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Sixty-six million years ago, an asteroid approximately 9 km in diameter hit the hydrocarbon- and sulfur-rich sedimentary rocks in what is now Mexico. Recent studies have shown that this impact at the Yucatan Peninsula heated the hydrocarbon and sulfur in these rocks, forming stratospheric soot and sulfate aerosols and causing extreme global cooling and drought. These events triggered a mass extinction, including dinosaurs, and led to the subsequent macroevolution of mammals. The amount of hydrocarbon and sulfur in rocks varies widely, depending on location, which suggests that cooling and extinction levels were dependent on impact site. Here we show that the probability of significant global cooling, mass extinction, and the subsequent appearance of mammals was quite low after an asteroid impact on the Earth’s surface. This significant event could have occurred if the asteroid hit the hydrocarbon-rich areas occupying approximately 13% of the Earth’s surface. The site of asteroid impact, therefore, changed the history of life on Earth.

The mass extinction of life 66 million years ago at the Cretaceous/Paleogene boundary, marked by the extinctions of dinosaurs and shallow marine organisms, is important because it led to the macroevolution of mammals and appearance of humans. The current hypothesis for the extinction is that an asteroid impact in present-day Mexico formed condensed aerosols in the stratosphere, which caused the cessation of photosynthesis and global near-freezing conditions. Here, we show that the stratospheric aerosols did not induce darkness that resulted in milder cooling than previously thought. We propose a new hypothesis that latitude-dependent climate changes caused by massive stratospheric soot explain the known mortality and survival on land and in oceans at the Cretaceous/Paleogene boundary. The stratospheric soot was ejected from the oil-rich area by the asteroid impact and was spread globally. The soot aerosols caused sufficiently colder climates at mid–high latitudes and drought with milder cooling at low latitudes on land, in addition to causing limited cessation of photosynthesis in global oceans within a few months to two years after the impact, followed by surface-water cooling in global oceans in a few years. The rapid climate change induced terrestrial extinctions followed by marine extinctions over several years.

The effective radiative forcing (ERF) of anthropogenic gases and aerosols under present-day conditions relative to preindustrial conditions is estimated using the Meteorological Research Institute Earth System Model version 2.0 (MRI-ESM2.0) as part of the Radiative Forcing Model Intercomparison Project (RFMIP) and Aerosol and Chemistry Model Intercomparison Project (AerChemMIP), endorsed by the sixth phase of the Coupled Model Intercomparison Project (CMIP6). The global mean total anthropogenic net ERF estimate at the top of the atmosphere is 1.96 W m−2 and is composed primarily of positive forcings due to carbon dioxide (1.85 W m−2), methane (0.71 W m−2), and halocarbons (0.30 W m−2) and negative forcing due to the total aerosols (− 1.22 W m−2). The total aerosol ERF consists of 23% from aerosol-radiation interactions (− 0.32 W m−2), 71% from aerosol-cloud interactions (− 0.98 W m−2), and slightly from surface albedo changes caused by aerosols (0.08 W m−2). The ERFs due to aerosol-radiation interactions consist of opposing contributions from light-absorbing black carbon (BC) (0.25 W m−2) and from light-scattering sulfate (− 0.48 W m−2) and organic aerosols (− 0.07 W m−2) and are pronounced over emission source regions. The ERFs due to aerosol-cloud interactions (ERFaci) are prominent over the source and downwind regions, caused by increases in the number concentrations of cloud condensation nuclei and cloud droplets in low-level clouds. Concurrently, increases in the number concentration of ice crystals in high-level clouds (temperatures < –38 °C), primarily induced by anthropogenic BC aerosols, particularly over tropical convective regions, cause both substantial negative shortwave and positive longwave ERFaci values in MRI-ESM2.0. These distinct forcings largely cancel each other; however, significant longwave radiative heating of the atmosphere caused by high-level ice clouds suggests the importance of further studies on the interactions of aerosols with ice clouds. Total anthropogenic net ERFs are almost entirely positive over the Arctic due to contributions from the surface albedo reductions caused by BC. In the Arctic, BC provides the second largest contribution to the positive ERFs after carbon dioxide, suggesting a possible important role of BC in Arctic surface warming.

