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At least 271 records · Page 15

Schottky contacts to N-polar GaN with SiN interlayer for elevated temperature operation

In this Letter, we unveil the high-temperature limits of N-polar GaN Schottky contacts enhanced by a low-pressure chemical vapor deposited (LPCVD) SiN interlayer. Compared to conventional Schottky diodes, the insertion of a 5 nm SiN lossy dielectric interlayer in-between Ni and N-polar GaN increases the turn-on voltage (V ON ) from 0.4 to 0.9 V and the barrier height ($\phi_B$) from 0.4 to 0.8 eV. This modification also reduces the leakage current at zero bias significantly: at room temperature, the leakage current in the conventional Schottky diode is >103 larger than that observed in the device with the SiN interlayer, while at 200 °C, this ratio increases to 105. Thus, the rectification ratio (ION/IOFF) at ±1.5 V reduces to less than one at 250 °C for the conventional Schottky diode, whereas for SiN-coated diodes, rectification continues until 500 °C. The I–V characteristics of the diode with an SiN interlayer can be recovered after exposure to 400 °C or lower. Contact degradation occurs at 500 °C, although devices are not destroyed yet. Here, we report N-polar GaN Schottky contact operation up to 500 °C using an LPCVD SiN interlayer.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Dynamics of carrier injection through V-defects in long wavelength GaN LEDs

The efficiency of high-power operation of multiple quantum well (QW) light emitting diodes (LEDs) to a large degree depends on the realization of uniform hole distribution between the QWs. In long wavelength InGaN/GaN QW LEDs, the thermionic interwell hole transport is hindered by high GaN barriers. However, in polar LED structures, these barriers may be circumvented by the lateral hole injection via semipolar {$10\bar{1}1$} QWs that form on the facets of V-defects. The efficiency of such carrier transfer depends on the transport time since transport in the semipolar QWs is competed by recombination. In this work, we study the carrier transfer from the semipolar to polar QWs by time-resolved photoluminescence in long wavelength (green to red) LEDs. We find that the carrier transfer through the semipolar QWs is fast, a few tens of picoseconds with the estimated room temperature ambipolar diffusion coefficient of ∼5.5 cm 2 /s. With diffusion much faster than recombination, the hole transport from the p-side of the structure to the polar QWs should proceed without a substantial loss, contributing to the high efficiency of long wavelength GaN LEDs.

Crystallographic defects↗

Spatially-resolved dynamic sampling of different phasic magnetic resonances of nanoparticle ensembles in a magnetotactic bacterium Magnetospirillum magnetotacticum

Abstract Nanoscaled magnetic particle ensembles are promising building blocks for realizing magnon based binary logic. Element-specific real-space monitoring of magnetic resonance modes with sampling rates in the GHz regime is imperative for the experimental verification of future complex magnonic devices. Here we present the observation of different phasic magnetic resonance modes using the element-specific technique of time-resolved scanning transmission x-ray microscopy within a chain of dipolarly coupled Fe 3 O 4 nanoparticles (40–50 nm particle size) inside a single cell of a magnetotactic bacterium Magnetospirillum magnetotacticum . The particles are probed with 25 nm resolution at the Fe L 3 x-ray absorption edge in response to a microwave excitation of 4.07 GHz. A plethora of resonance modes is observed within multiple particle segments oscillating in- and out-of-phase, well resembled by micromagnetic simulations.

time-resolved scanning transmission x-ray microsco↗

Self-assembled nanocolumns in Bi 2 Se 3 grown by molecular beam epitaxy

Layered van der Waals (vdW) materials grown by physical vapor deposition techniques are generally assumed to have a weak interaction with the substrate during growth. This leads to films with relatively small domains that are usually triangular and a terraced morphology. In this paper, we demonstrate that Bi 2 Se 3 , a prototypical vdW material, will form a nano-column morphology when grown on GaAs(001) substrates. This morphology is explained by a relatively strong film/substrate interaction, long adatom diffusion lengths, and a high reactive selenium flux. In conclusion, this discovery paves the way toward growth of self-assembled vdW structures even in the absence of strain.

