基于零维杂化锑基氯化物的可逆荧光发射转化

Reversible Emission Transformations in Zero-dimensional Hybrid Antimony Chlorides

零维有机-无机杂化金属卤化物因可调控的自陷态激子发射在发光和显示等领域具有很好的应用前景。特别是同时具有单线态和三线态激子发射双带光谱的零维金属卤化物在白光固态照明应用中极具潜力。本工作报道了两种零维杂化锑基氯化物(C_(24)H_(20)P)_(2)SbCl_(5)(Ⅰ)和(C_(24)H_(20)P)_(2)SbCl_(5)·H_(2)O·0.5DMF(Ⅱ)(C_(24)H_(20)P为四苯基膦,Ph4P)。在低能量光子(如360 nm)激发下,化合物Ⅰ和Ⅱ分别呈现出由自陷态激子发射的红色和黄色的单峰宽带光谱。此外,当用高能量光子(如310 nm)激发时,Ⅱ的光谱呈现出双带白光发射,除黄光发射带外,还出现了一个源于单线态自陷激发发射的蓝光发射带。研究表明,通过引入和去除DMF和水分子,化合物Ⅰ和Ⅱ能实现可逆转化。该研究揭示了小分子对零维杂化金属卤化物晶体结构的调控机制,从而实现单带发射和双带发射之间的转变,为设计具有小分子传感应用的零维金属卤化物奠定了研究基础。

Zero-dimensional(0D)hybrid metal halides with tunable self-trapped exciton(STE)emissions are promising for lighting and displaying applications.In particular,0D hybrid metal halides with dual-band emissions arising from singlet and triplet STEs have potentials in white-light solid-state lighting.Herein,two 0D hybrid antimony chlorides,(C_(24)H_(20)P)_(2)SbCl_(5)(Ⅰ)and(C_(24)H_(20)P)_(2)SbCl_(5)⋅H_(2)O⋅0.5DMF(Ⅱ)(C_(24)H_(20)P=tetraphenylphosphonium,Ph4P)are reported.The compoundsⅠandⅡexhibit single broadband red and yellow emissions upon low-energy(LE)photons(e.g.360 nm)excitation,respectively,arising from their triplet STEs.In addition,upon high-energy(HE)photons(e.g.310 nm)excitation,the compoundⅡshows a dual-band emission with an additional blue emission band deriving from singlet STEs,exhibiting a warm-white emission.Intriguingly,a reversible phase transformation betweenⅠandⅡis achieved through a dynamic insertion and extraction of DMF and water molecules.This work unravels the effect of small molecules on the crystalline structures and the conversion between single-and dual-band emission properties in 0D antimony halides,which could guide the design of 0D hybrid metal halides for sensor applications.