  Confining materials to two-dimensional forms changes the behavior of
electrons and enables new devices. However, most materials are challenging to
produce as uniform thin crystals. Here, we present a new synthesis approach
where crystals are grown in a nanoscale mold defined by atomically-flat van der
Waals (vdW) materials. By heating and compressing bismuth in a vdW mold made of
hexagonal boron nitride (hBN), we grow ultraflat bismuth crystals less than 10
nanometers thick. Due to quantum confinement, the bismuth bulk states are
gapped, isolating intrinsic Rashba surface states for transport studies. The
vdW-molded bismuth shows exceptional electronic transport, enabling the
observation of Shubnikov-de Haas quantum oscillations originating from the
(111) surface state Landau levels, which have eluded previous studies. By
measuring the gate-dependent magnetoresistance, we observe multi-carrier
quantum oscillations and Landau level splitting, with features originating from
both the top and bottom surfaces. Our vdW-mold growth technique establishes a
platform for electronic studies and control of bismuth's Rashba surface states
and topological boundary modes. Beyond bismuth, the vdW-molding approach
provides a low-cost way to synthesize ultrathin crystals and directly integrate
them into a vdW heterostructure.
