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Impact of Ship Emissions on Marine Boundary Layer NO(x) and SO2 Distributions over the Pacific Basin

The impact of ship emissions on marine boundary layer (MBL) NO(x) and SO2 levels over the Pacific Ocean has been explored by comparing predictions (with and without ships) from a global chemical transport model (GCTM) against compiled airborne observations of MBL NO(x) and SO2. For latitudes above 15 N, which define that part of the Pacific having the heaviest shipping, this analysis revealed significant model over prediction for NOx and a modest under prediction for SO2 when ship emissions were considered. Possible reasons for the difference in NO(x) and SO2 were explored using a full-chemistry box model. These results revealed that for an actual plume setting the NO(x) lifetime could be greatly shortened by chemical processes promoted by ship plume emissions themselves. Similar chemical behavior was not found for SO2.

Davis, D. D.↗

Missing OH Reactivity in the Global Marine Boundary Layer

The hydroxyl radical (OH) reacts with thousands of chemical species in the atmosphere, initiating their removal and the chemical reaction sequences that produce ozone, secondary aerosols, and gas-phase acids. OH reactivity, which is the inverse of OH lifetime,influences the OH abundance and the ability of OH to cleanse the atmosphere. The NASA Atmospheric Tomography (ATom) campaign used instruments on the NASA DC-8 aircraft to measure OH reactivity and more than 100 trace chemical species. ATom presented a unique opportunity to test the completeness of the OH reactivity calculated from the chemical species measurements by comparing it to the measured OH reactivity over two oceans across four seasons. Although, throughout much of the free troposphere, the calculated OH reactivity was below the limit-of-detection for the ATom instrument used to measure OH reactivity, the instrument was able to measure the OH reactivity in and just above the marine boundary layer. The mean measured value of OH reactivity in the marine boundary layer across all latitudes and all ATom deployments was 1.9 s-1, which is 0.5 s-1larger than the mean calculated OH reactivity. The missing OH reactivity, the difference between the measured and calculated OH reactivity, varied between 0 s-1to 3.5 s-1, with the highest values over the Northern Hemisphere Pacific Ocean. Correlations of missing OH reactivity with formaldehyde, dimethyl sulfide, butanal, and sea surface temperature suggest the presence of unmeasured or unknown volatile organic compounds or oxygenated volatile organic compounds associated with ocean emissions.

NASA Atmospheric Tomography (ATom)↗

Low Ozone in the Marine Boundary Layer of the Tropical Pacific Ocean

Aircraft measurements of ozone, its key precursors, and a variety of chemical tracers were made in the troposphere of the western and central Pacific in October 1991. These data are presented and analyzed to examine the occurrence of low ozone concentrations in the remote marine boundary layer of the tropical and equatorial Pacific Ocean. The data from these flights out of Guam, covering an area extending from the equator to 20 N and from south of the Philippines to Hawaii, show average O3 concentrations as low as 8-9 ppb (ppb=10(exp-9)v/v) at altitudes of 0.3-0.5 km in the boundary layer. Individual measurements as low as 2-5 ppb were recorded. Low O3 concentrations do not always persist in space and time. High O3, generally associated with the transport of upper tropospheric air, was also encountered in the boundary layer. In practically all cases, O3 increased to values as large as 25-30 ppb within 2 km above the boundary layer top. Steady state model computations are used to suggest that these low O3 concentrations are a result of net photochemical O3 destruction in a low NO environment, sea-surface deposition, and extremely low net entrainment rates (1-2 mm per second) from the free troposphere. Day/night measurements of ethane, propane, gaseous and aerosol Cl suggest that daytime (morning) Cl atom concentrations in the vicinity of 10(exp 5) molecules per cubic centimeter may be present in the marine boundary layer. This Cl atom abundance can be rationalized only if sea salt aerosols can release free chlorine (Cl2) to the gas phase in the presence of sun light (and possibly O3). These Cl atom concentrations, however, are still insufficient and Cl (or Br) chemistry is not likely to be an important cause of the observed low O3.

