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Abstract Van der Waals (vdW) ferroelectrics have attracted significant attention for their potential in next-generation nano-electronics. Two-dimensional (2D) group-IV monochalcogenides have emerged as a promising candidate due to their strong room temperature in-plane polarization down to a monolayer limit. However, their polarization is strongly coupled with the lattice strain and stacking orders, which impact their electronic properties. Here, we utilize four-dimensional scanning transmission electron microscopy (4D-STEM) to simultaneously probe the in-plane strain and out-of-plane stacking in vdW SnSe. Specifically, we observe large lattice strain up to 4% with a gradient across ~50 nm to compensate lattice mismatch at domain walls, mitigating defects initiation. Additionally, we discover the unusual ferroelectric-to-antiferroelectric domain walls stabilized by vdW force and may lead to anisotropic nonlinear optical responses. Our findings provide a comprehensive understanding of in-plane and out-of-plane structures affecting domain properties in vdW SnSe, laying the foundation for domain wall engineering in vdW ferroelectrics. 

Recent advances in ferroic materials have identified topological defects as promising candidates for enabling additional functionalities in future electronic systems. The generation of stable and customizable polar topologies is needed to achieve multistates that enable beyond-binary device architectures. In this study, we show how to autonomously pattern on-demand highly tunable striped closure domains in pristine rhombohedral-phase BiFeO3 thin films through precise scanning of a biased atomic force microscopy tip along carefully designed paths. By employing this strategy, we generate and manipulate closed-loop structures with high spatial resolution in an automated manner, allowing the creation of highly tunable and intricate topological domain structures that exhibit distinct polarization configurations without the need for electrode deposition or complex heterostructure growth. As a proof-of-concept for ferroelectric beyond-binary memory devices, we use such topological domains as multistates, engineering an alphabet and automating the symbolic writing/reading process using autonomous microscopy. The resulting information density is compared with that of current commercially available memory devices, demonstrating the potential of ferroelectric topological domains for multistate information storage applications. 

The bulk photovoltaic (BPV) effect, which generates steady photocurrents and above-bandgap photovoltages in non-centrosymmetric materials when exposed to light, holds great potential for advancing optoelectronic and photovoltaic technologies. However, its influence on the reconfiguration of ferroelectric domain structure remains underexplored. In this study, we developed a phase-field model to understand the BPV effect in ferroelectric oxides. Our model reveals that variations in BPV currents across domains create opposing charges at domain walls, enhancing the electric field within domains to ~1000 kV/cm. The strong electric fields can reorient the ferroelectric polarization and enable ultrafast domain wall movements and nonvolatile domain switching on the picosecond scale. Applying anisotropic strain can further strengthen this effect, enablingmore precise control of domain switching. Our findings advance the fundamental understanding of BPV effect in ferroelectrics, paving the ways for developing opto-ferroelectric memory technologies and highefficiency photovoltaic applications via precise domain engineering. 

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 Pb0.6Sr0.4TiO3. 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. 

Perovskite materials, of which strontium titanate (STO) and its thin films are an example, have attracted significant scientific interest because of their desirable properties and the potential to tune thermal conductivity by employing several techniques. Notably, strontium titanate thin films on silicon (Si) substrates serve as a fundamental platform for integrating various oxides onto Si substrates, making it crucial to understand the thermal properties of STO on Si. This work investigates the thermal conductivity of STO thin films on an Si substrate for varying film thicknesses (12, 50, 80, and 200 nm) at room temperature (∼300 K). The thin films are deposited using molecular beam epitaxy on the Si substrate and their thermal conductivity is characterized using the frequency domain thermoreflectance (FDTR) method. The measured values range from 7.4 ± 0.74 for the 200 nm thick film to 0.8 ± 0.1 W m−1 K−1 for the 12 nm thick film, showing a large effect of the film thickness on the thermal conductivity values. The trend of the values is diminishing with the corresponding decrease in the thin film thickness, with a reduction of 38%–93% in the thermal conductivity values, for film thicknesses ranging from 200 to 12 nm. This reduction in the values is relative to the bulk single crystal values of STO, which may range from 11 to 13.5 W m−1 K−1 [Yu et al., Appl. Phys. Lett. 92, 191911 (2008) and Fumega et al., Phys. Rev. Mater. 4, 033606 (2020)], as measured by our FDTR-based experiment. The study also explores the evaluation of volumetric heat capacity (Cp). The measured volumetric heat capacity for the 200 nm thin film is 3.07 MJ m−3 K−1, which is in reasonable agreement with the values available in the literature. 

Abstract We developed a physical model to fundamentally understand the conductive filament (CF) formation and growth behavior in the switching layer during electroforming process in the metal-oxide-based resistive random-access memories (RRAM). The effects of the electrode and oxide layer properties on the CF morphology evolution, current-voltage characteristic, local temperature, and electrical potential distribution have been systematically explored. It is found that choosing active electrodes with lower oxygen vacancy formation energy and oxides with small Lorenz number (ratio of thermal and electrical conductivity) enables CF formation at a smaller electroforming voltage and creates a CF with more homogeneous morphology. This work advances our understanding of the kinetic behaviors of the CF formation and growth during the electroforming process and could potentially guide the oxide and electrode materials selection to realize a more stable and functional RRAM.