We present a survey of the structural and magnetic properties of submonolayer transition metal dioxides on the (001) surfaces of the heavy face-centered cubic (fcc) noble metals Ir and Pt performed by spin-averaged scanning tunneling microscopy (STM) and spin-polarized (SP-)STM. Our STM results confirm that deposition of Co, Fe, Mn, and Cr on the (2 × 1) oxygen-reconstructed Ir(001) surface leads to the formation of quasi one-dimensional chains with a (3 × 1) unit cell. As recently predicted by density functional theory [Ferstl et al., Phys. Rev. Lett. 117, 046101 (2016)], our SP-STM images of FeO2 and MnO2 on Ir(001) show a two-fold periodicity along the chains which is characteristic for an antiferromagnetic coupling along the chains. In addition, these two materials also exhibit spontaneous, permanent, and long-range magnetic coupling across the chains. Whereas we find a ferromagnetic inter-chain coupling for FeO2/Ir(001), the magnetic coupling of MnO2 on Ir(001) appears to be a non-collinear 120 • spin spiral, resulting in a (9 × 2) magnetic unit cell. On Pt(001) patches of (3 × 1)-reconstructed oxide chains could only be prepared by transition metal (Co, Fe, and Mn) deposition onto the cold substrate and subsequent annealing in an oxygen atmosphere. Again SP-STM on MnO2/Pt(001) reveals a very large, (15 × 2) magnetic unit cell which can tentatively be explained by a commensurate 72 • spin spiral. Large scale SP-STM images reveal a long wavelength spin rotation along the MnO2 chain.

No abstract

The Ruderman-Kittel-Kasuya-Yosida (RKKY) interaction mediates collinear magnetic interactions via the conduction electrons of a non-magnetic spacer, resulting in a ferro-or antiferromagnetic magnetization in magnetic multilayers. The resulting spin-polarized charge transport effects have found numerous applications. Recently it has been discovered that heavy non-magnetic spacers are able to mediate an indirect magnetic coupling that is non-collinear and chiral. This Dzyaloshinskii-Moriya-enhanced RKKY (DME-RKKY) interaction causes the emergence of a variety of interesting magnetic structures, such as skyrmions and spin spirals. Applications using these magnetic quasi-particles require a thorough understanding and fine-tuning of the balance between the Dzyaloshinskii-Moriya interaction and other magnetic interactions, e.g., the exchange interaction and magnetic anisotropy contributions. Here, we show by spin-polarized scanning tunneling microscopy that the spin structure of manganese oxide chains on Ir(001) can reproducibly be switched from chiral to collinear antiferromagnetic interchain interactions by increasing the oxidation state of MnO2 while the reverse process can be induced by thermal reduction. The underlying structural change is revealed by low-energy electron diffraction intensity data (LEED-IV) analysis. Density functional theory calculations suggest that the magnetic transition may be caused by a significant increase of the Heisenberg exchange upon oxidation.