The rise of two-dimensional (2D) graphene-cognated crystals with nonzero band gaps like transition metal dichalcogenides has led to a rapidly increasing interest in their dimensionality-dependent anisotropic properties, which bear high potential for ultrathin electronics. 2D crystals of the III–VI metal chalcogenide InSe represent a new kind of material class predestined for the use in optoelectronic applications as highly responsive photodetectors and field-effect transistors. We present a solution-processable method for 2D ultrathin InSe nanosheets (≤5 nm with ligands, lateral sizes up to ∼800 μm) with a detailed characterization of the sheet formation by a lamellar ligand templated growth. Optical and electrical transport properties, as well as in depth analysis of the crystal structure and stoichiometry of the colloidal nanosheets by electron and atomic force microscopy, X-ray photoelectron spectroscopy, and scattering methods complete this comprehensive study on a wet-chemical alternative to produce ultrathin InSe nanosheets.
Colloidal quantum dots assembled into quantum dot solids usually suffer from poor conductivity. The most common charge transport mechanism through the solid is hopping transport where the hopping probability depends on the barrier type (stabilizing/connecting ligand molecule) and the interparticle distance. It is demonstrated that the electronic structure of the ligand molecule strongly alters the transport behavior through CuInSe2 quantum dot solids. Transport measurements and optical‐pump terahertz‐probe experiments after a ligand exchange to fully conjugated molecules show an increase of the conductivity by orders of magnitude, as well as a change of the hopping transport mechanism. This change is not due to a reduced interparticle distance, but the electronic structure: the obtained frequency‐dependent complex conductivities point toward an efficient hole transport enabled by an alignment of the quantum dot valence bands and ligand states.
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