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At least 163 records · Page 9

Global Importance of Secondary Ice Production

Measured ice crystal number concentrations are often orders of magnitude higher than the number concentrations of ice nucleating particles, indicating the existence of secondary ice production (SIP) in clouds. Here, we present the first study to examine the global importance of SIP through the droplet shattering during freezing of rain, ice-ice collision fragmentation, and rime splintering, using a global climate model. Our results show that SIP happens quite uniformly in the two hemispheres and dominates the ice formation in the moderately cold clouds with temperatures warmer than –15°C. SIP decreases the global annual average liquid water path by –14.6 g m –2 (–22%), increases the ice water path by 8.7 g m –2 (23%), improving the model agreement with observations. SIP changes the global annual average shortwave, longwave, and net cloud forcing by 2.1, –1.0, and 1.1 W m –2 , respectively, highlighting the importance of SIP on cloud properties on the global scale.

54 ENVIRONMENTAL SCIENCES↗

Cold-Air Outbreaks in the Marine Boundary Layer Experiment (COMBLE) Field Campaign Report

The Cold-Air Outbreaks in the Marine Boundary Layer Experiment (COMBLE) was conducted successfully between 1 December 2019 and 31 May 2020 around the Norwegian Sea. COMBLE deployed the U.S. Department of Energy Atmospheric Radiation Measurement (ARM) first Mobile Facility (AMF1) along the coast of northern Scandinavia, at an arctic latitude (70°N), and an array of additional instruments on Bear Island (75°N) in the Norwegian Sea. The instruments deployed at these two sites collected a large array of in situ and remote-sensing observations of atmospheric conditions, clouds, precipitation, and aerosol. The main objective of COMBLE is to quantify the properties of shallow convective clouds that develop as part of an air-mass transformation process when cold air blows over open water. The two COMBLE sites are located at ~1,200 km and ~500 km from the cold source, i.e., arctic ice edge, respectively.

54 ENVIRONMENTAL SCIENCES↗

AWARE: The Atmospheric Radiation Measurement (ARM) West Antarctic Radiation Experiment

The U.S. Department of Energy Atmospheric Radiation Measurement (ARM) West Antarctic Radiation Experiment (AWARE) performed comprehensive meteorological and aerosol measurements and ground-based atmospheric remote sensing at two Antarctic stations using the most advanced instrumentation available. A suite of cloud research radars, lidars, spectral and broadband radiometers, aerosol chemical and microphysical sampling equipment, and meteorological instrumentation was deployed at McMurdo Station on Ross Island from December 2015 through December 2016. A smaller suite of radiometers and meteorological equipment, including radiosondes optimized for surface energy budget measurement, was deployed on the West Antarctic Ice Sheet between 4 December 2015 and 17 January 2016. AWARE provided Antarctic atmospheric data comparable to several well-instrumented high Arctic sites that have operated for many years and that reveal numerous contrasts with the Arctic in aerosol and cloud microphysical properties. These include persistent differences in liquid cloud occurrence, cloud height, and cloud thickness. Antarctic aerosol properties are also quite different from the Arctic in both seasonal cycle and composition, due to the continent’s isolation from lower latitudes by Southern Ocean storm tracks. Antarctic aerosol number and mass concentrations are not only non-negligible but perhaps play a more important role than previously recognized because of the higher sensitivities of clouds at the very low concentrations caused by the large-scale dynamical isolation. Antarctic aerosol chemical composition, particularly organic components, has implications for local cloud microphysics. The AWARE dataset, fully available online in the ARM Program data archive, offers numerous case studies for unique and rigorous evaluation of mixed-phase cloud parameterization in climate models.

54 ENVIRONMENTAL SCIENCES↗

Examining the Ice-Nucleating Particles from the North Slope of Alaska (ExINP-NSA) (Final Campaign Report)

