Neogene cooling driven by land surface reactivity rather than increased weathering fluxes.

The long-term cooling, decline in the partial pressure of carbon dioxide, and the establishment of permanent polar ice sheets during the Neogene period1,2 have frequently been attributed to increased uplift and erosion of mountains and consequent increases in silicate weathering, which removes atmospheric carbon dioxide3,4. However, geological records of erosion rates are potentially subject to averaging biases5,6, and the magnitude of the increase in weathering fluxes-and even its existence-remain debated7-9. Moreover, an increase in weathering scaled to the proposed erosional increase would have removed nearly all carbon from the atmosphere10, which has led to suggestions of compensatory carbon fluxes11-13 in order to preserve mass balance in the carbon cycle. Alternatively, an increase in land surface reactivity-resulting from greater fresh-mineral surface area or an increase in the supply of reactive minerals-rather than an increase in the weathering flux, has been proposed to reconcile these disparate views8,9. Here we use a parsimonious carbon cycle model that tracks two weathering-sensitive isotopic tracers (stable 7Li/6Li and cosmogenic 10Be/9Be) to show that an increase in land surface reactivity is necessary to simultaneously decrease atmospheric carbon dioxide, increase seawater 7Li/6Li and retain constant seawater 10Be/9Be over the past 16 million years. We find that the global silicate weathering flux remained constant, even as the global silicate weathering intensity-the fraction of the total denudation flux that is derived from silicate weathering-decreased, sustained by an increase in erosion. Long-term cooling during the Neogene thus reflects a change in the partitioning of denudation into weathering and erosion. Variable partitioning of denudation and consequent changes in silicate weathering intensity reconcile marine isotope and erosion records with the need to maintain mass balance in the carbon cycle and without requiring increases in the silicate weathering flux.