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DOE OSTI2024

Burning conditions and transportation pathways determine biomass-burning aerosol properties in the Ascension Island marine boundary layer

African biomass-burning aerosol (BBA) in the southeast Atlantic Ocean (SEA) marine boundary layer (MBL) is an important contributor to Earth’s radiation budget yet its representation remains poorly constrained in regional and global climate models. Data from the Layered Atlantic Smoke Interactions with Clouds (LASIC) field campaign on Ascension Island (-7.95° N, -14.36° E) detail how fire source regions (burning conditions and fuel type), transport pathways, and longer-term chemical processing affect the chemical, microphysical, and optical properties of the BBA in the remote MBL between June and September of 2017. Ten individual plume events characterize the seasonal evolution of BBA characteristics. Inefficient burning conditions, determined by the mass ratio of refractory black carbon to above-background carbon monoxide (rBC:ΔCO), enhance organic- and sulfate-rich aerosol concentrations in June–July. In contrast, the heart of the burning season exhibited higher rBC:ΔCO values indicative of efficient burning conditions, correlating with more rBC-enriched BBA. Toward the end of the burning season, a mix of burning conditions results in increased variation of the BBA properties. The BBA transit to Ascension Island was predominantly through slow-moving pathways in the MBL and lower free troposphere (FT), facilitating prolonged chemical transformations through heterogeneous and aqueous phase processes. Heterogeneous oxidation can persist for up to 10 days, resulting in a considerable decrease in organic aerosol (OA) mass. OA to rBC mass ratios (OA:rBC) in the MBL between 2 and 5 contrast to higher values of 5 to 15 observed in the nearby FT. Conversely, early-season aqueous-phase processes primarily contributed to aerosol oxidation and some aerosol production, but not appreciable aerosol removal. These two chemical processes yield more light-absorbing BBA in the MBL than in the FT and explain the notably low scattering albedo at 530 nm (SSA 530 ) values (< 0.80) at Ascension Island. This study establishes a robust correlation between SSA 530 and OA:rBC across both MBL and FT, underscoring the dependency of optical properties on chemical composition. These findings highlight how the interplay between chemical composition and atmospheric processing can be improved in global and regional climate models. Questions remain on the mixing of aerosols with different pathway histories, and on what accounts for the doubling of the mass absorption coefficient in the boundary layer.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

Aerosol size distribution properties associated with cold-air outbreaks in the Norwegian Arctic

The aerosol particles serving as cloud condensation and ice nuclei contribute to key cloud processes associated with cold-air outbreak (CAO) events but are poorly constrained in climate models due to sparse observations. Here we retrieve aerosol number size distribution modes from measurements at Andenes, Norway, during the Cold-Air Outbreaks in the Marine Boundary Layer Experiment (COMBLE) and at Zeppelin Observatory, approximately 1000 km upwind from Andenes at Svalbard. During CAO events at Andenes, the sea-spray-mode number concentration is correlated with strong over-ocean winds with a mean of 8±4 cm −3 that is 71 % higher than during non-CAO conditions. Additionally, during CAO events at Andenes, the mean Hoppel minimum diameter is 6 nm smaller than during non-CAO conditions, though the estimated supersaturation is lower, and the mean number concentration of particles that likely activated in-cloud is 109±61 cm −3 with no statistically significant difference from the non-CAO mean of 99±66 cm −3 . For CAO trajectories between Zeppelin Observatory and Andenes, the upwind-to-downwind change in number concentration is the largest for the accumulation mode with a mean decrease of 93±95 cm −3 , likely attributable primarily to precipitation scavenging. These characteristic properties of aerosol number size distributions during CAO events provide guidance for evaluating CAO aerosol–cloud interaction processes in models.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS2024

Aerosol Size Distribution Properties Associated With Cold-Air Outbreaks in the Norwegian Arctic

