Anne Jefferson

INDOEX aerosol: A comparison and summary of chemical, microphysical, and optical properties observed from land, ship, and aircraft

converged on values of about 3.8 ± 0.3 m 2 g � 1 , providing a firm constraint upon the description and modeling of haze optical properties. MSE values trended lower with more dilute haze but became more variable in clean air or regions of low concentrations. This cross-platform comparison resolved a number of measurement differences but also revealed that regional characterization from different platforms results in differences linked to variability in time and space. This emphasizes the need to combine such efforts with coordinated satellite and modeling studies able to characterize large-scale regional structure and variability. These comparisons also indicate that ‘‘closure’’ between chemical, microphysical, and optical properties across platforms to better than about 20% will require significant improvements in techniques, calibration procedures, and comparison efforts. INDEX TERMS: 0305 Atmospheric Composition and Structure: Aerosols and particles (0345, 4801); 0345 Atmospheric Composition and Structure: Pollution—urban and regional (0305); 0394 Atmospheric Composition and Structure: Instruments and techniques; KEYWORDS: INDOEX, data comparison, optical properties, chemistry, microphysics, size distributions

Photoisomerization of OCIO: a possible mechanism for polar ozone depletion

CONNECTIONS between polar ozone depletion and halocarbon chemistry have been established by a number of studies1–10. Recent attempts to account quantitatively for the observed rate of ozone decline in Antarctica in terms of known photochemical processes have not been entirely successful, and it seems that further chemical ozone-depleting mechanisms may be needed, particularly if the transport of ozone into the polar regions competes with chemical losses. Spectroscopic and photochemical data indicate that photolysis of OCIO may provide a further ozone loss mechanism that has not previously been considered. Here we report laboratory studies of OCIO spectroscopy and photoproducts which suggest that atomic Cl and O2 are formed to some extent in the photodis-sociation process. This evidence points towards possible photo-isomerization to the unstable species ClOO, (or at least to a similar metastable intermediate) probably by way of the 2B2 excited state of OClO, thus reinforcing the idea that photolysis of OC1O may contribute to polar ozone depletion.

Arctic organic aerosol measurements show particles from mixed combustion in spring haze and from frost flowers in winter.

0.07 m gm �3 in summer to 0.43 m gm �3 in winter, and 0.35 m gm �3 in spring, showing a transition in OM composition between spring and winter. Most of the OM in spring could be attributed to anthropogenic sources, consisting primarily of alkane and carboxylic acid functional groups and correlated to elemental tracers of industrial pollution, biomass burning, and shipping emissions. PMF analysis associated OM with two factors, a Mixed Combustion factor (MCF) and an Ocean‐derived factor (ODF). Back trajectory analysis revealed that the highest fractions of the MCF were associated with air masses that had originated from northeastern Asia and the shipping lanes south of the Bering Straits. The ODF consisted of organic hydroxyl groups and correlated with organic and inorganic seawater components. The ODF accounted for more than 55% of OM in winter when the sampled air masses originated along the coastal and lake regions of the Northwest Territories of Canada. Frost flowers with organic‐salt coatings that arise by brine rejection during sea ice formation may account for this large source of carbohydrate‐like OM during the ice‐ covered winter season. While the anthropogenic sources contributed more than 0.3 m gm �3 of the springtime haze OM, ocean‐derived particles provided comparable OM sources in winter. Citation: Shaw, P. M., L. M. Russell, A. Jefferson, and P. K. Quinn (2010), Arctic organic aerosol measurements show particles from mixed combustion in spring haze and from frost flowers in winter, Geophys. Res. Lett., 37, L10803,

Clouds, Aerosol, and Precipitation in the Marine Boundary Layer: An ARM Mobile Facility Deployment

© Copyright 2015 American Meteorological Society (AMS). Permission to use figures, tables, and brief excerpts from this work in scientific and educational works is hereby granted provided that the source is acknowledged. Any use of material in this work that is determined to be “fair use” under Section 107 of the U.S. Copyright Act September 2010 Page 2 or that satisfies the conditions specified in Section 108 of the U.S. Copyright Act (17 USC §108, as revised by P.L. 94-553) does not require the AMS’s permission. Republication, systematic reproduction, posting in electronic form, such as on a web site or in a searchable database, or other uses of this material, except as exempted by the above statement, requires written permission or a license from the AMS. Additional details are provided in the AMS Copyright Policy, available on the AMS Web site located at (https://www.ametsoc.org/) or from the AMS at 617-227-2425 or copyrights@ametsoc.org.

