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This study analyzes 27 cumuliform and stratiform clouds sampled aboard the CIRPAS Twin Otter during the 2004 International Consortium for Atmospheric Research on Transport and Transformation (ICARTT) experiment. The data set was used to assess cloud droplet closure using (1) a detailed adiabatic cloud parcel model and (2) a state-of-the-art cloud droplet activation parameterization. A unique feature of the data set is the sampling of highly polluted clouds within the vicinity of power plant plumes. Remarkable closure was achieved (much less than the 20% measurement uncertainty) for both parcel model and parameterization. The highly variable aerosol did not complicate the cloud droplet closure, since the clouds had low maximum supersaturation and were not sensitive to aerosol variations (which took place at small particle sizes). The error in predicted cloud droplet concentration was mostly sensitive to updraft velocity. Optimal closure is obtained if the water vapor uptake coefficient is equal to 0.06, but can range between 0.03 and 1.0. The sensitivity of cloud droplet prediction error to changes in the uptake coefficient, organic solubility and surface tension depression suggest that organics exhibit limited solubility. These findings can serve as much needed constraints in modeling of aerosol-cloud interactions in the North America; future in situ studies will determine the robustness of our findings.

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.

Context. The ongoing Gaia-ESO Public Spectroscopic Survey is using FLAMES at the VLT to obtain high-quality medium-resolution Giraffe spectra for about 10(5) stars and high-resolution UVES spectra for about 5000 stars. With UVES, the Survey has already observed 1447 FGK-type stars. Aims. These UVES spectra are analyzed in parallel by several state-of-the-art methodologies. Our aim is to present how these analyses were implemented, to discuss their results, and to describe how a final recommended parameter scale is defined. We also discuss the precision (method-to-method dispersion) and accuracy (biases with respect to the reference values) of the final parameters. These results are part of the Gaia-ESO second internal release and will be part of its first public release of advanced data products. Methods. The final parameter scale is tied to the scale defined by the Gaia benchmark stars, a set of stars with fundamental atmospheric parameters. In addition, a set of open and globular clusters is used to evaluate the physical soundness of the results. Each of the implemented methodologies is judged against the benchmark stars to define weights in three different regions of the parameter space. The final recommended results are the weighted medians of those from the individual methods. Results. The recommended results successfully reproduce the atmospheric parameters of the benchmark stars and the expected T(eff)-log g relation of the calibrating clusters. Atmospheric parameters and abundances have been determined for 1301 FGK-type stars observed with UVES. The median of the method-to-method dispersion of the atmospheric parameters is 55K for T(eff), 0.13 dex for log g and 0.07 dex for [Fe/H]. Systematic biases are estimated to be between 50−100 K for T(eff), 0.10−0.25 dex for log g and 0.05−0.10 dex for [Fe/H]. Abundances for 24 elements were derived: C, N, O, Na, Mg, Al, Si, Ca, Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn, Y, Zr, Mo, Ba, Nd, and Eu. The typical method-to-me

Vertical transport associated with cumulus clouds is important to the redistribution of gases, particles and energy, with subsequent consequences for many aspects of the climate system. Previous studies have suggested that detrainment from clouds can be comparable to the updraft mass flux, and thus represents an important contribution to vertical transport. In this study, we describe a new method to deduce the amounts of gross detrainment and entrainment experienced by non-precipitating cumulus cloud using aircraft observations. The method utilizes equations for three conserved variables: cloud mass, total water, and moist static energy. Optimizing these three equations leads to estimates of the mass fractions of adiabatic mixed-layer air, entrained air and detrained air that the sampled cloud has experienced. The method is applied to six flights of the CIRPAS Twin Otter during the Gulf of Mexico Atmospheric Composition and Climate Study (GoMACCS) which took place in the Houston, Texas region during the summer of 2006 during which 176 small, non-precipitating cumulus were sampled. Our analysis suggests that, on average, these clouds were comprised of 30 to 70% mixed-layer air with entrained air comprising most of the remainder. The mass fraction of detrained air was less than 2% for a majority of the clouds, although 15% of them did exhibit detrained air fractions larger than 10%. Entrained and detrained air mass fraction both increased with altitude, and the largest detrainment events were almost al associated with air that was at their level of neutral buoyancy, findings that are consistent with previous studies.

Widely-used Tropical Cyclone (TC) models include regional air-sea coupled dynamical models such as COAMPS-TC (Hao, et al, 2013), HWRF (Tallapragada, et al., 2014; Kim, et al., 2014) and GFDL (Bender et al., 2007; Gall, et al., 2011), global dynamical models such as GFS and ECMWF, and statistical-dynamical intensity-prediction models such as SHIPS, STIPS, L-GEM, RII (DeMaria and Kaplan, 1999; DeMaria, et al., 2005; Knaff et al., 2005; Jones, et al., 2006; DeMaria, 2009; DeMaria, 2010; Kaplan, et al., 2010). All of these models benefit from improved 3-D spatial observational plus enhanced temporal resolution, i.e. better 4-D capability. The need for enhanced 4-D profile observations is driven by the need for enhanced model resolution of the physics of small-scale processes such as convective events, boundary layer air-sea transfer processes and upper troposphere outflow jets. These requirements demand a concurrent enhancement in 4-D profile observational capability at finer spatial and temporal scales. Observations and observational strategies for initial condition specification and forecast validation within and around TCs require continual improvement to match these model demands while providing a basis for improvements in process understanding and parameterization on increasingly smaller scales.

