Large polarization gradients and temperature-stable responses in compositionally-graded ferroelectrics

Anoop R. Damodaran, Shishir Pandya, Yubo Qi, Shang-Lin Hsu, Shi Liu, Christopher Nelson, Arvind Dasgupta, Peter Ercius, Colin Ophus, Liv R. Dedon, Josh C. Agar, Hongling Lu, Jialan Zhang, Andrew M. Minor, Andrew M. Rappe, Lane W. Martin

A range of modern applications require large and tunable dielectric, piezoelectric or pyroelectric response of ferroelectrics. Such effects are intimately connected to the nature of polarization and how it responds to externally applied stimuli. Ferroelectric susceptibilities are, in general, strongly temperature dependent, diminishing rapidly as one transitions away from the ferroelectric phase transition (TC). In turn, researchers seek new routes to manipulate polarization to simultaneously enhance susceptibilities and broaden operational temperature ranges. Here, we demonstrate such a capability by creating composition and strain gradients in Ba1-xSrxTiO3 films which result in spatial polarization gradients as large as 35 μC cm(-2) across a 150 nm thick film. These polarization gradients allow for large dielectric permittivity with low loss (ɛr≈775, tan δ<0.05), negligible temperature-dependence (13% deviation over 500 °C) and high-dielectric tunability (greater than 70% across a 300 °C range). The role of space charges in stabilizing polarization gradients is also discussed.