Abstract:  Advancements in coherent control of vibrational dynamics lie in the development of novel noninvasive imaging techniques that provide information about biological species with molecular specificity. Of particular interest is development of coherent anti-Stokes Raman scattering (CARS) spectroscopy, which contains vibrational finger-prints of molecules. CARS is a nonlinear optical process utilizing ultrafast laser pulses to generate strong, molecular-specific signals that can be used for molecular detection. CARS imaging techniques are based on selective excitation of predetermined Raman transitions via ultrafast laser pulse manipulation. Methods implementing ultrafast pulse shaping and chirped delayed pulses will be discussed to control vibrational mode excitation in CARS spectroscopy. The role of the intramolecular processes, such as the coupling between Raman vibrational modes, that occur on a femtosecond time scale and affect the ultrafast energy redistribution, will be elucidated.