Pressure-driven multiple optoelectronic evolution in CsMoO3(IO3) with dual functional [MoO6] and [IO3] groups

Exploring optoelectronic functional materials has been of growing interest, due to their potential applications in information and energy storage. Pressure, as a direct way of modulating the localized groups of materials, has the potential to induce significant changes in optoelectronic properties. Herein, we adopt the pressure method to synergistically modulate the configuration of dual functional groups in CsMoO3(IO3) (i.e., lone-pair electrons [IO3] and second-order Jahn–Teller [MoO6] groups). Under pressure, CsMoO3(IO3) undergoes an isostructural phase transition, resulting in multiple optoelectronic changes of the “colorless-to-brown” piezochromism, the second harmonic generation “on-to-off” transformation, and the enhancement of the photocurrent switching ratio (× ∼10 times). First-principles calculations are also employed to explain the structure–property relationship. This work will shed light on further advancements in functional materials with multiple optoelectronic properties in extreme environments.