Current austenitic stainless steel storage reservoirs for hydrogen isotopes (e.g. deuterium and tritium) have performance and operational life-limiting interactions (e.g. embrittlement) with H-isotopes. Aluminum alloys (e.g.AA2219), alternatively, have very low H-isotope solubilities, suggesting high resistance towards aging vulnerabilities. This report summarizes the work performed during the life of the Lab Directed Research and Development in the Nuclear Weapons investment area (165724), and provides invaluable modeling and experimental insights into the interactions of H isotopes with surfaces and bulk AlCu-alloys. The modeling work establishes and builds a multi-scale framework which includes: a density functional theory informed bond-order potential for classical molecular dynamics (MD), and subsequent use of MD simulations to inform defect level dislocation dynamics models. Furthermore, low energy ion scattering and thermal desorption spectroscopy experiments are performed to validate these models and add greater physical understanding to them. ACKNOWLEDGMENTS Sandia National Laboratories is a multiprogram laboratory managed and operated by Sandia Corporation, a wholly owned subsidiary of Lockheed Martin Corporation, for the US Department of Energy's National Nuclear Security Administration under contract DE-AC04-94AL85000 (SAND2014-3909 J). This work was performed under a Laboratory Directed Research and Development (LDRD) project. The authors appreciate the valuable discussions with the reviewers. We thank Professor Wei Cai of Stanford University for his contributions to the dislocation dynamics algorithm development. Additionally, we would like to thank Dorian Balch (8254), Chris San Marchi (8367), Brian Somerday (8367), and James Foulk (8256) for thoughtful conversation in framing the outline for this project.