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Observations and theories related to Antarctic ozone changes

In 1985, there was a report of a large, sudden, and unanticipated decrease in the abundance of springtime Antarctic ozone over the last decade. By 1987, ozone decreases of more than 50 percent in the total column, and 95 percent locally between 15 and 20 km, had been observed. The scientific community quickly rose to the challenge of explaining this remarkable discovery; theoreticians soon developed a series of chemical and dynamical hypotheses to explain the ozone loss. Three basic theories were proposed to explain the springtime ozone hole. (1) The ozone hole is caused by the increasing atmospheric loadings of manmade chemicals containing chlorine (chlorofluorocarbons (CFC's) and bromine (halons)). These chemicals efficiently destroy ozone in the lower stratosphere in the Antarctic because of the special geophysical conditions, of an isolated air mass (polar vortex) with very cold temperatures, that exist there. (2) The circulation of the atmosphere in spring has changed from being predominantly downward over Antarctica to upward. This would mean that ozone poor air from the troposphere, instead of ozone rich air from the upper stratosphere, would be transported into the lower Antarctic stratosphere. (3) The abundance of the oxides of nitrogen in the lower Antarctic stratosphere is periodically enhanced by solar activity. Nitrogen oxides are produced in the upper mesosphere and thermosphere and then transported downward into the lower stratosphere in Antarctica, resulting in the chemical destruction of ozone. The climatology and trends of ozone, temperature, and polar stratospheric clouds are discussed. Also, the transport and chemical theories for the Antarctic ozone hole are presented.

Hartmann, D.↗

THERMS Technology Commercialization Fund Final Report

The technology commercialization fund assisted with the design and development of an intermediate scale packed be thermal energy storage system. Presented in this final report is the design, testing, and modeling of a 100 kWh th radial packed-bed. Air is used as a heat transfer fluid and 3/8” pea gravel is used as the storage medium. Testing has demonstrated the formation of a thermocline within the packed-bed. An air charging temperature of 450 °C was achieved resulting in a charging power of 26.5 kWh th . The radial packed-bed was charged for 5 hours and discharged for 5 hours. Minimal temperature variation was observed at the bottom, middle, and top axial locations of the radial packed-bed which suggests that buoyancy and hydrodynamics in the injection well had a minimal effect on the uniformity of air flow through the bed during charging and discharging. This indicates that the forced convection in a radial direction is dominating the flow regime compared to the buoyancy. The findings of this study suggest an increased air duct diameter through the air heater will increase the charging temperature and increase air mass flow through the system. Increased mass flow through the packed-bed is hypothesized to shorten the thermocline length. Modeled and measured results are compared, and it is here determined that a more comprehensive CFD model will aid in the understanding of air flow and thermocline evolution within the packed-bed.

25 ENERGY STORAGE↗

Data on incident solar energy

Instrumentation for solar irradiance monitoring, and radiation scales are discussed in a survey of incident solar energy data. The absolute accuracy and intrinsic reliability of the values of the solar constant and zero air mass solar spectrum proposed by the Institute of Environmental Sciences as an ASTM standard are evaluated. Extraterrestrial observations are used for deriving solar irradiance data at ground level for widely varying atmospheric parameters, with special reference to air pollution. The effects of diffuse sky radiance and those of varying slopes of the solar energy collecting surface are examined. Average values of solar energy available at different locations in the United States are included.

Thekaekara, M. P.↗

Rapid Measurements of Aerosol Ionic Composition and 3-10 nm Particle Size Distributions On The NASA P3 To Better Quantify Processes Affecting Aerosols Advected From East Asia

The Particle Into Liquid Sample (PILS) was deployed on the NASA P3 for airborne measurements of fine particle ionic chemical composition. The data have been quality assured and reside in the NASA data archive. We have analyzed our data to characterize the sources and atmospheric processing of fine aerosol particles advected from the region during the experiments. Fine particle water-soluble potassium was found to serve as a useful aerosol tracer for biomass smoke. Ratios of PILS potassium to sulfate are used as a means of estimating the percent contribution of biomass burning to fine particle mass in mixed plumes advecting from Asia. The high correlations between K+ and NO3(sup -) and NH4(sup +)' indicated that biomass burning was a significant source of these aerosol compounds in the region. It is noteworthy that the air mass containing the highest concentrations of fine particles recorded in all of ACE-Asia and TRACE-P appeared to be advecting from the Bejing/Tientsin urban region and also had the highest K(+), NO3(sup -) and NH4(sup +) concentrations of both studies. Based on K+/SO4(sup 2-) ratio's, we estimated that the plume was composed of approx. 60% biomass burning emissions, possibly from the use of bio-fuels in the urban regions.