The aerosol particles serving as cloud condensation and ice nuclei contribute to key cloud processes associated with cold-air outbreak (CAO) events but are poorly constrained in climate models due to sparse observations. Here we retrieve aerosol number size distribution modes from measurements at Andenes, Norway, during the Cold-Air Outbreaks in the Marine Boundary Layer Experiment (COMBLE) and at Zeppelin Observatory, approximately 1000 km upwind from Andenes at Svalbard. During CAO events at Andenes, the sea-spray-mode number concentration is correlated with strong over-ocean winds with a mean of 8±4 cm−3 that is 71 % higher than during non-CAO conditions. Additionally, during CAO events at Andenes, the mean Hoppel minimum diameter is 6 nm smaller than during non-CAO conditions, though the estimated supersaturation is lower, and the mean number concentration of particles that likely activated in-cloud is 109±61 cm−3 with no statistically significant difference from the non-CAO mean of 99±66 cm−3. For CAO trajectories between Zeppelin Observatory and Andenes, the upwind-to-downwind change in number concentration is the largest for the accumulation mode with a mean decrease of 93±95 cm−3, likely attributable primarily to precipitation scavenging. These characteristic properties of aerosol number size distributions during CAO events provide guidance for evaluating CAO aerosol–cloud interaction processes in models.

accumulation mode particle scavenging↗

DOE OSTI2015

Final Technical Report for Interagency Agreement No. DE-SC0005453 “Characterizing Aerosol Distributions, Types, and Optical and Microphysical Properties using the NASA Airborne High Spectral Resolution Lidar (HSRL) and the Research Scanning Polarimeter (RSP)”

Measurements of the vertical profile of atmospheric aerosols and aerosol optical and microphysical characteristics are required to: 1) determine aerosol direct and indirect radiative forcing, 2) compute radiative flux and heating rate profiles, 3) assess model simulations of aerosol distributions and types, and 4) establish the ability of surface and space-based remote sensors to measure the indirect effect. Consequently the ASR program calls for a combination of remote sensing and in situ measurements to determine aerosol properties and aerosol influences on clouds and radiation. As part of our previous DOE ASP project, we deployed the NASA Langley airborne High Spectral Resolution Lidar (HSRL) on the NASA B200 King Air aircraft during major field experiments in 2006 (MILAGRO and MaxTEX), 2007 (CHAPS), 2009 (RACORO), and 2010 (CalNex and CARES). The HSRL provided measurements of aerosol extinction (532 nm), backscatter (532 and 1064 nm), and depolarization (532 and 1064 nm). These measurements were typically made in close temporal and spatial coincidence with measurements made from DOE-funded and other participating aircraft and ground sites. On the RACORO, CARES, and CalNEX missions, we also deployed the NASA Goddard Institute for Space Studies (GISS) Research Scanning Polarimeter (RSP). RSP provided intensity and degree of linear polarization over a broad spectral and angular range enabling column-average retrievals of aerosol optical and microphysical properties. Under this project, we analyzed observations and model results from RACORO, CARES, and CalNex and accomplished the following objectives. 1. Identified aerosol types, characterize the vertical distribution of the aerosol types, and partition aerosol optical depth by type, for CARES and CalNex using HSRL data as we have done for previous missions. 2. Investigated aerosol microphysical and macrophysical properties using the RSP. 3. Used the aerosol backscatter and extinction profiles measured by the HSRL to characterize the planetary boundary layer height (PBL) and the transition zone thickness, for the RACORO and CARES and CalNex campaigns as we have done for previous campaigns. 4. Investigated how optical properties measured by HSRL vary near clouds. 5. Assessed model simulations of aerosol spatial distributions and optical and microphysical properties.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2018

Characteristics of Water Vapor Turbulence Profiles in Convective Boundary Layers During the Wet and Dry Seasons Over Darwin

