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Outstanding charge transport in molecular crystals is of great importance in modern electronics and optoelectronics. The widely adopted strategies to enhance charge transport, such as restraining intermolecular vibration, are mostly limited to organic molecules, which are nearly inoperative in 2D inorganic molecular crystals currently. In this contribution, charge transport in 2D inorganic molecular crystals is improved by integrating charge‐delocalized Se8 rings as building blocks, where the delocalized electrons on Se8 rings lift the intermolecular orbitals overlap, offering efficient charge transfer channels. Besides, α‐Se flakes composed of charge‐delocalized Se8 rings possess small exciton binding energy. Benefitting from these, α‐Se flake exhibits excellent photodetection performance with an ultrafast response rate (~5 μs) and a high detectivity of 1.08 × 1011 Jones. These findings contribute to a deeper understanding of the charge transport of 2D inorganic molecular crystals composed of electron‐delocalized inorganic molecules and pave the way for their potential application in optoelectronics. [ABSTRACT FROM AUTHOR]

Zn metal anode suffers from dendrite growth and side reactions during cycling, significantly deteriorating the lifespan of aqueous Zn metal batteries. Herein, we introduced an ultrathin and ultra‐flat Sb2O3 molecular crystal layer to stabilize Zn anode. The in situ optical and atomic force microscopes observations show that such a 10 nm Sb2O3 thin layer could ensure uniform under‐layer Zn deposition with suppressed tip growth effect, while the traditional WO3 layer undergoes an uncontrolled up‐layer Zn deposition. The superior regulation capability is attributed to the good electronic‐blocking ability and low Zn affinity of the molecular crystal layer, free of dangling bonds. Electrochemical tests exhibit Sb2O3 layer can significantly improve the cycle life of Zn anode from 72 h to 2800 h, in contrast to the 900 h of much thicker WO3 even in 100 nm. This research opens up the application of inorganic molecular crystals as the interfacial layer of Zn anode. [ABSTRACT FROM AUTHOR]

The unique intermolecular van der Waals force in emerging two‐dimensional inorganic molecular crystals (2DIMCs) endows them with highly tunable structures and properties upon applying external stimuli. Using high pressure to modulate the intermolecular bonding, here we reveal the highly tunable charge transport behavior in 2DIMCs for the first time, from an insulator to a semiconductor. As pressure increases, 2D α‐Sb2O3 molecular crystal undergoes three isostructural transitions, and the intermolecular bonding enhances gradually, which results in a considerably decreased band gap by 25 % and a greatly enhanced charge transport. Impressively, the in situ resistivity measurement of the α‐Sb2O3 flake shows a sharp drop by 5 orders of magnitude in 0–3.2 GPa. This work sheds new light on the manipulation of charge transport in 2DIMCs and is of great significance for promoting the fundamental understanding and potential applications of 2DIMCs in advanced modern technologies. [ABSTRACT FROM AUTHOR]