Climate influences near-surface biogeochemical processes and thereby determines the partitioning of carbon dioxide (CO2) in shale, and yet the controls on carbon (C) weathering fluxes remain poorly constrained. Using a dataset that characterizes biogeochemical responses to climate forcing in shale regolith, we implement a numerical model that describes the effects of water infiltration events, gas exchange, and temperature fluctuations on soil respiration and mineral weathering at a seasonal timescale. Our modeling approach allows us to quantitatively disentangle the controls of transient climate forcing and biogeochemical mechanisms on C partitioning. We find that ~3% of soil CO2 (1.02 mol C/m2/y) is exported to the subsurface during large infiltration events. Here, net atmospheric CO2 drawdown primarily occurs during spring snowmelt, governs the aqueous C exports (61%), and exceeds the CO2 flux generated by pyrite and petrogenic organic matter oxidation (~0.2 mol C/m2/y). We show that shale CO2 consumption results from the temporal coupling between soil microbial respiration and carbonate weathering. This coupling is driven by the impacts of hydrologic fluctuations on fresh organic matter availability and CO2 transport to the weathering front. Diffusion-limited transport of gases under transient hydrological conditions exerts an important control on CO2(g) egress patterns and thus must be considered when inferring soil CO2 drawdown from the gas phase composition. Our findings emphasize the importance of seasonal climate forcing in shaping the net contribution of shale weathering to terrestrial C fluxes and suggest that warmer conditions could reduce the potential for shale weathering to act as a CO2 sink.

The aviation industry faces a formidable challenge to cap its climate impact in the face of continued growth in passengers and freight. Liquid hydrogen (LH2) is one of the alternative jet fuels under consideration as it does not produce carbon dioxide upon combustion. We conducted a well-to-wake life cycle assessment of CO2 emissions and non-CO2 climate change impacts per passenger-distance for 17 different hydrogen production routes, as well as conventional jet fuel and biofuels. Six other environmental and health impact categories were also considered. The Boeing 787-800 was used as the reference aircraft, and a range of flight distances were explored. Contrail cirrus contributes around 81 ± 31% of the combustion climate impacts for LH2, compared to 32 ± 7% for conventional jet fuel, showing that research is needed to reduce uncertainty in the case of LH2. The life cycle impacts of the two dominant commercial LH2 pathways are on average 8 and 121% larger than conventional jet fuel. Some novel LH2 pathways do show considerable potential for life cycle climate impact reductions versus conventional fuel (up to -205 ± 78%). LH2 from renewable energy is not climate neutral, though, at best -67 ± 10% compared to conventional over the life cycle.

Green alder (Alnus alnobetula), a tall multi-stemmed deciduous shrub, is widespread at high elevations in the Central European Alps. Its growth form frequently leads to asymmetric radial growth and anomalous growth ring patterns, making development of representative ring-width series a challenge. In order to assess the variability among radii of one shoot, among shoots belonging to one stock and among stocks, 60 stem discs were sampled at treeline on Mt. Patscherkofel (Tyrol, Austria). Annual increments were measured along 188 radii and analyzed in terms of their variability by applying dendrochronological techniques. Results revealed a high agreement in ring-width variation among radii of one shoot, among shoots of one stock and largely among stocks from different sites, confirming the pronounced limitation of radial stem growth by climate forcing at the alpine treeline. In contrast to this, a high variability in both absolute growth rates and long-term growth trends was found, which we attribute to different microsite conditions and disturbances. These factors also override climate control of radial growth under growth-limiting environmental conditions. Based on our findings we provide recommendations for the number of samples needed to carry out inter- and intra-annual studies of radial growth in this multi-stemmed clonal shrub.

