Journal
PHYSICAL REVIEW E
Volume 87, Issue 2, Pages -Publisher
AMER PHYSICAL SOC
DOI: 10.1103/PhysRevE.87.020401
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Funding
- National Basic Research Project of China [2012YQ12006005, 2009CB930701, 2009CB930704, 2007CB936804]
- National Natural Science Foundation of China [90923003, 10874233, 10874234, 20703064, 11034006, 11227407]
- CAS [KJCX2-EW-W04]
- U.S. National Science Foundation [0906025]
- U.S. Department of Energy, Basic Energy Sciences, Materials Sciences and Engineering Division
- Nanometer Structure Consortium at Lund University, nmC@LU
- Division Of Materials Research
- Direct For Mathematical & Physical Scien [0906025] Funding Source: National Science Foundation
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Using p-aminothiophenol (PATP) molecules on a gold substrate and high-vacuum tip-enhanced Raman spectroscopy (HV-TERS), we show that the vibrational spectra of these molecules are distinctly different from those in typical surface-enhanced Raman spectroscopy. Detailed first-principles calculations help to assign the Raman peaks in the TERS measurements as Raman-active and IR-active vibrational modes of dimercaptoazobenzene (DMAB), providing strong spectroscopic evidence for the dimerization of PATP molecules to DMAB under the TERS setup. The activation of the IR-active modes is due to enhanced electromagnetic field gradient effects within the gap region of the highly asymmetric tip-surface geometry. Fermi resonances are also observed in HV-TERS. These findings help to broaden the versatility of TERS as a promising technique for ultrasensitive molecular spectroscopy. DOI:10.1103/PhysRevE.87.020401
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