Ultrafast Multidimensional Spectroscopy of Semiconductors and Strongly Correlated Materials

Abstract

This work develops a systematic approach to ultrafast multidimensional spectroscopy of novel solid-state materials. In a series of measurements, it addresses different spectral regions from visible to mid-infrared frequencies and functional materials with technological importance. Multidimensional measurements investigate ultrafast correlations and transient dynamics in asymmetric spectral regions, targeting the interplay of high- and low-energy excitations and other fundamental processes unseen in standard pump-probe experiments. Hereby, phase-sensitive detection of mid-infrared fields provides access to the complex dielectric function of the material and distinguishes thermal and non-thermal effects. Tentative measurements on a high-temperature superconductor raise interesting questions about coherent dynamics in strongly correlated electron materials and the application of this method in future experiments.