ALBERT

Description: The Arctic environment is undergoing rapid changes such as faster warming than the global average and exceptional melting of glaciers in Greenland. Black carbon (BC) particles, which are a short-lived climate pollutant, are one cause of Arctic warming and glacier melting. However, the sources of BC particles are still uncertain. We simulated the potential emission sensitivity of atmospheric BC present over the Arctic (north of 66° N) using the Flexpart Lagrangian transport model (version 10.1). This version includes a new aerosol wet removal scheme, which better represents particle-scavenging processes than older versions did. Arctic BC at the surface (0–500 m) and high altitudes (4750–5250 m) is sensitive to emissions in high latitude (〉 60° N) and mid-latitude (30–60° N) regions, respectively. Geospatial sources of Arctic BC were quantified, with a focus on emissions from anthropogenic activities and biomass burning in 2010. We found that anthropogenic sources contributed 82 % and 83 % of annual Arctic BC at the surface and high altitudes, respectively. Arctic surface BC comes predominantly from anthropogenic emissions in Russia (56 %), with gas flaring from the Yamalo-Nenets Autonomous Okrug and Komi Republic being the main source (31 % of Arctic surface BC). These results highlight the need for regulations to control BC emissions from gas flaring to mitigate the rapid changes in the Arctic environment. In summer, combined biomass burning in Siberia, Alaska, and Canada contributes 56–85 % (75 % on average) and 40–72 % (57 %) of Arctic BC at the surface and high altitudes, respectively. A large fraction (40 %) of BC in the Arctic at high altitudes comes from anthropogenic emissions in East Asia, which suggests that the rapidly growing economies of developing countries could have a non-negligible effect on the Arctic. To our knowledge, this is the first year-round evaluation of Arctic BC sources that has been performed using the new wet deposition scheme in Flexpart. The study provides a scientific basis for actions to mitigate the rapidly changing Arctic environment.

Description: The super-eruption of Los Chocoyos, newly dated to 80.6 kyrs ago, in Guatemala was one of the largest volcanic events of the past 100 000 years. Recent petrologic data show that the eruption released very large amounts of climate-relevant sulfur and ozone destroying chlorine and bromine gases. Using the recently released Earth System Model CESM2(WACCM6) we simulate the impacts of the sulfur- and halogen-rich Los Chocoyos (~ 15° N) eruption on the pre-industrial Earth System for the eruption month January. Our model results show that enhanced modeled sulfate burden and aerosol optical depth (AOD) persists for five years, while the volcanic halogens stay elevated for nearly 15 years. As a consequence the eruption leads to a collapse of the ozone layer with global mean column ozone values dropping to 50 DU (80 % decrease) leading to a 550 % increase in surface UV over the first five years with potential impacts on the biosphere. The volcanic eruption shows an asymmetric hemispheric response with enhanced aerosol, ozone, UV, and climate signals over the Northern Hemisphere (NH). Surface climate is impacted globally due to peak AOD of 〉 6 leading to a maximum surface cooling of 〉 6 K, precipitation and terrestrial net primary production (NPP) decreases of 〉 25 %, and sea ice area increases of 40 % in the first three years. Locally, a wetting (〉 100 %) and strong increase of NPP (〉 700 %) over Northern Africa is simulated in the first five years related to a southwards shift of the Inter-Tropical Convergence Zone to the southern tropics. The ocean responds with El-Niño conditions in the first two years which are masked by the strong volcanic induced surface cooling. Recovery to pre-eruption ozone levels and climate takes 15 and 30 years respectively. The long lasting surface cooling is sustained by sea ice/ocean changes in the Arctic showing an immediate sea ice area increase followed by a decrease of poleward ocean heat transport at 60° N lasting up to 20 years. In contrast, when simulating Los Chocoyos conventionally, including sulfur and neglecting halogens, we simulate larger sulfate burden and AOD, more pronounced surface climate changes and an increase of column ozone. Comparing our aerosol chemistry ESM results to other super-eruption simulations with aerosol climate models we find a higher surface climate impact per injected sulfur amount than previous studies for our different sets of model experiments, since CESM2(WACCM6) creates smaller aerosols with a longer lifetime partly due to the interactive aerosol chemistry. As the model uncertainties for the climate response to super eruptions are very large observational evidence from paleo archives and a coordinated model intercomparison would help to improve our understanding of the climate and environment response.

