Picosecond Ultrasonics in Magnetic Topological Insulator MnBi2Te4.

MnBi2Te4 is a magnetic topological insulator with layered A-type antiferromagnetic order. It exhibits a rich layer- and magnetic-state dependent topological phase diagram; however, much about the coupling between spin, charge, and lattice remains to be explored. In this work, we report that MnBi2Te4 is an excellent acoustic phonon cavity by realizing phonon frequency combs using picosecond ultrasonics. With the generated acoustic phonon wavepackets, we demonstrate that the timing and phase of acoustic echoes can be used to detect the presence of stacking faults between van der Waals layers buried deep within the crystal. Furthermore, by implementing this nondestructive ultrafast optical measurement in conjunction with time-resolved magneto-optical Kerr effect experiments, we uncover that out-of-plane vibrations in MnBi2Te4 do not couple to the magnetic order, i.e. there is no appreciable magnetostriction. Our work points out how a well-developed technique can probe the structural defects and phonon pulse engineering in layered topological insulators.

Anomalous Second Harmonic Generation from Atomically Thin MnBi2Te4.

MnBi2Te4 is a van der Waals topological insulator with intrinsic intralayer ferromagnetic exchange and A-type antiferromagnetic interlayer coupling. Theoretically, it belongs to a class of structurally centrosymmetric crystals whose layered antiferromagnetic order breaks inversion symmetry for even layer numbers, making optical second harmonic generation (SHG) an ideal probe of the coupling between the crystal and magnetic structures. Here, we perform magnetic field and temperature-dependent SHG measurements on MnBi2Te4 flakes ranging from bulk to monolayer thickness. We find that the dominant SHG signal from MnBi2Te4 is unexpectedly unrelated to both magnetic state and layer number. We suggest that surface SHG is the likely source of the observed strong SHG, whose symmetry matches that of the MnBi2Te4-vacuum interface. Our results highlight the importance of considering the surface contribution to inversion symmetry-breaking in van der Waals centrosymmetric magnets.

Interlayer electronic coupling on demand in a 2D magnetic semiconductor.

When monolayers of two-dimensional (2D) materials are stacked into van der Waals structures, interlayer electronic coupling can introduce entirely new properties, as exemplified by recent discoveries of moiré bands that host highly correlated electronic states and quantum dot-like interlayer exciton lattices. Here we show the magnetic control of interlayer electronic coupling, as manifested in tunable excitonic transitions, in an A-type antiferromagnetic 2D semiconductor CrSBr. Excitonic transitions in bilayers and above can be drastically changed when the magnetic order is switched from the layered antiferromagnetic ground state to a field-induced ferromagnetic state, an effect attributed to the spin-allowed interlayer hybridization of electron and hole orbitals in the latter, as revealed by Green's function-Bethe-Salpeter equation (GW-BSE) calculations. Our work uncovers a magnetic approach to engineer electronic and excitonic effects in layered magnetic semiconductors.

Tunable interaction between excitons and hybridized magnons in a layered semiconductor.

The interaction between distinct excitations in solids is of both fundamental interest and technological importance. One such interaction is the coupling between an exciton, a Coulomb bound electron-hole pair, and a magnon, a collective spin excitation. The recent emergence of van der Waals magnetic semiconductors1 provides a platform to explore these exciton-magnon interactions and their fundamental properties, such as strong correlation2, as well as their photospintronic and quantum transduction3 applications. Here we demonstrate the precise control of coherent exciton-magnon interactions in the layered magnetic semiconductor CrSBr. We varied the direction of an applied magnetic field relative to the crystal axes, and thus the rotational symmetry of the magnetic system4. Thereby, we tuned not only the exciton coupling to the bright magnon, but also to an optically dark mode via magnon-magnon hybridization. We further modulated the exciton-magnon coupling and the associated magnon dispersion curves through the application of uniaxial strain. At a critical strain, a dispersionless dark magnon band emerged. Our results demonstrate an unprecedented level of control of the opto-mechanical-magnonic coupling, and a step towards the predictable and controllable implementation of hybrid quantum magnonics5-11.

Visualizing moiré ferroelectricity via plasmons and nano-photocurrent in graphene/twisted-WSe2 structures.

Ferroelectricity, a spontaneous and reversible electric polarization, is found in certain classes of van der Waals (vdW) materials. The discovery of ferroelectricity in twisted vdW layers provides new opportunities to engineer spatially dependent electric and optical properties associated with the configuration of moiré superlattice domains and the network of domain walls. Here, we employ near-field infrared nano-imaging and nano-photocurrent measurements to study ferroelectricity in minimally twisted WSe2. The ferroelectric domains are visualized through the imaging of the plasmonic response in a graphene monolayer adjacent to the moiré WSe2 bilayers. Specifically, we find that the ferroelectric polarization in moiré domains is imprinted on the plasmonic response of the graphene. Complementary nano-photocurrent measurements demonstrate that the optoelectronic properties of graphene are also modulated by the proximal ferroelectric domains. Our approach represents an alternative strategy for studying moiré ferroelectricity at native length scales and opens promising prospects for (opto)electronic devices.

Reversible strain-induced magnetic phase transition in a van der Waals magnet.

Mechanical deformation of a crystal can have a profound effect on its physical properties. Notably, even small modifications of bond geometry can completely change the size and sign of magnetic exchange interactions and thus the magnetic ground state. Here we report the strain tuning of the magnetic properties of the A-type layered antiferromagnetic semiconductor CrSBr achieved by designing a strain device that can apply continuous, in situ uniaxial tensile strain to two-dimensional materials, reaching several percent at cryogenic temperatures. Using this apparatus, we realize a reversible strain-induced antiferromagnetic-to-ferromagnetic phase transition at zero magnetic field and strain control of the out-of-plane spin-canting process. First-principles calculations reveal that the tuning of the in-plane lattice constant strongly modifies the interlayer magnetic exchange interaction, which changes sign at the critical strain. Our work creates new opportunities for harnessing the strain control of magnetism and other electronic states in low-dimensional materials and heterostructures.

Highly anisotropic excitons and multiple phonon bound states in a van der Waals antiferromagnetic insulator.

Two-dimensional (2D) semiconductors enable the investigation of light-matter interactions in low dimensions1,2. Yet, the study of elementary photoexcitations in 2D semiconductors with intrinsic magnetic order remains a challenge due to the lack of suitable materials3,4. Here, we report the observation of excitons coupled to zigzag antiferromagnetic order in the layered antiferromagnetic insulator NiPS3. The exciton exhibits a narrow photoluminescence linewidth of roughly 350 µeV with near-unity linear polarization. When we reduce the sample thickness from five to two layers, the photoluminescence is suppressed and eventually vanishes for the monolayer. This suppression is consistent with the calculated bandgap of NiPS3, which is highly indirect for both the bilayer and the monolayer5. Furthermore, we observe strong linear dichroism (LD) over a broad spectral range. The optical anisotropy axes of LD and of photoluminescence are locked to the zigzag direction. Furthermore, their temperature dependence is reminiscent of the in-plane magnetic susceptibility anisotropy. Hence, our results indicate that LD and photoluminescence could probe the symmetry breaking magnetic order parameter of 2D magnetic materials. In addition, we observe over ten exciton-A1g-phonon bound states on the high-energy side of the exciton resonance, which we interpret as signs of a strong modulation of the ligand-to-metal charge-transfer energy by electron-lattice interactions. Our work establishes NiPS3 as a 2D platform for exploring magneto-exciton physics with strong correlations.