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Emma C. Regan

Publications and source records attributed to Emma C. Regan.

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Phason-mediated interlayer exciton diffusion in WS2/WSe2 moiré heterostructure

Moiré potentials in two-dimensional materials have been proven to be of fundamental importance to fully understand the electronic structure of van der Waals heterostructures, from superconductivity to correlated excitonic states. However, understanding how the moiré phonons, so-called phasons, affect the properties of the system still remains an uncharted territory. In this work, we demonstrate how phasons are integral to properly describing and understanding low-temperature interlayer exciton diffusion in WS2/WSe2 heterostructure. We perform photoluminescence (PL) spectroscopy to understand how the coupling between the layers, affected by their relative orientation, impacts the excitonic properties of the system. Samples fabricated with stacking angles of 0° and 60° are investigated taking into account the stacking angle dependence of the two common moiré potential profiles. Additionally, we present spatially and time-resolved exciton diffusion measurements, looking at the photoluminescence emission in a temperature range from 30 K to 250 K. An accurate potential for the two configurations are computed via density functional theory (DFT) calculations. Finally, we perform molecular dynamics simulation in order to visualize the phasons motion, estimating the phason speed at different temperatures, providing novel insights into the mechanics of exciton propagation at low temperatures that cannot be explained within the frame of classical exciton diffusion alone.

cond-mat.mtrl-sci

Nature of novel moiré exciton states in WSe$_2$/WS$_2$ heterobilayers

Moiré patterns of transition metal dichalcogenide (TMD) heterobilayers have proven to be an ideal platform to host unusual correlated electronic phases, emerging magnetism, and correlated exciton physics. While the existence of novel moiré excitonic states is established through optical measurements, the microscopic nature of these states is still poorly understood, often relying on empirically fit models. Here, combining large-scale first-principles GW-BSE calculations and micro-reflection spectroscopy, we identify the nature of the exciton resonances in WSe$_2$/WS$_2$ moiré superlattices, discovering a surprisingly rich set of moiré excitons that cannot be even qualitatively captured by prevailing continuum models. Our calculations reveal moiré excitons with distinct characters, including modulated Wannier excitons and previously unindentified intralayer charge-transfer excitons. Signatures of these distinct excitonic characters are confirmed experimentally via the unique carrier-density and magnetic-field dependences of different moiré exciton resonances. Our study highlights the highly non-trivial exciton states that can emerge in TMD moiré superlattices, and suggests novel ways of tuning many-body physics in moiré systems by engineering excited-states with specific spatial characters.

cond-mat.mes-hall

Correlated interlayer exciton insulator in double layers of monolayer WSe2 and moiré WS2/WSe2

Moiré superlattices in van der Waals heterostructures have emerged as a powerful tool for engineering novel quantum phenomena. Here we report the observation of a correlated interlayer exciton insulator in a double-layer heterostructure composed of a WSe2 monolayer and a WS2/WSe2 moiré bilayer that are separated by an ultrathin hexagonal boron nitride (hBN). The moiré WS2/WSe2 bilayer features a Mott insulator state at hole density p/p0 = 1, where p0 corresponds to one hole per moiré lattice site. When electrons are added to the Mott insulator in the WS2/WSe2 moiré bilayer and an equal number of holes are injected into the WSe2 monolayer, a new interlayer exciton insulator emerges with the holes in the WSe2 monolayer and the electrons in the doped Mott insulator bound together through interlayer Coulomb interactions. The excitonic insulator is stable up to a critical hole density of ~ 0.5p0 in the WSe2 monolayer, beyond which the system becomes metallic. Our study highlights the opportunities for realizing novel quantum phases in double-layer moiré systems due to the interplay between the moiré flat band and strong interlayer electron interactions.

