Kinetically Stabilized 4 f –5 d Pyrochlore Thin Films: A Route to Magnetic Fragmentation
Abstract Magnetic fragmentation in 4f–5d pyrochlores, such as Ho2Ir2O7, offers a route to monopole-driven physics, but translating this physics into thin-film form remains a severe synthesis problem. The challenge is to crystallize the pyrochlore phase by creating a metastable precursor that preserves iridium chemistry within a narrow kinetic window. Here we identify plume thermalization as the key synthesis variable that controls this metastable pathway. In pulsed-laser deposition followed by in situ solid-phase epitaxy (SPE), xenon, the heaviest stable noble gas, mass-selectively governs plume kinetics and produces an atomically flat metastable amorphous precursor with uniform Ho/Ir chemistry. Structural probes and X-ray photoelectron spectroscopy confirm that this precursor retains local pyrochlore connectivity without long-range translational order. The SPE-stabilized crystalline films are single-phase, [111]-oriented, electrically conductive, and magnetically active. Mass-selective plume control can open the narrow kinetic window required to synthesize and explore new magnetic pyrochlore materials.
Authors
- M. Moretti Sala (ORCID: https://orcid.org/0000-0002-9744-9976)
- Hongze Li (ORCID: https://orcid.org/0000-0002-3017-383X)
- Jianshi Zhou (ORCID: https://orcid.org/0000-0002-7667-5640)
- Jak Chakhalian (ORCID: https://orcid.org/0000-0001-8168-9441)
- Jiayun Pei (ORCID: https://orcid.org/0000-0002-4366-9658)
- M. Kareev (ORCID: https://orcid.org/0009-0001-8838-5608)
- Christoph J. Sahle (ORCID: https://orcid.org/0000-0001-8645-3163)
- Michael Terilli (ORCID: https://orcid.org/0000-0003-0361-8642)
- Zelong Li (ORCID: https://orcid.org/0000-0002-5322-5065)
- Jungho Kim (ORCID: https://orcid.org/0000-0003-4560-6375)
- Xun Jia (ORCID: https://orcid.org/0000-0002-3446-4570)
- Maryia Zinouyeva (ORCID: https://orcid.org/0009-0001-4063-5006)
- Christian Zaprianov (ORCID: https://orcid.org/0000-0003-2021-6290)
- Yue Cao
Institutions
- Rutgers, The State University of New Jersey (US)
- Argonne National Laboratory (US)
- Chinese Academy of Sciences (CN)
- European Synchrotron Radiation Facility (FR)
- University of Chicago (US)
- Institute of High Energy Physics (CN)
- The University of Texas at Austin (US)
- Politecnico di Milano (IT)
Publication Details
- Journal
- Nano Letters
- Published
- 2026-10-28
- DOI
- https://doi.org/10.1021/acs.nanolett.6c04477
- Primary Topic
- Advanced Condensed Matter Physics
- Type
- article
- Field-Weighted Citation Impact
- 0.00
Funders
- National Science Foundation
- U.S. Department of Energy
- Gordon and Betty Moore Foundation
- National Natural Science Foundation of China
- Office of Science
- Materials Research Science and Engineering Center, Harvard University
- Division of Materials Research
- Basic Energy Sciences
- Argonne National Laboratory