Bonding and Electronic Nature of the Anionic Framework in LaPd3S4

Research output: Contribution to journalResearch articleContributedpeer-review

Contributors

  • Tanya Berry - , Johns Hopkins University (Author)
  • Michael Nicklas - , Max Planck Institute for Chemical Physics of Solids (Author)
  • Qun Yang - , Max Planck Institute for Chemical Physics of Solids (Author)
  • Walter Schnelle - , Max Planck Institute for Chemical Physics of Solids (Author)
  • Rafał Wawrzyńczak - , Max Planck Institute for Chemical Physics of Solids (Author)
  • Tobias Förster - , Helmholtz-Zentrum Dresden-Rossendorf (Author)
  • Johannes Gooth - , Max Planck Institute for Chemical Physics of Solids (Author)
  • Claudia Felser - , Max Planck Institute for Chemical Physics of Solids, Würzburg-Dresden Cluster of Excellence ct.qmat (Author)
  • Tyrel M. McQueen - , Johns Hopkins University (Author)

Abstract

Double Dirac materials are a topological phase of matter in which a non-symmorphic symmetry enforces greater electronic degeneracy than normally expected - up to eightfold. The cubic palladium bronzes NaPd3O4 and LaPd3S4 are built of Pd3X4 (X = O, S) anionic frameworks that are ionically bonded to A cations (A = Na, La). These materials were recently identified computationally as harboring eightfold fermions. Here we report the preparation of single crystals and electronic properties of LaPd3S4. Measurements down to T = 0.45 K and in magnetic fields up to μ0H = 65 T are consistent with normal Fermi liquid physics of a Dirac metal in the presence of dilute magnetic impurities. This interpretation is further confirmed by analysis of specific heat, magnetization measurements and comparison to density functional theory (DFT) calculations. Through a bonding analysis of the DFT electronic structure of NaPd3O4 and LaPd3S4, we identify the origin of the stability of the anionic Pd3X4 framework at higher electron counts for X = S than X = O, and propose chemical tuning strategies to enable shifting the 8-fold fermion points to the Fermi level.

Details

Original languageEnglish
Pages (from-to)10390-10398
Number of pages9
JournalChemistry of materials
Volume34
Issue number23
Publication statusPublished - 13 Dec 2022
Peer-reviewedYes