Cameron Stuart McNaughton

Size distributions and mixtures of dust and black carbon aerosol in Asian outflow: Physiochemistry and optical properties

[1] During Transport and Chemical Evolution over the Pacific (TRACE-P) and Asian Aerosol Characterization Experiment (ACE-Asia) we measured the dry size distribution of Asian aerosols, their state of mixing, and the optical properties of dust, black carbon (BC) and other aerosol constituents in combustion and/or dust plumes. Optical particle sizing in association with thermal heating extracted volatile components and resolved sizes for dust and refractory soot that usually dominated light absorption. BC was internally mixed with volatile aerosol in � 85% of accumulation mode particles and constituted � 5–15% of their mass. These optically effective sizes constrained the soot and dust size distributions and the imaginary part of the dust refractive index, k, to 0.0006 ± 0.0001. This implies a single-scatter albedo, v (550 nm), for dust ranging from 0.99+ for Dp <1 m mt o� 0.90 at Dp =1 0mm and a size-integrated campaign average near 0.97 ± 0.01. The typical mass scattering efficiency for the dust was � 0.3 m 2 g � 1 , and the mass absorption efficiency (MAE) was 0.009 m 2 g � 1 . Less dust south of 25� N and stronger biomass burning signatures resulted in lower values for v of � 0.82 in plumes aloft. Chemically inferred elemental carbon was moderately correlated with BC light absorption (R 2 = 0.40), while refractory soot volume between 0.1 and 0.5 mm was highly correlated (R 2 = 0.79) with absorption. However, both approaches yield an MAE for BC mixtures of � 7±2m 2 g � 1 and higher than calculated MAE values for BC of 5 m 2 g � 1 . The increase in the mass fraction of soot and BC in pollution aerosol in the presence of elevated dust appears to be due to uptake of the volatile components onto the coarse dust. This predictably lowered v for the accumulation mode from 0.84 in typical pollution to � 0.74 in high-dust events. A chemical transport model revealed good agreement between model and observed BC absorption for most of SE Asia and in biomass plumes but underestimated BC for combustion sources north of 25� N by a factor of � 3. INDEX TERMS: 0305 Atmospheric Composition and Structure: Aerosols and particles (0345, 4801); 0350 Atmospheric Composition and Structure: Pressure, density, and temperature; 0360 Atmospheric Composition and Structure: Transmission and scattering of radiation; 0365 Atmospheric Composition and Structure: Troposphere—composition and chemistry; 0368 Atmospheric Composition and Structure: Troposphere— constituent transport and chemistry; KEYWORDS: dust, black carbon, absorption, single scatter albedo

Biomass burning and pollution aerosol over North America: Organic components and their influence on spectral optical properties and humidification response

[1] Thermal analysis of aerosol size distributions provided size resolved volatility up to temperatures of 400C during extensive flights over North America (NA) for the INTEX/ICARTT experiment in summer 2004. Biomass burning and pollution plumes identified from trace gas measurements were evaluated for their aerosol physiochemical and optical signatures. Measurements of soluble ionic mass and refractory black carbon (BC) mass, inferred from light absorption, were combined with volatility to identify organic carbon at 400C (VolatileOC) and the residual or refractory organic carbon, RefractoryOC. This approach characterized distinct constituent mass fractions present in biomass burning and pollution plumes every 5–10 min. Biomass burning, pollution and dust aerosol could be stratified by their combined spectral scattering and absorption properties. The ‘‘nonplume’’ regional aerosol exhibited properties dominated by pollution characteristics near the surface and biomass burning aloft. VolatileOC included most water-soluble organic carbon. RefractoryOC dominated enhanced shortwave absorption in plumes from Alaskan and Canadian forest fires. The mass absorption efficiency of this RefractoryOC was about 0.63 m 2 g � 1 at 470 nm and 0.09 m 2 g � 1 at 530 nm. Concurrent measurements of the humidity dependence of scattering, g, revealed the OC component to be only weakly hygroscopic resulting in a general decrease in g with increasing OC mass fractions. Under ambient humidity conditions, the systematic relations between physiochemical properties and g lead to a well-constrained dependency on the absorption per unit dry mass for these plume types that may be used to challenge remotely sensed and modeled optical properties.