Description: The stratospheric ozone layer shields surface life from harmful ultraviolet radiation. Following the Montreal Protocol ban of long-lived ozone depleting substances (ODSs), rapid depletion of total column ozone (TCO) ceased in the late 1990s and ozone above 32 km now enjoys a clear recovery. However, there is still no confirmation of TCO recovery, and evidence has emerged that ongoing quasi-global (60° S–60° N) lower stratospheric ozone decreases may be responsible, dominated by low latitudes (30° S–30° N). Chemistry climate models (CCMs) used to project future changes predict that lower stratospheric ozone will decrease in the tropics by 2100, but not at mid-latitudes (30°–60°). Here, we show that CCMs display an ozone decline similar to that observed in the tropics over 1998–2016, likely driven by a increase of tropical upwelling. On the other hand, mid-latitude lower stratospheric ozone is observed to decrease, while CCMs show an increase. Despite opposing lower stratospheric ozone changes, which should induce opposite temperature trends, CCM and observed temperature trends agree; we demonstrate that opposing model-observation stratospheric water vapour (SWV) trends, and their associated radiative effects, explain why temperature changes agree in spite of opposing ozone trends. We provide new evidence that the observed mid-latitude trends can be explained by enhanced mixing between the tropics and extratropics. We further show that the temperature trends are consistent with the observed mid-latitude ozone decrease. Together, our results suggest that large scale circulation changes expected in the future from increased greenhouse gases (GHGs) may now already be underway, but that most CCMs are not simulating well mid-latitude ozone layer changes. The reason CCMs do not exhibit the observed changes urgently needs to be understood to improve confidence in future projections of the ozone layer.

Description: Remote sensing observations from the AERONET and GAW networks are intermittent in time and have a limited field-of-view. A global high-resolution simulation (GEOS5 Nature Run) is used to conduct an Observing System Simulation Experiment (OSSE) for AERONET and GAW observations of AOT and AAOT and estimate the spatio-temporal representativity of individual sites for larger areas (from 0.5° to 4° in size). G5NR and the OSSE are evaluated and shown to have sufficient skill, although daily AAOT variability is significantly underestimated while the frequency of AAOT observations is over-estimated (both resulting in an under-estimation of temporal representativity errors in AAOT). Yearly representation errors are provided for a host of scenarios: varying grid-box size, temporal collocation protocols, and site altitudes are explored. Monthly representation errors are shown to correlate strongly throughout the year, with a pronounced annual cycle. The collocation protocol for AEROCOM model evaluation (using daily data) is shown to be sub-optimal and the use of hourly data advocated instead. A previous subjective ranking of site spatial representativity (Kinne et al., 2013) is analysed and a new objective ranking proposed. Several sites are shown to have yearly representation errors in excess of 40 %. Lastly, a recent suggestion by Wang et al. (2018) that AERONET observations of AAOT suffer a positive representation bias of 30 % globally is analysed and evidence is provided that this bias is likely an overestimate (the current paper finds 4 %) due methodological choices.