Biogenic isoprene fluxes were measured onboard the CIRPAS Twin Otter aircraft as part of the California Airborne Biogenic volatile organic compound (BVOC) Emission Research in Natural Ecosystem Transects (CABERNET) campaign during June 2011. The airborne virtual disjunct eddy covariance (AvDEC) approach used measurements from a proton transfer reaction mass spectrometer (PTR–MS) and a wind radome probe to directly determine fluxes of isoprene over 7400 km of flight paths focusing on areas of California predicted to have the largest emissions. The fast Fourier transform (FFT) approach was used to calculate fluxes of isoprene over long transects of more than 15 km, most commonly between 50 and 150 km. The continuous wavelet transformation (CWT) approach was used over the same transects to also calculate instantaneous isoprene fluxes with localization of both frequency and time independent of non-stationarities. Fluxes were generally measured by flying consistently at 400m±50m (a.g.l.) altitude, and extrapolated to the surface according to the determined flux divergence determined in the racetrack-stacked profiles. The wavelet-derived surface fluxes of isoprene averaged to 2 km spatial resolution showed good correspondence to basal emission factor (BEF) land-cover data sets used to drive BVOC emission models. The surface flux of isoprene was close to zero over Central Valley crops and desert shrublands, but was very high (up to 15 mgm−2 h−1) above oak woodlands, with clear dependence of emissions on temperature and oak density. Isoprene concentrations of up to 8 ppb were observed at aircraft height on the hottest days and over the dominant source regions.

During the 2011 Eastern Pacific Emitted Aerosol Cloud Experiment (E-PEACE) and 2013 Nucleation in California Experiment (NiCE) field campaigns, a predominantly organic aerosol (> 85% by mass) was observed in the free troposphere over marine stratocumulus off the coast of California. These particles originated from a densely forested region in the Northwestern United States. The organic mass spectrum resolved by positive matrix factorization is consistent with the mass spectra of previously measured biogenic organic aerosol. Particulate organic mass exhibits a latitudinal gradient that corresponds to the geographical distribution of vegetation density and composition, with the highest concentration over regions impacted by densely populated monoterpene sources. Due to meteorological conditions during summer months, cloud-clearing events transport aerosol from the Northwestern United States into the free troposphere above marine stratocumulus. Based on the variation of meteorological variables with altitude, dry air containing enhanced biogenic organic aerosol is shown to entrain into the marine boundary layer. Fresh impacts on cloud water composition are observed north of San Francisco, CA which is consistent with fresh continental impacts on the marine atmosphere at higher latitudes. Continental aerosol size distributions are bimodal. Particles in the 100 nm mode are impacted by biogenic sources, while particles in the ~ 30 nm mode may originate from fresh biogenic emissions. Continental aerosol in the 100 nm mode is cloud condensation nuclei active and may play a role in modulating marine stratocumulus microphysics.

In-situ aircraft measurements of aerosol chemical and cloud microphysical properties were conducted during the CalWater campaign in February and March 2011 over the Sierra Nevada Mountains and the coastal waters of central California. The main objective was to elucidate the impacts of aerosol properties on clouds and precipitation forming processes. In order to accomplish this, we compared contrasting cases of clouds that ingested aerosols from different sources. The results showed that clouds containing pristine oceanic air had low cloud drop concentrations and started to develop rain 500 m above their base. This occurred both over the ocean and over the Sierra Nevada, mainly in the early morning when the radiatively cooled stable continental boundary layerwas decoupled fromthe cloud base. Supercooled rain dominated the precipitation that formed in growing convective clouds in the pristine air, up to the −21 °C isotherm level. A contrasting situation was documented in the afternoon over the foothills of the Sierra Nevada, when the clouds ingested high pollution aerosol concentrations produced in the Central Valley. This led to slow growth of the cloud drop effective radius with height and suppressed and even prevented the initiation of warm rain while contributing to the development of ice hydrometeors in the form of graupel. Our results show that cloud condensation and ice nuclei were the limiting factors that controlled warm rain and ice processes, respectively,while the unpolluted clouds in the same air mass produced precipitation quite efficiently. These findings provide the motivation for deeper investigations into the nature of the aerosols seeding clouds.

Highly supercooled rain and drizzle from cloud tops at 12 to 21 C down to the 0 isotherm was documented by aircraft observations in clouds over a wide range of meteorological situations under relatively pristine marine aerosol conditions. The Gulfstream-1 aircraft during the CalWater campaign in February and early March 2011 measured clouds over the coastal waters of northern California, orographically triggered convective clouds over the foothills of the Sierra Nevada, and orographic layer clouds over Yosemite National Park. Supercooled drizzle in layer clouds near Juneau, Alaska, was measured by the Wyoming King Air as part of a FAA project to study aircraft icing in this region. Low concentrations of cloud condensation nuclei (CCN) were commonly observed in all of these clouds, allowing for the formation of clouds with small concentrations of mostly large drops that coalesced into supercooled drizzle and raindrops. Another common observation was the absence of ice nuclei (IN) and/or ice crystals in measurable concentrations, associated with persistent supercooled drizzle and rain. Average ice crystal concentrations were 0.007 l 1 at the top of convective clouds at 12 C and 0.03 l 1 in the case of layer clouds at 21 C. In combination, these two conditions of low concentrations of CCN and very few IN provide ideal conditions for the formation of highly supercooled drizzle and rain. These results help explain the anomalously high incidences of aircraft icing at cold temperatures in U.S. west coast clouds and highlight the need to include aerosol effects when simulating aircraft icing with cloud models.

