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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 (SiNx). Here, a seeded growth technique for crystallizing CrTe2films 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 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.more » « less
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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.more » « less
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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.more » « less
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Optical excitation of chiral phonons plays a vital role in studying the phonon-driven magnetic phenomena in solids. Transition metal dichalcogenides host chiral phonons at high symmetry points of the Brillouin zone, providing an ideal platform to explore the interplay between chiral phonons and valley degree of freedom. Here, we investigate the helicity-resolved magneto-Raman response of monolayer MoS2 and identify a doubly degenerate Brillouin-zone-center chiral phonon mode at ∼270cm−1. Our wavelength- and temperature-dependent measurements show that this chiral phonon is activated through the resonant excitation of 𝐴 exciton. Under an out-of-plane magnetic field, the chiral phonon exhibits giant Zeeman splitting, which corresponds to an effective magnetic moment of ∼2.5𝜇𝐵. Moreover, we carry out theoretical calculations based on the morphic effects in nonmagnetic crystals, which reproduce the linear Zeeman splitting and Raman cross section of the chiral phonon. Our study provides important insights into lifting the chiral phonon degeneracy in an achiral covalent material, paving a route to excite and control chiral phonons.more » « less
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The oxides of platinum group metals are promising for future electronics and spintronics due to the delicate interplay of spin-orbit coupling and electron correlation energies. However, their synthesis as thin films remains challenging due to their low vapour pressures and low oxidation potentials. Here we show how epitaxial strain can be used as a control knob to enhance metal oxidation. Using Ir as an example, we demonstrate the use of epitaxial strain in engineering its oxidation chemistry, enabling phase-pure Ir or IrO2 films despite using identical growth conditions. The observations are explained using a density-functional-theory-based modified formation enthalpy framework, which highlights the important role of metal-substrate epitaxial strain in governing the oxide formation enthalpy. We also validate the generality of this principle by demonstrating epitaxial strain effect on Ru oxidation. The IrO2 films studied in our work further revealed quantum oscillations, attesting to the excellent film quality. The epitaxial strain approach we present could enable growth of oxide films of hard-to-oxidize elements using strain engineering.more » « less
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Two-dimensional van der Waals (vdWs) materials have gathered a lot of attention recently. However, the majority of these materials have Curie temperatures that are well below room temperature, making it challenging to incorporate them into device applications. In this work, we synthesized a room-temperature vdW magnetic crystal Fe5GeTe2 with a Curie temperature T$$_c = 332$$ K, and studied its magnetic properties by vibrating sample magnetometry (VSM) and broadband ferromagnetic resonance (FMR) spectroscopy. The experiments were performed with external magnetic fields applied along the c-axis (H$$\parallel$$c) and the ab-plane (H$$\parallel$$ab), with temperatures ranging from 300 to 10 K. We have found a sizable Landé g-factor difference between the H$$\parallel$$c and H$$\parallel$$ab cases. In both cases, the Landé g-factor values deviated from g = 2. This indicates contribution of orbital angular momentum to the magnetic moment. The FMR measurements reveal that Fe5GeTe2 has a damping constant comparable to Permalloy. With reducing temperature, the linewidth was broadened. Together with the VSM data, our measurements indicate that Fe5GeTe2 transitions from ferromagnetic to ferrimagnetic at lower temperatures. Our experiments highlight key information regarding the magnetic state and spin scattering processes in Fe5GeTe2, which promote the understanding of magnetism in Fe5GeTe2, leading to implementations of Fe5GeTe2 based room-temperature spintronic devices.more » « less
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