Description: Light-absorbing organic carbon aerosol – colloquially known as brown carbon (BrC) – is emitted from combustion processes and has a brownish or yellowish visual appearance, caused by enhanced light absorption at shorter visible and ultraviolet wavelengths (0.3 μm ≲ λ ≲ 0.5 μm). Recently, optical properties of atmospheric BrC aerosols have become the topic of intense research, but little is known about how BrC deposition onto snow surfaces affects the spectral snow albedo, which can alter the resulting radiative forcing and in-snow photochemistry. Wildland fires in close proximity to the cryosphere, such as peatland fires that emit large quantities of BrC, are becoming more common at high latitudes, potentially affecting nearby snow and ice surfaces. In this study, we describe the artificial deposition of BrC aerosol with known optical, chemical, and physical properties onto the snow surface and we monitor its spectral radiative impact and compare it directly to modeled values. First, using small-scale combustion of Alaskan peat, BrC aerosols were artificially deposited onto the snow surface. UV-vis absorbance and total organic carbon (TOC) concentration of snow samples were measured for samples with and without artificial BrC deposition. These measurements were used to estimate the imaginary part of the refractive index of deposited BrC aerosol with a volume mixing rule. Single particle optical properties were calculated using Mie theory, and these values were used to show that the measured spectral snow albedo of snow with deposited BrC was in general agreement with modeled spectral snow albedo using calculated BrC optical properties. The instantaneous radiative forcing by impurities present in the snow before the deposition experiments was found to increase the instantaneous radiative forcing at the surface of the natural snow at our site by 1.23 (+0.14/−0.11) W m−2 per ppm of BrC deposited. However, we estimate that deposition onto a clean snowpack without light-absorbing impurities would have resulted in a more than twice as large instantaneous radiative forcing of 2.68 (+0.27/−0.22) W m−2 per ppm of BrC deposited.

Description: Aerosol iodine isotopes are pivotal links in atmospheric circulation of iodine in both atmospheric and nuclear sciences, while their sources, temporal change and transport are still not well understood. This work presents the day-resolution temporal variation of iodine-129 (129I) and iodine-127 (127I) in aerosols from Xi'an, northwest China during 2017/2018. Both iodine isotopes have significant fluctuations with time, showing highest levels in winter, approximately two to three times higher than in other seasons, but the correlation between 129I and 127I reflects they have different sources. Aerosol 127I is found to be noticeably positively correlated with air quality index and five air pollutants. Enhanced fossil fuel combustion and inverse weather conditions can explain the increased concentrations and peaks of 127I in winter. The change of 129I confirms that source and level of 129I in the monsoonal region were alternatively dominated by the 129I-enriched East Asian winter monsoon and 129I-poor East Asian summer monsoon. The mean 129I/127I of (101 ± 124) × 10−10 provides an atmospheric background level for the purpose of nuclear environmental safety monitoring. This study suggests that locally discharged stable 127I and externally input 129I are likely involved into fine particles formation in urban air, shedding insights into long-range transport of air pollutants and iodine's role in particulate formation in urban atmosphere.

Description: Multifunctional organic nitrates, including carbonyl nitrates, are important species formed in NOx rich atmospheres by the degradation of VOCs. These compounds have been shown to play a key role in the transport of reactive nitrogen and consequently in the ozone budget, but also to be important components of the total organic aerosol. However, very little is known about their reactivity in both gas and condensed phases. Following a previous study we published on the gas-phase reactivity of β-nitrooxy ketones, the photolysis and the reaction with OH radicals of 4-nitrooxy-2-butanone and 5-nitrooxy-2-pentanone, respectively a β-nitrooxy ketone and a γ-nitrooxy ketone, were investigated for the first time in simulation chambers. Ambient photolysis frequencies calculated for 40° latitude North were found to be (4.2 ± 0.6) × 10−5 s−1 and (2.2 ± 0.7) × 10−5 s−1 for 4-nitrooxy-2-butanone and 5-nitrooxy-2-pentanone, respectively. These results demonstrate that photolysis is a very efficient sink for these compounds with atmospheric lifetimes of few hours. It was also concluded that, similarly to α-nitrooxy ketones, β-nitrooxy ketones have enhanced UV absorption cross sections and quantum yields equal or close to unity. γ-nitrooxy ketones have been shown to have lower enhancement of cross sections which can easily be explained by the increasing distance between the two chromophore groups. Thanks to a products study, branching ratio between the two possible photodissociation pathways are also proposed. Rate constants for the reaction with OH radicals were found to be (2.9 ± 1.0) × 10−12 cm3 molecule−1 s−1 and (3.3 ± 0.9) × 10−12 cm3 molecule−1 s−1, respectively. These experimental data are in good agreement with rate constants estimated by the SAR of Kwok and Atkinson (1995) when using the parametrization proposed by Suarez-Bertoa et al. (2012) for carbonyl nitrates. Comparison with photolysis rates suggests that OH-initiated oxidation of carbonyl nitrates is a less efficient sink that photodissociation but is not negligible in polluted area.

