ABSTRACTGeometries and electronic properties associated with growth patterns, energy gaps, and relative stabilities of (InAs)12n (n = 1–16) nanowires and nanosheets (nanoclusters) are systemically investigated at the GGA‐PBE level. The relative stabilities of (InAs)12n by means of the calculated fragmentation energies and cluster binding energies are determined and discussed. Particularly, the calculated energy gaps of (InAs)12n nanowires (2.261–2.271 eV) and nanosheets (2.228–2.412 eV) are distinctly localized at the regions of visible light energy ranges, indicating that large‐sized (InAs)12n nanosheets or nanowires are relatively wide‐band semiconductor nanomaterial; the calculated density of states reveals large‐sized porous (InAs)12n nanosheets and nanowires with a large surface area and narrow pore size distribution and slight thickness exhibit ultrahigh specific capacitance of trapping solar light energies and high light‐to‐electricity conversion efficiencies in solar energy absorption or conversion or photovoltaics. Consequently, (InAs)12n‐based nanomaterials are favorable for optoelectronic and energy miniaturized devices. Interestingly, the variable sizes depended energy gaps of (InAs)12n nanosheets manifest quantum size effect. Especially, the gradually increased charge‐transfers in large size (InAs)12n nanowires and nanosheets with their sizes can significantly lead to the ionic bonding and metallic characteristic, which can stabilize themselves. Comparison with experiment results available is made.
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