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Chemically-synthesized single-crystalline silver nanowire (AgNW) probes can combine the scanning tunneling microscopy (STM) technique with tip-enhanced Raman scattering spectroscopy (TERS) for complementary morphological and chemical information with nanoscale spatial resolution. However, its performance has been limited by the blunt nanowire tip geometry, the insulating surfactant layer coating AgNW surfaces, and the thermal-induced mechanical vibrations. Here, we report a reproducible fabrication method for the preparation of sharp-tip AgNW-based TERS probes. By removing the polyvinylpyrrolidone (PVP) surfactant molecules from the AgNW surfaces for stable electrical conductivity and controlling the protruding length with μm-level accuracy for improved mechanical stability, we demonstrate atomic-resolution STM imaging with the sharp-tip AgNW probe. Furthermore, the sharp-tip AgNW has an excellent TER enhancement (∼1.1 × 10 6 ), which is about 66 folds of that achieved by regular AgNWs. Our experiments demonstrate that AgNWs with clean interfaces and the proper tip geometry can provide reliable and reproducible STM and TER characterizations, which remove the hurdles preventing the implementation of AgNW in STM-based near-field optical applications for a broad community.
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Adaptive tip-enhanced nano-spectroscopy
Abstract 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 × 10 4 -fold TEPL enhancement of a WSe 2 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.
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- Award ID(s):
- 1709822
- PAR ID:
- 10294032
- Date Published:
- Journal Name:
- Nature Communications
- Volume:
- 12
- Issue:
- 1
- ISSN:
- 2041-1723
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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- Free Publicly Accessible Full Text
-
Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.1038/s41467-021-23818-1
