Increasing energy needs demand radical improvement in energy storage technology. A robust molecular-level understanding of interfacial electrochemical processes will enable discoveries of fundamentally new concepts and advanced energy systems, such as the state-of-the-art lithium ion batteries. Lithium manganese oxide (LMO) with spinel structure is an excellent platform for studying fundamental electrochemical processes at the cathode surface. Atomic layer deposition (ALD) is a thin film technique with the capability of molecular-thickness control and conformality to substrate shape.  Thus, ALD of LMO and subsequent ALD of ultrathin protective coatings on the LMO will facilitate detailed interfacial studies, offering great insight into the molecular-level understanding. LMO has already been successfully deposited by ALD and the ratio of lithium content in LMO can be precisely controlled by adjusting the Li₂O:MnO₂ ALD cycle ratio.