Search

Leveraging aerosol data from multiple airborne and surface-based field campaigns encompassing diverse environmental conditions, we calculate statistics of the oxalate-sulfate mass ratio (median: 0.0217; 95% confidence interval: 0.0154-0.0296; R = 0.76; N = 2,948). Ground-based measurements of the oxalate-sulfate ratio fall within our 95% confidence interval, suggesting the range is robust within the mixed layer for the submicrometer particle size range. We demonstrate that dust and biomass burning emissions can separately bias this ratio toward higher values by at least one order of magnitude. In the absence of these confounding factors, the 95% confidence interval of the ratio may be used to estimate the relative extent of aqueous processing by comparing inferred oxalate concentrations between air masses, with the assumption that sulfate primarily originates from aqueous processing.

Cloud drop number concentrations ( N d ) over the western North Atlantic Ocean (WNAO) are generally highest during the winter (DJF) and lowest in summer (JJA), in contrast to aerosol proxy variables (aerosol optical depth, aerosol index, surface aerosol mass concentrations, surface cloud condensation nuclei (CCN) concentrations) that generally peak in spring (MAM) and JJA with minima in DJF. Using aircraft, satellite remote sensing, ground-based in situ measurement data, and reanalysis data, we characterize factors explaining the divergent seasonal cycles and furthermore probe into factors influencing N d on seasonal timescales. The results can be summarized well by features most pronounced in DJF, including features associated with cold-air outbreak (CAO) conditions such as enhanced values of CAO index, planetary boundary layer height (PBLH), low-level liquid cloud fraction, and cloud-top height, in addition to winds aligned with continental outflow. Data sorted into high- and low- N d days in each season, especially in DJF, revealed that all of these conditions were enhanced on the high- N d days, including reduced sea level pressure and stronger wind speeds. Although aerosols may be more abundant in MAM and JJA, the conditions needed to activate those particles into cloud droplets are weaker than in colder months, which is demonstrated by calculations of the strongest (weakest) aerosol indirect effects in DJF (JJA) based on comparing N d to perturbations in four different aerosol proxy variables (total and sulfate aerosol optical depth, aerosol index, surface mass concentration of sulfate). We used three machine learning models and up to 14 input variables to infer about most influential factors related to N d for DJF and JJA, with the best performance obtained with gradient-boosted regression tree (GBRT) analysis. The model results indicated that cloud fraction was the most important input variable, followed by some combination (depending on season) of CAO index and surface mass concentrations of sulfate and organic carbon. Future work is recommended to further understand aspects uncovered here such as impacts of free tropospheric aerosol entrainment on clouds, degree of boundary layer coupling, wet scavenging, and giant CCN effects on aerosol- N d relationships, updraft velocity, and vertical structure of cloud properties such as adiabaticity that impact the satellite estimation of N d ., Competing Interests: Competing interests. The authors declare that they have no conflict of interest.

Coastal southeast Florida experiences a wide range of aerosol conditions, including African dust, biomass burning (BB) aerosols, as well as sea salt and other locally-emitted aerosols. These aerosols are important sources of cloud condensation nuclei (CCN), which play an essential role in governing cloud radiative properties. As marine environments dominate the surface of Earth, CCN characteristics in coastal southeast Florida have broad implications for other regions with the added feature that this site is perturbed by both natural and anthropogenic emissions. This study investigates the influence of different air mass types on CCN concentrations at 0.2% (CCN 0.2% ) and 1.0% (CCN 1.0% ) supersaturation (SS) based on ground site measurements during selected months in 2013, 2017, and 2018. Average CCN 0.2% and CCN 1.0% concentrations were 373 ± 200 cm -3 and 584 ± 323 cm -3 , respectively, for four selected days with minimal presence of African dust and BB (i.e., background days). CCN concentrations were not elevated on the four days with highest influence of African dust (289 ± 104 cm -3 [0.2% SS] and 591 ± 302 cm -3 [1.0% SS]), consistent with high dust mass concentrations comprised of coarse particles that are few in number. In contrast, CCN concentrations were substantially enhanced on the five days with the greatest impact from BB (1408 ± 976 cm -3 [0.2% SS] and 3337 ± 1252 cm -3 [1.0% SS]). Ratios of CCN 0.2% :CCN 1.0% were used to compare the hygroscopicity of the aerosols associated with African dust, BB, and background days. Average ratios were similar for days impacted by African dust and BB (0.54 ± 0.17 and 0.55 ± 0.17, respectively). A 29% higher average ratio was observed on background days (0.71 ± 0.14), owing in part to a strong presence of sea salt and reduced presence of more hydrophobic species such as those of a carbonaceous or mineral-dust nature. Finally, periods of heavy rainfall were shown to effectively decrease both CCN 0.2% and CCN 1.0% concentrations. However, the rate varied at which such concentrations increased after the rain. This work contributes knowledge on the nucleating ability of African dust and BB in a marine environment after varying periods of atmospheric transport (days to weeks). The results can be used to understand the hygroscopicity of these air mass types, predict how they may influence cloud properties, and provide a valuable model constraint when predicting CCN concentrations in comparable situations., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.

