  High throughput characterization and processing techniques are becoming
increasingly necessary to navigate multivariable, data-driven design challenges
for sensors and electronic devices. For two-dimensional materials, device
performance is highly dependent upon a vast array of material properties
including number of layers, lattice strain, carrier concentration, defect
density, and grain structure. In this work, laser-crystallization was used to
locally pattern and transform hundreds of regions of amorphous MoS2 thin films
into 2D 2H-MoS2. A high throughput Raman spectroscopy approach was subsequently
used to assess the process-dependent structural and compositional variations
for each illuminated region, yielding over 5500 distinct non-resonant,
resonant, and polarized Raman spectra. The rapid generation of a comprehensive
library of structural and compositional data elucidated important trends
between structure-property-processing relationships involving
laser-crystallized MoS2, including the relationships between grain size, grain
orientation, and intrinsic strain. Moreover, extensive analysis of
structure/property relationships allowed for intelligent design, and evaluation
of major contributions to, device performance in MoS2 chemical sensors. In
particular, it is found that sensor performance is strongly dependent on the
orientation of the MoS2 grains relative to the crystal plane.
