Improved Polycyclic Aromatic Hydrocarbon and n-Alkane Determination in Speleothems through Cleanroom Sample Processing.

Interest in paleoenvironmental reconstructions from biomarkers in speleothems is increasing, thanks in part to the capacity of speleothems to grow continuously and to resist postdepositional alteration. In particular, the possibility exists to link high-resolution and accurately dated fire and vegetation records with isotopic data of climatic and paleoenvironmental interactions at the local and regional scale. However, the scarcity of existing methods for the quantification of organic molecules in stalagmites, together with the issues of sample availability, contamination, and low concentrations, complicate this approach. In this work, we developed a novel method for the simultaneous determination of 18 polycyclic aromatic hydrocarbons (PAHs) and 26 n-alkanes (C10-C35) and then tested it on "clean" calcite and aragonite stalagmite samples from cave KNI-51 in the Australian tropics. The method involves subsampling by using a hand-held drill, complete dissolution of the matrix in hydrochloric acid, then liquid-liquid extraction, and GC-MS analysis. Sample preparation was carried out in a 10 000 class clean room built entirely in stainless steel to avoid contamination. Detection limits were 0.3-9 ng for PAHs and 6-44 ng for n-alkanes. Measurable concentrations of fire-derived PAH compounds, namely, phenanthrene, pyrene, benzo( e)pyrene, and indeno(123- cd)pyrene, were detected in only one sample, which dates to the year ∼2004 CE, when a fire burned vegetation over the cave; n-alkanes were detected in all samples in the range C23-C35, with no odd-even preference.

Extreme rainfall activity in the Australian tropics reflects changes in the El Niño/Southern Oscillation over the last two millennia.

Assessing temporal variability in extreme rainfall events before the historical era is complicated by the sparsity of long-term "direct" storm proxies. Here we present a 2,200-y-long, accurate, and precisely dated record of cave flooding events from the northwest Australian tropics that we interpret, based on an integrated analysis of meteorological data and sediment layers within stalagmites, as representing a proxy for extreme rainfall events derived primarily from tropical cyclones (TCs) and secondarily from the regional summer monsoon. This time series reveals substantial multicentennial variability in extreme rainfall, with elevated occurrence rates characterizing the twentieth century, 850-1450 CE (Common Era), and 50-400 CE; reduced activity marks 1450-1650 CE and 500-850 CE. These trends are similar to reconstructed numbers of TCs in the North Atlantic and Caribbean basins, and they form temporal and spatial patterns best explained by secular changes in the dominant mode of the El Niño/Southern Oscillation (ENSO), the primary driver of modern TC variability. We thus attribute long-term shifts in cyclogenesis in both the central Australian and North Atlantic sectors over the past two millennia to entrenched El Niño or La Niña states of the tropical Pacific. The influence of ENSO on monsoon precipitation in this region of northwest Australia is muted, but ENSO-driven changes to the monsoon may have complemented changes to TC activity.

Sensitivity of northwest Australian tropical cyclone activity to ITCZ migration since 500 CE.

Tropical cyclones (TCs) regularly form in association with the intertropical convergence zone (ITCZ), and thus, its positioning has implications for global TC activity. While the poleward extent of the ITCZ has varied markedly over past centuries, the sensitivity with which TCs responded remains poorly understood from the proxy record, particularly in the Southern Hemisphere. Here, we present a high-resolution, composite stalagmite record of ITCZ migrations over tropical Australia for the past 1500 years. When integrated with a TC reconstruction from the Australian subtropics, this time series, along with downscaled climate model simulations, provides an unprecedented examination of the dependence of subtropical TC activity on meridional shifts in the ITCZ. TCs tracked the ITCZ at multidecadal to centennial scales, with a more southward position enhancing TC-derived rainfall in the subtropics. TCs may play an increasingly important role in Western Australia's moisture budgets as subtropical aridity increases due to anthropogenic warming.

Expansion and Contraction of the Indo-Pacific Tropical Rain Belt over the Last Three Millennia.

The seasonal north-south migration of the intertropical convergence zone (ITCZ) defines the tropical rain belt (TRB), a region of enormous terrestrial and marine biodiversity and home to 40% of people on Earth. The TRB is dynamic and has been shown to shift south as a coherent system during periods of Northern Hemisphere cooling. However, recent studies of Indo-Pacific hydroclimate suggest that during the Little Ice Age (LIA; AD 1400-1850), the TRB in this region contracted rather than being displaced uniformly southward. This behaviour is not well understood, particularly during climatic fluctuations less pronounced than those of the LIA, the largest centennial-scale cool period of the last millennium. Here we show that the Indo-Pacific TRB expanded and contracted numerous times over multi-decadal to centennial scales during the last 3,000 yr. By integrating precisely-dated stalagmite records of tropical hydroclimate from southern China with a newly enhanced stalagmite time series from northern Australia, our study reveals a previously unidentified coherence between the austral and boreal summer monsoon. State-of-the-art climate model simulations of the last millennium suggest these are linked to changes in the structure of the regional manifestation of the atmosphere's meridional circulation.

Orbital control of western North America atmospheric circulation and climate over two glacial cycles.

The now arid Great Basin of western North America hosted expansive late Quaternary pluvial lakes, yet the climate forcings that sustained large ice age hydrologic variations remain controversial. Here we present a 175,000 year oxygen isotope record from precisely-dated speleothems that documents a previously unrecognized and highly sensitive link between Great Basin climate and orbital forcing. Our data match the phasing and amplitudes of 65°N summer insolation, including the classic saw-tooth pattern of global ice volume and on-time terminations. Together with the observation of cold conditions during the marine isotope substage 5d glacial inception, our data document a strong precessional-scale Milankovitch forcing of southwestern paleoclimate. Because the expansion of pluvial lakes was associated with cold glacial conditions, the reappearance of large lakes in the Great Basin is unlikely until ca. 55,000 years into the future as climate remains in a mild non-glacial state over the next half eccentricity cycle.