Chloride (Cl−) displacement from sea salt particles is an extensively studied phenomenon with implications for human health, visibility, and the global radiation budget. Past works have investigated ...Cl− depletion over the northwest Atlantic (NWA); however, an updated, multi-seasonal, and geographically expanded account of sea salt reactivity over the region is needed. This study uses chemically resolved mass concentrations and meteorological data from the airborne Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment (ACTIVATE) to quantify seasonal, spatial, and meteorological trends in Cl− depletion and to explore the importance of quantifying (1) non-sea salt sources of Na+ and (2) mass concentrations of lost Cl− (instead of relative amounts displaced). Lost Cl− mass concentrations are lowest in December–February and March, moderate around Bermuda in June, and highest in May (median losses of 0.04, 0.04, 0.66, and 1.76 µg m−3, respectively), with losses in May that are high enough to potentially accelerate tropospheric oxidation rates. Inorganic acidic species can account for all Cl− depletion in December–February, March, and June near Bermuda but none of the lost Cl− in May, suggesting that organic acids may be of importance for Cl− displacement in certain months. Contributions of dust to Na+ are not important seasonally but may cause relevant overestimates of lost Cl− in smoke and dust plumes. Higher percentages of Cl− depletion often do not correspond to larger mass concentrations of lost Cl−, so it is highly recommended to quantify the latter to place depletion reactions in context with their role in atmospheric oxidation and radiative forcing.
We evaluate the sensitivity of the size calibrations of
two commercially available, high-resolution optical particle sizers to
changes in aerosol composition and complex refractive index (RI). The
...Droplet Measurement Technologies Ultra-High Sensitivity Aerosol Spectrometer (UHSAS) and the TSI, Inc. Laser Aerosol Spectrometer (LAS) are
two commonly used instruments for measuring the portion of the aerosol size
distribution with diameters larger than nominally 60–90 nm. Both instruments
illuminate particles with a laser and relate the single-particle light
scattering intensity and count rate measured over a wide range of angles to
the size-dependent particle concentration. While the optical block geometry
and flow system are similar for each instrument, a significant difference
between the two models is the laser wavelength (1054 nm for the UHSAS and
633 nm for the LAS) and intensity (about 100 times higher for the UHSAS), which
may affect the way each instrument sizes non-spherical or absorbing
aerosols. Here, we challenge the UHSAS and LAS with laboratory-generated,
mobility-size-classified aerosols of known chemical composition to quantify
changes in the optical size response relative to that of ammonium sulfate
(RI of 1.52+0i at 532 nm) and NIST-traceable polystyrene latex spheres
(PSLs with RI of 1.59+0i at 589 nm). Aerosol inorganic salt species are
chosen to cover the real refractive index range of 1.32 to 1.78, while
chosen light-absorbing carbonaceous aerosols include fullerene soot,
nigrosine dye, humic acid, and fulvic acid standards. The instrument
response is generally in good agreement with the electrical mobility
diameter. However, large undersizing deviations are observed for the
low-refractive-index fluoride salts and the strongly absorbing nigrosine dye and fullerene soot particles. Polydisperse size distributions for both fresh
and aged wildfire smoke aerosols from the recent Fire Influence on Regional
to Global Environments Experiment and Air Quality (FIREX-AQ) and the Cloud,
Aerosol, and Monsoon Processes Philippines Experiment (CAMP2Ex)
airborne campaigns show good agreement between both optical sizers and
contemporaneous electrical mobility sizing and particle time-of-flight mass
spectrometric measurements. We assess the instrument uncertainties by
interpolating the laboratory response curves using previously reported RIs
and size distributions for multiple aerosol type classifications. These
results suggest that, while the optical sizers may underperform for strongly
absorbing laboratory compounds and fresh tailpipe emissions measurements,
sampling aerosols within the atmospherically relevant range of refractive
indices are likely to be sized to better than ±10 %–20 % uncertainty over the submicron aerosol size range when using instruments calibrated with
ammonium sulfate.
