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The bulk photovoltaic effect (BPVE), which uniquely exists in non-centrosymmetric materials, has been received extensive attention recently due to its potential to overcome the theoretical Shockley-Queisser limit in traditional p-n junction solar cells. Here, freestanding single-domain BiFeO 3 membranes are exfoliated from miscut SrTiO 3 substrates by dissolving Sr 3 Al 2 O 6 sacrificial layers, and transferred on SiO 2 /Si substrates. This study finds that the freestanding BiFeO 3 membranes maintain the single-domain structure and exhibits the significantly enhanced bulk photovoltaic response (≈200% enhancement), compared to the strained BiFeO 3 films. The comprehensive atomic imaging analyses manifest that the freestanding BiFeO 3 membrane demonstrates the bigger noncentral ion (Fe) displacement, which results in the larger in-plane ferroelectric polarization and substantial increase in the BPVE photocurrent. This work not only provides an effective approach to enhance the BPVE of ferroelectric oxide films, but also can potentially promote the exploration of BPVE of oxide membranes integrated with silicon-based or 2D electronics., (© 2024 Wiley‐VCH GmbH.)

Complex oxides offer a wide range of functional properties, and recent advances in the fabrication of freestanding membranes of these oxides are adding new mechanical degrees of freedom to this already rich functional ecosystem. Here, photoactuation is demonstrated in freestanding thin film resonators of ferroelectric Barium Titanate (BaTiO 3 ) and paraelectric Strontium Titanate (SrTiO 3 ). The free-standing films, transferred onto perforated supports, act as nano-drums, oscillating at their natural resonance frequency when illuminated by a frequency-modulated laser. The light-induced deflections in the ferroelectric BaTiO 3 membranes are two orders of magnitude larger than in the paraelectric SrTiO 3 ones. Time-resolved X-ray micro-diffraction under illumination and temperature-dependent holographic interferometry provide combined evidence for the photostrictive strain in BaTiO 3 originating from a partial screening of ferroelectric polarization by photo-excited carriers, which decreases the tetragonality of the unit cell. These findings showcase the potential of photostrictive freestanding ferroelectric films as wireless actuators operated by light., (© 2024 Wiley‐VCH GmbH.)

Interfaces formed by correlated oxides offer a critical avenue for discovering emergent phenomena and quantum states. However, the fabrication of oxide interfaces with variable crystallographic orientations and strain states integrated along a film plane is extremely challenging by conventional layer-by-layer stacking or self-assembling. Here, the creation of morphotropic grain boundaries (GBs) in laterally interconnected cobaltite homostructures is reported. Single-crystalline substrates and suspended ultrathin freestanding membranes provide independent templates for coherent epitaxy and constraint on the growth orientation, resulting in seamless and atomically sharp GBs. Electronic states and magnetic behavior in hybrid structures are laterally modulated and isolated by GBs, enabling artificially engineered functionalities in the planar matrix. This work offers a simple and scalable method for fabricating unprecedented innovative interfaces through controlled synthesis routes as well as providing a platform for exploring potential applications in neuromorphics, solid-state batteries, and catalysis., (© 2022 Wiley-VCH GmbH.)

Hafnia-based compounds have considerable potential for use in nanoelectronics due to their compatibility with complementary metal-oxide-semiconductor devices and robust ferroelectricity at nanoscale sizes. However, the unexpected ferroelectricity in this class of compounds often remains elusive due to the polymorphic nature of hafnia, as well as the lack of suitable methods for the characterization of the mixed/complex phases in hafnia thin films. Herein, the preparation of centimeter-scale, crack-free, freestanding Hf 0.5 Zr 0.5 O 2 (HZO) nanomembranes that are well suited for investigating the local crystallographic phases, orientations, and grain boundaries at both the microscopic and mesoscopic scales is reported. Atomic-level imaging of the plan-view crystallographic patterns shows that more than 80% of the grains are the ferroelectric orthorhombic phase, and that the mean equivalent diameter of these grains is about 12.1 nm, with values ranging from 4 to 50 nm. Moreover, the ferroelectric orthorhombic phase is stable in substrate-free HZO membranes, indicating that strain from the substrate is not responsible for maintaining the polar phase. It is also demonstrated that HZO capacitors prepared on flexible substrates are highly uniform, stable, and robust. These freestanding membranes provide a viable platform for the exploration of HZO polymorphic films with complex structures and pave the way to flexible nanoelectronics., (© 2022 Wiley-VCH GmbH.)