Weber, Rodney J.↗

A study of optimum cowl shapes and flow port locations for minimum drag with effective engine cooling, volume 2

The listings, user's instructions, sample inputs, and sample outputs of two computer programs which are especially useful in obtaining an approximate solution of the viscous flow over an arbitrary nonlifting three dimensional body are provided. The first program performs a potential flow solution by a well known panel method and readjusts this initial solution to account for the effects of the boundary layer displacement thickness, a nonuniform but unidirectional onset flow field, and the presence of air intakes and exhausts. The second program is effectually a geometry package which allows the user to change or refine the shape of a body to satisfy particular needs without a significant amount of human intervention. An effort to reduce the cruise drag of light aircraft through an analytical study of the contributions to the drag arising from the engine cowl shape and the foward fuselage area and also that resulting from the cooling air mass flowing through intake and exhaust sites on the nacelle is presented. The programs may be effectively used to determine the appropriate body modifications or flow port locations to reduce the cruise drag as well as to provide sufficient air flow for cooling the engine.

Fox, S. R.↗

Comments on "Atlantic Tropical Cyclogenetic Processes during SOP-3 NAMMA in the GEOS-5 Global Data Assimilation and Forecast System"

Considerable attention has been given to the potential negative impacts of the Saharan air layer (SAL) in recent years. Researchers recently raised questions about the negative impacts of Dunion and Velden and other studies in terms of storms that reached at least tropical storm strength and suggested that the SAL was an intrinsic part of the tropical cyclone environment for both storms that weaken after formation and those that intensify. Braun also suggested that several incorrect assumptions underlie many of the studies on the negative impacts of the SAL, including assumptions that most low-to-midlevel dry tropical air is SAL air, that the SAL is dry throughout its depth, and that the proximity of the SAL to storms struggling to intensify implies some role in that struggle. The recent paper by Reale et al.(RL1) is an example of the problems inherent in some of these assumptions. In their paper, RL1 analyze a simulation from the Global Earth Observing System (GEOS-5) global model and describe an extensive tongue of warm, dry air that stretches southward from at least 30 deg N (the northern limit of their plots) and wraps into a low pressure system during the period 26-29 August 2006, suppressing convection and possibly development of the African easterly wave associated with that low pressure system. They attributed the warm, dry tongue to the SAL (i.e., heating of the air mass during passage over the Sahara and radiative warming of the dust layer). Whether it was their intention, the implication is that this entire feature is due solely to the SAL and not to other possible sources of dry air or warmth. In addition, they suggested that a cool tongue of air in the boundary layer located directly beneath the elevated warm, dry tongue (forming a thermal dipole) was possibly the result of reduced solar radiation caused by an overlying dust layer. They stated that "the cool anomaly in the lower levels does not have any plausible explanation relying only on transport." In this comment, evidence from satellite and global meteorological analyses is presented that casts considerable doubt upon RL1 s interpretation of the GEOS-5 forecasts and their conclusion that the results implied a negative role of the SAL. We show that the major portion of the warm, dry air aloft was located in a nearly dust-free slot between two Saharan dust outbreaks, had a significant source from the midlatitudes (>30 N), and was likely driven by strong subsidence warming and drying. In addition, when wind fields are examined in a reference frame moving with the wave, National Centers for Environmental Prediction (NCEP) global meteorological analyses suggest that the cool tongue in the boundary layer can be readily explained by transport of cooler air from higher latitudes. At the very least, it offers a plausible alternative explanation for the cool tongue that does not rely on radiative impacts of the dust.

Braun, Scott A.↗

Issues and opportunities in space photovoltaics

Space power sources are becoming a central focus for determining man's potential and schedule for exploring and utilizing the benefits of space. The ability to search, probe, survey, and communicate throughout the universe will depend on providing adequate power to the instruments to do these jobs. Power requirements for space platforms are increasing and will continue to increase into the 21st century. Photovoltaics have been a dependable power source for space for the last 30 years and have served as the primary source of power on virtually all DOD and NASA satellites. The performance of silicon (Si) solar cells has increased from 10 percent air mass zero (AM0) solar energy conversion efficiency in the early 60's to almost 15 percent on today's spacecraft. Some technologists even think that the potential for solar photovoltaics has reached a plateau. However, present and near-future Air Force and NASA requirements show needs that, if the problems are looked upon as opportunities, can elevate the photovoltaic power source scientist and array structure engineer into the next technological photovoltaic growth curve.