An intercomparison of lidar-derived aerosol optical properties with airborne measurements near Tokyo during ACE-Asia

[1] During the ACE-Asia intensive observation period (IOP), an intercomparison experiment with ground-based lidars and aircraft observations was conducted near Tokyo. On 23 April 2001, four Mie backscatter lidars were simultaneously operated in the Tokyo region, while the National Center for Atmospheric Research C-130 aircraft flew a steppedascent profile between the surface and 6 km over Sagami Bay southwest of Tokyo. The C-130 observation package included a tracking Sun photometer and in situ packages measuring aerosol optical properties, aerosol size distribution, aerosol ionic composition, and SO2 concentration. The three polarization lidars suggested that the observed modest concentrations of Asian dust in the free troposphere extended up to an altitude of 8 km. We found a good agreement in the backscattering coefficient at 532 nm among lidars and in situ 180� backscatter nephelometer observations. The intercomparison indicated that the aerosol layer between 1.6 and 3.5 km was a remarkably stable and homogenous in mesoscale. We also found reasonable agreement between the aerosol extinction coefficients (sa � 0.03 km � 1 ) derived from the airborne tracking Sun photometer, in situ optical instruments, and those estimated from the lidars above the planetary boundary layer (PBL). We also found considerable vertical variation of the aerosol depolarization ratio (da) and a negative correlation between da and the backscattering coefficient (da) below 3.5 km. Airborne measurements of size-dependent optical parameters (e.g., the fine mode fraction of scattering) and of aerosol ionic compositions suggests that the mixing ratio of the accumulation-mode and coarse-mode (dust) aerosols was primarily responsible for the observed variation of da. Aerosol observations during the intercomparison period captured the following three types of layers in the atmosphere: a PBL (surface to 1.2–1.5 km) where fine (mainly sulfate) particles with a low da (<10%) dominated; an intermediate layer (between the top of the PBL and 3.5 km) where fine particles and dust particles were moderately externally mixed, giving moderate da; and an upper layer (above � 3.5 km) where dust dominated, giving a high da (30%). A substantial dust layer between 4.5 and 6.5 km was observed just west of Japan by the airborne instruments and found to have a lidar ratio of 50.4 ± 9.4 sr. This agrees well with nighttime Raman lidar measurements made later on this same dust layer as it passed over Tokyo, which found a lidar ratio of 46.5 ± 10.5 sr. INDEX TERMS: 0305 Atmospheric Composition and Structure: Aerosols and particles

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.

On the flux of oxygenated volatile organic compounds from organic aerosol oxidation

Previous laboratory and field studies suggest that oxidation of organic aerosols can be a source of oxygenated volatile organic compounds (OVOC). Using measurements of atmospheric oxidants and aerosol size distributions performed on the NASA DC-8 during the INTEX-NA campaign, we estimate the potential magnitude of the continental summertime OVOC flux from organic aerosol oxidation by OH to be as large as ∼70 pptv C/day in the free troposphere. Contributions from O_3, H_2O_2, photolysis, and other oxidants may increase this estimate. These processes may provide a large, diffuse source of OVOC that has not been included in current atmospheric models, and thus have a significant impact on our understanding of organic aerosol, OVOC, PAN, and HO_x chemistry. The potential importance and highly uncertain nature of our estimate highlights the need for more field and laboratory studies on organic aerosol composition and aging.

Spatial distribution and size evolution of particles in Asian outflow: Significance of primary and secondary aerosols during ACE-Asia and TRACE-P

areas as high as 1200 mm 2 cm � 3 . Concentrations of sulfuric acid generally appeared insufficient for binary nucleation, but observations, models, and theory are consistent with a ternary nucleation mechanism involving H2SO4-H2O-NH3. Growth rates of � 2n m h � 1 can be explained by the condensation of sulfuric acid at a rate of 2 ± 1 � 10 6 molecules cm � 3 s � 1 . Aerosol volatility suggested increasing neutralization of the aerosol during growth. Size distribution measurements suggest that weak (mean condensation nuclei (CN) 3–13 nm � 500 cm � 3 ) new particle production was a common occurrence in the region. However, new particle production was enhanced by � 1 order of magnitude (mean CN 3–13 nm � 5000 cm � 3 ) in postfrontal air masses associated with offshore flow during cloud-free conditions. Fog and clouds appear to be regionally important in modulating nucleation events through scavenging of secondary aerosol and through depletion of gas-phase precursors through enhanced heterogeneous chemistry. Our results indicate that only 10–30% of the total aerosol population consists of aged secondary aerosols after � 2 days of transport from source regions. In spite of their high production during nucleation events, secondary aerosols advected out over the Pacific Ocean will have a small impact upon indirect forcing and a negligible impact upon direct forcing compared to primary aerosol emissions and the species that condense upon them. INDEX TERMS: 0305 Atmospheric Composition and Structure: Aerosols and particles (0345, 4801); 4801 Oceanography: Biological and Chemical: Aerosols (0305); 0345 Atmospheric Composition and Structure: Pollution—urban and regional (0305); 0368 Atmospheric Composition and Structure: Troposphere—constituent transport and chemistry; 9320 Information Related to Geographic Region: Asia;

