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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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All sourcesNASA NTRSDOE OSTI
NASA NTRS1991

GLObal Backscatter Experiment (GLOBE) Pacific survey mission

NASA conducted the GLObal Backscatter Experiment (GLOBE) Survey Mission over the near coastal and remote Pacific Ocean during 6 to 30 Nov. 1989 (GLOBE 1) and 13 May to 5 Jun. 1990 (GLOBE 2). These missions studied the optical, physical, and chemical properties of atmospheric aerosols. Particular emphasis was given to the magnitude and spatial variability of aerosol backscatter coefficients at mid-infrared wavelengths, and to the remote middle and upper troposphere, where these aerosol properties are poorly understood. Survey instruments were selected to provide either direct beta measurements at the key wavelengths, empirical links with long term or global scale aerosol climatologies, or aerosol microphysics data required to model any of these quantities. The survey deployment included both long distance 6 to 8 hour transit flights and detailed 4 to 6 hour local flights. Several general features were observed from preliminary Survey data analyses. Validation and intercomparison results have shown good agreement, usually better than a factor of two. Atmospheric aerosols frequently exhibited a three layer vertical structure, with (1) high and fairly uniform backscatter in the shallow cloud capped marine boundary layer; (2) moderate and highly variable backscatter in a deeper overlaying cloud pumped layer; and (3) low, regionally uniform, but seasonally and latitudinally variable backscatter in the middle and upper troposphere. The survey missions represent two isolated snapshots of a small portion of the global aerosol system. Consequently, Survey results can best be understood by synthesizing them with the more comprehensive GLOBE data base, which is being compiled at NASA-Marshall.

Bowdle, David A.↗
NASA NTRS2012

Sensitivity of Marine Warm Cloud Retrieval Statistics to Algorithm Choices: Examples from MODIS Collection 6

The optical and microphysical structure of warm boundary layer marine clouds is of fundamental importance for understanding a variety of cloud radiation and precipitation processes. With the advent of MODIS (Moderate Resolution Imaging Spectroradiometer) on the NASA EOS Terra and Aqua platforms, simultaneous global/daily 1km retrievals of cloud optical thickness and effective particle size are provided, as well as the derived water path. In addition, the cloud product (MOD06/MYD06 for MODIS Terra and Aqua, respectively) provides separate effective radii results using the l.6, 2.1, and 3.7 ~m spectral channels. Cloud retrieval statistics are highly sensitive to how a pixel identified as being "notclear" by a cloud mask (e.g., the MOD35/MYD35 product) is determined to be useful for an optical retrieval based on a 1-D cloud model. The Collection 5 MODIS retrieval algorithm removed pixels associated with cloud'edges as well as ocean pixels with partly cloudy elements in the 250m MODIS cloud mask - part of the so-called Clear Sky Restoral (CSR) algorithm. Collection 6 attempts retrievals for those two pixel populations, but allows a user to isolate or filter out the populations via CSR pixel-level Quality Assessment (QA) assignments. In this paper, using the preliminary Collection 6 MOD06 product, we present global and regional statistical results of marine warm cloud retrieval sensitivities to the cloud edge and 250m partly cloudy pixel populations. As expected, retrievals for these pixels are generally consistent with a breakdown of the ID cloud model. While optical thickness for these suspect pixel populations may have some utility for radiative studies, the retrievals should be used with extreme caution for process and microphysical studies.

Platnick, Steven↗
NASA NTRS1990

Thermal advection and stratification effects on surface winds and the low level meridional mass transport

Statistical tests are performed on the Seasat scatterometer observations to examine if and to what degree thermal advection and stratification effects manifest themselves in these remotely sensed measurements of mean wind and wind stress over the ocean. On the basis of a two layer baroclinic boundary layer model which is presented, it is shown that the thermal advection and stratification of the entire boundary layer as well as the geostrophic forcing influence the modeled near surface wind and wind stress profiles. Evidence of diurnal variation in the stratification under barotropic conditions is found in the data, with the daytime marine boundary layer being more convective than its nighttime counterpart. The temporal and spacial sampling pattern of the satellite makes it impossible to recover the full diurnal cycle, however. The observed effects of the thermal advection are shown to be statistically significant during the day (and presumed more convective) hours, causing a systematic increase in the poleward transport of mass and heat. The statistical results are in a qualitative agreement with the model simulations and cannot be reproduced in randomized control tests.

