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Abstract
Peaks, dips, and intermediate line shapes have been observed in surface-enhanced coherent Raman spectroscopy. Here, we report an experimental observation of a peculiar line shape revealing both a peak and a dip as two vibrational transitions of pyridazine in the presence of aggregated gold nanoparticles. We propose a simple model based on plasmonic phase effects and quantum chemistry calculations, and compare the simulated coherent (SECARS) and incoherent (SERS) Raman signals from several complexes. Complex SECARS line shapes provide additional information compared to SERS and can be used as a tool in nanoscale sensing and spectroscopy.
Additional information
Funding
Funding. This work was supported by the National Science Foundation [grant number EEC-0540832 (MIRTHE ERC)], PHY-1068554, PHY-1241032 (INSPIRE CREATIV), and PHY-1307153, the Office of Naval Research, and the Robert A. Welch Foundation (Awards A-1261 and A-1547).