ABSTRACT
New particle formation in the free troposphere is a major source of cloud condensation nuclei globally. The prevailing view is that in the free troposphere, new particles are formed predominantly in convective cloud outflows. We present another mechanism using global observations. We find that during stratospheric air intrusion events, the mixing of descending ozone-rich stratospheric air with more moist free tropospheric background results in elevated hydroxyl radical (OH) concentrations. Such mixing is most prevalent near the tropopause where the sulfur dioxide (SO2) mixing ratios are high. The combination of elevated SO2 and OH levels leads to enhanced sulfuric acid concentrations, promoting particle formation. Such new particle formation occurs frequently and over large geographic regions, representing an important particle source in the midlatitude free troposphere.
ABSTRACT
In-situ marine cloud droplet number concentrations (CDNCs), cloud condensation nuclei (CCN), and CCN proxies, based on particle sizes and optical properties, are accumulated from seven field campaigns: ACTIVATE; NAAMES; CAMP2EX; ORACLES; SOCRATES; MARCUS; and CAPRICORN2. Each campaign involves aircraft measurements, ship-based measurements, or both. Measurements collected over the North and Central Atlantic, Indo-Pacific, and Southern Oceans, represent a range of clean to polluted conditions in various climate regimes. With the extensive range of environmental conditions sampled, this data collection is ideal for testing satellite remote detection methods of CDNC and CCN in marine environments. Remote measurement methods are vital to expanding the available data in these difficult-to-reach regions of the Earth and improving our understanding of aerosol-cloud interactions. The data collection includes particle composition and continental tracers to identify potential contributing CCN sources. Several of these campaigns include High Spectral Resolution Lidar (HSRL) and polarimetric imaging measurements and retrievals that will be the basis for the next generation of space-based remote sensors and, thus, can be utilized as satellite surrogates.
ABSTRACT
Combined lidar and polarimeter retrievals of aerosol, cloud, and ocean microphysical properties involve single-scattering cloud calculations that are time consuming. We create a look-up table to speed up these calculations for water droplets in the atmosphere. In our new Lorenz-Mie look-up table we tabulate the light scattering by an ensemble of homogeneous isotropic spheres at wavelengths starting from 0.35 µm. The look-up table covers liquid water cloud particles with radii in the range of 0.001-500 µm while gaining an increase of up to 104 in computational speed. The covered complex refractive indices range from 1.25 to 1.36 for the real part and from 0 to 0.001 for the imaginary part. We show that we can precisely compute inherent optical properties for the particle size distributions ranging up to 100 µm for the effective radius and up to 0.6 for the effective variance. We test wavelengths from 0.35 to 2.3 µm and find that the elements of the normalized scattering matrix as well as the asymmetry parameter, the absorption, backscatter, extinction, and scattering coefficients are precise to within 1% for 96.7%-100% of cases depending on the inherent optical property. We also provide an example of using the look-up table with in situ measurements to determine agreement with remote sensing. The table together with C++, Fortran, MATLAB, and Python codes to interpolate the complex refractive index and apply different particle size distributions are freely available online.
ABSTRACT
Ångström exponents (α) allow reconstruction of aerosol optical spectra over a broad range of wavelengths from measurements at two or more wavelengths. Hyperspectral measurements of atmospheric aerosols provide opportunities to probe measured spectra for information inaccessible from only a few wavelengths. Four sets of hyperspectral in situ aerosol optical coefficients (aerosol-phase total extinction, σ ext, and absorption, σ abs; liquid-phase soluble absorption from methanol, σ MeOH-abs, and water, σ DI-abs, extracts) were measured from biomass burning aerosols (BBAs). Hyperspectral single scattering albedo (ω), calculated from σ ext and σ abs, provide spectral resolution over a wide spectral range rare for this optical parameter. Observed spectral shifts between σ abs and σ MeOH-abs/σ DI-abs argue in favor of measuring σ abs rather than reconstructing it from liquid extracts. Logarithmically transformed spectra exhibited curvature better fit by second-order polynomials than linear α. Mapping second order fit coefficients (a 1, a 2) revealed samples from a given fire tended to cluster together, that is, aerosol spectra from a given fire were similar to each other and somewhat distinct from others. Separation in (a 1, a 2) space for spectra with the same α suggest additional information in second-order parameterization absent from the linear fit. Spectral features found in the fit residuals indicate more information in the measured spectra than captured by the fits. Above-detection σ MeOH-abs at 0.7 µm suggests assuming all absorption at long visible wavelengths is BC to partition absorption between BC and brown carbon (BrC) overestimates BC and underestimates BrC across the spectral range. Hyperspectral measurements may eventually discriminate BBA among fires in different ecosystems under variable conditions.
