An improved understanding of the optical properties of secondary organic aerosol (SOA) particles is needed to better predict their climate impacts. Here, SOA was produced by reacting 1-methylnaphthalene or longifolene with hydroxyl radicals (OH) under variable ammonia (NH3), nitrogen oxide (NOx), and relative humidity (RH) conditions. In the presence of NH3 and NOx, longifolene-derived aerosols had relatively high single scattering albedo (SSA) values and low absorption coefficients at 375 nm independent of RH, suggesting that the longifolene SOA is mostly scattering. In 1-methylnaphthalene experiments, the resulting SSA and SOA mass absorption coefficient (MACorg) values suggest the formation of light-absorbing SOA, and the addition of high NOx and high NH3 enhanced the SOA absorption. Under intermediate-NOx dry conditions, the MACorg values increased from 0.13 m2 g−1 in NH3-free conditions to 0.28 m2 g−1 in high-NH3 conditions. Under high-NH3 conditions, the MACorg value further increased to 0.36 m2 g−1 with an increase in RH. Under dry high-NOx conditions, the MACorg value increased from 0.42 to 0.67 m2 g−1 with the addition of NH3, while with elevated RH, the MACorg value reached 0.70 m2 g−1. The time series of MACorg showed increasing trends only in the presence of NH3. Composition analysis of SOA suggests that organonitrates, nitroorganics, and other nitrogen-containing organic compounds (NOCs) are potential chromophores in the 1-methylnaphthalene SOA. Significant formation of NOCs was observed in the presence of high-NOx and NH3 and was enhanced under elevated RH. The data have been collected in an environmental chamber, oxidizing 30-100 ppbv of 1-methylnaphthalene and 70-100 ppbv of longifolene under different levels of nitrogen oxides, ammonia, and relative humidity. Microphysical properties (size distribution and absorption and scattering coefficients) of SOA along with its composition were monitored throughout the experiment. Submitted data include the time series of the calculated mass absorption coefficient and single scattering albedo at 375 nm, derived real and imaginary components of the refractive index, organic nitrate to organic ratio, and organic and nitrate mass concentrations. The data have been analyzed using Wavemetrics Igor Pro, specifically the software written specifically to analyze the data obtained from Aerodyne's aerosol mass spectrometers (i.e., Squirrel and Pika). Other calculations were also carried out in Igor Pro. More details are provided in the related manuscripts. Please see README file.
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Vertical profiles of light absorption and scattering associated with black carbon particle fractions in the springtime Arctic above 79° N
Abstract. Despite the potential importance of black carbon (BC) for radiative forcing of the Arctic atmosphere, vertically resolved measurements of the particle light scattering coefficient (σsp) and light absorption coefficient (σap) in the springtime Arctic atmosphere are infrequent, especially measurements at latitudes at or above 80∘ N. Here, relationships among vertically distributed aerosol optical properties (σap, σsp and single scattering albedo or SSA), particle microphysics and particle chemistry are examined for a region of the Canadian archipelago between 79.9 and 83.4∘ N from near the surface to 500 hPa. Airborne data collected during April 2015 are combined with ground-based observations from the observatory at Alert, Nunavut and simulations from the Goddard Earth Observing System (GEOS) model, GEOS-Chem, coupled with the TwO-Moment Aerosol Sectional (TOMAS) model (collectively GEOS-Chem–TOMAS; Kodros et al., 2018) to further our knowledge of the effects of BC on light absorption in the Arctic troposphere. The results are constrained for σsp less than 15 Mm−1, which represent 98 % of the observed σsp, because the single scattering albedo (SSA) has a tendency to be lower at lower σsp, resulting in a larger relative contribution to Arctic warming. At 18.4 m2 g−1, the average BC mass absorption coefficient (MAC) from the combined airborne and Alert observations is substantially higher than the two averaged modelled MAC values (13.6 and 9.1 m2 g−1) for two different internal mixing assumptions, the latter of which is based on previous observations. The higher observed MAC value may be explained by an underestimation of BC, the presence of small amounts of dust and/or possible differences in BC microphysics and morphologies between the observations and model. In comparing the observations and simulations, we present σap and SSA, as measured, and σap∕2 and the corresponding SSA to encompass the lower modelled MAC that is more consistent with accepted MAC values. Median values of the measured σap, rBC and the organic component of particles all increase by a factor of 1.8±0.1, going from near-surface to 750 hPa, and values higher than the surface persist to 600 hPa. Modelled BC, organics and σap agree with the near-surface measurements but do not reproduce the higher values observed between 900 and 600 hPa. The differences between modelled and observed optical properties follow the same trend as the differences between the modelled and observed concentrations of the carbonaceous components (black and organic). Model-observation discrepancies may be mostly due to the modelled ejection of biomass burning particles only into the boundary layer at the sources. For the assumption of the observed MAC value, the SSA range between 0.88 and 0.94, which is significantly lower than other recent estimates for the Arctic, in part reflecting the constraint of σsp<15 Mm−1. The large uncertainties in measuring optical properties and BC, and the large differences between measured and modelled values here and in the literature, argue for improved measurements of BC and light absorption by BC and more vertical profiles of aerosol chemistry, microphysics and other optical properties in the Arctic.
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- NSF-PAR ID:
- 10211176
- Date Published:
- Journal Name:
- Atmospheric Chemistry and Physics
- Volume:
- 20
- Issue:
- 17
- ISSN:
- 1680-7324
- Page Range / eLocation ID:
- 10545 to 10563
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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- Free Publicly Accessible Full Text
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Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.5194/acp-20-10545-2020