This study explores water vapor turbulence in the convective boundary layer (CBL) using the Raman lidar observations the Atmospheric Radiation Measurement (ARM) site located at Darwin, Australia. These observations have temporal and vertical resolutions of 10 s and 37.5 m, respectively. An autocovariance technique has been used to separate out the random instrument error from the atmospheric variability during time periods when the CBL is cloud-free, quasi-stationary and well mixed. We identified 62 cases, comprising of 13 monsoon and 49 non-monsoon events, over the 5-year data record period. The seasonal variations of the vertical profiles of integral scale, variance, coefficient of the structure function, and skewness were analyzed and compared with similar observations from the Raman lidar at the ARM Southern Great Plains (SGP) site. The monsoon shows larger median variance profiles than the non-monsoon. The median profile of the variance from the non-monsoon and the SGP site are found to have similar magnitudes between 0.3-0.75 zi, while the median variance profile from the monsoon and the SGP are approximately the same between 0.9-1.1 zi. The variance and coefficient of the structure function are linearly related by height, with larger slopes in the monsoon season suggesting larger dissipation rates in that season relative to the non-monsoon. The median value in the skewness is mostly positive below 0.6 zi and above this it becomes negative until it crosses zero just below 1.0 zi. Its smallest value is seen at around 0.95 zi and it remains positive above 1.0 zi.

Osman, Mohammed K.↗

DOE OSTI2021

Radiosonde Observations of Environments Supporting Deep Moist Convection Initiation during RELAMPAGO-CACTI

The Remote Sensing of Electrification, Lightning, and Mesoscale/Microscale Processes with Adaptive Ground Observations (RELAMPAGO) and Cloud, Aerosol, and Complex Terrain Interactions (CACTI) projects deployed a high-spatiotemporal-resolution radiosonde network to examine environments supporting deep convection in the complex terrain of central Argentina. This study aims to characterize atmospheric profiles most representative of the near-cloud environment (in time and space) to identify the mesoscale ingredients affecting storm initiation and growth. Spatiotemporal autocorrelation analysis of the soundings reveals that there is considerable environmental heterogeneity, with boundary layer thermodynamic and kinematic fields becoming statistically uncorrelated on scales of 1–2 h and 30 km. Using this as guidance, we examine a variety of environmental parameters derived from soundings collected within close proximity (30 km in space and 30 min in time) of 44 events over 9 days where the atmosphere either: 1) supported the initiation of sustained precipitating convection, 2) yielded weak and short-lived precipitating convection, or 3) produced no precipitating convection in disagreement with numerical forecasts from convection-allowing models (i.e., Null events). There are large statistical differences between the Null event environments and those supporting any convective precipitation. Null event profiles contained larger convective available potential energy, but had low free-tropospheric relative humidity, higher freezing levels, and evidence of limited horizontal convergence near the terrain at low levels that likely suppressed deep convective growth. Here, we also present evidence from the radiosonde and satellite measurements that flow–terrain interactions may yield gravity wave activity that affects CI outcome.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS1971

Electronic research and technology requirements for marine resources

The Woods Hole air/space oceanographic program for 1969 is discussed. Studies included: (1) monitoring the sharp temperature boundary of the Gulf Stream by microwave and infrared observation, (2) spectrophotometry of the Gulf Stream and the adjacent continental slope and shelf water over Georges Bank, (3) interpretation of cloud and other meteorological data in terms of the effects of wind and sun on the upper ocean, (4) a sea state test plan, (5) systems research, and (6) ocean data recovery by aircraft and satellite.

Ewing, G. C.↗

NASA NTRS1973

Use of the SRI electronic satellite image analysis console for mapping southern Arizona plant communities from ERTS-1 imagery

Cloud-free imagery covering the Tucson, Ariz., region for the period from August 22 to November 2, 1972, was used to determine the utility of ERTS-1 data for discriminating boundaries between plant communities. The following studies were made from imagery analyzed by use of an Electronic Satellite Image Analysis Console: (1) console-generated color composites from MSS-5 and MSS-6 bands were recorded photographically from the console color monitor. The color photographs were then used to compare with short-term changes in vegetative cover observed on the ground; (2) using the console, microdensitometric traces were made along selected traverses to quantify changes in scene irradiance across the image field; (3) quantitative plant coverage data, collected at ground-truth stations along the traverses, were compared with the densitometric values.