The glacial-interglacial variability of precipitation and its driving mechanism in monsoonal regions has long been a subject of debate. However, there are few records of quantitative climate reconstruction dating to the last glacial cycle in areas dominated by the Asian summer monsoon. Here, using a pollen-based quantitative climate reconstruction based on three sites in areas exposed to the Asian summer monsoon, we demonstrate that climate has undergone great variability over the past 68 ka. The differences between the last glacial and the Holocene optimum could have been as much as 35%-51% for precipitation, and 5-7 °C for mean annual temperature. Our findings also reveal regional heterogeneity during the abrupt climate events of Heinrich Event 1 and Younger Dryas, that drove drier conditions in southwestern China dominated by the Indian summer monsoon, and a wetter climate in central eastern China. The pattern of variation in reconstructed precipitation, exhibiting strong glacial-interglacial variability, is broadly consistent with the stalagmite δ18O records from Southwest China and South Asia. Our results of reconstruction quantify the sensitivity of the MIS3 precipitation to orbital insolation changes, and highlight the prominent influence of interhemispheric temperature gradients on Asian monsoon variability. Comparison with transient simulations and major climate forcings has shown that the mode of precipitation variability during the transition from the last glacial maximum to the Holocene has been significantly modulated by weak or collapsed Atlantic meridional overturning circulation events in addition to insolation forcing.

Sustainable aviation fuel (SAF) can reduce aviation\'s CO2 and non-CO2 impacts. We quantify the change in contrail properties and climate forcing in the North Atlantic resulting from different blending ratios of SAF and demonstrate that intelligently allocating the limited SAF supply could multiply its overall climate benefit by factors of 9-15. A fleetwide adoption of 100% SAF increases contrail occurrence (+5%), but lower nonvolatile particle emissions (-52%) reduce the annual mean contrail net radiative forcing (-44%), adding to climate gains from reduced life cycle CO2 emissions. However, in the short term, SAF supply will be constrained. SAF blended at a 1% ratio and uniformly distributed to all transatlantic flights would reduce both the annual contrail energy forcing (EFcontrail) and the total energy forcing (EFtotal, contrails + change in CO2 life cycle emissions) by ∼0.6%. Instead, targeting the same quantity of SAF at a 50% blend ratio to ∼2% of flights responsible for the most highly warming contrails reduces EFcontrail and EFtotal by ∼10 and ∼6%, respectively. Acknowledging forecasting uncertainties, SAF blended at lower ratios (10%) and distributed to more flights (∼9%) still reduces EFcontrail (∼5%) and EFtotal (∼3%). Both strategies deploy SAF on flights with engine particle emissions exceeding 1012 m-1, at night-time, and in winter.

Ecotron facilities allow accurate control of many environmental variables coupled with extensive monitoring of ecosystem processes. They therefore require multivariate perturbation of climate variables, close to what is observed in the field and projections for the future. Here, we present a new method for creating realistic climate forcing for manipulation experiments and apply it to the UHasselt Ecotron experiment. The new methodology uses data derived from the best available regional climate model projection and consists of generating climate forcing along a gradient representative of increasingly high global mean air temperature anomalies. We first identified the best-performing regional climate model simulation for the ecotron site from the Coordinated Regional Downscaling Experiment in the European domain (EURO-CORDEX) ensemble based on two criteria: (i) highest skill compared to observations from a nearby weather station and (ii) representativeness of the multi-model mean in future projections. The time window is subsequently selected from the model projection for each ecotron unit based on the global mean air temperature of the driving global climate model. The ecotron units are forced with 3-hourly output from the projections of the 5-year period in which the global mean air temperature crosses the predefined values. With the new approach, Ecotron facilities become able to assess ecosystem responses on changing climatic conditions, while accounting for the co-variation between climatic variables and their projection in variability, well representing possible compound events. The presented methodology can also be applied to other manipulation experiments, aiming at investigating ecosystem responses to realistic future climate change.

The assassination of Julius Caesar in 44 BCE triggered a power struggle that ultimately ended the Roman Republic and, eventually, the Ptolemaic Kingdom, leading to the rise of the Roman Empire. Climate proxies and written documents indicate that this struggle occurred during a period of unusually inclement weather, famine, and disease in the Mediterranean region; historians have previously speculated that a large volcanic eruption of unknown origin was the most likely cause. Here we show using well-dated volcanic fallout records in six Arctic ice cores that one of the largest volcanic eruptions of the past 2,500 y occurred in early 43 BCE, with distinct geochemistry of tephra deposited during the event identifying the Okmok volcano in Alaska as the source. Climate proxy records show that 43 and 42 BCE were among the coldest years of recent millennia in the Northern Hemisphere at the start of one of the coldest decades. Earth system modeling suggests that radiative forcing from this massive, high-latitude eruption led to pronounced changes in hydroclimate, including seasonal temperatures in specific Mediterranean regions as much as 7 °C below normal during the 2 y period following the eruption and unusually wet conditions. While it is difficult to establish direct causal linkages to thinly documented historical events, the wet and very cold conditions from this massive eruption on the opposite side of Earth probably resulted in crop failures, famine, and disease, exacerbating social unrest and contributing to political realignments throughout the Mediterranean region at this critical juncture of Western civilization.