cond-mat.mes-hall

Imaging Generalized Wigner Crystal States in a WSe2/WS2 Moiré Superlattice

The Wigner crystal state, first predicted by Eugene Wigner in 1934, has fascinated condensed matter physicists for nearly 90 years2-14. Studies of two-dimensional (2D) electron gases first revealed signatures of the Wigner crystal in electrical transport measurements at high magnetic fields2-4. More recently optical spectroscopy has provided evidence of generalized Wigner crystal states in transition metal dichalcogenide (TMDC) moiré superlattices. Direct observation of the 2D Wigner crystal lattice in real space, however, has remained an outstanding challenge. Scanning tunneling microscopy (STM) in principle has sufficient spatial resolution to image a Wigner crystal, but conventional STM measurements can potentially alter fragile Wigner crystal states in the process of measurement. Here we demonstrate real-space imaging of 2D Wigner crystals in WSe2/WS2 moiré heterostructures using a novel non-invasive STM spectroscopy technique. We employ a graphene sensing layer in close proximity to the WSe2/WS2 moiré superlattice for Wigner crystal imaging, where local STM tunneling current into the graphene sensing layer is modulated by the underlying electron lattice of the Wigner crystal in the WSe2/WS2 heterostructure. Our measurement directly visualizes different lattice configurations associated with Wigner crystal states at fractional electron fillings of n = 1/3, 1/2, and 2/3, where n is the electron number per site. The n=1/3 and n=2/3 Wigner crystals are observed to exhibit a triangle and a honeycomb lattice, respectively, in order to minimize nearest-neighbor occupations. The n = 1/2 state, on the other hand, spontaneously breaks the original C3 symmetry and forms a stripe structure in real space. Our study lays a solid foundation toward the fundamental understanding of rich Wigner crystal states in WSe2/WS2 moiré heterostructures.

cond-mat.mes-hall

Optical detection of Mott and generalized Wigner crystal states in WSe2/WS2 moiré superlattices

Moiré superlattices are emerging as a new route for engineering strongly correlated electronic states in two-dimensional van der Waals heterostructures, as recently demonstrated in the correlated insulating and superconducting states in magic-angle twisted bilayer graphene and ABC trilayer graphene/boron nitride moiré superlattices. Transition metal dichalcogenide (TMDC) moiré heterostructures provide another exciting model system to explore correlated quantum phenomena, with the addition of strong light-matter interactions and large spin-orbital coupling. Here we report the optical detection of strongly correlated phases in semiconducting WSe2/WS2 moiré superlattices. Our sensitive optical detection technique reveals a Mott insulator state at one hole per superlattice site (ν = 1), and surprising insulating phases at fractional filling factors ν = 1/3 and 2/3, which we assign to generalized Wigner crystallization on an underlying lattice. Furthermore, the unique spin-valley optical selection rules of TMDC heterostructures allow us to optically create and investigate low-energy spin excited states in the Mott insulator. We reveal an especially slow spin relaxation lifetime of many microseconds in the Mott insulating state, orders-of-magnitude longer than that of charge excitations. Our studies highlight novel correlated physics that can emerge in moiré superlattices beyond graphene.

cond-mat.mes-hall

Resolving spin, valley, and moiré quasi-angular momentum of interlayer excitons in WSe2/WS2 heterostructures

Moiré superlattices provide a powerful way to engineer properties of electrons and excitons in two-dimensional van der Waals heterostructures. The moiré effect can be especially strong for interlayer excitons, where electrons and holes reside in different layers and can be addressed separately. In particular, it was recently proposed that the moiré superlattice potential not only localizes interlayer exciton states at different superlattice positions, but also hosts an emerging moiré quasi-angular momentum (QAM) that periodically switches the optical selection rules for interlayer excitons at different moiré sites. Here we report the observation of multiple interlayer exciton states coexisting in a WSe2/WS2 moiré superlattice and unambiguously determine their spin, valley, and moiré QAM through novel resonant optical pump-probe spectroscopy and photoluminescence excitation spectroscopy. We demonstrate that interlayer excitons localized at different moiré sites can exhibit opposite optical selection rules due to the spatially-varying moiré QAM. Our observation reveals new opportunities to engineer interlayer exciton states and valley physics with moiré superlattices for optoelectronic and valleytronic applications.

cond-mat.mes-hall

Valley-dependent Exciton Fine Structure and Autler-Townes Doublets from Berry Phases in Monolayer Molybdenum Diselenide

