Highly tunable ground and excited state excitonic dipoles in multilayer 2H-MoSe2.

The fundamental properties of an exciton are determined by the spin, valley, energy, and spatial wavefunctions of the Coulomb-bound electron and hole. In van der Waals materials, these attributes can be widely engineered through layer stacking configuration to create highly tunable interlayer excitons with static out-of-plane electric dipoles, at the expense of the strength of the oscillating in-plane dipole responsible for light-matter coupling. Here we show that interlayer excitons in bi- and tri-layer 2H-MoSe2 crystals exhibit electric-field-driven coupling with the ground (1s) and excited states (2s) of the intralayer A excitons. We demonstrate that the hybrid states of these distinct exciton species provide strong oscillator strength, large permanent dipoles (up to 0.73 ± 0.01 enm), high energy tunability (up to ~200 meV), and full control of the spin and valley characteristics such that the exciton g-factor can be manipulated over a large range (from -4 to +14). Further, we observe the bi- and tri-layer excited state (2s) interlayer excitons and their coupling with the intralayer excitons states (1s and 2s). Our results, in good agreement with a coupled oscillator model with spin (layer)-selectivity and beyond standard density functional theory calculations, promote multilayer 2H-MoSe2 as a highly tunable platform to explore exciton-exciton interactions with strong light-matter interactions.

Nanoscale mapping of surface strain in tapered nanorods using confocal photoluminescence spectroscopy.

The strain occurs spontaneously at the heterogeneous interfaces of virtually all crystalline materials. Consequently, the analysis across multiple interfaces requires a complementary characterization scheme with a resolution that fits the deformation scale. By implementing two-photon confocal laser scanning nanoscopy with an axial resolution of 10 nm, we extract the surface strain from the photoluminescence (PL) spectra, epitomized by a 2-fold enhancement at the tapered tips in comparison to the substrate of ZnO nanorods. We firstly traced the well-established contribution from quantum confinement (QC) to PL shift in three geometrically classified regions: (I) a strongly tapered region where the diameter increases from 3 to 20 nm; (II) a weakly tapered region with a gradually increasing diameter from 20 to 58 nm; (III) round cylindrical region interfacing the sapphire substrate. The measured PL shift influenced by the deformation is significantly stronger than the attained QC effect. Particularly, surface strain at the strongly tapered region turned out to drastically increase the PL shift which matches well with the analysis based on the surface to volume ratio incorporating mechanical parameters such as the compliance tensor component, strain dislocation constant, and surface stress. The surface strain increased at a lower temperature, further disclosing its inherent dependence on the thermal expansion coefficients in clear contrast to the temperature-invariant characteristics of QC.

Electrically driven strain-induced deterministic single-photon emitters in a van der Waals heterostructure.

Quantum confinement in transition metal dichalcogenides (TMDCs) enables the realization of deterministic single-photon emitters. The position and polarization control of single photons have been achieved via local strain engineering using nanostructures. However, most existing TMDC-based emitters are operated by optical pumping, while the emission sites in electrically pumped emitters are uncontrolled. Here, we demonstrate electrically driven single-photon emitters located at the positions where strains are induced by atomic force microscope indentation on a van der Waals heterostructure consisting of graphene, hexagonal boron nitride, and tungsten diselenide. The optical, electrical, and mechanical properties induced by the local strain gradient were systematically analyzed. The emission at the indentation sites exhibits photon antibunching behavior with a g(2)(0) value of ~0.3, intensity saturation, and a linearly cross-polarized doublet, at 4 kelvin. This robust spatial control of electrically driven single-photon emitters will pave the way for the practical implementation of integrated quantum light sources.

Optical read-out of Coulomb staircases in a moiré superlattice via trapped interlayer trions.

Moiré patterns with a superlattice potential can be formed by vertically stacking two layered materials with a relative twist or lattice constant mismatch. In transition metal dichalcogenide-based systems, the moiré potential landscape can trap interlayer excitons (IXs) at specific atomic registries. Here, we report that spatially isolated trapped IXs in a molybdenum diselenide/tungsten diselenide heterobilayer device provide a sensitive optical probe of carrier filling in their immediate environment. By mapping the spatial positions of individual trapped IXs, we are able to spectrally track the emitters as the moiré lattice is filled with excess carriers. Upon initial doping of the heterobilayer, neutral trapped IXs form charged IXs (IX trions) uniformly with a binding energy of ~7 meV. Upon further doping, the empty superlattice sites sequentially fill, creating a Coulomb staircase: stepwise changes in the IX trion emission energy due to Coulomb interactions with carriers at nearest-neighbour moiré sites. This non-invasive, highly local technique can complement transport and non-local optical sensing techniques to characterize Coulomb interaction energies, visualize charge correlated states, or probe local disorder in a moiré superlattice.

Spin-layer locking of interlayer excitons trapped in moiré potentials.