Levy, Gad↗
NASA NTRSDate not supplied

Remote Marine Aerosol Properties over the Western North Atlantic Ocean during NAAMES

The overarching goal of this postdoctoral project is: quantitatively assess and constrain the aerosol budgets in the remote North Atlantic marine boundary layer, under a wide range of aerosol emission sources, meteorological states to improve process-level understanding of marine aerosol-cloud interactions critical to adequately link observations and climate modelling.

Aerosol NAAMES↗
NASA NTRS2015

Three-Dimensional Distribution of a Major Desert Dust Outbreak over East Asia in March 2008 Derived from IASI Satellite Observations

We describe the daily evolution of the three-dimensional (3D) structure of a major dust outbreak initiated by an extratropical cyclone over East Asia in early March 2008, using new aerosol retrievals derived from satellite observations of IASI (Infrared Atmospheric Sounding Interferometer). A novel auto-adaptive Tikhonov-Phillips-type approach called AEROIASI is used to retrieve vertical profiles of dust extinction coefficient at 10 microns for most cloud-free IASI pixels, both over land and ocean. The dust vertical distribution derived from AEROIASI is shown to agree remarkably well with along-track transects of Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) spaceborne lidar vertical profiles (mean biases less than 110 meters, correlation of 0.95, and precision of 260 meters for mean altitudes of the dust layers). AEROIASI allows the daily characterization of the 3D transport pathways across East Asia of two dust plumes originating from the Gobi and North Chinese deserts. From AEROIASI retrievals, we provide evidence that (i) both dust plumes are transported over the Beijing region and the Yellow Sea as elevated layers above a shallow boundary layer, (ii) as they progress eastward, the dust layers are lifted up by the ascending motions near the core of the extratropical cyclone, and (iii) when being transported over the warm waters of the Japan Sea, turbulent mixing in the deep marine boundary layer leads to high dust concentrations down to the surface. AEROIASI observations and model simulations also show that the progression of the dust plumes across East Asia is tightly related to the advancing cold front of the extratropical cyclone.

Cuesta, Juan↗
NASA NTRS1987

Measurements of nitric oxide in the boundary layer and free troposphere over the Pacific Ocean

Measurements of NO and O3 are presented from 13 aircraft flights made over the Pacific Ocean in the autumn of 1983 during one phase of the NASA Global Tropospheric Experiment. All of the flights were made between 15 deg and 42 deg N and from the coast of California to west of the Hawaiian Islands. Within the upper marine boundary layer the median daytime mixing ratio of NO was near 1 part per trillion by volume (pptv). Values of NO less than 10 pptv were often observed up to altitudes near 6 km. Thus for the location and season of the measurements, a net photochemical destruction of O3 would be anticipated for the boundary layer region and to altitudes of 2-3 km. At higher altitudes of 7-11 km in the free troposphere, larger mixing ratios and greater variability were usually observed for NO. Both features are consistent with observed examples of injection of NO and O3 from the lower stratosphere and with the injection of NO from towering, electrically active, cumulonimbus clouds.

Ridley, B. A.↗
NASA NTRS2008

Modeling the Impact of Drizzle and 3D Cloud Structure on Remote Sensing of Effective Radius

Remote sensing of cloud particle size with passive sensors like MODIS is an important tool for cloud microphysical studies. As a measure of the radiatively relevant droplet size, effective radius can be retrieved with different combinations of visible through shortwave infrared channels. MODIS observations sometimes show significantly larger effective radii in marine boundary layer cloud fields derived from the 1.6 and 2.1 pm channel observations than for 3.7 pm retrievals. Possible explanations range from 3D radiative transport effects and sub-pixel cloud inhomogeneity to the impact of drizzle formation on the droplet distribution. To investigate the potential influence of these factors, we use LES boundary layer cloud simulations in combination with 3D Monte Carlo simulations of MODIS observations. LES simulations of warm cloud spectral microphysics for cases of marine stratus and broken stratocumulus, each for two different values of cloud condensation nuclei density, produce cloud structures comprising droplet size distributions with and without drizzle size drops. In this study, synthetic MODIS observations generated from 3D radiative transport simulations that consider the full droplet size distribution will be generated for each scene. The operational MODIS effective radius retrievals will then be applied to the simulated reflectances and the results compared with the LES microphysics.

