Higher-dimensional Fermiology in bulk moir\'e metals

Abstract

In the past decade, moir\'e materials have revolutionized how we engineer and control quantum phases of matter. Among incommensurate materials, moir\'e materials are aperiodic composite crystals whose long-wavelength moir\'e superlattices enable tunable properties without chemically modifying their layers. To date, nearly all reports of moir\'e materials have investigated van der Waals heterostructures assembled far from thermodynamic equilibrium. Here we introduce a conceptually new approach to synthesizing high-mobility moir\'e materials in thermodynamic equilibrium. We report a new family of foliated superlattice materials (Sr$_6$TaS$_8$)$_{1+\delta}$(TaS$_2$)$_8$ that are exfoliatable van der Waals crystals with atomically incommensurate lattices. Lattice mismatches between alternating layers generate moir\'e superlattices, analogous to those of 2D moir\'e heterobilayers, that are coherent throughout these crystals and are tunable through their synthesis conditions without altering their chemical composition. High-field quantum oscillation measurements map the complex Fermiology of these moir\'e metals, which can be tuned via the moir\'e superlattice structure. We find that the Fermi surface of the structurally simplest moir\'e metal is comprised of over 40 distinct cross-sectional areas, the most observed in any material to our knowledge. This can be naturally understood by postulating that bulk moir\'e materials can encode electronic properties of higher-dimensional superspace crystals in ways that parallel well-established crystallographic methods used for incommensurate lattices. More broadly, our work demonstrates a scalable synthesis approach potentially capable of producing moir\'e materials for electronics applications and evidences a novel material design concept for accessing a broad range of physical phenomena proposed in higher dimensions.