Toughening Ceramics down to Cryogenic Temperatures by Reentrant Strain-Glass Transition

Ceramics, often exhibiting important functional properties like piezoelectricity, superconductivity, and magnetism, are usually mechanically brittle at room temperature and even more brittle at low temperature due to their ionic or covalent bonding nature. The brittleness in their working temperature range (mostly from room down to cryogenic temperatures) has been a limiting factor for the usefulness of these ceramics. In this Letter, we report a surprising ``low-temperature toughening'' phenomenon in a La-doped ${\mathrm{CaTiO}}_{3}$ perovskite ceramic, where a $2.5\ifmmode\times\else\texttimes\fi{}$ increase of fracture toughness ${K}_{\mathrm{IC}}$ from 1.9 to $4.8\text{ }\text{ }\mathrm{MPa}\text{ }{\mathrm{m}}^{1/2}$ occurs when cooling from above room temperature (323 K) down to a cryogenic temperature of 123 K, the lowest temperature our experiment can reach. In situ microscopic observations in combination with macroscopic characterizations show that this desired but counterintuitive phenomenon stems from a reentrant strain-glass transition, during which nanosized orthorhombic ferroelastic domains gradually emerge from the existing tetragonal ferroelastic matrix. The temperature stability of this unique microstructure and its stress-induced transition into the macroscopic orthorhombic phase provide a low-temperature toughening mechanism over a wide temperature range and explain the observed phenomenon. Our finding may open a way to design tough ceramics with a wide temperature range and shed light on the nature of reentrant transitions in other ferroic systems.