AeroCom phase III multi-model evaluation of the aerosol life cycle and optical properties using ground- and space-based remote sensing as well as surface in situ observations

Within the framework of the AeroCom (Aerosol Comparisons between Observations and Models) initiative, the state-of-the-art modelling of aerosol optical properties is assessed from 14 global models participating in the phase III control experiment (AP3). The models are similar to CMIP6/AerChemMIP Earth System Models (ESMs) and provide a robust multi-model ensemble. Inter-model spread of aerosol species lifetimes and emissions appears to be similar to that of mass extinction coefficients (MECs), suggesting that aerosol optical depth (AOD) uncertainties are associated with a broad spectrum of parameterised aerosol processes. Total AOD is approximately the same as in AeroCom phase I (AP1) simulations. However, we find a 50% decrease in the optical depth (OD) of black carbon (BC), attributable to a combination of decreased emissions and lifetimes. Relative contributions from sea salt (SS) and dust (DU) have shifted from being approximately equal in AP1 to SS contributing about 2/3 of the natural AOD in AP3. This shift is linked with a decrease in DU mass burden, a lower DU MEC, and a slight decrease in DU lifetime, suggesting coarser DU particle sizes in AP3 compared to AP1. Relative to observations, the AP3 ensemble median and most of the participating models underestimate all aerosol optical properties investigated, that is, total AOD as well as fine and coarse AOD (AOD(f), AOD(c)), Angstrom exponent (AE), dry surface scattering (SCdry), and absorption (AC(dry)) coefficients. Compared to AERONET, the models underestimate total AOD by ca. 21% +/- 20% (as inferred from the ensemble median and interquartile range). Against satellite data, the ensemble AOD biases range from -37% (MODIS-Terra) to -16% (MERGED-FMI, a multi-satellite AOD product), which we explain by differences between individual satellites and AERONET measurements themselves. Correlation coefficients (R) between model and observation AOD records are generally high (R > 0.75), suggesting that the models are capable of capturing spatiotemporal variations in AOD. We find a much larger underestimate in coarse AOD(c) (similar to-45% +/- 25 %) than in fine AOD(f) (similar to-15% +/- 25 %) with slightly increased inter-model spread compared to total AOD. These results indicate problems in the modelling of DU and SS. The AOD(c) bias is likely due to missing DU over continental land masses (particularly over the United States, SE Asia, and S. America), while marine AERONET sites and the AATSR SU satellite data suggest more moderate oceanic biases in AOD(c). Column AEs are underestimated by about 10% +/- 16 %. For situations in which measurements show AE > 2, models underestimate AERONET AE by ca. 35 %. In contrast, all models (but one) exhibit large overestimates in AE when coarse aerosol dominates (bias ca. +140% if observed AE < 0.5). Simulated AE does not span the observed AE variability. These results indicate that models overestimate particle size (or underestimate the fine-mode fraction) for fine-dominated aerosol and underestimate size (or overestimate the fine-mode fraction) for coarse-dominated aerosol. This must have implications for lifetime, water uptake, scattering enhancement, and the aerosol radiative effect, which we can not quantify at this moment. Comparison against Global Atmosphere Watch (GAW) in situ data results in mean bias and inter-model variations of -35% +/- 25% and -20% +/- 18% for SCdry and AC(dry), respectively. The larger underestimate of SCdry than AC(dry) suggests the models will simulate an aerosol single scattering albedo that is too low. The larger underestimate of SCdry than ambient air AOD is consistent with recent findings that models overestimate scattering enhancement due to hygroscopic growth. The broadly consistent negative bias in AOD and surface scattering suggests an underestimate of aerosol radiative effects in current global aerosol models. Considerable inter-model diversity in the simulated optical properties is often found in regions that are, unfortunately, not or only sparsely covered by ground-based observations. This includes, for instance, the Sahara, Amazonia, central Australia, and the South Pacific. This highlights the need for a better site coverage in the observations, which would enable us to better assess the models, but also the performance of satellite products in these regions. Using fine-mode AOD as a proxy for present-day aerosol forcing estimates, our results suggest that models underestimate aerosol forcing by ca. -15 %, however, with a considerably large interquartile range, suggesting a spread between -35% and +10 %.Peer reviewe

Methane at Svalbard and over the European Arctic Ocean

Methane (CH4) is a powerful greenhouse gas. Its atmospheric mixing ratios have been increasing since 2005. Therefore, quantification of CH4 sources is essential for effective climate change mitigation. Here we report observations of the CH4 mixing ratios measured at the Zeppelin Observatory (Svalbard) in the Arctic and aboard the research vessel (RV) Helmer Hanssen over the Arctic Ocean from June 2014 to December 2016, as well as the long-term CH4 trend measured at the Zeppelin Observatory from 2001 to 2017. We investigated areas over the European Arctic Ocean to identify possible hotspot regions emitting CH4 from the ocean to the atmosphere, and used state-of-the-art modelling (FLEXPART) combined with updated emission inventories to identify CH4 sources. Furthermore, we collected air samples in the region as well as samples of gas hydrates, obtained from the sea floor, which we analysed using a new technique whereby hydrate gases are sampled directly into evacuated canisters. Using this new methodology, we evaluated the suitability of ethane and isotopic signatures (δ13C in CH4) as tracers for ocean-to-atmosphere CH4 emission. We found that the average methane / light hydrocarbon (ethane and propane) ratio is an order of magnitude higher for the same sediment samples using our new methodology compared to previously reported values, 2379.95 vs. 460.06, respectively. Meanwhile, we show that the mean atmospheric CH4 mixing ratio in the Arctic increased by 5.9±0.38 parts per billion by volume (ppb) per year (yr−1) from 2001 to 2017 and ∼8 pbb yr−1 since 2008, similar to the global trend of ∼ 7–8 ppb yr−1. Most large excursions from the baseline CH4 mixing ratio over the European Arctic Ocean are due to long-range transport from land-based sources, lending confidence to the present inventories for high-latitude CH4 emissions. However, we also identify a potential hotspot region with ocean–atmosphere CH4 flux north of Svalbard (80.4∘ N, 12.8∘ E) of up to 26 nmol m−2s−1 from a large mixing ratio increase at the location of 30 ppb. Since this flux is consistent with previous constraints (both spatially and temporally), there is no evidence that the area of interest north of Svalbard is unique in the context of the wider Arctic. Rather, because the meteorology at the time of the observation was unique in the context of the measurement time series, we obtained over the short course of the episode measurements highly sensitive to emissions over an active seep site, without sensitivity to land-based emissions

