  Conventional lithography methods involving pattern transfer through resist
templating face challenges of material compatibility with various process
solvents. Other approaches of direct material writing often compromise pattern
complexity and overlay accuracy. Here we explore a concept based on the moir\'e
interference of molecular beams to directly pattern complex three-dimensional
(3D) surfaces made by any evaporable materials, such as metals, oxides and
organic semiconductors. Our proposed approach, termed the Molecular-Beam
Holographic Lithography (MBHL), relies on precise control over angular
projections of material flux passing through nanoapertures superimposed on the
substrate, emulating the interference of coherent laser beams in interference
lithography. Incorporating with our computational lithography (CL) algorithm,
we have demonstrated self-aligned overlay of multiple material patterns to
yield binary up to quinary superlattices, with a critical dimension and overlay
accuracy on the order of 50 and 2 nanometers, respectively. The process is
expected to substantially expand the boundary of materials combination for
high-throughput fabrication of complex superstructures of translational
symmetry on arbitrary substrates, enabling new nanoimaging, sensing, catalysis,
and optoelectronic devices.
