Blue Light Emitting Defective Nanocrystals Composed of Earth-Abundant Elements

Hansen, Eric C.; Liu, Yun; Utzat, Hendrik; Bertram, Sophie N.; Grossman, Jeffrey C.; Bawendi, Moungi G.

doi:10.1002/anie.201911436

Title: Blue Light Emitting Defective Nanocrystals Composed of Earth-Abundant Elements

Journal Article · Wed Nov 06 00:00:00 EST 2019 · Angewandte Chemie (International Edition)

DOI:https://doi.org/10.1002/anie.201911436· OSTI ID:1800517

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Massachusetts Institute of Technology (MIT), Cambridge, MA (United States)

Abstract Copper‐based ternary (I–III–VI) chalcogenide nanocrystals (NCs) are compositionally‐flexible semiconductors that do not contain lead (Pb) or cadmium (Cd). Cu‐In‐S NCs are the dominantly studied member of this important materials class and have been reported to contain optically‐active defect states. However, there are minimal reports of In‐free compositions that exhibit efficient photoluminescence (PL). Here, we report a novel solution‐phase synthesis of ≈4 nm defective nanocrystals (DNCs) composed of copper, aluminum, zinc, and sulfur with ≈20 % quantum yield and an attractive PL maximum of 450 nm. Extensive spectroscopic characterization suggests the presence of highly localized electronic states resulting in reasonably fast PL decays (≈1 ns), large vibrational energy spacing, small Stokes shift, and temperature‐independent PL linewidth and PL lifetime (between room temperature and ≈5 K). Furthermore, density functional theory (DFT) calculations suggest PL transitions arise from defects within a CuAl ₅ S ₈ crystal lattice, which supports the experimental observation of highly‐localized states. The results reported here provide a new material with unique optoelectronic characteristics that is an important analog to well‐explored Cu‐In‐S NCs.

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Research Organization:: Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE); US Air Force Office of Scientific Research (AFOSR); National Science Scholarship; National Science Foundation (NSF); USDOE

Grant/Contract Number:: FG02-07ER46454; AC02-05CH11231; DMR-1419807; ACI-1053575; 1541959

OSTI ID:: 1800517

Alternate ID(s):: OSTI ID: 1577001

Journal Information:: Angewandte Chemie (International Edition), Vol. 59, Issue 2; ISSN 1433-7851

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 15 works

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