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Multiferroic (0.285) BaTiO₃- (0.725) BiFeO₃ (BTO-BFO) and Pb _0.52 Zr _0.48 TiO ₃ (PZT) heterostructures are promising candidates for photonics and spintronics. Our BTO-BFO structures exhibit enhanced coupling between electric, magnetic, optical, and structural orders parameters. Furthermore, our PZT structures display ferroelectricity as well as enhanced switching response of their electrical polarization. In our work, we focused on probing ultrafast dynamics and nonlinear light-matter interactions in these structures. We have probed second harmonic generation, transient birefringence, and magneto-optical Kerr effects. In addition, in BTO-BFO heterostructures, we have generated and investigated coherent acoustic phonons. Our studies are important to gain a fundamental understanding of the dynamical processes in these newly developed structures.