Van der Waals heterostructures offer attractive opportunities to design quantum materials. For instance, transition metal dichalcogenides (TMDs) possess three quantum degrees of freedom: spin, valley index and layer index. Furthermore, twisted TMD heterobilayers can form moiré patterns that modulate the electronic band structure according to the atomic registry, leading to spatial confinement of interlayer excitons (IXs). Here we report the observation of spin-layer locking of IXs trapped in moiré potentials formed in a heterostructure of bilayer 2H-MoSe2 and monolayer WSe2. The phenomenon of locked electron spin and layer index leads to two quantum-confined IX species with distinct spin-layer-valley configurations. Furthermore, we observe that the atomic registries of the moiré trapping sites in the three layers are intrinsically locked together due to the 2H-type stacking characteristic of bilayer TMDs. These results identify the layer index as a useful degree of freedom to engineer tunable few-level quantum systems in two-dimensional heterostructures.

Real-time device-scale imaging of conducting filament dynamics in resistive switching materials.

ReRAM is a compelling candidate for next-generation non-volatile memory owing to its various advantages. However, fluctuation of operation parameters are critical weakness occurring failures in 'reading' and 'writing' operations. To enhance the stability, it is important to understand the mechanism of the devices. Although numerous studies have been conducted using AFM or TEM, the understanding of the device operation is still limited due to the destructive nature and/or limited imaging range of the previous methods. Here, we propose a new hybrid device composed of ReRAM and LED enabling us to monitor the conducting filament (CF) configuration on the device scale during resistive switching. We directly observe the change in CF configuration across the whole device area through light emission from our hybrid device. In contrast to former studies, we found that minor CFs were formed earlier than major CF contributing to the resistive switching. Moreover, we investigated the substitution of a stressed major CF with a fresh minor CF when large fluctuation of operation voltage appeared after more than 50 times of resistive switching in atmospheric condition. Our results present an advancement in the understanding of ReRAM operation mechanism, and a step toward stabilizing the fluctuations in ReRAM switching parameters.

Flexible GaN Light-Emitting Diodes Using GaN Microdisks Epitaxial Laterally Overgrown on Graphene Dots.

The epitaxial lateral overgrowth (ELOG) of GaN microdisks on graphene microdots and the fabrication of flexible light-emitting diodes (LEDs) using these microdisks is reported. An ELOG technique with only patterned graphene microdots is used, without any growth mask. The discrete micro-LED arrays are transferred onto Cu foil by a simple lift-off technique, which works reliably under various bending conditions.

Microtube Light-Emitting Diode Arrays with Metal Cores.

We report the fabrication and characteristics of vertical microtube light-emitting diode (LED) arrays with a metal core inside the devices. To make the LEDs, gallium nitride (GaN)/indium gallium nitride (In(x)Ga(1-x)N)/zinc oxide (ZnO) coaxial microtube LED arrays were grown on an n-GaN/c-aluminum oxide (Al2O3) substrate. The microtube LED arrays were then lifted-off the substrate by wet chemical etching of the sacrificial ZnO microtubes and the silicon dioxide (SiO2) layer. The chemically lifted-off LED layer was then transferred upside-down on other supporting substrates. To create the metal cores, titanium/gold and indium tin oxide were deposited on the inner shells of the microtubes, forming n-type electrodes inside the metal-cored LEDs. The characteristics of the resulting devices were determined by measuring electroluminescence and current-voltage characteristic curves. To gain insights into the current-spreading characteristics of the devices and understand how to make them more efficient, we modeled them computationally.

Nanoscale Single-Element Color Filters.

Visible-light filters constructed from nanostructured materials typically consist of a metallic grating and rely on the excitation of surface plasmon polaritons (SPPs). In order to operate at full efficiency, the number of grating elements needs to be maximized such that light can couple more efficiently to the SPPs through improved diffraction. Such conditions impose a limitation on the compactness of the filter since a larger number of grating elements represents a larger effective size. For emerging applications involving nanoscale transmitters or receivers, a device that can filter localized excitations is highly anticipated but is challenging to realize through grating-type filters. In this work, we present the design of an optical filter operating with a single element, marking a departure from diffractive plasmonic coupling. Our device consists of a ZnO nanorod enclosed by two layers of Ag film. For diffraction-limited light focused on the nanorod, narrow passbands can be realized and tuned via variation of the nanorod diameter across the visible spectrum. The spectral and spatial filtering originates from scattering cancellation localized at the nanorod due to the cavity and nanorod exhibiting opposite effective dipole moments. This ability to realize high-performance optical filtering at the ultimate size introduces intriguing possibilities for nanoscale near-field communication or ultrahigh resolution imaging pixels.

Epitaxial GaN microdisk lasers grown on graphene microdots.

Direct epitaxial growth of inorganic compound semiconductors on lattice-matched single-crystal substrates has provided an important way to fabricate light sources for various applications including lighting, displays and optical communications. Nevertheless, unconventional substrates such as silicon, amorphous glass, plastics, and metals must be used for emerging optoelectronic applications, such as high-speed photonic circuitry and flexible displays. However, high-quality film growth requires good matching of lattice constants and thermal expansion coefficients between the film and the supporting substrate. This restricts monolithic fabrication of optoelectronic devices on unconventional substrates. Here, we describe methods to grow high-quality gallium nitride (GaN) microdisks on amorphous silicon oxide layers formed on silicon using micropatterned graphene films as a nucleation layer. Highly crystalline GaN microdisks having hexagonal facets were grown on graphene dots with intermediate ZnO nanowalls via epitaxial lateral overgrowth. Furthermore, whispering-gallery-mode lasing from the GaN microdisk with a Q-factor of 1200 was observed at room temperature.