Spontaneous strain variations through the low temperature phase transitions of deuterated lawsonite

Michael A. Carpenter 1 , Hinrich-Wilhelm Meyer 1 , Peter Sondergeld 2 , Stefan Marion 3  and Kevin S. Knight 4
  • 1 Department of Earth Sciences, University of Cambridge, Downing Street, Cambridge CB2 3EQ, U.K.
  • 2 Institut für Experimentalphysik, Universität Wien, Strudlhofgasse 4, A-1090 Vienna, Austria
  • 3 University of Oslo, Centre for Materials Science, N-0349 Oslo, Norway
  • 4 ISIS Facility, Rutherford Appleton Laboratory, Chilton, Didcot, Oxfordshire, OX11 OQX, U.K.

Abstract

High resolution neutron powder diffraction has been used to determine lattice parameter variations of deuterated lawsonite across the Cmcm ↔ Pmcn and Pmcn ↔ P21cn phase transitions, in the temperature interval 1.6-505 K. The variations are reversible through heating and cooling cycles. Strain analysis, based on a displacive model of the transitions with saturation temperatures to describe the temperature-independent behavior as T → 0 K, shows that the data are consistent with a tricritical transition at 271 ± 2 K and a second-order transition at 155 ± 1 K. Comparisons with strains from published dilatation data for a natural (hydrogenated) sample highlight aspects of the transitions that are most dependent on the behavior of protons in the structure. Replacing H by D causes the low temperature transition point to be increased by ~27 K and an anomaly in the strain evolution of the Pmcn transition to increase from ~225 to ~250 K. The transition point of the hightemperature transition remains the same within ± ~2 K. We conclude that proton ordering and displacive contributions are both important in the 271 K transition, though with the displacive component providing the initial symmetry-breaking mechanism. Structural changes that are more dependent on the behavior of H or D become important ~20-50 K below this. Strains for the Pmcn ↔ P21cn transition are consistent with a transition driven by a single order parameter. The data are used to determine values for strain/order parameter coupling coefficients for calculation of elastic anomalies due to the phase transitions.

Purchase article
Get instant unlimited access to the article.
$42.00
Log in
Already have access? Please log in.


or
Log in with your institution

Journal + Issues

Search