David Ascienzo

Observation of structural inhomogeneity at degraded Fe-doped SrTiO3 interfaces

We report on the detection of structural inhomogeneity across anode and cathode interfaces in electrically degraded reduced and oxidized Fe-doped SrTiO3 (Fe:STO) single crystals by optical second harmonic generation (SHG) spectroscopy. SHG spectra were collected from several regions across the anode and cathode interfaces in both degraded reduced and oxidized Fe:STO crystals. We identify the formation of defect concentration gradients along both degraded reduced and oxidized anode interfaces. While the broken symmetries decrease from the outer region towards the central region of the reduced anode, the opposite trend is seen in the degraded oxidized anode. These results are attributed to the formation of centrosymmetric Fe4+:Ti4+-O6 octahedral structures in the central region of the reduced samples degraded anode and non-centrosymmetric Jahn-Teller distortions in the central region of the oxidized samples degraded anode. The observed changes in SHG intensity from the outer region towards the central reg...

Demonstration of ultra-high recyclable energy densities in domain-engineered ferroelectric films

Dielectric capacitors have the highest charge/discharge speed among all electrical energy devices, but lag behind in energy density. Here we report dielectric ultracapacitors based on ferroelectric films of Ba(Zr0.2,Ti0.8)O3 which display high-energy densities (up to 166 J cm–3) and efficiencies (up to 96%). Different from a typical ferroelectric whose electric polarization is easily saturated, these Ba(Zr0.2,Ti0.8)O3 films display a much delayed saturation of the electric polarization, which increases continuously from nearly zero at remnant in a multipolar state, to a large value under the maximum electric field, leading to drastically improved recyclable energy densities. This is achieved by the creation of an adaptive nano-domain structure in these perovskite films via phase engineering and strain tuning. The lead-free Ba(Zr0.2,Ti0.8)O3 films also show excellent dielectric and energy storage performance over a broad frequency and temperature range. These findings may enable broader applications of dielectric capacitors in energy storage, conditioning, and conversion.Dielectric capacitors offer high-power delivery materials for energy-storage, yet suffer from low energy densities. Here, the authors prepared ferroelectric Ba(Zr0.2,Ti0.8)O3 that utilizes polydomain nanostructures to delay electric polarization saturation and boost energy densities.

Investigation of Electric Field–Induced Structural Changes at Fe-Doped SrTiO3 Anode Interfaces by Second Harmonic Generation

We report on the detection of electric field–induced second harmonic generation (EFISHG) from the anode interfaces of reduced and oxidized Fe-doped SrTiO3 (Fe:STO) single crystals. For the reduced crystal, we observe steady enhancements of the susceptibility components as the imposed dc-voltage increases. The enhancements are attributed to a field-stabilized electrostriction, leading to Fe:Ti-O bond stretching and bending in Fe:Ti-O6 octahedra. For the oxidized crystal, no obvious structural changes are observed below 16 kV/cm. Above 16 kV/cm, a sharp enhancement of the susceptibilities occurs due to local electrostrictive deformations in response to oxygen vacancy migrations away from the anode. Differences between the reduced and oxidized crystals are explained by their relative oxygen vacancy and free carrier concentrations which alter internal electric fields present at the Pt/Fe:STO interfaces. Our results show that the optical SHG technique is a powerful tool for detecting structural changes near perovskite-based oxide interfaces due to field-driven oxygen vacancy migration.

Ultrafast optical detection of magnetic inhomogeneity in ferromagnetic La0.67Ca0.33MnO3

Optically excited spin wave resonances in ferromagnetic La0.67Ca0.33MnO3 (LCMO) thin films are probed by subpicosecond Kerr-rotation experiments at 10 K. We identify an extra fundamental mode along with the confined spin wave modes, whose frequency and intensity are independent of film thickness, but depend strongly on the applied magnetic field. We attribute the origin of this mode to magnetic inhomogeneity at the FM ground state. Our results show that the picosecond time-resolved magneto-optical method is a powerful tool for detecting dynamic magnetic inhomogeneity in colossal magneto-resistance manganites.