期刊
SCIENCE CHINA-MATERIALS
卷 65, 期 6, 页码 1594-1600出版社
SCIENCE PRESS
DOI: 10.1007/s40843-021-1937-y
关键词
lead-free; 0D metal halides; photophysical mechanism; antimony halide; white-light-emitting diode
资金
- Guangxi National Science Foundation [2020GXNSFDA238004]
- Bagui Scholar Project of Guangxi Province
Zero-dimensional metal halides have unique optoelectronic properties, with a synthesized antimony-based metal halide exhibiting broadband orange emission and dual emission peaks attributed to different exciton transitions. The presence of strong anharmonic electron-phonon interaction and singlet and triplet self-trapped excitons contribute to the observed characteristics. Additionally, a stable white-light-emitting diode with high color rendering index was successfully fabricated based on the excellent emission and stability of the metal halide.
Zero-dimensional (0D) metal halides are in a blossoming status for their fascinating optoelectronic properties. Herein, an antimony-based metal halide of (C16H28N)(2)-SbCl5 (C16H28N+ = benzyltripropylammonium cations), where the isolated [SbCl5](2-) clusters are surrounded by C16H28N+ to form a 0D square-pyramidal structure, was synthesized and investigated. The (C16H28N)(2)SbCl5 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, (C16H28N)(2)SbCl5 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). Temperature-dependent Raman spectra clearly revealed the characteristics of multi-phonon coupling, demonstrating a strong anharmonic electron-phonon interaction in (C16H28N)(2)SbCl5. Temperature-dependent emission spectra and density functional theory results illustrated that the observed dual-band emission originated from singlet and triplet STEs in [SbCl5](2-) units. Combined with the efficient emission and excellent stability of (C16H28N)(2)SbCl5, a stable white-light-emitting diode with an ultra-high color rendering index of 96.6 was fabricated.
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