Zero-dimensional(0D)metal halides are in a blossoming status for their fascinating optoelectronic properties.Herein,an antimony-based metal halide of(C_(16)H_(28)N)_(2)SbCl_(5)(C_(16)H_(28)N^(+)=benzyltripropylammoniu...Zero-dimensional(0D)metal halides are in a blossoming status for their fascinating optoelectronic properties.Herein,an antimony-based metal halide of(C_(16)H_(28)N)_(2)SbCl_(5)(C_(16)H_(28)N^(+)=benzyltripropylammonium cations),where the isolated[SbCl_(5)]_(2)−clusters are surrounded by C_(16)H_(28)N^(+)to form a 0D square-pyramidal structure,was synthesized and investigated.The(C_(16)H_(28)N)_(2)SbCl_(5)exhibited a broadband orange emission at 633 nm upon the low-energy irradiation(400 nm)with a near-unity photoluminescence quantum efficiency(97.8%).Interestingly,(C_(16)H_(28)N)_(2)SbCl_(5)showed an additional emission peak at 477 nm upon the higher-energy irradiation(300 nm),which is attributed to the transformation of the doublet of spin-orbit couplings into two independent self-trapped excitons(STEs).Temperaturedependent Raman spectra clearly revealed the characteristics of multi-phonon coupling,demonstrating a strong anharmonic electron-phonon interaction in(C_(16)H_(28)N)_(2)SbCl_(5).Temperature-dependent emission spectra and density functional theory results illustrated that the observed dual-band emission originated from singlet and triplet STEs in[SbCl_(5)]_(2)−units.Combined with the efficient emission and excellent stability of(C_(16)H_(28)N)_(2)SbCl_(5),a stable white-light-emitting diode with an ultra-high color rendering index of 96.6 was fabricated.展开更多
基金financially supported by Guangxi National Science Foundation project(2020GXNSFDA238004)the Bagui Scholar Project of Guangxi Province。
文摘Zero-dimensional(0D)metal halides are in a blossoming status for their fascinating optoelectronic properties.Herein,an antimony-based metal halide of(C_(16)H_(28)N)_(2)SbCl_(5)(C_(16)H_(28)N^(+)=benzyltripropylammonium cations),where the isolated[SbCl_(5)]_(2)−clusters are surrounded by C_(16)H_(28)N^(+)to form a 0D square-pyramidal structure,was synthesized and investigated.The(C_(16)H_(28)N)_(2)SbCl_(5)exhibited a broadband orange emission at 633 nm upon the low-energy irradiation(400 nm)with a near-unity photoluminescence quantum efficiency(97.8%).Interestingly,(C_(16)H_(28)N)_(2)SbCl_(5)showed an additional emission peak at 477 nm upon the higher-energy irradiation(300 nm),which is attributed to the transformation of the doublet of spin-orbit couplings into two independent self-trapped excitons(STEs).Temperaturedependent Raman spectra clearly revealed the characteristics of multi-phonon coupling,demonstrating a strong anharmonic electron-phonon interaction in(C_(16)H_(28)N)_(2)SbCl_(5).Temperature-dependent emission spectra and density functional theory results illustrated that the observed dual-band emission originated from singlet and triplet STEs in[SbCl_(5)]_(2)−units.Combined with the efficient emission and excellent stability of(C_(16)H_(28)N)_(2)SbCl_(5),a stable white-light-emitting diode with an ultra-high color rendering index of 96.6 was fabricated.
