Supplementary material: XRF core scanning data, CaCO3 values, foraminiferal carbon and oxygen isotope data, Mg/Ca data, clay mineralogy and helium isotope results

The Paleocene-Eocene Thermal Maximum (PETM; ~56 Ma) is associated with abrupt climate change, carbon cycle perturbation, ocean acidification, as well as biogeographic shifts in marine and terrestrial biota that were largely reversed as the climatic transient waned. We report a clear exception to the behavior of the PETM as a reversing climatic transient in the eastern North Atlantic (Deep-Sea Drilling Project Site 401, Bay of Biscay) where the PETM initiates a greatly prolonged environmental change compared to other places on Earth where records exist. The observed environmental perturbation extended well past the d13C recovery phase and up to 650 kyr after the PETM onset according to our extraterrestrial 3He-based age-model. We observe a strong decoupling of planktic foraminiferal d18O and Mg/Ca values during the PETM d13C recovery phase, which in combination with results from helium isotopes and clay mineralogy, suggests that the PETM triggered a hydrologic change in western Europe that increased freshwater flux and the delivery of weathering products to the eastern North Atlantic. This state change persisted long after the carbon-cycle perturbation had stopped. We hypothesize that either long-lived continental drainage patterns were altered by enhanced hydrological cycling induced by the PETM, or alternatively that the climate system in the hinterland area of Site 401 was forced into a new climate state that was not easily reversed in the aftermath of the PETM.

Isotope record and major element chemistry of intestitial waters of ODP Leg 104 sites

The variations in major elements and isotope composition (87Sr/86Sr, delta18O, deltaD) of interstitial waters in Leg 104 sediments is most probably caused by the alteration of volcanic matter. A reaction scheme where volcanic glass reacts with pore-water magnesium and potassium to form trioctahedral smectite, phillipsite, and chert is proposed. Model calculations demonstrate that the pore waters may evolve their negative 6180 signatures without recourse to unreasonably large amounts of volcanic detritus or external sources.

Stable carbon isotope record of benthic foraminifera across the Paleocene-Eocene thermal maximum in the New Jersey Coastal Plain

In the New Jersey Coastal Plain, a silty to clayey sedimentary unit (the Marlboro Formation) represents deposition during the Paleocene-Eocene thermal maximum (PETM). This interval is remarkably different from the glauconitic sands and silts of the underlying Paleocene Vincentown and overlying Eocene Manasquan Formation. We integrate new and published stable isotope, biostratigraphic, lithostratigraphic and ecostratigraphic records, constructing a detailed time frame for the PETM along a depth gradient at core sites Clayton, Wilson Lake, Ancora and Bass River (updip to downdip). The onset of the PETM, marked by the base of the carbon isotope excursion (CIE), is within the gradual transition from glauconitic silty sands to silty clay, and represented fully at the updip sites (Wilson Lake and Clayton). The CIE "core" interval is expanded at the updip sites, but truncated. The CIE "core" is complete at the Bass River and Ancora sites, where the early part of the recovery is present (most complete at Ancora). The extent to which the PETM is expressed in the sediments is highly variable between sites, with a significant unconformity at the base of the overlying lower Eocene sediments. Our regional correlation framework provides an improved age model, allowing better understanding of the progression of environmental changes during the PETM. High-resolution benthic foraminiferal data document the change from a sediment-starved shelf setting to a tropical, river-dominated mud-belt system during the PETM, probably due to intensification of the hydrologic cycle. The excellent preservation of foraminifera during the PETM and the lack of severe benthic extinction suggest there was no extreme ocean acidification in shelf settings.

Stable isotope record of benthic foraminifera in late Pleistocene sediments

Variations in the contribution of North Atlantic Deep Water (NADW), relative to North Pacific Deep Water (NPDW), to the Southern Ocean, are assessed by comparing delta13C records from the mid-depth North Atlantic, deep Southern Ocean, and deep equatorial Pacific Ocean. In general, the relative contribution of NADW was greater during interglaciations than glaciations of the past 550,000 years. An increase in the NADW flux to the Southern Ocean since the last glaciation was proposed to have resulted in higher atmospheric CO2 in the Holocene (Broecker and Peng, 1989, doi:10.1029/GB003i003p00215). Glacial-interglacial variations in the proportion of NADW in the Southern Ocean may have also influenced atmospheric CO2 levels over the past 550,000 years. The greatest relative flux of NADW to the Southern Ocean occurred during interglacial stage 11. Faunal data suggest that the North Atlantic polar front and southern Indian Ocean subtropical convergence zone were located farthest poleward during stage 11. Warmth in these locations and a strong southward flux of NADW during stage 11 may be causally linked by the NADW formation process/warm water return route (Gordon, 1986, doi:10.1029/JC091iC04p05037). Time series analysis indicates that delta13C variations in the deep Southern Ocean occur at the same frequencies as the Earth's orbital variations and are coherent and in phase with delta18O. At most, 50% of the glacial-interglacial delta13C amplitude in the Southern Ocean is due changes in the contribution of NADW. The remainder is probably due to mean ocean delta13C changes.

