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This study examines the Arctic surface air temperature response to regional aerosol emissions reductions using three fully coupled chemistry–climate models: National Center for Atmospheric Research-Community Earth System Model version 1, Geophysical Fluid Dynamics Laboratory-Coupled Climate Model version 3 (GFDL-CM3) and Goddard Institute for Space Studies-ModelE version 2. Each of these models was used to perform a series of aerosol perturbation experiments, in which emissions of different aerosol types (sulfate, black carbon (BC), and organic carbon) in different northern mid-latitude source regions, and of biomass burning aerosol over South America and Africa, were substantially reduced or eliminated. We find that the Arctic warms in nearly every experiment, the only exceptions being the U.S. and Europe BC experiments in GFDL-CM3 in which there is a weak and insignificant cooling. The Arctic warming is generally larger than the global mean warming (i.e. Arctic amplification occurs), particularly during non-summer months. The models agree that changes in the poleward atmospheric moisture transport are the most important factor explaining the spread in Arctic warming across experiments: the largest warming tends to coincide with the largest increases in moisture transport into the Arctic. In contrast, there is an inconsistent relationship (correlation) across experiments between the local radiative forcing over the Arctic and the simulated Arctic warming, with this relationship being positive in one model (GFDL-CM3) and negative in the other two. Our results thus highlight the prominent role of poleward energy transport in driving Arctic warming and amplification, and suggest that the relative importance of poleward energy transport and local forcing/feedbacks is likely to be model dependent.

 

Observational records of meteorological and chemical variables are imprinted by an unknown combination of anthropogenic activity, natural forcings, and internal variability. With a 15-member initial-condition ensemble generated from the CESM2-WACCM6 chemistry-climate model for 1950–2014, we extract signals of anthropogenic (‘forced’) change from the noise of internally arising climate variability on observed tropospheric ozone trends. Positive trends in free tropospheric ozone measured at long-term surface observatories, by commercial aircraft, and retrieved from satellite instruments generally fall within the ensemble range. CESM2-WACCM6 tropospheric ozone trends are also bracketed by those in a larger ensemble constructed from five additional chemistry-climate models. Comparison of the multi-model ensemble with observed tropospheric column ozone trends in the northern tropics implies an underestimate in regional precursor emission growth over recent decades. Positive tropospheric ozone trends clearly emerge from 1950 to 2014, exceeding 0.2 DU yr⁻¹at 20–40 N in all CESM2-WACCM6 ensemble members. Tropospheric ozone observations are often only available for recent decades, and we show that even a two-decade record length is insufficient to eliminate the role of internal variability, which can produce regional tropospheric ozone trends oppositely signed from ensemble mean (forced) changes. By identifying regions and seasons with strong anthropogenic change signals relative to internal variability, initial-condition ensembles can guide future observing systems seeking to detect anthropogenic change. For example, analysis of the CESM2-WACCM6 ensemble reveals year-round upper tropospheric ozone increases from 1995 to 2014, largest at 30 S–40 N during boreal summer. Lower tropospheric ozone increases most strongly in the winter hemisphere, and internal variability leads to trends of opposite sign (ensemble overlaps zero) north of 40 N during boreal summer. This decoupling of ozone trends in the upper and lower troposphere suggests a growing prominence for tropospheric ozone as a greenhouse gas despite regional efforts to abate warm season ground-level ozone.

 

The sensitivity of sea ice to fire emissions highlights climate model uncertainty related to the accuracy of prescribed forcings. 

