- Award ID(s):
- 2127733
- NSF-PAR ID:
- 10394202
- Date Published:
- Journal Name:
- Atmospheric Chemistry and Physics
- Volume:
- 22
- Issue:
- 5
- ISSN:
- 1680-7324
- Page Range / eLocation ID:
- 3067 to 3096
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
Anthropogenic and natural emissions contribute to enhanced concentrations of aerosols in the Arctic winter and early spring, with most attention being paid to anthropogenic aerosols that contribute to so-called Arctic haze. Less-well-studied wintertime sea-spray aerosols (SSAs) under Arctic haze conditions are the focus of this study, since they can make an important contribution to wintertime Arctic aerosol abundances. Analysis of field campaign data shows evidence for enhanced local sources of SSAs, including marine organics at Utqiaġvik (formerly known as Barrow) in northern Alaska, United States, during winter 2014. Models tend to underestimate sub-micron SSAs and overestimate super-micron SSAs in the Arctic during winter, including the base version of the Weather Research Forecast coupled with Chemistry (WRF-Chem) model used here, which includes a widely used SSA source function based on Gong et al. (1997). Quasi-hemispheric simulations for winter 2014 including updated wind speed and sea-surface temperature (SST) SSA emission dependencies and sources of marine sea-salt organics and sea-salt sulfate lead to significantly improved model performance compared to observations at remote Arctic sites, notably for coarse-mode sodium and chloride, which are reduced. The improved model also simulates more realistic contributions of SSAs to inorganic aerosols at different sites, ranging from 20 %–93 % in the observations. Two-thirds of the improved model performance is from the inclusion of the dependence on SSTs. The simulation of nitrate aerosols is also improved due to less heterogeneous uptake of nitric acid on SSAs in the coarse mode and related increases in fine-mode nitrate. This highlights the importance of interactions between natural SSAs and inorganic anthropogenic aerosols that contribute to Arctic haze. Simulation of organic aerosols and the fraction of sea-salt sulfate are also improved compared to observations. However, the model underestimates episodes with elevated observed concentrations of SSA components and sub-micron non-sea-salt sulfate at some Arctic sites, notably at Utqiaġvik. Possible reasons are explored in higher-resolution runs over northern Alaska for periods corresponding to the Utqiaġvik field campaign in January and February 2014. The addition of a local source of sea-salt marine organics, based on the campaign data, increases modelled organic aerosols over northern Alaska. However, comparison with previous available data suggests that local natural sources from open leads, as well as local anthropogenic sources, are underestimated in the model. Missing local anthropogenic sources may also explain the low modelled (sub-micron) non-sea-salt sulfate at Utqiaġvik. The introduction of a higher wind speed dependence for sub-micron SSA emissions, also based on Arctic data, reduces biases in modelled sub-micron SSAs, while sea-ice fractions, including open leads, are shown to be an important factor controlling modelled super-micron, rather than sub-micron, SSAs over the north coast of Alaska. The regional results presented here show that modelled SSAs are more sensitive to wind speed dependence but that realistic modelling of sea-ice distributions is needed for the simulation of local SSAs, including marine organics. This study supports findings from the Utqiaġvik field campaign that open leads are the primary source of fresh and aged SSAs, including marine organic aerosols, during wintertime at Utqiaġvik; these findings do not suggest an influence from blowing snow and frost flowers. To improve model simulations of Arctic wintertime aerosols, new field data on processes that influence wintertime SSA production, in particular for fine-mode aerosols, are needed as is improved understanding about possible local anthropogenic sources.more » « less
-
Abstract. Changes in anthropogenic aerosol emissions have strongly contributed to global and regional trends in temperature, precipitation, and other climate characteristics and have been one of the dominant drivers of decadal trends in Asian and African precipitation. These and other influences on regional climate from changes in aerosol emissions are expected to continue and potentially strengthen in the coming decades. However, a combination of large uncertainties in emission pathways, radiative forcing, and the dynamical response to forcing makes anthropogenic aerosol a key factor in the spread of near-term climate projections, particularly on regional scales, and therefore an important one to constrain. For example, in terms of future emission pathways, the uncertainty in future global aerosol and precursor gas emissions by 2050 is as large as the total increase in emissions since 1850. In terms of aerosol effective radiative forcing, which remains the largest source of uncertainty in future climate change projections, CMIP6 models span a factor of 5, from −0.3 to −1.5 W m−2. Both of these sources of uncertainty are exacerbated on regional scales. The Regional Aerosol Model Intercomparison Project (RAMIP) will deliver experiments designed to quantify the role of regional aerosol emissions changes in near-term projections. This is unlike any prior MIP, where the focus has been on changes in global emissions and/or very idealised aerosol experiments. Perturbing regional emissions makes RAMIP novel from a scientific standpoint and links the intended analyses more directly to mitigation and adaptation policy issues. From a science perspective, there is limited information on how realistic regional aerosol emissions impact local as well as remote climate conditions. Here, RAMIP will enable an evaluation of the full range of potential influences of realistic and regionally varied aerosol emission changes on near-future climate. From the policy perspective, RAMIP addresses the burning question of how local and remote decisions affecting emissions of aerosols influence climate change in any given region. Here, RAMIP will provide the information needed to make direct links between regional climate policies and regional climate change. RAMIP experiments are designed to explore sensitivities to aerosol type and location and provide improved constraints on uncertainties driven by aerosol radiative forcing and the dynamical response to aerosol changes. The core experiments will assess the effects of differences in future global and regional (Africa and the Middle East, East Asia, North America and Europe, and South Asia) aerosol emission trajectories through 2051, while optional experiments will test the nonlinear effects of varying emission locations and aerosol types along this future trajectory. All experiments are based on the shared socioeconomic pathways and are intended to be performed with 6th Climate Model Intercomparison Project (CMIP6) generation models, initialised from the CMIP6 historical experiments, to facilitate comparisons with existing projections. Requested outputs will enable the analysis of the role of aerosol in near-future changes in, for example, temperature and precipitation means and extremes, storms, and air quality.