Role of convection in redistributing formaldehyde to the upper troposphere over North America and the North Atlantic during the summer 2004 INTEX campaign

Measurements of formaldehyde (CH2O) from a tunable diode laser absorption spectrometer (TDLAS) were acquired onboard the NASA DC-8 aircraft during the summer 2004 INTEX-NA campaign to test our understanding of convection and CH2O production mechanisms in the upper troposphere (UT, 6–12 km) over continental North America and the North Atlantic Ocean. The present study utilizes these TDLAS measurements and results from a box model to (1) establish sets of conditions by which to distinguish “background” UT CH2O levels from those perturbed by convection and other causes; (2) quantify the CH2O precursor budgets for both air mass types; (3) quantify the fraction of time that the UT CH2O measurements over North America and North Atlantic are perturbed during the summer of 2004; (4) provide estimates for the fraction of time that such perturbed CH2O levels are caused by direct convection of boundary layer CH2O and/or convection of CH2O precursors; (5) assess the ability of box models to reproduce the CH2O measurements; and (6) examine CH2O and HO2 relationships in the presence of enhanced NO. Multiple tracers were used to arrive at a set of UT CH2O background and perturbed air mass periods, and 46% of the TDLAS measurements fell within the latter category. In general, production of CH2O from CH4 was found to be the dominant source term, even in perturbed air masses. This was followed by production from methyl hydroperoxide, methanol, PAN-type compounds, and ketones, in descending order of their contribution. At least 70% to 73% of the elevated UT observations were caused by enhanced production from CH2O precursors rather than direct transport of CH2O from the boundary layer. In the presence of elevated NO, there was a definite trend in the CH2O measurement–model discrepancy, and this was highly correlated with HO2 measurement–model discrepancies in the UT.

Simulating marine boundary layer clouds over the eastern Pacific in a regional climate model with double-moment cloud microphysics

A double-moment cloud microphysics scheme with a prognostic treatment of aerosols inside clouds has been implemented into the International Pacific Research Center Regional Atmospheric Model (iRAM) to simulate marine boundary layer clouds over the eastern Pacific and to study aerosol-cloud interactions, including the aerosol indirect effect. This paper describes the new model system and presents a comparison of model results with observations. The results show that iRAM with the double-moment cloud microphysics scheme is able to reproduce the major features, including the geographical patterns and vertical distribution of the basic cloud parameters such as cloud droplet number, liquid water content, or droplet effective radii over the eastern Pacific reasonably well. However, the model tends to underestimate cloud droplet number concentrations near the coastal regions strongly influenced by advection of continental aerosols and precursor gases. In addition, the average location of the stratocumulus deck off South America is shifted to the northwest compared with the satellite observations. We apply the new model system to assess the indirect aerosol effect over the eastern Pacific by comparing a simulation with preindustrial aerosol to an otherwise identical simulation with present-day aerosol. Resulting changes in the cloud droplet number concentration are particularly pronounced in Gulf of Mexico and along the Pacific coastlines with local changes up to 70 cm(-3) (50% of the present-day value). The modeled domain-averaged 3-month (August-October) mean change in top-of-atmosphere net cloud forcing over the ocean owing to changes in the aerosol burden by anthropogenic activities is -1.6W m(-2) (Less)

Evaluating Primary Marine Aerosol Production and Atmospheric Roll Structures in Hawaii’s Natural Oceanic Wind Tunnel*

AbstractTopography-induced steady-state accelerated wind flow in the Alenuihaha Channel between the islands of Hawaii and Maui provides about 100 km of fetch with winds that can nearly double over trade wind speed. Here ship- and aircraft-based observations of meteorological parameters and aerosols in Hawaii’s orographic natural “wind tunnel” are used for the study of sea salt aerosol (SSA) production, evolution, and related optical effects under clean oceanic conditions. There are certain advantages of channel measurements, such as a broad and uniform upstream area usually filled with background aerosol, stationary flow, and known fetch, but also some difficulties, like vigorous entrainment and persistent presence of organized structures (rolls). It is found that marine boundary layer (MBL) rolls are a common occurrence near the Hawaiian Islands even when cloud streets are not visible in satellite imagery. The presence of rolls tends to enhance the variability of ambient aerosol concentration and probabl...