Room Temperature Ferromagnetism Research Articles

Spin-degree manipulation for one-dimensional room-temperature ferromagnetism in a haldane system.

The intricate correlation between lattice geometry, topological behavior and charge degrees of freedom plays a key role in determining the physical and chemical properties of a quantum-magnetic system. Herein, we investigate the introduction of the unusual oxidation state as an alternative pathway to modulate the magnetic ground state in the well-known S = 1 Haldane system nickelate Y2BaNiO5 (YBNO). YBNO is topologically reduced to incorporate d9-Ni+ (S = 1/2) in the one-dimensional Haldane chain system. The random distribution of Ni+ for the first time results in the emergence of a one-dimensional ferromagnetic phase with a transition temperature far above room temperature. Theoretical calculations reveal that the antiferromagnetic interplay can evolve into ferromagnetic interactions with the presence of oxygen vacancies, which promotes the formation of ferromagnetic order within one-dimensional nickel chains. The unusual electronic instabilities in the nickel-based Haldane system may offer new possibilities towards unconventional physical and chemical properties from quantum interactions.

Prediction of intrinsic room-temperature ferromagnetism in two-dimensional CrInX2 (X = S, Se, Te) monolayers.

Herein, using density functional theory, novel two-dimensional (2D) CrInX2 (X = S, Se, Te) structures are predicted to be practical ferromagnetic (FM) semiconductors. Phonon vibrations and molecular dynamics simulations verified their structural and thermodynamic stability. Sizable fully spin-polarized band gaps of 1.03 and 0.69 eV are found for CrInS2 and CrInSe2, while CrInTe2 exhibits half-metallic band nature (at 0 K with a perfect lattice). The high magnetic anisotropy energies are responsible for their long-range spin polarization. The Curie temperatures (Tc) are estimated to be 347, 397 and 447 K for CrInS2, CrInSe2 and CrInTe2, respectively, all well above the room-temperature. The high Tc originates from unusual FM direct exchange, the efficient super-exchange coupling between neighboring Cr eg-orbitals with zero virtual exchange gaps and the presence of dual Cr-X-Cr super-exchange channels. Our systematic study of the CrInX2 monolayer suggests that it could be a promising material for spintronics applications.

Structure-dependent spin-polarized electron transport in twin-crystal Cu1-xEuxO semiconductors.

In this work, Eu-doped twin copper oxide (twin Cu1-xEuxO) was synthesized using the gas-liquid phase chemical deposition method in combination with high-temperature oxidation. The incorporation of Eu3+ ions was affected by their diffusivity and the related charge trapping mechanisms. The twin Cu1-xEuxO configuration exhibited significant room-temperature ferromagnetism. From our analysis, it was demonstrated that as the Eu3+ doping concentration increased, the saturation magnetization first increased and then gradually decreased, reaching a peak at 0.82 at%. A p-type to an n-type semiconducting transition was also recorded as the doping concentration increased. A significant anomalous Hall effect characterized by a maximum anomalous Hall coefficient of 1.65, and a maximum Hall conductivity mobility of 16.50 Ohm-1 cm-1 and 250.59 cm2 v-1 s-1, respectively, were derived for the twin Cu1-xEuxO, doped with 0.82 at% at room temperature. First-principles computational simulations were also conducted to elucidate the underlying mechanisms of the magnetic properties, the p-type to n-type transition, and the interplay between the spin-polarized states associated with 4f and carriers. In twin Cu1-xEuxO, the anomalous Hall effect originated from the contribution of the edge-to-jump scattering mechanism. The latter can be significantly enhanced by doping with Eu atoms, which yields the manifestation of the oblique scattering mechanism. Our work paves the way for the development of twin Cu1-xEuxO material structures, which emerge as an ideal candidate for future spintronic applications.

First-principles predictions of room-temperature ferromagnetism in orthorhombic MnX2 (X = O, S) monolayers.

Two-dimensional ferromagnets with high spin-polarization at ambient temperature are of considerable interest because they might be useful for making nanoscale spintronic devices. We report that even though bulk phases of MnO2 are generally antiferromagnetic with low ordering temperatures, the corresponding MnO2 and MnS2 monolayers are ferromagnetic, and MnS2 is a high temperature half metallic ferromagnet. Based on first-principles calculations, we find that the MnO2 monolayer is an intrinsic ferromagnetic semiconductor with a Curie temperature TC of ∼300 K, while the half-metallic MnS2 monolayer has a remarkably high TC of ∼1150 K. Both compounds have substantial magnetocrystalline anisotropy, out of plane in the case of MnO2 monolayers, and in plane along the b-axis of orthorhombic MnS2 monolayer. Interestingly, a metal-insulator phase transition occurs in the MnS2 monolayer when the applied biaxial strain is beyond -2%. Tuning near this metal-insulator transition offers additional possibilities for devices. The present work shows that MnX2 (X = O, S) monolayers have the properties required for ultrathin nano-spintronic devices.

