources at the inland site but did not find clear evidence of marine warm INPs at either site. We episodically detected warm INPs from long-range-transported sources at both sites. By extending the FLEXPART modeling using a meteorological reanalysis, we demonstrate that long-range-transported warm INPs were observed only when the upper tropospheric jet provided transport to cloud tops. Using radar-derived hydrometeor classifications, we demonstrate that hydrometeors over the terrestrially influenced inland site were more likely to be in the ice phase for cloud temperatures between 0 and −10 ∘C. We thus conclude that terrestrial and long-range-transported aerosol were important sources of warm INPs during this atmospheric river. Meteorological details such as transport mechanism and cloud structure were important in determining (i) warm INP source and injection temperature and (ii) ultimately the impact of warm INPs on mixed-phase cloud properties.

Ice nucleating particles (INPs) influence cloud properties and can affect the overall precipitation efficiency. Developing a parameterization of INPs in global climate models has proven challenging. More INP measurements – including studies of their spatial distribution, sources and sinks, and fundamental freezing mechanisms – must be conducted in order to further improve INP parameterizations. In this paper, an immersion mode INP measurement technique is modified and automated using a software-controlled, real-time image stream designed to leverage optical changes of water droplets to detect freezing events. For the first time, heat transfer properties of the INP measurement technique are characterized using a finite-element-analysis-based heat transfer simulation to improve accuracy of INP freezing temperature measurement. The heat transfer simulation is proposed as a tool that could be used to explain the sources of bias in temperature measurements in INP measurement techniques and ultimately explain the observed discrepancies in measured INP freezing temperatures between different instruments. The simulation results show that a difference of +8.4 °C between the well base temperature and the headspace gas results in an up to 0.6 °C stratification of the aliquot, whereas a difference of +4.2 °C or less results in a thermally homogenous water volume within the error of the thermal probe, ±0.2 °C. The results also show that there is a strong temperature gradient in the immediate vicinity of the aliquot, such that without careful placement of temperature probes, or characterization of heat transfer properties of the water and cooling environment, INP measurements can be biased toward colder temperatures. Based on a modified immersion mode technique, the Automated Ice Spectrometer (AIS), measurements of the standard test dust illite NX are reported and compared against six other immersion mode droplet assay techniques featured in Hiranuma et al. (2015) that used wet suspensions. AIS measurements of illite NX INP freezing temperatures compare reasonably with others, falling within the 5 °C spread in reported spectra. The AIS as well as its characterization of heat transfer properties allows higher confidence in accuracy of freezing temperature measurement, allows higher throughput of sample analysis, and enables disentanglement of the effects of heat transfer rates on sample volumes from time dependence of ice nucleation.