Platnick, Steven↗
DOE OSTI2023

Observations of Offshore Internal Boundary Layers

The growth of the marine internal boundary layer (MIBL, height h i ) with the shore-normal distance x, is a topic of continuing interest because of its applications in coastal dispersion, offshore wind farm siting, coastal air-sea fluxes and in evaporative ducting. Available data on MIBL are only scarce, given its difficult to measure the variability of coastal winds. During Coupled Air-Sea Processes and Electromagnetic Research (CASPER) campaigns an array of instrumentation was deployed to measure offshore spatial variability and its effect on electromagnetic wave propagation. Meteorological sensors (flux towers and remote sensing) were deployed along the coast of Point Mugu, California, on a research vessel and FLoating Instrument Platform (FLIP) provided surface layer and boundary layer observations. In this article, measurements from multiple remote sensing instruments, such as synchronized triple Doppler lidars, small boat operations with tethered lifting system, and radiosondes provide a holistic view of the MIBL growth and its spatial variability from the coast. A convective and stable MIBL observed during two intensive operating period days showed distinct growth characteristics off the coast of Point-Mugu. During stable stratified atmospheric conditions, an MIBL was observed at least up to 47 km from the coast. The growth of the MIBL within the nearshore adjustment zone was influenced by surrounding atmospheric, oceanographic, and topographic conditions. A new parameterization scheme is developed based on advection-diffusion balance equations accounting for upstream turbulence and compared with h i observations from Doppler lidar and profiles from small boat. An evaluation of existing IBL theories was also conducted.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Indirect Measurements of the Composition of Ultrafine Particles in the Arctic Late-Winter

In this work, we present indirect measurements of size-resolved ultrafine particle composition conducted during the Ocean-Atmosphere-Sea Ice-Snowpack (OASIS) Campaign in Utqiagvik, Alaska, during March 2009. This study focuses on measurements of size-resolved particle hygroscopicity and volatility measured over two periods of the campaign. During a period that represents background conditions in this location, particle hygroscopic growth factors (HGF) at 90% relative humidity ranged from 1.45 to 1.51, which combined with volatility measurements suggest a mixture of ~30% ammoniated sulfates and ~70% oxidized organics. Two separate regional ultrafine particle growth events were also observed during this campaign. Event 1 coincided with elevated levels of H2SO4 and solar radiation. These particles were highly hygroscopic (HGF = 2.1 for 35 nm particles), but were almost fully volatilized at 160 °C. The air masses associated with both events originated over the Arctic Ocean. Event 1 was influenced by the upper marine boundary layer (200–350 m AGL), while Event 2 spent more time closer to the surface (50–150 m AGL) and over open ocean leads, suggesting marine influence in growth processes. Event 2 particles were slightly less hygroscopic (HGF = 1.94 for 35 nm and 1.67 for 15 nm particles), and similarly volatile. We hypothesize that particles formed during both events contained 60–70% hygroscopic salts by volume, with the balance for Event 1 being sulfates and oxidized organics for Event 2. These observations suggest that primary sea spray may be an important initiator of ultrafine particle formation events in the Arctic late-winter, but a variety of processes may be responsible for condensational growth.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS2003

Column Closure Studies of Lower Tropospheric Aerosol and Water Vapor During ACE-Asia Using Airborne Sunphotometer, Airborne In-Situ and Ship-Based Lidar Measurements

We assess the consistency (closure) between solar beam attenuation by aerosols and water vapor measured by airborne sunphotometry and derived from airborne in-situ, and ship-based lidar measurements during the April 2001 Asian Pacific Regional Aerosol Characterization Experiment (ACE-Asia). The airborne data presented here were obtained aboard the Twin Otter aircraft. Comparing aerosol extinction o(550 nm) from four different techniques shows good agreement for the vertical distribution of aerosol layers. However, the level of agreement in absolute magnitude of the derived aerosol extinction varied among the aerosol layers sampled. The sigma(550 nm) computed from airborne in-situ size distribution and composition measurements shows good agreement with airborne sunphotometry in the marine boundary layer but is considerably lower in layers dominated by dust if the particles are assumed to be spherical. The sigma(550 nm) from airborne in-situ scattering and absorption measurements are about approx. 13% lower than those obtained from airborne sunphotometry during 14 vertical profiles. Combining lidar and the airborne sunphotometer measurements reveals the prevalence of dust layers at altitudes up to 10 km with layer aerosol optical depth (from 3.5 to 10 km altitude) of approx. 0.1 to 0.2 (500 nm) and extinction-to-backscatter ratios of 59-71 sr (523 nm). The airborne sunphotometer aboard the Twin Otter reveals a relatively dry atmosphere during ACE- Asia with all water vapor columns less than 1.5 cm and water vapor densities w less than 12 g/cu m. Comparing layer water vapor amounts and w from the airborne sunphotometer to the same quantities measured with aircraft in-situ sensors leads to a high correlation (r(sup 3)=0.96) but the sunphotometer tends to underestimate w by 7%.

