Photon echoes in impulsive optical spectroscopy of phonons
Jan Adriaan Leegwater, Shaul Mukamel
Multidimensional off resonant spectroscopy of crystals using a train of optical pulses can be effectively used to probe nuclear dynamics in solids. We predict a clear photon echo signal even in the absence of inhomogeneous broadening. This technique may be used for studying phonon dynamics in solids, in structurally frozen systems such as glasses, and in systems where the validity of the concept of phonons is not equally well established, such as liquids and gases. With this technique it is also possible to obtain information on the lifetime of phonons. We predict a long time tail of the nonlinear signal proportional to t−n/5, where n is the order of the response function studied.
The Journal of Chemical Physics•Feb 8, 1995•51 citations