In compositionally complex materials, there is controversy on the effect of enthalpy versus entropy on the structure and short-range ordering in so-called high-entropy materials. To help address this controversy, we synthesized and probed 40 M ₄ AlC ₃ layered carbide phases containing two to nine metals and found that short-range ordering from enthalpy was present until the entropy increased enough to achieve complete disordering of the transition metals in their atomic planes. We transformed all of these layered carbide phases into two-dimensional (2D) sheets and showed the effects of the order versus disorder on their surface properties and electronic behavior. This study suggests the key effect that the competition between enthalpy and entropy has on short-range order in multicompositional materials.

Transition metal carbides have been adopted in energy storage, conversion, and extreme environment applications. Advancements in their 2D counterparts, known as MXenes, enable the design of unique structures at the ~1 nm thickness scale. Alkali cations have been essential in MXenes manufacturing processing, storage, and applications, however, exact interactions of these cations with MXenes are not fully understood. In this study, using Ti₃C₂T_x, Mo₂TiC₂T_x, and Mo₂Ti₂C₃T_x MXenes, we present how transition metal vacancy sites are occupied by alkali cations, and their effect on MXene structure stabilization to control MXene’s phase transition. We examine this behavior using in situ high-temperature x-ray diffraction and scanning transmission electron microscopy, ex situ techniques such as atomic-layer resolution secondary ion mass spectrometry, and density functional theory simulations. In MXenes, this represents an advance in fundamentals of cation interactions on their 2D basal planes for MXenes stabilization and applications. Broadly, this study demonstrates a potential new tool for ideal phase-property relationships of ceramics at the atomic scale.

Carbon nanomaterials such as nanotubes, nanoflakes/nanowalls, and graphene have been used as electron sources due to their superior field electron emission (FEE) characteristics. However, these materials show poor stability and short lifetimes, which prevent their use in practical device applications. The aim of this study was to find an innovative nanomaterial possessing both high robustness and reliable FEE behavior. Herein, a hybrid structure of self-organized multi-layered graphene (MLG)–boron doped diamond (BDD) nanowall materials with superior FEE characteristics was successfully synthesized using a microwave plasma enhanced chemical vapor deposition process. Transmission electron microscopy reveals that the as-prepared carbon clusters have a uniform, dense, and sharp nanowall morphology with sp³ diamond cores encased by an sp² MLG shell. Detailed nanoscale investigations conducted using peak force-controlled tunneling atomic force microscopy show that each of the core–shell structured carbon cluster fields emits electrons equally well. The MLG–BDD nanowall materials show a low turn-on field of 2.4 V μm⁻¹, a high emission current density of 4.2 mA cm⁻² at an applied field of 4.0 V μm⁻¹, a large field enhancement factor of 4500, and prominently high lifetime stability (lasting for 700 min), which demonstrate the superiority of these materials over other hybrid nanostructured materials. The potential of these MLG-BDD hybrid nanowall materials in practical device applications was further illustrated by the plasma illumination behavior of a microplasma device with these materials as the cathode, where a low threshold voltage of 330 V (low threshold field of 330 V mm⁻¹) and long plasma stability of 358 min were demonstrated. The fabrication of these hybrid nanowalls is straight forward and thereby opens up a pathway for the advancement of next-generation cathode materials for high brightness electron emission and microplasma-based display devices.

In this article, we report on the properties of indium tin oxide (ITO) deposited on thin-film silicon layers designed for the application as carrier selective contacts for silicon heterojunction (SHJ) solar cells. We find that ITO deposited on hydrogenated nanocrystalline silicon (nc-Si:H) layers presents a significant drop on electron mobility ${\mu} _{{\rm{e}}}$ in comparison to layers deposited on hydrogenated amorphous silicon films (a-Si:H). The nc-Si:H layers are not only found to exhibit a larger crystallinity than a-Si:H, but are also characterized by a considerably increased surface rms roughness. As we can see from transmission electron microscopy (TEM), this promotes the growth of smaller and fractured features in the initial stages of ITO growth. Furthermore, secondary ion mass spectrometry profiles show different penetration depths of hydrogen from the thin film silicon layers into the ITO, which might both influence ITO and device passivation properties. Comparing ITO to aluminum doped zinc oxide (AZO), we find that AZO can actually exhibit superior properties on nc-Si:H layers. We assess the impact of the modified ITO R $_{\rm{sh}}$ on the series resistance $R_{s}$ of SHJ solar cells with >23% efficiency for optimized devices. This behavior should be considered when designing solar cells with amorphous or nanocrystalline layers as carrier selective contacts.