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The rapid progress on developing new and improved multifunctional materials, for optoelectronic and spin based phenomena/devices, have increased the importance of the fundamental understanding of their coherent states and nonlinear optical properties. This study is aimed at characterizing, modeling, and controlling the fundamental electronic, phononic, and spin properties of several classes of materials through nonequilibrium and nonlinear light-matter interactions, coupled with a novel design of the material phases, interfaces, and heterostructures. This research directly addresses the Grand Challenges identified in the Basic Energy Sciences Advisory Committee report "Directing Matter and Energy: Five Challenges for Science and the Imagination" (Hemminger, 2007) [1], in particular, the area: "Matter far beyond equilibrium" and addresses the questions, "How do remarkable properties of matter emerge from complex correlations of the atomic or electronic constituents and how can we control these properties?" and "How do we design and perfect atom- and energy-efficient synthesis of revolutionary new forms of matter with tailored properties?". The knowledge gained from these fundamental studies can provide new information for a broad community to provide concepts for the next generation of multifunctional materials and devices, and resulted in several publications and conference presentations. The materials studied in this dissertation included multiferroic BaTiO3-BiFeO3 [2], ferroelectric Pb0.52Zr0.48TiO3 (PZT), InAs/AlAsSb multi-quantum-well [3], lead halide perovskite [4], n-type InAsP films [5, 6], and nanolaminate plasmonic crystals [7]. Probing multiferroics, which are materials that can exhibit ferromagnetic, ferroelectric, and ferroelastic orders simultaneously in a single phase, was a main focus of this study. BiFeO3 (BFO) is the most widely investigated multiferroic due to its high Neel and Curie temperatures and has antiferromagnetic and ferroelectric properti