Measuring Local Atomic Structure Variations through the Depth of Ultrathin (<20 nm) ALD Aluminum Oxide: Implications for Lithium-Ion Batteries

Understanding the atomic structure of ultrathin (x film deposited onto a carbon nanotube (CNT) substrate without a contribution from the substrate. We couple these diffraction measurements with pair distribution function (PDF) analysis and iterative reverse Monte Carlo-molecular statics (RMC-MS) modeling to compare atomic structure metrics at different positions in the film depth. We interpret the modeling results considering the three-dimensional (3D) concentric cylindrical sample geometry of a CNT with uniform AlOx coating. These measurements confirm a two-phase bulk/interface structural model proposed previously for ALD AlOx and indicate that the interfacial layer at the CNT–AlOx interface is 2.5 nm thick5 times larger than previously reported. This report demonstrates direct measurement of atomic structural variations across nanoscale material interfaces that is of broad interest for electrochemical applications and will help inform the use of ALD coatings to stabilize lithium-ion battery interfaces.