Quantum confinement of two-dimensional excitons in van der Waals materials via electrostatic trapping, lithographic patterning, Moiré potentials, and chemical implantation has enabled significant advances in tailoring light emission from nanostructures. While such approaches rely on complex preparation of materials, natural edges are a ubiquitous feature in layered materials and provide a different approach for investigating quantum-confined excitons. Here, we observe that certain edge sites of monolayer black phosphorus (BP) strongly localize the intrinsic quasi-one-dimensional excitons, yielding sharp spectral lines in photoluminescence, with nearly an order of magnitude line width reduction. Through structural characterization of BP edges using transmission electron microscopy and first-principles GW plus Bethe-Salpeter equation (GW-BSE) calculations of exemplary BP nanoribbons, we find that certain atomic reconstructions can strongly quantum-confine excitons resulting in distinct emission features, mediated by local strain and screening. We observe linearly polarized luminescence emission from edge reconstructions that preserve the mirror symmetry of the parent BP lattice, in agreement with calculations. Furthermore, we demonstrate efficient electrical switching of localized edge excitonic luminescence, whose sites act as excitonic transistors for emission. Localized emission from BP edges motivates exploration of nanoribbons and quantum dots as hosts for tunable narrowband light generation, with future potential to create atomic-like structures for quantum information processing applications as well as exploration of exotic phases that may reside in atomic edge structures.
Using four-wave mixing microscopy, we measure the coherent response and ultrafast dynamics of excitons and trions in MoSe<sub>2</sub> monolayers grown by molecular beam epitaxy on thin films of hexagonal boron nitride. We assess inhomogeneous and homogeneous broadenings in the transition spectral lineshape. The impact of phonons on the homogeneous dephasing is inferred <i>via</i> the temperature dependence of the dephasing. Four-wave mixing mapping, combined with atomic force microscopy, reveals spatial correlations between exciton oscillator strength, inhomogeneous broadening and the sample morphology. The quality of the coherent optical response of epitaxially grown transition metal dichalcogenides now becomes comparable to the samples produced by mechanical exfoliation, enabling the coherent nonlinear spectroscopy of innovative materials, like magnetic layers or Janus semiconductors.
Twisted bilayer graphene heterostructures have recently emerged as a well-established platform for studying strongly correlated phases, such as correlated insulating, superconducting, and topological states. Extending this notion to twisted multilayer graphene heterostructures has exhibited more diverse correlated phases, as some fundamental properties related to symmetry and band structures are correspondingly modified. Here, we report the observations of correlated states in twisted monolayer–trilayer (Bernal stacked) graphene heterostructures. Correlated phases at integer fillings of the moiré unit cell are revealed at a high displacement field and stabilized with a moderate magnetic field on the electron-doping side at a twist angle of 1.45°, where the lift of degeneracy at the integer fillings is observed in the Landau fan diagram. Our results demonstrate the effectiveness of moiré engineering in an extended structure and provide insights into electric-field tunable correlated phases.
We fabricate polariton cavities in hBN with Q-factors > 70. Our approach is based on strong, resonant phonon excitation at 7.3 µm with femtosecond pulses causing the sample to “unzip” and produce a phonon reflection.
Read moreTwo-dimensional (2D) materials and their heterostructures exhibit intriguing optoelectronic properties; thus, they are good platforms for exploring fundamental research and further facilitating real device applications. The key is to preserve the high quality and intrinsic properties of 2D materials and their heterojunction interface even in production scale during the transfer and assembly process so as to apply in semiconductor manufacturing field. In this study, we successfully adopted a wet transfer existing method to separate mediator-assisted wafer-scale from SiO<sub>2</sub>/Si growing wafer for the first time with intermediate annealing to fabricate wafer-scale MoS<sub>2</sub>/h-BN and WS<sub>2</sub>/h-BN heterostructures on a SiO<sub>2</sub>/Si wafer. Interestingly, the high-quality wafer-scale 2D material heterostructure optical properties were enhanced and confirmed by Raman and photoluminescence spectroscopy. Our approach can be applied to other 2D materials and expedite mass production for industrial applications.