An aircraft field study (POST; Physics of Stratocumulus Top) was conducted off the central California coast in July and August 2008 to deal with the known difficulty of measuring entrainment rates in the radiatively important stratocumulus (Sc) prevalent in that area. The Center for Interdisciplinary Remotely-Piloted Aircraft Studies Twin Otter research aircraft flew 15 quasi-Lagrangian flights in unbroken Sc and carried a full complement of probes including three high-data-rate probes: ultrafast temperature probe, particulate volume monitor probe, and gust probe. The probes’ colocation near the nose of the Twin Otter permitted estimation of entrainment fluxes and rates with an in-cloud resolution of 1m. Results include the following: Application of the conditional sampling variation of classical mixed layer theory for calculating the entrainment rate into cloud top for POST flights is shown to be inadequate for most of the Sc. Estimated rates resemble previous results after theory is modified to take into account both entrainment and evaporation at cloud top given the strong wind shear and mixing at cloud top. Entrainment rates show a tendency to decrease for large shear values, and the largest rates are for the smallest temperature jumps across the inversion. Measurements indirectly suggest that entrained parcels are primarily cooled by infrared flux divergence rather than cooling from droplet evaporation, while detrainment at cloud top causes droplet evaporation and cooling in the entrainment interface layer above cloud top.

Airborne flux measurements of isoprene were performed over the Californian oak belts surrounding the Central Valley. The authors demonstrate for the first time 1) the feasibility of airborne eddy covariance measurements of reactive biogenic volatile organic compounds; 2) the effect of chemistry on the vertical transport of reactive species, such as isoprene; and 3) the applicability of wavelet analysis to estimate regional fluxes of biogenic volatile organic compounds. These flux measurements demonstrate that instrumentation operating at slower response times (e.g., 1–5 s) can still be used to determine eddy covariance fluxes in the mixed layer above land, where typical length scales of 0.5–3km were observed. Flux divergence of isoprene measured in the planetary boundary layer (PBL) is indicative of OH densities in the range of 4–7 3 106 molecules per cubic centimeter and allows extrapolation of airborne fluxes to the surface with Damk€ohler numbers (ratio between the mixing time scale and the chemical time scale) in the range of 0.3–0.9. Most of the isoprene is oxidized in the PBL with entrainment fluxes of about 10% compared to the corresponding surface fluxes. Entrainment velocities of 1–10 cm s21 were measured. The authors present implications for parameterizing PBL schemes of reactive species in regional and global models.

We analyse the cloud microphysical response to entrainment mixing in warm cumulus clouds observed from the CIRPAS Twin Otter during the GoMACCS field campaign near Houston, Texas, in summer 2006. Cloud drop size distributions and cloud liquid water contents from the Artium Flight phase-Doppler interferometer in conjunction with meteorological observations are used to investigate the degree to which inhomogeneous versus homogeneous mixing is preferred as a function of height above cloud base, distance from cloud edge and aerosol concentration. Using four complete days of data with 101 cloud penetrations (minimum 300m in length), we find that inhomogeneous mixing primarily explains liquid water variability in these clouds. Furthermore, we show that there is a tendency for mixing to be more homogeneous towards the cloud top, which we attribute to the combination of increased turbulent kinetic energy and cloud drop size with altitude which together cause the Damko¨ hler number to increase by a factor of between 10 and 30 from cloud base to cloud top. We also find that cloud edges appear to be air from cloud centres that have been diluted solely through inhomogeneous mixing. Theory predicts the potential for aerosol to affect mixing type via changes in drop size over the range of aerosol concentrations experienced (moderately polluted rural sites to highly polluted urban sites). However, the observations, while consistent with this hypothesis, do not show a statistically significant effect of aerosol on mixing type.

An unusually intense African dust event affected a large area of the western Atlantic and eastern Caribbean in early April 2010. Measurements made east of Barbados from the Center for Interdisciplinary Remotely Piloted Aircraft Studies (CIRPAS) Twin Otter research aircraft are used to characterize particle size distributions; vertical distributions of aerosols, temperature, and moisture; and processes leading to the observed stratification in the boundary layer. The vertical profiles of various aerosol characterizations were similar on both days and show three layers with distinct aerosol and thermodynamic characteristics: the Saharan Air Layer (SAL; ~2.2 km 500 m), a subcloud layer (SCL; surface to ~500m), and an intermediate layer extending between them. The SAL and SCL display well-mixed aerosol and thermodynamic characteristics; but the most significant horizontal and vertical variations in aerosols and thermodynamics occur in the intermediate layer. The aerosol variability observed in the intermediate layer is likely associated withmodification by shallow cumulus convection occurring sometime in the prior history of the air mass as it is advected across the Atlantic. A comparison of the thermodynamic structure observed in the event from its origin over Africa with that when it reached Barbados indicates that the lower part of the SAL was moistened by surface fluxes as the air mass was advected across the Atlantic. Mixing diagrams using aerosol concentrations and water vapor mixing ratios as conserved parameters provide insight into the vertical transports and mixing processes that may explain the observed aerosol and thermodynamic variability in each layer.

