Combinatorial synthesis consists of high throughput fabrication and rapid characterization of compositionally varying samples to speed up the process of materials development. In this thesis, synthesis of composition spreads of artificial multiferroic thin film heterostructures consisting of alternating layers of (PTO) - (CFO) has been demonstrated using our combinatorial pulsed laser deposition (PLD) system. In the spread samples, the average composition changes continuously from pure PTO to pure CFO so that we can observe the changes in physical properties as a function of average composition.

      The coexistence of ferromagnetic and ferroelectric properties has been observed in a large extended region between pure CFO and PTO. An unexpected peak in the dielectric property has been observed in the middle of the spread, and it was identified as the composition where the ferroelectric phase transition takes place in PTO doped with CFO. The   of ferroelectricity is found to be tunable from 500 ℃ to room temperature by controlling the average volume ratio of CFO and PTO. We have also found that the magnetic anisotropy in the materials changes by introducing PTO to CFO.