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Abstract 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 CrXTe₃(X=Ge, Si) using high-resolution Raman scattering. Unlike conventional optical phonons, the highestA_gmode in CrGeTe₃splits 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 Ge₂Te₆clusters, 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 CrSiTe₃, 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. 

Excitons, which are Coulomb bound electron-hole pairs, are composite bosons and thus at low temperature can form a superfluid state with a single well-defined amplitude and phase. We directly image this macroscopic exciton superfluid state in an hBN-separated MoSe₂-WSe₂heterostructure. At high density, we identify quasi-long-range order over the entire active area of our sample, through spatially resolved coherence measurements. By varying the exciton density and sample temperature, we map out the phase diagram of the superfluid. We observe the superfluid phase persisting to a temperature of 15 K, which is in excellent agreement with theoretical predictions. This works paves the way to realizing on chip superfluid structures capable of studying fundamental physical behaviors and quantum devices that use superfluidity. 

Kagome lattices have emerged as an ideal platform for exploring exotic quantum phenomena in materials. Here, we report the discovery of Ti-based kagome metal YbTi3Bi4 which we characterize using angle-resolved photoemission spectroscopy (ARPES) and magneto-transport, in combination with density functional theory calculations. Our ARPES results reveal the complex fermiology of YbTi3Bi4 and provide spectroscopic evidence of four flat bands. Our measurements also show the presence of multiple van Hove singularities originating from Ti 3d orbitals and a linearly-dispersing gapped Dirac-like bulk state at the point in accord with our theoretical calculations. Our study establishes YbTi3Bi4 as a platform for exploring exotic phases in the wider LnTi3Bi4 (Ln = lanthanide) family of materials. 

One-dimensional (1D) van der Waals materials have emerged as an intriguing playground to explore novel electronic and optical effects. We report on inorganic one-dimensional SbPS4 nanotube bundles obtained via mechanical exfoliation from bulk crystals. The ability to mechanically exfoliate SbPS4 nanobundles offers the possibility of applying modern 2D material fabrication techniques to create mixed-dimensional van der Waals heterostructures. We find that SbPS4 can readily be exfoliated to yield long (>10 μm) nanobundles with thicknesses that range from 1.3 to 200 nm. We investigated the optical response of semiconducting SbPS4 nanobundles and discovered that upon excitation with blue light, they emit bright and ultra-broadband red light with a quantum yield similar to that of hBN-encapsulated MoSe2. We discovered that the ultra-broadband red light emission is a result of a large ∼1 eV exciton binding energy and a ∼200 meV exciton self-trapping energy, unprecedented in previous material studies. Due to the bright and ultra-broadband light emission, we believe that this class of inorganic 1D van der Waals semiconductors has numerous potential applications, including on-chip tunable nanolasers, and applications that require ultraviolet to visible light conversion, such as lighting and sensing. Overall, our findings open avenues for harnessing the unique characteristics of these nanomaterials, advancing both fundamental research and practical optoelectronic applications.< 

Abstract Spectrally narrow optical resonances can be used to generate slow light, i.e., a large reduction in the group velocity. In a previous work, we developed hybrid 2D semiconductor plasmonic structures, which consist of propagating optical frequency surface-plasmon polaritons interacting with excitons in a semiconductor monolayer. Here, we use coupled exciton-surface plasmon polaritons (E-SPPs) in monolayer WSe 2 to demonstrate slow light with a 1300 fold decrease of the SPP group velocity. Specifically, we use a high resolution two-color laser technique where the nonlinear E-SPP response gives rise to ultra-narrow coherent population oscillation (CPO) resonances, resulting in a group velocity on order of 10 5  m/s. Our work paves the way toward on-chip actively switched delay lines and optical buffers that utilize 2D semiconductors as active elements.