Aircraft sampling of the stratocumulus-topped boundary layer (STBL) during the Physics of Stratocumulus Top (POST) experiment was primarily achieved using sawtooth flight patterns, during which the atmospheric layer 100m above and below cloud top was sampled at a frequency of once every 2 min. The large data set that resulted from each of the 16 flights document the complex structure and variability of this interfacial region in a variety of conditions. In this study, we first describe some properties of the entrainment interface layer (EIL), where strong gradients in turbulent kinetic energy (TKE), potential temperature and moisture can be found. We find that defining the EIL by the first two properties tends to yield similar results, but that moisture can be a misleading tracer of the EIL. These results are consistent with studies using large-eddy simulations. We next utilize the POST data to shed light on and constrain processes relevant to entrainment, a key process in the evolution of the STBL that to-date is not well-represented even by high resolution models. We define “entrainment efficiency” as the ratio of the TKE consumed by entrainment to that generated within the STBL (primarily by cloud-top cooling). We find values for the entrainment efficiency that vary by 1.5 orders of magnitude, which is even greater than the one order magnitude that previous modeling results have suggested. Our analysis also demonstrates that the entrainment efficiency depends on the strength of the stratification of the EIL, but not on the TKE in the cloud top region. The relationships between entrainment efficiency and other STBL parameters serve as novel observational constraints for simulations of entrainment in such systems.

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.

This study investigates the ability of a droplet activation parameterization (which considers the effects of entrainment and mixing) to reproduce observed cloud droplet number concentration (CDNC) in ambient clouds. Predictions of the parameterization are compared against cloud averages of CDNC from ambient cumulus and stratocumulus clouds sampled during CRYSTAL‐FACE (Key West, Florida, July 2002) and CSTRIPE (Monterey, California, July 2003), respectively. The entrainment parameters required by the parameterization are derived from the observed liquid water content profiles. For the cumulus clouds considered in the study, CDNC is overpredicted by 45% with the adiabatic parameterization. When entrainment is accounted for, the predicted CDNC agrees within 3.5%. Cloud‐averaged CDNC for stratocumulus clouds is well captured when entrainment is not considered. In all cases considered, the entraining parameterization compared favorably against a statistical correlation developed from observations to treat entrainment effects on droplet number. These results suggest that including entrainment effects in the calculation of CDNC, as presented here, could address important overprediction biases associated with using adiabatic CDNC to represent cloud‐scale average values.

Aircraft-based measurements of aerosol lightscattering coefficient, cloud condensation nuclei (CCN) measured directly or by proxy, and aerosol chemical composition are reported for three different years in the region of the large stratocumulus deck off the California coast. Receptor modeling is used to differentiate the contributions of the main aerosol sources to the light scattering and CCN activity. The contribution of anthropogenic sources to the two climatically important aerosol parameters (for direct and indirect forcing) varied from year to year but, on average, was found to be 67% in the case of CCN concentration and 57% in the case of light-scattering coefficient.

Airborne measurements in regions of varying meteorology and pollution are used to quantify the contribution of organic acids and a mass spectral marker for oxygenated aerosols, m/z 44, to the total organic aerosol budget. Organic acids and m/z 44 separately are shown to exhibit their highest organic mass fractions in the vicinity of clouds. The contribution of such oxygenated species is shown to increase as a function of relative humidity, aerosol hygroscopicity (and decreasing organic mass fraction), and is typically greater off the California coast versus the continental atmospheres studied. Reasons include more efficient chemistry and partitioning of organic acid precursors with increasing water in the reaction medium, and high aqueous‐phase processing times in boundary layers with higher cloud volume fractions. These results highlight the importance of secondary organic aerosol formation in both wet aerosols and cloud droplets.

Surface, airborne, and satellite measurements over the eastern Pacific Ocean off the coast of California during the period between 2005 and 2007 are used to explore the relationship between ocean chlorophyll a, aerosol, and marine clouds. Periods of enhanced chlorophyll a and wind speed are coincident with increases in particulate diethylamine and methanesulfonate concentrations. The measurements indicate that amines are a source of secondary organic aerosol in the marine atmosphere. Subsaturated aerosol hygroscopic growth measurements indicate that the organic component during periods of high chlorophyll a and wind speed exhibit considerable water uptake ability. Increased average cloud condensation nucleus (CCN) activity during periods of increased chlorophyll a levels likely results from both size distribution and aerosol composition changes. The available data over the period of measurements indicate that the cloud microphysical response, as represented by either cloud droplet number concentration or cloud droplet effective radius, is likely influenced by a combination of atmospheric dynamics and aerosol perturbations during periods of high chlorophyll a concentrations.

In this study, we evaluate eight autoconversion parameterizations against integration of the Kinetic Collection Equation (KCE) for cloud size distributions measured during the NASA CRYSTAL-FACE and CSTRIPE campaigns. KCE calculations are done using both the observed data and fits of these data to a gamma distribution function; it is found that the fitted distributions provide a good approximation for calculations of total coalescence but not for autoconversion because of fitting errors near the drop-drizzle separation size. Parameterizations that explicitly compute autoconversion tend to be in better agreement with KCE but are subject to substantial uncertainty, about an order of magnitude in autoconversion rate. Including turbulence effects on droplet collection increases autoconversion by a factor of 1.82 and 1.24 for CRYSTAL-FACE and CSTRIPE clouds, respectively; this enhancement never exceeds a factor of 3, even under the most aggressive collection conditions. Shifting the droplet-drizzle separation radius from 20 to 25 mm results in about a twofold uncertainty in autoconversion rate. The polynomial approximation to the gravitation collection kernel used to develop parameterizations provides computation of autoconversion that agree to within 30%. Collectively, these uncertainties have an important impact on autoconversion but are all within the factor of 10 uncertainty of autoconversion parameterizations. Incorporating KCE calculations in GCM simulations of aerosol-cloud interactions studies is computationally feasible by using precalculated collection kernel tables and can quantify the autoconversion uncertainty associated with application of parameterizations.