Schmid, B.↗
DOE OSTI2023

Natural marine cloud brightening in the Southern Ocean

Abstract. The number of cloud droplets per unit volume (Nd) is a fundamentally important property of marine boundary layer (MBL) liquid clouds that, at constant liquid water path, exerts considerable controls on albedo. Past work has shown that regional Nd has a direct correlation to marine primary productivity (PP) because of the role of seasonally varying, biogenically derived precursor gases in modulating secondary aerosol properties. These linkages are thought to be observable over the high-latitude oceans, where strong seasonal variability in aerosol and meteorology covary in mostly pristine environments. Here, we examine Nd variability derived from 5 years of MODIS Level 2-derived cloud properties in a broad region of the summer eastern Southern Ocean and adjacent marginal seas. We demonstrate latitudinal, longitudinal and temporal gradients in Nd that are strongly correlated with the passage of air masses over high-PP waters that are mostly concentrated along the Antarctic Shelf poleward of 60∘ S. We find that the albedo of MBL clouds in the latitudes south of 60∘ S is significantly higher than similar liquid water path (LWP) clouds north of this latitude.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS2002

In-Situ Measurements of HCN and CH3CN in the Pacific Troposphere: Sources, Sinks, and Comparisons with Spectroscopic Observations

We report the first in-situ measurements of hydrogen cyanide (HCN) and acetonitrile (CH3CN) from the Pacific troposphere (0-12 km) obtained during the NASA/Trace-P mission (Feb.-April, 2001). Mean HCN and CH3CN mixing ratios of 243 (+/-118) ppt and 149 (+/-56) ppt respectively, were measured. The in-situ observations correspond to a total HCN column of 4.4-4.9 x 10(exp 15) molec. cm(exp -2) and a CH3CN column of 2.8-3.0 x 10(exp 15) molec. cm(exp -2). This HCN column is in good agreement with available spectroscopic observations. The atmospheric concentrations of HCN and CH3CN were greatly influenced by outflow of pollution from Asia. There is a linear relationship between the mixing ratios of HCN and CH3CN, and in turn these are well correlated with tracers of biomass combustion (e.g. CH3Cl, CO). Relative enhancements with respect to known tracers of biomass combustion within selected plumes in the free troposphere, and pollution episodes in the boundary layer allow an estimation of a global biomass burning source of 0.8+/-0.4 Tg (N)/y for HCN and 0.4+/-0.1 Tg (N)/y for CH3CN. In comparison, emissions from automobiles and industry are quite small (<0.05 Tg (N)/y). The vertical structure of HCN and CH3CN indicated reduced mixing ratios in the MBL (Marine Boundary Layer). Using, a simple box model, the observed gradients across the top of the MBL are used to derive an oceanic flux of 6.7 x 10(exp -15) g (N) cm(exp -2)/s for HCN and 4.8 x 10(exp -15) g (N) cm(exp -2)/s for CH3CN. An air-sea exchange model is used to conclude that this flux can be maintained if the oceans are under-saturated in HCN and CH3CN by 23% and 17%, respectively. It is inferred that oceanic loss is a dominant sink for these nitrites, and they deposit some 1.3 Tg (N) of nitrogen annually to the oceans. Assuming reaction with OH radicals and loss to the oceans as the major removal processes, a mean atmospheric residence time of 4.7 months for HCN and 5.1 months for CH3CN is calculated. A global budget analysis shows that the sources and sinks of HCN and CH3CN are roughly in balance. There are indications that biogenic sources may also be present. Mechanisms involved in nitrate formation during combustion and removal in the oceans are poorly understood.

Singh, Hanwant B.↗
NASA NTRS2002

Linking Horizontal And Vertical Transports of Biomass Fire Emissions to the Tropical Atlantic Ozone Paradox during the Northern Hemisphere Winter Season: II. 1998-1999.

