Publisher: American Chemical Society (ACS)

Issue: 20

License: [{"start"=>{"date-parts"=>[[2022, 10, 4]], "date-time"=>"2022-10-04T00:00:00Z", "timestamp"=>1664841600000}, "content-version"=>"vor", "delay-in-days"=>0, "URL"=>"https://creativecommons.org/licenses/by/4.0/"}]

Publication date(s): 2022/10/26 (print) 2022/10/04 (online)

Pages: 8045-8051

Volume: 22 Issue: 20

Journal: Nano Letters

Link: [{"URL"=>"https://pubs.acs.org/doi/pdf/10.1021/acs.nanolett.2c01596", "content-type"=>"application/pdf", "content-version"=>"vor", "intended-application"=>"unspecified"}, {"URL"=>"https://pubs.acs.org/doi/pdf/10.1021/acs.nanolett.2c01596", "content-type"=>"unspecified", "content-version"=>"vor", "intended-application"=>"similarity-checking"}]

URL: http://dx.doi.org/10.1021/acs.nanolett.2c01596

We have synthesized the first reported example of quantum confined high-entropy (HE) nanoparticles, using the lanthanide oxysulfide, Ln2SO2, system as the host phase for an equimolar mixture of Pr, Nd, Gd, Dy, and Er. A uniform HE phase was achieved via the simultaneous thermolysis of a mixture of lanthanide dithiocarbamate precursors in solution. This was confirmed by powder X-ray diffraction and high-resolution scanning transmission electron microscopy, with energy dispersive X-ray spectroscopic mapping confirming the uniform distribution of the lanthanides throughout the particles. The nanoparticle dispersion displayed a significant blue shift in the absorption and photoluminescence spectra relative to our previously reported bulk sample with the same composition, with an absorption edge at 330 nm and a λmax at 410 nm compared to the absorption edge at 500 nm and a λmax at 450 nm in the bulk, which is indicative of quantum confinement. We support this postulate with experimental and theoretical analysis of the bandgap energy as a function of strain and surface effects (ligand binding) as well as calculation of the exciton Bohr radiii of the end member compounds.