Abstract
The kagome motif is a versatile platform for condensed matter physics, hosting rich interactions between magnetic, electronic, and structural degrees of freedom. In recent years, the discovery of a charge density wave (CDW) in the AV3Sb5 superconductors and structurally-derived bond density waves (BDW) in FeGe and ScV6Sn6 have stoked the search for new kagome platforms broadly exhibiting density wave (DW) transitions. In this work, we evaluate the known AM6X6 chemistries and construct a stability diagram that summarizes the structural relationships among the >125 member family. Subsequently, we introduce our discovery of the broader LnNb6Sn6 (Ln:Ce-Nd,Sm,Gd-Tm,Lu,Y) family of kagome metals and an analogous DW transition in LuNb6Sn6. Our X-ray scattering measurements clearly indicate a (1/3, 1/3, 1/3) ordering wave vector ((Formula presented) superlattice) and diffuse scattering on half-integer L-planes. Our analysis of the structural data supports the “rattling mode” DW model proposed for ScV6Sn6 and paints a detailed picture of the steric interactions between the rare-earth filler element and the host Nb-Sn kagome scaffolding. We also provide a broad survey of the magnetic properties within the HfFe6Ge6-type LnNb6Sn6 members, revealing a number of complex antiferromagnetic and metamagnetic transitions throughout the family. This work integrates our new LnNb6Sn6 series of compounds into the broader AM6X6 family, providing new material platforms and forging a new route forward at the frontier of kagome metal research.
| Original language | English |
|---|---|
| Pages (from-to) | 5279-5292 |
| Number of pages | 14 |
| Journal | Journal of the American Chemical Society |
| Volume | 147 |
| Issue number | 6 |
| DOIs | |
| State | Published - Feb 12 2025 |
Funding
This research was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division (material development, crystal growth, characterization, X-ray, ARPES, and theory). Early aspects of the work (project conception, phase diagram mapping from literature, DFT) was sponsored by the Laboratory Directed Research and Development Program of Oak Ridge National Laboratory, managed by UT-Battelle, LLC, for the US Department of Energy. This work is based on research conducted at the Center for High-Energy X-ray Sciences (CHEXS), which is supported by the National Science Foundation (BIO, ENG, and MPS Directorates) under award DMR-2342336. W.R.M., S.M., A.T., and D.M. acknowledge support from the Gordon and Betty Moore Foundation\u2019s EPiQS Initiative, Grant GBMF9069 awarded to D.M., S.D.W., and S.J.G.A. gratefully acknowledge support via the UC Santa Barbara NSF Quantum Foundry funded via the Q-AMASE-i program under award DMR-1906325. G.P. acknowledges support from the University of West Georgia. X-ray scattering and ARPES measurements used resources at 4-ID and 21-ID-1 beamlines of the National Synchrotron Light Source II, a US Department of Energy Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory under contract no. DE-SC0012704. This research used resources of the Compute and Data Environment for Science (CADES) at the Oak Ridge National Laboratory, which is supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC05-00OR22725. We thank Seunghwan Do for his discussions and feedback. We thank Jong Keum and the X-ray laboratory of the Oak Ridge National Laboratory Spallation Neutron Source (SNS) for use of their Photonic Science Laue camera and Rigaku XtaLab PRO diffractometer. This manuscript has been authored by UT-Battelle, LLC, under contract DE-AC05-00OR22725 with the US Department of Energy (DOE). The US government retains and the publisher, by accepting the article for publication, acknowledges that the US government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for US government purposes. DOE will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan ( https://www.energy.gov/doe-public-access-plan ).