Adaptive tip-enhanced nano-spectroscopy

Dong Yun Lee, Chulho Park, Jinseong Choi, Yeonjeong Koo, Mingu Kang, Mun Seok Jeong, Markus B. Raschke, and Kyoung-Duck Park 
Nature Communications 12, 3465 (2021).
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Tip-enhanced nano-spectroscopy, such as tip-enhanced photoluminescence (TEPL) and tip-enhanced Raman spectroscopy (TERS), generally suffers from inconsistent signal enhancement and difficulty in polarization-resolved measurement. To address this problem, we present adaptive tip-enhanced nano-spectroscopy optimizing the nano-optical vector-field at the tip apex. Specifically, we demonstrate dynamic wavefront shaping of the excitation field to effectively couple light to the tip and adaptively control for enhanced sensitivity and polarization-controlled TEPL and TERS. Employing a sequence feedback algorithm, we achieve ~4.4 × 10⁴-fold TEPL enhancement of a WSe₂ monolayer which is >2× larger than the normal TEPL intensity without wavefront shaping. In addition, with dynamical near-field polarization control in TERS, we demonstrate the investigation of conformational heterogeneity of brilliant cresyl blue molecules and the controllable observation of IR-active modes due to a large gradient field effect. Adaptive tip-enhanced nano-spectroscopy thus provides for a systematic approach towards computational nanoscopy making optical nano-imaging more robust and widely deployable.