Crystal-chemical origins of the ultrahigh conductivity of metallic delafossites

Yi Zhang, Fred Tutt, Guy N. Evans, Prachi Sharma, Greg Haugstad, Ben Kaiser, Justin Ramberger, Samuel Bayliff, Yu Tao, Mike Manno, Javier Garcia-Barriocanal, Vipul Chaturvedi, Rafael M. Fernandes, Turan Birol, William E. Seyfried and Chris Leighton ()
Additional contact information
Yi Zhang: University of Minnesota
Fred Tutt: University of Minnesota
Guy N. Evans: University of Minnesota
Prachi Sharma: University of Minnesota
Greg Haugstad: University of Minnesota
Ben Kaiser: University of Minnesota
Justin Ramberger: University of Minnesota
Samuel Bayliff: University of Minnesota
Yu Tao: University of Minnesota
Mike Manno: University of Minnesota
Javier Garcia-Barriocanal: University of Minnesota
Vipul Chaturvedi: University of Minnesota
Rafael M. Fernandes: University of Minnesota
Turan Birol: University of Minnesota
William E. Seyfried: University of Minnesota
Chris Leighton: University of Minnesota

Nature Communications, 2024, vol. 15, issue 1, 1-14

Abstract: Abstract Despite their highly anisotropic complex-oxidic nature, certain delafossite compounds (e.g., PdCoO2, PtCoO2) are the most conductive oxides known, for reasons that remain poorly understood. Their room-temperature conductivity can exceed that of Au, while their low-temperature electronic mean-free-paths reach an astonishing 20 μm. It is widely accepted that these materials must be ultrapure to achieve this, although the methods for their growth (which produce only small crystals) are not typically capable of such. Here, we report a different approach to PdCoO2 crystal growth, using chemical vapor transport methods to achieve order-of-magnitude gains in size, the highest structural qualities yet reported, and record residual resistivity ratios ( > 440). Nevertheless, detailed mass spectrometry measurements on these materials reveal that they are not ultrapure in a general sense, typically harboring 100s-of-parts-per-million impurity levels. Through quantitative crystal-chemical analyses, we resolve this apparent dichotomy, showing that the vast majority of impurities are forced to reside in the Co-O octahedral layers, leaving the conductive Pd sheets highly pure (∼1 ppm impurity concentrations). These purities are shown to be in quantitative agreement with measured residual resistivities. We thus conclude that a sublattice purification mechanism is essential to the ultrahigh low-temperature conductivity and mean-free-path of metallic delafossites.

Date: 2024
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DOI: 10.1038/s41467-024-45239-6

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