The Examining the Ice-Nucleating Particles from the North Slope of Alaska (ExINP-NSA) campaign was conducted at the National Oceanic and Atmospheric Administration’s (NOAA) Barrow Atmospheric Baseline Observatory (71.3230° N, 156.6114° W, “BRW” hereafter), next to the Atmospheric Radiation Measurement (ARM) user facility NSA site and ~ 6 km northeast of the town of Utqiaġvik. The location of the NSA site is shown in Figure 1. Our observing period began in October 2021 and continued until May 2024. This campaign was funded by the U.S. Department of Energy (DOE) Office of Science Early Career Research Program through grant number DE-SC001879. This grant contains funding for three ARM field campaigns. The previous field campaigns were performed at ARM’s Southern Great Plains atmospheric observatory in Oklahoma (SGP; 36.6073° N, 97.4876° W) and the ARM’s Eastern North Atlantic atmospheric observatory on Graciosa Island, Azores (ENA; 39.0916° N, 28.0257° W). The ExINP-NSA campaign aims included: • Determining the number concentration of ice-nucleating particles (n INPs ) active at temperatures spanning the range of heterogeneous freezing processes (from ≈−30 °C to 0 °C) using a combination of online and offline measurements, • Determining whether local meteorological conditions and/or synoptic scale air mass transport impact INP abundance and/or ice nucleation efficiency, • Examining if the physicochemical properties of INPs relate to aerosol chemistry, and • Assessing if there is a similarity in INP properties across three ARM sites Multi-seasonal datasets of INP abundance in the NSA region were delivered from this campaign. This campaign also allowed researchers to perform a comprehensive analysis of atmospheric INPs based on long- term ground-based measurements in the Alaskan Arctic. Our data and results from the ExINP-NSA campaign will help refine current earth system models. One of the stated goals of ARM is to advance aerosol-cloud ice interaction, which will be a direct result of this campaign. Current earth system models poorly represent INPs, and the 15-minute time resolution data over several seasons generated during this campaign will provide an invaluable resource, especially combined with the datasets generated during two previous ARM ExINP campaigns. These datasets will allow for a greater understanding of ice nucleation processes as they may (or may not) relate to local meteorological processes and aerosol chemistry and will eventually help further the understanding of the Earth’s atmospheric processes and energy balance.

54 ENVIRONMENTAL SCIENCES↗

A Triple-Moment Representation of Ice in the Predicted Particle Properties (P3) Microphysics Scheme

In the original Predicted Particle Properties (P3) bulk microphysics scheme, all ice-phase hydrometeors are represented by one or more “free” ice categories, where the physical properties evolve smoothly through changes to the four prognostic variables (per category), and with a two-moment representation of the particle size distribution. As such, the spectral dispersion cannot evolve independently, which thus results in limitations in representation of ice—in particular, hail—due to necessary constraints in the scheme to prevent excessive gravitational size sorting. To overcome this, P3 has been modified to include a three-moment representation of the size distribution of each ice category through the addition of a fifth prognostic variable, the sixth moment of the size distribution. The details of the three-moment ice parameterization in P3 are provided. The behavior of the modified scheme, with the single-ice-category configuration, is illustrated through simulations in a simple 1D kinematic model framework as well as with near large-eddy-resolving (250-m grid spacing) 3D simulations of a hail-producing supercell. It is shown that the three-moment ice configuration controls size sorting in a physically based way and leads to an improved capacity to simulate large, heavily rimed ice (hail), including mean and maximum sizes and reflectivity, and thus an overall improvement in the representation of ice-phase particles in the P3 scheme.

54 ENVIRONMENTAL SCIENCES↗

Sensitivity of Cloud-Radiative Effects to Cloud Fraction Parametrizations in Tropical, Mid-Latitude and Arctic Kilometre-Scale Simulations

The Regional Atmosphere (RA) configuration of the Met Office Unified Model currently requires different cloud fraction parametrizations (CFP) for tropical and midlatitude simulations. To explore the scope for unification of these two RA configurations, this paper presents a detailed evaluation of simulations over tropical, midlatitude and arctic domains, with two different diagnostic CFPs, a prognostic CFP, and no CFP at all. Furthermore, a novel, hybrid approach was used that treats liquid cloud diagnostically and ice cloud prognostically. Using observations from three U.S. Department of Energy Atmospheric Radiation Measurement supersites, it is shown that none of these CFPs stands out as superior over all domains. Over the frequently overcast Arctic, the all-or-nothing approach best captures the cloud radiative properties. Conversely, CFPs are of benefit in regions with frequent partial cloudiness, such as the midlatitudes and the tropics. However, their improved cloud radiative properties often hide an error compensation. All models underestimate overcast, low-base cloud with small water paths in convective environments. In addition, mid-latitude overcast, low-base, optically thick clouds in the morning, possibly associated with overnight convection, are frequently too broken. Diagnostic schemes compensate for these errors by producing spurious, scattered afternoon cloud, which could be due to a correct cloud response to too eager convective initiation. Winter clouds over the midlatitudes are improved when liquid cloud is represented diagnostically with a bimodal saturation-departure PDF, without error compensation. While it is difficult to unify the RA across the globe around a single CFP scheme, the newly proposed Hybrid scheme performs reasonably well for cloud cover across all regions. It also exhibits SW biases that are smaller than most other configurations and is less affected by excessive liquid water paths and compensating errors than fully diagnostic schemes. Surface precipitation is fairly insensitive to the CFP in the simulations shown here.

