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Patrick Y. Chuang
,
Athanasios Nenes
,
James N. Smith
,
Richard C. Flagan
, and
John H. Seinfeld

Abstract

A new instrument for measuring cloud condensation nuclei (CCN) on board small aircraft is described. Small aircraft are attractive mainly because they are less costly, but they require instruments that are designed for minimum weight, volume, and power consumption; that are robust; and that are capable of autonomous operation and making measurements at a frequency appropriate for aircraft speeds. The instrument design combines the streamwise gradient technique previously reported by J. G. Hudson, and the alternating gradient condensation nuclei counter described by W. A. Hoppel et al. Field and laboratory measurements, and modeling studies show that this combination exhibits poor sensitivity for the measurement of CCN spectra; for the climatically important range of critical supersaturations, 0.03%–1%, the measured variable, droplet diameter, varies only by 30%. The ability to resolve CCN spectra using this method is therefore in question. Studies of this instrument in a fixed supersaturation mode show that it can measure CCN at a single supersaturation in the range of 0.1%–2%. Calibration and testing of the instrument in this mode is described. The instrument is capable of making accurate, high-frequency (>0.1 Hz) measurements of CCN at a fixed supersaturation, while satisfying the constraints for small aircraft.

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Georgia Sotiropoulou
,
Anna Lewinschal
,
Paraskevi Georgakaki
,
Vaughan Phillips
,
Sachin Patade
,
Annica M. L. Ekman
, and
Athanasios Nenes

Abstract

Ice formation remains one of the most poorly represented microphysical processes in climate models. While primary ice production (PIP) parameterizations are known to have a large influence on the modeled cloud properties, the representation of secondary ice production (SIP) is incomplete and its corresponding impact is therefore largely unquantified. Furthermore, ice aggregation is another important process for the total cloud ice budget, which also remains largely unconstrained. In this study we examine the impact of PIP, SIP and ice aggregation on Arctic clouds, using the Norwegian Earth System model version 2 (NorESM2). Simulations with both prognostic and diagnostic PIP show that heterogeneous freezing alone cannot reproduce the observed cloud ice content. The implementation of missing SIP mechanisms (collisional break-up, drop-shattering and sublimation break-up) in NorESM2 improves the modeled ice properties, while improvements in liquid content occur only in simulations with prognostic PIP. However, results are sensitive to the description of collisional break-up. This mechanism, which dominates SIP in the examined conditions, is very sensitive to the treatment of the sublimation correction factor, a poorly-constrained parameter that is included in the utilized parameterization. Finally, variations in ice aggregation treatment can also significantly impact cloud properties, mainly through its impact on collisional break-up efficiency. Overall, enhancement in ice production though the addition of SIP mechanisms and the reduction of ice aggregation (in line with radar observations of shallow Arctic clouds) result in enhanced cloud cover and decreased TOA radiation biases, compared to satellite measurements, especially during the cold months.

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Craig A. Stroud
,
Athanasios Nenes
,
Jose L. Jimenez
,
Peter F. DeCarlo
,
J. Alex Huffman
,
Roelof Bruintjes
,
Eiko Nemitz
,
Alice E. Delia
,
Darin W. Toohey
,
Alex B. Guenther
, and
Sreela Nandi

Abstract

Measurements of aerosol size distribution, chemical composition, and cloud condensation nuclei (CCN) concentration were performed during the Chemical Emission, Loss, Transformation, and Interactions with Canopies (CELTIC) field program at Duke Forest in North Carolina. A kinetic model of the cloud activation of ambient aerosol in the chamber of the CCN instrument was used to perform an aerosol–CCN closure study. This study advances prior investigations by employing a novel fitting algorithm that was used to integrate scanning mobility particle sizer (SMPS) measurements of aerosol number size distribution and aerosol mass spectrometer (AMS) measurements of the mass size distribution for sulfate, nitrate, ammonium, and organics into a single, coherent description of the ambient aerosol in the size range critical to aerosol activation (around 100-nm diameter). Three lognormal aerosol size modes, each with a unique internally mixed composition, were used as input into the kinetic model. For the two smaller size modes, which control CCN number concentration, organic aerosol mass fractions for the defined cases were between 58% and 77%. This study is also unique in that the water vapor accommodation coefficient was estimated based on comparing the initial timing for CCN activation in the instrument chamber with the activation predicted by the kinetic model. The kinetic model overestimated measured CCN concentrations, especially under polluted conditions. Prior studies have attributed a positive model bias to an incomplete understanding of the aerosol composition, especially the role of organics in the activation process. This study shows that including measured organic mass fractions with an assumed organic aerosol speciation profile (pinic acid, fulvic acid, and levoglucosan) and an assumed organic aerosol solubility of 0.02 kg kg−1 still resulted in a significant model positive bias for polluted case study periods. The slope and y intercept for the CCN predicted versus CCN observed regression was found to be 1.9 and −180 cm−3, respectively. The overprediction generally does not exceed uncertainty limits but is indicative that a bias exists in the measurements or application of model. From this study, uncertainties in the particle number and mass size distributions as the cause for the model bias can be ruled out. The authors are also confident that the model is including the effects of growth kinetics on predicted activated number. However, one cannot rule out uncertainties associated with poorly characterized CCN measurement biases, uncertainties in assumed organic solubility, and uncertainties in aerosol mixing state. Sensitivity simulations suggest that assuming either an insoluble organic fraction or external aerosol mixing were both sufficient to reconcile the model bias.

