Quantum Critical Points in Ferroelectric Relaxors: Stuffed Tungsten Bronze K3Li2Ta5O15 and Lead Pyrochlore (Pb2Nb2O7)

Abstract

We have synthesised ceramic specimens of the tetragonal tungsten bronze K3Li2Ta5O15 (KLT) and characterized its phase transition via X-ray, dielectric permittivity, ultrasonic spectroscopy and heat capacity measurements. The space group of KLT is reported as both P4/mbm or Cmmm with the orthorhombic distortion occurring when there are higher partial pressures of volatile K and Li used within the closed crucibles for the solid state synthesis. The data show strong relaxor behaviour, with the temperature at which the two dielectric relative permittivity peaks decreasing with 104 K $\geqslant$ Tm1 $\geqslant$ 69 K and 69 K $\geqslant$ Tm2 $\geqslant$ 46 K as probe frequency f is reduced from 1 MHz to 316 Hz. The data satisfy a Vogel-Fulcher model with an extrapolated freezing temperature for {\epsilon}' and {\epsilon}" of Tf1 = + 15.8 and - 11.8 K and Tf2 = - 5.0 and - 15.0 K for f $\rightarrow$ 0 (tending to dc). Therefore by tuning frequency, the transition could be shifted to absolute zero suggesting KLT has a relaxor-type quantum critical point. In addition, we have reanalysed the conflicting literature for Pb2Nb2O7 pyrochlore which suggests that this is also a relaxor-type quantum critical point as the freezing temperature from Vogel-Fulcher fitting is below absolute zero. Since the transition temperature evidenced in the dielectric data at ca. 100 kHz shifts below zero Kelvin for very low frequencies, heat capacity data collected in the zero-frequency (dc) limit, should not indicate a transition. Both of these materials show promise as possible new relaxor-type quantum critical points within non-perovskite based structures as multiple compounds are reported with low-temperature transitions.