ABSTRACT
The warm Gulf Stream sea surface temperatures strongly impact the evolution of winter clouds behind atmospheric cold fronts. Such cloud evolution remains challenging to model. The Gulf Stream is too wide within the ERA5 and MERRA2 reanalyses, affecting the turbulent surface fluxes. Known problems within the ERA5 boundary layer (too-dry and too-cool with too strong westerlies), ascertained primarily from ACTIVATE 2020 campaign aircraft dropsondes and secondarily from older buoy measurements, reinforce surface flux biases. In contrast, MERRA2 winter surface winds and air-sea temperature/humidity differences are slightly too weak, producing surface fluxes that are too low. Reanalyses boundary layer heights in the strongly forced winter cold-air-outbreak regime are realistic, whereas late-summer quiescent stable boundary layers are too shallow. Nevertheless, the reanalysis biases are small, and reanalyses adequately support their use for initializing higher-resolution cloud process modeling studies of cold-air outbreaks.
ABSTRACT
North American pollution outflow is ubiquitous over the western North Atlantic Ocean, especially in winter, making this location a suitable natural laboratory for investigating the impact of precipitation on aerosol particles along air mass trajectories. We take advantage of observational data collected at Bermuda to seasonally assess the sensitivity of aerosol mass concentrations and volume size distributions to accumulated precipitation along trajectories (APT). The mass concentration of particulate matter with aerodynamic diameter less than 2.5 µm normalized by the enhancement of carbon monoxide above background (PM2.5/ΔCO) at Bermuda was used to estimate the degree of aerosol loss during transport to Bermuda. Results for December-February (DJF) show that most trajectories come from North America and have the highest APTs, resulting in a significant reduction (by 53 %) in PM2.5/ΔCO under high-APT conditions (> 13.5 mm) relative to low-APT conditions (< 0.9 mm). Moreover, PM2.5/ΔCO was most sensitive to increases in APT up to 5 mm (-0.044 µg m-3 ppbv-1 mm-1) and less sensitive to increases in APT over 5 mm. While anthropogenic PM2.5 constituents (e.g., black carbon, sulfate, organic carbon) decrease with high APT, sea salt, in contrast, was comparable between high- and low-APT conditions owing to enhanced local wind and sea salt emissions in high-APT conditions. The greater sensitivity of the fine-mode volume concentrations (versus coarse mode) to wet scavenging is evident from AErosol RObotic NETwork (AERONET) volume size distribution data. A combination of GEOS-Chem model simulations of the 210Pb submicron aerosol tracer and its gaseous precursor 222Rn reveals that (i) surface aerosol particles at Bermuda are most impacted by wet scavenging in winter and spring (due to large-scale precipitation) with a maximum in March, whereas convective scavenging plays a substantial role in summer; and (ii) North American 222Rn tracer emissions contribute most to surface 210Pb concentrations at Bermuda in winter (~75 %-80 %), indicating that air masses arriving at Bermuda experience large-scale precipitation scavenging while traveling from North America. A case study flight from the ACTIVATE field campaign on 22 February 2020 reveals a significant reduction in aerosol number and volume concentrations during air mass transport off the US East Coast associated with increased cloud fraction and precipitation. These results highlight the sensitivity of remote marine boundary layer aerosol characteristics to precipitation along trajectories, especially when the air mass source is continental outflow from polluted regions like the US East Coast.
ABSTRACT
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.
ABSTRACT
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.
