Co-Leads: Jon-Paul Maria & Adri van Duin [NEW]
Description
Crystals with high configurational entropy, engineered through chemical formulation, exhibit unique composition-structure-property combinations that are absent when chemical order prevails. These high-entropy materials follow unexpected crystal chemistry rules and hold promise for new functional properties. IRG2 endeavors to identify and understand these rules through an integrative effort linking theory, synthesis, characterization, and computation. The hypothesis driving this research is that high configurational entropy leads to high solubility for atoms in “misfit” local environments, which produces a spectrum of local energies and disordered geometries that collectively generate new macroscopic responses. The IRG seeks to understand how local structures relate to specific formulations and how short-range disorder couples over longer length scales. With this understanding, we will uncover the predictive rules for high-entropy crystal chemistry.
IRG2 is organized into four interwoven thrusts. Three of these are property-driven and endeavor to understand:
- How electronic and ionic transport can be maximized in high-entropy perovskites and fluorites
- How local distortions can influence global symmetry and polar ordering in high-entropy perovskites with disorder on both cation sublattices
- How electron correlation and magnetism manifest in high-entropy rock salts and pyrochlores.
In each case we explore the limits of misfit cations in a parent high-symmetry structure, where the misfits are chosen so as to influence property evolution. An overarching multiscale theory and modeling effort couples to machine learning to predict structure, defect chemistry, and properties in all materials of interest. At small length scales first-principles calculations model and predict the entire landscape of local distortions in particular formulations and link them to local properties such as ion migration barrier, defect formation energy, band structure, and polarizability. First-principles data feeds phase-field and stochastic models at higher length scales to connect formulation, local structure, electronic structure, and crystal structure to cooperative responses, and microstructures.
Featured Publications
Saugata Sarker, Yu Wang, Yongwen Sun, Caeli Benyacko, Saeed S.I. Almishal, Tao Zhou, Zhiyu Zhang, Jadupati Nag, Himirkanti Sarkar, Jeffrey Shallenberger, Hemant Yennawar, Yang Yang, Jon-Paul Maria, Zhiqiang Mao, and Venkatraman Gopalan. High Entropy Wide-Bandgap Borates with Broadband Luminescence and Large Nonlinear Optical properties. Adv. Functional Mat. 2026, e25925. DOI: 10.1002/adfm.202525925
Saeed S. I. Almishal, Pat Kezer, Jacob T. Sivak, Yasuyuki Iwabuchi, Sai Venkata Gayathri Ayyagari, Saugata Sarker, Matthew Furst, Gerald Bejger, Billy Yang, Simon Gelin, Nasim Alem, Ismaila Dabo, Christina M. Rost, Susan B. Sinnott, Vincent Crespi, Venkatraman Gopalan, Roman Engel-Herbert, John T. Heron, and Jon-Paul Maria. Chemically-Disordered Transparent Conductive Perovskites With High Crystalline Fidelity. Science Advances. 2025, 12, 42. DOI: 10.1002/advs.202509868
Gerald R. Bejger, Mary Kathleen Caucci, Saeed S. I. Almishal, Billy Yang, Jon-Paul Maria, Susan B. Sinnott, and Christina M. Rost. Lanthanide L-edge spectroscopy of high-entropy oxides: insights into valence and phase stability. J. Mater. Chem. A. 2025, 13, 29060-29069. DOI: 10.1039/D5TA03815D
Saeed S. I. Almishal, Matthew Furst, Yueze Tan, Jacob T. Sivak, Gerald Bejger, Joseph Petruska, Sai Venkata Gayathri Ayyagari, Dhiya Srikanth, Nasim Alem, Christina M. Rost, Susan B. Sinnott, Long-Qing Chen, and Jon-Paul Maria. Thermodynamics-inspired high-entropy oxide synthesis. Nature Communications, 2025, 16, 8211. DOI: 10.1038/s41467-025-63567-z
Saeed S.I. Almishal, Jacob T. Sivak, George N. Kotsonis, Yueze Tan, Matthew Furst, Dhiya Srikanth, Vincent H. Crespi, Venkatraman Gopalan, John T. Heron, Long-Qing Chen, Christina M. Rost, Susan B. Sinnott, Jon-Paul Maria. Untangling individual cation roles in rock salt high-entropy oxides. Acta Materialia, 279, 2024. DOI: 10.1016/j.actamat.2024.120289
Sangmin Yoo, Sieun Chae, Tony Chiang, Matthew Webb, Tao Ma, Hanjong Paik, Yongmo Park, Logan Williams, Kazuki Nomoto, Huili G. Xing, Susan Trolier-McKinstry, Emmanouil Kioupakis, John T. Heron, Wei D. Lu. Efficient data processing using tunable entropy-stabilized oxide memristors. Nat. Electron. 2024 DOI: 10.1038/s41928-024-01169-1
Acknowledgements
Publications that report work supported by the MRSEC should include an acknowledgement in the form "ABC and XYZ acknowledge support from the Penn State Materials Research Science and Engineering Center Center for Nanoscale Science under National Science Foundation award DMR-2011839." If all co-authors performed their work under MRSEC support, then the ABC/XYZ initials can be omitted. Work produced using MRSEC facilities should include an acknowledgement thereof as described on the facilities pages.