Low-temperature elastic anomalies in CaTiO3: dynamical characterization

Abstract

Pulse–echo ultrasonic measurements of elastic coefficients of CaTiO3 show anomalous behavior around 200 K, with a notable rise in the attenuation coefficient. Molecular dynamics simulation is used to simulate the elastic response of a mono-domain (MDm) and a poly-domain (PDm) configuration of CaTiO3 using the Vashishta–Raman interatomic potential. The PDm is obtained by cooling the melt from 3600 to 300 K at a rate of 0.5 K ps−1, so that it recrystallizes to the PDm orthorhombic configuration. The elastic behavior is simulated in the temperature range from 300 to 20 K. In the MDm, it is observed that the bulk modulus varies linearly with temperature, while in the PDm an anomalous hardening is seen around 210 K. The bulk modulus of the PDm fluctuates strongly and is lower than that of the MDm. Neither the pair correlation function nor the Ti–Ti–O bonding angle indicate a true structural phase transition in this range of temperatures. Given the absence of any apparent change in the structure, a possible explanation for this phenomenon is the emergence of a certain class of dynamical instability associated with domain wall motion. Curiously, the pressure fluctuations in both the MDm and PDm configurations follow a power law distribution f ∼ P−α, with the exponent independent of applied strain and temperature. Time series for pressure are used to analyze the dynamics by time-delay reconstruction techniques. The calculus of embedding and correlation dimension indicates that in the polycrystalline configuration, low-dimension dynamics (<26) appears, which tend to disappear at higher temperatures.