Global Budget and Radiative Forcing of Black Carbon Aerosol: Constraints from Pole-to-Pole (HIPPO) Observations across the Pacific

We use a global chemical transport model (GEOS-Chem) to interpret aircraft curtain observations of black carbon (BC) aerosol over the Pacific from 85°N to 67°S during the 2009–2011 HIAPER (High-Performance Instrumented Airborne Platform for Environmental Research) Pole-to-Pole Observations (HIPPO) campaigns. Observed concentrations are very low, implying much more efficient scavenging than is usually implemented in models. Our simulation with a global source of $6.5 Tg a^{−1}$ and mean tropospheric lifetime of 4.2 days (versus 6.8 ± 1.8 days for the Aerosol Comparisons between Observations and Models (AeroCom) models) successfully simulates BC concentrations in source regions and continental outflow and captures the principal features of the HIPPO data but is still higher by a factor of 2 (1.48 for column loads) over the Pacific. It underestimates BC absorbing aerosol optical depths (AAODs) from the Aerosol Robotic Network by 32% on a global basis. Only 8.7% of global BC loading in GEOS-Chem is above 5 km, versus 21 ± 11% for the AeroCom models, with important implications for radiative forcing estimates. Our simulation yields a global BC burden of 77 Gg, a global mean BC AAOD of 0.0017, and a top-of-atmosphere direct radiative forcing (TOA DRF) of $0.19 W m^{−2}$, with a range of $0.17–0.31 W m^{−2}$ based on uncertainties in the BC atmospheric distribution. Our TOA DRF is lower than previous estimates $(0.27 \pm 0.06 W m^{−2}$ in AeroCom, $0.65–0.9 W m^{−2}$ in more recent studies). We argue that these previous estimates are biased high because of excessive BC concentrations over the oceans and in the free troposphere.Engineering and Applied Science

A signature of aged biogenic compounds detected from airborne VOC measurements in the high arctic atmosphere in March/April 2018

During the PAMARCMiP 2018 campaign (March and April 2018) a proton-transfer-reaction mass spectrometer (PTR-MS) was deployed onboard the POLAR 5 research aircraft and sampled the high Arctic atmosphere under Arctic haze conditions. More than 100 compounds exhibited levels above 1 pmol/mol in at least 25% of the measurements. We used acetone mixing ratios, ozone concentrations, and back trajectories to identify periods with and without long-range transport from continental sources. During two flights, surface ozone depletion events (ODE) were observed that coincided with enhanced levels of acetone, and methylethylketone, and ice nucleating particles (INP).Air masses with continental influence contained elevated levels of compounds associated with aged biogenic emissions and anthropogenic pollution (e.g., methanol, peroxyacetylnitrate (PAN), acetone, acetic acid, meth-ylethylketone (MEK), proprionic acid, and pentanone). Almost half of all positively detected compounds (>100) in the high Arctic atmosphere can be associated with terpene oxidation products, likely produced from mono-terpenes and sesquiterpenes emitted from boreal forests. We speculate that the transport of biogenic terpene emissions may constitute an important control of the High Arctic aerosol burden. The sum concentration of the detected aerosol forming vapours is-12 pmol/mol, which is of the same order than measured dimethylsulfide (DMS) mixing ratios and their mass density corresponds to approximately one fifth of the measured non-black -carbon particles

Concentrations and size distributions of black carbon in the surface snow of Eastern Antarctica in 2011

The Tenth Symposium on Polar Science/Ordinary sessions: [OM] Polar Meteorology and Glaciology, Thu. 5 Dec. / 2F Auditorium , National Institute of Polar Researc