The horizontal and vertical transport of biomass fire emissions in West Africa during November 1998 through February 1999, are examined using all available data including wind, fire, aerosol, precipitation, lightning and outgoing longwave radiation. Ozonesonde data from the Aerosols99 Trans-Atlantic cruise are also included with rain and wind analyses. The results here support earlier studies that ozone and ozone precursors associated with biomass burning are confined to the lower troposphere primarily due to the lack of deep convection over land areas. Ozone and its precursors are horizontally transported equatorward or towards the west by winds in the 1000-700 hPa layers. However, rising adiabatic motions associated with the diurnal evolution of the West African n can transport ozone and its precursors vertically into the free troposphere above the marine boundary layer. Moreover, lightning from South America, Central Africa and mesoscale convective systems in the Gulf of Guinea can lead to elevated ozone mixing ratios in the middle and upper troposphere.

Jenkins, Gregory S.↗
NASA NTRS2014

Assessment of NASA GISS CMIP5 and Post-CMIP5 Simulated Clouds and TOA Radiation Budgets Using Satellite Observations. Part I: Cloud Fraction and Properties

Although many improvements have been made in phase 5 of the Coupled Model Intercomparison Project (CMIP5), clouds remain a significant source of uncertainty in general circulation models (GCMs) because their structural and optical properties are strongly dependent upon interactions between aerosol/cloud microphysics and dynamics that are unresolved in such models. Recent changes to the planetary boundary layer (PBL) turbulence and moist convection parameterizations in the NASA GISS Model E2 atmospheric GCM(post-CMIP5, hereafter P5) have improved cloud simulations significantly compared to its CMIP5 (hereafter C5) predecessor. A study has been performed to evaluate these changes between the P5 and C5 versions of the GCM, both of which used prescribed sea surface temperatures. P5 and C5 simulated cloud fraction (CF), liquid water path (LWP), ice water path (IWP), cloud water path (CWP), precipitable water vapor (PWV), and relative humidity (RH) have been compared to multiple satellite observations including the Clouds and the Earth's Radiant Energy System-Moderate Resolution Imaging Spectroradiometer (CERES-MODIS, hereafter CM), CloudSat- Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO; hereafter CC), Atmospheric Infrared Sounder (AIRS), and Advanced Microwave Scanning Radiometer for Earth Observing System (AMSR-E). Although some improvements are observed in the P5 simulation on a global scale, large improvements have been found over the southern midlatitudes (SMLs), where correlations increased and both bias and root-mean-square error (RMSE) significantly decreased, in relation to the previous C5 simulation, when compared to observations. Changes to the PBL scheme have resulted in improved total column CFs, particularly over the SMLs where marine boundary layer (MBL) CFs have increased by nearly 20% relative to the previous C5 simulation. Globally, the P5 simulated CWPs are 25 gm22 lower than the previous C5 results. The P5 version of the GCM simulates PWV and RH higher than its C5 counterpart and agrees well with the AMSR-E and AIRS observations. The moister atmospheric conditions simulated by P5 are consistent with the CF comparison and provide a strong support for the increase in MBL clouds over the SMLs. Over the tropics, the P5 version of the GCM simulated total column CFs and CWPs are slightly lower than the previous C5 results, primarily as a result of the shallower tropical boundary layer in P5 relative to C5 in regions outside the marine stratocumulus decks.

General circulation models↗
NASA NTRS2017

BrO and Inferred Bry Profiles over the Western Pacific: Relevance of Inorganic Bromine Sources and a Bry Minimum in the Aged Tropical Tropopause Layer

