Anisotropy-Driven Crystallization of Dimensionally Resolved Quasi-1D van der Waals Nanostructures

08 May 2023, Version 1
This content is a preprint and has not undergone peer review at the time of posting.


Unusual behavior in solids emerge from the complex interplay between crystalline order, composition, and dimensionality. In crystals comprising of weakly-bound one-dimensional (1D) or quasi-1D (q-1D) chains, properties such as charge density waves, topologically protected states, and indirect-to-direct band gap crossovers have been predicted to arise. However, the experimental demonstration of many of these nascent physics in 1D or q-1D van der Waals (vdW) crystals is obscured by the highly anisotropic bonding between the chains, stochasticity of top-down exfoliation, and lack of synthetic strategies to control bottom-up growth. Herein, we report the directed crystallization of a model q-1D vdW phase, Sb2S3, into dimensionally resolved nanostructures. We demonstrate the uncatalyzed growth of highly crystalline Sb2S3 nanowires, nanoribbons, and quasi-2D nanosheets with thicknesses in the range of 10 to 100 nm from the bottom-up crystallization of [Sb4S6]n chains. We found that dimensionally resolved nanostructures emerge from two distinct chemical vapor growth pathways defined by diverse covalent intra-chain and anisotropic vdW inter-chain interactions and precise precursor ratios. At sub-100 nm nanostructure thicknesses, we observe the hardening of phonon modes, blue-shifting of optical band gaps, and emergence of a new high-energy photoluminescence peak, suggesting a confinement-induced indirect-to-direct optical band gap crossover. The directional growth of weakly bound 1D ribbons or chains into well-resolved nanocrystalline morphologies provides opportunities to develop ordered nanostructures and hierarchical assemblies that are suitable for a wide range of optoelectronic and quantum devices.


van der Waals
one dimensional

Supplementary materials

Supplementary Information
This file includes the following: Supplementary Section 1: Chemical Vapor Deposition (CVD) Setup and Methodology Supplementary Section 2: Materials and Characterization Supplementary Section 3: Additional Discussion of Results Supplementary Section 4: Additional Characterization Data Figures S1 to S14 Tables S1 to S8


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