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Confining materials to two-dimensional forms changes the behavior ofelectrons and enables new devices. However, most materials are challenging toproduce as uniform thin crystals. Here, we present a new synthesis approachwhere crystals are grown in a nanoscale mold defined by atomically-flat van derWaals (vdW) materials. By heating and compressing bismuth in a vdW mold made ofhexagonal boron nitride (hBN), we grow ultraflat bismuth crystals less than 10nanometers thick. Due to quantum confinement, the bismuth bulk states aregapped, isolating intrinsic Rashba surface states for transport studies. ThevdW-molded bismuth shows exceptional electronic transport, enabling theobservation of Shubnikov-de Haas quantum oscillations originating from the(111) surface state Landau levels, which have eluded previous studies. Bymeasuring the gate-dependent magnetoresistance, we observe multi-carrierquantum oscillations and Landau level splitting, with features originating fromboth the top and bottom surfaces. Our vdW-mold growth technique establishes aplatform for electronic studies and control of bismuth's Rashba surface statesand topological boundary modes. Beyond bismuth, the vdW-molding approachprovides a low-cost way to synthesize ultrathin crystals and directly integratethem into a vdW heterostructure.

Exceptional electronic transport and quantum oscillations in thin bismuth crystals grown inside van der Waals materials