Prediction of High‐Temperature Superconductivity in Monolayer h‐AlH2$\left(\text{AlH}\right)_{2}$ at Ambient Pressure

Although hydrides such as have been experimentally confirmed to possess high superconducting critical temperature () of 250‐260 K under 170‐200 GPa, it is still a tough challenge to be applied. It is highly anticipated to find hydride superconductors with relatively high at low or ambient pressure. Reducing the dimensionality of materials can induce unexpected properties that are distinct from their bulk counterparts, whether it can modulate the superconducting properties deserves further investigation. Here, we theoretically predict a new two‐dimensional (2D) monolayer aluminum hydride h‐ under ambient pressure based on the first‐principles calculations. Since the electronic structures of h‐ reveal the metallicity, the electron‐phonon coupling (EPC) and possible phonon‐mediated superconductivity have been investigated. Based on the isotropic Eliashberg equation, the calculated EPC constant λ of h‐ is 1.16, and the is up to 42.6 K. The EPC mainly originates from the coupling between electrons of Al‐s,,, and H‐s orbitals and the in‐plane vibration modes of H atoms. Especially, the can be enhanced to 63.7 K by applying 3% biaxial tensile strain. Thus, the predicted h‐ provides a new platform for finding hydride superconductors in low‐dimensional materials at ambient pressure.This article is protected by copyright. All rights reserved.