A High-Resolution Multitechniques Approach to Characterize Bio-Organo-Mineral Associations Within Rock Samples: Tracking Biological vs Abiotic Processes? Towards a Better Understanding of the Deep Carbon Cycle.

Abstract:

Among all elements, carbon plays one of the major roles for the sustainability of life on Earth. Past considerations of the carbon cycle have mainly focused on surface processes occurring at the atmosphere, oceans and shallow crustal environments. By contrast, little is known about the Deep Carbon cycle whereas both geochemical and biological processes may induce organic carbon production and/or consumption at depth. Indeed, the nowadays-recognized capability of geochemical processes such as serpentinization to generate abiotic organic compounds as well as the existence of a potentially important intraterrestrial life raises questions about the limit of biotic/abiotic carbon on Earth's deep interior and how it impacts global biogeochemical cycles. It is then mandatory to increase our knowledge on the nature and extent of carbon reservoirs along with their sources, sinks and fluxes in the subsurface.

This implies to be able to finely characterize organomineral associations within crustal rocks although it might be hampered by the scarceness and heterogeneous micrometric spatial distribution of organic molecules in natural rocks. We then developed an in situ analytical strategy based on the combination of high-resolution techniques to track organic molecules at the pore level in natural rocks and to determine their biological or abiotic origin. We associated classical high-resolution techniques and synchrotron-based imaging techniques in order to characterize their nature and localization (SEM/TEM, coupled CLSM/Raman spectroscopy, Tof-SIMS) along with their 3D-distribution relatively to mineral phases (S-FTIR, S-DeepUV, XANES, Biphoton microscopy).

The effectiveness of this approach to shed light on the speciation and nature of carbon in subsurface environments will be illustrated through the study of (i) subsurface ecosystems and abiotic organic carbon within ultramafic rocks of the oceanic lithosphere as putative analogs for the nature and functioning of primitive ecosystems on Earth and of (ii) ecosystems inhabiting Archean craton and potentially playing a role in punk-rock karstification processes and rocks weathering.