TY - JOUR
T1 - InP-quantum-dot-in-ZnS-matrix solids for thermal and air stability
AU - Lee, Seungjin
AU - Sagar, Laxmi Kishore
AU - Li, Xiyan
AU - Dong, Yitong
AU - Chen, Bin
AU - Gao, Yuan
AU - Ma, Dongxin
AU - Levina, Larissa
AU - Grenville, Aidan
AU - Hoogland, Sjoerd
AU - de Arquer, F. Pelayo García
AU - Sargent, Edward H.
N1 - Funding Information:
This work is supported by the Natural Sciences and Engineering Research Council of Canada (NSERC, grant number 537463-18). The authors acknowledge Huawei Canada for its financial support. This research was also supported by the National Research Foundation (NRF) of Korea (NRF-2020R1A6A3A03038131). We thank D. Kopilovic, E. Palmiano, L. Levina, and R. Wolowiec for the technical support.
Publisher Copyright:
© 2020 American Chemical Society
PY - 2020/11/24
Y1 - 2020/11/24
N2 - InP/ZnS core/shell colloidal quantum dots (QDs) are promising candidates as Cd- and Pb-free emitters owing to their high photoluminescence quantum yield, narrow emission linewidth, and color tunability in the visible range. However, the stability of QD solid films remains an issue: they are vulnerable to oxygen, moisture, and heat. Here, we report the encapsulation of InP/ZnS QDs in a lattice-matched ZnS matrix. We do so by developing a biphasic ligand exchange and uniting it with a sol−gel film assembly. Conventional ZnS precursors, which rely on neutral thiourea, fail to stabilize the QDs in highly polar solvents, leading to their agglomeration prior to matrix formation. Here, we substitute thiourea with ammonium thiocyanate-an ionic compound isomer of thiourea-to stabilize InP/ZnS QDs in a ZnS matrix precursor solution. The stabilized QD and precursor solution is then cast and annealed to trigger the formation of a homogeneous and robust ZnS matrix that protects the QDs. The resulting QD solid films show invariant optical properties following annealing at 200 °C for 1 h under ambient conditions, under continuous laser excitation at 60 mW cm−2 for 180 min, and also after a month of storage under ambient conditions. In contrast, the control film exhibits significant degradation of its optical properties after annealing at 200 °C for 1 h, under laser excitation within 20 min, and under ambient conditions within 10 days.
AB - InP/ZnS core/shell colloidal quantum dots (QDs) are promising candidates as Cd- and Pb-free emitters owing to their high photoluminescence quantum yield, narrow emission linewidth, and color tunability in the visible range. However, the stability of QD solid films remains an issue: they are vulnerable to oxygen, moisture, and heat. Here, we report the encapsulation of InP/ZnS QDs in a lattice-matched ZnS matrix. We do so by developing a biphasic ligand exchange and uniting it with a sol−gel film assembly. Conventional ZnS precursors, which rely on neutral thiourea, fail to stabilize the QDs in highly polar solvents, leading to their agglomeration prior to matrix formation. Here, we substitute thiourea with ammonium thiocyanate-an ionic compound isomer of thiourea-to stabilize InP/ZnS QDs in a ZnS matrix precursor solution. The stabilized QD and precursor solution is then cast and annealed to trigger the formation of a homogeneous and robust ZnS matrix that protects the QDs. The resulting QD solid films show invariant optical properties following annealing at 200 °C for 1 h under ambient conditions, under continuous laser excitation at 60 mW cm−2 for 180 min, and also after a month of storage under ambient conditions. In contrast, the control film exhibits significant degradation of its optical properties after annealing at 200 °C for 1 h, under laser excitation within 20 min, and under ambient conditions within 10 days.
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U2 - 10.1021/acs.chemmater.0c02870
DO - 10.1021/acs.chemmater.0c02870
M3 - Article
AN - SCOPUS:85096750463
SN - 0897-4756
VL - 32
SP - 9584
EP - 9590
JO - Chemistry of Materials
JF - Chemistry of Materials
IS - 22
ER -