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Register a new userMagneto-optical response of chromium trihalide monolayers: chemical trends
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Added by
Alejandro Molina-Sanchez Ph.D
Publication date
2019
fields
Physics
and research's language is
English
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Chromium trihalides (CrI$_3$, CrBr$_3$ and CrCl$_3$) form a prominent family of isostructural insulating layered materials in which ferromagnetic order has been observed down to the monolayer. Here we provide a comprehensive computational study of magneto-optical properties that are used as probes for the monolayer ferromagnetic order: magnetic circular dichroism and magneto-optic Kerr effect. Using a combination of density functional and Bethe-Salpeter theories, we calculate both the optical absorption and the magneto-optical Kerr angle spectra, including both excitonic effects and spinorial wave functions. We compare the magneto-optical response of the chromium trihalides series and we find that its strength is governed by the spin-orbit coupling of the ligand atoms (I, Br, Cl).
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The mechanical properties of magnetic materials are instrumental for the development of the magnetoelastic theory and the optimization of strain-modulated magnetic devices. In particular, two-dimensional (2D) magnets hold promise to enlarge these concepts into the realm of low-dimensional physics and ultrathin devices. However, no experimental study on the intrinsic mechanical properties of the archetypal 2D magnet family of the chromium trihalides has thus far been performed. Here, we report the room temperature layer-dependent mechanical properties of atomically thin CrI3 and CrCl3, finding that bilayers of CrI3 and CrCl3 have Youngs moduli of 62.1 GPa and 43.4 GPa, with the highest sustained strain of 6.09% and 6.49% and breaking strengths of 3.6 GPa and 2.2 GPa, respectively. Both the elasticity and strength of the two materials decrease with increased thickness, which is attributed to a weak interlayer interaction that enables interlayer sliding under low levels of applied load. The mechanical properties observed in the few-layer chromium trihalide crystals provide evidence of outstanding plasticity in these materials, which is qualitatively demonstrated in their bulk counterparts. This study will contribute to various applications of the van der Waals magnetic materials, especially for their use in magnetostrictive and flexible devices.
The discovery of spontaneous magnetism in van der Waal (vdW) magnetic monolayers has opened up an unprecedented platform for investigating magnetism in purely two-dimensional systems. Recently, it has been shown that the magnetic properties of vdW magnets can be easily tuned by adjusting the relative composition of halides. Motivated by these experimental advances, here we derive a model for a trihalide CrClBrI monolayer from symmetry principles and we find that, in contrast to its single-halide counterparts, it can display highly anisotropic nearest- and next-to-nearest neighbor Dzyaloshinskii-Moriya and Heisenberg interactions. Depending on the parameters, the DM interactions are responsible for the formation of exotic chiral spin states, such as skyrmions and spin cycloids, as shown by our Monte Carlo simulations. Focusing on a ground state with a two-sublattice unit cell, we find spin-wave bands with nonvanishing Chern numbers. The resulting magnon edge states yield a magnon thermal Hall conductivity that changes sign as function of temperature and magnetic field, suggesting chromium trihalides as a candidate for testing topological magnon transport in two-dimensional noncollinear spin systems.
We perform photoluminescence experiments at 4K on two different transition metal diselenide monolayers, namely MoSe2 and WSe2 in magnetic fields $B_z$ up to 9T applied perpendicular to the sample plane. In MoSe2 monolayers the valley polarization of the neutral and the charged exciton (trion) can be tuned by the magnetic field, independent of the excitation laser polarization. In the investigated WSe2 monolayer sample the evolution of the trion valley polarization depends both on the applied magnetic field and the excitation laser helicity, while the neutral exciton valley polarization depends only on the latter. Remarkably we observe a reversal of the sign of the trion polarization between WSe2 and MoSe2. For both systems we observe a clear Zeeman splitting for the neutral exciton and the trion of about $pm2$meV at $B_zmp9$T. The extracted Land{e}-factors for both exciton complexes in both materials are $gapprox -4$.
Magnetic skyrmions are nano-scale spin structures that are promising for ultra-dense memory and logic devices. Recent progresses in two-dimensional magnets encourage the idea to realize skyrmionic states in freestanding monolayers. However, monolayers such as CrI3 lack Dzyaloshinskii-Moriya interactions (DMI) and thus do not naturally exhibit skyrmions but rather a ferromagnetic state. Here we propose the fabrication of Cr(I,X)3 Janus monolayers, in which the Cr atoms are covalently bonded to the underlying I ions and top-layer Br or Cl atoms. By performing first-principles calculations and Monte-Carlo simulations, we identify strong enough DMI, which leads to not only helical cycloid phases, but also to intrinsic skyrmionic states in Cr(I,Br)3 and magnetic-field-induced skyrmions in Cr(I,Cl)3.
Properties of semiconductors are largely defined by crystal imperfections including native defects. Van der Waals (vdW) semiconductors, a newly emerged class of materials, are no exception: defects exist even in the purest materials and strongly affect their electrical, optical, magnetic, catalytic and sensing properties. However, unlike conventional semiconductors where energy levels of defects are well documented, they are experimentally unknown in even the best studied vdW semiconductors, impeding the understanding and utilization of these materials. Here, we directly evaluate deep levels and their chemical trends in the bandgap of MoS2, WS2 and their alloys by transient spectroscopic study. One of the deep levels is found to follow the conduction band minimum of each host, attributed to the native sulfur vacancy. A switchable, DX center - like deep level has also been identified, whose energy lines up instead on a fixed level across different hosts, explaining a persistent photoconductivity above 400K.
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