Ferroelastic domain walls in ferroelectric materials possess two properties that are known to affect phonon transport: a change in crystallographic orientation and a lattice strain. Changing populations and spacing of nanoscale-spaced ferroelastic domain walls lead to the manipulation of phonon-scattering rates, enabling the control of thermal conduction at ambient temperatures. In the present work, lead zirconate titanate (PZT) thin-film membrane structures were fabricated to reduce mechanical clamping to the substrate and enable a subsequent increase in the ferroelastic domain wall mobility. Under application of an electric field, the thermal conductivity of PZT increases abruptly at ∼100 kV/cm by ∼13% owing to a reduction in the number of phonon-scattering domain walls in the thermal conduction path. The thermal conductivity modulation is rapid, repeatable, and discrete, resulting in a bistable state or a "digital" modulation scheme. The modulation of thermal conductivity due to changes in domain wall configuration is supported by polarization-field, mechanical stiffness, and in situ microdiffraction experiments. This work opens a path toward a new means to control phonons and phonon-mediated energy in a digital manner at room temperature using only an electric field.

Ferroelectric/ferroelastic domain reorientation was measured in a 1.9 m thick tetragonal{001} oriented PbZr0.3Ti0.70O3 thin film doped with 1% Mn under different mechanical boundary constraints. Domain reorientation was quantified through the intensity changes in the 002/200 Bragg reflections as a function of applied electric field. To alter the degree of clamping, films were undercut from the underlying substrate by 0%, ~25%, ~50%, or ~75% of the electrode area. As the amount of declamping from the substrate increased from 0% to ~75%, the degree of ferroelectric/ferroelastic domain reorientation in the films increased more than six fold at three times the coercive field. In a film that was ~ 75% released from the substrate, approximately 26% of 90° domains were reoriented under the maximum applied field; this value for domain reorientation compares favorably to bulk ceramics of similar compositions. An estimate for the upper limit of 90° domain reorientation in a fully released film under these conditions was determined to be 32%. It was also found that the different clamping conditions strongly influence the amount of reorientation upon removing the applied field, with higher remanence of preferred domain orientations observed in declamped films.

In recent years, there has been an increased interest in octahedral rotations in perovskite materials, particularly on their response to strain in epitaxial thin films. The current theoretical framework assumes that rotations are affected primarily through the change in inplane lattice parameters imposed by coherent heteroepitaxy on a substrate of different lattice constant. This model, which permits prediction of the thin-film rotational pattern using firstprinciples density functional theory, has not been tested quantitatively over a range of strain states. To assess the validity of this picture, coherent LaAlO 3 thin films were grown on SrTiO 3 , NdGaO 3 , LaSrAlO 4 , NdAlO 3 , and YAlO 3 substrates to achieve strain states ranging from +3.03% to-2.35%. The out-of-plane and in-plane octahedral rotation angles were extracted from the intensity of superlattice reflections measured using synchrotron x-ray diffraction. Density functional calculations show that no measurable change in intrinsic defect concentration should occur throughout the range of accessible strain states. Thus, the measured rotation angles were compared with those calculated previously for defect-free films. [Hatt and Spaldin, Phys. Rev. B 82, 195402 (2010)]. Good agreement between theory and experiment was found, suggesting that the current framework correctly captures the appropriate physics in LaAlO 3 .