Journal of Chemical Physics, Vol.120, No.3, 1466-1476, 2004
Nonresonant holeburning in the Terahertz range: Brownian oscillator model
The response to the field sequence of nonresonant hole burning, a pump-wait-probe experiment originally designed to investigate slow relaxation in complex systems, is calculated for a model of Brownian oscillators, thus including inertial effects. In the overdamped regime the model predictions are very similar to those of the purely dissipative stochastic models investigated earlier, including the possibility to discriminate between dynamic homogeneous and heterogeneous relaxation. The case of underdamped oscillations is of particular interest when low-frequency excitations in glassy systems are considered. We show that also in this situation a frequency selective modification of the response should be feasable. This means that it is possible to specifically address various parts of the spectrum. An experimental realization of nonresonant holeburning in the Terahertz regime therefore is expected to shed further light on the nature of the vibrations around the so-called boson peak. (C) 2004 American Institute of Physics.