Controlling multidimensional off-resonant-Raman and infrared vibrational spectroscopy by finite pulse band shapes

Abstract

Closed expressions are derived which incorporate pulse shaping effects in femtosecond nonlinear optical signals involving various combinations of temporally well-separated vibrationally resonant infrared and electronically off-resonant Raman pulses. Combinations of broadband and narrow band pulses that yield multidimensional extensions of coherent anti-Stokes Raman and sum frequency generation spectroscopy are presented. © 2009 American Institute of Physics.