Full access
Lynn M. Russell
,
Armin Sorooshian
,
John H. Seinfeld
,
Bruce A. Albrecht
,
Athanasios Nenes
,
Lars Ahlm
,
Yi-Chun Chen
,
Matthew Coggon
,
Jill S. Craven
,
Richard C. Flagan
,
Amanda A. Frossard
,
Haflidi Jonsson
,
Eunsil Jung
,
Jack J. Lin
,
Andrew R. Metcalf
,
Robin Modini
,
Johannes Mülmenstädt
,
Greg Roberts
,
Taylor Shingler
,
Siwon Song
,
Zhen Wang
, and
Anna Wonaschütz

Aerosol–cloud–radiation interactions are widely held to be the largest single source of uncertainty in climate model projections of future radiative forcing due to increasing anthropogenic emissions. The underlying causes of this uncertainty among modeled predictions of climate are the gaps in our fundamental understanding of cloud processes. There has been significant progress with both observations and models in addressing these important questions but quantifying them correctly is nontrivial, thus limiting our ability to represent them in global climate models. The Eastern Pacific Emitted Aerosol Cloud Experiment (E-PEACE) 2011 was a targeted aircraft campaign with embedded modeling studies, using the Center for Interdisciplinary Remotely-Piloted Aircraft Studies (CIRPAS) Twin Otter aircraft and the research vessel Point Sur in July and August 2011 off the central coast of California, with a full payload of instruments to measure particle and cloud number, mass, composition, and water uptake distributions. EPEACE used three emitted particle sources to separate particle-induced feedbacks from dynamical variability, namely 1) shipboard smoke-generated particles with 0.05–1-μm diameters (which produced tracks measured by satellite and had drop composition characteristic of organic smoke), 2) combustion particles from container ships with 0.05–0.2-μm diameters (which were measured in a variety of conditions with droplets containing both organic and sulfate components), and 3) aircraft-based milled salt particles with 3–5-μm diameters (which showed enhanced drizzle rates in some clouds). The aircraft observations were consistent with past large-eddy simulations of deeper clouds in ship tracks and aerosol– cloud parcel modeling of cloud drop number and composition, providing quantitative constraints on aerosol effects on warm-cloud microphysics.

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Annmarie G. Carlton
,
Joost de Gouw
,
Jose L. Jimenez
,
Jesse L. Ambrose
,
Alexis R. Attwood
,
Steven Brown
,
Kirk R. Baker
,
Charles Brock
,
Ronald C. Cohen
,
Sylvia Edgerton
,
Caroline M. Farkas
,
Delphine Farmer
,
Allen H. Goldstein
,
Lynne Gratz
,
Alex Guenther
,
Sherri Hunt
,
Lyatt Jaeglé
,
Daniel A. Jaffe
,
John Mak
,
Crystal McClure
,
Athanasios Nenes
,
Thien Khoi Nguyen
,
Jeffrey R. Pierce
,
Suzane de Sa
,
Noelle E. Selin
,
Viral Shah
,
Stephanie Shaw
,
Paul B. Shepson
,
Shaojie Song
,
Jochen Stutz
,
Jason D. Surratt
,
Barbara J. Turpin
,
Carsten Warneke
,
Rebecca A. Washenfelder
,
Paul O. Wennberg
, and
Xianling Zhou

Abstract

The Southeast Atmosphere Studies (SAS), which included the Southern Oxidant and Aerosol Study (SOAS); the Southeast Nexus (SENEX) study; and the Nitrogen, Oxidants, Mercury and Aerosols: Distributions, Sources and Sinks (NOMADSS) study, was deployed in the field from 1 June to 15 July 2013 in the central and eastern United States, and it overlapped with and was complemented by the Studies of Emissions, Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS) campaign. SAS investigated atmospheric chemistry and the associated air quality and climate-relevant particle properties. Coordinated measurements from six ground sites, four aircraft, tall towers, balloon-borne sondes, existing surface networks, and satellites provide in situ and remotely sensed data on trace-gas composition, aerosol physicochemical properties, and local and synoptic meteorology. Selected SAS findings indicate 1) dramatically reduced NOx concentrations have altered ozone production regimes; 2) indicators of “biogenic” secondary organic aerosol (SOA), once considered part of the natural background, were positively correlated with one or more indicators of anthropogenic pollution; and 3) liquid water dramatically impacted particle scattering while biogenic SOA did not. SAS findings suggest that atmosphere–biosphere interactions modulate ambient pollutant concentrations through complex mechanisms and feedbacks not yet adequately captured in atmospheric models. The SAS dataset, now publicly available, is a powerful constraint to develop predictive capability that enhances model representation of the response and subsequent impacts of changes in atmospheric composition to changes in emissions, chemistry, and meteorology.

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