ABSTRACT
A particle-into-liquid sampler (PILS) was coupled to a flow-through conductivity cell to provide a continuous, nondestructive, online measurement in support of offline ion chromatography analysis. The conductivity measurement provides a rapid assessment of the total ion concentration augmenting slower batch-sample data from offline analysis and is developed primarily to assist airborne measurements, where fast time-response is essential. A conductivity model was developed for measured ions and excellent closure was derived for laboratory-generated aerosols (97% conductivity explained, R2 > 0.99). The PILS-conductivity measurement was extensively tested throughout the NASA Cloud, Aerosol and Monsoon Processes: Philippines Experiment (CAMP2Ex) during nineteen research flights. A diverse range of ambient aerosol was sampled from biomass burning, fresh and aged urban pollution, and marine sources. Ambient aerosol did not exhibit the same degree of closure as the laboratory aerosol, with measured ions only accountable for 43% of the conductivity. The remaining fraction of the conductivity was examined in combination with ion charge balance and found to provide additional supporting information for diagnosing and modeling particle acidity. An urban plume case study was used to demonstrate the utility of the measurement for supplementing compositional data and augmenting the temporal capability of the PILS.
ABSTRACT
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.
ABSTRACT
The Korea - United States Air Quality Study (May - June 2016) deployed instrumented aircraft and ground-based measurements to elucidate causes of poor air quality related to high ozone and aerosol concentrations in South Korea. This work synthesizes data pertaining to aerosols (specifically, particulate matter with aerodynamic diameters <2.5 micrometers, PM2.5) and conditions leading to violations of South Korean air quality standards (24-hr mean PM2.5 < 35 µg m-3). PM2.5 variability from AirKorea monitors across South Korea is evaluated. Detailed data from the Seoul vicinity are used to interpret factors that contribute to elevated PM2.5. The interplay between meteorology and surface aerosols, contrasting synoptic-scale behavior vs. local influences, is presented. Transboundary transport from upwind sources, vertical mixing and containment of aerosols, and local production of secondary aerosols are discussed. Two meteorological periods are probed for drivers of elevated PM2.5. Clear, dry conditions, with limited transport (Stagnant period), promoted photochemical production of secondary organic aerosol from locally emitted precursors. Cloudy humid conditions fostered rapid heterogeneous secondary inorganic aerosol production from local and transported emissions (Transport/Haze period), likely driven by a positive feedback mechanism where water uptake by aerosols increased gas-to-particle partitioning that increased water uptake. Further, clouds reduced solar insolation, suppressing mixing, exacerbating PM2.5 accumulation in a shallow boundary layer. The combination of factors contributing to enhanced PM2.5 is challenging to model, complicating quantification of contributions to PM2.5 from local versus upwind precursors and production. We recommend co-locating additional continuous measurements at a few AirKorea sites across South Korea to help resolve this and other outstanding questions: carbon monoxide/carbon dioxide (transboundary transport tracer), boundary layer height (surface PM2.5 mixing depth), and aerosol composition with aerosol liquid water (meteorologically-dependent secondary production). These data would aid future research to refine emissions targets to further improve South Korean PM2.5 air quality.
ABSTRACT
A new aircraft-mounted probe for collecting samples of cloud water has been designed, fabricated, and extensively tested. Following previous designs, the probe uses inertial separation to remove cloud droplets from the airstream, which are subsequently collected and stored for offline analysis. We report details of the design, operation, and modelled and measured probe performance. Computational fluid dynamics (CFD) was used to understand the flow patterns around the complex interior geometrical features that were optimized to ensure efficient droplet capture. CFD simulations coupled with particle tracking and multiphase surface transport modelling provide detailed estimates of the probe performance across the entire range of flight operating conditions and sampling scenarios. Physical operation of the probe was tested on a Lockheed C-130 Hercules (fuselage mounted) and de Havilland Twin Otter (wing pylon mounted) during three airborne field campaigns. During C-130 flights on the final field campaign, the probe reflected the most developed version of the design and a median cloud water collection rate of 4.5 mL min-1 was achieved. This allowed samples to be collected over 1-2 min under optimal cloud conditions. Flights on the Twin Otter featured an inter-comparison of the new probe with a slotted-rod collector, which has an extensive airborne campaign legacy. Comparison of trace species concentrations showed good agreement between collection techniques, with absolute concentrations of most major ions agreeing within 30 %, over a range of several orders of magnitude.