54 ENVIRONMENTAL SCIENCES↗

Highly supercooled riming and unusual triple-frequency radar signatures over McMurdo Station, Antarctica

Abstract. Riming of ice crystals by supercooled water droplets is an efficient ice growth process, but its basic properties are still poorly known. While it has been shown to contribute significantly to surface precipitation at mid-latitudes, little is known about its occurrence at high latitudes. In Antarctica, two competing effects can influence the occurrence of riming: (i) the scarcity of supercooled liquid water clouds due to the extremely low tropospheric temperatures and (ii) the low aerosol concentration, which may lead to the formation of fewer and larger supercooled drops potentially resulting in an enhanced riming efficiency. In this work, by exploiting the deployment of an unprecedented number of multiwavelength remote sensing systems (including triple-frequency radar measurements) in West Antarctica, during the Atmospheric Radiation Measurements West Antarctic Radiation Experiment (AWARE) field campaign, we evaluate the riming incidence at McMurdo Station and find that riming occurs at much lower temperatures when compared to previous results in the mid-latitudes. This suggests the possible occurrence of a common atmospheric state over Antarctica that includes a rather stable atmosphere inhibiting turbulent mixing, and a high riming efficiency driven by large cloud droplets. We then focus on a peculiar case study featuring a persistent layer with a particularly pronounced riming signature in triple-frequency radar data but only a relatively modest amount of supercooled liquid water. In-depth analysis of the radar observations suggests that such signatures can only be explained by the combined effects of moderately rimed aggregates or similarly shaped florid polycrystals and a narrow particle size distribution (PSD). Simulations of this case study performed with a one-dimensional bin model indicate that similar triple-frequency radar observations can be reproduced when narrow PSDs are simulated. Such narrow PSDs can in turn be explained by two key factors: (i) the presence of a shallow homogeneous droplet or humidified aerosol freezing layer aloft seeding an underlying supercooled liquid layer, and (ii) the absence of turbulent mixing throughout a stable polar atmosphere that sustains narrow PSDs, as hydrometeors grow from the nucleation region aloft to ice particles of several millimeters in size, by vapor deposition and then riming.

54 ENVIRONMENTAL SCIENCES↗

The Role of In-Cloud Wet Removal in Simulating Aerosol Vertical Profiles and Cloud Radiative Forcing

Among the physical processes controlling aerosol vertical profiles, in-cloud wet removal is of utmost importance while its representation in global climate models (GCMs) is crude. In this study, we implement into the Community Atmosphere Model version 6 (CAM6) a physically based aerosol wet removal parameterization scheme that explicitly treats aerosol activation, removal and resuspension. Evaluation against in-situ observations shows that the default scheme substantially overestimates the upper tropospheric black carbon (BC) and sea salt mass. Our physically based scheme reduces BC and sea salt mass by a factor of 10 and 1,000, respectively, in better agreement with observations. Also, the new scheme slightly increases number of aerosol particles between 12 nm and 4.8 μm in diameter, thereby mitigating the aerosol number underestimation in the default scheme. Our new scheme reduces the overestimation of coarse-mode aerosol (0.5–4.8 μm) number. Overall, the aerosol property changes (mass decrease and number increase) reduce the cloud condensation nuclei (CCN) concentration at low supersaturation (i.e., 0.02% and 0.1%), and increase CCN at high supersaturations (i.e., 0.5% and 1%). Consequently, the global annual mean cloud liquid water path increases by 1.89 g m -2 and the ice water path increases by 0.51 g m -2 . The global annual mean shortwave, longwave, and net cloud radiative forcing change by -1.06, 0.57, and -0.48 W m -2 , respectively. Further improvement is needed to reflect the real physics that the removal efficiencies for aerosol mass and number are disproportionate and to advect cloud-borne (activated) aerosols for a complete aerosol lifecycle.

