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Bonding and Electronic Nature of the Anionic Framework in LaPd3S4

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Nicklas,  Michael
Michael Nicklas, Physics of Quantum Materials, Max Planck Institute for Chemical Physics of Solids, Max Planck Society;

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Yang,  Qun
Inorganic Chemistry, Max Planck Institute for Chemical Physics of Solids, Max Planck Society;

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Schnelle,  Walter
Walter Schnelle, Inorganic Chemistry, Max Planck Institute for Chemical Physics of Solids, Max Planck Society;

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Wawrzyńczak,  Rafał
Inorganic Chemistry, Max Planck Institute for Chemical Physics of Solids, Max Planck Society;

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Gooth,  Johannes
Nanostructured Quantum Matter, Max Planck Institute for Chemical Physics of Solids, Max Planck Society;

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Felser,  Claudia
Claudia Felser, Inorganic Chemistry, Max Planck Institute for Chemical Physics of Solids, Max Planck Society;

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Citation

Berry, T., Nicklas, M., Yang, Q., Schnelle, W., Wawrzyńczak, R., Förster, T., et al. (2022). Bonding and Electronic Nature of the Anionic Framework in LaPd3S4. Chemistry of Materials, 34(23), 10390-10398. doi:10.1021/acs.chemmater.2c02147.


Cite as: https://hdl.handle.net/21.11116/0000-000C-7B5E-2
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 mu 0H = 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.