Turner, R. M.↗

NASA NTRS1976

Empirical models of high latitude electric fields

Model cross sections of the high latitude dawn-dusk electric field based on OGO-6 data are presented for the signature profiles, most frequently encountered for both + and -Y orientations of the interplanetary magnetic field. Line integrals give a total potential of 76 keV in each case. To illustrate extremes, examples of model cross-sections with total potentials of 23 keV and 140 keV are also given. Model convection patterns are also presented utilizing OGO-6 data on boundary locations at other magnetic local times. When this information is combined with characteristic field geometries in the region of the Harang discontinuity, and is supplemented by data from Ba+ cloud motions in the polar cap, it becomes possible to construct realistic convection patterns on the nightside which deviate from the usual sun-aligned patterns. The observational models presented are of limited applicability as a consequence of the variability of observed distributions. These limitations are emphasized with particular attention given to several types of recurrent deviations which have not previously been discussed.

Heppner, J. P.↗

NASA NTRS1999

Climatic Implications of the Observed Temperature Dependence of the Liquid Water Path of Low Clouds

The uncertainty in the global climate sensitivity to an equilibrium doubling of carbon dioxide is often stated to be 1.5-4.5 K, largely due to uncertainties in cloud feedbacks. The lower end of this range is based on the assumption or prediction in some GCMs that cloud liquid water behaves adiabatically, thus implying that cloud optical thickness will increase in a warming climate if the physical thickness of clouds is invariant. Satellite observations of low-level cloud optical thickness and liquid water path have challenged this assumption, however, at low and middle latitudes. We attempt to explain the satellite results using four years of surface remote sensing data from the Atmospheric Radiation Measurements (ARM) Cloud And Radiation Testbed (CART) site in the Southern Great Plains. We find that low cloud liquid water path is insensitive to temperature in winter but strongly decreases with temperature in summer. The latter occurs because surface relative humidity decreases with warming, causing cloud base to rise and clouds to geometrically thin. Meanwhile, inferred liquid water contents hardly vary with temperature, suggesting entrainment depletion. Physically, the temperature dependence appears to represent a transition from higher probabilities of stratified boundary layers at cold temperatures to a higher incidence of convective boundary layers at warm temperatures. The combination of our results and the earlier satellite findings imply that the minimum climate sensitivity should be revised upward from 1.5 K.

DelGenio, Anthony↗

NASA NTRS1999

Synthesis of Large Molecules in Cometary Ice Analogs: Physical Properties Related to Self-Assembly Processes

The combination of realistic laboratory simulations and infrared observations have revolutionized our understanding of interstellar dust and ice-the main component of comets. Since comets and carbonaceous micrometeorites may have been important sources of volatiles and carbon compounds on the early Earth, their organic composition may be related to the origin of life. Ices on grains in molecular clouds contain a variety of simple molecules. The D/H ratios of the comets Hale-Bopp and Hyakutake are consistent with a primarily interstellar ice mixture. Within the cloud and especially in the presolar nebula through the early solar system, these icy grains would have been photoprocessed by the ultraviolet producing more complex species such as hexamethylenetetramine, polyoxymethylenes, and simple keones. We reported at the 1999 Bioastronomy meeting laboratory simulations studied to identify the types of molecules which could have been generated in pre-cometary ices. Experiments were conducted by forming a realistic interstellar mixed-molecular ice (H2O, CH3OH, NH3 and CO) at approximately 10 K under high vacuum irradiated with UV light from a hydrogen plasma lamp. The gas mixture was typically 100:50:1:1, however when different ratios were used material with similar characteristics was still produced. The residue that remained after warming to room temperature was analyzed by HPLC, and by several mass spectrometric methods. This material contains a rich mixture of complex compounds with mass spectral profiles resembling those found in IDPs and meteorites. Surface tension measurements show that an amphiphilic component is also present. These species do not appear in various controls or in unphotolyzed samples. Residues from the simulations were also dispersed in aqueous media for microscopy. The organic material forms 10-40 gm diameter droplets that fluoresce at 300-450 nm under UV excitation. These droplets have a morphology and internal structure which appear strikingly similar to those produced by extracts of the Murchison meteorite. Together, these results suggest a link between organic material photochemically synthesized on the cold grains in dense, interstellar molecular clouds and compounds that may have contributed to the organic inventory of the primitive Earth. For example, the amphiphilic properties of such compounds permit self-assembly into the membranous boundary structures that required for the first forms of cellular life.