54 ENVIRONMENTAL SCIENCES↗

Using Machine Learning to Generate a GISS ModelE Calibrated Physics Ensemble (CPE)

A neural network (NN) surrogate of the NASA GISS ModelE atmosphere (version E3) is trained on a perturbed parameter ensemble (PPE) spanning 45 physics parameters and 36 outputs. The NN is leveraged in a Markov Chain Monte Carlo (MCMC) Bayesian parameter inference framework to generate a second posterior constrained ensemble coined a “calibrated physics ensemble,” or CPE. The CPE members are characterized by diverse parameter combinations and are, by definition, close to top-of-atmosphere radiative balance, and must broadly agree with numerous hydrologic, energy cycle and radiative forcing metrics simultaneously. Global observations of numerous cloud, environment, and radiation properties (provided by global satellite products) are crucial for CPE generation. The inference framework explicitly accounts for discrepancies (or biases) in satellite products during CPE generation. We demonstrate that product discrepancies strongly impact calibration of important model parameter settings (e.g., convective plume entrainment rates; fall speed for cloud ice). Structural improvements new to E3 are retained across CPE members (e.g., stratocumulus simulation). Notably, the framework improved the simulation of shallow cumulus and Amazon rainfall while not degrading radiation fields, an upgrade that neither default parameters nor Latin Hypercube parameter searching achieved. Analyses of the initial PPE suggested several parameters were unimportant for output variation. However, many “unimportant” parameters were needed for CPE generation, a result that brings to the forefront how parameter importance should be determined in PPEs. From the CPE, two diverse 45-dimensional parameter configurations are retained to generate radiatively-balanced, auto-tuned atmospheres that were used in two E3 submissions to CMIP6.

54 ENVIRONMENTAL SCIENCES↗

Freezing Processes in Southern Ocean Mixed Phase Clouds (Final Technical Report)

Southern Ocean (SO) low-level clouds remain a challenge for Earth system models to represent accurately. This project utilized DOE ARM observations and the Community Atmosphere Model (CAM) to improve process-level understanding of aerosol-cloud interactions and cloud microphysics for SO mixed-phase clouds. Specifically, our efforts include two main topics: 1) investigate the SO aerosol, cloud condensation nuclei (CCN), and ice nucleating particle (INP) population based on observations and determine predictive skill of simulating SO INPs, and 2) assess the ice formation pathways, including ice nucleation and secondary ice production, in SO mixed phase clouds utilizing a combination of observations and modeling tools. Studies focused on SO aerosol and INP resulted four manuscripts. Ice formation pathways in SO mixed phase clouds were investigated, revealing observed evidence of SIP active across all mixed phase temperatures. However, a key finding of this project is that despite significant progress in predicting SO INPs, the role of INP variability in SO cloud phase, precipitation, and radiative properties remain unknown due to challenges in microphysics parameterizations.

54 ENVIRONMENTAL SCIENCES↗

Model Intercomparison of the Impacts of Varying Cloud Droplet–Nucleating Aerosols on the Life Cycle and Microphysics of Isolated Deep Convection

The microphysical impacts of aerosol particles on scattered isolated deep convective cells near Houston, Texas, on 19 June 2013, are examined using multiple cloud-resolving model (CRM) simulations initialized with vertical profiles of low and high concentrations of cloud droplet–nucleating aerosols. These simulations formed part of the Model Intercomparison Project (MIP) conducted by the Deep Convective Working Group of the Aerosol, Cloud, Precipitation and Climate (ACPC) initiative. Each CRM generated a field of convective cells representing those observed during the case study with varying degrees of accuracy. The Tracking and Object-Based Analysis of Clouds (tobac) cell-tracking algorithm was applied to each MIP CRM simulation to track relatively long-lived convective cells (20–60 min). Most of the CRMs produced similar aerosol loading impacts on the warm phase of tracked cell properties with reduced autoconversion and accretion growth of rain, increased cloud water, reduced rainfall, and reduced near-surface evaporation of rain. The sign of aerosol impacts on the warm-phase properties of the convective cells was also quite consistent over cell lifetimes with the greatest magnitude of influence in the first half of the life cycle in most CRMs. In contrast, the ice-phase response to aerosol loading was highly variable among CRMs and included increases or decreases in ice amounts at inconsistent stages of the cell life cycle and midlevel versus upper-level changes in ice. This intermodel variability in ice is indicative both of the complex indirect interactions between aerosols and ice-phase processes in deep convection and their associated parameterizations.