Singh, Hanwant B.↗

Optically relevant turbulence parameters in the Marine boundary layer

Shipboard measurements of temperature and velocity fluctuations were performed to determine optical propagation properties of the marine boundary layer. Empirical expressions describing the temperature structure parameter in terms of the Richardson Number overland were used to analyze data obtained for open ocean conditions. Likewise, profiles of mean wind and velocity fluctuation spectra derived from shipboard observations were utilized to calculate associated boundary layer turbulence parameters. In general, there are considerable differences between the open-ocean results of this study and previously determined overland results.

Davidson, K. L.↗

Parameterizing Grid-Averaged Longwave Fluxes for Inhomogeneous Marine Boundary Layer Clouds

This paper examines the relative impacts on grid-averaged longwave flux transmittance (emittance) for Marine Boundary Layer (MBL) cloud fields arising from horizontal variability of optical depth tau and cloud sides, First, using fields of Landsat-inferred tau and a Monte Carlo photon transport algorithm, it is demonstrated that mean all-sky transmittances for 3D variable MBL clouds can be computed accurately by the conventional method of linearly weighting clear and cloudy transmittances by their respective sky fractions. Then, the approximations of decoupling cloud and radiative properties and assuming independent columns are shown to be adequate for computation of mean flux transmittance. Since real clouds have nonzero geometric thicknesses, cloud fractions A'(sub c) presented to isotropic beams usually exceed the more familiar vertically projected cloud fractions A(sub c). It is shown, however, that when A(sub c)less than or equal to 0.9, biases for all-sky transmittance stemming from use of A(sub c) as opposed to A'(sub c) are roughly 2-5 times smaller than, and opposite in sign to, biases due to neglect of horizontal variability of tau. By neglecting variable tau, all-sky transmittances are underestimated often by more than 0.1 for A(sub c) near 0.75 and this translates into relative errors that can exceed 40% (corresponding errors for all-sky emittance are about 20% for most values of A(sub c). Thus, priority should be given to development of General Circulation Model (GCM) parameterizations that account for the effects of horizontal variations in unresolved tau, effects of cloud sides are of secondary importance. On this note, an efficient stochastic model for computing grid-averaged cloudy-sky flux transmittances is furnished that assumes that distributions of tau, for regions comparable in size to GCM grid cells, can be described adequately by gamma distribution functions. While the plane-parallel, homogeneous model underestimates cloud transmittance by about an order of magnitude when 3D variable cloud transmittances are less than or equal to 0.2 and by approx. 20% to 100% otherwise, the stochastic model reduces these biases often by more than 80%.

Barker, Howard W.↗

Comparison of Marine Boundary Layer Cloud Properties from CERES-MODIS Edition 4 and DOE ARM AMF Measurements at the Azores

Marine boundary layer (MBL) cloud properties derived from the NASA Clouds and the Earth's Radiant Energy System (CERES) project using Terra and Aqua Moderate Resolution Imaging Spectroradiometer (MODIS) data are compared with observations taken at the Department of Energy Atmospheric Radiation Measurement (ARM) Mobile Facility at the Azores (AMF-Azores) site from June 2009 through December 2010. Cloud properties derived from ARM ground-based observations were averaged over a 1 h interval centered at the satellite overpass time, while the CERES-MODIS (CM) results were averaged within a 30 km×30 km grid box centered over the Azores site. A total of 63 daytime and 92 nighttime single-layered overcast MBL cloud cases were selected from 19 months of ARM radar-lidar and satellite observations. The CM cloud top/base heights (Htop/Hbase) were determined from cloud top/base temperatures (Ttop/Tbase) using a regional boundary layer lapse rate method. For daytime comparisons, the CM-derived Htop (Hbase), on average, is 0.063 km (0.068 km) higher (lower) than its ARM radar-lidar-observed counterpart, and the CM-derived Ttop and Tbase are 0.9 K less and 2.5 K greater than the surface values with high correlations (R(sup 2) = 0.82 and 0.84, respectively). In general, the cloud top comparisons agree better than the cloud base comparisons, because the CM cloud base temperatures and heights are secondary products determined from cloud top temperatures and heights. No significant day-night difference was found in the analyses. The comparisons of MBL cloud microphysical properties reveal that when averaged over a 30 km× 30 km area, the CM-retrieved cloud droplet effective radius (re) at 3.7 micrometers is 1.3 micrometers larger than that from the ARM retrievals (12.8 micrometers), while the CM-retrieved cloud liquid water path (LWP) is 13.5 gm( exp -2) less than its ARM counterpart (114.2 gm( exp-2) due to its small optical depth (9.6 versus 13.7). The differences are reduced by 50% when the CM averages are computed only using the MODIS pixel nearest the AMF site. Using the effective radius retrieved using 2.1 micrometers channel to calculate LWP can reduce the difference between the CM and ARM microwave radiometer retrievals from 13.7 to 2.1 gm2. The 10% differences between the ARM and CERES-MODIS LWP and r(sub e) retrievals are within the uncertainties of the ARM LWP (approximately 20gm( exp -2)) and r(sub e) (approximately 10%) retrievals; however, the 30% difference in optical depth is significant. Possible reasons contributing to this discrepancy are increased sensitivities in optical depth from both surface retrievals when τ is approximately 10 and topography. The τ differences vary with wind direction and are consistent with the island orography.Much better agreement in τ is obtained when using only those data taken when the wind is from the northeast, where topographical effects on the sampled clouds are minimal.

