The chemical carrier doping of molecular Mott insulators has been poorly investigated to date due to its difficulty. In this study, iodine doping of a molecular Mott insulator, lithium phthalocyanine crystallized in the x‐form (x‐LiPc), was performed to obtain metallic x‐LiPcI. Crystal structure analysis revealed that iodine atoms penetrated channels of x‐LiPc and formed one‐dimensional chains. The Raman spectroscopy of x‐LiPcI indicated the existence of linear I5−, demonstrating a transition from a half‐filled band of the Mott insulating state to a 2/5‐filled band of the metallic state. Electrical resistivity measurements confirmed the metallic nature of x‐LiPcI, whereas a thermally activated behavior was observed for pristine x‐LiPc. Furthermore, the x‐LiPc Mott insulator was reproduced by dedoping iodine from x‐LiPcI, suggesting that the electronic state can be reversibly tuned between the Mott insulating and metallic states by chemical doping and dedoping.

The chemical carrier doping of molecular Mott insulators has been poorly investigated to date due to its difficulty. In this study, iodine doping of a molecular Mott insulator, lithium phthalocyanine crystallized in the x‐form (x‐LiPc), was performed to obtain metallic x‐LiPcI. Crystal structure analysis revealed that iodine atoms penetrated channels of x‐LiPc and formed one‐dimensional chains. The Raman spectroscopy of x‐LiPcI indicated the existence of linear I5−, demonstrating a transition from a half‐filled band of the Mott insulating state to a 2/5‐filled band of the metallic state. Electrical resistivity measurements confirmed the metallic nature of x‐LiPcI, whereas a thermally activated behavior was observed for pristine x‐LiPc. Furthermore, the x‐LiPc Mott insulator was reproduced by dedoping iodine from x‐LiPcI, suggesting that the electronic state can be reversibly tuned between the Mott insulating and metallic states by chemical doping and dedoping.

Leitfähige Materialien. In ihrer Zuschrift (e202206428) berichten Masaki Matsuda et al. über einen reversiblen Isolator‐Metall‐Übergang durch chemische Dotierung und Dedotierung eines Mott‐Isolators. Die Ergebnisse weisen den Weg zu einer neuen Klasse stark korrelierter Materialien.

Conducting Materials. In their Communication (e202206428), Masaki Matsuda et al. report a reversible insulator–metal transition by chemical doping and dedoping of a Mott insulator. The results could lead to a new class of strongly correlated materials.