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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. Here 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 200K. 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 demonstrate that Raman scattering effectively probes high-frequency nonlinear phonon modes, offering insight into the generation of long-lived, tunable phonon frequency combs with potential applications in ultrafast material control and phonon-based technologies. Nonlinear optical phonons often exhibit rapid decay. Here, the authors demonstrate long-lived nonlinear optical phonons through the spontaneous formation of phonon frequency combs in CrXTe 3 (X=Ge,Si).

Electron spins in van der Waals materials are playing a crucial role in recent advances in condensed-matter physics and spintronics. However, nuclear spins in van der Waals materials remain an unexplored quantum resource. Here we report 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. 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. Further, we detect strong electron-mediated nuclear–nuclear spin coupling that is five orders of magnitude larger than the direct nuclear-spin dipolar coupling, enabling multi-qubit operations. Our work opens new avenues for the manipulation of nuclear spins in van der Waals materials for quantum information science and technology. Unlike electron spins, nuclear spins in van der Waals materials remain a largely untapped quantum resource. Here we report the fast coherent control of nuclear spins and strong electron-mediated nuclear–nuclear spin coupling in hexagonal boron nitride.

The recently proposed concept of graphene photodetectors offers remarkable properties such as unprecedented compactness, ultrabroadband detection, and an ultrafast response speed. However, owing to the low optical absorption of pristine monolayer graphene, the intrinsically low responsivity of graphene photodetectors significantly hinders the development of practical devices. To address this issue, numerous efforts have thus far been made to enhance the light–graphene interaction using plasmonic structures. These approaches, however, can be significantly advanced by leveraging the other critical aspect of graphene photoresponsivity enhancement—electrical junction control. It has been reported that the dominant photocarrier generation mechanism in graphene is the photothermoelectric (PTE) effect. Thus, the two energy conversion mechanisms involved in the graphene photodetection process are light-to-heat and heat-to-electricity conversions. In this work, we propose a meticulously designed device architecture to simultaneously enhance the two conversion efficiencies. Specifically, a gap plasmon structure is used to absorb a major portion of the incident light to induce localized heating, and a pair of split gates is used to produce a p-n junction in graphene to augment the PTE current generation. The gap plasmon structure and the split gates are designed to share common key components so that the proposed device architecture concurrently realizes both optical and electrical enhancements. We experimentally demonstrate the dominance of the PTE effect in graphene photocurrent generation and observe a 25-fold increase in the generated photocurrent compared to the un-enhanced cases. While further photocurrent enhancement can be achieved by applying a DC bias, the proposed device concept shows vast potential for practical applications.Optics: designing lightweight, broadband graphene photodetectorsAmerican scientists have developed graphene photodetectors with unprecedented compactness, ultra-broadband detection, and ultrafast response speeds. In addition to being inexpensive, lightweight, and compact, graphene has unique optical and electrical properties, including a zero bandgap, ultrahigh carrier mobility, and thermal conductance that make it ideal for use in photodetectors. However, as graphene is just one monolayer, it absorbs light very weakly, thus hindering the development of practical photodetectors. A team of researchers led by Vladimir Shalaev from Purdue University in the United States has developed a plasmonic-enhanced graphene photodetector with a 25-fold increase in photocurrent generation compared with conventional graphene devices. Moreover, further enhancement can be achieved by the application of a direct current bias, opening the door for useful applications that require small devices with broad operational bandwidths and excellent responsivity.

Recently, there has been a growing interest in two-dimensional van der Waals (vdW) magnets owing to their unique two-dimensional magnetic phenomena and potential applications. Most vdW ferromagnets have the Curie temperature below room temperature, highlighting the need to explore how to enhance their magnetism. In our previous report, we successfully increased the Curie temperature of the prototypical vdW magnet Cr2Ge2Te6 using a NiO overlayer. In layered materials, the presence of wrinkles is often observed and evaluating them using optical microscopy proves to be useful; however, there have been limited investigations into the optical constants of vdW magnets, hampering progress in understanding their optical properties. In this study, we present the optical constants of Cr2Ge2Te6 obtained through ellipsometry measurements. To account for the presence of wrinkles, we model a vacuum region between the substrate and the vdW magnet, and we calculate the reflectivity as a function of wavelength and vacuum thickness to visualize the optical image. Furthermore, we discuss the relationship between the optical constants and the electronic structure of the material.

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.

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. Here 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 (X=Ge, Si) using high-resolution Raman scattering. Unlike conventional optical phonons, the highest A mode in CrGeTe splits into equidistant, sharp peaks forming a frequency comb that persists for hundreds of oscillations and survives up to 200K. These modes correspond to localized oscillations of Ge Te 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 , demonstrating the generalizability of this phenomenon. Our findings demonstrate that Raman scattering effectively probes high-frequency nonlinear phonon modes, offering insight into the generation of long-lived, tunable phonon frequency combs with potential applications in ultrafast material control and phonon-based technologies.

Recently, there has been a growing interest in two-dimensional van der Waals (vdW) magnets owing to their unique two-dimensional magnetic phenomena and potential applications. Most vdW ferromagnets have the Curie temperature below room temperature, highlighting the need to explore how to enhance their magnetism. In our previous report, we successfully increased the Curie temperature of the prototypical vdW magnet Cr[sub.2]Ge[sub.2]Te[sub.6] using a NiO overlayer. In layered materials, the presence of wrinkles is often observed and evaluating them using optical microscopy proves to be useful; however, there have been limited investigations into the optical constants of vdW magnets, hampering progress in understanding their optical properties. In this study, we present the optical constants of Cr[sub.2]Ge[sub.2]Te[sub.6] obtained through ellipsometry measurements. To account for the presence of wrinkles, we model a vacuum region between the substrate and the vdW magnet, and we calculate the reflectivity as a function of wavelength and vacuum thickness to visualize the optical image. Furthermore, we discuss the relationship between the optical constants and the electronic structure of the material.

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.

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.

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.