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Optical phonon engineering through nonlinear effects has been utilized in ultrafast control of material properties. However, nonlinear optical phonons typically exhibit rapid decay due to strong mode-mode couplings, limiting their effectiveness in temperature or frequency sensitive applications. In this study, we report the observation of long-lived nonlinear optical phonons through the spontaneous formation of phonon frequency combs in the van der Waals material CrXTe$_3$ (X=Ge, Si) using high-resolution Raman scattering. Unlike conventional optical phonons, the highest $A_g$ mode in CrGeTe$_3$ splits into equidistant, sharp peaks forming a frequency comb that persists for hundreds of oscillations and survives up to 100K before decaying. These modes correspond to localized oscillations of Ge$_2$Te$_6$ clusters, isolated from Cr hexagons, behaving as independent quantum oscillators. Introducing a cubic nonlinear term to the harmonic oscillator model, we simulate the phonon time evolution and successfully replicate the observed comb structure. Similar frequency comb behavior is observed in CrSiTe$_3$, demonstrating the generalizability of this phenomenon. Our findings reveal that Raman scattering effectively probes high-frequency nonlinear phonon modes, providing new insight into generating long-lived, tunable phonon frequency combs with applications in ultrafast material control and phonon-based technologies., Comment: 22 pages, 10 figures

In the fundamental understanding of magnetic interactions between atoms in solids, the crystal lattice is one of the key parameters. As the effective tool for controlling the lattice using tensile stress is limited, there are only few demonstrations of the control in magnetic properties with expanding the lattice structure. Here, we observe that the Curie temperature (Tc) of quasi two-dimensional Cr2Ge2Te6 with NiO overlayer doubles from ~60 K to ~120 K, describe a clear correlation of magnetic properties with lattice expansion, which is characterized by several probes and computational approaches, and address on the mechanisms leading to the increase in Tc via the change in exchange interactions.

The search of novel topological phases, such as the quantum anomalous Hall insulator (QAHI) or the axion insulator, has motivated different schemes to introduce magnetism into topological insulators. One scheme is to introduce ferromagnetic dopants in topological insulators. However, it is generally challenging and requires carefully engineered growth/heterostructures or relatively low temperatures to observe the QAHI due to issues such as the added disorder with ferromagnetic dopants. Another promising scheme is using the magnetic proximity effect with a magnetic insulator to magnetize the topological insulator. Most of these heterostructures are synthesized so far by growth techniques such as molecular beam epitaxy and metallic organic chemical vapor deposition. These are not readily applicable to allow mixing and matching many of the available ferromagnetic and topological insulators due to difference in growth conditions and lattice mismatch. Here, we demonstrate that the magnetic proximity effect can still be obtained in stacked heterostructures assembled via the dry transfer of exfoliated micrometer-sized thin flakes of van der Waals topological insulator and magnetic insulator materials (BiSbTeSe2/Cr2Ge2Te6), as evidenced in the observation of an anomalous Hall effect (AHE). Furthermore, devices made from these heterostructures can allow modulation of the AHE when controlling the carrier density via electrostatic gating. These results show that simple mechanical transfer of magnetic van der Waals materials provides another possible avenue to magnetize topological insulators by magnetic proximity effect, a key step towards further realization of novel topological phases such as QAHI and axion insulators., Comment: 22 pages, 10 figures

Van der Waals layered materials are a focus of materials research as they support strong quantum effects and can easily form heterostructures. Electron spins in van der Waals materials played crucial roles in many recent breakthroughs, including topological insulators, two-dimensional (2D) magnets, and spin liquids. However, nuclear spins in van der Waals materials remain an unexplored quantum resource. Here we report the first demonstration of optical polarization and coherent control of nuclear spins in a van der Waals material at room temperature. We use negatively-charged boron vacancy ($V_B^-$) spin defects in hexagonal boron nitride to polarize nearby nitrogen nuclear spins. Remarkably, we observe the Rabi frequency of nuclear spins at the excited-state level anti-crossing of $V_B^-$ defects to be 350 times larger than that of an isolated nucleus, and demonstrate fast coherent control of nuclear spins. We also detect strong electron-mediated nuclear-nuclear spin coupling that is 5 orders of magnitude larger than the direct nuclear spin dipolar coupling, enabling multi-qubit operations. Nitrogen nuclear spins in a triangle lattice will be suitable for large-scale quantum simulation. Our work opens a new frontier with nuclear spins in van der Waals materials for quantum information science and technology.

The recently discovered spin defects in hexagonal boron nitride (hBN), a layered van der Waals material, have great potential in quantum sensing. However, the photoluminescence and the contrast of the optically detected magnetic resonance (ODMR) of hBN spin defects are relatively low so far, which limits their sensitivity. Here we report a record-high ODMR contrast of 46$\%$ at room temperature, and simultaneous enhancement of the photoluminescence of hBN spin defects by up to 17-fold by the surface plasmon of a gold-film microwave waveguide. Our results are obtained with shallow boron vacancy spin defects in hBN nanosheets created by low-energy He$^+$ ion implantation, and a gold-film microwave waveguide fabricated by photolithography. We also explore the effects of microwave and laser powers on the ODMR, and improve the sensitivity of hBN spin defects for magnetic field detection. Our results support the promising potential of hBN spin defects for nanoscale quantum sensing.

Atom-like defects in two-dimensional (2D) hexagonal boron nitride (hBN) have recently emerged as a promising platform for quantum information science. Here we investigate single-photon emissions from atomic defects in boron nitride nanotubes (BNNTs). We demonstrate the first optical modulation of the quantum emission from BNNTs with a near-infrared laser. This one-dimensional system displays bright single-photon emission as well as high stability at room temperature and is an excellent candidate for optomechanics. The fast optical modulation of single-photon emission from BNNTs shows multiple electronic levels of the system and has potential applications in optical signal processing.