Coupling of the Structure and Magnetism to Spin Splitting in Hybrid Organic-Inorganic Perovskites.

Hybrid organic-inorganic perovskites are famous for the diversity of their chemical compositions, phases, phase transitions, and associated physical properties. We use a combination of experimental and computational techniques to reveal a strong coupling between structure, magnetism, and spin splitting in a representative of the largest family of hybrid organic-inorganic perovskites: the formates. With the help of first-principles simulations, we find spin splitting in both conduction and valence bands of [NH2NH3]Co(HCOO)3 induced by spin-orbit interactions, which can reach up to 14 meV. Our magnetic measurements reveal that this material exhibits canted antiferromagnetism below 15.5 K. The direction of the associated antiferromagnetic order parameter is strongly coupled with spin splitting in the centrosymmetric phase, allowing for the creation and annihilation of spin splitting through the application of a magnetic field. Furthermore, the structural phase transition to the experimentally observed polar Pna21 phase completely changes the aforementioned spin splitting and its coupling to magnetic degrees of freedom. This reveals that in [NH2NH3]Co(HCOO)3, the structure and magnetism are strongly coupled to spin splitting and can be manipulated through electric and magnetic fields. We believe that our findings offer an important step toward a fundamental understanding and practical applications of materials with coupled properties.

Temperature Evolution of Magnon Propagation Length in Tm3Fe5O12 Thin Films: Roles of Magnetic Anisotropy and Gilbert Damping.

The magnon propagation length, ⟨ξ⟩, of a ferro-/ferrimagnet (FM) is one of the key factors that controls the generation and propagation of thermally driven magnonic spin current in FM/heavy metal (HM) bilayer based spincaloritronic devices. For the development of a complete physical picture of thermally driven magnon transport in FM/HM bilayers over a wide temperature range, it is of utmost importance to understand the respective roles of temperature-dependent Gilbert damping (α) and effective magnetic anisotropy (Keff) in controlling the temperature evolution of ⟨ξ⟩. Here, we report a comprehensive investigation of the temperature-dependent longitudinal spin Seebeck effect (LSSE), radio frequency transverse susceptibility, and broad-band ferromagnetic resonance measurements on Tm3Fe5O12 (TmIG)/Pt bilayers grown on different substrates. We observe a significant drop in the LSSE voltage below 200 K independent of TmIG film thickness and substrate choice. This is attributed to the noticeable increases in effective magnetic anisotropy field, HKeff (∝Keff) and α that occur within the same temperature range. From the TmIG thickness dependence of the LSSE voltage, we determined the temperature dependence of ⟨ξ⟩ and highlighted its correlation with the temperature-dependent HKeff and α in TmIG/Pt bilayers, which will be beneficial for the development of rare-earth iron garnet based efficient spincaloritronic nanodevices.

Large Thermo-Spin Effects in Heusler Alloy-Based Spin Gapless Semiconductor Thin Films.

Recently, Heusler alloy-based spin gapless semiconductors (SGSs) with high Curie temperature (TC) and sizable spin polarization have emerged as potential candidates for tunable spintronic applications. We report comprehensive investigation of the temperature-dependent ANE and intrinsic longitudinal spin Seebeck effect (LSSE) in CoFeCrGa thin films grown on MgO substrates. Our findings show that the anomalous Nernst coefficient for the MgO/CoFeCrGa (95 nm) film is ≈1.86 µV K-1 at room temperature, which is nearly 2 orders of magnitude higher than that of the bulk polycrystalline sample of CoFeCrGa (≈0.018 µV K-1) and almost 3 orders of magnitude higher than that of the half-metallic ferromagnet La1-xNaxMnO3 (≈0.005 µV K-1) but comparable to that of the magnetic Weyl semimetal Co2MnGa thin film (≈2-3 µV K-1). Furthermore, the LSSE coefficient for our MgO/CoFeCrGa (95 nm)/Pt (5 nm) heterostructure is ≈20.5 nV K-1 Ω-1 at room temperature, which is twice larger than that of the half-metallic ferromagnetic La0.7Sr0.3MnO3 thin films (≈9 nV K-1 Ω-1). We show that both ANE and LSSE coefficients follow identical temperature dependences and exhibit a maximum at ≈225 K, which is understood as the combined effects of inelastic magnon scatterings and reduced magnon population at low temperatures. Our analyses not only indicate that the extrinsic skew scattering is the dominating mechanism for ANE in these films but also provide critical insights into the functional form of the observed temperature-dependent LSSE at low temperatures. Furthermore, by employing radio frequency transverse susceptibility and broad-band ferromagnetic resonance in combination with the LSSE measurements, we establish a correlation among the observed LSSE signal, magnetic anisotropy, and Gilbert damping of the CoFeCrGa thin films, which will be beneficial for fabricating tunable and highly efficient Heusler alloy-based spin caloritronic nanodevices.