This work presents an analysis of the effect of climate change on surface ozone discussing the related penalties and benefits around the globe from the global modelling perspective based on simulations with five CMIP6 (Coupled Model Intercomparison Project Phase 6) Earth System Models. As part of AerChemMIP (Aerosol Chemistry Model Intercomparison Project) all models conducted simulation experiments considering future climate (ssp370SST) and present-day climate (ssp370pdSST) under the same future emissions trajectory (SSP3-7.0). A multi-model global average climate change benefit on surface ozone of −0.96 ± 0.07 ppbv °C−1 is calculated which is mainly linked to the dominating role of enhanced ozone destruction with higher water vapour abundances under a warmer climate. Over regions remote from pollution sources, there is a robust decline in mean surface ozone concentration on an annual basis as well as for boreal winter and summer varying spatially from −0.2 to −2 ppbv °C−1, with strongest decline over tropical oceanic regions. The implication is that over regions remote from pollution sources (except over the Arctic) there is a consistent climate change benefit for baseline ozone due to global warming. However, ozone increases over regions close to anthropogenic pollution sources or close to enhanced natural biogenic volatile organic compounds emission sources with a rate ranging regionally from 0.2 to 2 ppbv C−1, implying a regional surface ozone penalty due to global warming. Overall, the future climate change enhances the efficiency of precursor emissions to generate surface ozone in polluted regions and thus the magnitude of this effect depends on the regional emission changes considered in this study within the SSP3_7.0 scenario. The comparison of the climate change impact effect on surface ozone versus the combined effect of climate and emission changes indicates the dominant role of precursor emission changes in projecting surface ozone concentrations under future climate change scenarios.

Anthropogenic NO x emissions have altered the biogeochemical nitrogen cycle since the Industrial Revolution, yet Arctic ice core nitrate (NO 3 − ) records are inconsistent with post-1970s NO x emission reductions. Here we show a NO 3 − deposition history covering 1800–2020 using an ice core from the southeastern Greenland dome with high snow accumulation. The ice core NO 3 − concentrations are particularly disconnected from NO x source regions during the peak pollution period and post-1990s. A global chemical transport model reproduced these discordances between total NO 3 − and NO x emissions by altering gaseous HNO 3 and particulate NO 3 − (p-NO 3 − ) ratios and subsequently NO 3 − lifetime. This result and correlations with acidity parameters recorded in the ice core, suggest that acidity-driven gas-particle partitioning of NO 3 − regulates its transport to Arctic regions alongside changes in NO x emissions. In the future, despite NO x reductions, the increase in proportion of p-NO 3 − with longer atmospheric lifetime becomes crucial to control the Arctic NO 3 − burden. A Greenland ice core reveals that Arctic atmospheric nitrate since the Industrial Revolution has been controlled not only by NOx emissions but also by atmospheric acidity, affecting its gas-particle partitioning, lifetime, and long-range transport.

Simulations by six Coupled Model Intercomparison Project Phase 6 (CMIP6) Earth system models indicate that the seasonal cycle of baseline tropospheric ozone at northern midlatitudes has been shifting since the mid-20th century. Beginning in ∼ 1940, the magnitude of the seasonal cycle increased by ∼10 ppb (measured from seasonal minimum to maximum), and the seasonal maximum shifted to later in the year by about 3 weeks. This shift maximized in the mid-1980s, followed by a reversal – the seasonal cycle decreased in amplitude and the maximum shifted back to earlier in the year. Similar changes are seen in measurements collected from the 1970s to the present. The timing of the seasonal cycle changes is generally concurrent with the rise and fall of anthropogenic emissions that followed industrialization and the subsequent implementation of air quality emission controls. A quantitative comparison of the temporal changes in the ozone seasonal cycle at sites in both Europe and North America with the temporal changes in ozone precursor emissions across the northern midlatitudes found a high degree of similarity between these two temporal patterns. We hypothesize that changing precursor emissions are responsible for the shift in the ozone seasonal cycle; this is supported by the absence of such seasonal shifts in southern midlatitudes where anthropogenic emissions are much smaller. We also suggest a mechanism by which changing emissions drive the changing seasonal cycle: increasing emissions of NOx allow summertime photochemical production of ozone to become more important than ozone transported from the stratosphere, and increasing volatile organic compounds (VOCs) lead to progressively greater photochemical ozone production in the summer months, thereby increasing the amplitude of the seasonal ozone cycle. Decreasing emissions of both precursor classes then reverse these changes. The quantitative parameter values that characterize the seasonal shifts provide useful benchmarks for evaluating model simulations, both against observations and between models.

Observed trends in tropospheric ozone, an important air pollutant and short-lived climate forcer (SLCF), are estimated using available surface and ozonesonde profile data for 1993–2019, using a coherent methodology, and compared to modeled trends (1995–2015) from the Arctic Monitoring Assessment Program SLCF 2021 assessment. Increases in observed surface ozone at Arctic coastal sites, notably during winter, and concurrent decreasing trends in surface carbon monoxide, are generally captured by multi-model median trends. Wintertime increases are also estimated in the free troposphere at most Arctic sites, with decreases during spring months. Winter trends tend to be overestimated by the multi-model medians. Springtime surface ozone increases in northern coastal Alaska are not simulated while negative springtime trends in northern Scandinavia are not always reproduced. Possible reasons for observed changes and model performance are discussed including decreasing precursor emissions, changing ozone dry deposition, and variability in large-scale meteorology.