Environmental snapshots from ACE-Asia

On five occasions spanning the Asian Pacific Regional Aerosol Characterization Experiment (ACE-Asia) field campaign in spring 2001, the Multiangle Imaging Spectroradiometer spaceborne instrument took data coincident with high-quality observations by instruments on two or more surface and airborne platforms. The cases capture a range of clean, polluted, and dusty aerosol conditions. With a three-stage optical modeling process, we synthesize the data from over 40 field instruments into layer-by-layer environmental snapshots that summarize what we know about the atmospheric and surface states at key locations during each event. We compare related measurements and discuss the implications of apparent discrepancies, at a level of detail appropriate for satellite retrieval algorithm and aerosol transport model validation. Aerosols within a few kilometers of the surface were composed primarily of pollution and Asian dust mixtures, as expected. Medium- and coarse-mode particle size distributions varied little among the events studied; however, column aerosol optical depth changed by more than a factor of 4, and the near-surface proportion of dust ranged between 25% and 50%. The amount of absorbing material in the submicron fraction was highest when near-surface winds crossed Beijing and the Korean Peninsula and was considerably lower for all other cases. Having simultaneous single-scattering albedo measurements at more than one wavelength would significantly reduce the remaining optical model uncertainties. The consistency of component particle microphysical properties among the five events, even in this relatively complex aerosol environment, suggests that global, satellite-derived maps of aerosol optical depth and aerosol mixture (air-mass-type) extent, combined with targeted in situ component microphysical property measurements, can provide a detailed global picture of aerosol behavior.

An intercomparison of aerosol light extinction and 180° backscatter as derived using in situ instruments and Raman lidar during the INDOEX field campaign

[1] Aircraft in situ and Raman lidar profiles of aerosol light extinction (ep) and 180 backscattering (p) are compared for 6 days during the Indian Ocean Experiment (INDOEX). The measurements of ep and p were made from the National Center for Atmospheric Research C-130 aircraft using two integrating nephelometers to measure light scattering and one Radiance Research Particle Soot Absorption Photometer to measure light absorption. Particulate 180 backscattering was measured in situ using a new instrument, the 180 backscatter nephelometer. The Institute for Tropospheric Research Raman lidar was located on the island of Hulule (4.18N, 73.53E), and all of the in situ profiles presented are from descents into the Hulule airport. Aerosol optical depth was also measured from Hulule using a Sun photometer, and these data are included in the intercomparison. On average, the lidar-derived values of ep and p are 30% larger than the in situ-derived values to a 95% confidence interval. Possible reasons for the overall discrepancy are (1) a low bias in the in situ measurements because of losses in the C-130 Community Aerosol Inlet; (2) underestimation of the humidification effect on light extinction in the in situ measurements; (3) overestimation of ep and p in the lidar because of subvisible cloud contamination; (4) errors in data processing that could be biasing either measurement, though the lidar retrievals are especially sensitive to this type of error. Temporal and spatial variability also appear to be the source of at least some of the discrepancy in two of the six cases, none of which are well collocated. INDEX TERMS: 0305 Atmospheric Composition and Structure: Aerosols and particles (0345, 4801); 0394 Atmospheric Composition and Structure: Instruments and techniques; 0360 Atmospheric Composition and Structure: Transmission and scattering of radiation; 0345 Atmospheric Composition and Structure: Pollutionurban and regional (0305); KEYWORDS: aersol, optical, lidar, in situ, comparison, INDOEX

Aerosol impacts on drizzle properties in warm clouds from ARM Mobile Facility maritime and continental deployments