-
Anthropogenic sulfate aerosols are estimated to have offset sixty percent of greenhouse-gas-induced warming in the Arctic, a region warming four times faster than the rest of the world. However, sulfate radiative forcing estimates remain uncertain because the relative contributions from anthropogenic versus natural sources to total sulfate aerosols are unknown. Here we measure sulfur isotopes of sulfate in a Summit, Greenland ice core from 1850 to 2006 CE to quantify the contribution of anthropogenic sulfur emissions to ice core sulfate. We use a Keeling Plot to determine the anthropogenic sulfur isotopic signature (δ34Santhro = +2.9 0.3 ‰), and compare this result to a compilation of sulfur isotope measurements of oil and coal. Using δ34Santhro, we quantify anthropogenic sulfate concentration separated from natural sulfate. Anthropogenic sulfate concentration increases to 68 ± 7% of non-sea-salt sulfate (65.1 ± 20.2 µg kg-1) during peak anthropogenic emissions from 1960 to 1990 and decreases to 45 ± 11% of non-sea-salt sulfate (25.4 ± 12.8 µg kg-1) from 1996 to 2006. These observations provide the first long-term record of anthropogenic sulfate distinguished from natural sources (e.g., volcanoes, dimethyl sulfide), and can be used to evaluate model characterization of anthropogenic sulfate aerosol fraction and radiative forcing over the industrial era. These data include sulfur isotopes of sulfate measurements from a Greenland ice core from 1850-2006. The preindustrial dataset (1200-1850) is uploaded to the Arctic data center here: doi:10.18739/A2N873162more » « less
-
Abstract Anthropogenic sulfate aerosols are estimated to have offset 60% of greenhouse-gas-induced warming in the Arctic, a region warming four times faster than the rest of the world. However, sulfate radiative forcing estimates remain uncertain because the relative contributions from anthropogenic versus natural sources to total sulfate aerosols are unknown. Here we measure sulfur isotopes of sulfate in a Summit, Greenland ice core from 1850 to 2006 CE to quantify the contribution of anthropogenic sulfur emissions to ice core sulfate. We use a Keeling plot to determine the anthropogenic sulfur isotopic signature (δ34Santhro= +2.9 ± 0.3 ‰), and compare this result to a compilation of sulfur isotope measurements of oil and coal. Using δ34Santhro, we quantify anthropogenic sulfate concentration separated from natural sulfate. Anthropogenic sulfate concentration increases to 67 ± 7% of non-sea-salt sulfate (65.1 ± 20.2
µ g kg−1) during peak anthropogenic emissions from 1960 to 1990 and decreases to 45 ± 11% of non-sea-salt sulfate (25.4 ± 12.8µ g kg−1) from 1996 to 2006. These observations provide the first long-term record of anthropogenic sulfate distinguished from natural sources (e.g. volcanoes, dimethyl sulfide), and can be used to evaluate model characterization of anthropogenic sulfate aerosol fraction and radiative forcing over the industrial era. -
Anthropogenic sulfate aerosols are estimated to have offset sixty percent of greenhouse-gas-induced warming in the Arctic, a region warming four times faster than the rest of the world. However, sulfate radiative forcing estimates remain uncertain because the relative contributions from anthropogenic versus natural sources to total sulfate aerosols are unknown. Here we measure sulfur isotopes of sulfate in a Summit, Greenland ice core from 1850 to 2006 CE to quantify the contribution of anthropogenic sulfur emissions to ice core sulfate. We use a Keeling Plot to determine the anthropogenic sulfur isotopic signature (δ34Santhro = +2.9 ± 0.3 ‰), and compare this result to a compilation of sulfur isotope measurements of oil and coal. Using δ34Santhro, we quantify anthropogenic sulfate concentration separated from natural sulfate. Anthropogenic sulfate concentration increases to 68 ± 7% of non-sea-salt sulfate (65.1 ± 20.2 µg kg-1) during peak anthropogenic emissions from 1960 to 1990 and decreases to 45 ± 11% of non-sea-salt sulfate (25.4 ± 12.8 µg kg-1) from 1996 to 2006. These observations provide the first long-term record of anthropogenic sulfate distinguished from natural sources (e.g., volcanoes, dimethyl sulfide), and can be used to evaluate model characterization of anthropogenic sulfate aerosol fraction and radiative forcing over the industrial era.more » « less