Design principles for optimizing pyroelectric responses of doped HfO ₂

Abstract Ferroelectric HfO 2 is an emerging pyroelectric material with promising energy-harvesting applications. Herein, via ab-initio molecular dynamics simulations, we investigate the role of dopants in tailoring the pyroelectricity in ferroelectric HfO 2 . We demonstrate that dopant perturbs the local bonding environment of host HfO 2 structure, giving rise to notable pyroelectricity. The pyroelectric response is further enhanced at the ferroelectric-to-paraelectric phase transition, characterized by a Curie temperature that reduces with increasing doping concentrations. The reduction is more pronounced for dopants with ionic radii smaller than the host. The present work highlights the efficient tuning of pyroelectric response in ferroelectric HfO 2 by doping.