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Chasing Vibro-Polariton Fingerprints in Infrared and Raman Spectra Using Surface Lattice Resonances on Extended
Francesco Verdelli1, Jeff J P M Schulpen2, Andrea Baldi3
1Dutch Institute for Fundamental Energy Research, Eindhoven 5600HH, The Netherlands.
We achieved vibrational strong coupling between polymer bonds and light using gold nanoparticle arrays. However, this coupling was not observed in Raman spectra, suggesting new experimental approaches are needed.
Area of Science:
- Plasmonics and spectroscopy
- Materials science
Background:
- Surface lattice resonances (SLRs) enhance light-matter interactions.
- Particle arrays offer open systems with high field confinement for SLRs.
- Previous studies often used Fabry-Perot cavities.
Purpose of the Study:
- To experimentally investigate vibrational strong coupling (VSC) of C=O bonds in poly(methyl methacrylate) (PMMA).
- To couple PMMA C=O bonds to SLRs on gold particle arrays.
- To compare VSC in open systems versus traditional cavities.
Main Methods:
- Fabrication of gold particle arrays with tunable periods.
- Infrared (IR) extinction spectroscopy to observe spectral changes.
- Raman spectroscopy and micro-Raman mapping to detect polaritonic signatures.
Main Results:
- Vibrational strong coupling was confirmed via splitting of C=O resonance into lower and upper vibro-polaritons in IR spectra.
- Tuning the array period effectively controlled the coupling strength.
- No polariton signatures were detected in Raman spectra or micro-Raman mapping.
Conclusions:
- Gold particle arrays enable VSC with external radiation.
- IR spectroscopy clearly shows VSC, but Raman spectroscopy does not.
- Alternative cavity designs or experimental strategies are required for observing VSC in Raman spectra.
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