Although the use of sub-fossil testate amoebae as a proxy for raised bog hydrology in Holocene paleoecological studies is well-established, some detailed aspects of species-environment relationships remain under-researched. One such issue is the effect of bog surface microtopography on the climatic sensitivity of testate amoeba communities. Although it has been suggested that some microforms-especially hummocks-may be less sensitive to climatic forcing than others, this has rarely been objectively tested. To investigate this, subfossil testate amoebae assemblages have been examined in a series of shallow cores collected along a hummock-lawn-hollow transect from a bog in central Ireland and the resulting reconstructed water table records, dated using 210Pb, have been compared with instrumental weather data. Testate amoebae communities in the hollow microform were found to be significantly less diverse than those in the hummock and lawn, and both the hummock and lawn showed statistically significant correlations with instrumental temperature and precipitation data. Therefore, whilst the suggestion that paleoecological investigations should target intermediate bog microforms remains sound, the notion that hummock-based testate amoebae hydrological data are climatically-insensitive is challenged.

While brown carbon is a strongly-light-absorbing type of organic aerosol that is capable of significant regional radiative forcing, it has been neglected from climate models, which results in differences between model predictions and measured data. This also results from uncertainty regarding the relationship between the chemical composition of brown carbon and its optical properties. Herein, here was utilized a time-dependent density functional theory (TD-DFT) approach to model the \"real-world\" absorption of thirty polycyclic aromatic hydrocarbons (PAHs) and twenty-five derivatives (ten nitro-PAHs and fifteen oxygenated-PAHs) present in the atmosphere over three Southern European cities (Porto, Florence and Athens). These data were corrected both for \"real-world\" experimental concentration of these molecules over these cities, and for their theoretical fluorescence yield. These results indicate that the absorption of the molecules more relevant for climate forcing are at ~330, ~360 and ~440 nm. Furthermore, the absorption is explained mainly by PAH and oxygenated-PAH molecules, while nitro-PAHs provide only negligible contributions. Porto should be the city to be most affected by radiative forcing induced by these molecules, while Florence and Athens appear to be similarly affected. Finally, these models also demonstrate that absorption at ~330 nm is explained by both PAH and oxygenated-PAH molecules, while absorption at ~360 and ~440 nm is only attributed to oxygenated-PAHs. More specifically, from the fifty-five studied molecules, only coronene (a PAH), 1,8-naphthalic anhydride, 6-H-benzo[cd]pyrene-6-one and 7H-benz[de]anthracence-7-one (three oxygenated-PAHs) provide relevant contributions to radiative forcing.

We have implemented a parameterization for forming ice in large-scale cirrus clouds that accounts for the changes in updrafts associated with a spectrum of waves acting within each time step in the model. This allows us to account for the frequency of homogeneous and heterogeneous freezing events that occur within each time step of the model and helps to determine more realistic ice number concentrations as well as changes to ice number concentrations. The model is able to fit observations of ice number at the lowest temperatures in the tropical tropopause but is still somewhat high in tropical latitudes with temperatures between 195°K and 215°K. The climate forcings associated with different representations of heterogeneous ice nuclei (IN or INPs) are primarily negative unless large additions of IN are made, such as when we assumed that all aircraft soot acts as an IN. However, they can be close to zero if it is assumed that all background dust can act as an INP irrespective of how much sulfate is deposited on these particles. Our best estimate for the forcing of anthropogenic aircraft soot in this model is -0.2 ± 0.06 W/m2, while that from anthropogenic fossil/biofuel soot is -0.093 ± 0.033 W/m2. Natural and anthropogenic open biomass burning leads to a net forcing of -0.057 ± 0.05 W/m2.