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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 highestAgmode 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.more » « lessFree, publicly-accessible full text available December 1, 2026
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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.more » « less
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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.more » « less
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Abstract Kagomé metals are widely recognized, versatile platforms for exploring topological properties, unconventional electronic correlations, magnetic frustration, and superconductivity. In theRV6Sn6family of materials (R= Sc, Y, Lu), ScV6Sn6hosts an unusual charge density wave ground state as well as structural similarities with theAV3Sb5system (A= K, Cs, Rb). In this work, we combine Raman scattering spectroscopy with first-principles lattice dynamics calculations to reveal phonon mixing processes in the charge density wave state of ScV6Sn6. In the low temperature phase, we find at least four new peaks in the vicinity of the V-containing totally symmetric mode near 240 cm−1suggesting that the density wave acts to mix modes ofP6/mmmand$$R\bar{3}m$$ symmetry - a result that we quantify by projecting phonons of the high symmetry state onto those of the lower symmetry structure. We also test the stability of the short-range ordered density wave state under compression and propose that both physical and chemical pressure quench the effect. We discuss these findings in terms of symmetry and the structure-property trends that can be unraveled in this system.more » « less
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