Isothermal pressure-derived metastable states in 2D hybrid perovskites showing enduring bandgap narrowing

Materials in metastable states, such as amorphous ice and supercooled condensed matter, often exhibit exotic phenomena. To date, achieving metastability is usually accomplished by rapid quenching through a thermodynamic path function, namely, heating-cooling cycles. However, heat can be detrimental to organic-containing materials because it can induce degradation. Alternatively, the application of pressure can be used to achieve metastable states that are inaccessible via heating-cooling cycles. Here we report metastable states of 2D organic-inorganic hybrid perovskites reached through structural amorphization under compression followed by recrystallization via decompression. Remarkably, such pressure-derived metastable states in 2D hybrid perovskites exhibit enduring bandgap narrowing by as much as 8.2% with stability under ambient conditions. The achieved metastable states in 2D hybrid perovskites via compression-decompression cycles offer an alternative pathway toward manipulating the properties of these soft materials.