Read moreHow to fabricate high-quality microcavities simply and at low cost without causing damage to environmentally sensitive active layers such as perovskites are crucial for the studies of exciton-polaritons, however, it remains challenging in the field of microcavity fabrication. Usually, once the top mirror is deposited, the detuning of the microcavity is fixed and there is no easy way to tune it. Here, we have developed a method for deterministically transferring silver mirrors, which is relatively simple and guarantees the active layer from damaging of high temperature, particle bombardment, etc., during the deposition of the top mirror. Furthermore, with the help of a glass probe, we demonstrate a replaceable silver transfer method to tune the detuning of the microcavity, thereby changing the coupling of photons and excitons therein. The developed deterministic and replaceable silver mirror transfer methods will provide the capability to fabricate high-quality and tunable microcavities and play an active role in the development of the exciton-polariton field.
Read moreA key advantage of utilizing van-der-Waals (vdW) materials as defect-hosting platforms for quantum applications is the controllable proximity of the defect to the surface or the substrate allowing for improved light extraction, enhanced coupling with photonic elements, or more sensitive metrology. However, this aspect results in a significant challenge for defect identification and characterization, as the defect's properties depend on the the atomic environment. This study explores how the environment can influence the properties of carbon impurity centers in hexagonal boron nitride (hBN). It compares the optical and electronic properties of such defects between bulk-like and few-layer films, showing alteration of the zero-phonon line energies and their phonon sidebands, and enhancements of inhomogeneous broadenings. To disentangle the mechanisms responsible for these changes, including the atomic structure, electronic wavefunctions, and dielectric screening, it combines ab initio calculations with a quantum-embedding approach. By studying various carbon-based defects embedded in monolayer and bulk hBN, it demonstrates that the dominant effect of the change in the environment is the screening of density-density Coulomb interactions between the defect orbitals. The comparative analysis of experimental and theoretical findings paves the way for improved identification of defects in low-dimensional materials and the development of atomic scale sensors for dielectric environments.
Read morePropagation of light-emitting quasiparticles is of central importance across the fields of condensed matter physics and nanomaterials science. We experimentally demonstrate diffusion of excitons in the presence of a continuously tunable Fermi sea of free charge carriers in a monolayer semiconductor. Light emission from tightly bound exciton states in electrically gated WSe<sub>2</sub> monolayer is detected using spatially and temporally resolved microscopy. The measurements reveal a nonmonotonic dependence of the exciton diffusion coefficient on the charge carrier density in both electron and hole doped regimes. Supported by analytical theory describing exciton-carrier interactions in a dissipative system, we identify distinct regimes of elastic scattering and quasiparticle formation determining exciton diffusion. The crossover region exhibits a highly unusual behavior of an increasing diffusion coefficient with increasing carrier densities. Temperature-dependent diffusion measurements further reveal characteristic signatures of freely propagating excitonic complexes dressed by free charges with effective mobilities up to 3 × 10<sup>3</sup> cm<sup>2</sup>/(V s).
Read moreWe observe Floquet states driven by the time-periodic oscillations in self-energy due to an exciton in a monolayer Van der Waals semiconductor.
Read moreTwo-dimensional (2D) semiconductors with point defects are predicted to host a variety of bound exciton complexes analogous to trions and biexcitons due to strong many-body effects. However, despite the common observation of defect-mediated subgap emission, the existence of such complexes remains elusive. Here, we report the observation of bound exciton (BX) complex manifolds in monolayer MoSe<sub>2</sub> with intentionally created monoselenium vacancies (V<sub>Se</sub>) using proton beam irradiation. The emission intensity of different BX peaks is found to exhibit contrasting dependence on electrostatic doping near the onset of free electron injection. The observed trend is consistent with the model in which free excitons exist in equilibrium with excitons bound to neutral and charged V<sub>Se</sub> defects, which act as deep acceptors. These complexes are more strongly bound than trions and biexcitons, surviving up to around 180 K, and exhibit moderate valley polarization memory, indicating partial free exciton character.