Multi-laboratory compilation of atmospheric methane data for the year 2021; obspack_ch4_1_NRT_v4.0_2022-03-03

This product is constructed using the Observation Package (ObsPack) framework [Masarie et al., 2014; www.earth-syst-sci-data.net/6/375/2014/]. The framework is designed to bring together atmospheric greenhouse gas (GHG) observations from a variety of sampling platforms, prepare them with specific applications in mind, and package and distribute them in a self-consistent and well-documented product. ObsPack products are intended to support GHG budget studies and represent a new generation of cooperative value-added GHG data products

Multi-laboratory compilation of atmospheric carbon dioxide data for the years 2020-2021; obspack_co2_1_NRT_v6.1.1_2021-05-17

This product is constructed using the Observation Package (ObsPack) framework [Masarie et al., 2014; www.earth-syst-sci-data.net/6/375/2014/]. The framework is designed to bring together atmospheric greenhouse gas (GHG) observations from a variety of sampling platforms, prepare them with specific applications in mind, and package and distribute them in a self-consistent and well-documented product. ObsPack products are intended to support GHG budget studies and represent a new generation of cooperative value-added GHG data products

Multi-laboratory compilation of atmospheric carbon dioxide data for the years 2020-2021; obspack_co2_1_NRT_v6.1_2021-02-02

A full list of all contributors for this product can be found at www.esrl.noaa.gov/gmd/ccgg/obspack/providerlist/obspack_co2_1_NRT_v6.1_2021-02-02.html This product is constructed using the Observation Package (ObsPack) framework [Masarie et al., 2014; www.earth-syst-sci-data.net/6/375/2014/]. The framework is designed to bring together atmospheric greenhouse gas (GHG) observations from a variety of sampling platforms, prepare them with specific applications in mind, and package and distribute them in a self-consistent and well-documented product. ObsPack products are intended to support GHG budget studies and represent a new generation of cooperative value-added GHG data products

The fingerprint of the summer 2018 drought in Europe on ground-based atmospheric CO2 measurements

During the summer of 2018, a widespread drought developed over Northern and Central Europe. The increase in temperature and the reduction of soil moisture have influenced carbon dioxide (CO2) exchange between the atmosphere and terrestrial ecosystems in various ways, such as a reduction of photosynthesis, changes in ecosystem respiration, or allowing more frequent fires. In this study, we characterize the resulting perturbation of the atmospheric CO2 seasonal cycles. 2018 has a good coverage of European regions affected by drought, allowing the investigation of how ecosystem flux anomalies impacted spatial CO2 gradients between stations. This density of stations is unprecedented compared to previous drought events in 2003 and 2015, particularly thanks to the deployment of the Integrated Carbon Observation System (ICOS) network of atmospheric greenhouse gas monitoring stations in recent years. Seasonal CO2 cycles from 48 European stations were available for 2017 and 2018. Earlier data were retrieved for comparison from international databases or national networks. Here, we show that the usual summer minimum in CO2 due to the surface carbon uptake was reduced by 1.4 ppm in 2018 for the 10 stations located in the area most affected by the temperature anomaly, mostly in Northern Europe. Notwithstanding, the CO2 transition phases before and after July were slower in 2018 compared to 2017, suggesting an extension of the growing season, with either continued CO2 uptake by photosynthesis and/or a reduction in respiration driven by the depletion of substrate for respiration inherited from the previous months due to the drought. For stations with sufficiently long time series, the CO2 anomaly observed in 2018 was compared to previous European droughts in 2003 and 2015. Considering the areas most affected by the temperature anomalies, we found a higher CO2 anomaly in 2003 (+3 ppm averaged over 4 sites), and a smaller anomaly in 2015 (+1 ppm averaged over 11 sites) compared to 2018. This article is part of the theme issue ‘Impacts of the 2018 severe drought and heatwave in Europe: from site to continental scale'

Multi-laboratory compilation of atmospheric methane data for the years 2020-2021; obspack_ch4_1_NRT_v3.0_2021-05-18

This product is constructed using the Observation Package (ObsPack) framework [Masarie et al., 2014; www.earth-syst-sci-data.net/6/375/2014/]. The framework is designed to bring together atmospheric greenhouse gas (GHG) observations from a variety of sampling platforms, prepare them with specific applications in mind, and package and distribute them in a self-consistent and well-documented product. ObsPack products are intended to support GHG budget studies and represent a new generation of cooperative value-added GHG data products