Rare Earth Elements and Actinides Progress in Computational Science Applications

Advances and challenges in nuclear and radiochemistry

Rare earth elements (REEs) and actinides are critical to electronics, communication, military applications, and green energy systems. They also play a large role in nuclear waste challenges with critical national importance. Actinides are still among some of the least studied elements in the periodic table, due to their short half-lives and radioactivity, which demand expert facilities for research. Computational modeling greatly aids in understanding REEs and actinides; however, electronic structure modeling of these elements presents limitations. High Performance Computing (HPC) has had a direct impact not only on technical advances and access to information on a global scale but also on investigations of REEs and actinides. This work discusses recent advances in molecular and data driven modeling that are essential to the study of REEs and actinides, effects of computational science in nuclear and radiochemical applications, and advances and challenges in the exascale era of supercomputing.

Dr. Deborah Penchoff is the Associate Director of the Innovative Computing Laboratory (ICL) at the University of Tennessee (UTK) and holds a faculty appointment in the UTK Department of Nuclear Engineering. She is a fellow of the Howard H. Baker Jr. Center for Public Policy and a cochair of the Diversity, Equity, and Inclusion Action Committee (DEIAC) in the UTK Department of Nuclear Engineering. Prior to these roles, she was a scientist at the Radiochemistry Center of Excellence and at the Institute for Nuclear Security, where she directed and managed the Scientific Fellows Program. She in an expert in applying high-performance computing (HPC) and data science for national security applications with focus on bonding and reactivity of Rare Earth Elements (REEs) and actinides. Her research focuses on computational science, including development of protocols for efficient utilization of HPC resources, data science, data analytics, machine learning, and molecular computational modeling.
These have been applied across a wide range of interdisciplinary research fields, such as critical materials and shortage of REEs, radiotherapy for cancer treatment, predictive capabilities for epidemiology, selective separations, sequestration of uranium from seawater, radiochemistry, nuclear forensics, and nuclear waste.
Dr. Penchoff obtained a PhD in Physical Chemistry with an Interdisciplinary Graduate Minor in Computational Sciences (IGMCS) at UTK while pursuing her research at the Oak Ridge National Laboratory and UTK Joint Institute for Computational Sciences (JICS). Dr. Penchoff is the chair of the Computational Science Applications for REEs and Actinides session and chair of the Data Science and Artificial Intelligence in Nuclear and Radiochemistry session in the American Chemical Society (ACS) Division of Nuclear Chemistry and Technology (ACS-NUCL). She is also the newly Elected Member-at-Large of the ACS-NUCL Executive Committee. Dr. Penchoff is also an XSEDE Campus Champion and a co-organizer of the Radiobioassay and Radiochemical Measurements Conference. While at UTK, Dr. Penchoff has been the recipient of multiple awards including a Faculty Service Award in the Department of Nuclear Engineering, an Outstanding Teaching Award from the ACS Student Affiliates, and an Outstanding Teaching Award
from the Department of Chemistry. Prior to her career in science, Dr. Penchoff was a financial analyst at IBM.

Dr. Theresa Windus is a Distinguished Professor and Liberal Arts and Sciences Dean's Professor in the Department of Chemistry at Iowa State University and a scientist at the Department of Energy's Ames Laboratory where she is a member of the Critical Materials Institute. She is also a Co-Director and Deputy Director for the Molecular Sciences Software Institute (MolSSI), the Director for the DOE NWChemEx Exascale Computing Project, and a former Co-Chair for the DOE Review of Exascale Computational and Data Requirements for Basic Energy Sciences. Prior to her position at Iowa State University, Dr. Windus was a Senior Scientist and Technical Group Lead at Pacific Northwest National Laboratory (PNNL) where she led a multidisciplinary team focusing on enabling computational resources for users at PNNL. There she also served as the technical group lead for the Molecular Sciences Software Group and led the development of NWChem - a leading worldwide software. Dr. Windus' current research
interests are rare earth and heavy element chemistry, catalysis, aerosol formation, cellulose degradation, photochemistry, and design and development of efficient and novel massively parallel chemistry algorithms. She is an elected Councilor for the PHYS division of the American Chemical Society (ACS), serves on the Chemists with Disabilities Committee (ACS), is a Fellow of the ACS and of the American Association for the Advancement of Science, and has won multiple awards for her teaching and research.

