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Zero-dimensional heterometallic halide hybrids have emerged as multifunctional emitters, due to their multiple emission features. Herein, high pressure is employed to regulate the multiple emissions of (C9NH20)9[Pb3Br11](MnBr4)2. Pressure-triggered rigidness of [Pb3Br11]5- alters the emission equilibrium of STEs, generating a new blue-shifted STE emission. Meanwhile, [MnBr4]2- contraction promotes the confinement effect to increase the 4D-6A1 transition efficiency. Notably, [Pb3Br11]5- could act as ‘antenna' to enhance the Mn2+ emission with blocked back-energy transfer. It indicates that enough incident energy could excite the STE emission and 4D-6A1 transitions simultaneously, which clarifies the conventional understanding of the emission origin at ambient conditions.

Zero-dimensional heterometallic halide hybrids have emerged as multifunctional emitters, due to their multiple emission features. Herein, high pressure is employed to regulate the multiple emissions of (C9NH20)9[Pb3Br11](MnBr4)2. Pressure-triggered rigidness of [Pb3Br11]5- alters the emission equilibrium of STEs, generating a new blue-shifted STE emission. Meanwhile, [MnBr4]2- contraction promotes the confinement effect to increase the 4D-6A1 transition efficiency. Notably, [Pb3Br11]5- could act as 'antenna' to enhance the Mn2+ emission with blocked back-energy transfer. It indicates that enough incident energy could excite the STE emission and 4D-6A1 transitions simultaneously, which clarifies the conventional understanding of the emission origin at ambient conditions. In zero-dimensional metal halide of (C9NH20)9[Pb3Br11](MnBr4)2, the [Pb3Br11]5- trimer acts as 'antenna' to enhance the [MnBr4]2- emission at high pressure, resolving distinct photoluminescent contributions of individual metal-halogen fragments. [ABSTRACT FROM AUTHOR]