We report measurements of bromine monoxide (BrO) and use an observationally constrained chemical box model to infer total gas-phase inorganic bromine (Br(sub y)) over the tropical western Pacific Ocean (tWPO) during the CONTRAST field campaign (January-February 2014). The observed BrO and inferred Bry profiles peak in the marine boundary layer (MBL), suggesting the need for a bromine source from sea-salt aerosol (SSA), in addition to organic bromine (CBry ). Both profiles are found to be C-shaped with local maxima in the upper free troposphere (FT). The median tropospheric BrO vertical column density (VCD) was measured as 1.6 x 10(exp 13) molec cm(exp -2), compared to model predictions of 0.9 x 10(exp 13) molec cm(exp -2) in GEOS-Chem (CBr(sub y) but no SSA source), 0.4 x 10(exp 13) molec cm(exp -2) in CAM-Chem (CBr(sub y) and SSA), and 2.1 x 10(exp 13) molec cm(exp -2) in GEOS-Chem (CBry and SSA). Neither global model fully captures the Cshape of the Br(sun y) profile. A local Br(sub y) maximum of 3.6 ppt (2.9-4.4 ppt; 95% confidence interval, CI) is inferred between 9.5 and 13.5 km in air masses influenced by recent convective outflow. Unlike BrO, which increases from the convective tropical tropopause layer (TTL) to the aged TTL, gas-phase Br(sub y) decreases from the convective TTL to the aged TTL. Analysis of gas-phase Br(sub y) against multiple tracers (CFC-11, H2O/O3 ratio, and potential temperature) reveals a Br(sub y) minimum of 2.7 ppt (2.3-3.1 ppt; 95% CI) in the aged TTL, which agrees closely with a stratospheric injection of 2.6 +/- 0.6 ppt of inorganic Br(sub y) (estimated from CFC-11 correlations), and is remarkably insensitive to assumptions about heterogeneous chemistry. Bry increases to 6.3 ppt (5.6-7.0 ppt; 95% CI) in the stratospheric "middleworld" and 6.9 ppt (6.5-7.3 ppt; 95% CI) in the stratospheric "overworld". The local Br(sub y) minimum in the aged TTL is qualitatively (but not quantitatively) captured by CAM-Chem, and suggests a more complex partitioning of gas-phase and aerosol Br(sub y) species than previously recognized. Our data provide corroborating evidence that inorganic bromine sources (e.g., SSA-derived gas-phase Br(sub y) ) are needed to explain the gas-phase Br(sub y) budget in the upper free troposphere and TTL. They are also consistent with observations of significant bromide in Upper Troposphere-Lower Stratosphere aerosols. The total Br(sub y) budget in the TTL is currently not closed, because of the lack of concurrent quantitative measurements of gas-phase Br(sub y) species (i.e., BrO, HOBr, HBr, etc.) and aerosol bromide. Such simultaneous measurements are needed to (1) quantify SSA-derived Br(sub y) in the upper FT, (2) test Br(sub y) partitioning, and possibly explain the gas-phase Br(sub y) minimum in the aged TTL, (3) constrain heterogeneous reaction rates of bromine, and (4) account for all of the sources of Br(sub y) to the lower stratosphere.

Atmospheric Chemistry; bromine; troposphere; CONTR↗
DOE OSTI2022

Cloud adjustments from large-scale smoke–circulation interactions strongly modulate the southeastern Atlantic stratocumulus-to-cumulus transition

Smoke from southern Africa blankets the southeastern Atlantic Ocean from June to October, producing strong and competing aerosol radiative effects. Smoke effects on the transition between overcast stratocumulus and scattered cumulus clouds are investigated along a Lagrangian (air-mass-following) trajectory in regional climate and large eddy simulation models. Results are compared with observations from three recent field campaigns that took place in August 2017: ObseRvations of Aerosols above CLouds and their intEractionS (ORACLES), CLouds and Aerosol Radiative Impacts and Forcing: Year 2017 (CLARIFY), and Layered Atlantic Smoke Interactions with Clouds (LASIC). The case study is set up around the joint ORACLES–CLARIFY flight that took place near Ascension Island on 18 August 2017. Smoke sampled upstream on an ORACLES flight on 15 August 2017 likely entrained into the marine boundary layer later sampled during the joint flight. The case is first simulated with the WRF-CAM5 regional climate model in three distinct setups: (1) FireOn, in which smoke emissions and any resulting smoke–cloud–radiation interactions are included; (2) FireOff, in which no smoke emissions are included; (3) RadOff, in which smoke emissions and their microphysical effects are included but aerosol does not interact directly with radiation. Over the course of the Lagrangian trajectory, differences in free tropospheric thermodynamic properties between FireOn and FireOff are nearly identical to those between FireOn and RadOff, showing that aerosol–radiation interactions are primarily responsible for the free tropospheric effects. These effects are non-intuitive: in addition to the expected heating within the core of the smoke plume, there is also a “banding” effect of cooler temperature (~1–2 K) and greatly enhanced moisture (>2 g kg -1 ) at the plume top. This banding effect is caused by a vertical displacement of the former continental boundary layer in the free troposphere in the FireOn simulation resulting from anomalous diabatic heating due to smoke absorption of sunlight that manifests primarily as a few hundred meters per day reduction in large-scale subsidence over the ocean. A large eddy simulation (LES) is then forced with free tropospheric fields taken from the outputs for the WRF-CAM5 FireOn and FireOff runs. Cases are run by selectively perturbing one variable (e.g., aerosol number concentration, temperature, moisture, vertical velocity) at a time to better understand the contributions from different indirect (microphysical), “large-scale” semi-direct (above-cloud thermodynamic and subsidence changes), and “local” semi-direct (below-cloud smoke absorption) effects. Despite a more than 5-fold increase in cloud droplet number concentration when including smoke aerosol concentrations, minimal differences in cloud fraction evolution are simulated by the LES when comparing the base case with a perturbed aerosol case with identical thermodynamic and dynamic forcings. A factor of 2 decrease in background free tropospheric aerosol concentrations from the FireOff simulation shifts the cloud evolution from a classical entrainment-driven “deepening–warming” transition to trade cumulus to a precipitation-driven “drizzle-depletion” transition to open cells, however. The thermodynamic and dynamic changes caused by the WRF-simulated large-scale adjustments to smoke diabatic heating strongly influence cloud evolution in terms of both the rate of deepening (especially for changes in the inversion temperature jump and in subsidence) and in cloud fraction on the final day of the simulation (especially for the moisture “banding” effect). Such large-scale semi-direct effects would not have been possible to simulate using a small-domain LES model alone.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS2022

