High-sensitivity of initial SrO growth on the residual resistivity in epitaxial thin films of SrRuO₃ on SrTiO₃ (001)

The growth of SrRuO$_3$ (SRO) thin film with high-crystallinity and low residual resistivity (RR) is essential to explore its intrinsic properties. Here, utilizing the adsorption-controlled growth technique, the growth condition of initial SrO layer on TiO$_2$-terminated SrTiO$_3$ (STO) (001) substrate was found to be crucial for achieving a low RR in the resulting SRO film grown afterward. The optimized initial SrO layer shows a $c$(2 x 2) superstructure that was characterized by electron diffraction, and a series of SRO films with different thicknesses ($t$s) were then grown. The resulting SRO films exhibit excellent crystallinity with orthorhombic-phase down to $t \approx$ 4.3 nm, which was confirmed by high resolution X-ray measurements. From azimuthal X-ray scan for SRO orthorhombic (021) reflection, we uncover four structural domains with a dominant domain of orthorhombic SRO [001] along cubic STO [010] direction. The dominant domain population depends on $t$, STO miscut angle (${\alpha}$), and miscut direction (${\beta}$), giving a volume fraction of about 92 $\%$ for $t \approx$ 26.6 nm and (${\alpha}$, ${\beta}$) ~ (0.14$^{\rm o}$, 5$^{\rm o}$). On the other hand, metallic and ferromagnetic properties were well preserved down to $t \approx$ 1.2 nm. Residual resistivity ratio (RRR = ${\rho}$(300 K)/${\rho}$(5 K)) reduces from 77.1 for $t \approx$ 28.5 nm to 2.5 for $t \approx$ 1.2 nm, while ${\rho}$(5 K) increases from 2.5 $\mu\Omega$cm for $t \approx$ 28.5 nm to 131.0 $\mu\Omega$cm for $t \approx$ 1.2 nm. The ferromagnetic onset temperature ($T_c\prime$) of around 151 K remains nearly unchanged down to $t \approx$ 9.0 nm and decreases to 90 K for $t \approx$ 1.2 nm. Our finding thus provides a practical guideline to achieve high crystallinity and low RR in ultra-thin SRO films by simply adjusting the growth of initial SrO layer.