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Watson, Thomas B.

Publications and source records attributed to Watson, Thomas B..

Reconciling Observed and Predicted Tropical Rainforest OH Concentrations

We present OH observations made in Amazonas, Brazil during the Green Ocean Amazon campaign (GoAmazon2014/5) from February to March of 2014. The average diurnal variation of OH peaked with a midday (10:00–15:00) average of 1.0 × 10 6 (±0.6 × 10 6 ) molecules cm -3 . This was substantially lower than previously reported in other tropical forest photochemical environments (2–5 × 10 6 molecules cm -3 ) while the simulated OH reactivity was lower. The observational data set was used to constrain a box model to examine how well current photochemical reaction mechanisms can simulate observed OH. We used one near-explicit mechanism (MCM v3.3.1) and four condensed mechanisms (i.e., RACM2, MOZART-T1, CB05, CB6r2) to simulate OH. A total of 14 days of analysis shows that all five chemical mechanisms were able to explain the measured OH within instrumental uncertainty of 40% during the campaign in the Amazonian rainforest environment. Future studies are required using more reliable NO x and VOC measurements to further investigate discrepancies in our understanding of the radical chemistry in the tropical rainforest.

54 ENVIRONMENTAL SCIENCES↗

Hydroxymethanesulfonate (HMS) Formation during Summertime Fog in an Arctic Oil Field

Hydroxymethanesulfonate (HMS) is produced in the aqueous-phase reaction of formaldehyde (HCHO) and sulfur dioxide (SO 2 ) and has been proposed as a significant contributor to midlatitude wintertime pollution events. In this work, we report HMS detection within submicrometer atmospheric aerosols during frequent late summer, regional fog events in an Arctic oil field. The number fraction of individual particles containing HMS increased during fog periods, consistent with aqueous-phase formation. The single-particle mass spectra showed the primary particle signature (oil field emissions), plus secondary oxidized organics and sulfate, consistent with aqueous-phase processing. HMS mass concentrations ranged from below the ion chromatography limit of detection (0.3 ng/m 3 ) to 1.6 ng/m 3 , with sulfate concentrations of 37-222 ng/m 3 . HCHO and SO 2 measurements suggest that the fog HMS production rate is ~10 times higher in the oil fields than in the upwind Beaufort Sea. Aqueous-phase reactions of local oil field emissions during frequent summertime regional fog events likely have downwind impacts on Arctic aerosol composition. The potential for fog-based HMS production was estimated to be an order of magnitude higher in Fairbanks and Anchorage, AK, than in the oil fields and may explain the missing organosulfate source contributing to Fairbanks air quality.

54 ENVIRONMENTAL SCIENCES↗

Long-range transported North American wildfire aerosols observed in marine boundary layer of eastern North Atlantic

Wildfire is a major source of biomass burning aerosols, which greatly impact Earth climate. Tree species in North America (NA) boreal forests can support high-intensity crown fires, resulting in elevated injection height and longer lifetime (on the order of months) of the wildfire aerosols. Given the long lifetime, the properties of aged NA wildfire aerosols are required to understand and quantify their effects on radiation and climate. Here we present comprehensive characterization of climatically relevant properties, including optical properties and cloud condensation nuclei (CCN) activities of aged NA wildfire aerosols, emitted from the record-breaking Canadian wildfires in August 2017. Despite the extreme injection height of ~12 km, some of the wildfire plumes descended into the marine boundary layer in the eastern North Atlantic over a period of ~2 weeks, owing to the dry intrusions behind mid-latitude cyclones. The aged wildfire aerosols have high single scattering albedos at 529 nm (ω 529 ; 0.92–0.95) while low absorption Ångström exponents (Å abs ) at 464 nm/648 nm (0.7–0.9). In comparison, Å abs of fresh/slightly aged ones are typically 1.4–3.5. This low Å abs 529 and low Å abs ~110 nm diameter) with thick non-absorbing coatings. The accelerated descent of the wildfire plume also led to strong increase of CCN concentration at the supersaturation levels representative of marine low clouds. The hygroscopicity parameter, κ CCN , of the aged wildfire aerosols varies from 0.2 to 0.4, substantially lower than that of background marine boundary layer aerosols. However, the high fraction of particles with large diameter (i.e., within accumulation size ranges, ~100–250 nm) compensates for the low values of κ, and as a result, the aged NA wildfire aerosols contribute more efficiently to CCN population. These results provide direct evidence that the long-range transported NA wildfires can strongly influence CCN concentration in remote marine boundary layer, therefore the radiative properties of marine low clouds. Given the expected increases of NA wildfire intensity and frequency and regular occurrence of dry intrusion following mid-latitude cyclones, the influence of NA wildfire aerosols on CCN and clouds in remote marine environment need to be further examined.

54 ENVIRONMENTAL SCIENCES↗