The objective is to develop new materials for detection and identification of actinide isotopes and fission products from nuclear processing, reprocessing, and high level nuclear wastes. An experimental and computational project relevant to actinide forensic chemistry through study of actinide identification, separation and detection by engineered mesoporous materials is proposed. The focus is the interaction of actinides and fission products with engineered mesoporous materials of its kind in bringing together recent advances in bulk and interfacial sciences. The intellectual merit of the proposed study is the novel approach to actinide and fission product detection, separation and sequestration through computational nanoscience and interfacial science. The proposal brings together the expertise of nano materials chemistry (P. Yang), actinide chemistry (H. Nitsche) and relativistic quantum chemistry (K. Balasubramanian) and will culminate in a better understanding of mesoscale complexity at interfaces. The project goals include the design of: mesoporous materials and functionalized mesoporous substrates to selectively separate and identify actinides, selective chemical receptor sites on the surface of mesoporous materials that are capable of selectively separating or detecting the desired actinide element, and mesoporous materials with selectivity for the desired oxidation states of the actinides. The proposed work promises to have several broader impacts. It is interdisciplinary as it encompasses broad collaborative experimental-theory efforts that combine interfacial chemistry and the design of suitable functional receptors assisted by state-of-the-art relativistic computations. The proposal promotes the training of graduate students and postdoctoral students with interdisciplinary orientation in nuclear, materials and computational chemistry as well as university-DOE National lab interactions through educational and minority outreach efforts.