Calculations indicate that high vibrational states of oxygen and chlorine can be excited using a series of nonresonant Raman pulses, where both the pump and the Stokes pulses are chirped with linear frequency sweeps. Most of the previously reported coherent processes (such as simple adiabatic passage) are seriously degraded when rotational effects are included. However, we find that the laser pulse parameters (intensity and bandwidth) required to invert population into high vibrational states via Raman chirped adiabatic passage are achievable using technology that is currently available. Applications to homonuclear diatomic molecules are discussed in detail. © 1999 American Institute of Physics.