Aerosol-cloud interaction↗

Impacts of Synoptic-Scale Dynamics on Clouds and Radiation in High Southern Latitudes

High-latitudinal mixed-phase clouds significantly affect Earth's radiative balance. Observations of cloud and radiative properties from two field campaigns in the Southern Ocean and Antarctica were compared with two global climate model simulations. A cyclone compositing method was used to quantify “dynamics-cloud-radiation” relationships relative to the extratropical cyclone centers. Observations show larger asymmetry in cloud and radiative properties between western and eastern sectors at McMurdo compared with Macquarie Island. Most observed quantities at McMurdo are higher in the western (i.e., post-frontal) than the eastern (frontal) sector, including cloud fraction, liquid water path (LWP), net surface shortwave and longwave radiation (SW and LW), except for ice water path (IWP) being higher in the eastern sector. Here, the two models were found to overestimate cloud fraction and LWP at Macquarie Island but underestimate them at McMurdo Station. IWP is consistently underestimated at both locations, both sectors, and in all seasons. Biases of cloud fraction, LWP, and IWP are negatively correlated with SW biases and positively correlated with LW biases. The persistent negative IWP biases may have become one of the leading causes of radiative biases over the high southern latitudes, after correcting the underestimation of supercooled liquid water in the older model versions. By examining multi-scale factors from cloud microphysics to synoptic dynamics, this work will help increase the fidelity of climate simulations in this remote region.

58 GEOSCIENCES↗

Insights on sources and formation mechanisms of liquid-bearing clouds over MOSAiC examined from a Lagrangian framework

Understanding Arctic stratiform liquid-bearing cloud life cycles and properly representing these life cycles in models is crucial for evaluations of cloud feedbacks as well as the faithfulness of climate projections for this rapidly warming region. Examination of cloud life cycles typically requires analyses of cloud evolution and origins on short time scales, on the order of hours to several days. Measurements from the recent Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) expedition provide a unique view of the current state of the central Arctic over an annual cycle. Here, we use the MOSAiC radiosonde measurements to detect liquid-bearing cloud layers over full atmospheric columns and to examine the cloud-generating air masses’ properties. We perform 5-day (120 h) back-trajectory calculations for every detected cloud and cluster them using a unique set of variables extracted from these trajectories informed by ERA5 reanalysis data. This clustering method enables us to separate between the air mass source regions such as ice-covered Arctic and midlatitude open water. We find that moisture intrusions into the central Arctic typically result in multilayer liquid-bearing cloud structures and that more than half of multilayer profiles include overlying liquid-bearing clouds originating in different types of air masses. Finally, we conclude that Arctic cloud formation via prolonged radiative cooling of elevated stable subsaturated air masses circulating over the Arctic can occur frequently (up to 20% of detected clouds in the sounding data set) and may lead to a significant impact of ensuing clouds on the surface energy budget, including net surface warming in some cases.

54 ENVIRONMENTAL SCIENCES↗

Bulk cloud microphysical properties as seen from numerical simulation and remote sensing products: case study of a hailstorm event over the La Plata Basin

Hailstorms develop over the La Plata Basin, in south-eastern South America, more often during later winter and early austral spring, between September and October. These systems have significant socioeconomic impacts over the region. Thus, a better understanding of how atmospheric drivers modulate the formation of hailstorms is important to improve the forecast of such phenomena. In this study, we selected a hailstorm event observed over the eastern La Plata Basin during 14–15 July 2016 to evaluate the performance of the Brazilian developments on the Regional Atmospheric Modelling System (BRAMS) model. The ability of the model in simulating cloud microphysical properties was evaluated by comparing simulations driven by different global forcings against in situ and remote sensing observations. The model results showed good skill in capturing the basic characteristics of the thunderstorm, particularly in terms of the spatial distribution of hydrometeors. The simulated spatial distribution of hail covers locations where hail fall was reported. The BRAMS simulations suggest that, despite relatively low values of the convective available potential energy (CAPE) (700–1000 J kg -1 ), environments with strong 0–8-km bulk shear (60–70 kt, ~30.9–36.0 m s –1 ) can promote the formation of ice clouds and hail fall over the eastern La Plata Basin. To be more conclusive, however, further research is needed to understand how different combinations of CAPE and shear affect hail formation over the region.

