TY - JOUR
T1 - Coupling Intracompound Charge Transfer and Cluster-Centered Excited States in Cu(I) Halide Hybrids for Efficient White Light Emission
AU - Liu, Xing
AU - Li, Yue
AU - Zhou, Lei
AU - Li, Ming
AU - Zhou, Yuanyuan
AU - He, Rongxing
N1 - X.L. and Y.L. contributed equally to this work. The authors acknowledge the financial supports from National Natural Science Foundation of China (Grant No. 21803044), Frontier and Applied Basic Research of Chongqing (Grant No. cstc2018jcyjAX0191), and Program for Innovation Team Building at Institutions of Higher Education in Chongqing (CXTDX201601011). Y.Z. acknowledges startup grants, Initiation Grant – Faculty Niche Research Areas (IG‐FNRA) 2020/21, and Interdisciplinary Matching Scheme 2020/21 of the Hong Kong Baptist University (HKBU).
Publisher Copyright:
© 2022 Wiley-VCH GmbH.
PY - 2022/11/4
Y1 - 2022/11/4
N2 - 0D hybrid organic–inorganic metal halides have attracted significant interest due to their unique optoelectronic properties, but attainment of efficient and stable white light emission (WLE) in such compounds remains a challenge. Here, efficient WLE via a molecular design that couples intracompound charge transfer and cluster-centered excited states in 0D halide hybrids is demonstrated. Two Cu(I) halide hybrids, K(18-crown-6)Cu2Br3 and Na4(18-crown-6)5In2Cu4Br14·8H2O, are synthesized wherein luminescent [Cu4Br6]2− clusters are isolated from each other and surrounded by 18-crown-6 coordinated alkali metal cations. In the case of K(18-crown-6)Cu2Br3, [Cu4Br6]2− clusters are only partially isolated, leading to strong orange emission with a photoluminescence quantum yield (PLQY) of 53% under UV excitation. Strikingly, to a larger extent of isolation as that, in Na4(18-crown-6)5In2Cu4Br14·8H2O as a result of the incorporation of nonemissive [InBr4]− clusters, intense white light emission with a PLQY of 97% is achieved. The dual cluster-centered states, coupled with a mixed metal-to-ligand and halide-to-ligand charge transfer state, are responsible for this bright white luminescence. This work provides new design principles for expanding the materials library for single-component, solid-state WLE.
AB - 0D hybrid organic–inorganic metal halides have attracted significant interest due to their unique optoelectronic properties, but attainment of efficient and stable white light emission (WLE) in such compounds remains a challenge. Here, efficient WLE via a molecular design that couples intracompound charge transfer and cluster-centered excited states in 0D halide hybrids is demonstrated. Two Cu(I) halide hybrids, K(18-crown-6)Cu2Br3 and Na4(18-crown-6)5In2Cu4Br14·8H2O, are synthesized wherein luminescent [Cu4Br6]2− clusters are isolated from each other and surrounded by 18-crown-6 coordinated alkali metal cations. In the case of K(18-crown-6)Cu2Br3, [Cu4Br6]2− clusters are only partially isolated, leading to strong orange emission with a photoluminescence quantum yield (PLQY) of 53% under UV excitation. Strikingly, to a larger extent of isolation as that, in Na4(18-crown-6)5In2Cu4Br14·8H2O as a result of the incorporation of nonemissive [InBr4]− clusters, intense white light emission with a PLQY of 97% is achieved. The dual cluster-centered states, coupled with a mixed metal-to-ligand and halide-to-ligand charge transfer state, are responsible for this bright white luminescence. This work provides new design principles for expanding the materials library for single-component, solid-state WLE.
KW - DFT calculation
KW - hybrid copper halide
KW - lead-free
KW - single-component white-light-emitting phosphor
KW - solid-state lighting
UR - http://www.scopus.com/inward/record.url?scp=85135508752&partnerID=8YFLogxK
UR - https://onlinelibrary.wiley.com/doi/10.1002/adom.202200944
U2 - 10.1002/adom.202200944
DO - 10.1002/adom.202200944
M3 - Journal article
AN - SCOPUS:85135508752
SN - 2195-1071
VL - 10
JO - Advanced Optical Materials
JF - Advanced Optical Materials
IS - 21
M1 - 2200944
ER -