Read moreHigh light absorption (∼15%) and strong photoluminescence (PL) emission in monolayer (1L) transition metal dichalcogenides (TMDs) make them ideal candidates for optoelectronic device applications. Competing interlayer charge transfer (CT) and energy transfer (ET) processes control the photocarrier relaxation pathways in TMD heterostructures (HSs). In TMDs, long-distance ET can survive up to several tens of nm, unlike the CT process. Our experiment shows that an efficient ET occurs from the 1Ls WSe<sub>2</sub>-to-MoS<sub>2</sub> with an interlayer hexagonal boron nitride (hBN), due to the resonant overlapping of the high-lying excitonic states between the two TMDs, resulting in enhanced HS MoS<sub>2</sub> PL emission. This type of unconventional ET from the <i>lower-to-higher</i> optical bandgap material is not typical in the TMD HSs. With increasing temperature, the ET process becomes weaker due to the increased electron-phonon scattering, destroying the enhanced MoS<sub>2</sub> emission. Our work provides new insight into the long-distance ET process and its effect on the photocarrier relaxation pathways.
Read moreCoherent optical manipulation of electronic bandstructures via Floquet Engineering is a promising means to control quantum systems on an ultrafast time scale. However, the ultrafast switching on/off of the driving field comes with questions regarding the limits of the Floquet formalism (which is defined for an infinite periodic drive) through the switching process and to what extent the transient changes can be driven adiabatically. Experimentally addressing these questions has been difficult, in large part due to the absence of an established technique to measure coherent dynamics through the duration of the pulse. Here, using multidimensional coherent spectroscopy we explicitly excite, control, and probe a coherent superposition of excitons in the <i>K</i> and <i>K</i>' valleys in monolayer WS<sub>2</sub>. With a circularly polarized, red-detuned pump pulse, the degeneracy of the <i>K</i> and <i>K</i>' excitons can be lifted, and the phase of the coherence rotated. We directly measure phase rotations greater than π during the 100 fs driving pulse and show that this can be described by a combination of the AC-Stark shift of excitons in one valley and the Bloch-Siegert shift of excitons in the opposite valley. Despite showing a smooth evolution of the phase that directly follows the intensity envelope of the nonresonant pump pulse, the process is not perfectly adiabatic. By measuring the magnitude of the macroscopic coherence as it evolves before, during, and after the nonresonant pump pulse we show that there is additional decoherence caused by power broadening in the presence of the nonresonant pump. This nonadiabaticity arises as a result of interactions with the otherwise adiabatic Floquet states and may be a problem for many applications, such as manipulating qubits in quantum information processing; however, these measurements also suggest ways such effects can be minimized or eliminated.
Read moreSince hBN is a wide bandgap semiconductor(~5.96eV), electroluminescence has not been demonstrated at deep-ultraviolet frequencies. We report deep-ultraviolet electroluminescence from tunnel-injected charge carriers in hBN. Our work shows potentials for hBN based deep-ultraviolet light-emitting devices.
Read moreAbstract Integration of graphene and hexagonal boron nitride (hBN) in lateral heterostructures has provided a route to broadly engineer the material properties by quantum confinement of electrons or introduction of novel electronic and magnetic states at the interface. In this work we demonstrate lateral heteroepitaxial growth of graphene nanoribbons (GNRs) passivated by hBN using high-temperature molecular beam epitaxy (HT-MBE) to grow graphene in oriented hBN trenches formed ex-situ by catalytic nanoparticle etching. High-resolution atomic force microscopy (AFM) reveals that GNRs grow epitaxially from the etched hBN edges, and merge to form a GNR network passivated by hBN. Using conductive AFM we probe the nanoscale electrical properties of the nanoribbons and observe quasiparticle interference patterns caused by intervalley scattering at the graphene/hBN interface, which carries implications for the potential transport characteristics of hBN passivated GNR devices.
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