Description: The spatial distribution and properties of submicron organic aerosols (OA) are among the key sources of uncertainty in our understanding of aerosol effects on climate. Uncertainties are particularly large over remote regions of the free troposphere and Southern Ocean, where very little data has been available, and where OA predictions from AeroCom Phase II global models span a factor of 400–1000, greatly exceeding the model spread over source regions. The (nearly) pole-to-pole vertical distribution of non-refractory aerosols was measured with an aerosol mass spectrometer onboard the NASA DC8 aircraft as part of the Atmospheric Tomography (ATom) mission during the northern hemisphere summer (August 2016) and winter (February 2017). This study presents the first extensive characterization of OA mass concentrations and their level of oxidation in the remote atmosphere. OA and sulfate are the major contributors by mass to submicron aerosols in the remote troposphere, together with sea salt in the marine boundary layer. Sulfate was dominant in the lower stratosphere. OA concentrations have a strong seasonal and zonal variability, with the highest levels measured in the summer and over the regions influenced by the biomass burning from Africa (up to 10 μg sm−3). Lower concentrations (~ 0.1–0.3 μg sm−3) are observed in the northern mid- and high-latitudes and very low concentrations (

Description: Measurements of long-lived trace gases (SF6, CFC-11, CFC-12, HCFC-12, CCl4, N2O, CH4, H2O, and CO) performed with the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) have been used to infer the stratospheric and mesospheric meridional circulation. The MIPAS data set covers the time period from July 2002 to April 2012. The method used for this purpose was the direct inversion of the two-dimensional continuity equation. Monthly climatologies of circulation fields are presented along with their variabilities. Stratospheric circulation is found to be highly variable over the year, with a quite robust annual cycle. The new method allows to track the evolution of various circulation patterns over the year in more detail than before.The deep branch of the Brewer-Dobson circulation and the mesospheric overturning pole-to-pole circulation are no separate but intertwined phenomena. The latitude of stratospheric uplift in the middle and upper stratosphere is found to be quite variable and is not always found at tropical latitudes. The usual schematic of stratospheric circulation with the deep and the shallow branch of the Brewer-Dobson circulation and the mesospheric overturning circulation is an idealization which best describes the observed atmosphere around Equinox. Sudden stratospheric warmings cause increased year-to year variability.

Description: Iron is the most abundant transition element in airborne PM, primarily existing as Fe(II) or Fe(III). Generally, the fraction of water-soluble iron is greater in urban areas compared to areas dominated by crustal emissions. To better understand the origin of water-soluble iron in urban areas, tail-pipe emission samples were collected from 32 vehicles with emission certifications of Tier 0, low emission vehicles (LEV I), tier two low emission vehicles (LEV II), ultralow emission vehicles (ULEV), superultra-low emission vehicles (SULEV), and partial-zero emission vehicles (PZEV). Components quantified included gases, inorganic ions, EC/OC, total metals and water-soluble metals. In addition, naphthalene and various classes of C12–C18 intermediate volatility organic compounds (IVOC) were quantified for a subset of vehicles: aliphatic, single ring aromatic (SRA), and polar (material not classified as either aliphatic or SRA). Iron solubility in the tested vehicles ranged from 0–82 % (average = 30 %). X-ray absorption near edge structure (XANES) spectroscopy showed that Fe(III) was the primary oxidation state in 14 of the 16 tested vehicles, confirming that the presence of Fe(II) was not the main driver of water-soluble Fe. Correlation of water-soluble iron to sulfate was insignificant, as was correlation to every chemical component, except to naphthalene and some C12–C18 IVOCs with R2 values as high as 0.56. A controlled benchtop study confirmed that naphthalene, alone, increases iron solubility from soils by a factor of 5.5 and that oxidized naphthalene species are created in the extract solution. These results suggest that the large driver in water-soluble iron from primary vehicle tail-pipe emissions is related to the organic composition of the PM, indicating the organic fraction of the PM influences the behavior and solubility of iron.