arXiv2025
In the past decade, moiré materials have revolutionized how we engineer and control quantum phases of matter. Among incommensurate materials, moiré materials are aperiodic composite crystals whose long-wavelength moiré superlattices enable tunable properties without chemically modifying their layers. To date, nearly all reports of moiré materials have investigated van der Waals heterostructures assembled far from thermodynamic equilibrium. Here we introduce a conceptually new approach to synthesizing high-mobility moiré materials in thermodynamic equilibrium. We report a new family of foliated superlattice materials (Sr$_6$TaS$_8$)$_{1+δ}$(TaS$_2$)$_8$ that are exfoliatable van der Waals crystals with atomically incommensurate lattices. Lattice mismatches between alternating layers generate moiré superlattices, analogous to those of 2D moiré 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 moiré metals, which can be tuned via the moiré superlattice structure. We find that the Fermi surface of the structurally simplest moiré 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 moiré 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 moiré materials for electronics applications and evidences a novel material design concept for accessing a broad range of physical phenomena proposed in higher dimensions.