arXiv subjects

X. -Y. Zhu

Publications and source records attributed to X. -Y. Zhu.

At least 19 recordsLinked to original sources

arXiv2026

Observation of Coherent Ferron Emission and Propagation

Excitation of ordered quantum phases gives rise to collective modes and quasiparticles, as exemplified by spin waves and magnons emerging from magnetic order. Extending this paradigm to ferroelectric materials suggests the existence of polarization waves and their fundamental quanta, ferrons. Here, we report the generation and transport of polarization waves, i.e., coherent ferrons, in the van der Waals ferroelectric material NbOI2. Upon excitation by a short laser pulse, the polarization wave emits intense and narrow-band terahertz (THz) radiation at the ferroelectric transverse optical phonon frequency, modulates the ferroelectric order parameter, and propagates uniaxially along the polar axis at hypersonic velocities of ~105 m/s. These long-lived, uniaxial, and dipole-carrying polarization waves may find applications in narrow-band THz emission, ferronic information processing, and coherent electric control.

cond-mat.mtrl-sci↗

arXiv2025

Rydberg Exciton Dynamics in the Blockade Regime of Cu2O

Hosting giant Rydberg excitons with principal quantum numbers up to n = 30, cuprous oxide (Cu2O) provides a rare solid-state setting for exploring Rydberg physics, as exemplified by the blockade effect. Here we access the strongly interaction regime at high excitation densities (10^14-10^16/cm^3) and resolve the corresponding blockade dynamics for n = 2-7 using time-resolved spectroscopy. We find that Rydberg blockades are primarily governed by resonant dipolar interactions and that exciton recombination is coupled to the blockade itself. These findings demonstrate the potential for manipulating Rydberg exctions in the strongly interacting blockade regime in a solid state system.

cond-mat.other↗

arXiv2025

Space-time duality in polariton dynamics

The spatial and temporal dynamics of wave propagation are intertwined. A common manifestation of this duality emerges in the spatial and temporal decay of waves as they propagate through a lossy medium. A complete description of the non-Hermitian wave dynamics in such a lossy system, capturing temporal and spatial decays, necessitates the use of complex-valued frequency and/or wavenumber Eigen-values. Here, we demonstrate that the propagation of polaritons - hybrid light-matter quasiparticles - can be broadly controlled in space and time by temporally shaping their photonic excitation. Using time-domain terahertz near-field nanoscopy, we study plasmon polaritons in bilayer graphene at sub-picosecond time scales. Suppressed spatial decay of polaritons is implemented by temporally engineering the excitation waveform. Polaritonic space-time metrology data agree with our dynamic model. Through the experimental realization and visualization of polaritonic space-time duality, we uncover the effects of the spatio-temporal engineering of wave dynamics; these are applicable to acoustic, photonic, plasmonic, and electronic systems.

physics.optics↗

arXiv2025

Observing the Birth of Rydberg Exciton Fermi Polarons on a Moire Fermi Sea

The optical spectra of two-dimensional (2D) semiconductors are dominated by tightly bound excitons and trions. In the low doping limit, trions are often described as three-body quasiparticles consisting of two electrons and one hole or vice versa. However, trions are more rigorously understood as quasiparticles arising from the interaction between an exciton and excitation of the Fermi sea - referred to as exciton Fermi polaron. Here we employ pump-probe spectroscopy to directly observe the formation of exciton Fermi polarons in a model system composed of a WSe2 monolayer adjacent to twisted bilayer graphene (tBLG). Following the pump-injection of Rydberg excitons in WSe2, a time-delayed probe pulse tracks the development of Rydberg exciton Fermi polarons as interactions with localized carriers in the tBLG moire superlattice evolve. Both the exciton Fermi polaron relaxation rate and binding energy are found to increase with electron or hole density. Our findings provide insight into the optical response of fundamental excitations in 2D Van der Waals systems and reveal how many-body interactions give rise to emergent quasiparticles.

