Structural refinements of lawsonite have been obtained at pressures up to 16.5 GPa using angle-dispersive powder diffraction with synchrotron radiation on a natural sample contained in a diamond anvil cell. Lawsonite compresses smoothly and relatively isotropically up to 10 GPa. Its bulk modulus is 126.1(6) GPa (for K′= 4), consistent with previous results. A trend of decreasing Si–O–Si angle indicates that compression is accommodated partly through the narrowing of the cavities containing Ca and H2O in the [001]ortho direction. At 10–11 GPa there is a phase transition from Cmcm to P21/m symmetry. The occurrence of a mixed-phase region, spanning >1 GPa, indicates that the transition is first order in character. The phase transition occurs through a shearing of (010)ortho sheets containing AlO6 octahedral chains in the [100]ortho direction, which causes an increase in βmono. Across the transition, the number of oxygens coordinated to Ca increases from 8 to 9, causing an increase in the average Ca–O bond length. The compressibility of P21/m lawsonite could not be determined due to solidification of the methanol/ethanol pressure-transmitting medium. On the basis of an experiment in which the P21/m lawsonite structure was heated to 200°C at 12.0 GPa, we predict a shallow positive P-T slope for the phase transition, and therefore no stability field for P21/m lawsonite in the Earth.

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