Combining tip-enhanced Raman and photoluminescence with active atomic force tip interaction, I will discuss novel approaches for the study of photo-physical and photo-chemical processes in molecules and nano-solids. As example, we nano-image the exciton behavior and its correlation with defects, grain boundaries, and local strain in different transition metal di-chalcogenides (TMDs). Further, we are able to achieve TEPL spectroscopy of the otherwise forbidden radiative emission from excitonic dark states with the optical antenna tip coupling to its out-of-plane transition dipole moment. We achieve room temperature contrast, not possible in conventional approaches, due to the ultrafast radiative dark exciton to the tip-antenna mode with few-nm tip-sample gap localized mode volume induced Purcell factor of &gt; 2x10<sup>3</sup>. With the atomic-force microscope controlled antenna tip we demonstrate correlative nano-opto-mechanical switching and programmable modulation of the exciton emission. This hybrid tip-enhanced nano-spectroscopy and -imaging method allows to probe and control neutral-, multi-, localized-, and dark-excitons and their correlation with lattice and electronic structural heterogeneities in 2D materials and molecular systems. <br/>

Multimodal tip-enhanced spectroscopy

255th National Meeting (2018)

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