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The cause of changes in atmospheric carbon dioxide (CO 2 ) during the recent ice ages is yet to be fully explained. Most mechanisms for glacial-interglacial CO 2 change have centred on carbon exchange with the deep ocean, owing to its large size and relatively rapid exchange with the atmosphere 1 . The Southern Ocean is thought to have a key role in this exchange, as much of the deep ocean is ventilated to the atmosphere in this region 2 . However, it is difficult to reconstruct changes in deep Southern Ocean carbon storage, so few direct tests of this hypothesis have been carried out. Here we present deep-sea coral boron isotope data that track the pH-and thus the CO 2 chemistry-of the deep Southern Ocean over the past forty thousand years. At sites closest to the Antarctic continental margin, and most influenced by the deep southern waters that form the ocean's lower overturning cell, we find a close relationship between ocean pH and atmospheric CO 2 : during intervals of low CO 2 , ocean pH is low, reflecting enhanced ocean carbon storage; and during intervals of rising CO 2 , ocean pH rises, reflecting loss of carbon from the ocean to the atmosphere. Correspondingly, at shallower sites we find rapid (millennial- to centennial-scale) decreases in pH during abrupt increases in CO 2 , reflecting the rapid transfer of carbon from the deep ocean to the upper ocean and atmosphere. Our findings confirm the importance of the deep Southern Ocean in ice-age CO 2 change, and show that deep-ocean CO 2 release can occur as a dynamic feedback to rapid climate change on centennial timescales.

Earth's mightiest ocean current, the Antarctic Circumpolar Current (ACC), regulates the exchange of heat and carbon between the ocean and the atmosphere, and influences vertical ocean structure, deep-water production and the global distribution of nutrients and chemical tracers. The eastward-flowing ACC occupies a unique circumglobal pathway in the Southern Ocean that was enabled by the tectonic opening of key oceanic gateways during the break-up of Gondwana (for example, by the opening of the Tasmanian Gateway, which connects the Indian and Pacific oceans). Although the ACC is a key component of Earth's present and past climate system, the timing of the appearance of diagnostic features of the ACC (for example, low zonal gradients in water-mass tracer fields) is poorly known and represents a fundamental gap in our understanding of Earth history. Here we show, using geophysically determined positions of continent-ocean boundaries, that the deep Tasmanian Gateway opened 33.5 ± 1.5 million years ago (the errors indicate uncertainty in the boundary positions). Following this opening, sediments from Indian and Pacific cores recorded Pacific-type neodymium isotope ratios, revealing deep westward flow equivalent to the present-day Antarctic Slope Current. We observe onset of the ACC at around 30 million years ago, when Southern Ocean neodymium isotopes record a permanent shift to modern Indian-Atlantic ratios. Our reconstructions of ocean circulation show that massive reorganization and homogenization of Southern Ocean water masses coincided with migration of the northern margin of the Tasmanian Gateway into the mid-latitude westerly wind band, which we reconstruct at 64° S, near to the northern margin. Onset of the ACC about 30 million years ago coincided with major changes in global ocean circulation and probably contributed to the lower atmospheric carbon dioxide levels that appear after this time.

Global climate and the concentration of atmospheric carbon dioxide (CO2) are correlated over recent glacial cycles. The combination of processes responsible for a rise in atmospheric CO2 at the last glacial termination (23,000 to 9,000 years ago), however, remains uncertain. Establishing the timing and rate of CO2 changes in the past provides critical insight into the mechanisms that influence the carbon cycle and helps put present and future anthropogenic emissions in context. Here we present CO2 and methane (CH4) records of the last deglaciation from a new high-accumulation West Antarctic ice core with unprecedented temporal resolution and precise chronology. We show that although low-frequency CO2 variations parallel changes in Antarctic temperature, abrupt CO2 changes occur that have a clear relationship with abrupt climate changes in the Northern Hemisphere. A significant proportion of the direct radiative forcing associated with the rise in atmospheric CO2 occurred in three sudden steps, each of 10 to 15 parts per million. Every step took place in less than two centuries and was followed by no notable change in atmospheric CO2 for about 1,000 to 1,500 years. Slow, millennial-scale ventilation of Southern Ocean CO2-rich, deep-ocean water masses is thought to have been fundamental to the rise in atmospheric CO2 associated with the glacial termination, given the strong covariance of CO2 levels and Antarctic temperatures. Our data establish a contribution from an abrupt, centennial-scale mode of CO2 variability that is not directly related to Antarctic temperature. We suggest that processes operating on centennial timescales, probably involving the Atlantic meridional overturning circulation, seem to be influencing global carbon-cycle dynamics and are at present not widely considered in Earth system models.

Geological and geochemical evidence indicates that the Antarctic ice sheet formed during the Eocene-Oligocene transition, 33.5-34.0 million years ago. Modelling studies suggest that such ice-sheet formation might have been triggered when atmospheric carbon dioxide levels (pCO2atm) fell below a critical threshold of approximately 750 p.p.m.v., but the timing and magnitude of pCO2atm relative to the evolution of the ice sheet has remained unclear. Here we use the boron isotope pH proxy on exceptionally well-preserved carbonate microfossils from a recently discovered geological section in Tanzania to estimate pCO2atm before, during and after the climate transition. Our data suggest that are reduction in pCO2atm occurred before the main phase of ice growth,followed by a sharp recovery to pre-transition values and then a more gradual decline. During maximum ice-sheet growth, pCO2atm was between approximately 450 and approximately 1,500 p.p.m.v., with a central estimate of approximately 760 p.p.m.v. The ice cap survived the period of pCO2atm recovery,although possibly with some reduction in its volume, implying (as models predict) a nonlinear response to climate forcing during melting. Overall, our results confirm the central role of declining pCO2atm in the development of the Antarctic ice sheet (in broad agreement with carbon cycle modelling) and help to constrain mechanisms and feedbacks associated with the Earth's biggest climate switch of the past 65 Myr.