High entropy (HE) semiconducting materials pose a vast, novel potential research space, with promising applications in thermoelectric materials and catalysis. HE materials are so called, as they have multiple principal elements scattered randomly throughout a single crystalline phase, leading to intrinsically high levels of configurational entropy. While there is significant work in this area, synthesis of HE materials continues to be a challenge, with very few widely applicable synthetic procedures. Current routes suffer from a range of issues, such as high processing temperatures and extended heating times as well as hyper-specificity or only being suitable for nanoparticle synthesis.<br/><br/>In this work, we present dithiocarbamate based molecular precursors as a versatile, facile route to HE materials across both bulk and nano length scales, taking the lanthanide oxysulfide system as an exemplar. We confirmed samples were HE via the use of scanning transmission electron microscopy energy dispersive X-ray spectroscopic mapping (STEM-EDX) and powder X-ray diffraction (XRD). We also performed various optical characterizations, in the form of UV-visible absorption spectroscopy as well as both steady state and time resolved photoluminescence.<br/><br/>We were able to produce materials at both bulk and nano length scales of very similar composition, allowing for a direct observation of quantum confinement effects, using density functional theory modelling to confirm that the effect observed was indeed quantum confinement. This, being the first observation of its kind in a high entropy material reported to date.

Synthesis of high entropy lanthanide oxysulfides across a range of length scales via the thermolysis of a molecular precursor cocktail

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