This work examines the efficacy of various physically based approaches derived from one-dimensional adiabatic parcel model frameworks (a numerical model and a simplified parameterization) to parameterize the cloud droplet distribution characteristics for computing cloud effective radius and autoconversion rate in regional/global atmospheric models. Evaluations are carried out for integrations with single (average) and distributions of updraft velocity, assuming that (1) conditions at smax are reflective of the cloud column or (2) cloud properties vary vertically, in agreement with one-dimensional parcel theory. The predicted droplet distributions are then compared against in situ cloud droplet observations obtained during the CRYSTAL-FACE and CSTRIPE missions. Good agreement of droplet relative dispersion between parcel model frameworks indicates that the parameterized parcel model essentially captures one-dimensional dynamics; the predicted distributions are overly narrow, with relative dispersion being a factor of 2 lower than observations. However, if conditions at cloud maximum supersaturation are used to predict relative dispersion and applied throughout the cloud column, better agreement is seen with observations, especially if integrations are carried out over the distribution of updraft velocity. When considering the efficiency of the method, calculating cloud droplet spectral dispersion at smax is preferred for linking aerosol with droplet distributions in large-scale models.

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.

We report an extensive airborne characterization of aerosol downwind of a massive bovine source in the San Joaquin Valley (California) on two flights during July 2007. The Center for Interdisciplinary Remotely-Piloted Aircraft Studies (CIRPAS) Twin Otter probed chemical composition, particle size distribution, mixing state, sub- and supersaturated water uptake behavior, light scattering properties, and the interrelationship between these parameters and meteorology. Total PM1.0 levels and concentrations of organics, nitrate, and ammonium were enhanced in the plume from the source as compared to the background aerosol. Organics dominated the plume aerosol mass (∼56–64%), followed either by sulfate or nitrate, and then ammonium.

We present statistical comparisons of properties of clouds generated by Large Eddy Simulations (LES) with aircraft observations of nonprecipitating, warm cumulus clouds made in the vicinity of Houston, TX during the Gulf of Mexico Atmospheric Composition and Climate Study (GoMACCS), carried out in the summer of 2006. Aircraft data were sampled with the Center for Interdisciplinary Remotely Piloted Aircraft Studies (CIRPAS) Twin Otter airplane. Five flights (days) that are most suitable for studying aerosol-cloud interactions are selected from the 22 flights. The model simulations are initiated with observed environmental profiles. The simulations are used to generate an ensemble of thousands of cumulus clouds for statistically meaningful evaluations. Statistical comparisons focus on the properties of a set of dynamical and thermodynamical variables, sampled either in the cloud or the cloud updraft core. The set of variables includes cloud liquid water content (LWC), number mixing ratio of cloud droplets (Nd), cloud effective radius (re), updraft velocity (w), and the distribution of cloud sizes. In general, good agreement between the simulated and observed clouds is achieved in the normalized frequency distribution functions, the profiles averaged over the cloudy regions, the cross-cloud averages, and the cloud size distributions, despite big differences in sample size between the model output and the aircraft data. Some unresolved differences in frequency distributions of w and possible differences in cloud fraction are noted. These comparisons suggest that the LES is able to successfully generate the cumulus cloud populations that were present during GoMACCS. The extent to which this is true will depend on the specific application.

Aircraft – based measurements of aerosol hygroscopicity, both in the form of sizeresolved, diameter growth factors and in the dependence of particle light scattering on relative humidity, are presented for the marine boundary layer of the southern California coastal zone. The chemical composition of the aerosol is collated with the hygroscopicity data, both to examine the nature of aerosol aging and as input for receptor type modeling. The data suggest an increase in aerosol hygroscopicity with altitude, possibly associated with oxidation of organic films. The receptor modeling suggests three distinct aerosol types/sources for this venue: marine, biomass burning and pollution. Model output is used in regression analyses to derive a prognostic mixing rule for the hygroscopicity of aerosol with these three sources.

A new instrument to measure the size-resolved hygroscopic growth of both sub- and super-micron atmospheric aerosol is described. It consists of two white-light optical particle counters measuring the same sample aerosol simultaneously at two different controlled relative humidities. Calibration with aerosols of different refractive index confirms the expected relative insensitivity of the instrument to index of refraction. Data obtained in the field from airborne sampling support the utility of the instrument in measuring differences in size-resolved hygroscopicity in the marine boundary layer and also in addressing the issue of kinetic limitations to aerosol condensational growth.

Giant hygroscopic aerosols were introduced into a solid marine stratocumulus cloud (200 m thick) by burning hygroscopic flares mounted on an aircraft. The cloud microphysical response in two parallel seeding plumes was observed using an instrumented aircraft making 16 transects of the plumes. The cloud drop size distribution width increased in the plumes due to an increased number of small cloud drops (3–5 mm) on the earlier transects and a 5-fold increase in the number of large drops (20–40 mm) relative to the background cloud 30 minutes later. The cloud effective diameter increased from about 11 mm in the background to 13 mm in the plumes. Although the giant nuclei were only a small fraction of the total aerosols produced by the flares, they dominated the cloud response. The merit of the seeding approach for controlled observational studies of aerosol-cloud interactions in marine stratocumulus was demonstrated.

Observations from a suite of platforms deployed in the coastal ocean are being combined with numerical models and simulations to investigate the processes that couple the atmosphere and ocean.

