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In this work we present a detailed structural characterization of Si-4H, anewly discovered bulk form of hexagonal silicon (Si) with potentialoptoelectronic applications. Using multi-scale imaging, we reveal ahierarchical structure in the morphology of Si-4H obtained from high-pressuresynthesis. We demonstrate discrete structural units, platelets, at anintermediate length-scale between the bulk pellets synthesized at highpressures and the flake-like crystallites inferred in previous studies. Directobservation of the platelets reveals their 2D structure, with planar facesspanning hundreds of nanometers to a few micrometers and thicknesses of onlytens of nanometers. We separated and dispersed small packets of quasi-singleplatelets, which enabled us to analyze the crystalline domains within eachgrain. With this view, we demonstrate that Si-4H platelets represent thesmallest crystalline structural units, which can bend at the single-domainlevel. Our characterization of the quasi-2D, flexible platelets of hexagonalSi-4H and proof of concept that the platelets can be dispersed and manipulatedquite simply demonstrate opportunities to design novel optoelectronic and solardevices.

Multi-scale characterization of hexagonal Si-4H: a hierarchical nanostructured material