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Probing Intermolecular Vibrational Symmetry Breaking in Self-Assembled Monolayers with Ultrahigh Vacuum Tip-Enhanced
Naihao Chiang, Nan Jiang1, Lindsey R Madison
1Department of Chemistry, University of Illinois at Chicago , Chicago, Illinois 60607, United States.
Journal of the American Chemical Society
|December 5, 2017
Summary
Ultrahigh vacuum tip-enhanced Raman spectroscopy (UHV-TERS) reveals how molecule-molecule interactions affect vibrational spectra. This technique allows direct nanoscale measurement of these interactions for surface-bound molecules.
Area of Science:
- Surface science
- Spectroscopy
- Nanotechnology
Background:
- Tip-enhanced Raman spectroscopy (TERS) offers high chemical sensitivity and structural specificity.
- Ultrahigh vacuum (UHV) environments are crucial for studying surface phenomena at the molecular level.
Purpose of the Study:
- To investigate the influence of intermolecular interactions on the vibrational spectra of N-N'-bis(2,6-diisopropylphenyl)-perylene-3,4:9,10-bis(dicarboximide) (PDI) molecules.
- To demonstrate the capability of UHV-TERS for nanoscale interaction measurements.
Main Methods:
- Utilizing ultrahigh vacuum tip-enhanced Raman spectroscopy (UHV-TERS).
- Employing theoretical calculations to complement experimental data.
- Adsorbing PDI on single-crystal silver (Ag) substrates (Ag(111) and Ag(100)).
Main Results:
- Observed lifting of vibrational degeneracy in PDI molecules on Ag surfaces.
- Identified the most perturbed vibrational mode associated with peripheral molecular amplitude.
- Demonstrated direct nanoscale measurement of molecule-molecule interactions.
Conclusions:
- UHV-TERS is a powerful tool for probing intermolecular interactions at the nanoscale.
- Understanding these interactions is vital for surface-bound molecules and materials science.
- This study advances fundamental knowledge of how intermolecular forces impact molecular vibrations on surfaces.
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