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 microphysical and optical properties were measured on board the CIRPAS Twin Otter aircraft during 16 flights at the Southern Great Plain (SGP) site in northern central Oklahoma as part of the Aerosol Intensive Operation period in May 2003. Within well-mixed boundary layers on four cloudy days, vertical profiles measured on board the Twin Otter show that dry aerosol size, volume concentration, and scattering coefficients all increased with increasing altitude, whereas the total number concentration remained essentially constant. A one-dimensional model, which uses simultaneous meteorological measurements as inputs, shows that the observed increase in aerosol volume concentration with increasing altitude is consistent with in-cloud sulfate production at the top of the boundary layer. The sulfate production rate was sufficiently fast to overcome the homogenization resulting from turbulent mixing. In contrast, on cloud-free days, measurements on a second aircraft show nearly uniform aerosol volume concentrations within well-mixed boundary layers. The observed vertical gradients in aerosol volume concentration suggest that even within well-mixed boundary layers, surface measurements may not be representative of aerosols properties (e.g., loading and scattering coefficients, etc.) at elevated altitudes, especially when SO2 concentration and cloud coverage are high.

During the July 2005 Marine Stratus/Stratocumulus Experiment (MASE) and the August-September 2006 Gulf of Mexico Atmospheric Composition and Climate Study (GoMACCS), the Center for Interdisciplinary Remotely-Piloted Aircraft Studies (CIRPAS) Twin Otter probed aerosols and cumulus clouds in the eastern Pacific Ocean off the coast of northern California and in southeastern Texas, respectively. An on-board particle-into-liquid sampler (PILS) quantified inorganic and organic acid species with e5- min time resolution. Ubiquitous organic aerosol layers above cloud with enhanced organic acid levels were observed in both locations. The data suggest that aqueousphase reactions to produce organic acids, mainly oxalic acid, followed by droplet evaporation is a source of elevated organic acid aerosol levels above cloud. Oxalic acid is observed to be produced more efficiently relative to sulfate as the cloud liquid water content increases, corresponding to larger and less acidic droplets. As derived from large eddy simulations of stratocumulus under the conditions of MASE, both Lagrangian trajectory analysis and diurnal cloudtop evolution provide evidence that a significant fraction of the aerosol mass concentration above cloud can be accounted for by evaporated droplet residual particles. Methanesulfonate data suggest that entrainment of free tropospheric aerosol can also be a source of organic acids above boundary layer clouds.

Measurements of both horizontal gradients and vertical profiles of aerosols, cloud droplets and thermodynamic parameters in the cloud topped marine boundary layer off of central California are presented. They suggest that, while aerosols can indeed modulate cloud albedo, other parameters such as sea surface temperature may similarly affect cloud albedo. Additionally, the impact of aerosols, through sedimentation and precipitation, on cloud optical depths and thus albedo is not always in accord with conventional expectations and can either enhance or decrease the albedo, depending on ambient conditions. Taken together, these results suggest that current estimates of indirect forcing by aerosols could be significantly in error.

The Department of Energy conducted the Cloud-Land Surface Interaction Campaign (CLASIC) in Poncha City Oklahoma, in June 2007. The purpose of the experiment was to study the influence of different surface conditions on properties of small cumulus clouds. The Oklahoma site provided climatologically arid surface in the western part of the state, and lush green conditions in the eastern part. The summer of 2007, however, was exceptionally wet, with flooded fields and rivers flowing over their banks. This had seriously adverse effect on the experiment.

Measurements were made by a new cloud condensation nuclei (CCN) instrument (CCNC3) during the Atmospheric Radiation Measurement (ARM) Program’s Aerosol Intensive Observational Period (IOP) in May 2003 in Lamont, Oklahoma. An inverse aerosol/CCN closure study is undertaken, in which the predicted number concentration of particles available for activation (NP) at the CCNC3 operating supersaturations is compared to that observed (NO). NP is based on Ko¨hler Theory, with assumed and inferred aerosol composition and mixing state, and the airborne aerosol size distribution measured by the Caltech Dual Automatic Classified Aerosol Detector (DACAD). An initial comparison of NO and NP, assuming the ambient aerosol is pure ammonium sulfate ((NH4)2SO4), results in closure ratios (NP/NO) ranging from 1.18 to 3.68 over the duration of the IOP, indicating that the aerosol is less hygroscopic than (NH4)2SO4. NP and NO are found to agree when the modeled aerosol population has characteristics of an external mixture of particles, in which insoluble material is preferentially distributed among particles with small diameters (<50 nm) and purely insoluble particles are present over a range of diameters. The classification of sampled air masses by closure ratio and aerosol size distribution is discussed in depth. Inverse aerosol/CCN closure analysis can be a valuable means of inferring aerosol composition and mixing state when direct measurements are not available, especially when surface measurements of aerosol composition and mixing state are not sufficient to predict CCN concentrations at altitude, as was the case under the stratified aerosol layer conditions encountered during the IOP.

During May 2003 the Department of Energy’s Atmospheric Radiation Measurement Program conducted an Intensive Operations Period (IOP) to measure the radiative effects of aerosol and clouds. A suite of both in situ and remote sensing measurements were available to measure aerosol and cloud parameters. This paper has three main goals: First, it focuses on comparison between in situ retrievals of the radiatively important drop effective radius re and various satellite, airborne, and surface remote sensing retrievals of the same parameter. On 17 May 2003, there was a fortuitous, near-simultaneous sampling of a stratus cloud by five different methods. The retrievals of re agree with one another to within !20%, which is approximately the error estimate for most methods. Second, a methodology for deriving a best estimate of re from these different instruments, with their different physical properties and sampling volumes, is proposed and applied to the 17 May event. Third, the paper examines the response of re to changes in aerosol on 3 days during the experiment and examines the consistency of remote sensing and in situ measurements of the effect of aerosol on re. It is shown that in spite of the generally good agreement in derived re, the magnitude of the response of re to changes in aerosol is quite sensitive to the method of retrieving re and to the aerosol proxy for cloud condensation nuclei. Nonphysical responses are sometimes noted, and it is suggested that further work needs to be done to refine these techniques.