We have extensively evaluated the response of cloud base drizzle rate (Rcb; mm d−1) in warm clouds to liquid water path (LWP; g m−2) and to cloud condensation nuclei (CCN) number concentration (NCCN; cm−3), an aerosol proxy. This evaluation is based on a 19 month long data set of Doppler radar, lidar, microwave radiometers, and aerosol observing systems from the Atmospheric Radiation Measurement (ARM) Mobile Facility deployments at the Azores and in Germany. Assuming 0.55% supersaturation to calculate NCCN, we found a power law Rcb=0.0015±0.0009⋅LWP1.68±0.05NCCN−0.66±0.08, indicating that Rcb decreases by a factor of 2–3 as NCCN increases from 200 to 1000 cm−3 for fixed LWP. Additionally, the precipitation susceptibility to NCCN ranges between 0.5 and 0.9, in agreement with values from simulations and aircraft measurements. Surprisingly, the susceptibility of the probability of precipitation from our analysis is much higher than that from CloudSat estimates but agrees well with simulations from a multiscale high-resolution aerosol-climate model. Although scale issues are not completely resolved in the intercomparisons, our results are encouraging, suggesting that it is possible for multiscale models to accurately simulate the response of LWP to aerosol perturbations.

Satellite retrieval of cloud condensation nuclei concentrations by using clouds as CCN chambers

Quantifying the aerosol/cloud-mediated radiative effect at a global scale requires simultaneous satellite retrievals of cloud condensation nuclei (CCN) concentrations and cloud base updraft velocities (Wb). Hitherto, the inability to do so has been a major cause of high uncertainty regarding anthropogenic aerosol/cloud-mediated radiative forcing. This can be addressed by the emerging capability of estimating CCN and Wb of boundary layer convective clouds from an operational polar orbiting weather satellite. Our methodology uses such clouds as an effective analog for CCN chambers. The cloud base supersaturation (S) is determined by Wb and the satellite-retrieved cloud base drop concentrations (Ndb), which is the same as CCN(S). Validation against ground-based CCN instruments at Oklahoma, at Manaus, and onboard a ship in the northeast Pacific showed a retrieval accuracy of ±25% to ±30% for individual satellite overpasses. The methodology is presently limited to boundary layer not raining convective clouds of at least 1 km depth that are not obscured by upper layer clouds, including semitransparent cirrus. The limitation for small solar backscattering angles of <25° restricts the satellite coverage to ∼25% of the world area in a single day.

The Two-Column Aerosol Project: Phase I - Overview and Impact of Elevated Aerosol Layers on Aerosol Optical Depth

The Two-Column Aerosol Project (TCAP), conducted from June 2012 through June 2013, was a unique study designed to provide a comprehensive data set that can be used to investigate a number of important climate science questions, including those related to aerosol mixing state and aerosol radiative forcing. The study was designed to sample the atmosphere between and within two atmospheric columns; one fixed near the coast of North America (over Cape Cod, MA) and a second moveable column over the Atlantic Ocean several hundred kilometers from the coast. The U.S. Department of Energys (DOE) Atmospheric Radiation Measurement (ARM) Mobile Facility (AMF) was deployed at the base of the Cape Cod column, and the ARM Aerial Facility was utilized for the summer and winter intensive observation periods. One important finding from TCAP is that four of six nearly cloud-free flight days had aerosol layers aloft in both the Cape Cod and maritime columns that were detected using the nadir pointing second-generation NASA high-spectral resolution lidar (HSRL-2). These layers contributed up to 60% of the total observed aerosol optical depth (AOD). Many of these layers were also intercepted by the aircraft configured for in situ sampling, and the aerosol in the layers was found to have increased amounts of biomass burning material and nitrate compared to aerosol found near the surface. In addition, while there was a great deal of spatial and day-to-day variability in the aerosol chemical composition and optical properties, no systematic differences between the two columns were observed.

Evaluation of ground‐based black carbon measurements by filter‐based photometers at two Arctic sites

Long-term measurements of the light absorption coefficient (b(abs)) obtained with a particle soot absorption photometer (PSAP), b(abs) (PSAP), have been previously reported for Barrow, Alaska, and ...