14C contamination testing in natural abundance laboratories: a new preparation method using wet chemical oxidation and some experiences

Substances enriched with radiocarbon can easily contaminate samples and laboratories used for natural abundance measurements. We have developed a new method using wet chemical oxidation for swabbing laboratories and equipment to test for 14C contamination. Here, we report the findings of 18 months’ work and more than 800 tests covering studies at multiple locations. Evidence of past and current use of enriched 14C was found at all but one location and a program of testing and communication was used to mitigate its effects. Remediation was attempted with mixed success and depended on the complexity and level of the contamination. We describe four cases from different situations

The potential of speleothems from Western Europe as recorders of regional climate: a critical assessment of the SISAL database

Western Europe is the region with the highest density of published speleothem δ18O (δ18Ospel) records worldwide. Here, we review these records in light of the recent publication of the Speleothem Isotopes Synthesis and AnaLysis (SISAL) database. We investigate how representative the spatial and temporal distribution of the available records is for climate in Western Europe and review potential sites and strategies for future studies. We show that spatial trends in precipitation δ18O are mirrored in the speleothems, providing means to better constrain the factors influencing δ18Ospel at a specific location. Coherent regional δ18Ospel trends are found over stadial-interstadial transitions of the last glacial, especially in high altitude Alpine records, where this has been attributed to a strong temperature control of δ18Ospel. During the Holocene, regional trends are less clearly expressed, due to lower signal-to-noise ratios in δ18Ospel, but can potentially be extracted with the use of statistical methods. This first assessment highlights the potential of the European region for speleothem palaeoclimate reconstruction, while underpinning the importance of knowing local factors for a correct interpretation of δ18Ospel

Distinguishing the vegetation and soil component of δ13C variation in speleothem records from degassing and prior calcite precipitation effects

The carbon isotopic signature inherited from soil/epikarst processes may be modified by degassing and prior calcite precipitation (PCP) before its imprint on speleothem calcite. Despite laboratory demonstration of PCP effects on carbon isotopes and increasingly sophisticated models of the governing processes, to date, there has been limited effort to deconvolve the dual PCP and soil/epikarst components in measured speleothem isotopic time series. In this contribution, we explore the feasibility, advantages, and disadvantages of using trace element ratios and &delta;44Ca to remove the overprinting effect of PCP on measured &delta;13C to infer the temporal variations in the initial &delta;13C of dripwater. In 8 examined stalagmites, the most widely utilized PCP indicators Mg/Ca and &delta;44Ca covary as expected. However, Sr/Ca does not show consistent relationships with &delta;44Ca so PCP is not universally the dominant control on Sr/Ca. From &delta;44Ca and Mg/Ca, our calculation of PCP as fCa, fraction of initial Ca remaining at the deposition of the stalagmite layer, yields multiple viable solutions depending on the assumed &delta;44Ca fractionation factor and inferred variation in DMg. Uncertainty in the effective fractionation of &delta;13C during degassing and precipitation contributes to uncertainty in the absolute value of estimated initial &delta;13C. Nonetheless, the trends in initial &delta;13C are less sensitive to these uncertainties. In coeval stalagmites from the same cave spanning 94 to 82 ka interval, trends in calculated initial &delta;13C are more similar than those in measured &delta;13C, and reveal a common positive anomaly initial &delta;13C during a stadial cooling event. During deglaciations, the trend of greater respiration rates and higher soil CO2 is captured in the calculated initial &delta;13C, despite the tendency of higher interglacial dripwater situation to favor more extensive PCP.</p

Permafrost-related hiatuses in stalagmites: Evaluating the potential for reconstruction of carbon cycle dynamics

Permafrost is widely present throughout the Northern Hemisphere high latitudes, and stores large amounts of carbon in the form of frozen soil organic matter. The response of permafrost regions to anthropogenic climate change remains uncertain, in part because of a lack of information on their response to past changes in global climate. Here we test the use of stalagmites from two caves in Siberia as a novel, precisely dated, and highly localised archive of past permafrost carbon cycle dynamics. Stalagmite growth at these sites is controlled by the presence/absence of permafrost above the cave over glacial-interglacial time scales. We target the transition layer between two subsequent growth phases (interglacials) and the interval directly following growth resumption after the last glacial in three stalagmites, as this is where a geochemical imprint of thaw-related processes in the frozen zone between surface and cave would be recorded. We apply a multi-proxy approach including carbon isotopes (δ13C and 14C) and trace element concentrations, combined with petrographic analyses and high-resolution U-Th chronology. Our dataset indicates complex growth patterns and possible intervals of microbial colonisation of the stalagmite surface in the transition layers. High-resolution U-Th ages confirm that the transition layer is not a single, long growth hiatus, but rather a period of extremely slow or episodic growth phases, possibly during “skipped” interglacials. However, we find no conclusive evidence for a geochemical signature related to permafrost degradation and related local carbon cycle dynamics, which might be related to insufficient sensitivity of the archive for high-frequency processes and/or insufficient measurement resolution

Climatic and in-cave influences on δ18O and δ13C in a stalagmite from northeastern India through the last deglaciation

Northeastern (NE) India experiences extraordinarily pronounced seasonal climate, governed by the Indian summer monsoon (ISM). The vulnerability of this region to floods and droughts calls for detailed and highly resolved paleoclimate reconstructions to assess the recurrence rate and driving factors of ISM changes. We use stable oxygen and carbon isotope ratios (δ18O and δ13C) from stalagmite MAW-6 from Mawmluh Cave to infer climate and environmental conditions in NE India over the last deglaciation (16–6ka). We interpret stalagmite δ18O as reflecting ISM strength, whereas δ13C appears to be driven by local hydroclimate conditions. Pronounced shifts in ISM strength over the deglaciation are apparent from the δ18O record, similarly to other records from monsoonal Asia. The ISM is weaker during the late glacial (LG) period and the Younger Dryas, and stronger during the Bølling-Allerød and Holocene. Local conditions inferred from the δ13C record appear to have changed less substantially over time, possibly related to the masking effect of changing precipitation seasonality. Time series analysis of the δ18O record reveals more chaotic conditions during the late glacial and higher predictability during the Holocene, likely related to the strengthening of the seasonal recurrence of the ISM with the onset of the Holocene

