Journal
ACS NANO
Volume 11, Issue 11, Pages 11466-11474Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.7b06183
Keywords
tip-enhanced Raman spectroscopy; spectromicroscopy; confined light; Stark shift; field-gradient-driven Raman; quadrupolar scattering; scanning tunneling microscopy
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Funding
- grant of NSF Center for Chemical Innovation [CHE-1414466]
- Direct For Mathematical & Physical Scien [1414466] Funding Source: National Science Foundation
- Division Of Chemistry [1414466] Funding Source: National Science Foundation
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Atomically terminated and nanoscopically smooth silver tips effectively focus light on the angstrom scale, allowing tip-enhanced Raman spectromicroscopy (TER-sm) with single molecule sensitivity and submolecular spatial resolution. Through measurements carried out on cobalt-tetraphenylporphyrin (CoTPP) adsorbed on Au(111), we highlight peculiarities of vibrational spectromicroscopy with light confined on the angstrom scale. Field-gradient-driven spectra; orientational fingerprinting, and sculpting of local fields by atomic morphology of the junction are elucidated through measurements that range from 2D arrays at room temperature to single molecule manipulations at 5 K. Notably, vibrational Stark tuning within molecules, reflecting intramolecular charge distributions, becomes accessible when light is more localized than the interrogated normal modes. The Stark images of CoTPP reveal that it is saddled, and the distortion is accompanied by charge transfer to gold through the two anchoring pyrroles.
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