arXiv subjects

Ewout van der Veer

Publications and source records attributed to Ewout van der Veer.

9 recordsLinked to original sources

arXiv2026

Super-tetragonal ferroelectric barium titanate through anionic overstoichiometry

Ferroelectric oxides, characterized by an electrical polarization that is switchable with an electric field, are an appealing class of materials for energy-efficient computing, electronics, and photonics. In thin films, the properties of ferroelectrics are commonly tuned using substrate-imposed epitaxial strain, an approach limited to biaxial strain states and a finite number of available substrates. Here, we demonstrate that is is possible to move beyond conventional epitaxial growth by using pulsed laser deposition under highly non-equilibrium conditions. Specifically, we show that this unconventional processing route allows us to stabilize a super-tetragonal phase of ferroelectric $\text{BaTiO}_3$. The key to this stabilization lies in the insertion of surplus oxygen atoms into the unit cell, resulting in peroxide bond formation that give rise to an aspect ratio of as high as 1.08. Notably, this super-tetragonal phase exhibits an enhanced ferroelectric polarization, reduced coercivity, lower leakage currents, and increased cycling endurance compared to conventional bulk-like $\text{BaTiO}_3$ films. These results, thus, showcase the potential of non-equilibrium growth for defect engineering to obtain emergent phases in complex oxides and tune their physical properties in thin films expanding the scope of traditional epitaxy.

cond-mat.mtrl-sci↗

arXiv2026

Domain-wall-to-domain interconversion in a polar conducting oxide

Domain walls in ferroic crystals are topological defects with a symmetry distinct from the domain interior, allowing them to display functionalities that are otherwise forbidden in the host material. Despite their unique properties, domain walls are strictly confined to two-dimensional interfaces, which hinders unveiling their true nature and limits their applicability. Here, we demonstrate reversible dimensionality control by expanding nanoscale domain walls into three-dimensional functional regions in polar epitaxial tungsten trioxide ($\text{WO}_3$). This domain-wall-to-domain interconversion is enabled by the conducting, non-polar domain walls adopting the parent-phase structure. An alternating electric field applied through a scanning probe tip induces localized heating, which expands this domain-wall phase into the adjacent polar domains. This approach enables reversible spatial control to switch between mutually exclusive properties of domains (polarity) and domain walls (conductivity), offering a new paradigm for reconfigurable oxide electronics.

cond-mat.mtrl-sci↗

arXiv2026

PdNeuRAM: forming-free, multi-bit Pd/HfO2 ReRAM for energy-efficient neuromorphic computing

Memristor technology shows great promise for energy-efficient computing, yet it grapples with challenges like resistance drift and inherent variability. For filamentary Resistive RAM (ReRAM), one of the most investigated types of memristive devices, the expensive electroforming step required to create conductive pathways results in increased power and area overheads and reduced endurance. In this study, we present novel HfO2-based forming-free ReRAM devices, PdNeuRAM, that operate at low voltages, support multi-bit functionality, and display reduced variability. Through a deep understanding and comprehensive material characterization, we discover the key process that allows this unique behavior: a Pd-O-Hf configuration that capitalizes on Pd innate affinity for integrating into HfO2. This structure actively facilitates charge redistribution at room temperature, effectively eliminating the need for electroforming. Moreover, the fabricated ReRAM device provides tunable resistance states for dense memory and reduces programming and reading energy by 43% and 73%, respectively, using spiking neural networks (SNN). This study reveals novel mechanistic insights and delineates a strategic roadmap for the realization of power-efficient and cost-effective ReRAM devices.

cond-mat.mtrl-sci↗

arXiv2026

Disentangling the ferroelectric phases of epitaxial hafnia

Since its discovery, ferroelectric hafnia has been extensively studied due to its CMOS-compatibility and ability to remain polarized at sub-10 nm thicknesses. The ferroelectric behaviour is generally attributed to a polar orthorhombic (OIII) phase. However, a second polar phase with rhombohedral symmetry (R-phase) has also been reported in epitaxial films. The nature of the R-phase remains disputed due to the subtle differences with the OIII-phase when probed by standard thin film characterisation techniques. Given the functional properties of ferroelectrics are crucially determined by the crystal symmetry, resolving this matter is imperative. In this work, we settle the controversy through extensive 3D reciprocal space surveys made possible via synchrotron-based grazing incidence diffraction from epitaxial films of both phases. These experiments, together with direct comparison of their temperature dependence and electrical responses, conclusively establish them as two distinct phases and provide insight into their key characteristics.

cond-mat.mtrl-sci↗

arXiv2025

Epitaxial Sr(Sn, Ge)$_{x}$Ti$_{1-x}$O$_{3}$ buffer layers for continuous strain engineering on SrTiO$_{3}$ substrates

