Ultrafast far-infrared dynamics probed by terahertz pulses: A frequency domain approach. I. Model systems

Time-resolved terahertz spectroscopy has become a widely used experimental tool for the investigation of ultrafast dynamics of polar systems in the far infrared. We have recently proposed an analytical method for the extraction of a transient two-dimensional susceptibility from the experimental data [Nemec, Kadlec, and Kuzel, J. Chem. Phys. 117, 8454 (2002)]. In the present paper the methodology of optical pump-terahertz probe experiments is further developed for direct application in realistic experimental situations. The expected two-dimensional transient response function is calculated for a number of model cases (including Drude dynamics of free carriers, harmonic and anharmonic oscillator modes); these results serve as a basis for the interpretation of experimental results. We discuss also the cases where only partial (one-dimensional) information about the system dynamics can be experimentally obtained.