cond-mat.mes-hall↗

arXiv2025

Polaritonic Quantum Matter

Polaritons are quantum mechanical superpositions of photon states with elementary excitations in molecules and solids. The light-matter admixture causes a characteristic frequency-momentum dispersion shared by all polaritons irrespective of the microscopic nature of material excitations that could entail charge, spin, lattice or orbital effects. Polaritons retain the strong nonlinearities of their matter component and simultaneously inherit ray-like propagation of light. Polaritons prompt new properties, enable new opportunities for spectroscopy/imaging, empower quantum simulations and give rise to new forms of synthetic quantum matter. Here, we review the emergent effects rooted in polaritonic quasiparticles in a wide variety of their physical implementations. We present a broad portfolio of the physical platforms and phenomena of what we term polaritonic quantum matter. We discuss the unifying aspects of polaritons across different platforms and physical implementations and focus on recent developments in: polaritonic imaging, cavity electrodynamics and cavity materials engineering, topology and nonlinearities, as well as quantum polaritonics.

cond-mat.mtrl-sci↗

arXiv2025

Roadmap for Photonics with 2D Materials

Triggered by the development of exfoliation and the identification of a wide range of extraordinary physical properties in self-standing films consisting of one or few atomic layers, two-dimensional (2D) materials such as graphene, transition metal dichalcogenides (TMDs), and other van der Waals (vdW) crystals currently constitute a wide research field protruding in multiple directions in combination with layer stacking and twisting, nanofabrication, surface-science methods, and integration into nanostructured environments. Photonics encompasses a multidisciplinary collection of those directions, where 2D materials contribute with polaritons of unique characteristics such as strong spatial confinement, large optical-field enhancement, long lifetimes, high sensitivity to external stimuli (e.g., electric and magnetic fields, heating, and strain), a broad spectral range from the far infrared to the ultraviolet, and hybridization with spin and momentum textures of electronic band structures. The explosion of photonics with 2D materials as a vibrant research area is producing breakthroughs, including the discovery and design of new materials and metasurfaces with unprecedented properties as well as applications in integrated photonics, light emission, optical sensing, and exciting prospects for applications in quantum information, and nanoscale thermal transport. This Roadmap summarizes the state of the art in the field, identifies challenges and opportunities, and discusses future goals and how to meet them through a wide collection of topical sections prepared by leading practitioners.

cond-mat.mtrl-sci↗

arXiv2025

Hidden States and Dynamics of Fractional Fillings in tMoTe2 Moiré Superlattices

The fractional quantum anomalous Hall (FQAH) effect was recently discovered in twisted MoTe2 bilayers (tMoTe2). Experiments to date have revealed Chern insulators from hole doping at v = -1, -2/3, -3/5, and -4/7 (per moiré unit cell). In parallel, theories predict that, between v = -1 and -3, there exist exotic quantum phases, such as the coveted fractional topological insulators (FTI), fractional quantum spin Hall (FQSH) states, and non-abelian fractional states. Here we employ transient optical spectroscopy on tMoTe2 to reveal nearly 20 hidden states at fractional fillings that are absent in static optical sensing or transport measurements. A pump pulse selectively excites charge across the correlated or pseudo gaps, leading to the disordering (melting) of correlated states. A probe pulse detects the subsequent melting and recovery dynamics via exciton and trion sensing. Besides the known states, we observe additional fractional fillings between v = 0 and -1 and a large number of states on the electron doping side (v > 0). Most importantly, we observe new states at fractional fillings of the Chern bands at v = -4/3, -3/2, -5/3, -7/3, -5/2, and -8/3. These states are potential candidates for the predicted exotic topological phases. Moreover, we show that melting of correlated states occurs on two distinct time scales, 2-4 ps and 180-270 ps, attributed to electronic and phonon mechanisms, respectively. We discuss the differing dynamics of the electron and hole doped states from the distinct moiré conduction and valence bands.

