Integration of c-axis oriented Bi3.15Nd0.85Ti2.95Hf0.05O12/La0.67Sr0.33MnO3 ferromagnetic-ferroelectric composite film on Si substrate.

A La0.67Sr0.33MnO3 (LSMO) ferromagnetic layer and a Nd3+/Hf4+ co-substituted Bi4Ti3O12 (Bi3.15Nd0.85Ti3-xHfxO12 (BNTHx, x = 0, 0.025, 0.05, 0.1 and 0.15)) ferroelectric layer were successively deposited onto the (00 l)-oriented LaNiO3 (LNO) layer buffered (001) Si substrate via all chemical solution deposition (CSD) method. As a result, the BNTHx/LSMO ferromagnetic-ferroelectric composite films integrated on Si substrate exhibit high c-axis orientation. The Nd3+/Hf4+ co-substituted BNTHx films have the lower leakage current and the better ferroelectric properties than the mono-substituted Bi4Ti3O12 (Bi3.15Nd0.85Ti3O12 and Bi4Ti2.95Hf0.05O12) films. In particular, the BNTH0.05/LSMO/LNO film has the lowest leakage current density of 2.5 × 10-7 A/cm2 at 200 kV/cm, and the highest remnant polarization (Pr) of 27.3 μC/cm2. The BNTH0.05/LSMO/LNO composite film also exhibits the soft ferromagnetism characteristics with a high saturated magnetization of 258 emu/cm3 at 300 K, and the excellent magnetoelectric (ME) effect. The variations of ME voltage coefficient α E values with DC bias magnetic field H bias shows that the BNTH0.05/LSMO/LNO film has the high α E value at near zero H bias. Moreover, at H bias = 0 Oe, the α E value gradually increases from zero with the increasing of the AC magnetic field frequency, and eventually reaches about 18.9 V/cm·Oe at 100 kHz, suggesting the existence of self-biased ME effect.