Capacitor technologies are as varied as the applications that they enable, but one of the common themes in advanced capacitors for consumer electronics is a desire for increased capacitance in smaller areas/volumes. The heroic advances of discrete capacitor manufacturers have kept pace with the increasing demands of miniaturization, but a time is quickly approaching when it appears that powder‐based fabrication techniques simply will not be able to achieve desired layer thicknesses and capacitance densities. Here, we review the current state of the art and recent advances in the processing science and technology of high‐permittivity thin films with a focus on industrially scalable solution‐based fabrication processes of perovskite ferroelectric systems that appear to offer the greatest promise for the fabrication of future nanoscale capacitors.

Controlling site disorder in ternary and multinary compounds enables tuning optical and electronic properties at fixed lattice constants and stoichiometries, moving beyond many of the challenges facing binary alloy systems. Here, we consider possible enhancements to energy-related applications through the integration of disorder-tunable materials in devices such as light-emitting diodes, photonics, photovoltaics, photocatalytic materials, batteries, and thermoelectrics. However, challenges remain in controlling and characterizing disorder. Focusing primarily on II–IV–V2 materials, we identify three metrics for experimentally characterizing cation site disorder. Complementary to these experiments, we discuss simulation methods to understand disordered materials. Nonidealities, such as off-stoichiometry and oxygen incorporation, can occur while synthesizing metastable disordered materials. While nonidealities may seem undesirable, we describe how if harnessed they could provide another knob for tuning disorder and subsequently properties. To illustrate the effects of disorder on device-relevant properties, we provide case examples of disordered materials and their potential in device applications.

An understanding of the heterostructural implications on alloying in the aluminum nitride-scandium nitride system (Al 1−x Sc x N) can highlight opportunities and design principles for enhancing desired material properties by leveraging nonequilibrium states. The fundamental thermodynamics, and therefore composition-and structuredependent mechanisms, underlying property evolution in this system have not been fully described, despite significant recent efforts driven by interest in enhanced piezoelectric performance. Practical realization of these enhanced properties, however, is hindered by the strong driving thermodynamic driving force for phase separation in the system, highlighting the need for increased study into the role of heterostructural alloying on the thermodynamics and composition-structure-property relationships in this system. With this need in mind, ab initio computed alloy thermodynamics and properties are compared to combinatorial thin-film synthesis and characterization to develop a more complete picture of the structure and property evolution across the Al 1−x Sc x N composition space. The combination of structural frustration and a flattened free-energy landscape lead to substantial increases in electromechanical response. The energy scale of alloy metastability is found to be much larger than previously reported, helping to explain difficulties in achieving homogeneous materials with high scandium concentration. Scandium substitution for aluminum softens the wurtzite crystal lattice, and energetic proximity to the competing hexagonal boron-nitride structure enhances the piezoelectric stress coefficient. Overall, this work provides insight into the understanding of the structure-processing-property relationships in the Al 1−x Sc x N system, suggests material design strategies for even greater property enhancements, and demonstrates the increased property tunability and underexplored nature of nonequilibrium heterostructural alloys.

MXenes are emerging two-dimensional (2D) materials for energy-storage applications and supercapacitors. Their surface chemistry, which determines critical properties, varies due to different synthesis conditions. In this work, we synthesized TiVC solid-solution MXenes by two different synthesis methods and investigated their surface functional groups. We performed etching of the TiVAlC MAX phase using two different solutions, a highly concentrated HF (50 wt % ≈ 29 M) and a mixture of LiF and HCl (1.9 M LiF/12 M HCl). Large-scale delamination of TiVCT x to produce single-flake suspension was achieved by further intercalation of the resultant MXene from LiF/HCl with tetrabutylammonium hydroxide (TBAOH). X-ray diffraction indicates a large interlayer spacing of 2.18 nm for TiVCT x MXene flakes. To investigate the structural stability and adsorption energy of different functional groups on TiVC MXenes, density functional theory (DFT) calculations were performed and supported with X-ray photoelectron spectroscopy (XPS) measurements. A higher concentration of O and a lower concentration of −F were achieved on the TiVC synthesized by LiF/HCl, both of which provide a more favorable surface chemistry for energy-storage applications. Our results provide the first systematic study on the effect of synthesis conditions on the surface chemistry of solid-solution TiVC MXenes.

Nitrides join the perovskite club Perovskite structured materials have a variety of uses as photovoltaics, capacitors, and micromechanical actuators, along with other applications. Oxides, halides, and chalcogenides all have large numbers of perovskite structured materials. Examples of perovskite nitrides are conspicuously absent, but Talley et al . managed to synthesize one (see the Perspective by Hong). Lanthanum tungsten nitride in the perovskite structure turns out to be piezoelectric, which is ideal for a variety of applications. Perovskite structured nitrides are very attractive because they could easily integrate with the large number of nitride-based semiconducting devices already in use. —BG