Epitaxial strain plays a key role in determining the structure and functionality of thin films, with the choice of substrate being traditionally used to control the magnitude of the applied strain. However, even in the large family of perovskite materials, this allows for only a limited, discrete set of strain states to be achieved. Here we report on an approach to controlling epitaxial strain for the growth of perovskite materials by involving a single SrTiO$_{3}$ substrate (the most available perovskite in single crystal form) and a buffer layer that consists of the solid solution Sr(Sn, Ge)$_{x}$Ti$_{1-x}$O$_{3}$, of which the lattice parameter can be tuned in a continuous fashion, from 3.880 Å up to 4.007 Å, while maintaining coherent epitaxial growth on SrTiO$_{3}$ with high quality interfaces. Using a BaTiO$_{3}$ overlayer as a model system, we show that changes to the buffer layer composition, i.e. increase of in-plane lattice parameter, change the strain state of BaTiO$_{3}$ from fully relaxed, through highly compressively strained, to an exotic state showing 'inverted' epitaxy in which the buffer layer is relaxed from the substrate but lattice matched to the overlayer.

cond-mat.mtrl-sci↗

arXiv2025

Polarity and anti-distortive polarons in WO3 through epitaxial shear strain

Bestowing CMOS-compatible binary oxides with additional functionalities is a powerful strategy toward the realization of oxide electronics. Ideal candidates are thin films which display a strong sensitivity to strain, chemical doping or nanoscale confinement. Among these, crystalline tungsten trioxide WO3 exhibits exceptional structural flexibility, enabling a wide range of functionalities. Here, we reveal the emergence of a previously unreported polar phase in epitaxial WO3 thin films. We accomplish this by imposing epitaxial shear strain, which stabilizes a low-symmetry triclinic structure that persists up to large film thicknesses and elevated temperatures. At the atomic scale, a change in the oxygen octahedral tilt pattern facilitates this symmetry lowering into a polar phase, which manifests as a periodic in-plane polarized stripe domain configuration with needle-like bifurcations at the microscale. The stripe domain walls further exhibit a strongly enhanced electrical conductivity in conjunction with a pronounced reduction of a distortive structural mode, providing the first experimental evidence for the formation of anti-distortive polarons recently predicted in WO3.

cond-mat.mtrl-sci↗

arXiv2025

Guidelines for the optimization of hafnia-based ferroelectrics through superlattice engineering

Hafnia-based ferroelectrics are revolutionizing the data storage industry and the field of ferroelectrics, with improved materials and devices being reported monthly. However, full understanding and control has not been reached yet and the ideal material still needs to be found. Here we report ferroelectric hafnia-zirconia superlattices made out of zirconium-substituted hafnia (Hf$_{1-x}$Zr$_x$O$_2$) sublayers of varying stoichiometries alternating with pure ZrO$_2$ sublayers. It is observed that the ZrO$_2$ layers in these superlattices act as a booster for the total remnant polarization (P$_r$). By combining the benefits of the ZrO$_2$ layers and the added interfaces, which help prevent breakdown, we fabricate superlattices with a total 87.5% ZrO$_2$ content, exhibiting record polarizations with a 2P$_r$ value of 84 $μ$C/cm$^2$ that can be cycled 10$^9$ times, while maintaining a 2P$_r$ > 20 $μ$C/cm$^2$. Next to these attractive properties, substitution of HfO$_2$ by the much more abundant ZrO$_2$ offers a significant step towards the sustainable application of these devices.

cond-mat.mtrl-sci↗

arXiv2023

Atomically resolved phase coexistence in VO2 thin films

Concurrent structural and electronic transformations in VO2 thin films are of twofold importance: enabling fine-tuning of the emergent electrical properties in functional devices, yet creating an intricate interfacial domain structure of transitional phases. Despite the importance of understanding the structure of VO2 thin films, a detailed real space atomic structure analysis in which also the oxygen atomic columns are resolved is lacking. Moreover, intermediate atomic structures have remained elusive due to the lack of robust atomically resolved quantitative analysis. Here, we directly resolve both V and O atomic columns and discover the presence of the strain-stabilized intermediate monoclinic (M2) phase nanolayers (less than 2 nm thick) in epitaxially grown VO2 films on a TiO2 (001) substrate, where the dominant part of VO2 undergoes a transition from the tetragonal (rutile) phase to the monoclinic M1 phase. We unfold the crucial role of imaging the spatial configurations of the oxygen anions (in addition to V cations) utilizing atomic-resolution electron microscopy. Our approach sets a direct pathway to unravel the structural transitions in wide range of correlated oxides, offering substantial implications for e.g. optoelectronics and ferroelectrics.

cond-mat.mtrl-sci↗

arXiv2020

Ferroelectric PbZr$_{1-x}$Ti$_x$O$_3$ by ethylene glycol-based chemical solution synthesis

We have investigated a water-stable sol-gel method based on ethylene glycol as a solvent and bridging ligand for the synthesis of ferroelectric lead zirconate titanate in bulk and thin film forms. This method offers lower toxicity of the solvent, higher stability towards atmospheric moisture and a simplified synthetic procedure compared to traditional sol-gel methods. Ceramic pellets of Nb-doped lead zirconate titanate (PNZT) in the rhombohedral phase were produced with high density and good piezoelectric properties, comparable to those reported in the literature and those found in commercial piezoelectric elements. In addition, a nine-layer thin film stack was fabricated from the same sol by spin coating onto platinized silicon substrates. The films were crack-free and showed a dense perovskite grain structure with a weak (111) orientation. Piezoelectric measurements of the film showed a piezoelectric coefficient comparable to literature values and good stability towards fatigue.

physics.chem-ph↗