Influence of adding manganese chromium-layered double oxide on the optical, magnetic and dielectric properties of cobalt spinel ferrite nanoparticles

Hydrotalcite-like materials such as layered double oxides (LDOs) are promising materials for many technological applications. Linking the multilayer structure of LDOs with the exceptional optical, magnetic, and dielectric properties of spinel ferrites could result in advanced nanocomposites for photovoltaic, magneto-recording, and high-frequency applications. For that purpose, nanocomposites of type manganese chromium-layered double oxide/cobalt spinel ferrite, (MnCr)-LDOx/CoFe2O4 (x = 1, 3, and 5 wt%), were produced by the co-precipitation route. X-ray diffraction (XRD) analysis showed the successful incorporation of MnCr-LDO in CoFe2O4 lattice. After a 5 wt% addition of MnCr-LDO, the lattice parameter of pure CoFe2O4 increased from 8.3832 Å to 8.4136 Å, the crystallite size increased from 18.7 nm to 21.7 nm, and the strain dropped from 2.15 to 2.04. Transmission electron microscopy (TEM) revealed cubic morphologies for (MnCr)-LDOx/CoFe2O4 nanocomposites. Two strong absorbance peaks appeared in the Ultraviolet- visible (UV-vis) spectra (at ∼270 and ∼370 cm−1). The energy band gap and Urbach energy were estimated for the prepared samples. The composite sample (MnCr)-LDO1 wt%/CoFe2O4 recorded the highest band gap values (Eg1 = 3.39 eV, Eg2 = 4.46 eV, and Eg3 = 5.89 eV), while the (MnCr)-LDO3 wt%/CoFe2O4 sample had a relatively high Urbach energy value (1.35 eV). Vibrating sample magnetometer (VSM) analysis showed room temperature ferromagnetic (RTFM) behavior for the prepared composites. The saturation magnetization (Ms) value declined as the MnCr-LDO addition to CoFe2O4 increased, and the (MnCr)-LDO3 wt%/CoFe2O4 sample acquired the highest Ms (64.428 emu g−1) among all the produced composites. Pure CoFe2O4 had a much higher coercivity (Hc = 1158.1 Oe) than (MnCr)-LDOx/CoFe2O4 (x = 1, 3, and 5 wt%) nanocomposites (Hc = 1119.8, 978.48, and 984.16 Oe). Moreover, complex impedance spectroscopy measurements were performed in frequency range of 50 Hz- 5 MHz using Nyquist plots and electric modulus analysis. Nyquist plots were fitted to an analogous electric circuit consisting of a resistor R1 connected in series to two parallel constant phase element- resistor circuits (CPE-R). On the other hand, a different circuit comprises of two CPE, capacitor (C1), and resistor all connected in parallel was used to model CoFe2O4.

Above-Room-Temperature Ferromagnetism in Copper-Doped Two-Dimensional Chromium-Based Nanosheets.

Two-dimensional ferromagnetic materials (2D-FMs) are expected to become ideal candidates for low-power, high-density information storage in next-generation spintronics devices due to their atomically ultrathin and intriguing magnetic properties. However, 2D-FMs with room-temperature Curie temperatures (Tc) are still rarely reported, which greatly hinders their research progress and practical applications. Herein, ultrathin Cu-doped Cr7Te8 FMs were successfully prepared and can achieve above-room-temperature ferromagnetism with perpendicular magnetic anisotropy via a facile chemical vapor deposition (CVD) method, which can be controlled down to an atomic thin layer of ∼3.4 nm. STEM-EDX quantitative analysis shows that the proportion of Cu to metal atoms is ∼5%. Moreover, based on the anomalous Hall effect (AHE) measurements in a six-terminal Hall bar device without any encapsulation as well as an out-of-plane magnetic field, the maximum Tc achieved ∼315 K when the thickness of the sample is ∼28.8 nm; even the ultrathin 7.6 nm sample possessed a near-room-temperature Tc of ∼275 K. Meanwhile, theoretical calculations elucidated the mechanism of the ferromagnetic enhancement of Cu-doped Cr7Te8 nanosheets. More importantly, the ferromagnetism of CVD-synthesized Cu-doped CrSe nanosheets can also be maintained above room temperature. Our work broadens the scope on room-temperature ferromagnets and their heterojunctions, promoting fundamental research and practical applications in next-generation spintronics.

