, with an average of 0.172 mg m À3 . Lower concentrations were measured in the Basin outflow regions and above the inversion layer. The SP2 afforded a quantification of the mixing state of rBC aerosols through modeling the scattering cross-section with a core-and-shell Mie model to determine coating thickness. The rBC particles above the inversion layer were more thickly coated by a light-scattering substance than those below, indicating a more aged aerosol in the free troposphere. Near the surface, as the LA plume is advected from west to east with the sea breeze, a coating of scattering material grows on rBC particles, coincident with a clear growth of ammonium nitrate within the LA Basin and the persistence of water-soluble organic compounds as the plume travels through the outflow regions. Detailed analysis of the rBC mixing state reveals two modes of coated rBC particles; a mode with smaller rBC core diameters ($90 nm) but thick (>200 nm) coating diameters and a mode with larger rBC cores ($145 nm) with a thin (<75 nm) coating. The "weekend effect" in the LA Basin results in more thickly coated rBC particles, coinciding with more secondary formation of aerosol.

Aircraft‐based measurements of aerosol composition, either bulk or single‐particle, and both subsaturated and supersaturated hygroscopicity were made in the Los Angeles Basin and its outflows during May 2010 during the CalNex field study. Aerosol composition evolves from source‐rich areas in the western Basin to downwind sites in the eastern Basin, evidenced by transition from an external to internal mixture, as well as enhancements in organic O : C ratio, the amount of organics and nitrate internally mixed on almost all particle types, and coating thickness on refractory black carbon (rBC). Transport into hot, dilute outflow regions leads to significant volatilization of semivolatile material, resulting in a unimodal aerosol comprising primarily oxygenated, low‐volatility, water‐soluble organics and sulfate. The fraction of particles with rBC or soot cores is between 27 and 51% based on data from a Single Particle Soot Photometer (SP2) and Aerosol Time of Flight Mass Spectrometer (ATOFMS). Secondary organics appear to inhibit subsaturated water uptake in aged particles, while CCN activity is enhanced with photochemical age. A biomass‐burning event resulted in suppression of subsaturated hygroscopicity but enhancement in CCN activity, suggesting that BB particles may be nonhygroscopic at subsaturated RH but are important sources of CCN. Aerosol aging and biomass burning can lead to discrepancies between subsaturated and supersaturated hygroscopicity that may be related to mixing state. In the cases of biomass burning aerosol and aged particles coated with secondary material, more than a single parameter representation of subsaturated hygroscopicity and CCN activity is needed.

[1] 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.

Abstract. This study utilizes large eddy simulation, aircraft measurements, and satellite observations to identify factors that bias the absolute magnitude of metrics of aerosol-cloudprecipitation interactions for warm clouds. The metrics considered are precipitation susceptibility S o , which examines rain rate sensitivity to changes in drop number, and a cloudprecipitation metric, χ, which relates changes in rain rate to those in drop size. While wide ranges in rain rate exist at fixed cloud drop concentration for different cloud liquid water amounts, χ and S o are shown to be relatively insensitive to the growth phase of the cloud for large datasets that include data representing the full spectrum of cloud lifetime. Spatial resolution of measurements is shown to influence the liquid water path-dependent behavior of S o and χ. Other factors of importance are the choice of the minimum rain rate threshold, and how to quantify rain rate, drop size, and the cloud condensation nucleus proxy. Finally, low biases in retrieved aerosol amounts owing to wet scavenging and high biases associated with above-cloud aerosol layers should be accounted for. The paper explores the impact of these effects for model, satellite, and aircraft data.

This study utilizes large eddy simulation, aircraft measurements, and satellite observations to identify factors that bias the absolute magnitude of metrics of aerosol-cloud-precipitation interactions for warm clouds. The metrics considered are precipitation susceptibility <i>S_o</i>, which examines rain rate sensitivity to changes in drop number, and a cloud-precipitation metric, &chi;, which relates changes in rain rate to those in drop size. While wide ranges in rain rate exist at fixed cloud drop concentration for different cloud liquid water amounts, &chi; and <i>S_o</i> are shown to be relatively insensitive to the growth phase of the cloud for large datasets that include data representing the full spectrum of cloud lifetime. Spatial resolution of measurements is shown to influence both the magnitude and liquid water path-dependent behavior of <i>S_o</i> and &chi;. Other factors of importance are the choice of how to quantify rain rate, drop size, and the cloud condensation nucleus proxy. Finally, low biases in retrieved aerosol amounts owing to wet scavenging and high biases associated with above-cloud aerosol layers should be accounted for. The paper explores the impact of these effects for model, satellite, and aircraft data

We report airborne organic aerosol (OA) measurements over Los Angeles carried out in May 2010 as part of the CalNex field campaign. The principal platform for the airborne data reported here was the CIRPAS Twin Otter (TO); airborne data from NOAA WP‐3D aircraft and Pasadena CalNex ground‐site data acquired during simultaneous TO flybys are also presented. Aerodyne aerosol mass spectrometer measurements constitute the main source of data analyzed. The increase in organic aerosol oxidation from west to east in the basin was sensitive to OA mass loading, with a greater spatial trend in O:C associated with lower mass concentration. Three positive matrix factorization (PMF) components (hydrocarbon‐like organic aerosol (HOA), semi‐volatile oxidized organic aerosol (SVOOA), and low volatility oxidized organic aerosol (LVOOA)) were resolved for the one flight that exhibited the largest variability in estimated O:C ratio. Comparison of the PMF factors with two optical modes of refractory black carbon (rBC)‐containing aerosol revealed that the coating of thinly coated rBC‐containing aerosol, dominant in the downtown region, is likely composed of HOA, whereas more thickly coated rBC‐containing aerosol, dominant in the Banning pass outflow, is composed of SVOOA and LVOOA. The correlation of water‐soluble organic mass to oxidized organic aerosol (OOA) is higher in the outflows than in the basin due to the higher mass fraction of OOA/OA in the outflows. By comparison, the average OA concentration over Mexico City MILAGRO (Megacity Initiative: Local and Global Research Observations) campaign was ∼7 times higher than the airborne average during CalNex.

Two case studies are discussed that evaluate the effect of ocean emissions on aerosol-cloud interactions. A review of the first case study from the eastern Pacific Ocean shows that simultaneous aircraft and space-borne observations are valuable in detecting links between ocean biota emissions and marine aerosols, but that the effect of the former on cloud microphysics is less clear owing to interference from background anthropogenic pollution and the difficulty with field experiments in obtaining a wide range of aerosol conditions to robustly quantify ocean effects on aerosol-cloud interactions. To address these limitations, a second case was investigated using remote sensing data over the less polluted Southern Ocean region. The results indicate that cloud drop size is reduced more for a fixed increase in aerosol particles during periods of higher ocean chlorophyll A. Potential biases in the results owing to statistical issues in the data analysis are discussed.