RESUMO
Solid-state nanopores are a key platform for single-molecule detection and analysis that allow engineering of their properties by controlling size, shape, and chemical functionalization. However, approaches relying on polymers have limits for what concerns hardness, robustness, durability, and refractive index. Nanopores made of oxides with high dielectric constant would overcome such limits and have the potential to extend the suitability of solid-state nanopores toward optoelectronic technologies. Here, we present a versatile method to fabricate three-dimensional nanopores made of different dielectric oxides with convex, straight, and concave shapes and demonstrate their functionality in a series of technologies and applications such as ionic nanochannels, ionic current rectification, memristors, and DNA sensing. Our experimental data are supported by numerical simulations that showcase the effect of different shapes and oxide materials. This approach toward robust and tunable solid-state nanopores can be extended to other 3D shapes and a variety of dielectrics.
RESUMO
Layered perovskites consist of stacks of inorganic semiconducting metal-halide octahedra lattices sandwiched between organic layers with typically dielectric behavior. The in-plane confinement of electrical carriers in such two-dimensional metal halide perovskites drives a large range of appealing electronic properties, such as strong exciton binding, anisotropic charge diffusion, and polarization-directionality. Heterostructures provide additional control on carrier diffusion and localization, and in-plane heterojunctions are interesting because of the associated high charge mobility. Here, this work demonstrates a versatile solution-based approach to fabricate in-plane heterostructures with different halide composition in two-dimensional lead-halide perovskite microcrystals. This leads to spatially separated halide phases with different band gap and light emission. Interestingly, the composition of the exchanged phase and the morphology of the phase boundary depends on the exchange route, which can be related to the preferred localization of the halides at the equatorial or axial octahedra positions that either leads to dissolution and recrystallization of the octahedra lattice (for bromide to iodide), or allows for ion diffusion within the lattice (for iodide to bromide). These detailed insights on the ion exchange processes in layered perovskites will stimulate the development of heterostructures that can be tailored for different applications such as photocatalysis, energy storage, and light emission.