Periodic oxygen-defective ZrO2−x films with room-temperature ferromagnetism produced by precisely controlling oxidation of metallic Zr foil

Ferromagnetism can be induced by introducing oxygen vacancies into metallic oxides. The oxygen deficiencies introduced into ZrO2 samples thus far have been present in unquantifiable concentrations and randomly scattered near the surface. We successfully produced room-temperature-ferromagnetic 9 μm-thick ZrO2−x films via a stepwise oxidation process consisting of annealing metallic Zr foil in air and under a controlled oxygen partial pressure. The ZrO2−x films are composed of a periodic structure with a spacing of 3–4 nm; this structure originated from the presence and absence of oxygen deficiencies. The unique structure in the ZrO2−x phase consisting of the periodic arrangements of oxygen deficiencies can be produced by the stepwise oxidation using Zr metal. Our proposed process should open the door for new applications of defect-driven ferromagnetic films of undoped magnetic oxides with a periodic oxygen-defective structure.

Hidden Valley Polarization, Piezoelectricity, and Dzyaloshinskii-Moriya Interactions of Janus Vanadium Dichalcogenides.

Due to the lack of inversion symmetry and the discovery of room-temperature ferromagnetism, two-dimensional semiconducting vanadium-based van der Waals transition-metal dichalcogenides (V-TMDs) are drawing attention for their possible application in spintronics and valleytronics. Here, we show the functional properties enriched by the broken inversion, out-of-plane mirror, and time-reversal symmetries of Janus H-VXY TMDs (X, Y = S, Se, Te). By first-principles calculations, we reveal the intrinsic xy easy-plane magnetism of the Janus vanadium-based TMD monolayers and systematically study their hidden valley polarization and giant magneto band structure. Their strong nearest-neighbor exchange strengths lead to near-room-temperature magnetic phase transitions. The Janus H-VXY system also exhibits piezoelectricity with nonzero e31 and e21. Interestingly, it is found that the right-handed Dzyaloshinskii-Moriya interaction has nonzero in-plane components in our Janus system, with fluctuating magnitudes determined by competence between relaxed bond-angle and atomic index of ligands.

Electronic structure and magnetic properties of CrI3 monolayer doped by rare earth metal atoms

CrI3 monolayer is a two-dimensional (2D) ferromagnetic (FM) semiconductor materials with broad application prospects in the field of spintronics due to its magnetic semiconductor feature and unique 2D structure. In this work, we employ first-principles calculations based on density functional theory to investigate the electronic structure and magnetic properties of CrI3 monolayer doped with rare earth (RE) metal atoms (RE = Sc, Y, La, Ce, Pr, Nd, Pm, Eu, Gd, Tm, and Lu). The results demonstrate that doping with RE atoms enables the control of total magnetic moments and a significantly enhancement of the Curie temperature of CrI3 monolayer. Especially, the Curie temperature of CrGdI6 monolayer reaches 347.58 K, which could be a promising candidate for realizing room temperature ferromagnetism. Furthermore, by applying strain and electric field, the CrREI6 monolayers exhibit metal, half-metal and spin gapless semiconductor properties. These findings not only provide valuable insights into the manipulation of electronic structure and magnetic properties in CrI3 monolayer but also establish RE doped CrI3 monolayer as a promising material for spintronic devices.

Efficient current-induced spin torques and field-free magnetization switching in a room-temperature van der Waals magnet

The discovery of magnetism in van der Waals (vdW) materials has established unique building blocks for the research of emergent spintronic phenomena. In particular, owing to their intrinsically clean surface without dangling bonds, the vdW magnets hold the potential to construct a superior interface that allows for efficient electrical manipulation of magnetism. Despite several attempts in this direction, it usually requires a cryogenic condition and the assistance of external magnetic fields, which is detrimental to the real application. Here, we fabricate heterostructures based on Fe 3 GaTe 2 flakes that have room-temperature ferromagnetism with excellent perpendicular magnetic anisotropy. The current-driven nonreciprocal modulation of coercive fields reveals a high spin-torque efficiency in the Fe 3 GaTe 2 /Pt heterostructures, which further leads to a full magnetization switching by current. Moreover, we demonstrate the field-free magnetization switching resulting from out-of-plane polarized spin currents by asymmetric geometry design. Our work could expedite the development of efficient vdW spintronic logic, memory, and neuromorphic computing devices.

