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Alternate stacking of a highly conducting metallic layer with a magnetictriangular layer found in delafossite PdCrO2 provides an excellent platform fordiscovering intriguing correlated quantum phenomena. Thin film growth of thematerial may enable not only tuning the basic physical properties beyond whatbulk materials can exhibit, but also developing novel hybrid materials byinterfacing with dissimilar materials, yet this has proven to be extremelychallenging. Here, we report the epitaxial growth of metallic delafossitePdCrO2 films by pulsed laser epitaxy (PLE). The fundamental role of the PLEgrowth conditions, epitaxial strain, and chemical and structuralcharacteristics of the substrate is investigated by growing under variousgrowth conditions and on various types of substrates. While strain plays alarge role in improving the crystallinities, the direct growth of epitaxialPdCrO2 films without impurity phases was not successful. We attribute thisdifficulty to both the chemical and structural dissimilarities between thesubstrates and volatile nature of PdO layer, which make nucleation of the rightphase difficult. This difficulty was overcome by growing CuCrO2 buffer layersbefore PdCrO2 were grown. Unlike PdCrO2, CuCrO2 films were rather readily grownwith a relatively wide growth window. Only monolayer thick buffer layer wassufficient to grow the correct PdCrO2 phase. This result indicates that theepitaxy of Pd-based delafossites is extremely sensitive to the chemistry andstructure of the interface, necessitating near perfect substrate materials. Theresulting films are commensurately strained and show an antiferromagnetictransition at 40 K that persists down to as thin as 3.6 nm in thickness.

Pulsed-laser epitaxy of metallic delafossite PdCrO$_2$ films