Biological aerosols represent a diverse subset of particulate matter that is emitted directly to the atmosphere in the form of (but not limited to) bacteria, fungal spores, pollens, viruses, and ...plant debris. These particles can have local air quality implications, but potentially play a larger climate role by acting as efficient ice nucleating particles (INPs) and cloud condensation nuclei. We have deployed a Wideband Integrated Bioaerosol Sensor on the NASA DC‐8 aircraft to (1) quantify boundary layer (BL) variability of fluorescent biological aerosol particle (FBAP) concentrations in the Southeast United States (SEUS), (2) link this variability explicitly to land cover heterogeneity in the region, and (3) examine the vertical profile of bioaerosols in the context of convective vertical redistribution. Flight‐averaged FBAP concentrations ranged between 0.1 and 0.43 scm−3 (cm−3 at standard temperature and pressure) with relatively homogeneous concentrations throughout the region; croplands showed the highest concentrations in the BL (0.37 scm−3), and lowest concentrations were associated with evergreen forests (0.24 scm−3). Observed FBAP concentrations are in generally good agreement with model parameterized emission rates for bacteria, and discrepancies are likely the result of fungal spore contributions. Shallow convection in the region is shown to be a relatively efficient lofting mechanism as the vertical transport efficiency of FBAP is at least equal to black carbon aerosol, suggesting that ground‐level FBAP survives transport into the free troposphere to be available for INP activation. Comparison of the fraction of coarse‐mode particles that were biological (fFBAP) suggested that the SEUS (fFBAP = 8.5%) was a much stronger source of bioaerosols than long‐range transport during a Saharan Air Layer (SAL) dust event (fFBAP = 0.17%) or summertime marine emissions in the Gulf of Mexico (fFBAP = 0.73%).
Key Points
The southeast USA region is a significant source of bioaerosols
Shallow convection allows vertical transport of bioaerosols
Emission rates from different land types are relatively homogeneous
Due to their fast evolution and large natural variability in macro- and microphysical properties, the accurate representation of boundary layer clouds in current climate models remains a challenge. ...One of the regions with large intermodel spread in the Coupled Model Intercomparison Project Phase 6 ensemble is the western North Atlantic Ocean. Here, statistically representative in situ measurements can help to develop and constrain the parameterization of clouds in global models. To this end, we performed comprehensive measurements of boundary layer clouds, aerosol, trace gases, and radiation in the western North Atlantic Ocean during the NASA Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment (ACTIVATE) mission. In total, 174 research flights with 574 flight hours for cloud and precipitation measurements were performed with the HU-25 Falcon during three winter (February–March 2020, January–April 2021, and November 2021–March 2022) and three summer seasons (August–September 2020, May–June 2021, and May–June 2022). Here we present a statistical evaluation of 16 140 individual cloud events probed by the fast cloud droplet probe and the two-dimensional stereo cloud probe during 155 research flights in a representative and repetitive flight strategy allowing for robust statistical data analyses. We show that the vertical profiles of distributions of the liquid water content and the cloud droplet effective diameter (ED) increase with altitude in the marine boundary layer. Due to higher updraft speeds, higher cloud droplet number concentrations (Nliquid) were measured in winter compared to summer despite lower cloud condensation nucleus abundance. Flight cloud cover derived from statistical analysis of in situ data is reduced in summer and shows large variability. This seasonal contrast in cloud coverage is consistent with a dominance of a synoptic pattern in winter that favors conditions for the formation of stratiform clouds at the western edge of cyclones (post-cyclonic). In contrast, a dominant summer anticyclone is concomitant with the occurrence of shallow cumulus clouds and lower cloud coverage. The evaluation of boundary layer clouds and precipitation in the Nliquid ED phase space sheds light on liquid, mixed-phase, and ice cloud properties and helps to categorize the cloud data. Ice and liquid precipitation, often masked in cloud statistics by a high abundance of liquid clouds, is often observed throughout the cloud. The ACTIVATE in situ cloud measurements provide a wealth of cloud information useful for assessing airborne and satellite remote-sensing products, for global climate and weather model evaluations, and for dedicated process studies that address precipitation and aerosol–cloud interactions.
