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Register a new userMagnetic order induced polarization anomaly of Raman scattering in 2D magnet CrI$_3$
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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.
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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.
Antiferromagnetism (AF) in AB-stacked centrosymmetric bilayer (BL) CrI$_3$ breaks both spatial inversion ($P$) and time-reversal ($T$) symmetries but maintains the combined $PT$ symmetry, thus inducing novel second-order nonlinear optical (NLO) responses such as second-harmonic generation (SHG), linear electric-optic effect (LEO) and bulk photovoltaic effect (BPVE). In this work, we calculate AF-induced NLO responses of the BL CrI$_3$ based on the density functional theory with the generalized gradient approximation (GGA) plus onsite Coulomb correlation (U), i.e., the GGA+U method. Interestingly, we find that the magnetic SHG, LEO and photocurrent in the AF BL CrI$_3$ are huge, being comparable or even larger than that of the well-known nonmagnetic noncentrosymmetric semiconductors. For example, the calculated SHG coefficients are in the same order of magnitude as that of MoS$_2$ monolayer (ML), the most promising 2D material for NLO devices. The calculated LEO coefficients are almost three times larger than that of MoS$_2$ ML. The calculated NLO photocurrent in the CrI$_3$ BL is among the largest values predicted so far for the BPVE materials. On the other hand, unlike nonmagnetic semiconductors, the NLO responses in the AF BL CrI$_3$ are nonreciprocal and also switchable by rotating magnetization direction. Therefore, our interesting findings indicate that the AF BL CrI$_3$ will not only provide a valuable platform for exploring new physics of low-dimensional magnetism but also have promising applications in magnetic NLO and LEO devices such as frequency conversion, electro-optical switches, and light signal modulators as well as high energy conversion efficiency photovoltaic solar cells.
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.
Spin-orbit torque enables electrical control of the magnetic state of ferromagnets or antiferromagnets. In this work we consider the spin-orbit torque in the 2-d Van der Waals antiferromagnetic bilayer CrI$_3$, in the $n$-doped regime. In the purely antiferromagnetic state, two individually inversion-symmetry broken layers of CrI$_3$ form inversion partners, like the well-studied CuMnAs and Mn$_2$Au. However, the exchange and anisotropy energies are similar in magnitude, unlike previously studied antiferromagnets, which leads to qualitatively different behaviors in this material. Using a combination of first-principles calculations of the spin-orbit torque and an analysis of the ensuing spin dynamics, we show that the deterministic electrical switching of the Neel vector is the result of dampinglike spin-orbit torque, which is staggered on the magnetic sublattices.
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