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 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.
Circularly polarized light carries light spin angular momentum, which may lead helicity-resolved Raman scattering to be sensitive to the electronic spin configuration in magnetic materials. Here, we demonstrate that all Raman modes in the 2D ferromagnet VI3 show different scattering intensities to left and right circularly polarized light at low temperatures, which gives direct evidence of the time-reversal symmetry breaking. By measuring the circular polarization of the dominant Raman mode with respect to the temperature and magnetic field, the ferromagnetic (FM) phase transition and hysteresis behavior can be clearly resolved. Besides the lattice excitations, quasielastic scattering is detected in the paramagnetic phase, and it gradually evolves into the acoustic magnon mode at 18.5 cm–1 in the FM state, which gives the spin wave gap that results from large magnetic anisotropy. Our findings demonstrate that helicity-resolved Raman spectroscopy is an effective tool to directly probe the ferromagnetism in 2D magnets.
One of the most promising avenues in 2D materials research is the synthesis of antiferromagnets employing 2D van der Waals (vdW) magnets. However, it has proven challenging, due in part to the complicated fabrication process and undesired adsorbates as well as the significantly deteriorated ferromagnetism at atomic layers. Here, the engineering of the antiferromagnetic (AFM) interlayer exchange coupling between atomically thin yet ferromagnetic CrTe 2 layers in an ultra-high vacuum-free 2D magnetic crystal, Cr 5 Te 8 is reported. By self-introducing interstitial Cr atoms in the vdW gaps, the emergent AFM ordering and the resultant giant magnetoresistance effect are induced. A large negative magnetoresistance (10%) with a plateau-like feature is revealed, which is consistent with the AFM interlayer coupling between the adjacent CrTe 2 main layers in a temperature window of 30 K below the Néel temperature. Notably, the AFM state has a relatively weak interlayer exchange coupling, allowing a switching between the interlayer AFM and ferromagnetic states at moderate magnetic fields. This work represents a new route to engineering low-power devices that underpin the emerging spintronic technologies, and an ideal laboratory to study 2D magnetism.
The intrinsic magnetic topological insulator MnBi 2 Te 4 has attracted significant interest recently as a promising platform for exploring exotic quantum phenomena. Here we report that, when atomically thin MnBi 2 Te 4 is deposited on a substrate such as silicon oxide or gold, there is a very strong mechanical coupling between the atomic layer and the supporting substrate. This is manifested as an intense low-frequency breathing Raman mode that is present even for monolayer MnBi 2 Te 4 . Interestingly, this coupling turns out to be stronger than the interlayer coupling between the MnBi 2 Te 4 atomic layers. We further found that these low-energy breathing modes are highly sensitive to sample degradation, and they become drastically weaker upon ambient air exposure. This is in contrast to the higher energy optical phonon modes which are much more robust, suggesting that the low-energy Raman modes found here can be an effective indicator of sample quality.
The development of the dry transfer method provides an abundant platform to construct various heterostructures of two-dimensional materials. However, the surface and interface cleanliness are essential to realize high electronical performance of heterostructures devices. Here, we demonstrated thermal annealing effect on the mobility and electrical transport properties of graphene on hexagonal boron nitride heterostructures devices. With different annealing temperature recipes for graphene on hexagonal boron nitride devices, we found annealing temperature at 300 °C can clean resist residual and achieve high mobility. Atomic force microscopy results also present a clean surface and small average root mean square roughness as low as 210 pm. Well defined oscillations and plateaus of electrical transport at low magnetic field indicate a high-quality graphene surface.
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