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Amphiboles are essential components of the continental crust and subduction zones showing anomalous anisotropic conductivity. Rock properties depend on the physical properties of their constituent minerals, which in turn depend on the crystal phonon and electron density of states. Here, to address the atomic-scale mechanism of the peculiar rock conductivity, we applied in situ temperature-dependent Raman spectroscopy, sensitive to both phonon and electron states, to Fe 2+ -rich amphiboles. The observed anisotropic resonance Raman scattering at elevated temperatures, in combination with density-functional-theory modelling, reveals a direction-dependent formation of mobile polarons associated with coupled FeO 6  phonons and electron transitions. Hence, temperature-activated electron-phonon excitations in hydrous iron-bearing chain and layered silicates are the atomistic source of anisotropic lithospheric conductivity. Furthermore, reversible delocalization of H +  occurs at similar temperatures even in a reducing atmosphere. The occurrence of either type of charge carriers does not require initial mixed-valence state of iron or high oxygen fugacity in the system.

Atomistic insight into lithospheric conductivity revealed by phonon–electron excitations in hydrous iron-bearing silicates