ABSTRACT
We present ground-based, advected aircraft engine emissions from flights taking off at Los Angeles International Airport. 275 discrete engine take-off plumes were observed on 18 and 25 May 2014 at a distance of 400 m downwind of the runway. CO2 measurements are used to convert the aerosol data into plume-average emissions indices that are suitable for modelling aircraft emissions. Total and non-volatile particle number EIs are of order 1016-1017 kg-1 and 1014-1016 kg-1, respectively. Black-carbon-equivalent particle mass EIs vary between 175-941 mg kg-1 (except for the GE GEnx engines at 46 mg kg-1). Aircraft tail numbers recorded for each take-off event are used to incorporate aircraft- and engine-specific parameters into the data set. Data acquisition and processing follow standard methods for quality assurance. A unique aspect of the data set is the mapping of aerosol concentration time series to integrated plume EIs, aircraft and engine specifications, and manufacturer-reported engine emissions certifications. The integrated data enable future studies seeking to understand and model aircraft emissions and their impact on air quality.
ABSTRACT
Aviation-related aerosol emissions contribute to the formation of contrail cirrus clouds that can alter upper tropospheric radiation and water budgets, and therefore climate. The magnitude of air-traffic-related aerosol-cloud interactions and the ways in which these interactions might change in the future remain uncertain. Modelling studies of the present and future effects of aviation on climate require detailed information about the number of aerosol particles emitted per kilogram of fuel burned and the microphysical properties of those aerosols that are relevant for cloud formation. However, previous observational data at cruise altitudes are sparse for engines burning conventional fuels, and no data have previously been reported for biofuel use in-flight. Here we report observations from research aircraft that sampled the exhaust of engines onboard a NASA DC-8 aircraft as they burned conventional Jet A fuel and a 50:50 (by volume) blend of Jet A fuel and a biofuel derived from Camelina oil. We show that, compared to using conventional fuels, biofuel blending reduces particle number and mass emissions immediately behind the aircraft by 50 to 70 per cent. Our observations quantify the impact of biofuel blending on aerosol emissions at cruise conditions and provide key microphysical parameters, which will be useful to assess the potential of biofuel use in aviation as a viable strategy to mitigate climate change.
Subject(s)
Aircraft/instrumentation , Biofuels/analysis , Particulate Matter/analysis , Vehicle Emissions/analysis , Vehicle Emissions/prevention & control , Aerosols/analysis , Aerosols/chemistry , Global Warming/prevention & control , Greenhouse Effect/prevention & control , Particulate Matter/chemistryABSTRACT
In support of future satellite missions that aim to address the current shortcomings in measuring air quality from space, NASA's Deriving Information on Surface Conditions from Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER-AQ) field campaign was designed to enable exploration of relationships between column measurements of trace species relevant to air quality at high spatial and temporal resolution. In the DISCOVER-AQ data set, a modest correlation (r 2 = 0.45) between ozone (O3) and formaldehyde (CH2O) column densities was observed. Further analysis revealed regional variability in the O3-CH2O relationship, with Maryland having a strong relationship when data were viewed temporally and Houston having a strong relationship when data were viewed spatially. These differences in regional behavior are attributed to differences in volatile organic compound (VOC) emissions. In Maryland, biogenic VOCs were responsible for ~28% of CH2O formation within the boundary layer column, causing CH2O to, in general, increase monotonically throughout the day. In Houston, persistent anthropogenic emissions dominated the local hydrocarbon environment, and no discernable diurnal trend in CH2O was observed. Box model simulations suggested that ambient CH2O mixing ratios have a weak diurnal trend (±20% throughout the day) due to photochemical effects, and that larger diurnal trends are associated with changes in hydrocarbon precursors. Finally, mathematical relationships were developed from first principles and were able to replicate the different behaviors seen in Maryland and Houston. While studies would be necessary to validate these results and determine the regional applicability of the O3-CH2O relationship, the results presented here provide compelling insight into the ability of future satellite missions to aid in monitoring near-surface air quality.