Francis, Robert W.↗

Issues and opportunities in space photovoltaics

Space power sources are becoming a central focus for determining man's potential and schedule for exploring and utilizing the benefits of space. The ability to search, probe, survey, and communicate throughout the universe will depend on providing adequate power to the instruments to do these jobs. Power requirements for space platforms are increasing and will continue to increase into the 21st century. Photovoltaics have been a dependable power source for space for the last 30 years and have served as the primary source of power on virtually all DOD and NASA satellites. The performance of silicon (Si) solar cells has increased from 10 percent air mass zero (AM0) solar energy conversion efficiency in the early 60's to almost 15 percent on today's spacecraft. Some technologists even think that the potential for solar photovoltaics has reached a plateau. However, present and near-future Air Force and NASA requirements show needs that, if the problems are looked upon as opportunities, can elevate the photovoltaic power source scientist and array structure engineer into the next technological photovoltaic growth curve.

Francis, Robert W.↗

Icehouse Effect: A Polar Autumn and Winter Cooling Trend

The icehouse effect is a hypothesized polar climate trend toward cooling (or lack of warming) in response to greenhouse warming of adjacent lower latitudes. When greenhouse warmed air from lower latitudes moves over ice and snow, it generates a stronger, more stable, cappino, inversion than in a parallel case without greenhouse warming. Because the degree of decoupling between vertically adjacent air masses is directly dependent on the strength of the inversion, the capping inversion acts somewhat analogously to the walls and roof of the icehouse of generations past. What is inside the icehouse, namely the cold polar atmospheric boundary layer (ABL) air, is preserved by the "insulation" or decoupling, provided by the warm air aloft. Observations over the Arctic Ocean have shown an unexpected lack of any detectable surface warming trend over the past 40 years. This finding strongly contradicts climate model predictions that polar regions should show the strongest effect of greenhouse warming. It also stands in contrast to the consensus reached by the Intergovernmental Panel on Climate Change (IPCC), that human caused greenhouse warming is now detectable globally. One might ask: Are these Arctic observations wrong? Or, if right, is there a plausible physical explanation for them? The published observations mentioned above used about 50,000 soundings over the Arctic Ocean. Here I present a novel analysis of ALL available Arctic rawinsonde data north of 65N--a total of more than 1.1 million soundings. The analysis confirms the previously published result: There is indeed a slight climate-cooling trend in the vast majority of the data. Importantly, there are also select conditions (very strong and very weak stability of the ABL) which show a consistent, strong Arctic warming trend. It is the juxtaposition of these warming and cooling trends which defines a unique "icehouse signature" for which an explanation can be sought.

Wetzel, Peter J.↗

Wildfire Emission Transport and Its Impact on the Local Air Quality – Case Study Example from the LISTOS Campaign

The high O3 concentration and large aerosol backscatter were measured in New York City(NYC) region and Connecticut (CT) coastline between August 15-16, 2018 during the Long Island Sound Tropospheric Ozone Study (LISTOS) campaign. Two TOLNet ozone lidar systems, NASA Goddard Space Flight Center Tropospheric Ozone Differential Absorption Lidar (GSFC TROPOZ DIAL)and Langley Research Center (LaRC) Mobile Ozone Lidar (LMOL),were used to obtain vertical and temporal variation of local O3 concentration. The airborne High Altitude Lidar Observatory (HALO) system was used to detect the regional aerosol characteristic during this episode. The complex relationship between ozone and aerosol characteristics of wildfire emission layers was investigated. The HYSPLIT back-trajectory of the measured air parcel shows that the increase of the O3 concentration and aerosol backscatter are attributed to the significant wildfires in the Pacific Northwest and British Columbia regions during August 2018. Through correlation analyses, unique clustering relationships are identified between ozone and aerosol for different air mass types. This case study is further investigated in relation to satellite data from MODIS, MISR and CALIPSO to characterize plume behavior during transport. The importance of wildfire emission transport will be discussed in context of its impact to surface air quality at significant distances from fire events.

