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We used a combination of polarized Raman spectroscopy experiment and model magnetism–phonon coupling calculations to study the rich magneto-Raman effect in the two-dimensional (2D) magnet CrI 3 . We reveal a layered-magnetism–assisted phonon scattering mechanism below the magnetic onset temperature, whose Raman excitation breaks time-reversal symmetry, has an antisymmetric Raman tensor, and follows the magnetic phase transitions across critical magnetic fields, on top of the presence of the conventional phonon scattering with symmetric Raman tensors in N -layer CrI 3 . We resolve in data and by calculations that the first-order A g phonon of the monolayer splits into an N -fold multiplet in N -layer CrI 3 due to the interlayer coupling ( N ≥ 2 ) and that the phonons within the multiplet show distinct magnetic field dependence because of their different layered-magnetism–phonon coupling. We further find that such a layered-magnetism–phonon coupled Raman scattering mechanism extends beyond first-order to higher-order multiphonon scattering processes. Our results on the magneto-Raman effect of the first-order phonons in the multiplet and the higher-order multiphonons in N -layer CrI 3 demonstrate the rich and strong behavior of emergent magneto-optical effects in 2D magnets and underline the unique opportunities of spin–phonon physics in vanmore »
Abstract Spin and lattice are two fundamental degrees of freedom in a solid, and their fluctuations about the equilibrium values in a magnetic ordered crystalline lattice form quasiparticles termed magnons (spin waves) and phonons (lattice waves), respectively. In most materials with strong spin-lattice coupling (SLC), the interaction of spin and lattice induces energy gaps in the spin wave dispersion at the nominal intersections of magnon and phonon modes. Here we use neutron scattering to show that in the two-dimensional (2D) van der Waals honeycomb lattice ferromagnetic CrGeTe 3 , spin waves propagating within the 2D plane exhibit an anomalous dispersion, damping, and breakdown of quasiparticle conservation, while magnons along the c axis behave as expected for a local moment ferromagnet. These results indicate the presence of dynamical SLC arising from the zero-temperature quantum fluctuations in CrGeTe 3 , suggesting that the observed in-plane spin waves are mixed spin and lattice quasiparticles fundamentally different from pure magnons and phonons.
The influence of crystal thickness and interlayer interactions on the properties of heavy ion irradiated MoS 2
Ion irradiation is a versatile tool to introduce controlled defects into two-dimensional (2D) MoS2on account of its unique spatial resolution and plethora of ion types and energies available. In order to fully realise the potential of this technique, a holistic understanding of ion-induced defect production in 2D MoS2crystals of different thicknesses is mandatory. X-ray photoelectron spectroscopy, electron diffraction and Raman spectroscopy show that thinner MoS2crystals are more susceptible to radiation damage caused by 225 keV Xe+ions. However, the rate of defect production in quadrilayer and bulk crystals is not significantly different under our experimental conditions. The rate at which S atoms are sputtered as a function of radiation exposure is considerably higher for monolayer MoS2, compared to bulk crystals, leading to MoO3formation. P-doping of MoS2is observed and attributed to the acceptor states introduced by vacancies and charge transfer interactions with adsorbed species. Moreover, the out-of-plane vibrational properties of irradiated MoS2crystals are shown to be strongly thickness-dependent: in mono- and bilayer MoS2, the confinement of phonons by defects results in a blueshift of the
mode. Whereas, a redshift is observed in bulk crystals due to attenuation of the effective restoring forces acting on S atoms caused by vacanciesmore »
Abstract Optical manipulation of coherent phonon frequency in two-dimensional (2D) materials could advance the development of ultrafast phononics in atomic-thin platforms. However, conventional approaches for such control are limited to doping, strain, structural or thermal engineering. Here, we report the experimental observation of strong laser-polarization control of coherent phonon frequency through time-resolved pump-probe spectroscopic study of van der Waals (vdW) materials Fe 3 GeTe 2 . When the polarization of the pumping laser with tilted incidence is swept between in-plane and out-of-plane orientations, the frequencies of excited phonons can be monotonically tuned by as large as 3% (~100 GHz). Our first-principles calculations suggest the strong planar and vertical inter-atomic interaction asymmetry in layered materials accounts for the observed polarization-dependent phonon frequencies, as in-plane/out-of-plane polarization modifies the restoring force of the lattice vibration differently. Our work provides insightful understanding of the coherent phonon dynamics in layered vdW materials and opens up new avenues to optically manipulating coherent phonons.
Recent years have witnessed a much broader use of Brillouin inelastic light-scattering spectroscopy for the investigation of phonons and magnons in novel materials, nanostructures and devices. Driven by the developments in instrumentation and the strong need for accurate knowledge on the energies of elemental excitations, Brillouin–Mandelstam spectroscopy is rapidly becoming an essential technique that is complementary to Raman inelastic light-scattering spectroscopy. We provide an overview of recent progress in the Brillouin light-scattering technique, focusing on the use of this photonic method for the investigation of confined acoustic phonons, phononic metamaterials and magnon propagation and scattering. This Review emphasizes the emerging applications of Brillouin–Mandelstam spectroscopy for phonon-engineered structures and spintronic devices, and concludes with a perspective on future directions.