2023/01/10 by Sarah Thompson, Thompson, Sarah M., Cüneyt Şahin +11 · 1 citation
Materials Science · #Computational Physics (physics.comp-ph) #FOS: Physical sciences #Materials Science (cond-mat.mtrl-sci) #Mesoscale and Nanoscale Physics (cond-mat.mes-hall) #Nanocluster Synthesis and Applications #Optics (physics.optics) #Quantum Dots Synthesis And Properties #Quantum Physics (quant-ph)
paper · pdf · doi:10.48550/arxiv.2301.04223
openalex publication_date 2023/01/10 · openalex created_date 2023/01/13 · openalex updated_date 2026/07/28
Copper-doped zinc sulfide (ZnS:Cu) exhibits down-conversion luminescence in the UV, visible, and IR regions of the electromagnetic spectrum; the visible red, green, and blue emission is referred to as R-Cu, G-Cu, and B-Cu, respectively. The sub-bandgap emission arises from optical transitions between localized electronic states created by point defects, making ZnS:Cu a prolific phosphor material and an intriguing candidate material for quantum information science, where point defects excel as single-photon sources and spin qubits. Colloidal nanocrystals (NCs) of ZnS:Cu are particularly interesting as hosts for the creation, isolation, and measurement of quantum defects, since their size, composition, and surface chemistry can be precisely tailored for bio-sensing and opto-electronic applications. Here, we present a method for synthesizing colloidal ZnS:Cu NCs that emit primarily R-Cu, which has been proposed to arise from the CuZn-VS complex, an impurity-vacancy point defect structure analogous to well-known quantum defects in other materials that produce favorable optical and spin dynamics. First principles calculations confirm the thermodynamic stability and electronic structure of CuZn-VS. Temperature- and time-dependent optical properties of ZnS:Cu NCs show blueshifting luminescence and an anomalous plateau in the intensity dependence as temperature is increased from 19 K to 290 K, for which we propose an empirical dynamical model based on thermally-activated coupling between two manifolds of states inside the ZnS bandgap. Understanding of R-Cu emission dynamics, combined with a controlled synthesis method for obtaining R-Cu centers in colloidal NC hosts, will greatly facilitate the development of CuZn-VS and related complexes as quantum point defects in ZnS.