Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 136, Issue 10, Pages 3881-3887Publisher
AMER CHEMICAL SOC
DOI: 10.1021/ja411899k
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Funding
- NSF Center for Chemical Innovation at the Space-Time Limit [CHE-082913]
- Department of Energy, Office of Basic Energy Sciences [DE-FG02-09ER16109]
- National Science Foundation [CHE-1152547, CHE-0955689, DMR-1121262, DMR-0520513, DGE-1324585]
- Hierarchical Materials Cluster Program at NU
- Division Of Chemistry
- Direct For Mathematical & Physical Scien [0955689, 1152547, 0802913] Funding Source: National Science Foundation
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Tip-enhanced Raman spectroscopy (TEAS) provides chemical information for adsorbates with nanoscale spatial resolution, single-molecule sensitivity, and, when combined with scanning tunneling microscopy (STM), Angstrom-scale topographic resolution. Performing TERS under ultrahigh-vacuum conditions allows pristine and atomically smooth surfaces to be maintained, while liquid He cooling minimizes surface diffusion of adsorbates across the solid surface, allowing direct STM imaging. Low-temperature TER (LT-TER) spectra differ from room-temperature TER (RT-TER), RT surface-enhanced Raman (SER), and LT-SER spectra because the vibrational lines are narrowed and shifted, revealing additional chemical information about adsorbate-substrate interactions. As an example, we present LT-TER spectra for the rhodamine 6G (R6G)/Ag(111) system that exhibit such unique spectral shifts. The high spectral resolution of LT-TERS provides intramolecular insight in that the shifted modes are associated with the ethylamine moiety of R6G. LT-TERS is a promising approach for unraveling the intricacies of adsorbate-substrate interactions that are inaccessible by other means.
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