Low‐dimensional (low‐D) organic metal halide hybrids (OMHHs) have emerged as fascinating candidates for optoelectronics due to their integrated properties from both organic and inorganic components. However, for most of low‐D OMHHs, especially the zero‐D (0D) compounds, the inferior electronic coupling between organic ligands and inorganic metal halides prevents efficient charge transfer at the hybrid interfaces and thus limits their further tunability of optical and electronic properties. Here, using pressure to regulate the interfacial interactions, efficient charge transfer from organic ligands to metal halides is achieved, which leads to a near‐unity photoluminescence quantum yield (PLQY) at around 6.0 GPa in a 0D OMHH, [(C6H5)4P]2SbCl5.
- Award ID(s):
- 1709116
- NSF-PAR ID:
- 10099111
- Date Published:
- Journal Name:
- Journal of Materials Chemistry C
- Volume:
- 6
- Issue:
- 24
- ISSN:
- 2050-7526
- Page Range / eLocation ID:
- 6398 to 6405
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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Abstract Low‐dimensional (low‐D) organic metal halide hybrids (OMHHs) have emerged as fascinating candidates for optoelectronics due to their integrated properties from both organic and inorganic components. However, for most of low‐D OMHHs, especially the zero‐D (0D) compounds, the inferior electronic coupling between organic ligands and inorganic metal halides prevents efficient charge transfer at the hybrid interfaces and thus limits their further tunability of optical and electronic properties. Here, using pressure to regulate the interfacial interactions, efficient charge transfer from organic ligands to metal halides is achieved, which leads to a near‐unity photoluminescence quantum yield (PLQY) at around 6.0 GPa in a 0D OMHH, [(C6H5)4P]2SbCl5.
In situ experimental characterizations and theoretical simulations reveal that the pressure‐induced electronic coupling between the lone‐pair electrons of Sb3+and the π electrons of benzene ring (lp‐π interaction) serves as an unexpected “bridge” for the charge transfer. Our work opens a versatile strategy for the new materials design by manipulating the lp‐π interactions in organic–inorganic hybrid systems. -
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