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Abstract Realization of large effective phonon magnetic moment in monolayer MoS₂has established an important route for exploring intriguing magnetic phenomena in a nonmagnetic material. The sizable coupling between the orbital transition and the circularly polarized phonon results in the large effective phonon magnetic moment. In this work, using magneto-Raman spectroscopy, we investigate substitutional doping of magnetic atoms as a tuning knob of the electronic and phononic properties of MoS₂. We show that Fe-doping polarizes the spin of the conduction bands and introduces a localized Fe band underneath the conduction band. As a result, an additional orbital transition between the Mo 4dand Fe 3dstates emerges, producing an orbital-phonon hybridized mode at 283 cm⁻¹. Our magnetic field dependent measurements demonstrate that this new mode carries 2.8 ${\mu }_{\mathrm{B}}$effective phonon magnetic moment, which is comparable to that of the undoped MoS₂. Moreover, even though a long-range magnetic order is absent in Fe-doped MoS₂, the local magnetic moment of Fe modifies the nature of the spin fluctuation, producing monotonically increasing quasielastic scattering spectral weight as temperature decreases. Our results highlight two-dimensional dilute magnetic semiconductors synthesized by substitutional doping as a promising material platform to manipulate the phonon magnetic moment through orbital-phonon coupling. 

Abstract 2D van der Waals (vdW) magnets open landmark horizons in the development of innovative spintronic device architectures. However, their fabrication with large scale poses challenges due to high synthesis temperatures (>500 °C) and difficulties in integrating them with standard complementary metal‐oxide semiconductor (CMOS) technology on amorphous substrates such as silicon oxide (SiO₂) and silicon nitride (SiN_x). Here, a seeded growth technique for crystallizing CrTe₂films on amorphous SiN_x/Si and SiO₂/Si substrates with a low thermal budget is presented. This fabrication process optimizes large‐scale, granular atomic layers on amorphous substrates, yielding a substantial coercivity of 11.5 kilo‐oersted, attributed to weak intergranular exchange coupling. Field‐driven Néel‐type stripe domain dynamics explain the amplified coercivity. Moreover, the granular CrTe₂devices on Si wafers display significantly enhanced magnetoresistance, more than doubling that of single‐crystalline counterparts. Current‐assisted magnetization switching, enabled by a substantial spin–orbit torque with a large spin Hall angle (85) and spin Hall conductivity (1.02 ×  10⁷ℏ/2e  Ω⁻¹  m⁻¹), is also demonstrated. These observations underscore the proficiency in manipulating crystallinity within integrated 2D magnetic films on Si wafers, paving the way for large‐scale batch manufacturing of practical magnetoelectronic and spintronic devices, heralding a new era of technological innovation. 

Non-collinear spin texture has attracted great attention since it provides an important probe of the interaction between electron and topological spin textures. While it has been widely reported in chiral magnets, oxide heterostructures, and hybrid systems such as ferromagnet/heavy metal and ferromagnet/topological insulators, the study of non-collinear spin texture in two-dimensional (2D) van der Waals (vdW) dilute magnetic semiconductor (DMS) monolayers is relatively lacking, hindering the understanding at the atomically thin scale. Here, we probe the temperature-dependent antisymmetric humps in Hall resistivity by utilizing the proximity coupling of Fe-doped monolayer WSe2 (Fe:WSe2) synthesized using chemical vapor deposition on a Pt Hall bar. Multiple characterization methods were employed to demonstrate that Fe atoms substitutionally replace W atoms, making a 2D vdW DMS at room temperature. Distinct from the intrinsic anomalous Hall effect, we found the transverse Hall resistivity of Fe:WSe2 displaying two additional antisymmetric peak features in the temperature-dependent measurements. These peaks are attributed to the magnetic features at the Fe:WSe2 and Pt interface. Our work shows that a DMS synthesized from 2D vdW transition metal dichalcogenides is promising for realizing magnetic and spintronic applications. 

Perovskite oxide heterostructures host a large number of interesting phenomena such as ferroelectricity, which are often driven by octahedral distortions in the crystal that may induce polarization. SrHfO3 (SHO) is a perovskite oxide with a pseudocubic lattice parameter of 4.08 Å that previous density functional theory (DFT) calculations suggest can be stabilized in a ferroelectric P4mm phase when stabilized with sufficient compressive strain. Additionally, it is insulating and possesses a large band gap and a high dielectric constant, making it an ideal candidate for oxide electronic devices. To test the viability of epitaxial strain as a driver of ferroic phase transitions, SHO films were grown by hybrid molecular beam epitaxy (hMBE) with a tetrakis(ethylmethylamino)hafnium(IV) source on GdScO3 and TbScO3 substrates. Strained SHO phases were characterized using X-ray diffraction, X-ray absorption spectroscopy, and scanning transmission electron microscopy to determine the space group of the strained films, with the results compared to those of DFT-optimized models of phase stability versus strain. Contrary to past reports, we find that compressively strained SrHfO3 undergoes octahedral tilt distortions without associated ferroelectric polarization and most likely takes on the I4/mcm phase with the a0a0c– tilt pattern. 

