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

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.