cond-mat.str-el↗

arXiv2024

Time-Domain Signatures of Distinct Correlated Insulators in a Moiré Superlattice

Among expanding discoveries of quantum phases in moiré superlattices, correlated insulators stand out as both the most stable and most commonly observed. Despite the central importance of these states in moiré physics, little is known about their underlying nature. Here, we use pump-probe spectroscopy to show distinct time-domain signatures of correlated insulators at fillings of one (v = -1) and two (v = -2) holes per moiré unit cell in the angle-aligned WSe2/WS2 system. Following photo-doping, we find that the disordering time of the v = -1 state is independent of excitation density (n_ex), as expected from the characteristic phonon response time associated with a polaronic state. In contrast, the disordering time of the v = -2 state scales with (n_ex)^-0.5, in agreement with plasmonic screening from free holons and doublons. These states display disparate reordering behavior dominated either by first order (v = -1) or second order (v = -2) recombination, suggesting the presence of Hubbard excitons and free carrier-like holons/doublons, respectively. Our work delineates the roles of electron-phonon (e-ph) versus electron-electron (e-e) interactions in correlated insulators on the moiré landscape and establishes non-equilibrium responses as mechanistic signatures for distinguishing and discovering quantum phases.

cond-mat.str-el↗

arXiv2024

Two-Dimensional Moiré Polaronic Electron Crystals

Two-dimensional moiré materials have emerged as the most versatile platforms for realizing quantum phases of electrons. Here, we explore the stability origins of correlated states in WSe2/WS2 moiré superlattices. We find that ultrafast electronic excitation leads to melting of the Mott states on time scales five times longer than predictions from the charge hopping integrals and the melting rates are thermally activated, with activation energies of 18 and 13 meV for the one- and two-hole Mott states, respectively, suggesting significant electron-phonon coupling. DFT calculation of the one-hole Mott state confirms polaron formation and yields a hole-polaron binding energy of 16 meV. These findings reveal a close interplay of electron-electron and electron-phonon interactions in stabilizing the polaronic Mott insulators at transition metal dichalcogenide moiré interfaces.

cond-mat.str-el↗

arXiv2023

Evidence for Exciton Crystals in a 2D Semiconductor Heterotrilayer

Two-dimensional (2D) transition metal dichalcogenides (TMDC) and their moiré interfaces have been demonstrated for correlated electron states, including Mott insulators and electron/hole crystals commensurate with moiré superlattices. Here we present spectroscopic evidences for ordered bosons - interlayer exciton crystals in a WSe2/MoSe2/WSe2 trilayer, where the enhanced Coulomb interactions over those in heterobilayers have been predicted to result in exciton ordering. While the dipolar interlayer excitons in the heterobilayer may be ordered by the periodic moiré traps, their mutual repulsion results in de-trapping at exciton density n_ex larger than 10^11 cm^-2 to form mobile exciton gases and further to electron-hole plasmas, both accompanied by broadening in photoluminescence (PL) peaks and large increases in mobility. In contrast, ordered interlayer excitons in the trilayer are characterized by negligible mobility and by sharper PL peaks persisting to n_ex approximately 10^12 cm^-2. We present evidences for the predicted quadrupolar exciton crystal and its transitions to dipolar excitons either with increasing n_ex or by an applied electric field. These ordered interlayer excitons may serve as models for the exploration of quantum phase transitions and quantum coherent phenomena.

cond-mat.mes-hall↗

arXiv2023

Spontaneous Exciton Dissociation in Transition Metal Dichalcogenide Monolayers

Since the seminal work on MoS2 monolayers, photoexcitation in atomically-thin transition metal dichalcogenides (TMDCs) has been assumed to result in excitons with large binding energies (~ 200-600 meV). Because the exciton binding energies are order-of-magnitude larger than thermal energy at room temperature, it is puzzling that photocurrent and photovoltage generation have been observed in TMDC-based devices, even in monolayers with applied electric fields far below the threshold for exciton dissociation. Here, we show that the photoexcitation of TMDC monolayers results in a substantial population of free charges. Performing ultrafast terahertz (THz) spectroscopy on large-area, single crystal WS2, WSe2, and MoSe2 monolayers, we find that ~10% of excitons spontaneously dissociate into charge carriers with lifetimes exceeding 0.2 ns. Scanning tunnelling microscopy reveals that photo-carrier generation is intimately related to mid-gap defect states, likely via trap-mediated Auger scattering. Only in state-of-the-art quality monolayers14, with mid-gap trap densities as low as 10^9 cm^-2, does intrinsic exciton physics start to dominate the THz response. Our findings reveal that excitons or excitonic complexes are only the predominant quasiparticles in photo-excited TMDC monolayers at the limit of sufficiently low defect densities.

