LAUSR

Abstract Subsurface fluid systems are important for chemical weathering, ore formation and thermal evolution of the crust. Changes in the dynamics and distribution of subsurface fluid flow systems are controlled by changes in global and regional terrestrial climate, tectonics, and elevation. This paper concerns the dating of changes in ancient subsurface hydrologic systems. However, direct dating of water-rock interaction is challenging because of the lack of appropriate materials to date and the more open and complex nature of subsurface flow regimes. Here, we explore the prospects of using U-Pb dating of petrified (silicified) wood as a means of quantifying continental paleo-hydrology. Oxidizing fluids, often of meteoric origin, tend to leach and mobilize U from the country rock, but when such waters contact organic-rich material, U can become reduced and immobilized, resulting in U-rich silicified wood. We present in situ laser ablation ICPMS analyses of U-Pb isotopes and trace elements in petrified wood from the Upper Triassic Chinle Formation (225–208 Myr) in the Petrified Forest National Park in Arizona (USA), allowing us to establish a generalized workflow for making meaningful paleo-hydrologic interpretations of the U-Pb systematics of silicified wood. Wood characterized by brownish colors and preservation of cellular structure have low Fe contents and positive Ce anomalies, indicating silicification in reducing environments and isolation in relatively reduced conditions after silicification, resulting in closed system behavior of U and Pb. Wood characterized by vivid colors (orange, red, etc.) and little to no preservation of cellular structure are much higher in Fe and exhibit negative Ce anomalies, indicating influence by more oxidized fluids. The brownish samples yield U-Pb ages clustered between 250 and 200 Ma with a peak coinciding with the time of deposition (~220 Ma), which indicates that fossilization largely took place almost immediately after deposition and that U-Pb in quartz faithfully retains the time of such fossilization. In contrast, the orangish-reddish-whitish samples yield younger U-Pb ages, defining distinct errorchron ages, which reflect subsequent generations of quartz crystallization. Scatter associated with errorchrons are likely due to local (mm- to cm-scale) U or Pb mobility or variable initial Pb composition. Distinct younger age peaks appear to correlate with the timing of regional unconformities associated with tectonic or epeirogenic uplift. We suggest that uplift and exhumation may initiate the onset of oxidizing fluid systems, resulting in leaching and transport of U from the surroundings, followed by subsequent generations of quartz precipitation. In summary, U-Pb dating of petrified wood or silicified organic material, has high potential for dating paleo-hydrologic events. However, due to complexities in terrestrial hydrologic systems, interpretations of U-Pb systematics must be informed by accompanying geochemical and textural observations.