Black carbon and inorganic aerosols in Arctic snowpack

Key Points: • First ever measurements with a high‐accuracy single‐particle soot photometer of black carbon (BC) concentrations in Arctic snowpack • Topography and BC emission flux strongly influenced latitudinal variations of mass concentrations and size distributions of BC • Measured BC mass concentrations 2–25 times lower than previously reported show the importance of revalidating climate modelsBlack carbon (BC) deposited on snow lowers its albedo, potentially contributing to warming in the Arctic. Atmospheric distributions of BC and inorganic aerosols, which contribute directly and indirectly to radiative forcing, are also greatly influenced by depositions. To quantify these effects, accurate measurement of the spatial distributions of BC and ionic species representative of inorganic aerosols (ionic species hereafter) in snowpack in various regions of the Arctic is needed, but few such measurements are available. We measured mass concentrations of size-resolved BC (CMBC) and ionic species in snowpack by using a single-particle soot photometer and ion chromatography, respectively, over Finland, Alaska, Siberia, Greenland, and Spitsbergen during early spring in 2012–2016. Total BC mass deposited per unit area (DEPMBC) during snow accumulation periods was derived from CMBC and snow water equivalent (SWE). Our analyses showed that the spatial distributions of anthropogenic BC emission flux, total precipitable water, and topography strongly influenced latitudinal variations of CMBC, BC size distributions, SWE, and DEPMBC. The average size distributions of BC in Arctic snowpack shifted to smaller sizes with decreasing CMBC due to an increase in the removal efficiency of larger BC particles during transport from major sources. Our measurements of CMBC were lower by a factor of ~13 than previous measurements made with an Integrating Sphere/Integrating Sandwich spectrophotometer due mainly to interference from coexisting non-BC particles such as mineral dust. The SP2 data presented here will be useful for constraining climate models that estimate the effects of BC on the Arctic climate.Plain Language Summary Black carbon (BC) particles, commonly known as soot, are emitted from incomplete combustion of fossil fuels and biomass. They efficiently absorb solar radiation and thus heat the atmosphere. BC particles emitted at midlatitudes and in the Arctic are deposited onto snow in the Arctic, accelerating snowmelt in early spring by absorbing solar radiation. These processes contribute to warming in the Arctic. Calculations of this warming effect by using numerical models need to be validated by comparison with observed BC concentrations in snowpack. However, there are very few accurate records of concentrations of BC in snow because of technical difficulties in making these measurements. We developed a new laser-induced incandescence technique to measure BC concentrations in snowpack and applied it for the first time in six Arctic regions (Finland, Alaska, North and South Siberia, Greenland, and Spitsbergen). The BC concentrations we measured were highest in Finland and South Siberia, which are closer to large anthropogenic BC sources than the other regions, where our measured BC concentrations were much lower. On average, our BC concentrations were much lower than those previously measured by different techniques. Therefore, previous comparisons of modeled and observed BC concentrations need to be re-evaluated using the present data

アラスカにおける積雪中のブラックカーボン及び固体微粒子の空間分布

第6回極域科学シンポジウム分野横断セッション：[IA] 急変する北極気候システム及びその全球的な影響の総合的解明―GRENE北極気候変動研究事業研究成果報告2015―11月19日（木）　国立極地研究所 2階 大会議

Constraining the complex refractive index of black carbon particles using the complex forward-scattering amplitude

Black carbon is the largest contributor to global aerosol’s shortwave absorption in the current atmosphere and is an important positive climate forcer. The complex refractive index, m = mr + imi, the primary determinant of the absorbed and scattered energies of incident radiation per unit volume of particulate material, has not been accurately known for atmospheric black carbon material. An accurate value at visible wavelengths has been difficult to obtain due to the black carbon’s wavelength-scale irregularity and variability of aggregate shape, distribution in particle size, and mixing with other aerosol compounds. Here, we present a method to constrain a plausible (mr, mi) domain for black carbon from the observed distribution of the complex forward-scattering amplitude S(0°). This approach suppresses the biases due to the above-mentioned complexities. The S(0°) distribution of black carbon is acquired by performing single particle S(0°) measurements in a water medium after collecting atmospheric aerosols into water. We demonstrate the method operating at λ = 0.633 μm for constraining the refractive index of black carbon aerosols in the north-western Pacific boundary layer. From the plausible (mr, mi) domain consistent with the observed S(0°) distributions and the reported range of mass absorption cross-section, we conservatively select 1.95 + 0.96i as a recommendable value of the refractive index for uncoated black carbon at visible wavelengths. The recommendable value is 0.17 larger in mi than the widely used value 1.95 + 0.79i in current aerosol-climate models, implying a ∼16% underestimate of shortwave absorption by black carbon aerosols in current climate simulations.</p