The Optical Properties of the Maritime Aerosol and their Correlation to the Electrical Conductivity of the Marine Atmosphere

LONG-TERM GOAL: The long term goal is to have a capability of simultaneously measuring aerosol properties, optical properties, and electrical properties from an aircraft in the marine boundary layer. This involves integration of CN counters, particle spectrometers, nephelometers, Gerdien condenser, and radon detector onto the CIRPAS Twin Otter airplane, along with a suitable data acquisition system.Award Number: N0001499AF0000

Evolution of the vertical profile and flux of large sea-salt particles in a coastal zone

Journal of Geophysical Research, Vol. 106, No. D11, pp. 12,039 - 12,053, June 16, 2001.In the vicinity of the North Carolina Outer Banks we observed both steady onshore flow conditions and a continental air mass transition into a marine boundary layer. Using the CIRPAS Twin Otter aircraft, we measuredc hangesin the columnb urden of sea salt as the air mass was advected out to sea. We also measured the flux of whitecap-generatesde a-saltp articlesi n neutrallys tablea tmospherea t wind speedso f 4, 8, and1 2r n s- •. Productioonf saltp articleass s malla s0 .27/•mi n diametewr aso bserved. Furthermore,w e measureds alt particle size distributionsa t variousw ind speedsd uring alongs horew ind and near steadys tate conditionsU. sing thesem easurementsa s a frame of reference,w e discussth e very large differencesi n the reported size and flux of sea salt presentedi n the literature. The disagreemenitn reported salt fluxesi s larger for smallersizedp articles( almosta n order of magnitude)a nd is most likely due to assumptionms ade when the fluxesw ere computed,e speciallyt he particle dry depositionv elocitya nd air mass history.H owever,f or giant salt particlesw ith short atmosphericli fetimes (>-10/•m in diameter),t here is generala greementb etweenf luxesa nd size distributionsm easuredi n this studya nd previouso nes.R eported salt particle size distributionsin the literature also vary considerablyu nder similar steadyw ind and stability conditions.F rom these and our results it is clear that no more than half of the variance in salt particle concentration can be explainedb y wind speeda lone, suggestingth at the idea of "steadys tate" in the marine boundary layer rarely exists at midlatitudes

Observations of Sharp Oxalate Reductions in Stratocumulus Clouds at Variable Altitudes: Organic Acid and Metal Measurements During the 2011 E-PEACE Campaign

This work examines organic acid and metal concentrations in northeastern Pacific Ocean stratocumulus cloudwater samples collected by the CIRPAS Twin Otter between July and August 2011. Correlations between a suite of various monocarboxylic and dicarboxylic acid concentrations are consistent with documented aqueous-phase mechanistic relationships leading up to oxalate production. Monocarboxylic and dicarboxylic acids exhibited contrasting spatial profiles reflecting their different sources; the former were higher in concentration near the continent due to fresh organic emissions. Concentrations of sea salt crustal tracer species, oxalate, and malonate were positively correlated with low-level wind speed suggesting that an important route for oxalate and malonate entry in cloudwater is via some combination of association with coarse particles and gaseous precursors emitted from the ocean surface. Three case flights show that oxalate (and no other organic acid) concentrations drop by nearly an order of magnitude relative to samples in the same vicinity. A consistent feature in these cases was an inverse relationship between oxalate and several metals (Fe, Mn, K, Na, Mg, Ca), especially Fe. By means of box model studies we show that the loss of oxalate due to the photolysis of iron oxalato complexes is likely a significant oxalate sink in the study region due to the ubiquity of oxalate precursors, clouds, and metal emissions from ships, the ocean, and continental sources

Marine stratocumulus aerosol‐cloud relationships in the MASE‐II experiment: Precipitation susceptibility in eastern Pacific marine stratocumulus

Journal of Geophysical Research, Vol. 114, D24203The article of record as published may be located at http://dx.doi.org/10.1029/2009JD012774.Observational data on aerosol-cloud-drizzle relationships in marine stratocumulus are presented from the second Marine Stratus/Stratocumulus Experiment (MASE-II) carried out in July 2007 over the eastern Pacific near Monterey, California. Observations, carried out in regions of essentially uniform meteorology with localized aerosol enhancements due to ship exhaust (‘‘ship tracks’’), demonstrate, in accord with those from numerous other field campaigns, that increased cloud drop number concentration Nc and decreased cloud top effective radius re are associated with increased subcloud aerosol concentration

