Ferroelectric thin films are considered to be among the top candidates for room-temperature electrocaloric materials as they exhibit excellent electric properties and allow application of record high electric fields. At the same time, downsizing of ferroelectric electrocalorics brings about an unwanted but unavoidable depolarizing field that could critically alter or even destroy the films' electrocaloric properties. We use an atomistic first-principles-based computational approach that does not rely on the use of Maxwell relations (i) to reveal the critical role of the depolarizing field on the electrocaloric properties of ferroelectric ultrathin films, (ii) to demonstrate the contribution of nanodomains to the electrocaloric effect in such films, and (iii) to revisit the potential limitations of the indirect approach to study electrocaloric effect in nanoscale ferroelectrics.

• Received 9 February 2015
• Revised 12 May 2015
• Corrected 9 December 2015

DOI:https://doi.org/10.1103/PhysRevB.92.064101