Xi, Baike↗

Marine Boundary Layer Cloud Properties From AMF Point Reyes Satellite Observations

Cloud Diameter, C(sub D), offers a simple measure of Marine Boundary Layer (MBL) cloud organization. The diurnal cycle of cloud-physical properties and C(sub D) at Pt Reyes are consistent with previous work. The time series of C(sub D) can be used to identify distinct mesoscale organization regimes within the Pt. Reyes observation period.

Jensen, Michael↗

Use of long-lived radon daughters as indicators of exchange between the free troposphere and the marine boundary layer

Fluxes and exchange coefficients are derived for the transport of Sr-90, Pb-210, Bi-210, and Po-210 between the free troposphere and the marine boundary layer and between the boundary layer and the sea surface. Radionuclide concentrations previously measured near Hawaii are used in the derivations. Values obtained for the free troposphere/boundary layer exchange coefficient (expressed as a piston velocity) were 185, 228 and 203 m/d for Pb-210, Bi-210, and Sr-90, respectively. The magnitude of the local sea-surface source of Po-210 is also determined.

Kritz, M. A.↗

Roles of drizzle in a one-dimensional third-order turbulence closure model of the nocturnal stratus-topped marine boundary layer

This study focuses on the effects of drizzle in a one-dimensional third-order turbulence closure model of the nocturnal stratus-topped marine boundary layer. When the simulated drizzle rate is relatively small (maximum approximately equal to 0.6 mm/day), steady-state solutions are obtained. The boundary layer stabilizes essentially because drizzle causes evaporative cooling of the subcloud layer. This stabilization considerably reduces the buoyancy flux and turbulence kinetic energy below the stratus cloud. Thus, drizzle tends to decouple the cloud from the subcloud layer in the model, as suggested by many observational studies. In addition, the evaporation of drizzle in the subcloud layer creates small scattered clouds, which are likely to represent cumulus clouds, below the solid stratus cloud in the model. The sensitivity experiments show that these scattered clouds help maintain a coupled boundary layer. When the drizzle rate is relatively large (maximum approximately equal to 0.9 mm/day), the response of the model becomes transient with bursts in turbulent fluxes. This phenomenon is related to the formation of the scattered cloud layer below the solid stratus cloud. It appears that the model is inadequate to represent the heat and moisture transport by strong updrafts covering a small fractional area in cumulus convection.

