Background-Free Nonlinear Microspectroscopy with Vibrational Molecular Interferometry(full pdf)
Erik T. Garbacik, Jeroen P. Korterik, Cees Otto, Shaul Mukamel, Jennifer L. Herek, and Herman L. Offerhaus
Physical Review Letters
vol 107 p253902 dec16, 2011
We demonstrate a method for performing nonlinear microspectroscopy that provides an intuitive and unified description of the various signal contributions, and allows the direct extraction of the vibrational response. Three optical fields create a pair of Stokes Raman pathways that interfere in the same vibrational state. Frequency modulating one of the fields leads to amplitude modulations on all of the fields. This vibrational molecular interferometry technique allows imaging at high speed free of nonresonant background, and is able to distinguish between electronic and vibrational contributions to the total signal.