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Low-dimensional metal halide compounds, usually described as low-dimensional perovskites, present exciting properties as functional materials for a broad range of optoelectronic applications. These compounds are characterized by intense photoluminescence (PL), a narrow emission line width, and a high exciton binding energy. In particular, the mechanism behind the strong green emission of the zero-dimensional compound Cs 4 PbBr 6 has been the subject of intense debate. As a propertytuning tool, hydrostatic pressure was used to investigate the structural and optical properties of bulk Cs 4 PbBr 6 through synchrotron X-ray diffraction combined with Raman and PL spectroscopies. As a result, two structural phase transitions at 3.2 and 4.6 GPa were identified, with the latter not observed in previous investigations performed on nanocrystals. Also, the pressure dependence of the PL emission was recorded and compared with the previous results on Cs 4 PbBr 6 and CsPbBr 3 nanocrystals. Under the ambient conditions, strong green emission exhibits a subtle redshift, followed by a blueshift under pressure, being associated first with an intensity enhancement and subsequent quenching above 3 GPa. These results support the CsPbBr 3 luminescent inclusions as the PL emission mechanism in Cs 4 PbBr 6 .

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