Wang, Shouping↗

Horizontal variability of the marine boundary layer structure upwind of San Nicolas Island during FIRE, 1987

During the months of June and July 1987, the Marine Stratocumulus Intensive Field Observation Experiment of First ISCCP Regional Experiment (FIRE) was conducted in the Southern California offshore area in the vicinity of San Nicolas Island (SNI). The Naval Ocean Systems Center (NOSC) airborne platform was utilized during FIRE to investigate the upwind low level horizontal variability of the marine boundary layer structure to determine the representativeness of SNI-based measurements to upwind open ocean conditions. The NOSC airborne meteorological platform made three flights during FIRE, two during clear sky conditions (19 and 23 July), and one during two stratus conditions (15 July). The boundary layer structure variations associated with the stratus clouds of 15 July 1987 are discussed. Profiles of air temperature (AT) and relative humidity (RH) taken 'at' and 'upwind' of SNI do show differences between the so-called open ocean conditions and those taken near the island. However, the observed difference cannot be uniquely identified to island effects, especially since the upwind fluctuations of AT and RH bound the SNI measurements. Total optical depths measures at SNI do not appear to be greatly affected by any surface based aerosol effects created by the island and could therefore realistically represent open ocean conditions. However, if one were to use the SNI aerosol measurements to predict ship to ship EO propagation conditions, significant errors could be introduced due to the increased number of surface aerosols observed near SNI which may not be, and were not, characteristic of open ocean conditions. Sea surface temperature measurements taken at the island will not, in general, represent those upwind open ocean conditions. Also, since CTT's varied appreciably along the upwind radials, measurements of CTT over the island may not be representative of actual open ocean CTT's.

Jensen, Douglas R.↗

Exploring the Continuum of Stratiform and Cumulus Cloudiness: Observational Insights Related to Marine Boundary Layer Clouds

Low-level marine clouds take on a wide range of morphological states owing to external forcing and internal feedbacks. Rarely are shallow marine clouds adequately described by a single simplified framework but instead exhibit features that partially conform to several states that could be considered “limiting”. Perhaps the most apparent dichotomy is whether to consider shallow clouds as existing within a surface-driven mixed layer or as convective “plume” elements positioned on top. Do the rules that govern the limiting cases transition smoothly through the hybrid scenarios found in nature, or are there particular regions of attraction or repulsion?We have identified 3 ”axes” along which to investigate how the energetics, thermodynamics and cloud macro structure relate to the intermediate spaces between idealizations.

Ewan Crosbie↗

Observation of Trace Gases Seasonal Variability in the Marine Boundary Layer over the Atlantic Ocean during the ACTIVATE Field Campaign

High resolution in-situ measurements of carbon monoxide (CO), carbon dioxide (CO2), methane (CH4), and water vapor (H2O) were made onboard the NASA HU-25 aircraft during the ACTIVATE (Aerosol Cloud meteorology Interactions oVer the western Atlantic Experiment) campaign during 2020 and 2021 in different seasons (winter through summer) over the mid-latitude western Atlantic Ocean. As most of the flights focused on the marine boundary layer (MBL) during the campaign, these trace gas observations are an excellent data set to examine seasonal variability of trace gas background values in the MBL without the influence of localized point sources. We will describe the variability of these trace gases in the MBL background by filtering out concentrated point sources using back trajectory analysis along with trace gas ratios. Additionally, the ocean is a significant sink of anthropogenic CO2 capturing about one quarter of total anthropogenic carbon. By looking at the MBL CO2 variation as a function of season, we discuss observed changes in CO2 uptake over the ocean. These high accuracy observations of trace gas backgrounds in the MBL along with characterizing seasonal effects on oceanic sequestering of anthropogenic CO2 will improve the understanding of seasonal variations and change in climate and inverse modelling over the ocean.

Yonghoon Choi↗

Methane and nonmethane hydrocarbon concentrations in the Atlantic marine boundary layer

The reactions of reduced tropospheric trace gases with hydroxyl radicals are thought to play a significant role in global tropospheric photochemistry. Since tropospheric methane and nonmethane hydrocarbon (NMHC) concentrations will affect the tropospheric hydroxyl radical concentrations, accurate measurements of tropospheric CH4 and NMHC concentrations are necessary. Such measurements were, therefore, included in the first leg (from Hamburg, West Germany to Montevideo, Uruguay) of the 1980-1981 Antarctic Expedition. On the basis of the obtained data, a pronounced gradient between northern and southern hemispheric methane concentrations was observed in the marine boundary layer in the region of the intertropical convergence zone. Methane concentrations gradually decreased from about 1.70 ppmv at 40 deg N latitude to about 1.68 ppmv at 14 deg N latitude, then dropped sharply between 14 deg N and 10 deg N latitude to about 1.61 ppmv. NMHC data are also discussed.

