The Al-Fe(III)epidote miscibility gap in a metamorphic profile through the penninic series of the Tauern window,Austria

The compositional variations in epidotes, Ca₂Al₂(Fe³⁺, Al)-Si₃O₁₂(OH), from a prograde Mesozoic rock series in the Eastern Alps, Austria, are systematically related to metamorphic grade and the oxidation state of the rock. With increasing metamorphic grade the average composition of the zoned epidotes shifts to Fe³⁺-poorer compositions reflecting not only the effect of temperature and total pressure but also the concomitant decrease of the oxidation state of the rocks. Oxidized hematite-bearing assemblages are: 90 mole % Al₂FeEp (greenschists) 70 mole % Al₂FeEp (garnet amphibolites) 58 mole % Al₂FeEp (eclogites); reduced sulfidebearing assemblages are: 42 mole % Al₂FeEp (greenschists) 24 mole % Al₂FeEp (garnet amphibolites) 23 mole % Al₂FeEp (eclogites).A similar compositional evolution of the epidotes as in the spatial sequence of the samples can be observed within the single zoned crystals, reflecting the temporal changes of temperature, total pressure and oxygen fugacity during the prograde crystallization. The Fe³⁺-contents of core and rim decrease with increasing metamorphic grade and decreasing oxidation state. Generally the zoned epidotes consist of a Fe³⁺-rich core (90 to 63 mole % Al₂FeEp) and a Fe³⁺-poorer rim (55 to 23 mole % Al₂FeEp). Core and rim of the epidote crystals are separated by a compositional gap the extension of which is independent of the bulk rock composition, the oxidation state, and the mineralogical composition of the assemblages but becomes smaller with increasing metamorphic grade: 7253 mole % Al₂FeEp (low grade greenschists, 400° C) 6355 mole % Al₂FeEp (higher grade greenschists, 500° C), and 6055 mole % Al₂FeEp (garnet amphibolites, 500–550° C). At the temperature conditions of the highest grade garnet amphibolites and eclogites (550° C) the compositional gap closes at a composition of 58 mole % Al₂FeEp.The data presented thus confirm clearly the existence of an asymmetric miscibility gap in the monoclinic Al-Fe(III)-epidote solid solution series, which, for the first time, has been assumed by Strens (1964, 1965).A model is proposed that describes the prograde compositional evolution of the epidotes studied through the competing mechanisms of growth and diffusional Al-Fe³⁺ exchange and their dependence on metamorphic grade and oxidation state.