Mechanoluminescence (ML) has received widespread attention because of potential application in stress sensors and imaging. However, pursuing highly efficient ML remains a challenge due to multifactorial limitations such as pressure and loading rate. Here, we systematically investigate pressure-and ratedependent ML in Mn 2+ and Eu 3+ co-doped ZnS in a gigapascal pressure range by using a high-pressure dynamic diamond anvil cell and microsecond time-resolved fluorescent methods and demonstrate the giant tunability in both ML efficiency and wavelength. Compressed from ambient pressure to 11 GPa at different compression rates, ZnS: Mn 2+ , Eu 3+ exhibits a volcano shape in ML emission efficiency with an optimum at ∼3.5 GPa and ∼211.1 GPa/s, at least 1000-fold higher than that measured in the MPa range. The pressure-dependent ML is accompanied with a tunable yellow-to-red emission color change. A combination of high-pressure X-ray diffraction and photoluminescence measurements reveals that the pressure-and ratedependent ML behavior derives from pressure-induced strengthening of the crystal piezoelectric field and enhanced interaction between the host lattice and doped ions with a significant change of the energy level of the Mn ion. Significantly, the highly efficient ML of ZnS: Mn 2+ , Eu 3+ at the GPa level is reproducible under a compression-decompression process and can be manipulated on a micron scale, implying great potential in mechanical-optical energy conversion and application in dynamic pressure imaging, stress sensors, and multicolor displays.

Organic–inorganic halide perovskites possess flexible structures with tunable optical properties at high pressures, but the pressure-induced amorphization limits the understanding and exploration of the structure–property relationships. Herein, we report an edge-shared octahedral MAPbBr3 via multiple-stage transformation of the traditional corner-shared three-dimensional perovskites at high-pressure and high-temperature (P–T) conditions. In situ synchrotron X-ray diffraction reveals that upon heating at 8.7 GPa, the amorphized MAPbBr3 transforms into a high P–T structure above 654 K via multiple-stage crystallization. The high P–T phase is determined to be a monoclinic P2/m structure with layered edge-shared Pb–Br octahedra, which can be quenched to RT at high pressures but converts back to the initial cubic perovskite structure below 0.7 GPa under decompression. The Raman and optical measurements demonstrate that the high P–T phase has similar vibrational behavior and tunable optical properties to those of the pressure-induced amorphous phase, indicating the similarity in the local structure with the edge-shared PbBr6 octahedral frame and the MA organic cations between the high P–T phase and the amorphous state. The present results demonstrate the structural diversity and interconversion in MAPbBr3 by overcoming the large kinetic barrier derived from the anisotropic organic cations and disordering arrangement of the Pb–Br octahedra, providing new insights into the understanding of structural transitions and amorphization of halide perovskites.