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Magnetic ultrathin films grown on heavy metal substrates often exhibit rich spin structures due to the competition between various magnetic interactions such as Heisenberg exchange, Dzyaloshinskii-Moriya interaction and higher-order spin interactions. Here we employ spin-polarized scanning tunneling microscopy to study magnetic nano-skyrmion phase in Fe monolayer grown on Ir(111) substrate. Our observations show that the formation of nano-skyrmion lattice in the Fe/Ir(111) system depends sensitively on the growth conditions and various non-skyrmion spin states can be formed. Remarkably, the application of voltage pulses between the tip and the sample can trigger a non-skyrmion to skyrmion phase transition. The fact that nano-skyrmions can be created using voltage pulse indicates that the balance between the competing magnetic interactions can be affected by an external electric field, which is highly useful to design skyrmion-based spintronic devices with low energy consumption.

Room temperature grown Fe monolayer (ML) on the Ir(111) single crystal substrate has attracted great research interests as nano-skyrmion lattice can form under proper growth conditions. The formation of the nanoscale skyrmion, however, appears to be greatly affected by the diffusion length of the Fe adatoms on the Ir(111) surface. We made this observation by employing spin-polarized scanning tunneling microscopy to study skyrmion formation upon systematically changing the impurity density on the substrate surface prior to Fe deposition. Since the substrate surface impurities serve as pinning centers for Fe adatoms, the eventual size and shape of the Fe islands exhibit a direct correlation with the impurity density, which in turn determines whether skyrmion can be formed. Our observation indicates that skyrmion only forms when the impurity density is below 0.006/nm2, i.e., 12 nm averaged spacing between the neighboring defects. We verify the significance of Fe diffusion length by growing Fe on clean Ir(111) substrate at low temperature of 30 K, where no skyrmion was observed to form. Our findings signify the importance of diffusion of Fe atoms on the Ir(111) substrate, which affects the size, shape and lattice perfection of the Fe islands and thus the formation of skyrmion lattice.

Strongly correlated materials often exhibit an electronic phase separation (EPS) phenomena whose domain pattern is random in nature. The ability to control the spatial arrangement of the electronic phases at microscopic scales is highly desirable for tailoring their macroscopic properties and/or designing novel electronic devices. Here we report the formation of EPS nanoscale network in a mono-atomically stacked LaMnO3/CaMnO3/PrMnO3 superlattice grown on SrTiO3 (STO) (001) substrate, which is known to have an antiferromagnetic (AFM) insulating ground state. The EPS nano-network is a consequence of an internal strain relaxation triggered by the structural domain formation of the underlying STO substrate at low temperatures. The same nanoscale network pattern can be reproduced upon temperature cycling allowing us to employ different local imaging techniques to directly compare the magnetic and transport state of a single EPS domain. Our results confirm the one-to-one correspondence between ferromagnetic (AFM) to metallic (insulating) state in manganite. It also represents a significant step in a paradigm shift from passively characterizing EPS in strongly correlated systems to actively engaging in its manipulation.

Hexagonal LuFe2O4 is a promising charge-order (CO) driven multiferroic material with high charge and spin ordering temperatures. The coexisting charge and spin orders on Fe3+/Fe2+ sites result in novel magnetoelectric behaviors, but the coupling mechanism between the charge and spin orders remains elusive. Here, by tuning external pressure, we reveal three correlated spin-charge ordered phases in LuFe2O4: i) a centrosymmetric incommensurate three-dimensional CO with ferrimagnetism, ii) a non-centrosymmetric incommensurate quasi-two-dimensional CO with ferrimagnetism, and iii) a centrosymmetric commensurate CO with antiferromagnetism. Experimental in-situ single-crystal X-ray diffraction and X-ray magnetic circular dichroism measurements combined with density functional theory calculations suggest that the charge density redistribution caused by pressure-induced compression in the frustrated double-layer [Fe2O4] cluster is responsible for the correlated spin-charge phase transitions. The pressure-enhanced effective Coulomb interactions among Fe-Fe bonds drive the frustrated (1/3, 1/3) CO to a less frustrated (1/4, 1/4) CO, which induces the ferrimagnetic to antiferromagnetic transition. Our results not only elucidate the coupling mechanism among charge, spin and lattice degrees of freedom in LuFe2O4 but also provide a new way to tune the spin-charge orders in a highly controlled manner.

Organic spintronic devices have been appealing because of the long spin life time of the charge carriers in the organic materials and their low cost, flexibility and chemical diversity. In previous studies, the control of resistance of organic spin valves is generally achieved by the alignment of the magnetization directions of the two ferromagnetic electrodes, generating magnetoresistance.1 Here we employ a new knob to tune the resistance of organic spin valves by adding a thin ferroelectric interfacial layer between the ferromagnetic electrode and the organic spacer. We show that the resistance can be controlled by not only the spin alignment of the two ferromagnetic electrodes, but also by the electric polarization of the interfacial ferroelectric layer: the MR of the spin valve depends strongly on the history of the bias voltage which is correlated with the polarization of the ferroelectric layer; the MR even changes sign when the electric polarization of the ferroelectric layer is reversed. This new tunability can be understood in terms of the change of relative energy level alignment between ferromagnetic electrode and the organic spacer caused by the electric dipole moment of the ferroelectric layer. These findings enable active control of resistance using both electric and magnetic fields, opening up possibility for multi-state organic spin valves and shed light on the mechanism of the spin transport in organic spin valves.

An experimental study was conducted on controlling the growth mode of La0.7Sr0.3MnO3 thin films on SrTiO3 substrates using pulsed laser deposition (PLD) by tuning growth temperature, pressure and laser fluence. Different thin film morphology, crystallinity and stoichiometry have been observed depending on growth parameters. To understand the microscopic origin, the adatom nucleation, step advance processes and their relationship to film growth were theoretically analyzed and a growth diagram was constructed. Three boundaries between highly and poorly crystallized growth, 2D and 3D growth, stoichiometric and non-stoichiometric growth were identified in the growth diagram. A good fit of our experimental observation with the growth diagram was found. This case study demonstrates that a more comprehensive understanding of the growth mode in PLD is possible.