Ultra-fast electric field control of giant electrocaloric effect in ferroelectrics

Abstract

There is a surge of interest in developing environmentally friendly cooling technology based on the solid--state electrocaloric effect (ECE). Here, we point out that negative ECE with a fast cooling rate ($\approx$10${}^{11}$ K/s) can be achieved by driving solid crystals to a high--temperature phase with a properly designed electric field pulse. Specifically, we predict that an ultrafast electric field pulse can cause a negative ECE up to 35 K in PbTiO${}_3$ occurring on few picosecond time scales. We acquire and analyze these results by clarifying the mechanism of ECE during an adiabatic irreversible process; In addition to the conventional explanation of the ECE with entropy reallocation, we simply portray the ECE with the concept of internal energy redistribution. Electric field does work on a ferroelectric crystal and redistributes its internal energy. How the kinetic energy is redistributed determines the temperature change and strongly depends on the electric field temporal profile. This concept is supported by our all--atom molecular dynamics simulations of PbTiO${}_3$ and BaTiO${}_3$. Based on this improved understanding of ECE, we propose strategies for inducing both giant and negative ECE. This work offers a more general framework to understand the ECE and highlights the opportunities of electric--field engineering for controlled design of fast and efficient cooling technology.

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• Giant electrocaloric effect in thin film Pb Zr_0.95 Ti_0.05 O_3
• Advanced materials for solid-state refrigeration
• Direct measurement of giant electrocaloric effect in BaTiO3 multilayer thick film structure beyond theoretical prediction
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• Indirect but Efficient: Laser-Excited Electrons Can Drive Ultrafast Polarization Switching in Ferroelectric Materials
• Pressure-induced enhancement of non-polar to polar transition temperature in metallic LiOsO${}_3$
• Flexoelectricity-stabilized ferroelectric phase with enhanced reliability in ultrathin La:HfO2 films
• Sr-induced dipole scatter in BST: Insights from MD simulations using a transferable bond valence-based interatomic potential
• Tailoring the electrocaloric effect by internal bias fields and field protocols
• Domain Wall Acceleration by Ultrafast Field Application: An Ab Initio-Based Molecular Dynamics Study