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Many classes of two-dimensional (2D) materials have emerged as potentialplatforms for novel electronic and optical devices. However, the physicalproperties are strongly influenced by nanoscale heterogeneities in the form ofedges, grain boundaries, and nucleation sites. Using combined tip-enhancedRaman scattering (TERS) and photoluminescence (TEPL) nano-spectroscopy and-imaging, we study the associated effects on the excitonic properties inmonolayer WSe2 grown by physical vapor deposition (PVD). With <15 nm spatialresolution we resolve nonlocal nanoscale correlations of PL spectral intensityand shifts with crystal edges and internal twin boundaries associated with theexpected exciton diffusion length. Through an active atomic force tipinteraction we can control the crystal strain on the nanoscale, and tune thelocal bandgap in reversible (up to 24 meV shift) and irreversible (up to 48 meVshift) fashion. This allows us to distinguish the effect of strain from thedominant influence of defects on the PL modification at the differentstructural heterogeneities. Hybrid nano-optical and nano-mechanical imaging andspectroscopy thus enables the systematic study of the coupling of structuraland mechanical degrees of freedom to the nanoscale electronic and opticalproperties in layered 2D materials.

Hybrid tip-enhanced nano-spectroscopy and -imaging of monolayer WSe2 with local strain control