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Kelley, Kyle P.

Publications and source records attributed to Kelley, Kyle P..

On-demand nanoengineering of in-plane ferroelectric topologies

Hierarchical assemblies of ferroelectric nanodomains, so-called super-domains, can exhibit exotic morphologies that lead to distinct behaviours. Controlling these super-domains reliably is critical for realizing states with desired functional properties. Here we reveal the super-switching mechanism by using a biased atomic force microscopy tip, that is, the switching of the in-plane super-domains, of a model ferroelectric Pb 0.6 Sr 0.4 TiO 3 . We demonstrate that the writing process is dominated by a super-domain nucleation and stabilization process. A complex scanning-probe trajectory enables on-demand formation of intricate centre-divergent, centre-convergent and flux-closure polar structures. Correlative piezoresponse force microscopy and optical spectroscopy confirm the topological nature and tunability of the emergent structures. The precise and versatile nanolithography in a ferroic material and the stability of the generated structures, also validated by phase-field modelling, suggests potential for reliable multi-state nanodevice architectures and, thereby, an alternative route for the creation of tunable topological structures for applications in neuromorphic circuits.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Optical and electronic functionality arising from controlled defect formation in nanoscale complex oxide lateral epitaxy

Epitaxial crystallization of complex oxides provides the means to create materials with precisely selected composition, strain, and orientation, thereby controlling their functionalities. Extending this control to nanoscale three-dimensional geometries can be accomplished via a three-dimensional analog of oxide solid-phase epitaxy, lateral epitaxial crystallization. The orientation of crystals within laterally crystallized SrTiO 3 systematically changes from the orientation of the SrTiO 3 substrate. This evolution occurs as a function of lateral crystallization distance, with a rate of approximately 50° μm -1 . The mechanism of the rotation is consistent with a steady-state stress of tens of megapascal over a 100–nanometer scale region near the moving amorphous/crystalline interface arising from the amorphous-crystalline density difference. Second harmonic generation and piezoelectric force microscopy reveal that the laterally crystallized SrTiO 3 is noncentrosymmetric and develops a switchable piezoelectric response at room temperature, illustrating the potential to use lateral crystallization to control the functionality of complex oxides.

36 MATERIALS SCIENCE↗

Phase Transformations Driving Biaxial Stress Reduction During Wake-Up of Ferroelectric Hafnium Zirconium Oxide Thin Films

Biaxial stress is identified to play an important role in the polar orthorhombic phase stability in hafnium oxide-based ferroelectric thin films. However, the stress state during various stages of wake-up has not yet been quantified. In this work, the stress evolution with field cycling in hafnium zirconium oxide capacitors is evaluated. The remanent polarization of a 20 nm thick hafnium zirconium oxide thin film increases from 9.80 to 15.0 µC cm –2 following 10 6 field cycles. This increase in remanent polarization is accompanied by a decrease in relative permittivity that indicates that a phase transformation has occurred. The presence of a phase transformation is supported by nano-Fourier transform infrared spectroscopy measurements and scanning transmission electron microscopy that show an increase in ferroelectric phase content following wake-up. The stress of individual devices field cycled between pristine and 10 6 cycles is quantified using the sin 2 (ψ) technique, and the biaxial stress is observed to decrease from 4.3 ± 0.2 to 3.2 ± 0.3 GPa. The decrease in stress is attributed, in part, to a phase transformation from the antipolar Pbca phase to the ferroelectric Pca2 1 phase. This work provides new insight into the mechanisms controlling and/or accompanying polarization wake-up in hafnium oxide-based ferroelectrics.

36 MATERIALS SCIENCE↗