cond-mat.mes-hall↗

arXiv2022

Charge carrier coupling to the soft phonon mode in a ferroelectric semiconductor

Many crystalline solids possess strongly anharmonic soft phonon modes characterized by diminishing frequency as temperature approaches a critical point associated with a symmetry breaking phase transition. While electron-soft phonon coupling can introduce unique scattering channels for charge carriers in ferroelectrics, recent studies on the non-ferroelectric lead halide perovskites have also suggested the central role of anharmonic phonons bearing resemblance to soft modes in charge carrier screening. Here we apply coherent phonon spectroscopy to directly study electron coupling to the soft transverse optical (TO) phonon mode in a ferroelectric semiconductor SbSI. Photo-generated charge carriers in SbSI are found to be exceptionally long lived and are associated with a transient electro-optical effect that can be explained by interactions between charge carriers and thermally stimulated soft-phonon excitations. These results provide strong evidence for the role of electron-soft phonon coupling in the efficient screening of charge carriers and in reducing charge recombination rates, both desirable properties for optoelectronics.

cond-mat.mtrl-sci↗

arXiv2021

Spin-Orbit Coupled Exciton-Polariton Condensates in Lead Halide Perovskites

Spin-orbit coupling (SOC) is responsible for a range of spintronic and topological processes in condensed matter. Here we show photonic analogs of SOCs in exciton-polaritons and their condensates in microcavities composed of birefringent lead halide perovskite single crystals. The presence of crystalline anisotropy coupled with splitting in the optical cavity of the transverse electric (TE) and transverse magnetic (TM) modes gives rise to a non-Abelian gauge field, which can be described by the Rashba-Dresselhaus Hamiltonian near the degenerate points of the two polarization modes. With increasing density, the exciton polaritons with pseudospin textures undergo phase transitions to competing condensates with orthogonal polarizations. Unlike their pure photonic counterparts, these exciton polaritons and condensates inherit nonlinearity from their excitonic components and may serve as quantum simulators of many-body SOC processes.

cond-mat.quant-gas↗

arXiv2020

Decoding Ultrafast Polarization Responses in Lead Halide Perovskites by the Two-Dimensional Optical Kerr Effect

The ultrafast polarization response to incident light and ensuing exciton/carrier generation are essential to outstanding optoelectronic properties of lead halide perovskites (LHPs). A large number of mechanistic studies in the LHP field to date have focused on contributions to polarizability from organic cations and the highly polarizable inorganic lattice. For a comprehensive understanding of the ultrafast polarization response, we must additionally account for the nearly instantaneous hyperpolarizability response to the propagating light field itself. While light propagation is pivotal to optoelectronics and photonics, little is known about this in LHPs in the vicinity of the bandgap where stimulated emission, polariton condensation, superfluorescence, and photon recycling may take place. Here we develop two-dimensional optical Kerr effect (2D-OKE) spectroscopy to energetically dissect broadband light propagation and dispersive nonlinear polarization responses in LHPs. In contrast to earlier interpretations, the below-bandgap OKE responses in both hybrid CH3NH3PbBr3 and all-inorganic CsPbBr3 perovskites are found to originate from strong hyperpolarizability and highly anisotropic dispersions. In both materials, the nonlinear mixing of anisotropically propagating light fields result in convoluted oscillatory polarization dynamics. Based on a four-wave mixing model, we quantitatively derive dispersion anisotropies, reproduce 2D-OKE frequency correlations, and establish polarization dressed light propagation in single crystal LHPs. Moreover, our findings highlight the importance of distinguishing the often-neglected anisotropic light propagation from underlying coherent quasi-particle responses in various forms of ultrafast spectroscopy.

