Enhanced upconversion and photoconductive nanocomposites of lanthanide-doped nanoparticles functionalized with low-vibrational-energy inorganic ligands.

Abstract

Upconverting nanoparticles (UCNPs) convert near-infrared (IR) light into higher-energy visible light, allowing them to be used in applications such as biological imaging, nano-thermometry, and photodetection. It is well known that the upconversion luminescent efficiency of UCNPs can be enhanced by using a host material with low phonon energies, but the use of low-vibrational-energy inorganic ligands and non-epitaxial shells has been relatively underexplored. Here, we investigate the functionalization of lanthanide-doped NaYF₄ UCNPs with low-vibrational-energy Sn₂S₆^4- ligands. Raman spectroscopy and elemental mapping are employed to confirm the binding of Sn₂S₆^4- ligands to UCNPs. This binding enhances upconversion efficiencies up to a factor of 16, consistent with an increase in the luminescent lifetimes of the lanthanide ions. Annealing Sn₂S₆^4--capped UCNPs results in the formation of a nanocomposite comprised of UCNPs embedded within an interconnected matrix of SnS₂, enabling each UCNP to be electrically accessible through the semiconducting SnS₂ matrix. This facilitates the integration of UCNPs into electronic devices, which we demonstrate through the fabrication of a UCNP-SnS₂ photodetector that detects UV and near-IR light. Our findings show the promise of using inorganic capping agents to enhance the properties of UCNPs while facilitating their integration into optoelectronic devices.