Cloud Adjustments From Large-Scale Smoke–Circulation Interactions Strongly Modulate the Southeastern Atlantic Stratocumulus-to-Cumulus Transition

Smoke from southern Africa blankets the southeastern Atlantic Ocean from June to October, producing strong and competing aerosol radiative effects. Smoke effects on the transition between overcast stratocumulus and scattered cumulus clouds are investigated along a Lagrangian (air-mass-following) trajectory in regional climate and large eddy simulation models. Results are compared with observations from three recent field campaigns that took place in August 2017: ObseRvations of Aerosols above CLouds and their intEractionS (ORACLES), CLouds and Aerosol Radiative Impacts and Forcing: Year 2017 (CLARIFY), and Layered Atlantic Smoke Interactions with Clouds (LASIC). The case study is set up around the joint ORACLES–CLARIFY flight that took place near Ascension Island on 18 August 2017. Smoke sampled upstream on an ORACLES flight on 15 August 2017 likely entrained into the marine boundary layer later sampled during the joint flight. The case is first simulated with the WRF-CAM5 regional climate model in three distinct setups: (1) FireOn, in which smoke emissions and any resulting smoke–cloud–radiation interactions are included; (2) FireOff, in which no smoke emissions are included; (3) RadOff, in which smoke emissions and their microphysical effects are included but aerosol does not interact directly with radiation. Over the course of the Lagrangian trajectory, differences in free tropospheric thermodynamic properties between FireOn and FireOff are nearly identical to those between FireOn and RadOff, showing that aerosol–radiation interactions are primarily responsible for the free tropospheric effects. These effects are non-intuitive: in addition to the expected heating within the core of the smoke plume, there is also a “banding” effect of cooler temperature (∼1–2 K) and greatly enhanced moisture (>2 g kg−1) at the plume top. This banding effect is caused by a vertical displacement of the former continental boundary layer in the free troposphere in the FireOn simulation resulting from anomalous diabatic heating due to smoke absorption of sunlight that manifests primarily as a few hundred meters per day reduction in large-scale subsidence over the ocean. A large eddy simulation (LES) is then forced with free tropospheric fields taken from the outputs for the WRF-CAM5 FireOn and FireOff runs. Cases are run by selectively perturbing one variable (e.g., aerosol number concentration, temperature, moisture, vertical velocity) at a time to better understand the contributions from different indirect (microphysical), “large-scale” semi-direct (above-cloud thermodynamic and subsidence changes), and “local” semi-direct (below-cloud smoke absorption) effects. Despite a more than 5-fold increase in cloud droplet number concentration when including smoke aerosol concentrations, minimal differences in cloud fraction evolution are simulated by the LES when comparing the base case with a perturbed aerosol case with identical thermodynamic and dynamic forcings. A factor of 2 decrease in background free tropospheric aerosol concentrations from the FireOff simulation shifts the cloud evolution from a classical entrainment-driven “deepening–warming” transition to trade cumulus to a precipitation-driven “drizzle-depletion” transition to open cells, however. The thermodynamic and dynamic changes caused by the WRF-simulated large-scale adjustments to smoke diabatic heating strongly influence cloud evolution in terms of both the rate of deepening (especially for changes in the inversion temperature jump and in subsidence) and in cloud fraction on the final day of the simulation (especially for the moisture “banding” effect). Such large-scale semi-direct effects would not have been possible to simulate using a small-domain LES model alone.

