Education

Sc.B., 1983, Brown University
Ph.D., 1988, University of California at Berkeley

Honors and Awards

Joint Appointment with Savannah River National Laboratory, 2020; Carolina Distinguished Professor, 2018-Present; Charles H. Stone Award, ACS Carolina Piedmont Section, 2017; Breakthrough Leadership in Research Award, 2016-2017; South Carolina Governor's Award for Excellence in Scientific Research, 2016; University of South Carolina Trustee Professorship Award, 2012; Southern Chemist Award, 2011; Elected to the rank of Fellow of the American Chemical Society, 2011; South Carolina Section of the ACS Outstanding Chemist, 2010; Elected to the rank of Fellow of the AAAS, 2009; IPMI Henry J. Albert Award, 2009; President, South Carolina Academy of Science, 2006-2007; University of South Carolina Educational Foundation Award for Research in Science, Mathematics and Engineering, 2006; David W. Robinson Palmetto Professorship, 2000-present; Exxon Award in Solid State Chemistry, 1994; Paul M. Cook Career Development Professorship, 1993; Camille & Henry Dreyfus New Faculty Award, 1989.

Research Interests

Research Areas: Synthesis of new hierarchical wasteform materials for the effective immobilization of nuclear waste in persistent architectures:  Crystal growth of new oxide materials, Synthesis of new, structurally complex, scintillator materials, Investigation of optical, electronic and magnetic properties of new materials, Cooperative structure-property relationships.

Our research interests lie in the area of solid-state chemistry. The unifying theme in the research is the synthesis of novel solid-state materials and the correlation of structure with observed properties.

For over 20 years we have worked on the development of high-temperature solution crystal growth techniques that enable us to prepare single crystals of novel complex oxides. We have built upon our success in the adaptation and exploration of crystal growth methods and have synthesized hundreds of new compositions. A current focus is to develop the methodology to grow larger than millimeter-sized crystals for single crystal neutron diffraction experiments at the Spallation Neutron Source at Oak Ridge National Laboratory. We use crystal growth methods in the majority of our research projects.

We are developing new complex oxides in novel structure types that are highly luminescent and focus on complementary crystal growth approaches that are designed to create different classes of luminescent materials for solid-state lighting applications, including: a) the use of high temperature solutions to grow new complex rare earth containing oxides for solid state lighting and upconversion applications; b) the use of lower temperature hydrofluxes to create intrinsically luminescent oxides containing d0 transition elements and c) the use of fluxes stable under highly reducing conditions for the crystal growth of complex Eu²⁺ containing phosphors. These three approaches will permit the directed synthesis of oxides having specific mixed rare earth contents, and allow for the fine-tuning and synthetic control of their optical properties.

We have pioneered a new research direction, the growth of complex uranium-containing oxide and fluoride crystals for fundamental and practical reasons. In general, we utilize two complementary approaches to achieve the synthesis of new complex uranium-containing oxides and fluorides based on 1) the synthesis of polycrystalline powders having compositions predicted by radius ratio rules and 2) a materials discovery approach based on crystal growth from high-temperature solutions. The synthesis of both- small, high-quality crystals containing U(VI), U(V) and U(IV) cations for structure analyses and large, high-quality crystals for use in oriented magnetic measurements and single crystal neutron diffraction experiments is on-going.

The “Center for Hierarchical Waste Form Materials”, grew out of this uranium based research and was one of only four funded in 2016, and is the only one currently in South Carolina.  The mission of this new DOE center is to combine experiment and modeling to develop the chemistry and structure motifs needed to create hierarchical materials that effectively immobilize nuclear waste in persistent architectures.  Savannah River National Laboratory, where large amounts of nuclear waste are stored, is a member of this center.  The research plan of the center will address the disposal of waste stored at the Savannah River Site by developing the fundamental knowledge necessary to create new materials to safely sequester nuclear waste through the computationally-informed design of novel hierarchical materials, and by generating innovative chemical approaches and structure motifs through the use of advanced synthesis and characterization methods.  This center is well positioned to make a real impact in this important issue facing our nation.

The underlying theme in all areas under investigation is the desire to understand how structure and composition affect properties, which will ultimately allow us to synthesize compounds with specific structures and, consequently, specific properties.

Selected Publications

 

Breton, L. S., Klepov, V. V., zur Loye, H.-C., “Facile Oxide to Chalcogenide Conversion for Actinides using the Boron-Chalcogen Mixture Method”, DOI: 10.1021/JACS.0C06483.  J. Am. Chem. Soc., 2020, 142, 14365-14373.

 

Pace, K. A., Klepov, V. V, Deason, T. K., Smith, M. D., DiPrete, D. P., Amoroso, J. W., zur Loye, H.-C., “Expansion of the Na₃M^III(Ln/An)₆F₃₀ Series: Incorporation of Plutonium into a Highly Robust and Stable Framework”, DOI:10.1002/chem.202002774.  Chemistry a European Journal 2020, 26, 12941-12944.

 

Pace, K. A., Klepov, V. V, Christian, M. S., Morrison, G., Deason, T. K., Besmann, T. M., DiPrete, D. P., Amoroso, J. W., zur Loye, H.-C., “Targeting Complex Plutonium Oxides by Combining Crystal Chemical Reasoning with Density-Functional Theory Calculations: The Quaternary Plutonium Oxide Cs₂PuSi₆O₁₅”, DOI:10.1039/D0CC02674C.  Chem. Commun., 2020, 56, 9501-9504.

 

Ayer, G. B., Klepov, V. V., Smith, M. D., Hu, M., Yang, Z., Martin, C. R., Morrison, G., zur Loye, H.-C., “BaWO₂F₄: A Mixed Anion X-ray Scintillator with Excellent Photoluminescence Quantum Efficiency”, DOI:10.1039/D0DT02184A.  Dalton Trans., 2020, 49, 10734-10739.

 

Juillerat, C. A., Klepov, V. V., Morrison, G., Pace, K. A., zur Loye, H.-C., “Flux Crystal Growth:  A Versatile Technique to Reveal the Crystal Chemistry of Complex Uranium Oxides”, DOI:10.1039/C8DT04675A.  Dalton Trans.  2019, 48, 3162-3181.

 

Klepov, V. V., Pace, K. A., Calder, S., Felder, J. B., zur Loye, H.-C., “3d-Metal Induced Magnetic Ordering on U(IV) Atoms as a Route Toward U(IV) Magnetic Materials”, DOI:10.1021/jacs.9b00345.  J. Am. Chem. Soc., 2019, 141, 3838-3842.