Cooperative effects due to Zn–Sn replacement by Co-ions on the optical and magnetic properties of (ZnSn)1- xCoxO nanocomposites

In the present study, the structural, optical, and magnetic properties of (ZnSn)1-xCoxO nanocomposites (NCs) were reported. The transmission electron microscope (TEM) images of ZnSnO NCs showed mixed nanorods and nanosheets morphologies that completely transformed to mostly nanocubes with Co-ions incorporation. The optical band gap (Eg) of nanostructured ZnO, SnO, and ZnSnO NCs was 3.2, 4.5, and 3.9 eV, respectively. The estimated Eg value of all (ZnSn)1-xCoxO NCs was lower than the undoped ZnSnO NCs. The nanostructured ZnO revealed poor room-temperature ferromagnetic (RTFM) behavior whereas nanostructured SnO exhibited paramagnetic behavior at low magnetic field strength followed by diamagnetic behavior at high magnetic field strength. The (ZnSn)1-xCoxO NCs exhibited strong improvement in the RTFM, where the hybrid (ZnSn)60Co40O NCs exhibited the highest saturation magnetization (Ms) of 2 emu·g−1. This value was 5-times higher than the undoped ZnSnO NCs and 2-orders of magnitude higher than the pure ZnO phase. However, with increasing Co-content up to 50 %, the Ms was reduced to 1.16 emu·g−1 demonstrating the corruption of RTFM. The present study indicated the importance of composition utilization for tuning physical properties of (ZnSn)1-xCoxO NCs and improving the performance of these NCs in optoelectronic and spintronics applications.

The effect of composition on the structure, optical, and room-temperature ferromagnetic properties of hydrothermally synthesized (ZnSn)1-xCuxO nanocomposites

(ZnSn)1-xCuxO nanocomposites (NCs) with nanorods and nanosheet morphologies were synthesized by a facile hydrothermal technique. (ZnSn)1-xCuxO NCs exhibited a gradual band gap redshift from UV to visible spectral region with increasing Cu-content. The room temperature magnetic hysteresis loop indicated the improvement of room temperature ferromagnetic (RTFM) behavior of (ZnSn)1-xCuxO NCs compared with nanostructured ZnSnO NCs induced by the exchange interaction of Cu-bound polarons with the localized spins and free carriers. The (ZnSn)60Cu40O NCs exhibited the highest saturation magnetization (Ms) of 0.539 emu·g−1. Further increase in Cu-content resulted in the deterioration of crystalline domains and the reduction of Ms to 0.259 emu·g−1. This behavior revealed that the electronic and magnetic properties of (ZnSn)1-xCuxO NCs were so sensitive to the dopant concentration that need to be utilized for improving their performance as good candidate NCs for spintronic applications.

Growth of 2D Cr2 O3 -CrN Mosaic Heterostructures with Tunable Room-Temperature Ferromagnetism.

2D magnets have generated much attention due to their potential for spintronic devices. Heterostructures of 2D magnets are interesting platforms for exploring physical phenomena and applications. However, the controlled growth of 2D room-temperature ferromagnetic heterostructures is challenging. Here, one-pot chemical vapor deposition growth of stable 2D Cr2 O3 -CrN mosaic heterostructures (MHs) is reported with a controlled ratio of components that possess robust room-temperature ferromagnetism. The 2D MHs consist of Cr2 O3 flakes with embedded CrN subdomains and the CrN:Cr2 O3 ratio can be tuned from 0% to 100% during growth. By changing the CrN:Cr2 O3 ratio, the ferromagnetism of the MHs (e.g., saturation magnetization, coercive field), which originates from the interfacial coupling between Cr2 O3 and CrN, can be controlled. Importantly, the obtained Cr2 O3 -CrN MHs are stable in air at elevated temperatures and have robust ferromagnetism with Curie temperature >400K. This work presents a facile method for fabricating 2D MHs with tunable magnetism which will benefit high-temperature spintronics.