Dworkin, Jason P.↗

NASA NTRS2004

The Liquid-Water Oscillation in Modeling Boundary-Layer Cumuli with Third-Order Turbulence Closure Models

A hierarchy of third-order turbulence closure models are used to simulate boundary-layer cumuli in this study. An unrealistically strong liquid-water oscillation (LWO) is found in the fully prognostic model, which predicts all third moments. The LWO propagates from cloud base to cloud top with a speed of 1 m/s. The period of the oscillation is about 1000 s. Liquid-water buoyancy terms in the third-moment equations contribute to the LWO. The LWO mainly affects the vertical profiles of cloud fraction, mean liquid-water mixing ratio and the fluxes of liquid-water potential temperature and total water, but has less impact on the vertical profiles of other second-moments and third-moments. In order to minimize the LWO, a moderate large diffusion coefficient and a large turbulent dissipation at its originating level are needed. However, this approach distorts the vertical distributions of cloud fraction and liquid-water mixing ratio. A better approach is to parameterize liquid-water buoyancy more reasonably. A minimally prognostic model, which diagnoses all third moments except for vertical velocity, is shown to produce better results, compared to a fully prognostic model.

Cheng, A.↗

DOE OSTI2021

Fine Aerosol Acidity and Water during Summer in the Eastern North Atlantic

Aerosol pH governs many important atmospheric processes that occur in the marine boundary layer, including regulating halogen and sulfur chemistries, and nutrient fertilization of surface ocean waters. In this study, we investigated the acidity of PM1 over the eastern North Atlantic during the Aerosol and Cloud Experiments in Eastern North Atlantic (ACE-ENA) aircraft campaign. The ISORROPIA-II thermodynamic model was used to predict PM1 pH and water. We first investigated the sensitivities of PM1 pH and water predictions to gas-phase NH3 and HNO3 concentrations. Our sensitivity analysis indicated that even though NH3 and HNO3 were present at very low concentrations in the eastern North Atlantic during the campaign, PM1 pH calculations can still be sensitive to NH3 concentrations. Specifically, NH3 was needed to constrain the pH of populations of PM1 that had low mass concentrations of NH4+ and non-volatile cations (NVCs). We next assumed that gas-phase NH3 and HNO3 concentrations during the campaign were 0.15 and 0.09 µg m−3, respectively, based on previous measurements conducted in the eastern North Atlantic. Using the assumption that PM1 were internally mixed (i.e., bulk PM1), we determined that PM1 pH ranged from 0.3–8.6, with a mean pH of 5.0 ± 2.3. The pH depended on both Hair+ and Wi. Hair+ was controlled primarily by the NVCs/SO42− molar ratio, while Wi was controlled by the SO42− mass concentration and RH. Changes in pH with altitude were driven primarily by changes in SO42−. Since aerosols in marine atmospheres are rarely internally mixed, the scenario where non-sea salt species and sea-salt species were present in two separate aerosol modes in the PM1 (i.e., completely externally mixed) was also considered. Smaller pH values were predicted for the aerosol mode comprised only of non-sea salt species compared to the bulk PM1 (difference of around 1 unit on average). This was due to the exclusion of sea-salt species (especially hygroscopic alkaline NVCs) in this aerosol mode, which led to increases in Hair+ values and decreases in Wi values. This result demonstrated that assumptions of aerosol mixing states can impact aerosol pH predictions substantially, which will have important implications for evaluating the nature and magnitude of pH-dependent atmospheric processes that occur in the marine boundary layer.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2025

Advancing Aerosol Chemical Characterization and Vertical Profiling over the Southern Great Plains Using Uncrewed Aerial Sampling and Offline Aerosol Mass Spectrometry