In this work, we use Coupled Model Intercomparison Project Phase 6 (CMIP6) simulations from 10 Earth system models (ESMs) and general circulation models (GCMs) to study the fast climate responses on pre-industrial climate, due to present-day aerosols. All models carried out two sets of simulations: a control experiment with all forcings set to the year 1850 and a perturbation experiment with all forcings identical to the control, except for aerosols with precursor emissions set to the year 2014. In response to the pattern of all aerosols effective radiative forcing (ERF), the fast temperature responses are characterized by cooling over the continental areas, especially in the Northern Hemisphere, with the largest cooling over East Asia and India, sulfate being the dominant aerosol surface temperature driver for present-day emissions. In the Arctic there is a warming signal for winter in the ensemble mean of fast temperature responses, but the model-to-model variability is large, and it is presumably linked to aerosol-induced circulation changes. The largest fast precipitation responses are seen in the tropical belt regions, generally characterized by a reduction over continental regions and presumably a southward shift of the tropical rain belt. This is a characteristic and robust feature among most models in this study, associated with weakening of the monsoon systems around the globe (Asia, Africa and America) in response to hemispherically asymmetric cooling from a Northern Hemisphere aerosol perturbation, forcing possibly the Intertropical Convergence Zone (ITCZ) and tropical precipitation to shift away from the cooled hemisphere despite that aerosols' effects on temperature and precipitation are only partly realized in these simulations as the sea surface temperatures are kept fixed. An interesting feature in aerosol-induced circulation changes is a characteristic dipole pattern with intensification of the Icelandic Low and an anticyclonic anomaly over southeastern Europe, inducing warm air advection towards the northern polar latitudes in winter.

The Amazon basin is important for understanding the global climate because of its carbon cycle and as a laboratory for obtaining basic knowledge of the continental background atmosphere. Aerosol particles play an important role in the climate and weather, and knowledge of their compositions and mixing states is necessary to understand their influence on the climate. For this study, we collected aerosol particles from the Amazon basin during the Green Ocean Amazon (GoAmazon2014/5) campaign (February to March 2014) at the T3 site, which is located about 70 km from Manaus, and analyzed them using transmission electron microscopy (TEM). TEM has better spatial resolution than other instruments, which enables us to analyze the occurrences of components that attach to or are embedded within other particles. Based on the TEM results of more than 10 000 particles from several transport events, this study shows the occurrences of individual particles including compositions, size distributions, number fractions, and possible sources of materials that mix with other particles. Aerosol particles during the wet season were from both natural sources such as the Amazon forest, Saharan desert, Atlantic Ocean, and African biomass burning and anthropogenic sources such as Manaus and local emissions. These particles mix together at an individual particle scale. The number fractions of mineral dust and sea-salt particles increased almost 3-fold when long-range transport (LRT) from the African continent occurred. Nearly 20 % of mineral dust and primary biological aerosol particles had attached sea salts on their surfaces. Sulfates were also internally mixed with sea-salt and mineral dust particles. The TEM element mapping images showed that several components with sizes of hundreds of nanometers from different sources commonly occur within individual LRT aerosol particles. We conclude that many aerosol particles from natural sources change their compositions by mixing during transport. The compositions and mixing states of these particles after emission result in changes in their hygroscopic and optical properties and should be considered when assessing their effects on climate.

Ground-based measurements of black carbon (BC) were performed near an industrial source region in the early summer of 2014 and at a remote island in Japan in the spring of 2015. Here, we report the temporal variations in the transport, size distributions, and mixing states of the BC-containing particles. These particles were characterized using a continuous soot monitoring system, a single particle soot photometer, and an aerosol chemical speciation monitor. The effects of aging on the growth of BC-containing particles were examined by comparing the ground-based observations between the near-source and remote island sites. Secondary formation of sulfate and organic aerosols strongly affected the increases in BC coating (i.e., enhancement of cloud condensation nuclei activity) with air mass aging from the source to the outflow regions. The effects of wet removal on BC microphysics were elucidated by classifying the continental outflow air masses depending on the enhancement ratios of BC to CO (ΔBC ∕ ΔCO), which were used as an indicator of the transport efficiency of BC. It was found that ΔBC ∕ ΔCO ratios were controlled mainly by the wet removal during transport in the planetary boundary layer (PBL) on the timescale of 1–2 days. The meteorological conditions and backward trajectory analyses suggested that air masses strongly affected by wet removal originated mainly from a region in southern China (20–35° N) in the spring of 2015. Removal of large and thickly coated BC-containing particles was detected in the air masses that were substantially affected by the wet removal in the PBL, as predicted by Köhler theory. The size and water solubility of BC-containing particles in the PBL can be altered by the wet removal as well as the condensation of non-BC materials.