Dr. Charles Peterson is a scientist and HPC administrator at the Office of Advance Research Computing at the University of California, Los Angeles (UCLA). In this role, he enables computational research through consulting and collaboration in addition to training faculty, staff, and students to utilize UCLA's advance computing capabilities. Dr. Peterson is also an interdisciplinary researcher, collaborator and information technology professional with expertise in scientific computing and computational research applications across physics, chemistry, and material science. Prior to his work at UCLA, Dr. Peterson was instrumental in creating an advanced high-performance computing (HPC) network that enhanced research for many scientific groups at the North Texas Scientific Computing Center located at the University of North Texas (UNT). He is an active researcher in the development of computational methods for modeling and simulation of chemical properties of lanthanide and actinide
containing compounds. His collaborations with the Institute for Nuclear Security and the Howard H. Baker Jr. Center for Public Policy led to research development in thermochemical and spectroscopic properties of heavy element systems for nuclear forensics, separation chemistry, and other applications in national security.

Preface

Part I: Rare Earth Elements and Actinides: History and Global Challenges
Chapter 1: An Introduction to High Performance Computing and Its Intersection with Advances in Modeling Rare Earth Elements and Actinides, Deborah A. Penchoff, Edward Valeev, Heike Jagode, Piotr Luszczek, Anthony Danalis, George Bosilca, Robert J. Harrison, Jack Dongarra, and Theresa L. Windus
Chapter 2: The Periodic Table and the f Elements, Ana de Bettencourt-Dias
Chapter 3: Rare Earth Elements and Critical Materials: Uses and Availability, Deborah A. Penchoff, Charles B. Sims, and Theresa L. Windus
Chapter 4: A Brief Overview of Radiochemistry, Kenneth G. W. Inn, Julie G. Ezold, Ashleigh Kimberlin, Paul Benny, J. D. Auxier, Lætitia H. Delmau, and James L. E. Burn
Chapter 5: A Brief on Nuclear Waste at the Hanford Site and a Computational Analysis of Uranyl Nitrate with and without Tributyl Phosphate, Huei Meznarich and Deborah A. Penchoff

Part II: Advances in Supercomputing and Methods Development
Chapter 6: Computational Image Techniques for Analyzing Lanthanide and Actinide Morphology, Cody A. Nizinski, Cuong Ly, Luther W. McDonald, and Tolga Tasdizen
Chapter 7: Advances in Structure Prediction of Lanthanides and Actinides with Genetic Algorithms, Ashley E. Shields
Chapter 8: Opportunities for Computational Development in Laser Induced Breakdown Spectroscopy (LIBS), Jessica L. Bishop
Chapter 9: Computation of Vibrational Excitations in XPS Spectroscopy, Paul S. Bagus and Connie J. Nelin
Chapter 10: On the Finite Nuclear Effect and Gaussian Basis Sets for Four-Component Dirac Hartree--Fock Calculations, Shichao Sun, Torin F. Stetina, Tianyuan Zhang, and Xiaosong Li
Chapter 11: Tailored Computational Approaches to Interrogate Heavy Element Chemistry and Structure in Condensed Phase, Manh-Thuong Nguyen, Jun Zhang, David C. Cantu, Roger Rousseau, and Vassiliki-Alexandra Glezakou

Part III: Applications in Surface Science, Ligand Design, Binding Analysis, and Covalency
Chapter 12: Essential Aspects of Solvent Effects and Solution Conditions upon the Modeling and Simulation of Lanthanide and Actinide Complexes, Nitesh Kumar, Biswajit Sadhu, and Aurora E. Clark
Chapter 13: Targeted Alpha Therapy, Tara Mastren
Chapter 14: Electronic Structure and Spectroscopy of f-Element Tris(cyclopentadienyl) Complexes, Jing Su, Enrique R. Batista, and Ping Yang
Chapter 15: Development of an Open Source Tool for Basis Set Optimizations and Application to the Development of a Quadruple-Z Segmented Basis Set for Actinium, George Schoendorff
Chapter 16: Computational Modeling of Diphosphine Oxide and Diglycolamide Ligand Complexation to Lanthanides and Extraction from Acidic Media, David Poole, Federico Zahariev,Michael Del Viscio,Mark S. Gordon, Theresa L.Windus, and Marilu Perez Garcia
Chapter 17: Molecular Dynamics Simulations of U(III) and U(IV) in Molten Chlorides, Bo Li, Sheng Dai, and De-en Jiang

Editors' Biographies
Author Index
Subject Index