ABSTRACT
Despite controversies on the potential of hematopoietic stem cells (HSCs) to promote tissue repair, we previously showed that HSC transplantation could correct cystinosis, a multisystemic lysosomal storage disease, caused by a defective lysosomal membrane cystine transporter, cystinosin (CTNS gene). Addressing the cellular mechanisms, we here report vesicular cross-correction after HSC differentiation into macrophages. Upon coculture with cystinotic fibroblasts, macrophages produced tunneling nanotubes (TNTs) allowing transfer of cystinosin-bearing lysosomes into Ctns-deficient cells, which exploited the same route to retrogradely transfer cystine-loaded lysosomes to macrophages, providing a bidirectional correction mechanism. TNT formation was enhanced by contact with diseased cells. In vivo, HSCs grafted to cystinotic kidneys also generated nanotubular extensions resembling invadopodia that crossed the dense basement membranes and delivered cystinosin into diseased proximal tubular cells. This is the first report of correction of a genetic lysosomal defect by bidirectional vesicular exchange via TNTs and suggests broader potential for HSC transplantation for other disorders due to defective vesicular proteins.
Subject(s)
Hematopoietic Stem Cell Transplantation , Hematopoietic Stem Cells/cytology , Lysosomes/metabolism , Macrophages/cytology , Nanotubes , Animals , Cystinosis/metabolism , Cystinosis/pathology , Cystinosis/therapy , Fibroblasts , Hematopoietic Stem Cells/metabolism , Humans , Macrophages/metabolism , Mice , Mice, Inbred C57BL , Mice, TransgenicABSTRACT
Previous clinical studies with indapamide, an indoline antihypertensive drug with diuretic and vasodilating activities, have shown a dose relationship associated with potassium loss. Two placebo-controlled, randomized, double-blind, parallel clinical studies were, therefore, done to evaluate the safety and efficacy of a low dose (1.25 mg) of indapamide and to determine if an improved safety profile could be produced while maintaining efficacy with a 1.25-mg dose in patients with mild to moderate essential hypertension. Four hundred seventeen (417) adult patients with mild to moderate essential hypertension (sitting diastolic blood pressure greater-than-or-equal 95 mmHg and less-than-or-equal 110 mmHg) were enrolled in two clinical studies; 209 patients were randomized to indapamide 1.25 mg and 208 patients to placebo. Patients received single-blind placebo for a 4-week washout period followed by an 8-week double-blind treatment period during which patients received either indapamide 1.25 mg or placebo. The primary efficacy endpoint was the mean change from baseline to week 8 in sitting diastolic blood pressure. Secondary efficacy variables were the proportion of patients whose sitting diastolic blood pressure had decreased greater-than-or-equal 10 mmHg and/or had a sitting diastolic blood pressure of less-than-or-equal 90 mmHg (treatment success) at all visits and at endpoint, mean changes from baseline in sitting diastolic blood pressure at designated timepoints and at endpoint, and mean changes from baseline in standing diastolic blood pressure and in sitting and standing systolic blood pressure at all visits and at endpoint. Results of these trials were pooled in order to have a larger patient population in an attempt to detect trends not readily apparent with a smaller sample size. In the primary analysis, indapamide produced statistically significantly (p = 0.0001) greater reductions in sitting diastolic blood pressure than placebo after 8 weeks of therapy. In the secondary analysis, the percentage of indapamide-treated patients who achieved treatment success after 8 weeks of therapy was statistically significantly (p < 0.0001) higher compared to placebo-treated patients. In addition, indapamide produced a statistically significantly (p = 0.0001) superior reduction compared to placebo in sitting systolic and standing systolic and diastolic blood pressure after 8 weeks of therapy. The incidence of drug-related adverse events between patients in the indapamide and placebo groups was similar. There were no clinically meaningful differences in laboratory values, including serum potassium, between the patients in the indapamide and placebo groups. Low-dose (1.25 mg) indapamide proved to be safe and effective in the treatment of mild to moderate hypertension.