southeast Atlantic Ocean↗
NASA NTRS2015

Aircraft Measurements of BrO, IO, Glyoxal, NO2, H2O, O2-O2 and Aerosol Extinction Profiles in the Tropics: Comparison with Aircraft-/Ship-Based in Situ and Lidar Measurements

Tropospheric chemistry of halogens and organic carbon over tropical oceans modifies ozone and atmospheric aerosols, yet atmospheric models remain largely untested for lack of vertically resolved measurements of bromine monoxide (BrO), iodine monoxide (IO) and small oxygenated hydrocarbons like glyoxal (CHOCHO) in the tropical troposphere. BrO, IO, glyoxal, nitrogen dioxide (NO2), water vapor (H2O) and O2-O2 collision complexes (O4/ were measured by the University of Colorado Airborne Multi-AXis Differential Optical Absorption Spectroscopy (CU AMAXDOAS) instrument, aerosol extinction by high spectral resolution lidar (HSRL), in situ aerosol size distributions by an ultra high sensitivity aerosol spectrometer (UHSAS) and in situ H2O by vertical-cavity surface-emitting laser (VCSEL) hygrometer. Data are presented from two research flights (RF12, RF17) aboard the National Science Foundation/ National Center for Atmospheric Research Gulfstream V aircraft over the tropical Eastern Pacific Ocean (tEPO) as part of the "Tropical Ocean tRoposphere Exchange of Reactive halogens and Oxygenated hydrocarbons" (TORERO) project (January/February 2012). We assess the accuracy of O4 slant column density (SCD) measurements in the presence and absence of aerosols. Our O4-inferred aerosol extinction profiles at 477 nm agree within 6% with HSRL in the boundary layer and closely resemble the renormalized profile shape of Mie calculations constrained by UHSAS at low (sub-Rayleigh) aerosol extinction in the free troposphere. CU AMAX-DOAS provides a flexible choice of geometry, which we exploit to minimize the SCD in the reference spectrum (SCDREF, maximize signal-to-noise ratio) and to test the robustness of BrO, IO and glyoxal differential SCDs. The RF12 case study was conducted in pristine marine and free tropospheric air. The RF17 case study was conducted above the NOAA RV Ka'imimoana (TORERO cruise, KA-12-01) and provides independent validation data from ship-based in situ cavity-enhanced DOAS and MAX-DOAS. Inside the marine boundary layer (MBL) no BrO was detected (smaller than 0.5 pptv), and 0.2-0.55 pptv IO and 32-36 pptv glyoxal were observed. The near-surface concentrations agree within 30% (IO) and 10% (glyoxal) between ship and air-craft. The BrO concentration strongly increased with altitude to 3.0 pptv at 14.5 km (RF12, 9.1 to 8.6 deg N; 101.2 to 97.4 deg W). At 14.5 km, 5-10 pptv NO2 agree with model predictions and demonstrate good control over separating tropospheric from stratospheric absorbers (NO2 and BrO). Our profile retrievals have 12-20 degrees of freedom (DoF) and up to 500m vertical resolution. The tropospheric BrO vertical column density (VCD) was 1.5 x 10(exp 13) molec cm(exp -2) (RF12) and at least 0.5 x 10(exp 13) molec cm(exp -2) (RF17, 0- 10 km, lower limit). Tropospheric IO VCDs correspond to 2.1 x 10(exp 12) molec cm(exp -2) (RF12) and 2.5 x 10(exp 12) molec cm(exp -2) (RF17) and glyoxal VCDs of 2.6 x 10(exp 14) molec cm(exp -2) (RF12) and 2.7 x 10(exp 14) molec cm(exp -2) (RF17). Surprisingly, essentially all BrO as well as the dominant IO and glyoxal VCD fraction was located above 2 km (IO: 58 plus or minus 5 %, 0.1-0.2 pptv; glyoxal: 52 plus or minus 5 %, 3-20 pptv). To our knowledge there are no previous vertically resolved measurements of BrO and glyoxal from aircraft in the tropical free troposphere. The atmospheric implications are briefly discussed. Future studies are necessary to better understand the sources and impacts of free tropospheric halogens and oxygenated hydrocarbons on tropospheric ozone, aerosols, mercury oxidation and the oxidation capacity of the atmosphere.

Volkamer, R.↗