Nucleation in the free troposphere (FT) and subsequent growth of new particles represent a globally important source of cloud condensation nuclei (CCN). Whereas new particle formation (NPF) has been ...shown to occur frequently in the upper troposphere over tropical oceans, there have been few studies of NPF at lower altitudes. In addition, the impact of urban emissions and biomass burning on the NPF in tropical marine FT remains poorly understood. In this study, we examine NPF in the lower and mid-troposphere (3–8.5 km) over the tropical ocean and coastal region using airborne measurements during the recent Cloud, Aerosol and Monsoon Processes Philippines Experiment (CAMP2Ex). NPF was mostly observed above 5.5 km and coincided with elevated relative humidity (RH) and reduced condensation sink (CS), suggesting that NPF occurs in convective cloud outflow. The frequency of NPF increases with altitude, reaching ∼ 50 % above 8 km. An abrupt decrease in NPF frequency coincides with early monsoon transition and is attributed to increased CS resulting from reduced convective activity and more frequent transport of aged urban plumes. Surprisingly, a large fraction of NPF events in background air were observed in the early morning, and the NPF is likely made possible by very low CS despite low actinic flux. Convectively detrained biomass-burning plumes and fresh urban emissions enhance NPF as a result of elevated precursor concentrations and scavenging of pre-existing particles. In contrast, NPF is suppressed in aged urban plumes where the reactive precursors are mostly consumed, while CS remains relatively high. This study shows a strong impact of urban and biomass-burning emissions on the NPF in tropical marine FT. The results also illustrate the competing influences of different variables and interactions among anthropogenic emissions, convective clouds, and meteorology, which lead to NPF under a variety of conditions in tropical marine environments.
The NASA North Atlantic Aerosols and Marine Ecosystems Study (NAAMES) ship
and aircraft field campaign deployed to the western subarctic Atlantic
between the years 2015 and 2018. One of the primary ...goals of NAAMES is to
improve the understanding of aerosol–cloud interaction (ACI) over the
Atlantic Ocean under different seasonal regimes. ACIs currently represent the
largest source of uncertainty in global climate models. During three NAAMES
field campaigns (NAAMES-1 in November 2015, NAAMES-2 in May 2016, and
NAAMES-3 in September 2017), multiple 10 h science flights were conducted
using the NASA C-130 aircraft to measure marine boundary layer aerosol and
cloud properties. The standard flight pattern includes vertical spirals
where the C-130 transitioned from high altitude to low altitude (and vice
versa), collecting in situ measurements of aerosols, trace gases, clouds, and
meteorological parameters as a function of altitude. We examine the data
collected from 37 spirals during the three NAAMES field campaigns, and we
present a comprehensive characterization of the vertical profiles of aerosol
properties under different synoptic conditions and aerosol regimes. The
vertical distribution of submicron aerosol particles exhibited strong
seasonal variation, as well as elevated intra-seasonal variability depending
on emission sources and aerosol processes in the atmospheric column.
Pristine marine conditions and new particle formation were prevalent in the
wintertime (NAAMES-1) due to low biogenic emissions from the surface ocean
and reduced continental influence. Higher concentrations of submicron
aerosol particles were observed in the spring (NAAMES-2) due to strong
phytoplankton activity and the arrival of long-range-transported continental
plumes in the free troposphere with subsequent entrainment into the marine
boundary layer. Biomass burning from boreal wildfires was the main source of
aerosol particles in the region during the late summer (NAAMES-3) in both
the marine boundary layer and free troposphere.
Fires emit sufficient sulfur to affect local and regional air quality and climate. This study analyzes SO2 emission factors and variability in smoke plumes from US wildfires and agricultural fires, ...as well as their relationship to sulfate and hydroxymethanesulfonate (HMS) formation. Observed SO2 emission factors for various fuel types show good agreement with the latest reviews of biomass burning emission factors, producing an emission factor range of 0.47–1.2 g SO2 kg^(−1) C. These emission factors vary with geographic location in a way that suggests that deposition of coal burning emissions and application of sulfur-containing fertilizers likely play a role in the larger observed values, which are primarily associated with agricultural burning. A 0-D box model generally reproduces the observed trends of SO2 and total sulfate (inorganic + organic) in aging wildfire plumes. In many cases, modeled HMS is consistent with the observed organosulfur concentrations. However, a comparison of observed organosulfur and modeled HMS suggests that multiple organosulfur compounds are likely responsible for the observations but that the chemistry of these compounds yields similar production and loss rates as that of HMS, resulting in good agreement with the modeled results. We provide suggestions for constraining the organosulfur compounds observed during these flights, and we show that the chemistry of HMS can allow organosulfur to act as an S(IV) reservoir under conditions of pH > 6 and liquid water content >10^(−7) g sm^(−3). This can facilitate long-range transport of sulfur emissions, resulting in increased SO2 and eventually sulfate in transported smoke.