Liqiao Lei↗

Northwest Airlines flight experiments

An experiment was conducted in which real-time Total Ozone Mapping Spectrometer (TOMS) data was compared with Northwest Airlines upper air charts. It was demonstrated that the regions of steep gradient in total ozone corresponded with fronts in the upper troposphere, specifically breaks in the tropopause associated with jet streams. Other small scale structures in the ozone could be related to minor trough and ridge lines. This suggests that the relation between total ozone and tropopause height might apply even on relatively small scales, and an analysis produced high correlation coefficients provided that the air mass origin was considered. In a second test, cabin ozone mixing at 37,000 ft. varied from less than 100 ppb (300 DU total ozone) to greater than 300 ppb in a trough (400 DU total ozone). A third analysis showed that clear air turbulence was located where upper air fronts were in rapid motion as suggested by comparison of the 1200 UT synoptic charts and the ozone map taken about six hours later.

Krueger, Arlin J.↗

Improved Satellite Retrievals of NO2 and SO2 over the Canadian Oil Sands and Comparisons with Surface Measurements

Satellite remote sensing is increasingly being used to monitor air quality over localized sources such as the Canadian oil sands. Following an initial study, significantly low biases have been identified in current NO2 and SO2 retrieval products from the Ozone Monitoring Instrument (OMI) satellite sensor over this location resulting from a combination of its rapid development and small spatial scale. Air mass factors (AMFs) used to convert line-of-sight "slant" columns to vertical columns were re-calculated for this region based on updated and higher resolution input information including absorber profiles from a regional-scale (15 km × 15 km resolution) air quality model, higher spatial and temporal resolution surface reflectivity, and an improved treatment of snow. The overall impact of these new Environment Canada (EC) AMFs led to substantial increases in the peak NO2 and SO2 average vertical column density (VCD), occurring over an area of intensive surface mining, by factors of 2 and 1.4, respectively, relative to estimates made with previous AMFs. Comparisons are made with long-term averages of NO2 and SO2 (2005-2011) from in situ surface monitors by using the air quality model to map the OMI VCDs to surface concentrations. This new OMI-EC product is able to capture the spatial distribution of the in situ instruments (slopes of 0.65 to 1.0, correlation coefficients of greater than 0.9). The concentration absolute values from surface network observations were in reasonable agreement, with OMI-EC NO2 and SO2 biased low by roughly 30%. Several complications were addressed including correction for the interference effect in the surface NO2 instruments and smoothing and clear-sky biases in the OMI measurements. Overall these results highlight the importance of using input information that accounts for the spatial and temporal variability of the location of interest when performing retrievals.

surface concentration↗

Estimates of Lightning NOx Production Based on OMI NO2 Observations Over the Gulf of Mexico

We evaluate nitrogen oxide (NO(sub x) NO + NO2) production from lightning over the Gulf of Mexico region using data from the Ozone Monitoring Instrument (OMI) aboard NASAs Aura satellite along with detection efficiency-adjusted lightning data from the World Wide Lightning Location Network (WWLLN). A special algorithm was developed to retrieve the lightning NOx [(LNO(sub x)] signal from OMI. The algorithm in its general form takes the total slant column NO2 from OMI and removes the stratospheric contribution and tropospheric background and includes an air mass factor appropriate for the profile of lightning NO(sub x) to convert the slant column LNO2 to a vertical column of LNO(sub x). WWLLN flashes are totaled over a period of 3 h prior to OMI overpass, which is the time an air parcel is expected to remain in a 1 deg. x 1 deg. grid box. The analysis is conducted for grid cells containing flash counts greater than a threshold value of 3000 flashes that yields an expected LNO(sub x) signal greater than the background. Pixels with cloud radiance fraction greater than a criterion value (0.9) indicative of highly reflective clouds are used. Results for the summer seasons during 2007-2011 yield mean LNO(sub x) production of approximately 80 +/- 45 mol per flash over the region for the two analysis methods after accounting for biases and uncertainties in the estimation method. These results are consistent with literature estimates and more robust than many prior estimates due to the large number of storms considered but are sensitive to several substantial sources of uncertainty.

Lightning↗

Global-scale distribution of ozone in the remote troposphere from ATom and HIPPO airborne field missions