Recent helicity−resolved magneto−Raman spectroscopy measurement demonstrates large effective phonon magnetic moments of ~2.5 $$\mu_B$$ in monolayer MoS$$_2$$, highlighting resonant excitation of bright excitons as a feasible route to activate $$\Gamma$$−point circularly polarized phonons in transition metal dichalcogenides. However, a microscopic picture of this intriguing phenomenon remains lacking. In this work, we show that an orbital transition between the split conduction bands ($$\Delta_0$$ = 4 meV) of MoS$$_2$$ couples to the doubly degenerate $$E^{′′}$$ phonon mode ($$\Omega_0$$ = 33 meV), forming two hybridized states. Our phononic and electronic Raman scattering measurements capture these two states: (i) one with predominantly phonon contribution in the helicity−switched channels, and (ii) one with primarily orbital contribution in the helicity−conserved channels. An orbital−phonon coupling model successfully reproduces the large effective magnetic moments of the circularly polarized phonons and explains their thermodynamic properties. Strikingly, the Raman mode from the orbital transition is superimposed on a strong quasi−elastic scattering background, indicating the presence of spin fluctuations. As a result, the electrons excited to the conduction bands through the exciton exhibit paramagnetic behavior although MoS$$_2$$ is generally considered as a non-magnetic material. By depositing nanometer−thickness nickel thin films on monolayer MoS$$_2$$, we tune the electronic structure so that the A exciton perfectly overlaps with the 633 nm laser. The optimization of resonance excitation leads to pronounced tunability of the orbital−phonon hybridized states. Our results generalize the orbital−phonon coupling model of effective phonon magnetic moments to material systems beyond the paramagnets and magnets. 

Realization of large effective phonon magnetic moment in monolayer MoS$$_2$$ has established an important route for exploring intriguing magnetic phenomena in a nonmagnetic material. The sizable coupling between the orbital transition and the circularly polarized phonon results in the large effective phonon magnetic moment. In this work, using magneto-Raman spectroscopy, we investigate substitutional doping of magnetic atoms as a tuning knob of the electronic and phononic properties of MoS$$_2$$. We show that Fe-doping polarizes the spin of the conduction bands and introduces a localized Fe band underneath the conduction band. As a result, an additional orbital transition between the Mo 4$$d$$ and Fe 3$$d$$ states emerges, producing an orbital-phonon hybridized mode at 283 cm$$^{-1}$$. Our magnetic field dependent measurements demonstrate that this new mode carries 2.8 $$\mu_B$$ effective phonon magnetic moment, which is comparable to that of the undoped MoS$$_2$$. Moreover, even though a long-range magnetic order is absent in Fe-doped MoS$$_2$$, the local magnetic moment of Fe modifies the nature of the spin fluctuation, producing monotonically increasing quasielastic scattering spectral weight as temperature decreases. Our results highlight two-dimensional dilute magnetic semiconductors synthesized by substitutional doping as a promising material platform to manipulate the phonon magnetic moment through orbital-phonon coupling. 

The discovery of atomic monolayer magnetic materials has stimulated intense research activities in the two-dimensional (2D) van der Waals (vdW) materials community. The field is growing rapidly and there has been a large class of 2D vdW magnetic compounds with unique properties, which provides an ideal platform to study magnetism in the atomically thin limit. In parallel, based on tunneling magnetoresistance and magneto-optical effect in 2D vdW magnets and their heterostructures, emerging concepts of spintronic and optoelectronic applications such as spin tunnel field-effect transistors and spin-filtering devices are explored. While the magnetic ground state has been extensively investigated, reliable characterization and control of spin dynamics play a crucial role in designing ultrafast spintronic devices. Ferromagnetic resonance (FMR) allows direct measurements of magnetic excitations, which provides insight into the key parameters of magnetic properties such as exchange interaction, magnetic anisotropy, gyromagnetic ratio, spin-orbit coupling, damping rate, and domain structure. In this review article, we present an overview of the essential progress in probing spin dynamics of 2D vdW magnets using FMR techniques. Given the dynamic nature of this field, we focus mainly on broadband FMR, optical FMR, and spin-torque FMR, and their applications in studying prototypical 2D vdW magnets. We conclude with the recent advances in laboratory- and synchrotron-based FMR techniques and their opportunities to broaden the horizon of research pathways into atomically thin magnets. 

2D van der Waals (vdW) magnets open landmark horizons in the development of innovative spintronic device architectures. However, their fabrication with large scale poses challenges due to high synthesis temperatures (>500 °C) and difficulties in integrating them with standard complementary metal-oxide semiconductor (CMOS) technology on amorphous substrates such as silicon oxide (SiO2) and silicon nitride (SiNx). Here, a seeded growth technique for crystallizing CrTe2 films on amorphous SiNx/Si and SiO2/Si substrates with a low thermal budget is presented. This fabrication process optimizes large-scale, granular atomic layers on amorphous substrates, yielding a substantial coercivity of 11.5 kilo-oersted, attributed to weak intergranular exchange coupling. Field-driven Néel-type stripe domain dynamics explain the amplified coercivity. Moreover, the granular CrTe2 devices on Si wafers display significantly enhanced magnetoresistance, more than doubling that of single-crystalline counterparts. Current-assisted magnetization switching, enabled by a substantial spin–orbit torque with a large spin Hall angle (85) and spin Hall conductivity (1.02 ×  107 ℏ/2e  Ω⁻¹  m⁻¹), is also demonstrated. These observations underscore the proficiency in manipulating crystallinity within integrated 2D magnetic films on Si wafers, paving the way for large-scale batch manufacturing of practical magnetoelectronic and spintronic devices, heralding a new era of technological innovation.