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Jenny Hu

Publications and source records attributed to Jenny Hu.

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Moir\'e enabled spin pumping and preservation in MoSe2/WS2 heterobilayers

The spin degree of freedom is a fundamental quantum mechanical attribute with implications spanning from magnetism to quantum computing. Consequently, the relaxation of spin states for extended, Bloch electrons in solids has been studied for decades as it defines many of their properties and applications. We show that moir\'e patterns in layered materials can extend spin relaxation times by two orders of magnitude to 1 millisecond and beyond. This is achieved by suppressing spin mixing for electrons in 2D semiconductor heterostructures, particularly in the MoSe2/WS2 system, as we elucidate both experimentally and theoretically. The extended longitudinal lifetime facilitates spin alignment over 50% using only nanowatt levels of optical power. Our findings highlight the potential of moir\'e engineering for future quantum sensing and information processing.

cond-mat.mes-hall

Electric-field-tuned consecutive topological phase transitions between distinct correlated insulators in moire MoTe2/WSe2 heterobilayer

Consecutive topological phase transitions (TPTs) between strongly correlated electronic phases that differ simultaneously in symmetry breaking and topological order are of fundamental interest in condensed matter physics, yet are rarely realized experimentally. We report two consecutive electric-field-driven TPTs at half filling (nu = 1) in angle-aligned MoTe2/WSe2 moire heterobilayers. With increasing out-of-plane displacement field, a geometrically frustrated Mott insulator evolves into a ferromagnetic quantum anomalous Hall (QAH) Mott insulator, i.e., a spin-polarized topological Mott insulator without an observable charge-gap closure, and subsequently into an antiferromagnetic, valley-coherent Mott insulator (VC-AFM) accompanied by a continuous charge-gap collapse and the emergence of a critical metallic state. Layer-resolved magnetic circular dichroism (MCD), magneto-transport, and compressibility measurements jointly determine the phase diagram. The high-field evolution of the antiferromagnetic state reveals a metamagnetic-like transition at a critical field B*, above which a Chern insulating transport response reappears. Our results establish the MoTe2/WSe2 moire platform as a tunable realization of an extended Kane-Mele-Hubbard model hosting sequential correlation-topology-intertwined transitions.

cond-mat.str-el

Exciton-polaron Umklapp scattering in Wigner crystals

Strong Coulomb interactions in two-dimensional (2D) semiconductors give rise to tightly bound excitons, exciton polarons, and correlated electronic phases such as Wigner crystals (WCs), yet their mutual interplay remains poorly understood. Here we report the observation of multi-branch excitonic Umklapp scattering in both electron and hole WCs realized in ultraclean monolayer WSe$_2$, exhibiting exceptionally high melting temperatures (T$_c$ $\approx$ 20-30 K). Robust Wigner crystallization activates multiple finite-momentum optical resonances, including quasilinearly dispersing, light-like excitons and exciton polarons, extending far beyond the single excitonic Umklapp feature reported previously. Helicity-resolved magneto-optical measurements reveal a pronounced valley dependence of the scattering processes. Combined experiment and theory identify a polaron-induced brightening mechanism in which exciton polarons transfer oscillator strength from bright zero-momentum states to otherwise dark finite-momentum states, explaining the emergence of multiple Umklapp branches where conventional exciton-WC scattering is ineffective. These results establish WC polarons as a new quasiparticle paradigm and introduce polaron-induced Umklapp scattering as a general route to accessing finite-momentum many-body excitations in 2D quantum materials.

cond-mat.mes-hall

Deterministic fabrication of graphene hexagonal boron nitride moir\'e superlattices

The electronic properties of moir\'e heterostructures depend sensitively on the relative orientation between layers of the stack. For example, near-magic-angle twisted bilayer graphene (TBG) commonly shows superconductivity, yet a TBG sample with one of the graphene layers rotationally aligned to a hexagonal Boron Nitride (hBN) cladding layer provided the first experimental observation of orbital ferromagnetism. To create samples with aligned graphene/hBN, researchers often align edges of exfoliated flakes that appear straight in optical micrographs. However, graphene or hBN can cleave along either zig-zag or armchair lattice directions, introducing a 30 degree ambiguity in the relative orientation of two flakes. By characterizing the crystal lattice orientation of exfoliated flakes prior to stacking using Raman and second-harmonic generation for graphene and hBN, respectively, we unambiguously align monolayer graphene to hBN at a near-0 degree, not 30 degree, relative twist angle. We confirm this alignment by torsional force microscopy (TFM) of the graphene/hBN moir\'e on an open-face stack, and then by cryogenic transport measurements, after full encapsulation with a second, non-aligned hBN layer. This work demonstrates a key step toward systematically exploring the effects of the relative twist angle between dissimilar materials within moir\'e heterostructures.

cond-mat.mes-hall

Chemically Tailored Growth of 2D Semiconductors via Hybrid Metal-Organic Chemical Vapor Deposition

Two-dimensional (2D) semiconducting transition-metal dichalcogenides (TMDCs) are an exciting platform for new excitonic physics and next-generation electronics, creating a strong demand to understand their growth, doping, and heterostructures. Despite significant progress in solid-source (SS-) and metal-organic chemical vapor deposition (MOCVD), further optimization is necessary to grow highly crystalline 2D TMDCs with controlled doping. Here, we report a hybrid MOCVD growth method that combines liquid-phase metal precursor deposition and vapor-phase organo-chalcogen delivery to leverage the advantages of both MOCVD and SS-CVD. Using our hybrid approach, we demonstrate WS$_2$ growth with tunable morphologies - from separated single-crystal domains to continuous monolayer films - on a variety of substrates, including sapphire, SiO$_2$, and Au. These WS$_2$ films exhibit narrow neutral exciton photoluminescence linewidths down to 33 meV and room-temperature mobility up to 34 - 36 cm$^2$V$^-$$^1$s$^-$$^1$). Through simple modifications to the liquid precursor composition, we demonstrate the growth of V-doped WS$_2$, MoxW$_1$$_-$$_x$S$_2$ alloys, and in-plane WS$_2$-MoS$_2$ heterostructures. This work presents an efficient approach for addressing a variety of TMDC synthesis needs on a laboratory scale.

