First principles investigation of the effect of compositional variations on the terminal breakdown of antigorite in subduction zones

Serpentines are among the most abundant hydrous minerals in oceanic lithospheres formed by hydrothermal alteration of ultramafic mantle rocks (i.e. peridotites). Antigorite – the high temperature and pressure variety of serpentine – is considered to be the dominant water carrier within down-going oceanic slabs. The successive dehydration of antigorite during subduction of partially serpentinized oceanic lithospheres is strongly associated with the water cycle in the upper mantle and is expected to play an important role in the generation of arc magmatism (Ulmer & Trommsdorff, 1995; Schmidt & Poli, 1998), and influence rheological properties of oceanic slabs by processes such as dehydration embrittlement which is thought to trigger intermediate-to-deep focus earthquakes (Jung et al., 2004; Ferrand et al., 2017).

Antigorite is a hydrous phyllosilicate known for its polysomatism: The number of SiO₄ tetrahedra m along its a-cell periodicity. Previous electron microscopy studies reported the existence of antigorite within a wide range of m values (~13-23) depending on the pressure (P) and temperature (T) conditions (Mellini et al., 1987; Wunder et al., 2001). However, there is a lack of the combined structural and thermodynamic evidence about the stability of the different antigorite polysomes along the P,T-paths of subducting oceanic lithospheres.

We use a theoretical mineral physics approach based on first principles density functional theory calculations to quantify the phase diagrams of the terminal dehydration reactions of antigorite with different m-values between 13-19 under subarc depth P,T conditions. Our results elucidate the significance of the compositional variations of antigorite on the dehydration of serpentinized oceanic slabs during the progressive stages of subduction.