  Vapor-pressure mismatched materials such as transition metal chalcogenides
have emerged as electronic, photonic, and quantum materials with scientific and
technological importance. However, epitaxial growth of vapor-pressure
mismatched materials are challenging due to differences in the reactivity,
sticking coefficient, and surface adatom mobility of the mismatched species
constituting the material, especially sulfur containing compounds. Here, we
report a novel approach to grow chalcogenides - hybrid pulsed laser deposition
- wherein an organosulfur precursor is used as a sulfur source in conjunction
with pulsed laser deposition to regulate the stoichiometry of the deposited
films. Epitaxial or textured thin films of sulfides with variety of structure
and chemistry such as alkaline metal chalcogenides, main group chalcogenides,
transition metal chalcogenides and chalcogenide perovskites are demonstrated,
and structural characterization reveal improvement in thin film crystallinity,
and surface and interface roughness compared to the state-of-the-art. The
growth method can be broadened to other vapor-pressure mismatched chalcogenides
such as selenides and tellurides. Our work opens up opportunities for broader
epitaxial growth of chalcogenides, especially sulfide-based thin film
technological applications.
