Glasses consisting primarily of Ge, As, S, Se and Te (chalcogenides) constitute an important class of optical materials that can potentially enable a wide range of modern technologies including photonics, telecommunication, sensors and memory devices. However, successful compositional design of chalcogenides with optimized properties tailored for these technological applications needs formulation of accurate predictive models, which in turn requires fundamental data on the atomic structure and dynamics of these materials. This research program aims to use state-of-the-art experimental and simulation methods to study the atomic structure and to investigate dynamical phenomena in these glasses and in the liquids from which they derive. These results will be used to formulate and test models linking the microscopic structure and dynamics with the macroscopic properties, which will play key role in smart compositional engineering of these materials. Students in this research program will learn to investigate problems in the realm of "basic science" that underlies industrial applications. The use of experimental facilities at the Argonne National Laboratory (ANL) will enrich the graduate education and training experience through participation in a unique research environment and will foster intellectual exchange. This program will coordinate with the underrepresented minority-serving and K-12 outreach programs on campus to attract and recruit underrepresented graduate students and to increase the awareness of students in the science and technology of glassy materials. TECHNICAL DETAILS: This program seeks to study the structure-property relationships and to develop an atomic scale understanding of the structural mechanisms of transport and relaxation near the glass transition (Tg) in complex chalcogenide glasses in the Ge-As-S-Se-Te system. A combination of neutron/x-ray diffraction and Reverse Monte Carlo modeling will be used to obtain an unusually complete picture of the intermediate-range atomic structures of these materials for the first time. The temperature induced structural changes and the dynamics of exchange among structural species in these glasses and parent liquids will be characterized in situ with 77Se and 125Te nuclear magnetic resonance (NMR) spectroscopy at temperatures near and above Tg, and ex situ, on samples with different time-temperature histories by a combination of NMR and Raman spectroscopic techniques. These results will be used to develop predictive models, linking the atomic structure and dynamics with macroscopic physical properties, which are crucial for compositional optimization of these materials for a wide range of technological applications. This work includes significant training of graduate students in state-of-the-art spectroscopic, diffraction and simulation techniques.
