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Light Sci Appl. 2017 Nov 17;6(11):e17098. doi: 10.1038/lsa.2017.98. eCollection 2017 Nov.

Subnanometer-resolved chemical imaging via multivariate analysis of tip-enhanced Raman maps.

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Hefei National Laboratory for Physical Sciences at the Microscale and Synergetic Innovation Center of Quantum Information & Quantum Physics, University of Science and Technology of China, Hefei, Anhui 230026, China.
Department of Precision Machinery and Precision Instrumentation, University of Science and Technology of China, Hefei, Anhui 230026, China.


Tip-enhanced Raman spectroscopy (TERS) is a powerful surface analysis technique that can provide subnanometer-resolved images of nanostructures with site-specific chemical fingerprints. However, due to the limitation of weak Raman signals and the resultant difficulty in achieving TERS imaging with good signal-to-noise ratios (SNRs), the conventional single-peak analysis is unsuitable for distinguishing complex molecular architectures at the subnanometer scale. Here we demonstrate that the combination of subnanometer-resolved TERS imaging and advanced multivariate analysis can provide an unbiased panoramic view of the chemical identity and spatial distribution of different molecules on surfaces, yielding high-quality chemical images despite limited SNRs in individual pixel-level spectra. This methodology allows us to exploit the full power of TERS imaging and unambiguously distinguish between adjacent molecules with a resolution of ~0.4 nm, as well as to resolve submolecular features and the differences in molecular adsorption configurations. Our results provide a promising methodology that promotes TERS imaging as a routine analytical technique for the analysis of complex nanostructures on surfaces.


chemical imaging; hyperspectral imaging; multivariate analysis; nanoimaging; tip-enhanced Raman spectroscopy

Conflict of interest statement

The authors declare no conflict of interest.

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