| In this thesis, I discuss the theory, implementation and applications of coherent Raman scattering to imaging and sensing. A time domain interferometric method has been developed to collect high resolution shot-noise-limited Raman spectra over the Raman fingerprint regime and completely remove the electronic background signal in coherent Raman scattering. Compared with other existing coherent Raman microscopy methods, this time domain approach is proved to be simpler and more robust in rejecting background signal. We apply this method to image polymers and biological samples and demonstrate that the same setup can be used to collect two photon fluorescence and self phase modulation signals. A signal to noise ratio analysis is performed to show that this time domain method has a comparable signal to noise ratio to spectral domain methods, which we confirm experimentally. The coherent Raman method is also compared with spontaneous Raman scattering. The conditions under which coherent methods provide signal enhancement are discussed and experiments are performed to compare coherent Raman scattering with spontaneous Raman scattering under typical biological imaging conditions. A critical power, above which coherent Raman scattering is more sensitive than spontaneous Raman scattering, is experimentally determined to be ∼1mW in samples of high molecule concentration with a 75MHz laser system. This finding is contrary to claims that coherent methods provide many orders of magnitude enhancement under comparable conditions. In addition to the far field applications, I also discuss the combination of our time domain coherent Raman method with near field enhancement to explore the possibility of sensing and near field imaging. We report the first direct time-resolved coherent Raman measurement performed on a nanostructured substrate for molecule sensing. The preliminary results demonstrate that sub 20 fs pulses can be used to obtain coherent Raman spectra from a small number of molecules bound to a specially engineered metal structure and pave the way for a broad range of near field nonlinear experiments which require such short pulses. |