Cofer, W. R., III↗

Airborne Sunphotometry of African Dust and Marine Boundary Layer Aerosols in PRIDE

The Puerto Rico Dust Experiment (PRIDE) was conducted during summer 2000 to study the radiative, microphysical and transport properties of Saharan dust in the Caribbean region. During PRIDE, NASA Ames Research Center's six-channel airborne autotracking sunphotometer (AATS-6) was operated aboard a Piper Navajo airplane based at Roosevelt Roads Naval Station on the northeast coast of Puerto Rico. AATS-6 measurements were taken during 21 science flights off the coast of Puerto Rico in the western Caribbean. Data were acquired within and above the Marine Boundary Layer (MBL) and the Saharan Aerosol Layer (SAL) up to 5.5 km altitude tinder a wide range of dust loadings. Aerosol optical depth (AOD) spectra and columnar water vapor (CWV) values have been calculated from the AATS-6 measurements by using sunphotometer calibration data obtained at Mauna Loa Observatory (3A kin ASL) before (May) and after (October) PRIDE. Mid-visible AOD values measured near the surface during PRIDE ranged from 0.07 on the cleanest day to 0.55 on the most turbid day. Values measured above the MBL were as high as 0.35; values above the SAL were as low as 0.01. The fraction of total column AOD due to Saharan dust cannot be determined precisely from AATS-6 AOD data alone due to the uncertainty in the extent of vertical mixing of the dust down through the MBL. However, analyses of ground-based and airborne in-situ aerosol sampling measurements and ground-based aerosol lidar backscatter data should yield accurate characterization of the vertical mixing that will enable calculation of the Saharan dust AOD component from the sunphotometer data. Examples will be presented showing measured AATS-6 AOD spectra, calculated aerosol extinction and water vapor density vertical profiles, and aerosol size distributions retrieved by inversion of the AOD spectra. Near sea-surface AOD spectra acquired by AATS-6 during horizontal flight legs at 30 m ASL are available for validation of AOD derived from coincident satellite sensor (TOMS, MODIS, MISR) measurements. AATS-6 AOD data acquired during numerous aircraft ascents and descents through the MBL and the SAL should permit atmospheric column closure analyses with respect to aerosol optical depth, extinction, and size distribution by comparison with coincident aircraft-based in-situ particle size distribution measurements and ground-based (Cabras Island, Puerto Rico) micropulse lidar aerosol backscatter measurements. The aerosol information derived from the column closure analyses can be used subsequently to calculate radiative flux changes, which can then be compared with coincident spectral flux measurements taken from aboard the aircraft with a solar spectral flux radiometer.

Livingston, John M.↗

Senstitivity analysis of horizontal heat and vapor transfer coefficients for a cloud-topped marine boundary layer during cold-air outbreaks

The effects of external parameters on the surface heat and vapor fluxes into the marine atmospheric boundary layer (MABL) during cold-air outbreaks are investigated using the numerical model of Stage and Businger (1981a). These fluxes are nondimensionalized using the horizontal heat (g1) and vapor (g2) transfer coefficient method first suggested by Chou and Atlas (1982) and further formulated by Stage (1983a). In order to simplify the problem, the boundary layer is assumed to be well mixed and horizontally homogeneous, and to have linear shoreline soundings of equivalent potential temperature and mixing ratio. Modifications of initial surface flux estimates, time step limitation, and termination conditions are made to the MABL model to obtain accurate computations. The dependence of g1 and g2 in the cloud topped boundary layer on the external parameters (wind speed, divergence, sea surface temperature, radiative sky temperature, cloud top radiation cooling, and initial shoreline soundings of temperature, and mixing ratio) is studied by a sensitivity analysis, which shows that the uncertainties of horizontal transfer coefficients caused by changes in the parameters are reasonably small.