Recent advancements in uncrewed aerial systems (UASs) and particulate matter (PM) analytical techniques have provided opportunities for atmospheric research. In this study, we deployed the Department of Energy’s fixed-wing ArcticShark UAS to examine PM 2.5 composition at varying altitudes─within and above the planetary boundary layer (PBL)─over the Southern Great Plains atmospheric observatory (SGP). A total of 22 flights were conducted across March, June, and August 2023. Composite filter samples were collected during each flight and analyzed with offline aerosol mass spectrometry (AMS), complemented by on-board real-time sensors and ground-based instrumentation, to provide a comprehensive view of regional aerosol characteristics. Results show clear vertical and seasonal differences in the aerosol composition. Relative to ground-level measurements, aloft samples exhibited shifts in the distribution of organic and inorganic PM, with the organic composition varying distinctly across seasons. Particulate organic nitrogen (ON) was elevated, with bulk compositions similar in March and June but strongly altered in August, likely driven by biomass burning and enhanced photochemical activity. Combined AMS and chemical ionization mass spectrometry analyses detected amines, amides, and amino acids. PM above the planetary boundary layer was enriched in oxidized organic aerosols, while ground-level PM contained higher nitrate and sulfate. Seasonal differences in aqueous-phase processing were also observed, which were strongest in March during persistent cloud cover and weaker in the drier August period, suggesting a shift from aqueous- to gas-phase SOA formation. In conclusion, these findings highlight the value of UAS in advancing PM measurements and vertical profiling of aerosol composition.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS1984

Far-infrared sources in the vicinity of the supernova remnant W28

The W28 supernova remnant molecular cloud complex has been surveyed in the 40-250 micron spectral range with a three-sigma sensitivity of 100-165 Jy per beam. Only two sources have been found. One, located near the center of the SNR, has a luminosity of 54,000 solar luminosities and can be identified with the thermal radio source G6.6-0.1. The energizing source is probably an O-type ZAMS star. The second source, which is near the boundary of the SNR at a sharp gradient of OH absorption, has a luminosity of 6000 solar luminosities and has no radio counterpart. It is best explained as a B1 ZAMS star or a pre-main sequence object presumably formed from the impact of an expanding SNR with a molecular cloud. No far-IR emission is observed at the position of the CO molecular cloud, which seems to have been impacted by the SNR.

Odenwald, S. F.↗

DOE OSTI2024

The vertical-velocity skewness in the atmospheric boundary layer without buoyancy and Coriolis effects

One of the main features of near-neutral atmospheric boundary layer (ABL) turbulence is the positive vertical velocity skewness $Sk_w$ above the roughness sublayer or the buffer region in smooth-walls. The $Sk_w$ variations are receiving renewed interest in many climate-related parameterizations of the ABL given their significance to cloud formation and to testing sub-grid schemes for Large Eddy Simulations (LES). The vertical variations of $Sk_w$ are explored here using wind tunnel and flume experiments collected above smooth, rough, and permeable-walls in the absence of buoyancy and Coriolis effects. These laboratory experiments form a necessary starting point to probe the canonical structure of $Sk_w$ as they deal with a key limiting case (i.e., near-neutral conditions). Diagnostic models based on cumulant expansions, realizability constraints, and constant mass flux approach routinely employed in the convective boundary layer as well as prognostic models based on third-order budgets are used to explain variations in $Sk_w$ for the idealized laboratory conditions. The failure of flux-gradient relations to model $Sk_w$ from the gradients of the vertical velocity variance σ$_w^2$ are explained and corrections based on models of energy transport offered. Novel links between the diagnostic and prognostic models are also featured, especially for the inertial term in the third-order budget of the vertical velocity fluctuation. The co-spectral properties of w′/σ w vs w′ 2 /σ$_w^2$ are also presented for the first time to assess the dominant scales governing $Sk_w$ in the inner and outer layers, where w′ is the fluctuating vertical velocity and σ w is the vertical velocity standard deviation.>

Boundary layer flow↗

DOE OSTI2023

Biomass-burning smoke's properties and its interactions with marine stratocumulus clouds in WRF-CAM5 and southeastern Atlantic field campaigns