Ozone is a key constituent of the troposphere, where it drives photochemical processes, impacts air quality, and acts as a climate forcer. Large-scale in situ observations of ozone commensurate with the grid resolution of current Earth system models are necessary to validate model outputs and satellite retrievals. In this paper, we examine measurements from the Atmospheric Tomography (ATom; four deployments in 2016–2018) and the HIAPER Pole-to-Pole Observations (HIPPO; five deployments in 2009–2011) experiments, two global-scale airborne campaigns covering the Pacific and Atlantic basins. ATom and HIPPO represent the first global-scale, vertically resolved measurements of O3 distributions throughout the troposphere, with HIPPO sampling the atmosphere over the Pacific and ATom sampling both the Pacific and Atlantic. Given the relatively limited temporal resolution of these two campaigns, we first compare ATom and HIPPO ozone data to longer-term observational records to establish the representativeness of our dataset. We show that these two airborne campaigns captured on average 53 %, 54 %, and 38 % of the ozone variability in the marine boundary layer, free troposphere, and upper troposphere–lower stratosphere (UTLS), respectively, at nine well-established ozonesonde sites. Additionally, ATom captured the most frequent ozone concentrations measured by regular commercial aircraft flights in the northern Atlantic UTLS. We then use the repeated vertical profiles from these two campaigns to confirm and extend the existing knowledge of tropospheric ozone spatial and vertical distributions throughout the remote troposphere. We highlight a clear hemispheric gradient, with greater ozone in the Northern Hemisphere, consistent with greater precursor emissions and consistent with previous modeling and satellite studies. We also show that the ozone distribution below 8 km was similar in the extra-tropics of the Atlantic and Pacific basins, likely due to zonal circulation patterns. However, twice as much ozone was found in the tropical Atlantic as in the tropical Pacific, due to well-documented dynamical patterns transporting continental air masses over the Atlantic. Finally, we show that the seasonal variability of tropospheric ozone over the Pacific and the Atlantic basins is driven year-round by transported continental plumes and photochemistry, and the vertical distribution is driven by photochemistry and mixing with stratospheric air. This new dataset provides additional constraints for global climate and chemistry models to improve our understanding of both ozone production and loss processes in remote regions, as well as the influence of anthropogenic emissions on baseline ozone.

ATom, aircraft profiles, Atlantic pollution, ozone↗

Summertime tropospheric observations related to N(x)O(y) distributions and partitioning over Alaska - Arctic Boundary Layer Expedition 3A

Measurements of NO, NO2, PAN and NO(y) are presented for the summertime middle/lower troposphere over northern high latitudes. Chemical signatures from concurrent measurements of O3, CO, C2H2, C2H6, C3H8, C2Cl4, and H2O are used to characterize factors affecting the budget and distribution of N(x)O(y) in the Arctic and Sub-Arctic tropospheric air masses sampled over Alaska during the NASA Arctic Boundary Layer Expedition (ABLE 3A). The results implicate biomass burning in Siberia as the probable source of about one-third of the NO(y) abundance within the middle lower troposphere over Alaska and the downward transport of air from altitude in the vicinity of the tropopause as a major contributor to the abundance of NO(y) within the lower 6 km column over Alaska.

Sandholm, S. T.↗

Exploring the elevated water vapor signal associated with the free tropospheric biomass burning plume over the southeast Atlantic Ocean

In southern Africa, widespread agricultural fires produce substantial biomass burning (BB) emissions over the region. The seasonal smoke plumes associated with these emissions are then advected westward over the persistent stratocumulus cloud deck in the southeast Atlantic (SEA) Ocean, resulting in aerosol effects which vary with time and location. Much work has focused on the effects of these aerosol plumes, but previous studies have also described an elevated free tropospheric water vapor signal over the SEA. Water vapor influences climate in its own right, and it is especially important to consider atmospheric water vapor when quantifying aerosol-cloud interactions and aerosol radiative effects. Here we present airborne observations made during the NASA ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) campaign over the SEA Ocean. In observations collected from multiple independent instruments on the NASA P-3 aircraft (from near-surface to 6-7 km), we observe a strongly linear correlation between pollution indicators (carbon monoxide (CO) and aerosol loading) and atmospheric water vapor content, seen at all altitudes above the boundary layer. The focus of the current study is on the especially strong correlation observed during the ORACLES-2016 deployment (out of Walvis Bay, Namibia), but a similar relationship is also observed in the August 2017 and October 2018 ORACLES deployments. Using reanalyses from the European Centre for Medium-Range Weather Forecasts (ECMWF) and Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA-2), and specialized WRF-Chem simulations, we trace the plume-vapor relationship to an initial humid, smoky continental source region, where it mixes with clean, dry upper tropospheric air and then is subjected to conditions of strong westward advection, namely the southern African easterly jet (AEJ-S). Our analysis indicates that air masses likely left the continent with the same relationship between water vapor and carbon monoxide as was observed by aircraft. This linear relationship developed over the continent due to daytime convection within a deep continental boundary layer (up to ~5-6 km) and mixing with higher-altitude air, which resulted in fairly consistent vertical gradients in CO and water vapor, decreasing with altitude and varying in time, but this water vapor does not originate as a product of the BB combustion itself. Due to a combination of conditions and mixing between the smoky, moist continental boundary layer and the dry and fairly clean upper-troposphere air above (~6 km), the smoky, humid air is transported by strong zonal winds and then advected over the SEA (to the ORACLES flight region) following largely isentropic trajectories. Hybrid Single-Particle Lagrangian Integrated Trajectory model (HYSPLIT) back trajectories support this interpretation. This work thus gives insights into the conditions and processes which cause water vapor to covary with plume strength. Better understanding of this relationship, including how it varies spatially and temporally, is important to accurately quantify direct, semi-direct, and indirect aerosol effects over this region.