Tuning the magnetic properties of doped ZnS using transition metal doping: A multi-scale computational approach

Transition metal (TM)-doped dilute magnetic semiconductors (DMS) have emerged as promising materials for spintronic applications such as spin-polarized transport and information storage. However, achieving robust room-temperature ferromagnetism in DMS remains a key challenge. This work undertakes a comprehensive investigation of the effects of Ti- and Cr-doping and (Ti,Cr)-codoping on the structural, electronic, and magnetic properties of wurtzite ZnS using first-principles pseudopotential plane-wave self-consistent field calculations and Monte Carlo simulations. The first-principles DFT calculations were performed using the spin-polarized GGA+U approach to account for strong electron–electron interactions. Structural relaxations revealed expanded lattice parameters and bond lengths for the doped systems compared to pure ZnS, attributed to the larger ionic radii of the dopants. Formation energy calculations confirmed the thermodynamic stability of doping. The band structure and density of states analysis demonstrated the half-metallic nature of the doped ZnS systems with 100% spin polarization induced by strong hybridization between the TM-3d and S-3p states. This mediates robust ferromagnetic coupling, with total magnetic moments around 4-8 μB/cell depending on dopant type and concentration. To complement the zero-temperature DFT results, temperature-dependent Monte Carlo simulations using the single-spin flip Heat Bath algorithm were implemented. The modeling of magnetization, susceptibility, specific heat, and hysteresis loops enabled extracting Curie temperatures up to 427.6 K for 12.5% Cr-doped ZnS. The synergistic combination of first-principles DFT and Monte Carlo computational techniques provides significant insights into tailoring the magnetic properties of TM-doped ZnS dilute magnetic semiconductors. The tunability of structural, electronic, and magnetic characteristics through control of dopant selection and concentration demonstrates the promising potential of transition metal-doped ZnS for spintronic devices operable at room-temperature.

Room temperature ferroelectricity and ferromagnetism in Ni-substituted Bi5Ti3FeO15

Aurivillius-type bismuth layer-structured ferroelectric (BLSF) Bi5Ti3FeO15 (BTF) has recently attracted considerable attention as a typical multiferroic material because ferroelectric and magnetic orders coexist, but bulk BTF exhibits antiferromagnetic (AFM) orders and negligible intrinsic magnetoelectric (ME) coupling effects. In this study, nickel-substituted Bi5Ti3FeO15 (Bi5Ti3Fe0.5Ni0.5O15, abbreviated as BTF-Ni) was synthesized using a solid-state reaction method to explore and enhance both the magnetic and ferroelectric properties of BTF. Polarization-electric field P-E loops indicate that the BTF-Ni exhibits considerable maximum polarization P m of 11.9 μC/cm2 and remnant polarization P r of 5.8 μC/cm2, but still keeps a very high ferroelectric Curie temperature (FE T c) of 1029 K, which are much superior to those of pure BTF. Moreover, magnetization-magnetic field M-H loops indicate that BTF-Ni exhibits significant ferromagnetic properties with a large saturation magnetization M s of 60 memu/g, low coercive field H c of 31 Oe at room temperature, and a high ferromagnetic Curie temperature (FM T c) of 698 K, whereas pure BTF has an antiferromagnetic Néel temperature (T N) of 80 K. Our work suggests that nickel-substituted BTF is a potential room-temperature magnetoelectric multiferroic material.

Potential-tuned magnetic switches and half-metallicity transition in zigzag graphene nanoribbons

Realizing controllable room-temperature ferromagnetism in carbon-based materials is one of recent prospects. The magnetism in graphene nanostructures reported previously is mostly localized by breaking the local sublattice imbalance. Here, we predict a robustly potential-tuned ferromagnetic domain lying between the inter-chain carbon atoms inside the zigzag graphene nanoribbons. We show that the effective zigzag edges provide the strong correlation background through narrowing the band width, while the internal Van Hove filling (VHF) provides the strong ferromagnetic background inherited from the bulk. The induced ferromagnetism exhibit interesting switching effect when the nominal VHF crosses the intra- and inter-chain region by tuning the potential drops. We further observe a robust half-metallicity transition from one spin channel to another within the same magnetic phase. These novel properties provide promising ways to manipulate the spin degree of freedom in graphene nanostructures.