Aerosol and Cloud Microphysical Characteristics of Rifts and Gradients in Maritime Stratocumulus Clouds

A cloud rift is characterized as a large-scale, persistent area of broken, low-reflectivity stratocumulus clouds usually surrounded by a solid deck of stratocumulus. A rift observed off the coast of California was investigated using an instrumented aircraft to compare the aerosol, cloud microphysical, and thermodynamic properties in the rift with those of the surrounding solid stratocumulus deck. The microphysical characteristics in the solid stratocumulus deck differ substantially from those of a broken, cellular rift where cloud droplet concentrations are a factor of 2 lower than those in the solid cloud. Furthermore, cloud condensation nuclei (CCN) concentrations were found to be about 3 times greater in the solid-cloud area compared with those in the rift. Although drizzle was observed near cloud top in parts of the solid stratocumulus cloud, the largest drizzle rates were associated with the broken clouds within the rift area and with extremely large effective droplet sizes retrieved from satellite data. Minimal thermodynamic differences between the rift and solid cloud deck were observed. In addition to marked differences in particle concentrations, evidence of a mesoscale circulation near the solid cloud–rift boundary is presented. This mesoscale circulation may provide a mechanism for maintaining a rift, but further study is required to understand the initiation of a rift and the conditions that may cause it to fill. A review of results from previous studies indicates similar microphysical characteristics in rift features sampled serendipitously. These observations indicate that cloud rifts are depleted of aerosols through the cleansing associated with drizzle and are a manifestation of natural processes occurring in marine stratocumulus

On the presence of giant particles downwind of ships in the marine boundary layer

This study examines large oceangoing ships as a source of giant cloud condensation nuclei (D_p > 2 µm) due to wake and stack emissions off the California coast. Observed particle number concentrations behind 10 ships exceeded those in “control” areas, exhibiting number concentration enhancement ratios (ERs) for minimum threshold diameters of ~2, ~10, and ~20 µm as high as 2.7, 5.5, and 7.5, respectively. ER decreases with increasing downwind distance and altitude. ER becomes better correlated with ship size variables (gross tonnage, length, and beam) as the minimum size threshold increases from 2 to 20 µm, whereas ship speed has a less distinct relationship with ER. One case study of a container ship shows that there are higher concentrations of sea-salt tracer species behind it relative to adjacent control areas. These results have implications for cloud properties and precipitation in marine boundary layers exposed to ship traffic

The Marine Stratus/Stratocumulus Experiment (MASE): Aerosol-cloud relationships in marine stratocumulus

Journal of Geophysical Research, Vol. 112, D10209The article of record as published may be located at http://dx.doi.org/10.1029/2006JD007985.The Marine Stratus/Stratocumulus Experiment (MASE) field campaign was undertaken in July 2005 off the coast of Monterey, California to evaluate aerosol-cloud relationships in the climatically important regime of eastern Pacific marine stratocumulus. Aerosol and cloud properties were measured onboard the Center for Interdisciplinary Remotely-Piloted Aircraft Studies (CIRPAS) Twin Otter aircraft. One cloud that was clearly impacted by ship emissions as well as the ensemble of clouds observed over the entire mission are analyzed in detail. Results at both the individual and ensemble scales clearly confirm the Twomey effect (first indirect effect of aerosols) and demonstrate drizzle suppression at elevated aerosol number concentration. For the ship track impacted cloud, suppressed drizzle in the track led to a larger cloud liquid water path (LWP) at the same cloud thickness, in accord with the so-called second indirect effect. Ensemble averages over all clouds sampled over the entire 13-flight mission show the opposite effect of aerosol number concentration on LWP, presumably the result of other dynamic influences (e.g., updraft velocity and ambient sounding profile). Individual polluted clouds were found to exhibit a narrower cloud drop spectral width in accord with theoretical prediction (M.-L. Lu and J. H. Seinfeld, Effect of aerosol number concentration on cloud droplet dispersion: A large-eddy simulation study and implications for aerosol indirect forcing, Journal of Geophysical Research, 2006). This field experiment demonstrates both the indirect aerosol effect on ship track perturbed clouds, as well as the subtleties involved in extracting these effects over an ensemble of clouds sampled over a 1-month period

The Marine Stratus/Stratocumulus Experiment (MASE): Aerosol-cloud relationships in marine stratocumulus

