Zipper‐Like Dynamic Switching of Coordination Bonds Gives a Polar Bimetallic Halide toward Self‐Driven X‐ray Detection

Polar molecular crystals hold a promise for controlling bulk physical properties originated in their unique switchable polarity via structural transformation. However, the mechanisms for switching polarization are mainly limited to displacive and disorder-order phase transitions, which rarely involve the reconstruction of chemical bonds. Here, we have switched and tuned electric polarization in a bimetallic halide, (Neopentylammonium)