Journal article
Red Emission from Copper-Vacancy Color Centers in Zinc Sulfide Colloidal Nanocrystals
ACS nano, Vol.17(6), pp.5963-5973
03/28/2023
DOI: 10.1021/acsnano.3c00191
PMID: 36892080
Abstract
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 biosensing and optoelectronic 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.
Details
- Title: Subtitle
- Red Emission from Copper-Vacancy Color Centers in Zinc Sulfide Colloidal Nanocrystals
- Creators
- Sarah M. Thompson - University of PennsylvaniaCuneyt Sahin - University of IowaShengsong Yang - University of PennsylvaniaMichael E. Flatte - University of IowaChristopher B. Murray - University of PennsylvaniaLee C. Bassett - University of PennsylvaniaCherie R. Kagan - University of Pennsylvania
- Resource Type
- Journal article
- Publication Details
- ACS nano, Vol.17(6), pp.5963-5973
- Publisher
- Amer Chemical Soc
- DOI
- 10.1021/acsnano.3c00191
- PMID
- 36892080
- ISSN
- 1936-0851
- eISSN
- 1936-086X
- Number of pages
- 11
- Grant note
- DMR-2019444; DMR-1922278; DMR-1921877 / National Science Foundation; National Science Foundation (NSF) DGE-1845298 / National Science Foundation Graduate Research Fellowship; National Science Foundation (NSF)
- Language
- English
- Date published
- 03/28/2023
- Academic Unit
- Electrical and Computer Engineering; Physics and Astronomy
- Record Identifier
- 9984428789402771
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