SISALv2: A comprehensive speleothem isotope database with multiple age-depth models

Characterizing the temporal uncertainty in palaeoclimate records is crucial for analysing past climate change, correlating climate events between records, assessing climate periodicities, identifying potential triggers and evaluating climate model simulations. The first global compilation of speleothem isotope records by the SISAL (Speleothem Isotope Synthesis and Analysis) working group showed that age model uncertainties are not systematically reported in the published literature, and these are only available for a limited number of records (ca. 15 %, n = 107=691). To improve the usefulness of the SISAL database, we have (i) improved the database's spatiooral coverage and (ii) created new chronologies using seven different approaches for age depth modelling. We have applied these alternative chronologies to the records from the first version of the SISAL database (SISALv1) and to new records compiled since the release of SISALv1. This paper documents the necessary changes in the structure of the SISAL database to accommodate the inclusion of the new age models and their uncertainties as well as the expansion of the database to include new records and the qualitycontrol measures applied. This paper also documents the age depth model approaches used to calculate the new chronologies. The updated version of the SISAL database (SISALv2) contains isotopic data from 691 speleothem records from 294 cave sites and new age depth models, including age depth temporal uncertainties for 512 speleothems. SISALv2 is available at https://doi.org/10.17864/1947.256 (Comas-Bru et al., 2020a). © 2020 Author(s)

Aerosol forcing of the position of the intertropical convergence zone since AD1550

The position of the intertropical convergence zone is an important control on the distribution of low-latitude precipitation. Its position is largely controlled by hemisphere temperature contrasts1, 2. The release of aerosols by human activities may have resulted in a southward shift of the intertropical convergence zone since the early 1900s (refs 1, 3, 4, 5, 6) by muting the warming of the Northern Hemisphere relative to the Southern Hemisphere over this interval1, 7, 8, but this proposed shift remains equivocal. Here we reconstruct monthly rainfall over Belize for the past 456 years from variations in the carbon isotope composition of a well-dated, monthly resolved speleothem. We identify an unprecedented drying trend since ad 1850 that indicates a southward displacement of the intertropical convergence zone. This drying coincides with increasing aerosol emissions in the Northern Hemisphere and also marks a breakdown in the relationship between Northern Hemisphere temperatures and the position of the intertropical convergence zone observed earlier in the record. We also identify nine short-lived drying events since ad 1550 each following a large volcanic eruption in the Northern Hemisphere. We conclude that anthropogenic aerosol emissions have led to a reduction of rainfall in the northern tropics during the twentieth century, and suggest that geographic changes in aerosol emissions should be considered when assessing potential future rainfall shifts in the tropics

The SISAL database: a global resource to document oxygen and carbon isotope records from speleothems

Stable isotope records from speleothems provide information on past climate changes, most particularly information that can be used to reconstruct past changes in precipitation and atmospheric circulation. These records are increasingly being used to provide “out-of-sample” evaluations of isotope-enabled climate models. SISAL (Speleothem Isotope Synthesis and Analysis) is an international working group of the Past Global Changes (PAGES) project. The working group aims to provide a comprehensive compilation of speleothem isotope records for climate reconstruction and model evaluation. The SISAL database contains data for individual speleothems, grouped by cave system. Stable isotopes of oxygen and carbon (δ 18O, δ 13C) measurements are referenced by distance from the top or bottom of the speleothem. Additional tables provide information on dating, including information on the dates used to construct the original age model and sufficient information to assess the quality of each data set and to erect a standardized chronology across different speleothems. The metadata table provides location information, information on the full range of measurements carried out on each speleothem and information on the cave system that is relevant to the interpretation of the records, as well as citations for both publications and archived data. The compiled data are available at https://doi.org/10.17864/1947.147

Evaluating model outputs using integrated global speleothem records of climate change since the last glacial

Although quantitative isotopic data from speleothems has been used to evaluate isotope-enabled model simulations, currently no consensus exists regarding the most appropriate methodology through which to achieve this. A number of modelling groups will be running isotope-enabled palaeoclimate simulations in the framework of the Coupled Model Intercomparison Project Phase 6, so it is timely to evaluate different approaches to use the speleothem data for data-model comparisons. Here, we illustrate this using 456 globally-distributed speleothem δ18O records from an updated version of the Speleothem Isotopes Synthesis and Analysis (SISAL) database and palaeoclimate simulations generated using the ECHAM5-wiso isotope-enabled atmospheric circulation model. We show that the SISAL records reproduce the first-order spatial patterns of isotopic variability in the modern day, strongly supporting the application of this dataset for evaluating model-derived isotope variability into the past. However, the discontinuous nature of many speleothem records complicates procuring large numbers of records if data-model comparisons are made using the traditional approach of comparing anomalies between a control period and a given palaeoclimate experiment. To circumvent this issue, we illustrate techniques through which the absolute isotopic values during any time period could be used for model evaluation. Specifically, we show that speleothem isotope records allow an assessment of a model’s ability to simulate spatial isotopic trends. Our analyses provide a protocol for using speleothem isotopic data for model evaluation, including screening the observations to take into account the impact of speleothem mineralogy on 18O values, the optimum period for the modern observational baseline, and the selection of an appropriate time-window for creating means of the isotope data for palaeo time slices