The catalytic depletion of Antarctic stratospheric ozone is linked to anthropogenic emissions of chlorine and bromine. Despite its larger ozone-depleting efficiency, the contribution of ocean-emitted iodine to ozone hole chemistry has not been evaluated, due to the negligible iodine levels previously reported to reach the stratosphere. Based on the recently observed range (0.77 ± 0.1 parts per trillion by volume [pptv]) of stratospheric iodine injection, we use the Whole Atmosphere Community Climate Model to assess the role of iodine in the formation and recent past evolution of the Antarctic ozone hole. Our 1980–2015 simulations indicate that iodine can significantly impact the lower part of the Antarctic ozone hole, contributing, on average, 10% of the lower stratospheric ozone loss during spring (up to 4.2% of the total stratospheric column). We find that the inclusion of iodine advances the beginning and delays the closure stages of the ozone hole by 3 d to 5 d, increasing its area and mass deficit by 11% and 20%, respectively. Despite being present in much smaller amounts, and due to faster gas-phase photochemical reactivation, iodine can dominate (∼73%) the halogen-mediated lower stratospheric ozone loss during summer and early fall, when the heterogeneous reactivation of inorganic chlorine and bromine reservoirs is reduced. The stratospheric ozone destruction caused by 0.77 pptv of iodine over Antarctica is equivalent to that of 3.1 (4.6) pptv of biogenic very short-lived bromocarbons during spring (rest of sunlit period). The relative contribution of iodine to future stratospheric ozone loss is likely to increase as anthropogenic chlorine and bromine emissions decline following the Montreal Protocol. 

The Toba eruption ∼74,000 y ago was the largest volcanic eruption since the start of the Pleistocene and represents an important test case for understanding the effects of large explosive eruptions on climate and ecosystems. However, the magnitude and repercussions of climatic changes driven by the eruption are strongly debated. High-resolution paleoclimate and archaeological records from Africa find little evidence for the disruption of climate or human activity in the wake of the eruption in contrast with a controversial link with a bottleneck in human evolution and climate model simulations predicting strong volcanic cooling for up to a decade after a Toba-scale eruption. Here, we use a large ensemble of high-resolution Community Earth System Model (CESM1.3) simulations to reconcile climate model predictions with paleoclimate records, accounting for uncertainties in the magnitude of Toba sulfur emissions with high and low emission scenarios. We find a near-zero probability of annual mean surface temperature anomalies exceeding 4 °C in most of Africa in contrast with near 100% probabilities of cooling this severe in Asia and North America for the high sulfur emission case. The likelihood of strong decreases in precipitation is low in most of Africa. Therefore, even Toba sulfur release at the upper range of plausible estimates remains consistent with the muted response in Africa indicated by paleoclimate proxies. Our results provide a probabilistic view of the uneven patterns of volcanic climate disruption during a crucial interval in human evolution, with implications for understanding the range of environmental impacts from past and future supereruptions.

 

Dimethyl sulfide (DMS), emitted from the oceans, is the most abundant biological source of sulfur to the marine atmosphere. Atmospheric DMS is oxidized to condensable products that form secondary aerosols that affect Earth’s radiative balance by scattering solar radiation and serving as cloud condensation nuclei. We report the atmospheric discovery of a previously unquantified DMS oxidation product, hydroperoxymethyl thioformate (HPMTF, HOOCH 2 SCHO), identified through global-scale airborne observations that demonstrate it to be a major reservoir of marine sulfur. Observationally constrained model results show that more than 30% of oceanic DMS emitted to the atmosphere forms HPMTF. Coincident particle measurements suggest a strong link between HPMTF concentration and new particle formation and growth. Analyses of these observations show that HPMTF chemistry must be included in atmospheric models to improve representation of key linkages between the biogeochemistry of the ocean, marine aerosol formation and growth, and their combined effects on climate. 

Many Chemistry‐Climate Models (CCMs) include a simplified treatment of brominated very short‐lived (VSL^Br) species by assuming CH₃Br as a surrogate for VSL^Br. However, neglecting a comprehensive treatment of VSL^Brin CCMs may yield an unrealistic representation of the associated impacts. Here, we use the Community Atmospheric Model with Chemistry (CAM‐Chem) CCM to quantify the tropospheric and stratospheric changes between various VSL^Brchemical approaches with increasing degrees of complexity (i.e., surrogate, explicit, and full). Our CAM‐Chem results highlight the improved accuracy achieved by considering a detailed treatment of VSL^Brphotochemistry, including sea‐salt aerosol dehalogenation and heterogeneous recycling on ice‐crystals. Differences between the full and surrogate schemes maximize in the lowermost stratosphere and midlatitude free troposphere, resulting in a latitudinally dependent reduction of ∼1–7 DU in total ozone column and a ∼5%–15% decrease of the OH/HO₂ratio. We encourage all CCMs to include a complete chemical treatment of VSL^Brin the troposphere and stratosphere.