Chang, Y. V.↗

Estimating the Direct Radiative Effect of Absorbing Aerosols Overlying Marine Boundary Layer Clouds in the Southeast Atlantic Using MODIS and CALIOP

Absorbing aerosols such as smoke strongly absorb solar radiation, particularly at ultraviolet and visible/near-infrared (VIS/NIR) wavelengths, and their presence above clouds can have considerable implications. It has been previously shown that they have a positive (i.e., warming) direct aerosol radiative effect (DARE) when overlying bright clouds. Additionally, they can cause biased passive instrument satellite retrievals in techniques that rely on VIS/NIR wavelengths for inferring the cloud optical thickness (COT) and effective radius (re) of underlying clouds, which can in turn yield biased above-cloud DARE estimates. Here we investigate Moderate Resolution Imaging Spectroradiometer (MODIS) cloud optical property retrieval biases due to overlying absorbing aerosols observed by Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) and examine the impact of these biases on above-cloud DARE estimates. The investigation focuses on a region in the southeast Atlantic Ocean during August and September (2006-2011), where smoke from biomass burning in southern Africa overlies persistent marine boundary layer stratocumulus clouds. Adjusting for above-cloud aerosol attenuation yields increases in the regional mean liquid COT (averaged over all ocean-only liquid clouds) by roughly 6%; mean re increases by roughly 2.6%, almost exclusively due to the COT adjustment in the non-orthogonal retrieval space. It is found that these two biases lead to an underestimate of DARE. For liquid cloud Aqua MODIS pixels with CALIOP-observed above-cloud smoke, the regional mean above-cloud radiative forcing efficiency (DARE per unit aerosol optical depth (AOD)) at time of observation (near local noon for Aqua overpass) increases from 50.9Wm(sup-2)AOD(sup-1) to 65.1Wm(sup-2)AOD(sup -1) when using bias-adjusted instead of nonadjusted MODIS cloud retrievals.

aerosols↗

Diurnal variation in the turbulent structure of the cloudy marine boundary layer during FIRE 1987

During the 1987 FIRE marine stratocumulus experiment the U.K. Meteorological Office operated a set of turbulence probes attached to the tether cable of a balloon based on San Nicolas Island. Typically six probes were used; each probe is fitted with Gill propeller anemometers, a platinum resistance thermometer and wet and dry thermistors, to permit measurements of the fluxes of momentum, heat, and humidity. The orientation of each probe is determined from a pair of inclinometers and a three-axis magnetometer. Sufficient information is available to allow the measured wind velocities to be corrected for the motion of the balloon. On the 14 to 15 July measurements were made over the period 1530 to 1200 UTC and again, after a short break for battery recharging and topping-up the balloon, between 0400 to 0900 UTC. Data were therefore recorded from morning to early evening, and again for a period overnight. Six probes were available for the daytime measurements, five for the night. Data were recorded at 4 Hz for individual periods of a little over an hour. The intention was to keep a minimum of one probe at or just above cloud top; small changes in balloon height were necessary to accommodate changes in inversion height. The ability of the balloon system to make simultaneous measurements at several levels allows the vertical structure of the boundary layer to be displayed without resort to composites. Turbulent statistics were calculated from 2 hour periods, one straddling local noon and one at night. These were subdivided into half-hour averaging intervals for the evaluation of variances and fluxes.

Hignett, Phillip↗

Progress in Understanding the Impacts of 3-D Cloud Structure on MODIS Cloud Property Retrievals for Marine Boundary Layer Clouds

Theory: A novel framework based on 2-D Tayler expansion for quantifying the uncertainty in MODIS retrievals caused by sub-pixel reflectance inhomogeneity. (Zhang et al. 2016). How cloud vertical structure influences MODIS LWP retrievals. (Miller et al. 2016). Observation: Analysis of failed MODIS cloud property retrievals. (Cho et al. 2015). Cloud property retrievals from 15m resolution ASTER observations. (Werner et al. 2016). Modeling: LES-Satellite observation simulator (Zhang et al. 2012, Miller et al. 2016).

marine boundary layer↗