The Western North Atlantic Ocean (WNAO) and adjoining East Coast of North America are of great importance for atmospheric research and have been extensively studied for several decades. This broad region exhibits complex meteorological features and a wide range of conditions associated with gas and particulate species from many sources regionally and other continents. As Part 1 of a 2-part paper series, this work characterizes quantities associated with atmospheric chemistry, including gases, aerosols, and wet deposition, by analyzing available satellite observations, ground-based data, model simulations, and reanalysis products. Part 2 provides insight into the atmospheric circulation, boundary layer variability, three-dimensional cloud structure, properties, and precipitation over the WNAO domain. Key results include spatial and seasonal differences in composition along the North American East Coast and over the WNAO associated with varying sources of smoke and dust and meteorological drivers such as temperature, moisture, and precipitation. Spatial and seasonal variations of tropospheric carbon monoxide and ozone highlight different pathways toward the accumulation of these species in the troposphere. Spatial distributions of speciated aerosol optical depth and vertical profiles of aerosol mass mixing ratios show a clear seasonal cycle highlighting the influence of different sources in addition to the impact of intercontinental transport. Analysis of long-term climate model simulations of aerosol species and satellite observations of carbon monoxide confirm that there has been a significant decline in recent decades among anthropogenic constituents owing to regulatory activities.

This study focuses on the long-term aerosol and precipitation chemistry measurements from colocated monitoring sites in Southern Florida between 2013 and 2018. A positive matrix factorization (PMF) model identified six potential emission sources impacting the study area. The PMF model solution yielded the following source concentration profiles: (i) combustion; (ii) fresh sea salt; (iii) aged sea salt; (iv) secondary sulfate; (v) shipping emissions; and (vi) dust. Based on these results, concentration-weighted trajectory maps were developed to identify sources contributing to the PMF factors. Monthly mean precipitation pH values ranged from 4.98 to 5.58, being positively related to crustal species and negatively related to SO 4 2- . Sea salt dominated wet deposition volume-weighted concentrations year-round without much variability in its mass fraction in contrast to stronger seasonal changes in PM 2.5 composition where fresh sea salt was far less influential. The highest mean annual deposition fluxes were attributed to Cl - , NO 3 - , SO 4 2- , and Na + between April and October. Nitrate is strongly correlated with dust constituents (unlike sea salt) in precipitation samples, indicative of efficient partitioning to dust. Interrelationships between precipitation chemistry and aerosol species based on long-term surface data provide insight into aerosol-cloud-precipitation interactions., Competing Interests: Conflicts of Interest: The authors declare no conflict of interest.

Decades of atmospheric research have focused on the Western North Atlantic Ocean (WNAO) region because of its unique location that offers accessibility for airborne and ship measurements, gradients in important atmospheric parameters, and a range of meteorological regimes leading to diverse conditions that are poorly understood. This work reviews these scientific investigations for the WNAO region, including the East Coast of North America and the island of Bermuda. Over 50 field campaigns and long-term monitoring programs, in addition to 715 peer-reviewed publications between 1946 and 2019 have provided a firm foundation of knowledge for these areas. Of particular importance in this region has been extensive work at the island of Bermuda that is host to important time series records of oceanic and atmospheric variables. Our review categorizes WNAO atmospheric research into eight major categories, with some studies fitting into multiple categories (relative %): Aerosols (25%), Gases (24%), Development/Validation of Techniques, Models, and Retrievals (18%), Meteorology and Transport (9%), Air-Sea Interactions (8%), Clouds/Storms (8%), Atmospheric Deposition (7%), and Aerosol-Cloud Interactions (2%). Recommendations for future research are provided in the categories highlighted above.

Provision of clean water is among the most serious, long-term challenges in the world. To an ever increasing degree, sustainable water supply depends on the utilization of water of impaired initial quality. This is particularly true in developing nations and in water-stressed areas such as the American Southwest. One clear example is the Navajo Nation. The reservation covers 27,000 square miles, mainly in northeastern Arizona. Low population density coupled with water scarcity and impairment makes provision of clean water particularly challenging. The Navajos rely primarily on ground water, which is often present in deep aquifers or of brackish quality. Commonly, reverse osmosis (RO) is chosen to desalinate brackish ground water, since RO costs are competitive with those of thermal desalination, even for seawater applications. However, both conventional thermal distillation and RO are energy intensive, complex processes that discourage decentralized or rural implementation. In addition, both technologies demand technical experience for operation and maintenance, and are susceptible to scaling and fouling unless extensive feed pretreatment is employed. Membrane distillation (MD), driven by vapor pressure gradients, can potentially overcome many of these drawbacks. MD can operate using low-grade, sub-boiling sources of heat and does not require extensive operational experience. This presentation discusses a project on the Navajo Nation, Arizona (Native American tribal lands) that is designed to investigate and deploy an autonomous (off-grid) system to pump and treat brackish groundwater using solar energy. Βench-scale, hollow fiber MD experiment results showed permeate water fluxes from 21 L/m2·d can be achieved with transmembrane temperature differences between 40 and 80˚C. Tests run with various feed salt concentrations indicate that the permeate flux decreases only about 25% as the concentration increases from 0 to 14% (w/w), which is four times seawater salt concentration. The quality of the permeate water remains constant at about 1 mg/L regardless of the changes in the influent salt concentration. A nine-month MD field trial, using hollow fiber membranes and completely off-the-shelf components demonstrated that a scaled-up solar-driven MD system was practical and economically viable. Based on these results, a pilot scale unit will be constructed and deployed on the tribal lands.