Miocene strontium isotope record of DSDP Hole 30-289

A composite strontium isotopic seawater curve was constructed for the Miocene between 24 and 6 Ma by combining 87Sr/86Sr measurements of planktonic foraminifera from Deep Sea Drilling Project sites 289 and 588. Site 289, with its virtually continuous sedimentary record and high sedimentation rates (26 m/m.y.), was used for constructing the Oligocene to mid-Miocene part of the record, which included the calibration of 63 biostratigraphic datums to the Sr seawater curve using the timescale of Cande and Kent (1992 doi:10.1029/92JB01202). Across the Oligocene/Miocene boundary, a brief plateau occurred in the Sr seawater curve (87Sr/86Sr values averaged 0.70824) which is coincident with a carbon isotopic maximum (CM-O/M) from 24.3 to 22.6 Ma. During the early Miocene, the strontium isotopic curve was marked by a steep rise in 87Sr/86Sr that included a break in slope near 19 Ma. The rate of growth was about 60 ppm/m.y. between 22.5 and 19.0 Ma and increased to over 80 ppm/m.y. between 19.0 and 16 Ma. Beginning at ~16 Ma (between carbon isotopic maxima CM3 and CM4 of Woodruff and Savin (1991 doi:10.1029/91PA02561)), the rate of 87Sr/86Sr growth slowed and 87Sr/86Sr values were near constant from 15 to 13 Ma. After 13 Ma, growth in 87Sr/86Sr resumed and continued until ~9 Ma, when the rate of 87Sr/86Sr growth decreased to zero once again. The entire Miocene seawater curve can be described by a high-order function, and the first derivative (d87Sr/86Sr/dt) of this function reveals two periods of increased slope. The greatest rate of 87Sr/86Sr change occurred during the early Miocene between ~20 and 16 Ma, and a smaller, but distinct, period of increased slope also occurred during the late Miocene between ~12 and 9 Ma. These periods of steepened slope coincide with major phases of uplift and denudation of the Himalayan-Tibetan Plateau region, supporting previous interpretations that the primary control on seawater 87Sr/86Sr during the Miocene was related to the collision of India and Asia. The rapid increase in 87Sr/86Sr values during the early Miocene from 20 to 16 Ma imply high rates of chemical weathering and dissolved riverine fluxes to the oceans. In the absence of another source of CO2, these high rates of chemical weathering should have quickly resulted in a drawdown of atmospheric CO2 and climatic cooling through a reversed greenhouse effect. The paleoclimatic record, however, indicates a warming trend during the early Miocene, culminating in a climatic optimum between 17 and 14.5 Ma. We suggest that the high rates of chemical erosion and warm temperatures during the climatic optimum were caused by an increase in the contribution of volcanic CO2 from the eruption of the Columbia River Flood Basalts (CRFB) between 17 and 15 Ma. The decrease in the rate of CRFB eruptions at 15 Ma and the removal of atmospheric carbon dioxide by increased organic carbon burial in Monterey deposits eventually led to cooling and increased glaciation between ~14.5 and 13 Ma. The CRFB hypothesis helps to explain the significant time lag between the onset of increased rates of organic carbon burial in the Monterey at 17.5 Ma (as marked by increased delta13C values) and the climatic cooling and glaciation during the middle Miocene (as marked by the increase in delta18O values), which did not begin until ~14.5 Ma.

Strontium and oxygen isotope data for DSDP Hole 44-390A and ODP Leg 171 holes

Differences in regional responses to climate fluctuations are well documented on short time scales (e.g., El Niño-Southern Oscillation), but with the exception of latitudinal temperature gradients, regional patterns are seldom considered in discussions of ancient greenhouse climates. Contrary to the expectation of global warming or global cooling implicit in most treatments of climate evolution over millions of years, this paper shows that the North Atlantic warmed by as much as 6°C (1.5% decrease in d18O values of planktic foraminifera) during the Maastrichtian global cooling interval. We suggest that warming was the result of the importation of heat from the South Atlantic. Decreasing North Atlantic d18O values are also associated with increasing gradients in planktic d13C values, suggesting increasing surface-water stratification and a correlated strengthening of the North Atlantic Polar Front. If correct, this conclusion predicts arctic cooling during the late Maastrichtian. Beyond implications for the Maastrichtian, these data demonstrate that climate does not behave as if there is a simple global thermostat, even on geologic time scales.

Neodymium isotope record of ODP Site 177-1090

Age estimates for the opening of Drake Passage range from 49 to 17 million years ago (Ma), complicating interpretations of the relationship between ocean circulation and global cooling. Secular variations of neodymium isotope ratios at Agulhas Ridge (Southern Ocean, Atlantic sector) suggest an influx of shallow Pacific seawater approximately 41 Ma. The timing of this connection and the subsequent deepening of the passage coincide with increased biological productivity and abrupt climate reversals. Circulation/productivity linkages are proposed as a mechanism for declining atmospheric carbon dioxide. These results also indicate that Drake Passage opened before the Tasmanian Gateway, implying the late Eocene establishment of a complete circum-Antarctic pathway.