Values for Mie-equivalent aerosol asymmetry parameter (g) were derived using a variety of methods from the large suite of measurements (in situ and remote from surface and aircraft) made in Oklahoma during the 2003 aerosol Intensive Operations Period (IOP). Median values derived for dry asymmetry parameter at 550 nm ranged between 0.55 and 0.63 over all instruments and for all derivation methods, with the exception of one instrument which did not measure over the full size range of optically important aerosol. Median values for the ‘‘wet’’ asymmetry parameter (i.e., asymmetry parameter at humidity conditions closer to ambient) were between 0.59 and 0.72. Values for g derived for surface and airborne in situ measurements were highly correlated, but in situ and remote sensing measurements both at the surface and aloft did not agree as well because of vertical inhomogeneity of the aerosol. Radiative forcing calculations suggest that a 10% decrease in g would result in a 19% reduction in top of atmosphere radiative forcing for the conditions observed during the IOP. Comparison of the different methods for deriving g suggests that in computing the asymmetry parameter, aerosol size is the most important parameter to measure; composition is less important except for how it influences the hygroscopic growth (i.e., size) of particles.

In May 2003, the Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) Program sponsored the Aerosol Intensive Operating Period (AIOP) which was conducted over the ARM Climate Research Facility (ACRF) in central Oklahoma. One new instrument that flew in the AIOP, called Cadenza, employed a cavity ring-down technique to measure extinction coefficient and a reciprocal nephelometer technique to simultaneously measure scattering coefficient. This instrument is described in this paper, and measurements are compared to those of conventional instrumentation. Agreement between Cadenza extinction coefficient and that derived from combining nephelometer scattering and PSAP absorption (Neph + PSAP) was excellent, about 2%. Agreement between Cadenza scattering coefficient and TSI nephelometer scattering was also excellent, about 2%, well within the uncertainty of the nephelometer and Cadenza scattering measurements. Comparisons between these instruments, made for the special case of plumes, showed that Cadenza measured extinction and scattering several percent higher on average than the Neph + PSAP and nephelometer alone. This difference is likely due to differences in the instrument response time: The response time for Cadenza is 1 s while that for the nephelometer is a minimum of 8 s. Plumes, identified as originating from Siberian biomass burning, are characterized. Composite size distributions from wing-mounted probes showed that two of the plumes had significant large particle modes that resulted in high values of the effective radius. The effect of the large particle mode was not seen in the A ° ngstro¨m coefficient calculated from the in-cabin scattering measurements because of the characteristics of the aircraft inlet.

Aerosol size distributions were measured by a Scanning Mobility Particle Sizer (SMPS) on board the CIRPAS Twin Otter aircraft during 16 flights at the Southern Great Plains (SGP) site in northern central Oklahoma as part of the Aerosol Intensive Operation period in May 2003. During the same period a second SMPS was deployed at a surface station and provided continuous measurements. Combined with trace gas measurements at the SGP site and back trajectory analysis, the aerosol size distributions provided insights into the sources of aerosols observed at the SGP site. High particle concentrations, observed mostly during daytime, were well correlated with the sulfur dioxide (SO2) mixing ratios, suggesting nucleation involving sulfuric acid is likely the main source of newly formed particles at the SGP. Aerosols within plumes originating from wildfires in Central America were measured at the surface site. Vertically compact aerosol layers, which can be traced back to forest fires in East Asia, were intercepted at altitudes over 3000 m. Analyses of size-dependent particle growth rates for four periods during which high cloud coverage was observed indicate growth dominated by volume controlled reactions. Sulfate accounts for 50% to 72% of the increase in aerosol volume concentration; the rest of the volume concentration increase was likely due to secondary organic species. The growth law analyses and meteorological conditions indicate that the sulfate was produced mainly through aqueous oxidation of SO2 in clouds droplets and hydrated aerosol particles.

Raman lidar water vapor and aerosol extinction profiles acquired during the daytime over the Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) Southern Great Plains (SGP) site in northern Oklahoma (36.606 N, 97.50 W, 315 m) are evaluated using profiles measured by in situ and remote sensing instruments deployed during the May 2003 Aerosol Intensive Operations Period (IOP). The automated algorithms used to derive these profiles from the Raman lidar data were first modified to reduce the adverse effects associated with a general loss of sensitivity of the Raman lidar since early 2002. The Raman lidar water vapor measurements, which are calibrated to match precipitable water vapor (PWV) derived from coincident microwave radiometer (MWR) measurements were, on average, 5–10% (0.3–0.6 g/m3) higher than the other measurements. Some of this difference is due to out-of-date line parameters that were subsequently updated in the MWR PWV retrievals. The Raman lidar aerosol extinction measurements were, on average, about 0.03 km 1 higher than aerosol measurements derived from airborne Sun photometer measurements of aerosol optical thickness and in situ measurements of aerosol scattering and absorption. This bias, which was about 50% of the mean aerosol extinction measured during this IOP, decreased to about 10% when aerosol extinction comparisons were restricted to aerosol extinction values larger than 0.15 km 1. The lidar measurements of the aerosol extinction/backscatter ratio and airborne Sun photometer measurements of the aerosol optical thickness were used along with in situ measurements of the aerosol size distribution to retrieve estimates of the aerosol single scattering albedo (wo) and the effective complex refractive index. Retrieved values of wo ranged from (0.91–0.98) and were in generally good agreement with wo derived from airborne in situ measurements of scattering and absorption. Elevated aerosol layers located between about 2.6 and 3.6 km were o

