ABSTRACT As an important category of smart materials, light‐responsive metal‐organic materials, including photochromic materials, room‐temperature phosphorescent materials, and others, leverage optical signals to achieve the emergence, synergy, and integration of material properties. They offer advantages such as remote controllability and rapid response, demonstrating significant research value in fields like high‐density data storage, recognition and sensing, and intelligent response systems. However, key scientific challenges remain to be overcome, including the rational design and directional assembly strategies for novel target materials, elucidation of electron transfer (ET) and transition mechanisms during photoresponse processes, understanding the evolution of electronic structures and molecular configurations, and achieving precise regulation of light‐responsive functionalities. This review summarizes recent advances in the molecular design, assembly strategies, and structure‐dependent photoresponse properties of ET‐driven crystalline hybrid photochromic materials (CHPMs). The first section provides a brief discussion of CHPMs and the design principles based on ET strategies. Subsequent sections outline CHPMs exhibiting photomagnetic effects, room‐temperature phosphorescence (RTP), adsorption and separation properties, and x‐ray scintillator behaviors. Finally, conclusions and perspectives on CHPMs with specific light‐responsive functionalities are presented. These trends are expected to play a pivotal role in advancing the design and application of CHPMs and light‐responsive materials in general.
Chen et al. (Sat,) studied this question.