physics.app-ph↗

arXiv2020

Diffusivity Reveals Three Distinct Phases of Interlayer Excitons in MoSe2/WSe2 Heterobilayers

Charge separated interlayer excitons in transition metal dichalcogenide (TMDC) heterobilayers are being explored for moiré exciton lattices and exciton condensates. The presence of permanent dipole moments and the poorly screened Coulomb interaction make many body interactions particularly strong for interlayer excitons. Here we reveal two distinct phase transitions for interlayer excitons in the MoSe2/WSe2 heterobilayer using time and spatially resolved photoluminescence imaging: from trapped excitons in the moiré-potential to the modestly mobile exciton gas as exciton density increases to ne/h ~ 1011 cm-2 and from the exciton gas to the highly mobile charge separated electron/hole plasma for ne/h > 1012 cm-2. The latter is the Mott transition and is confirmed in photoconductivity measurements. These findings set fundamental limits for achieving quantum states of interlayer excitons.

cond-mat.mes-hall↗

arXiv2019

Seeing moiré superlattices

Moiré superlattices in van der Waals (vdW) heterostructures have given rise to a number of emergent electronic phenomena due to the interplay between atomic structure and electron correlations. A lack of a simple way to characterize moiré superlattices has impeded progress in the field. In this work we outline a simple, room-temperature, ambient method to visualize real-space moiré superlattices with sub-5 nm spatial resolution in a variety of twisted vdW heterostructures including but not limited to conducting graphene, insulating boron nitride and semiconducting transition metal dichalcogenides. Our method utilizes piezoresponse force microscopy, an atomic force microscope modality which locally measures electromechanical surface deformation. We find that all moiré superlattices, regardless of whether the constituent layers have inversion symmetry, exhibit a mechanical response to out-of-plane electric fields. This response is closely tied to flexoelectricity wherein electric polarization and electromechanical response is induced through strain gradients present within moiré superlattices. Moiré superlattices of 2D materials thus represent an interlinked network of polarized domain walls in a non-polar background matrix.

cond-mat.mes-hall↗

arXiv2018

Hundredfold Enhancement of Light Emission via Defect Control in Monolayer Transition-Metal Dichalcogenides

Two dimensional (2D) transition-metal dichalcogenide (TMD) based semiconductors have generated intense recent interest due to their novel optical and electronic properties, and potential for applications. In this work, we characterize the atomic and electronic nature of intrinsic point defects found in single crystals of these materials synthesized by two different methods - chemical vapor transport and self-flux growth. Using a combination of scanning tunneling microscopy (STM) and scanning transmission electron microscopy (STEM), we show that the two major intrinsic defects in these materials are metal vacancies and chalcogen antisites. We show that by control of the synthetic conditions, we can reduce the defect concentration from above $10^{13} /cm^2$ to below $10^{11} /cm^2$. Because these point defects act as centers for non-radiative recombination of excitons, this improvement in material quality leads to a hundred-fold increase in the radiative recombination efficiency.

cond-mat.mtrl-sci↗

arXiv2017

Trion Species-Resolved Quantum Beats in MoSe2

Monolayer photonic materials offer a tremendous potential for on-chip optoelectronic devices. Their realization requires knowledge of optical coherence properties of excitons and trions that have so far been limited to nonlinear optical experiments carried out with strongly inhomogenously broadened material. Here we employ h-BN encapsulated and electrically gated MoSe2 to reveal coherence properties of trion-species directly in the linear optical response. Autocorrelation measurements reveal long dephasing times up to T2=1.16+-0.05 ps for positively charged excitons. Gate dependent measurements provide evidence that the positively-charged trion forms via spatially localized hole states making this trion less prone to dephasing in the presence of elevated hole carrier concentrations. Quantum beat signatures demonstrate coherent coupling between excitons and trions that have a dephasing time up to 0.6 ps, a two-fold increase over those in previous reports. A key merit of the prolonged exciton/trion coherences is that they were achieved in a linear optical experiment, and thus are directly relevant to applications in nanolasers, coherent control, and on-chip quantum information processing requiring long photon coherence.

cond-mat.mes-hall↗