Atomistic Engineering of Phonons in Functional Oxide Heterostructures.

Engineering of phonons, that is, collective lattice vibrations in crystals, is essential for manipulating physical properties of materials such as thermal transport, electron-phonon interaction, confinement of lattice vibration, and optical polarization. Most approaches to phonon-engineering have been largely limited to the high-quality heterostructures of III-V compound semiconductors. Yet, artificial engineering of phonons in a variety of materials with functional properties, such as complex oxides, will yield unprecedented applications of coherent tunable phonons in future quantum acoustic devices. In this study, artificial engineering of phonons in the atomic-scale SrRuO3 /SrTiO3 superlattices is demonstrated, wherein tunable phonon modes are observed via confocal Raman spectroscopy. In particular, the coherent superlattices led to the backfolding of acoustic phonon dispersion, resulting in zone-folded acoustic phonons in the THz frequency domain. The frequencies can be largely tuned from 1 to 2 THz via atomic-scale precision thickness control. In addition, a polar optical phonon originating from the local inversion symmetry breaking in the artificial oxide superlattices is observed, exhibiting emergent functionality. The approach of atomic-scale heterostructuring of complex oxides will vastly expand material systems for quantum acoustic devices, especially with the viability of functionality integration.

Unconventional interlayer exchange coupling via chiral phonons in synthetic magnetic oxide heterostructures.

Chiral symmetry breaking of phonons plays an essential role in emergent quantum phenomena owing to its strong coupling to spin degree of freedom. However, direct experimental evidence of the chiral phonon-spin coupling is lacking. In this study, we report a chiral phonon-mediated interlayer exchange interaction in atomically controlled ferromagnetic metal (SrRuO3)-nonmagnetic insulator (SrTiO3) heterostructures. Owing to the unconventional interlayer exchange interaction, we have observed rotation of spins as a function of nonmagnetic insulating spacer thickness, resulting in a spin spiral state. The chiral phonon-spin coupling is further confirmed by phonon Zeeman effect. The existence of the chiral phonons and their interplay with spins along with our atomic-scale heterostructure approach unveil the crucial roles of chiral phonons in magnetic materials.

High-temperature optical properties of indium tin oxide thin-films.

Indium tin oxide (ITO) is one of the most widely used transparent conductors in optoelectronic device applications. We investigated the optical properties of ITO thin films at high temperatures up to 800 °C using spectroscopic ellipsometry. As temperature increases, amorphous ITO thin films undergo a phase transition at ~ 200 °C and develop polycrystalline phases with increased optical gap energies. The optical gap energies of both polycrystalline and epitaxial ITO thin films decrease with increasing temperature due to electron-phonon interactions. Depending on the background oxygen partial pressure, however, we observed that the optical gap energies exhibit reversible changes, implying that the oxidation and reduction processes occur vigorously due to the low oxidation and reduction potential energies of the ITO thin films at high temperatures. This result suggests that the electronic structure of ITO thin films strongly depends on temperature and oxygen partial pressure while they remain optically transparent, i.e., optical gap energies > 3.6 eV.