Toward far-field vibrational spectroscopy of single molecules at room temperature

J Phys Chem B. 2011 May 12;115(18):5425-30. doi: 10.1021/jp109652s. Epub 2011 Mar 7.

Abstract

We propose a new scheme for the extraction of chemically sensitive vibrational information from a single fluorescent molecule at room temperature. Our approach is based on a three-photon fluorescence excitation scheme, with selectivity in the production of a vibrational population of the ground state. We estimate the expected signal in perturbation theory for a standard dye molecule, compare its magnitude qualitatively to noise and various background sources, and discuss the experimental realization of this scheme.