A Thermal Expansion Coefficient Study of Several Magnetic Spin Materials via Capacitive Dilatometry

Abstract

The work presented in this thesis detail the measurement of the thermal expansion coefficient of three magnetic spin materials. Thermal expansion coefficient values were measured by capacitive dilatometry in several key low (T < 250 K) temperature regions specific to each material. This thesis is separated into several key parts.

The first part establishes the theory behind observing phase transitions through the thermal expansion coefficient. Beginning with the classical definitions of the specific heat, compressibility and thermal expansion coefficient, the three properties are related using a property known as the Grüneisen parameter. To first order, the parameter allows phase transitions to be observed by the thermal expansion coefficient.

The second part introduces capacitive dilatometry; a technique used to measure the thermal expansion coefficient. Three capacitive dilatometer devices are presented in this section. The silver compact dilatometer, the fused quartz dilatometer and the copper dilatometer. Each device discusses merits and weaknesses to their designs. Particular focus is made on the fused quartz dilatometer which was built during the duration of this thesis.

The third part presents research on three magnetic spin materials; LiHoF4, Tb2Ti2O7 and Ba3NbFe3Si2O14. These materials are studied individually focusing on specific aspects.

LiHoF4, a candidate material for the transverse field Ising model, provides insight to quantum phase transitions. Thermal expansion coefficient and magnetostriction along the c-axis for T ≈ 1.3-1.8 K and transverse field Ht ≈ 0-4 T were measured extracting critical points for a Ht-T phase diagram. Existing thermal expansion coefficient measurements had evidence of possible re-entrant behaviour. With a high density of low transverse field critical points it was established that LiHoF4 showed no evidence of re-entrant behaviour.

The highly debated material Tb2Ti2O7 has a rich, controversial low temperature behaviour. Originally believed to be a spin liquid, specific heat results propose a scenario involving a sample composition dependent ordered state. Still under considerably attention, thermal expansion coefficient measurements were performed for T < 1 K. The results are interpreted to either fit into the proposed scenario or provide evidence for an alternate scenario.

The material Ba3NbFe3Si2O14 exhibits a magnetoelectric multiferroic phase below TN ≈ 27 K; a phase where magnetic and electric order simultaneously exist. The formation of this phase is believed to have a similar structural shift observed in hexagonal perovskite multiferroic materials. The ferroelectric ordering in those materials are brought about through a centrosymmetric to non-centrosymmetric structural shift. The thermal expansion and thermal expansion coefficient coefficient along the a and c axis are measured for T > TN searching for a displacive structural phase transition.