Two-dimensional semiconductors (2DSCs) are attractive for a variety of optoelectronic and catalytic applications due to their ability to be fabricated as wide-area, monolayer-thick films and their unique optical and electronic...

Well-ordered nanoparticle arrays are attractive platforms for a variety of analytical applications, but the fabrication of such arrays is generally challenging. Here, it is demonstrated that scanning electrochemical cell microscopy (SECCM) can be used as a powerful, instantly reconfigurable tool for the fabrication of ordered nanoparticle arrays. Using SECCM, Ag nanoparticle arrays were straightforwardly fabricated via electrodeposition at the interface between a substrate electrode and an electrolyte-filled pipet. By dynamically monitoring the currents flowing in an SECCM cell, individual nucleation and growth events could be detected and controlled to yield individual nanoparticles of controlled size. Characterization of the resulting arrays demonstrate that this SECCM-based approach enables spatial control of nanoparticle location comparable with the terminal diameter of the pipet employed and straightforward control over the volume of material deposited at each site within an array. These results provide further evidence for the utility of probe-based electrochemical techniques such as SECCM as tools for surface modification in addition to analysis.

Organometallic halide perovskites have garnered significant attention in various fields of material science, particularly solar energy conversion, due to their desirable optoelectronic properties and compatibility with scalable fabrication techniques. It is often unclear, however, how carrier generation and transport within complex polycrystalline films are influenced by variations in local structure. Elucidating how distinct structural motifs within these heterogeneous systems affect behavior could help guide the continued improvement of perovskite-based solar cells. Here, we present studies applying scanning electron microscopy (SECCM) to map solar energy harvesting within well-defined model systems of organometallic halide perovskites. Methylammonium lead bromide (MAPbBr 3 ) single crystals were prepared via a low-temperature solution-based route, and their photoelectrochemical properties were mapped via SECCM using p-benzoquinone (BQ) in dichloromethane as a redox mediator. Correlated SECCM mapping and electron microscopy studies enabled facet-to-facet variations in photoelectrochemical performance to be revealed and carrier transport lengths to be evaluated. The photoelectrochemical behavior observed within individual single crystals was quite heterogeneous, attributable to local variations in crystal structure/ orientations, intrafacet junctions, and the presence of other structural defects. These observations underscore the significance of controlling the microstructure of single perovskite crystals, presenting a promising avenue for further enhancement of perovskitebased solar cells.

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