Achieving multifunctional optimization of halide optical materials through the precise modulation of intermolecular interactions is highly significant,yet it faces considerable challenges.Here,we propose a strategy of...Achieving multifunctional optimization of halide optical materials through the precise modulation of intermolecular interactions is highly significant,yet it faces considerable challenges.Here,we propose a strategy of π–π interactions microregulating to achieve the simultaneous optimization of multiple properties of halide optical materials.Using this strategy,we obtained a new lead-free zero-dimensional(0D)zinc halide[DPE]ZnCl_(4)(DPE=1,2-di(4-pyridyl)ethylene),in which the protonated DPE cations are orderly arranged via π–π interactions,facilitating the ordered embedding and local regulation of[ZnCl_(4)]^(2−) units within long-range one-dimensional cationic π–π stacking.As a result of these modifications,[DPE]ZnCl_(4) exhibits efficient blue light emission with a high photoluminescent quantum yield(PLQY)of 18.55%,far exceeding that of corresponding organic salt halides.Furthermore,this compound demonstrates an enhanced third-order nonlinear optical(NLO)response,with the modulation depth and the third-order NLO absorption coefficient reaching 0.70 and 3.81×10^(−10) m W^(−1),respectively,surpassing those of three-dimensional(3D)perovskite quantum dots and most organic–inorganic hybrid halides.Notably,the modulation of π–π interactions results in a significant breakthrough in water resistance,allowing[DPE]ZnCl_(4) to maintain excellent structural and performance stability in water for a week.This innovative strategy of π–π interaction modulation provides new avenues for the multifunctional regulation and waterproof design of halide optical materials,and it is expected to advance the development and functionalization of stable halide optical materials.展开更多
基金supported by the National Natural Science Foundation of China(22301317)Key Scientific and Technological Project of Henan Province(232102310376,232102311181 and 242102110035)+1 种基金the Specialized Research Fund for the Doctoral Program of Zhoukou Normal University(ZKNUC2021021)the University Student Scientific Research Innovation Foundation of Zhoukou Normal University(ZKNUD2024085).
文摘Achieving multifunctional optimization of halide optical materials through the precise modulation of intermolecular interactions is highly significant,yet it faces considerable challenges.Here,we propose a strategy of π–π interactions microregulating to achieve the simultaneous optimization of multiple properties of halide optical materials.Using this strategy,we obtained a new lead-free zero-dimensional(0D)zinc halide[DPE]ZnCl_(4)(DPE=1,2-di(4-pyridyl)ethylene),in which the protonated DPE cations are orderly arranged via π–π interactions,facilitating the ordered embedding and local regulation of[ZnCl_(4)]^(2−) units within long-range one-dimensional cationic π–π stacking.As a result of these modifications,[DPE]ZnCl_(4) exhibits efficient blue light emission with a high photoluminescent quantum yield(PLQY)of 18.55%,far exceeding that of corresponding organic salt halides.Furthermore,this compound demonstrates an enhanced third-order nonlinear optical(NLO)response,with the modulation depth and the third-order NLO absorption coefficient reaching 0.70 and 3.81×10^(−10) m W^(−1),respectively,surpassing those of three-dimensional(3D)perovskite quantum dots and most organic–inorganic hybrid halides.Notably,the modulation of π–π interactions results in a significant breakthrough in water resistance,allowing[DPE]ZnCl_(4) to maintain excellent structural and performance stability in water for a week.This innovative strategy of π–π interaction modulation provides new avenues for the multifunctional regulation and waterproof design of halide optical materials,and it is expected to advance the development and functionalization of stable halide optical materials.