The Berry phase of Bloch states can have profound effects on electron dynamics lead to novel transport phenomena, such as the anomalous Hall effect and the valley Hall effect. Recently, it was predicted that the Berry phase effect can also modify the exciton states in transition metal dichalcogenide monolayers, and lift the energy degeneracy of exciton states with opposite angular momentum through an effective valley-orbital coupling. Here, we report the first observation and control of the Berry-phase induced splitting of the 2p-exciton states in monolayer molybdenum diselenide using the intraexciton optical Stark spectroscopy. We observe the time-reversal-symmetric analog of the orbital Zeeman effect resulting from the valley-dependent Berry phase, which leads to energy difference of +14 (-14) meV between the $2p^+$ and $2p^-$ exciton states in +K (-K) valley, consistent with the ordering from our ab initio GW-BSE results. In addition, we show that the light-matter coupling between intraexciton states are remarkably strong, leading to prominent valley-dependent Autler-Townes doublet under resonant driving. Our study opens up new pathways to coherently manipulate the quantum states and excitonic excitation with infrared radiation in two-dimensional semiconductors.

cond-mat.mes-hall

Observation of Moiré Excitons in WSe2/WS2 Heterostructure Superlattices

Moiré superlattices provide a powerful tool to engineer novel quantum phenomena in two-dimensional (2D) heterostructures, where the interactions between the atomically thin layers qualitatively change the electronic band structure of the superlattice. For example, mini-Dirac points, tunable Mott insulator states, and the Hofstadter butterfly can emerge in different types of graphene/boron nitride moiré superlattices, while correlated insulating states and superconductivity have been reported in twisted bilayer graphene moiré superlattices. In addition to their dramatic effects on the single particle states, moiré superlattices were recently predicted to host novel excited states, such as moiré exciton bands. Here we report the first observation of moiré superlattice exciton states in nearly aligned WSe2/WS2 heterostructures. These moiré exciton states manifest as multiple emergent peaks around the original WSe2 A exciton resonance in the absorption spectra, and they exhibit gate dependences that are distinctly different from that of the A exciton in WSe2 monolayers and in large-twist-angle WSe2/WS2 heterostructures. The observed phenomena can be described by a theoretical model where the periodic moiré potential is much stronger than the exciton kinetic energy and creates multiple flat exciton minibands. The moiré exciton bands provide an attractive platform to explore and control novel excited state of matter, such as topological excitons and a correlated exciton Hubbard model, in transition metal dichalcogenides.

cond-mat.mes-hall

Silicon Color Filters for Light-Recycling Displays

We propose a set of silicon reflective transmission filters for light-recycling displays that are compatible with high-throughput nanofabrication technologies and have excellent angular stability.

physics.optics

Imaging of Iso-frequency Contours via Resonance-Enhanced Scattering in Near-Pristine Photonic Crystals

The iso-frequency contours of a photonic crystal are important for predicting and understanding exotic optical phenomena that are not apparent from high-symmetry band structure visualizations. Here, we demonstrate a method to directly visualize the iso-frequency contours of high-quality photonic crystal slabs that shows quantitatively good agreement with numerical results throughout the visible spectrum. Our technique relies on resonance-enhanced photon scattering from generic fabrication disorder and surface roughness, so it can be applied to general photonic and plasmonic crystals, or even quasi-crystals. We also present an analytical model of the scattering process, which explains the observation of iso-frequency contours in our technique. Furthermore, the iso-frequency contours provide information about the characteristics of the disorder and therefore serve as a feedback tool to improve fabrication processes.

physics.optics

Substrate-Independent Light Confinement in Bioinspired All-Dielectric Surface Resonators

Traditionally, photonic crystal slabs can support resonances that are strongly confined to the slab but also couple to external radiation. However, when a photonic crystal slab is placed on a substrate, the resonance modes become less confined, and as the index contrast between slab and substrate decreases, they eventually disappear. Using the scale structure of the Dione juno butterfly wing as an inspiration, we present a low-index zigzag surface structure that supports resonance modes even without index contrast with the substrate. The zigzag structure supports resonances that are contained away from the substrate, which reduces the interaction between the resonance and the substrate. We experimentally verify the existence of substrate-independent resonances in the visible wavelength regime. Potential applications include substrate-independent structural color and light guiding.

physics.optics