Much of the long-term carbon cycle in solid earth occurs in subduction zones, where processes of devolatilization, partial melting of carbonated rocks, and dissolution of carbonate minerals lead to the return of CO2 to the atmosphere via volcanic degassing. Release of COH fluids from hydrous and carbonate minerals influences C recycling and magmatism at subduction zones. Contradictory interpretations exist regarding the retention/storage of C in subducting plates and in the forearc to subarc mantle. Several lines of evidence indicate mobility of C, of uncertain magnitude, in forearcs. A poorly constrained fraction of the 40-115 Mt/yr of C initially subducted is released into fluids (by decarbonation and/or carbonate dissolution) and 18-43 Mt/yr is returned at arc volcanoes. Current estimates suggest the amount of C released into subduction fluids is greater than that degassed at arc volcanoes: the imbalance could reflect C subduction into the deeper mantle, beyond subarc regions, or storage of C in forearc/subarc reservoirs.We examine the fate of C in plate-interface ultramafic rocks, and by analogy serpentinized mantle wedge, via study of fluid-rock evolution of marble and variably carbonated serpentinite in the Ligurian Alps. Based on petrography, major and trace element concentrations, and carbonate C and O isotope compositions, we demonstrate that serpentinite dehydration at 2-2.5 GPa, 550 °C released aqueous fluids triggering breakdown of dolomite in nearby marbles, thus releasing C into fluids. Carbonate + olivine veins document flow of COH fluids and that the interaction of these COH fluids with serpentinite led to the formation of high-P carbonated ultramafic-rock domains (high-P ophicarbonates). We estimate that this could result in the retention of ~0.5-2.0 Mt C/yr in such rocks along subduction interfaces. As another means of C storage, 1 to 3 km-thick layers of serpentinized forearc mantle wedge containing 50 modal % dolomite could sequester 1.62 to 4.85 Mt C/yr.We stress that lithologically complex interfaces could contain sites of both C release and C addition, further confounding estimates of net C loss at forearc and subarc depths. Sites of C retention, also including carbonate veins and graphite as reduced carbonate, could influence the transfer of slab C to at least the depths beneath volcanic fronts
Metamorphic rocks are the records of plate tectonic processes whose reconstruction relies on correct estimates of the pressures and temperatures (P-T) experienced by these rocks through time. Unlike chemical geothermobarometry, elastic geobarometry does not rely on chemical equilibrium between minerals, so it has the potential to provide information on overstepping of reaction boundaries and to identify other examples of non-equilibrium behavior in rocks. Here we introduce a method that exploits the anisotropy in elastic properties of minerals to determine the unique P and T of entrapment from a single inclusion in a mineral host. We apply it to preserved quartz inclusions in garnet from eclogite xenoliths hosted in Yakutian kimberlites (Russia). Our results demonstrate that quartz trapped in garnet can be preserved when the rock reaches the stability field of coesite (the high-pressure and high-temperature polymorph of quartz) at 3 GPa and 850 °C. This supports a metamorphic origin for these xenoliths and sheds light on the mechanisms of craton accretion from a subducted crustal protolith. Furthermore, we show that interpreting P and T conditions reached by a rock from the simple phase identification of key inclusion minerals can be misleading.
Raman spectroscopy provides information on the residual strain state of host-inclusion systems that, coupled with the elastic geobarometry theory, can be used to retrieve the P-T conditions of inclusion entrapment. In situ Raman measurements of zircon and coesite inclusions in garnet from the ultrahigh-pressure Dora Maira Massif show that rounded inclusions exhibit constant Raman shifts throughout their entire volume. In contrast, we demonstrate that Raman shifts can vary from the center to the edges and corners of faceted inclusions. Step-by-step polishing of the garnet host shows that the strain in both rounded and prismatic inclusions is gradually released as the inclusion approaches the free surface of the host. More importantly, our experimental results coupled with selected numerical simulations demonstrate that the magnitude and the rate of the strain release also depend on the contrast in elastic properties between the host and the inclusion and on the inclusion crystallographic orientation with respect to the external surface. These results allowed us to give new methodological guidelines for determining the residual strain in host inclusion systems.
Elastic geobarometry for host-inclusion systems can provide new constraints to assess the pressure and temperature conditions attained during metamorphism. Current experimental approaches and theory are developed only for crystals immersed in a hydrostatic stress field, whereas inclusions experience deviatoric stress. We have developed a method to determine the strains in quartz inclusions from Raman spectroscopy using the concept of the phonon-mode Grüneisen tensor. We used ab initio Hartree-Fock/Density Functional Theory to calculate the wavenumbers of the Raman-active modes as a function of different strain conditions. Least-squares fits of the phonon-wavenumber shifts against strains have been used to obtain the components of the mode Grüneisen tensor of quartz (g 1 m and g 3 m) that can be used to calculate the strains in inclusions directly from the measured Raman shifts. The concept is demonstrated with the example of a natural quartz inclusion in eclogitic garnet from Mir kimberlite and has been validated against direct X-ray diffraction measurement of the strains in the same inclusion.
We have carried out ab initio hybrid Hartree-Fock/Density Functional Theory simulations to determine the structure and vibrational modes of zircon, ZrSiO 4 , as a function of different applied strains. The changes in phonon-mode wavenumbers are approximately linear in the unit-cell strains, and have been fitted to determine the components of the phonon-mode Grüneisen tensors of zircon which reproduce the change in measured Raman shifts with pressure. They can therefore be used to convert Raman shifts measured from zircon inclusions in metamorphic rocks into strains that in turn can be used to determine the metamorphic conditions at the time that the inclusion was trapped. Due to the strong anisotropy in the thermal pressure of zircon, the phonon-mode Grüneisen tensor is not able to reproduce the temperature-induced changes in Raman shifts. Because zircon inclusions are normally measured at room conditions this does not prevent the calculation of their entrapment conditions.
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