In
this work, we present an exfoliation method that produces cm2-area atomically flat surfaces from bulk layered single crystals,
with broad applications such as for the formation of lateral heterostructures
and for use as substrates for van der Waals epitaxy. Single crystals
of Bi2Se3 were grown using the Bridgman method
and examined with X-ray reciprocal space maps, Auger spectroscopy,
low-energy electron diffraction, and X-ray photoelectron spectroscopy.
An indium-bonding exfoliation technique was developed that produces
multiple ∼100 μm thick atomically flat, macroscopic (>1
cm2) slabs from each Bi2Se3 source
crystal. Two-dimensional X-ray diffraction and reciprocal space maps
confirm the high crystalline quality of the exfoliated surfaces. Atomic
force microscopy reveals that the exfoliated surfaces have an average
root-mean-square (RMS) roughness of ∼0.04 nm across 400 μm2 scans and an average terrace width of 70 μm between
step edges. First-principles calculations reveal exfoliation energies
of Bi2Se3 and a number of other layered compounds,
which demonstrate relevance of our method across the field of 2D materials.
While many potential applications exist, excellent lattice matching
with the III–V alloy space suggests immediate potential for
the use of these exfoliated layered materials as epitaxial substrates
for photovoltaic development.