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Register a new userTuning Inelastic Light Scattering via Symmetry Control in 2D Magnet CrI$_3$
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The coupling between spin and charge degrees of freedom in a crystal imparts strong optical signatures on scattered electromagnetic waves. This has led to magneto-optical effects with a host of applications, from the sensitive detection of local magnetic order to optical modulation and data storage technologies. Here, we demonstrate a new magneto-optical effect, namely, the tuning of inelastically scattered light through symmetry control in atomically thin chromium triiodide (CrI$_3$). In monolayers, we found an extraordinarily large magneto-optical Raman effect from an A$_{1g}$ phonon mode due to the emergence of ferromagnetic order. The linearly polarized, inelastically scattered light rotates by ~40$^o$, more than two orders of magnitude larger than the rotation from MOKE under the same experimental conditions. In CrI$_3$ bilayers, we show that the same A$_{1g}$ phonon mode becomes Davydov-split into two modes of opposite parity, exhibiting divergent selection rules that depend on inversion symmetry and the underlying magnetic order. By switching between the antiferromagnetic states and the fully spin-polarized states with applied magnetic and electric fields, we demonstrate the magnetoelectrical control over their selection rules. Our work underscores the unique opportunities provided by 2D magnets for controlling the combined time-reversal and inversion symmetries to manipulate Raman optical selection rules and for exploring emergent magneto-optical effects and spin-phonon coupled physics.
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The recent discovery of 2D magnets has revealed various intriguing phenomena due to the coupling between spin and other degree of freedoms (such as helical photoluminescence, nonreciprocal SHG). Previous research on the spin-phonon coupling effect mainly focuses on the renormalization of phonon frequency. Here we demonstrate that the Raman polarization selection rules of optical phonons can be greatly modified by the magnetic ordering in 2D magnet CrI$_3$. For monolayer samples, the dominant A$rm_{1g}$ peak shows abnormally high intensity in the cross polarization channel at low temperature, which is forbidden by the selection rule based on the lattice symmetry. While for bilayer, this peak is absent in the cross polarization channel for the layered antiferromagnetic (AFM) state and reappears when it is tuned to the ferromagnetic (FM) state by an external magnetic field. Our findings shed light on exploring the emergent magneto-optical effects in 2D magnets.
Exfoliated chromium triiodide (CrI$_3$) is a layered van der Waals (vdW) magnetic insulator that consists of ferromagnetic layers coupled through antiferromagnetic interlayer exchange. The resulting permutations of magnetic configurations combined with the underlying crystal symmetry produces tunable magneto-optical phenomena that is unique to the two-dimensional (2D) limit. Here, we report the direct observation of 2D magnons through magneto-Raman spectroscopy with optical selection rules that are strictly determined by the honeycomb lattice and magnetic states of atomically thin CrI$_3$. In monolayers, we observe an acoustic magnon mode of ~0.3 meV with cross-circularly polarized selection rules locked to the magnetization direction. These unique selection rules arise from the discrete conservation of angular momentum of photons and magnons dictated by threefold rotational symmetry in a rotational analogue to Umklapp scattering. In bilayers, by tuning between the layered antiferromagnetic and ferromagnetic-like states, we observe the switching of two magnon modes. The bilayer structure also enables Raman activity from the optical magnon mode at ~17 meV (~4.2 THz) that is otherwise Raman-silent in the monolayer. From these measurements, we quantitatively extract the spin wave gap, magnetic anisotropy, intralayer and interlayer exchange constants, and establish 2D magnets as a new system for exploring magnon physics.
The magnetic properties in two-dimensional van der Waals materials depend sensitively on structure. CrI3, as an example, has been recently demonstrated to exhibit distinct magnetic properties depending on the layer thickness and stacking order. Bulk CrI3 is ferromagnetic (FM) with a Curie temperature of 61 K and a rhombohedral layer stacking, while few-layer CrI3 has a layered antiferromagnetic (AFM) phase with a lower ordering temperature of 45 K and a monoclinic stacking. In this work, we use cryogenic magnetic force microscopy to investigate CrI3 flakes in the intermediate thickness range (25 - 200 nm) and find that the two types of magnetic orders hence the stacking orders can coexist in the same flake, with a layer of ~13 nm at each surface being in the layered AFM phase similar to few-layer CrI3 and the rest in the bulk FM phase. The switching of the bulk moment proceeds through a remnant state with nearly compensated magnetic moment along the c-axis, indicating formation of c-axis domains allowed by a weak interlayer coupling strength in the rhombohedral phase. Our results provide a comprehensive picture on the magnetism in CrI3 and point to the possibility of engineering magnetic heterostructures within the same material.
The physical properties of two-dimensional van der Waals (2D vdW) crystals depend sensitively on the interlayer coupling, which is intimately connected to the stacking arrangement and the interlayer spacing. For example, simply changing the twist angle between graphene layers can induce a variety of correlated electronic phases, which can be controlled further in a continuous manner by applying hydrostatic pressure to decrease the interlayer spacing. In the recently discovered 2D magnets, theory suggests that the interlayer exchange coupling strongly depends on layer separation, while the stacking arrangement can even change the sign of the magnetic exchange, thus drastically modifying the ground state. Here, we demonstrate pressure tuning of magnetic order in the 2D magnet CrI3. We probe the magnetic states using tunneling and scanning magnetic circular dichroism microscopy measurements. We find that the interlayer magnetic coupling can be more than doubled by hydrostatic pressure. In bilayer CrI3, pressure induces a transition from layered antiferromagnetic to ferromagnetic phases. In trilayer CrI3, pressure can create coexisting domains of three phases, one ferromagnetic and two distinct antiferromagnetic. The observed changes in magnetic order can be explained by changes in the stacking arrangement. Such coupling between stacking order and magnetism provides ample opportunities for designer magnetic phases and functionalities.
Crystal symmetry governs the nature of electronic Bloch states. For example, in the presence of time reversal symmetry, the orbital magnetic moment and Berry curvature of the Bloch states must vanish unless inversion symmetry is broken. In certain 2D electron systems such as bilayer graphene, the intrinsic inversion symmetry can be broken simply by applying a perpendicular electric field. In principle, this offers the remarkable possibility of switching on/off and continuously tuning the magnetic moment and Berry curvature near the Dirac valleys by reversible electrical control. Here we demonstrate this principle for the first time using bilayer MoS2, which has the same symmetry as bilayer graphene but has a bandgap in the visible that allows direct optical probing of these Berry-phase related properties. We show that the optical circular dichroism, which reflects the orbital magnetic moment in the valleys, can be continuously tuned from -15% to 15% as a function of gate voltage in bilayer MoS2 field-effect transistors. In contrast, the dichroism is gate-independent in monolayer MoS2, which is structurally non-centrosymmetric. Our work demonstrates the ability to continuously vary orbital magnetic moments between positive and negative values via symmetry control. This represents a new approach to manipulating Berry-phase effects for applications in quantum electronics associated with 2D electronic materials.
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