Imprinting Ferromagnetism and Superconductivity in Single Atomic Layers of Molecular Superlattices

Ferromagnetism and superconductivity are two antagonistic phenomena since ferromagnetic exchange fields tend to destroy singlet Cooper pairs. Reconciliation of these two competing phases has been achieved in vertically stacked heterostructures where these two orders are confined in different layers. However, controllable integration of these two phases in one atomic layer is a longstanding challenge. Here, an interlayer-space-confined chemical design (ICCD) is reported for the synthesis of dilute single-atom-doped TaS₂ molecular superlattice, whereby ferromagnetism is observed in the superconducting TaS₂ layers. The intercalation of 2H-TaS₂ crystal with bulky organic ammonium molecule expands its van der Waals gap for single-atom doping via co-intercalated cobalt ions, resulting in the formation of quasi-monolayer Co-doped TaS₂ superlattices. Isolated Co atoms are decorated in the basal plane of the TaS₂ via substituting the Ta atom or anchoring at a hollow site, wherein the orbital-selected p–d hybridization between Co and neighboring Ta and S atoms induces local magnetic moments with strong ferromagnetic coupling. This ICCD approach can be applied to various metal ions, enabling the synthesis of a series of crystal-size TaS₂ molecular superlattices.     

Interplay of Superconductivity and Ferromagnetism in UGe<Subscript>2</Subscript>

The emergence of pressure induced superconductivity (SC) under the background of ferromagnetic state in 5f-electron based itinerant ferromagnetic superconductor UGe₂ is studied in the single band model by using a mean-field approximation. The solutions to the coupled equations of superconducting gap (Δ) and magnetization (m) are obtained using Green’s function technique and equation of motion method. It is shown that there generally exists a coexistent (Δ≠0, m≠0) solution to the coupled equations of the order parameters in the temperature range 0<T<min (T _C,T _FM), where T _C and T _FM are respectively the superconducting and ferromagnetic transition temperatures. The study of electronic specific heat (C/T), density of states, free energy, etc. are also presented. The specific heat capacity at low temperature shows linear temperature dependence as opposed to the activated behavior. Density of states increases as opposed to the case of a standard ferromagnetic metal. Free energy study reveals that the superconducting ferromagnetic state has lower energy than the normal ferromagnetic state and, therefore, realized at low enough temperature. The agreement between theory and experimental results for UGe₂ is quite satisfactory.      

Room Temperature Ferromagnetism of Ge/MnAs Digital Alloys

The magnetic properties of Ge/MnAs digital alloys on GaAs (001) substrates, grown by molecular beam epitaxy, were investigated using a Quantum Design SQUID magnetometer. The Ge (1 nm)/MnAs (0.15 nm) digital alloy showed ferromagnetism up to 334 K with a coercive field of 576 Oe at room temperature, as determined from temperature-dependent magnetization and hysteresis loop measurements. The ferromagnetic and antiferromagnetic phases of a Ge₇/(Mn_0.5As_0.5)₁ superlattice, investigated using the full-potential linearized augmented plane wave (FLAPW) method yielded a ferromagnetic ground state with a high spin magnetic moment of Mn (3.45 _B) which induces only very small magnetic moments on its neighboring As or Ge atoms.     

Direct visualization of magnetic‐field‐induced magnetoelectric switching in multiferroic aurivillius phase thin films

Multiferroic materials displaying coupled ferroelectric and ferromagnetic order parameters could provide a means for data storage whereby bits could be written electrically and read magnetically, or vice versa. Thin films of Aurivillius phase Bi₆Ti_2.8Fe_1.52Mn_0.68O₁₈, previously prepared by a chemical solution deposition (CSD) technique, are multiferroics demonstrating magnetoelectric coupling at room temperature. Here, we demonstrate the growth of a similar composition, Bi₆Ti_2.99Fe_1.46Mn_0.55O₁₈, via the liquid injection chemical vapor deposition technique. High‐resolution magnetic measurements reveal a considerably higher in‐plane ferromagnetic signature than CSD grown films (M_S=24.25 emu/g (215 emu/cm³), M_R=9.916 emu/g (81.5 emu/cm³), H_C=170 Oe). A statistical analysis of the results from a thorough microstructural examination of the samples, allows us to conclude that the ferromagnetic signature can be attributed to the Aurivillius phase, with a confidence level of 99.95%. In addition, we report the direct piezoresponse force microscopy visualization of ferroelectric switching while going through a full in‐plane magnetic field cycle, where increased volumes (8.6% to 14% compared with 4% to 7% for the CSD‐grown films) of the film engage in magnetoelectric coupling and demonstrate both irreversible and reversible magnetoelectric domain switching.     