Abstract. A large part of the uncertainty in climate projections comes from uncertain aerosol properties and aerosol–cloud interactions as well as the difficulty in remotely sensing them. The southeastern Atlantic functions as a natural laboratory to study biomass-burning smoke and to constrain this uncertainty. We address these gaps by comparing the Weather Research and Forecasting with Chemistry Community Atmosphere Model (WRF-CAM5) to the multi-campaign observations ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS), CLARIFY (CLoud–Aerosol–Radiation Interaction and Forcing), and LASIC (Layered Atlantic Smoke Interactions with Clouds) in the southeastern Atlantic in August 2017 to evaluate a large range of the model's aerosol chemical properties, size distributions, processes, and transport, as well as aerosol–cloud interactions. Overall, while WRF-CAM5 is able to represent smoke properties and transport, some key discrepancies highlight the need for further analysis. Observations of smoke composition show an overall decrease in aerosol mean diameter as smoke ages over 4–12 d, while the model lacks this trend. A decrease in the mass ratio of organic aerosol (OA) to black carbon (BC), OA:BC, and the OA mass to carbon monoxide (CO) mixing ratio, OA:CO, suggests that the model is missing processes that selectively remove OA from the particle phase, such as photolysis and heterogeneous aerosol chemistry. A large (factor of ∼2.5) enhancement in sulfate from the free troposphere (FT) to the boundary layer (BL) in observations is not present in the model, pointing to the importance of properly representing secondary sulfate aerosol formation from marine dimethyl sulfide and gaseous SO2 smoke emissions. The model shows a persistent overprediction of aerosols in the marine boundary layer (MBL), especially for clean conditions, which multiple pieces of evidence link to weaker aerosol removal in the modeled MBL than reality. This evidence includes several model features, such as not representing observed shifts towards smaller aerosol diameters, inaccurate concentration ratios of carbon monoxide and black carbon, underprediction of heavy rain events, and little evidence of persistent biases in modeled entrainment. The average below-cloud aerosol activation fraction (NCLD/NAER) remains relatively constant in WRF-CAM5 between field campaigns (∼0.65), while it decreases substantially in observations from ORACLES (∼0.78) to CLARIFY (∼0.5), which could be due to the model misrepresentation of clean aerosol conditions. WRF-CAM5 also overshoots an observed upper limit on liquid cloud droplet concentration around NCLD= 400–500 cm−3 and overpredicts the spread in NCLD. This could be related to the model often drastically overestimating the strength of boundary layer vertical turbulence by up to a factor of 10. We expect these results to motivate similar evaluations of other modeling systems and promote model development to reduce critical uncertainties in climate simulations.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS1999

Seasonal and Interannual Variabilities in Tropical Tropospheric Ozone

This paper presents a detailed characterization of seasonal and interannual variability in tropical tropospheric column ozone (TCO). TCO time series are derived from 20 years (1979-1998) of total ozone mapping spectrometer (TOMS) data using the convective cloud differential (CCD) method. Our study identifies three regions in the tropics with distinctly different zonal characteristics related to seasonal and interannual variability. These three regions are the eastern Pacific, Atlantic, and western Pacific. Results show that in both the eastern and western Pacific seasonal-cycle variability of northern hemisphere (NH) TCO exhibits maximum amount during NH spring whereas largest amount in southern hemisphere (SH) TCO occurs during SH spring. In the Atlantic, maximum TCO in both hemispheres occurs in SH spring. These seasonal cycles are shown to be comparable to seasonal cycles present in ground-based ozonesonde measurements. Interannual variability in the Atlantic region indicates a quasi-biennial oscillation (QBO) signal that is out of phase with the QBO present in stratospheric column ozone (SCO). This is consistent with high pollution and high concentrations of mid-to-upper tropospheric O3-producing precursors in this region. The out of phase relation suggests a UV modulation of tropospheric photochemistry caused by the QBO in stratospheric O3. During El Nino events there is anomalously low TCO in the eastern Pacific and high values in the western Pacific, indicating the effects of convectively-driven transport of low-value boundary layer O3 (reducing TCO) and O3 precursors including H2O and OH. A simplified technique is proposed to derive high-resolution maps of TCO in the tropics even in the absence of tropopause-level clouds. This promising approach requires only total ozone gridded measurements and utilizes the small variability observed in TCO near the dateline. This technique has an advantage compared to the CCD method because the latter requires high-resolution footprint measurements of both reflectivity and total ozone in the presence of tropopause-level cloud tops.

Ziemke, J. R.↗