Intergranular Spin Dependent Tunneling Dominated Magnetoresistance in Helimagnetic Manganese Phosphide Thin Films.

Helical magnets are emerging as a novel class of materials for spintronics and sensor applications; however, research on their charge- and spin-transport properties in a thin film form is less explored. Herein, we report the temperature and magnetic field-dependent charge transport properties of a highly crystalline MnP nanorod thin film over a wide temperature range (2 K < T < 350 K). The MnP nanorod films of ~100 nm thickness were grown on Si substrates at 500 °C using molecular beam epitaxy. The temperature-dependent resistivity ρ(T) data exhibit a metallic behavior (dρ/dT > 0) over the entire measured temperature range. However, large negative magnetoresistance (Δρ/ρ) of up to 12% is observed below ~50 K at which the system enters a stable helical (screw) magnetic state. In this temperature regime, the Δρ(H)/ρ(0) dependence also shows a magnetic field-manipulated CONE + FAN phase coexistence. The observed magnetoresistance is dominantly governed by the intergranular spin dependent tunneling mechanism. These findings pinpoint a correlation between the transport and magnetism in this helimagnetic system.

Enhanced Magnetism and Anomalous Hall Transport through Two-Dimensional Tungsten Disulfide Interfaces.

The magnetic proximity effect (MPE) has recently been explored to manipulate interfacial properties of two-dimensional (2D) transition metal dichalcogenide (TMD)/ferromagnet heterostructures for use in spintronics and valleytronics. However, a full understanding of the MPE and its temperature and magnetic field evolution in these systems is lacking. In this study, the MPE has been probed in Pt/WS2/BPIO (biphase iron oxide, Fe3O4 and α-Fe2O3) heterostructures through a comprehensive investigation of their magnetic and transport properties using magnetometry, four-probe resistivity, and anomalous Hall effect (AHE) measurements. Density functional theory (DFT) calculations are performed to complement the experimental findings. We found that the presence of monolayer WS2 flakes reduces the magnetization of BPIO and hence the total magnetization of Pt/WS2/BPIO at T > ~120 K-the Verwey transition temperature of Fe3O4 (TV). However, an enhanced magnetization is achieved at T < TV. In the latter case, a comparative analysis of the transport properties of Pt/WS2/BPIO and Pt/BPIO from AHE measurements reveals ferromagnetic coupling at the WS2/BPIO interface. Our study forms the foundation for understanding MPE-mediated interfacial properties and paves a new pathway for designing 2D TMD/magnet heterostructures for applications in spintronics, opto-spincaloritronics, and valleytronics.

Spin Seebeck Effect in Iron Oxide Thin Films: Effects of Phase Transition, Phase Coexistence, And Surface Magnetism.

Understanding the effects of phase transition, phase coexistence, and surface magnetism on the longitudinal spin Seebeck effect (LSSE) in a magnetic system is essential to manipulate the spin to charge current conversion efficiency for spincaloritronic applications. We aim to elucidate these effects by performing a comprehensive study of the temperature dependence of the LSSE in biphase iron oxide (BPIO = α-Fe2O3 + Fe3O4) thin films grown on Si (100) and Al2O3 (111) substrates. A combination of a temperature-dependent anomalous Nernst effect (ANE) and electrical resistivity measurements show that the contribution of the ANE from the BPIO layer is negligible in comparison to the intrinsic LSSE in the Si/BPIO/Pt heterostructure, even at room temperature. Below the Verwey transition of the Fe3O4 phase, the total signal across BPIO/Pt is dominated by the LSSE. Noticeable changes in the intrinsic LSSE signal for both Si/BPIO/Pt and Al2O3/BPIO/Pt heterostructures around the Verwey transition of the Fe3O4 phase and the antiferromagnetic (AFM) Morin transition of the α-Fe2O3 phase are observed. The LSSE signal for Si/BPIO/Pt is found to be almost 2 times greater than that for Al2O3/BPIO/Pt; however, an opposite trend is observed for the saturation magnetization. Magnetic force microscopy reveals the higher density of surface magnetic moments of the Si/BPIO film in comparison to the Al2O3/BPIO film, which underscores the dominant role of interfacial magnetism on the LSSE signal and thereby explains the larger LSSE for Si/BPIO/Pt.