The Marine Stratus/Stratocumulus Experiment (MASE) field campaign was undertaken in July 2005 off the coast of Monterey, California to evaluate aerosol-cloud relationships in the climatically important regime of eastern Pacific marine stratocumulus. Aerosol and cloud properties were measured onboard the Center for Interdisciplinary Remotely-Piloted Aircraft Studies (CIRPAS) Twin Otter aircraft. One cloud that was clearly impacted by ship emissions as well as the ensemble of clouds observed over the entire mission are analyzed in detail. Results at both the individual and ensemble scales clearly confirm the Twomey effect (first indirect effect of aerosols) and demonstrate drizzle suppression at elevated aerosol number concentration. For the ship track impacted cloud, suppressed drizzle in the track led to a larger cloud liquid water path (LWP) at the same cloud thickness, in accord with the so-called second indirect effect. Ensemble averages over all clouds sampled over the entire 13-flight mission show the opposite effect of aerosol number concentration on LWP, presumably the result of other dynamic influences (e.g., updraft velocity and ambient sounding profile). Individual polluted clouds were found to exhibit a narrower cloud drop spectral width in accord with theoretical prediction (M.-L. Lu and J. H. Seinfeld, Effect of aerosol number concentration on cloud droplet dispersion: A large-eddy simulation study and implications for aerosol indirect forcing, Journal of Geophysical Research, 2006). This field experiment demonstrates both the indirect aerosol effect on ship track perturbed clouds, as well as the subtleties involved in extracting these effects over an ensemble of clouds sampled over a 1-month period

Aerosol-cloud relationships in continental shallow cumulus

Aerosol-cloud relationships are derived from 14 warm continental cumuli cases sampled during the 2006 Gulf of Mexico Atmospheric Composition and Climate Study (GoMACCS) by the Center for Interdisciplinary Remotely-Piloted Aircraft Studies (CIRPAS) Twin Otter aircraft. Cloud droplet number concentration is clearly proportional to the subcloud accumulation mode aerosol number concentration. An inverse correlation between cloud top effective radius and subcloud aerosol number concentration is observed when cloud depth variations are accounted for. There are no discernable aerosol effects on cloud droplet spectral dispersion; the averaged spectral relative dispersion is 0.30 ± 0.04. Aerosol-cloud relationships are also identified from comparison of two isolated cloud cases that occurred under different degrees of anthropogenic influence. Cloud liquid water content, cloud droplet number concentration, and cloud top effective radius exhibit subadiabaticity resulting from entrainment mixing processes. The degree of LWC subadiabaticity is found to increase with cloud depth. Impacts of subadiabaticity on cloud optical properties are assessed. It is estimated that owing to entrainment mixing, cloud LWP, effective radius, and cloud albedo are decreased by 50–85%, 5–35%, and 2–26%, respectively, relative to adiabatic values of a plane-parallel cloud. The impact of subadiabaticity on cloud albedo is largest for shallow clouds. Results suggest that the effect of entrainment mixing must be accounted for when evaluating the aerosol indirect effect

Water-soluble organic aerosol in the Los Angeles Basin and outflow regions: Airborne and ground measurements during the 2010 CalNex field campaign

A particle-into-liquid sampler coupled to a total organic carbon analyzer (PILS-TOC) quantified particulate water-soluble organic carbon (WSOC) mass concentrations during the May 2010 deployment of the Center for Interdisciplinary Remotely Piloted Aircraft Studies (CIRPAS) Twin Otter in the CalNex field study. WSOC data collected during 16 flights provide the first spatiotemporal maps of WSOC in the San Joaquin Valley, Los Angeles Basin, and outflow regions of the Basin. WSOC was consistently higher in concentration within the Los Angeles Basin, where sea breeze transport and Basin topography strongly influence the spatial distribution of WSOC. The highest WSOC levels were associated with fire plumes, highlighting the importance of both primary and secondary sources for WSOC in the region. Residual pollution layers enriched with WSOC are observed aloft up to an altitude of 3.2 km and the highest WSOC levels for each flight were typically observed above 500 m. Simultaneous ground WSOC measurements during aircraft overpasses in Pasadena and Riverside typically exhibit lower levels, especially when relative humidity (RH) was higher aloft suggestive of the influence of aerosol-phase water. This points to the underestimation of the radiative effects of WSOC when using only surface measurements. Reduced aerosol-phase water in the eastern desert outflow region likely promotes the re-partitioning of WSOC to the gas phase and suppression of processes to produce these species (partitioning, multiphase chemistry, photolytic production); as a result, WSOC is reduced relative to sulfate (but not as much as nitrate) as aerosol is advected from the Basin to the outflows