Dephasing-induced nonlinear vibrational spectroscopy

Advances in infrared laser technology have made it possible, for the first time, to perform nonlinear optical experiments directly on IR-active molecular vibrational modes. As a result, we are only just beginning to appreciate the profound difference between the nonlinear-optical behavior of electronic states and of vibrational states. The authors present an analysis of IR nonlinear optical experiments that predicts a wealth of new, dephasing-induced signals that provide unique information about the interactions between molecular vibrations and their surroundings. They also make a connection between their predictions and echo phenomena observed in anharmonically-coupled classical oscillators