Aerosol samples were collected by aircraft during the summer of 2004 in the Northeastern Pacific and compared to measurements of aerosol hygroscopicity. Chemical speciation analyses of the samples revealed that a significant portion of the marine aerosols was organic, and on average 8% of the total aerosol mass was insoluble organic material, tentatively attributed to natural marine emissions. Two chemical models were explored in an attempt to achieve closure between the marine aerosol chemical and physical properties through reproduction of the observed aerosol growth, both in the subsaturated and supersaturated regimes. Results suggest that at subsaturated relative humidities, the nonideal behavior of water activity with respect to aerosol chemistry has an important effect on aerosol growth. At supersaturations, the underprediction of critical supersaturations by all models suggests the hypothesis that formation of a complete monolayer by the insoluble organics may inhibit the activation of aerosols to form cloud droplets.

Aerosol light absorption can be intense close to local sources such as wildland and oil fires, with smoke that disperses into the boundary layer and, with enough lift, into the upper atmosphere where it may be transported around the globe. Filter-based methods such as the Particle Soot Absorption Photometer (PSAP) are most commonly used to quantify aerosol light absorption aloft. This paper reports first measurements of aerosol light absorption aloft with photoacoustic instrumentation (PA). Three examples of aerosol light absorption are presented. The first one illustrates a case of detached layers aloft arising from intercontinental, interoceanic transport of smoke from wildland fires in Siberia to the North American continent and the measurement campaign held at the Department of Energy Atmospheric Radiation Measurement Program Climate Research Facility in north central Oklahoma. Then, two examples of intense local fire smoke light absorption from the Coastal Stratocumulus Imposed Perturbation Experiment near Marina, California, USA, are presented. The first local fire was an oil fire burning in a storage tank near Moss Landing, California, USA, and smoke from this fire was very dark, indicating a low single scattering albedo. By contrast, the second local fire was predominantly burning wood, vegetation, and structures near Fort Ord in Marina, California, USA, and the smoke was very bright, indicating a high single scattering albedo. In all examples, PA measurements at 676 nm were compared with those from a PSAP modified to measure at three wavelengths, including 660 nm.

Oxalic acid is often the leading contributor to the total dicarboxylic acid mass in ambient organic aerosol particles. During the 2004 International Consortium for Atmospheric Research on Transport and Transformation (ICARTT) field campaign, nine inorganic ions (including SO4 2!) and five organic acid ions (including oxalate) were measured on board the Center for Interdisciplinary Remotely Piloted Aircraft Studies (CIRPAS) Twin Otter research aircraft by a particle-into-liquid sampler (PILS) during flights over Ohio and surrounding areas. Five local atmospheric conditions were studied: (1) cloud-free air, (2) power plant plume in cloud-free air with precipitation from scattered clouds overhead, (3) power plant plume in cloud-free air, (4) power plant plume in cloud, and (5) clouds uninfluenced by local pollution sources. The aircraft sampled from two inlets: a counterflow virtual impactor (CVI) to isolate droplet residuals in clouds and a second inlet for sampling total aerosol. A strong correlation was observed between oxalate and SO4 2! when sampling through both inlets in clouds. Predictions from a chemical cloud parcel model considering the aqueous-phase production of dicarboxylic acids and SO4 2! show good agreement for the relative magnitude of SO4 2! and oxalate growth for two scenarios: power plant plume in clouds and clouds uninfluenced by local pollution sources. The relative contributions of the two aqueous-phase routes responsible for oxalic acid formation were examined; the oxidation of glyoxylic acid was predicted to dominate over the decay of longer-chain dicarboxylic acids. Clear evidence is presented for aqueous-phase oxalic acid production as the primary mechanism for oxalic acid formation in ambient aerosols.

In May 2003, a Twin Otter airplane, equipped with instruments for making in situ measurements of aerosol optical properties, was deployed during the Atmospheric Radiation Measurements (ARM) Program’s Aerosol Intensive Operational Period in Oklahoma. Several of the Twin Otter flights were flown in formation with an instrumented light aircraft (Cessna 172XP) that makes routine in situ aerosol profile flights over the site. This paper presents comparisons of measured scattering coefficients at 467 nm, 530 nm, and 675 nm between identical commercial nephelometers aboard each aircraft. Overall, the agreement between the two nephelometers decreases with longer wavelength. During the majority of the flights, the Twin Otter flew with a diffuser inlet while the Cessna had a 1 mm impactor, allowing for an estimation of the fine mode fraction aloft. The fine mode fraction aloft was then compared to the results of a ground-based nephelometer. Comparisons are also provided in which both nephelometers operated with identical 1 mm impactors. These scattering coefficient comparisons are favorable at the longer wavelengths (i.e., 530 nm and 675 nm), yet differed by approximately 30% at 467 nm. Mie scattering calculations were performed using size distribution measurements, made during the level flight legs. Results are also presented from Cadenza, a new continuous wave cavity ring-down (CW-CRD) instrument, which compared favorably (i.e., agreed within 2%) with data from other instruments aboard the Twin Otter. With this paper, we highlight the significant implications of coarse mode (larger than 1 mm) aerosol aloft with respect to aerosol optical properties.