physics.app-ph

Millimeter-scale exfoliation of hBN with tunable flake thickness

As a two-dimensional (2D) dielectric material, hexagonal boron nitride (hBN) is in high demand for applications in photonics, nonlinear optics, and nanoelectronics. Unfortunately, the high-throughput preparation of macroscopic-scale, high-quality hBN flakes with controlled thickness is an ongoing challenge, limiting device fabrication and technological integration. Here, we present a metal thin-film exfoliation method to prepare hBN flakes with millimeter-scale dimension, near-unity yields, and tunable flake thickness distribution from 1-7 layers, a substantial improvement over scotch tape exfoliation. The single crystallinity and high quality of the exfoliated hBN are demonstrated with optical microscopy, atomic force microscopy, Raman spectroscopy, and second harmonic generation. We further explore a possible mechanism for the effectiveness and selectivity based on thin-film residual stress measurements, density functional theory calculations, and transmission electron microscopy imaging of the deposited metal films. We find that the magnitude of the residual tensile stress induced by thin film deposition plays a key role in determining exfoliated flake thickness in a manner which closely resembles 3D semiconductor spalling. Lastly, we demonstrate that our exfoliated, large-area hBN flakes can be readily incorporated as encapsulating layers for other 2D monolayers. Altogether, this method brings us one step closer to the high throughput, mass production of hBN-based 2D photonic, optoelectronic, and quantum devices.

cond-mat.mtrl-sci

Quantum control of exciton wavefunctions in 2D semiconductors

Excitons -- bound electron-hole pairs -- play a central role in light-matter interaction phenomena, and are crucial for wide-ranging applications from light harvesting and generation to quantum information processing. A long-standing challenge in solid-state optics has been to achieve precise and scalable control over the quantum mechanical state of excitons in semiconductor heterostructures. Here, we demonstrate a technique for creating tailored and tunable potential landscapes for optically active excitons in 2D semiconductors that enables in-situ wavefunction shaping at the nanoscopic lengthscale. Using nanostructured gate electrodes, we create localized electrostatic traps for excitons in diverse geometries such as quantum dots and rings, and arrays thereof. We show independent spectral tuning of multiple spatially separated quantum dots, which allows us to bring them to degeneracy despite material disorder. Owing to the strong light-matter coupling of excitons in 2D semiconductors, we observe unambiguous signatures of confined exciton wavefunctions in optical reflection and photoluminescence measurements. Our work introduces a new approach to engineering exciton dynamics and interactions at the nanometer scale, with implications for novel optoelectronic devices, topological photonics, and many-body quantum nonlinear optics.

cond-mat.mes-hall

Valley-coherent quantum anomalous Hall state in AB-stacked MoTe2/WSe2 bilayers

Moiré materials provide fertile ground for the correlated and topological quantum phenomena. Among them, the quantum anomalous Hall (QAH) effect, in which the Hall resistance is quantized even under zero magnetic field, is a direct manifestation of the intrinsic topological properties of a material and an appealing attribute for low-power electronics applications. The QAH effect has been observed in both graphene and transition metal dichalcogenide (TMD) moiré materials. It is thought to arise from the interaction-driven valley polarization of the narrow moiré bands. Here, we show surprisingly that the newly discovered QAH state in AB-stacked MoTe2/WSe2 moiré bilayers is not valley-polarized but valley-coherent. The layer- and helicity-resolved optical spectroscopy measurement reveals that the QAH ground state possesses spontaneous spin (valley) polarization aligned (anti-aligned) in two TMD layers. In addition, saturation of the out-of-plane spin polarization in both layers occurs only under high magnetic fields, supporting a canted spin texture. Our results call for a new mechanism for the QAH effect and highlight the potential of TMD moiré materials with strong electronic correlations and spin-orbit interactions for exotic topological states.

cond-mat.mes-hall

Moiré-localized interlayer exciton wavefunctions captured by imaging its electron and hole constituents

Interlayer excitons (ILXs) - electron-hole pairs bound across two atomically thin layered semiconductors - have emerged as attractive platforms to study exciton condensation, single-photon emission and other quantum-information applications. Yet, despite extensive optical spectroscopic investigations, critical information about their size, valley configuration and the influence of the moiré potential remains unknown. Here, we captured images of the time- and momentum-resolved distribution of both the electron and the hole that bind to form the ILX in a WSe2/MoS2 heterostructure. We thereby obtain a direct measurement of the interlayer exciton diameter of ~5.4 nm, comparable to the moiré unit-cell length of 6.1 nm. Surprisingly, this large ILX is well localized within the moiré cell to a region of only 1.8 nm - smaller than the size of the exciton itself. This high degree of localization of the interlayer exciton is backed by Bethe-Salpeter equation calculations and demonstrates that the ILX can be localized within small moiré unit cells. Unlike large moiré cells, these are uniform over large regions, thus allowing the formation of extended arrays of localized excitations for quantum technology.

physics.optics