In this thesis, both time-resolved, nonlinear optical spectroscopy and linear spectroscopy are used to investigate the interactions and dynamics of elementary excitations in strongly correlated electron systems. In the first part, we investigate the renormalization of magnetic elementary excitations in the transition metal oxide Cr2O3. We have created a non-equilibrium population of antiferromagnetic spin waves and characterized its dynamics, using frequency- and time-resolved optical spectroscopy of the exciton-magnon transition. We observed a time-dependent pump-probe line shape, which results from excitation induced renormalization of the spin wave band structure. We present a model that reproduces the basic characteristics of the data, in which we postulate the optical nonlinearity to be dominated by interactions with long-wavelength spin waves, and the dynamics due to spin wave thermalization. Using linear spectroscopy, coherent third-harmonic generation and pump-probe experiments, we measured the optical properties of the charge-transfer (CT) gap exciton in Sr2CuO2Cl2, an undoped model compound for high-temperature superconductors. A model is developed which explains the pronounced temperature dependence and newly observed Urbach tail in the linear absorption spectrum by a strong, phonon-mediated coupling between the charge-transfer exciton and ligand field excitations of the Cu atoms. The third-order nonlinear optical susceptibility within the Cu-O plane of Sr2CuO2Cl2 is fully characterized in both amplitude and phase, and symmetry based conclusions are made with respect to the spatial arrangement of the underlying charge distribution. Theoretical considerations ascribe a newly reported resonance in the third-order nonlinear susceptibility at 0.7 eV to a three-photon transition from the ground state to the charge-transfer exciton. An even parity intermediate state of Cudd character, is found to contribute to the transition. Finally, preliminary results of time-resolved pump-probe spectroscopy confirm that the CT exciton or one of its constituent parts couples strongly to phonons, and we suggest ultrafast thermalization with the lattice as the dominating mechanism underlying the dynamical properties.

Mots-clés de l'auteur: Ultrafast Optical Spectroscopy ; Many-Body Physics ; Collective Excitations ; Strongly Correlated Electron Systems.

The continuous evolution and development of experimental techniques is at the basis of any fundamental achievement in modern physics. Strongly correlated systems (SCS), more than any other, need to be investigated through the greatest variety of experimental techniques in order to unveil and crosscheck the numerous and puzzling anomalous behaviors characterizing them. The study of SCS fostered the improvement of many old experimental techniques, but also the advent of many new ones just invented in order to analyze the complex behaviors of these systems. Many novel materials, with functional properties emerging from macroscopic quantum behaviors at the frontier of modern research in physics, chemistry and materials science, belong to this class of systems. The volume presents a representative collection of the modern experimental techniques specifically tailored for the analysis of strongly correlated systems. Any technique is presented in great detail by its own inventor or by one of the world-wide recognized main contributors. The exposition has a clear pedagogical cut and fully reports on the most relevant case study where the specific technique showed to be very successful in describing and enlightening the puzzling physics of a particular strongly correlated system. The book is intended for advanced graduate students and post-docs in the field as textbook and/or main reference, but also for any other researcher in the field who appreciates consulting a single, but comprehensive, source or wishes to get acquainted, in a as painless as possible way, with the working details of a specific technique.