Wildfire smoke influences on air quality and atmospheric chemistry have been underscored by the increasing fire prevalence in recent years, and yet, the connection between fire, smoke emissions, and ...the subsequent transformation of this smoke in the atmosphere remains poorly constrained. Toward improving these linkages, we present a new method for coupling high time‐resolution satellite observations of fire radiative power with in situ observations of smoke aerosols and trace gases. We apply this technique to 13 fire plumes comprehensively characterized during the recent FIREX‐AQ mission and show that changes in fire radiative power directly translate into changes in conserved smoke tracers (CO2, CO, and black carbon aerosol) observed in the downwind smoke plume. The correlation is particularly strong for CO2 (mean r > 0.9). This method is important for untangling the competing effects of changing fire behavior versus the influence of dilution and atmospheric processing on the downwind evolution of measured smoke properties.
Key Points
Geostationary satellite observations of fire radiative power are highly correlated with in situ airborne measurements of primary‐emission smoke tracers
High‐resolution satellite observations are needed to disentangle how fire activity and plume dilution impact the downwind evolution of smoke
Diurnal fire activity for wildfires observed during FIREX‐AQ is best parameterized using a bimodal Gaussian distribution to inform models
The evolution of organic aerosol (OA) and aerosol size distributions within smoke plumes is uncertain due to the variability in rates of coagulation and OA condensation/evaporation between different ...smoke plumes and at different locations within a single plume. We use aircraft data from the FIREX-AQ campaign to evaluate differences in evolving aerosol size distributions, OA, and oxygen to carbon ratios (O:C) between and within smoke plumes during the first several hours of aging as a function of smoke concentration. The observations show that the median particle diameter increases faster in smoke of a higher initial OA concentration (1000 µg m.sup.-3 ), with diameter growth of over 100 nm in 8 h - despite generally having a net decrease in OA enhancement ratios - than smoke of a lower initial OA concentration (<100 µg m.sup.-3 ), which had net increases in OA. Observations of OA and O:C suggest that evaporation and/or secondary OA formation was greater in less concentrated smoke prior to the first measurement (5-57 min after emission). We simulate the size changes due to coagulation and dilution and adjust for OA condensation/evaporation based on the observed changes in OA. We found that coagulation explains the majority of the diameter growth, with OA evaporation/condensation having a relatively minor impact. We found that mixing between the core and edges of the plume generally occurred on timescales of hours, slow enough to maintain differences in aging between core and edge but too fast to ignore the role of mixing for most of our cases.
Marine biogenic particle contributions to atmospheric aerosol concentrations are not well understood though they are important for determining cloud optical and cloud-nucleating properties. Here we ...examine the relationship between marine aerosol measurements (with satellites and model fields of ocean biology) and meteorological variables during the North Atlantic Aerosols and Marine Ecosystems Study (NAAMES). NAAMES consisted of four field campaigns between November 2015 and April 2018 that aligned with the four major phases of the annual phytoplankton bloom cycle. The FLEXible PARTicle (FLEXPART) Lagrangian particle dispersion model is used to spatiotemporally connect these variables to ship-based aerosol and dimethyl sulfide (DMS) observations. We find that correlations between some aerosol measurements with satellite-measured and modeled variables increase with increasing trajectory length, indicating that biological and meteorological processes over the air mass history are influential for measured particle properties and that using only spatially coincident data would miss correlative connections that are lagged in time. In particular, the marine non-refractory organic aerosol mass correlates with modeled marine net primary production when weighted by 5 d air mass trajectory residence time (r=0.62). This result indicates that non-refractory organic aerosol mass is influenced by biogenic volatile organic compound (VOC) emissions that are typically produced through bacterial degradation of dissolved organic matter, zooplankton grazing on marine phytoplankton, and as a by-product of photosynthesis by phytoplankton stocks during advection into the region. This is further supported by the correlation of non-refractory organic mass with 2 d residence-time-weighted chlorophyll a (r=0.39), a proxy for phytoplankton abundance, and 5 d residence-time-weighted downward shortwave forcing (r=0.58), a requirement for photosynthesis. In contrast, DMS (formed through biological processes in the seawater) and primary marine aerosol (PMA) concentrations showed better correlations with explanatory biological and meteorological variables weighted with shorter air mass residence times, which reflects their localized origin as primary emissions. Aerosol submicron number and mass negatively correlate with sea surface wind speed. The negative correlation is attributed to enhanced PMA concentrations under higher wind speed conditions. We hypothesized that the elevated total particle surface area associated with high PMA concentrations leads to enhanced rates of condensation of VOC oxidation products onto PMA. Given the high deposition velocity of PMA relative to submicron aerosol, PMA can limit the accumulation of secondary aerosol mass. This study provides observational evidence for connections between marine aerosols and underlying ocean biology through complex secondary formation processes, emphasizing the need to consider air mass history in future analyses.
PDF