54 ENVIRONMENTAL SCIENCES↗

Tropical Cirrus in Global Storm-Resolving Models: 1. Role of Deep Convection

Pervasive cirrus clouds in the upper troposphere and tropical tropopause layer (TTL) influence the climate by altering the top-of-atmosphere radiation balance and stratospheric water vapor budget. These cirrus are often associated with deep convection, which global climate models must parameterize and struggle to accurately simulate. By comparing high-resolution global storm-resolving models from the Dynamics of the Atmospheric general circulation Modeled On Non-hydrostatic Domains (DYAMOND) intercomparison that explicitly simulate deep convection to satellite observations, we assess how well these models simulate deep convection, convectively generated cirrus, and deep convective injection of water into the TTL over representative tropical land and ocean regions. The DYAMOND models simulate deep convective precipitation, organization, and cloud structure fairly well over land and ocean regions, but with clear intermodel differences. All models produce frequent overshooting convection whose strongest updrafts humidify the TTL and are its main source of frozen water. Intermodel differences in cloud properties and convective injection exceed differences between land and ocean regions in each model. We argue that, with further improvements, global storm-resolving models can better represent tropical cirrus and deep convection in present and future climates than coarser-resolution climate models. To realize this potential, they must use available observations to perfect their ice microphysics and dynamical flow solvers.

54 ENVIRONMENTAL SCIENCES↗

Impact of Cloud Longwave Scattering on Radiative Fluxes Associated With the Madden-Julian Oscillation in the Indian Ocean and Maritime Continent

Previous studies suggested that cloud longwave radiation contributes to the development and maintenance of the Madden-Julian Oscillation (MJO) and model-based convection is highly sensitive to the radiation scheme. However, currently used radiation schemes do not take cloud longwave scattering into account, resulting in an overestimation of the outgoing longwave radiation (OLR) and an underestimation of the downward longwave flux at the surface. We use combined active and passive satellite cloud property retrievals to quantify the one-layer cloud OLR and heating rate (HR) biases introduced by neglecting cloud longwave scattering in the Indian Ocean and Maritime Continent in the context of MJO, with a focus on its phases 3, 5, and 6. Here, the results show that the satellite-detected one-layer cloud area consists primarily of ice clouds, particularly during the boreal winter in the 4-year study period. An increased ice cloud area fraction of one-layer cloud groups is present up to 5 days before the onset of MJO events. If longwave scattering is neglected, the composite mean OLR overestimation over the one-layer ice cloud area from 5 days before to 4 days after the MJO passage is approximately 3.5 to 5.0 W m –2 . Neglecting longwave scattering also leads to a HR underestimation at cloud base and an overestimation at cloud top, making the base-to-top heating gradient less sharp at the cloud-resolving scale.

54 ENVIRONMENTAL SCIENCES↗

High-Volume Precipitation Spectrometer (HVPS) Instrument Handbook

The high-volume precipitation spectrometer (HVPS) is a U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) user facility instrument for measuring hydrometeors larger than 150 μm. It is an open-path instrument located on the outside of the aircraft, typically below the wing. A laser sheet throws a shadowgraph image of the hydrometeor (cloud droplets or ice crystals) in the sample volume on a photodiode array. As the hydrometeor moves through the sample volume, this optical array records the moving shape and a two-dimensional picture can be recorded. At an air speed of 100 m/s, the sample volume is 310 l/s. The recorded images can be analyzed for size distributions, number concentrations, and further cloud properties detailed below. Hydrometeors in the range of 0.3-19.2 mm can be fully recorded at a 150 μm resolution; larger particles can only be sized along the direction of flight.

54 ENVIRONMENTAL SCIENCES↗

Sources and Composition of Organic Aerosols in the Central Arctic during Spring and Summer

Organic aerosols (OA) are a major component of Arctic aerosol mass and influence the region’s radiation budget, yet their sources and physicochemical properties remain largely unknown. We investigate OA sources and climate-relevant characteristics over the central Arctic Ocean in spring and summer, by applying positive matrix factorization to aerosol mass spectrometry data from two ship-based expeditions (2018 and 2020), complemented by total and interstitial aerosol measurements during fog periods. Six distinct OA factors were identified: haze-related OA, Arctic oxygenated OA, two mixed-OA types resembling biomass burning and primary marine OA linked to warm-air intrusions, marine OA, and hydrocarbon-related OA. Seasonal transitions strongly shaped OA composition. Following polar sunrise, highly oxygenated OA, likely formed secondarily from photo-oxidized volatile organic compounds, became dominant. After the polar vortex collapsed in May, episodic spikes in marine OA from the marginal ice zone appeared, alongside a reduced influence from Eurasian anthropogenic sources. These transitions influenced OA oxidation state and related properties including volatility, acidity, and hygroscopicity, highlighting the role of the Arctic spring atmosphere as an active photochemical reactor. Overall, OA was highly oxidized, with particles activated in fog during summer showing even greater oxidation, suggesting that central Arctic OA can be highly cloud active.

Arctic haze↗