54 ENVIRONMENTAL SCIENCES↗

Indicators of transport and vertical motion from correlations between in situ measurements in the Airborne Antarctic Ozone Experiment

Analysis of small-scale structure in the in situ measurements made from the ER-2 during the Airborne Antarctic Ozone Experiment shows the existence of a region at the boundary of the chemiclly perturbed region where the mixing ratios and small-scale structure of trace gases are influenced by transport across the boundary. This transition region is characterized by horizontal interchange and vertical layering of air parcels from within and outside of the chemically perturbed region and negative small-scale correlations between ClO and ozone. The horizontal transport in this region creates large surface areas between dissimilar air masses, providing the potential for substantial mixing. Correlations between ClO and O3 show that the transition region extends to 2-4 deg of latitude to either side of the boundary of the chemically perturbed region. A + or - 4-deg-wide transition region would contain nearly as much air as the chemically perturbed region proper. Analysis of water vapor and nitrous oxide data suggests that diabatic descent is associated with dehydration. This could be caused by strong radiative cooling of those polar stratospheric clouds in which enough water condenses for the particles to fall and dehydrate the air.

Murphy, D. M.↗

Exploring the Elevated Water Vapor Signal Associated With the Free Tropospheric Biomass Burning Plume Over the Southeast Atlantic Ocean

In southern Africa, widespread agricultural fires produce substantial biomass burning (BB) emissions over the region. The seasonal smoke plumes associated with these emissions are then advected westward over the persistent stratocumulus cloud deck in the southeast Atlantic (SEA) Ocean, resulting in aerosol effects which vary with time and location. Much work has focused on the effects of these aerosol plumes, but previous studies have also described an elevated free tropospheric water vapor signal over the SEA. Water vapor influences climate in its own right, and it is especially important to consider atmospheric water vapor when quantifying aerosol–cloud interactions and aerosol radiative effects. Here we present airborne observations made during the NASA ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) campaign over the SEA Ocean. In observations collected from multiple independent instruments on the NASA P-3 aircraft (from near-surface to 6–7 km), we observe a strongly linear correlation between pollution indicators (carbon monoxide (CO) and aerosol loading) and atmospheric water vapor content, seen at all altitudes above the boundary layer. The focus of the current study is on the especially strong correlation observed during the ORACLES-2016 deployment (out of Walvis Bay, Namibia), but a similar relationship is also observed in the August 2017 and October 2018 ORACLES deployments. Using reanalyses from the European Centre for Medium-Range Weather Forecasts (ECMWF) and Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA-2), and specialized WRF-Chem simulations, we trace the plume–vapor relationship to an initial humid, smoky continental source region, where it mixes with clean, dry upper tropospheric air and then is subjected to conditions of strong westward advection, namely the southern African easterly jet (AEJ-S). Our analysis indicates that air masses likely left the continent with the same relationship between water vapor and carbon monoxide as was observed by aircraft. This linear relationship developed over the continent due to daytime convection within a deep continental boundary layer (up to ∼5–6 km) and mixing with higher-altitude air, which resulted in fairly consistent vertical gradients in CO and water vapor, decreasing with altitude and varying in time, but this water vapor does not originate as a product of the BB combustion itself. Due to a combination of conditions and mixing between the smoky, moist continental boundary layer and the dry and fairly clean upper-troposphere air above (∼6 km), the smoky, humid air is transported by strong zonal winds and then advected over the SEA (to the ORACLES flight region) following largely isentropic trajectories. Hybrid Single-Particle Lagrangian Integrated Trajectory model (HYSPLIT) back trajectories support this interpretation. This work thus gives insights into the conditions and processes which cause water vapor to covary with plume strength. Better understanding of this relationship, including how it varies spatially and temporally, is important to accurately quantify direct, semi-direct, and indirect aerosol effects over this region.

Kristina Pistone↗