1) Generally spoken, no. Most vibrational modes strongly differ regarding their excitation efficiency (see https://en.wikipedia.org/wiki/Selection_rule#Vibrational_spectra and links therein) so you can't assume that a vibration that is well visible in Raman will care about IR.
2) However, in principle excited states can be probed both by Raman and IR so you can do time-dependent experiments:Article Femtosecond Stimulated Raman Spectroscopy
But for that you need special setups.
3) Internal vibrational redistribution is rather fast, so if you just irradiate with CW IR light, your sample will just warm up and you might start to see hot bands.
1) Generally spoken, no. Most vibrational modes strongly differ regarding their excitation efficiency (see https://en.wikipedia.org/wiki/Selection_rule#Vibrational_spectra and links therein) so you can't assume that a vibration that is well visible in Raman will care about IR.
2) However, in principle excited states can be probed both by Raman and IR so you can do time-dependent experiments:Article Femtosecond Stimulated Raman Spectroscopy
But for that you need special setups.
3) Internal vibrational redistribution is rather fast, so if you just irradiate with CW IR light, your sample will just warm up and you might start to see hot bands.
The light-material interaction is so weak that light itself will hardly achieve nonlinear vibrations. On the other hand, the strong nonlinearity of molecular vibration results higher-order Raman modes. Via this nonlinearity, it is easy to excite Raman-inactive phonon modes optically.