Effects of W/Co co-doping on the structural, multiferroic, dielectric and optical properties of filled tungsten bronze Ba4Sm2Fe2Nb8O30 ceramics

The structural, magnetic, ferroelectric, dielectric, magneto-dielectric and optical properties of W/Co co-substituted tungsten bronze Ba4Sm2Fe2Nb8-3x(W2Co)xO30 (0 ≤ x ≤ 0.3) ceramics were studied in detail. All the samples can be indexed with the tetragonal structure with the space group of P4bm. The room-temperature ferromagnetism with rather high ferromagnetic Curie temperature Tc was obtained in all compositions. The co-doping of W/Co ions obviously optimized the ferromagnetism and ferroelectricity. The composition x = 0.2 showed a superior multiferroicity with the remnant magnetization Mr of 0.15 emu/g and the remnant polarization Pr of 2.1μC/cm2 as well as the Tc of 886 K. The low-temperature relaxation was related to the thermal process of oxygen vacancies, while the another one around 300 K was ascribed to the localized hopping of electrons. The relative increment of magneto-dielectric constant (MDC) obeyed with the square term of magnetization in Ginzburg-Landau theory, implying the existence of intrinsic magneto-electric coupling effect. A relatively large MDC of 0.17 % was achieved in pure sample. In addition, two direct inter-band transitions with the narrow band gaps of ∼2.0 eV and ∼2.5 eV were demonstrated.

CO2 Stress-Driven Room Temperature Ferromagnetism of Ultrathin 2D Gallium Oxide.

Spintronic devices work by manipulating the spin of electrons other than charge transfer, which is of revolutionary significance and can largely reduce energy consumption in the future. Herein, ultrathin two-dimensional (2D) non-van der Waals (non-vdW) γ-Ga2O3 with room temperature ferromagnetism is successfully obtained by using supercritical CO2 (SC CO2). The stress effect of SC CO2 under different pressures selectively modulates the orientation and strength of covalent bonds, leading to the change of atomic structure including lattice expansion, introduction of O vacancy, and transition of Ga-O coordination (GaO4 and GaO6). Magnetic measurements show that pristine γ-Ga2O3 is nonferromagnetic, whereas the SC CO2 treated γ-Ga2O3 exhibits obvious ferromagnetic behavior with an optimal magnetization of 0.025emug-1 and a Curie temperature of 300 K.

Above-Room-Temperature Strong Ferromagnetism in 2D MnB Nanosheet.

Two-dimensional (2D) room-temperature (RT) ferromagnetic materials have amassed considerable interest in the field of fundamental physics for applications in next-generation spintronic devices owing to their physical properties. However, realizing strong RT ferromagnetism and a high Curie temperature (TC) in these 2D magnetic materials remains challenging. Herein, we develop a 2D MnB nanosheet for known 2D ferromagnets that demonstrates strong RT ferromagnetism and a record-high above-RT TC of ∼585.9 K. Through magnetic force microscopy, clear evidence of ferromagnetic behavior is observed at room temperature. Structural characterization and density functional theory calculations further reveal that (i) after exfoliation of bulk, -OH functional groups were introduced in addition to Mn-B bonds being formed, which increases MnB nanosheet TC to 585.9 K and (ii) the d3↑ spin configuration of Mn mainly contributed to the magnetic moment of MnB, and the hybridization between the dxz (dyz) and dz2 orbitals of the Mn atom provides a large contribution to magnetic anisotropy, which stabilizes the magnetic property of MnB. Our findings establish a strong experimental foundation for 2D MnB nanosheets as ideal materials for the construction of spintronic devices.

Non-stoichiometry induced 2H–1T phase interfaces and room-temperature ferromagnetism in defective molybdenum selenide

Magnetic semiconducting materials offer tremendous prospects for spin electronics but is challenging to achieve room-temperature ferromagnetism with unambiguous origin. Herein, a non-stoichiometry strategy is proposed to induce tunable magnetization in MoSe2−x nanoflowers via vacancy-controlled 2H–1T phase transition. The resultant MoSe2−x exhibits robust room-temperature ferromagnetism with significant positive correlation to the content of 1T phase and 2H–1T interfaces. Significant magnetic hysteresis and Curie transition above room temperature have been achieved, confirming the ferromagnetic feature of MoSe2−x. To examine the origin of ferromagnetism, formation energy and spin-polarized calculations have been conducted, indicating that the Se vacancy is beneficial for the formation of the 1T phase and interfacial spin polarization. Localized magnetic moments induced at the 2H–1T interfaces exhibit enhanced magnetism as compared to the net moments from the 1T orbital splitting, giving rise to strong coupling bound magnetic polarons. This work not only advances the understanding on the origin of magnetism in magnetic semiconductors, but also provides an effective route to generate ferromagnetism by defect and/or interface engineering that could be applied to multiferroics, spintronics, and valleytronics.