Boosting the superconducting spin valve effect in a metallic superconductor/ferromagnet heterostructure

Superconducting spin valves based on the superconductor/ferromagnet (S/F) proximity effect are considered to be a key element in the emerging field of superconducting spintronics. Here, we demonstrate the crucial role of the morphology of the superconducting layer in the operation of a multilayer S/F1/F2 spin valve. We study two types of superconducting spin valve heterostructures, with rough and with smooth superconducting layers, using transmission electron microscopy in combination with transport and magnetic characterization. We find that the quality of the S/F interface is not critical for the S/F proximity effect, as regards the suppression of the critical temperature of the S layer. However, it appears to be of paramount importance in the performance of the S/F1/F2 spin valve. As the morphology of the S layer changes from the form of overlapping islands to a smooth case, the magnitude of the conventional superconducting spin valve effect significantly increases. We attribute this dramatic effect to a homogenization of the Green function of the superconducting condensate over the S/F interface in the S/F1/F2 valve with a smooth surface of the S layer.

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High room-temperature magnetization in Co-doped TiO2 nanoparticles promoted by vacuum annealing for different durations

To clarify the contribution of oxygen vacancies to room-temperature ferromagnetism (RTFM) in cobalt doped TiO2(Co-TiO2),and in order to obtain the high level of magnetization suitable for spintronic devices,in this work,Co-TiO2 nano-particles are prepared via the sol-gel route,followed by vacuum annealing for different durations,and the influence of vacu-um annealing duration on the structure and room-temperature magnetism of the compounds is examined.The results reveal that with an increase in annealing duration,the concentration of oxygen vacancies rises steadily,while the saturation magnetiza-tion (Ms) shows an initial gradual increase,followed by a sharp decline,and even disappearance.The maximum Ms is as high as 1.19 emu/g,which is promising with respect to the development of spintronic devices.Further analysis reveals that oxygen va-cancies,modulated by annealing duration,play a critical role in tuning room-temperature magnetism.An appropriate concentra-tion of oxygen vacancies is beneficial in terms of promoting RTFM in Co-TiO2.However,excessive oxygen vacancies will result in a negative impact on RTFM,due to antiferromagnetic superexchange interactions originating from nearest-neighbor Co2+ions.     

2D Intrinsic Ferromagnetic MnP Single Crystals

2D intrinsic ferromagnetic materials are highly anticipated in spintronic devices due to their coveted 2D limited magnetism. However, 2D non‐layered intrinsic ferromagnets have received sporadic attention, which is largely attributed to the fact that their synthesis is still a great challenge. Significantly, manganese phosphide (MnP) is a promising non‐layered intrinsic ferromagnet with excellent properties. Herein, high‐quality 2D MnP single crystals formed over liquid metal tin (Sn) is demonstrated through a facile chemical vapor deposition technique. The introduction of liquid metal Sn provides a fertile ground for the growth of 2D MnP single crystals. Interestingly, 2D MnP single crystals maintain their intrinsic ferromagnetism and exhibit a Curie temperature above room temperature. The research enriches the diversity of 2D intrinsic ferromagnetic materials, opening up opportunities for further exploration of their unique properties and rich applications.     

Intrinsic Van Der Waals Magnetic Materials from Bulk to the 2D Limit: New Frontiers of Spintronics

2D van der Waals (vdW) magnets, which present intrinsic ferromagnetic/antiferromagnetic ground states at finite temperatures down to atomic‐layer thicknesses, open a new horizon in materials science and enable the potential development of new spin‐related applications. The layered structure of vdW magnets facilitates their atomic‐layer cleavability and magnetic anisotropy, which counteracts spin fluctuations, thereby providing an ideal platform for theoretically and experimentally exploring magnetic phase transitions in the 2D limit. With reduced dimensions, the susceptibility of 2D magnets to a large variety of external stimuli also makes them more promising than their bulk counterpart in various device applications. Here, the current status of characterization and tuning of the magnetic properties of 2D vdW magnets, particularly the atomic‐layer thickness, is presented. Various state‐of‐the‐art optical and electrical techniques have been applied to reveal the magnetic states of 2D vdW magnets. Other emerging 2D vdW magnets and future perspectives on the stacking strategy are also given; it is believed that they will excite more intensive research and provide unprecedented opportunities in the field of spintronics.