期刊
NANO LETTERS
卷 12, 期 10, 页码 5061-5067出版社
AMER CHEMICAL SOC
DOI: 10.1021/nl2039925
关键词
tip-enhanced Raman spectroscopy; scanning tunneling microscopy; ultrahigh vacuum; phthalocyanine; density functional theory
类别
资金
- National Science Foundation [CHE-0802913, CHE-0911145, CHE-0955689, EEC-0647560, EEC-0634750, DMR-1121262, CHE03-20751]
- AFOSR/DARPA Project [BAA07-61 (FA9550-08-1-0221)]
- Department of Energy Basic Energy Sciences [DE-FG02-09ER161 09, DE-FG02-03ER15457, DE-5C0001785]
- Direct For Mathematical & Physical Scien
- Division Of Materials Research [1121262] Funding Source: National Science Foundation
Multiple vibrational modes have been observed for copper phthalocyanine (CuPc) adlayers on Ag(111) using ultrahigh vacuum (UHV) tip-enhanced Raman spectroscopy (TERS). Several important new experimental features are introduced in this work that significantly advance the state-of-the-art in UHV-TERS. These include (1) concurrent sub-nm molecular resolution STM imaging using Ag tips with laser illumination of the tip-sample junction, (2) laser focusing and Raman collection optics that are external to the UHV-STM that has two cryoshrouds for future low temperature experiments, and (3) all sample preparation steps are carried out in UHV to minimize contamination and maximize spatial resolution. Using this apparatus we have been able to demonstrate a TERS enhancement factor of 7.1 X 10(5). Further, density-functional theory calculations have been carried out that allow quantitative identification of eight different vibrational modes in the TER spectra. The combination of molecular-resolution UHV-STM imaging with the detailed chemical information content of UHV-TERS allows the interactions between large polyatomic molecular adsorbates and specific binding sites on solid surfaces to be probed with unprecedented spatial and spectroscopic resolution.
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