36 MATERIALS SCIENCE↗

Deterministic fabrication of highly reproducible monochromatic quantum emitters in hexagonal boron nitride

Quantum emitters in hexagonal boron nitride are important room temperature single-photon sources. However, conventional fabrication methods yield quantum emitters with dispersed and inconsistent spectral profiles, limiting their potential for practical quantum applications, which demand reproducible high quality single-photon sources. Here, we report the deterministic creation of highly reproducible monochromatic quantum emitters by applying carbon-ion implantation on freestanding hexagonal boron nitride flakes, while a carbon mask with suitable thickness was adapted to optimize the implantation results. Quantum emitters fabricated using this approach exhibited thermally limited monochromaticity, with an emission center wavelength of 590.7 ± 2.7 nm, a narrow full width at half maximum of 7.1 ± 1.7 nm, an emission rate of 1 MHz without optical engineering, and exceptional stability under ambient conditions. Density functional theory calculations and scanning transmission electron microscopy suggest that these emitters are comprised of boron centered carbon tetramers. This method provides a reliable single-photon source for optical quantum computing and potential future industry-scale applications.

Hua, Muchuan [Argonne National Laboratory (ANL), A↗

Nanodiamonds with SiV colour centres for quantum technologies

Properties of silicon-vacancy (SiV) colour centres in ultra-nanosize diamonds are studied. Nanodiamonds are obtained at a high temperature and pressure, which induced transformations in mixtures of organic and hetero-organic compounds without metal-catalysts. The size distribution of grown nanodiamonds is determined by the methods of transmission electron microscopy and atomic-force microscopy, as well as by using the model of phonon spatial localisation. In addition, Raman spectra of various nanodiamonds and luminescence properties of SiV-centres are investigated. (laser applications and other topics in quantum electronics)

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Benchmarking of X‐Ray Fluorescence Microscopy with Ion Beam Implanted Samples Showing Detection Sensitivity of Hundreds of Atoms

Abstract Single impurities in insulators are now often used for quantum sensors and single photon sources, while nanoscale semiconductor doping features are being constructed for electrical contacts in quantum technology devices, implying that new methods for sensitive, non‐destructive imaging of single‐ or few‐atom structures are needed. X‐ray fluorescence (XRF) can provide nanoscale imaging with chemical specificity, and features comprising as few as 100 000 atoms have been detected without any need for specialized or destructive sample preparation. Presently, the ultimate limits of sensitivity of XRF are unknown – here, gallium dopants in silicon are investigated using a high brilliance, synchrotron source collimated to a small spot. It is demonstrated that with a single‐pixel integration time of 1 s, the sensitivity is sufficient to identify a single isolated feature of only 3000 Ga impurities (a mass of just 350 zg). With increased integration (25 s), 650 impurities can be detected. The results are quantified using a calibration sample consisting of precisely controlled numbers of implanted atoms in nanometer‐sized structures. The results show that such features can now be mapped quantitatively when calibration samples are used, and suggest that, in the near future, planned upgrades to XRF facilities might achieve single‐atom sensitivity.

36 MATERIALS SCIENCE↗

Injection mechanisms in a III -nitride light-emitting diode as seen by self-emissive electron microscopy

Here, we report on the investigation of an electrically biased high efficiency green III-nitride light-emitting diode (LED) by electron emission microscopy (EEM) using a low-energy electron microscope (LEEM). The surface of the LED was activated to negative electron affinity via deposition of a submonolayer of Cs. With the illumination column of the LEEM turned off, upon electrical injection of the LED, we directly image the hot electrons generated by eeh Auger-Meitner nonradiative processes that diffuse through the top p-Ga N layer and emit out the surface of the biased LED. By determining the source of emitted electrons using complementary electron emission spectroscopy measurements, EEM allows us to effectively map the carrier density within the LED. Using EEM, we observed nonelectron emitting regions with a density of approximately 3 × 10 8 cm -2 , identified as V-shaped defects (V-defects). This is confirmed through the corresponding dark spots of panchromatic cathodoluminescence measurements of the same sample and by plan-view transmission electron microscopy. The absence of electron emission at the sidewall of the V-defects can be attributed to several factors, including reduced carrier density in the sidewall quantum wells due to carriers traveling fast through the semipolar sidewalls before being injected into the planar quantum wells, the reduced population of hot electrons surviving diffusion through the thicker p-GaN filling in the V-defect before emission onto vacuum, and a smaller Auger-Meitner coefficient for the low In content semipolar sidewall quantum wells. The stronger electron emission observed at the ridges of most V-defects compared to the planar quantum well regions indicates larger local injected carrier densities, confirming that V-defect sidewalls allow for strong lateral carrier injection when compared to the weaker vertical injection away from the V-defect as evidenced by the weaker electron emission intensity away from the V-defects.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Restriction-In-Motion of Surface Ligands Enhances Photoluminescence of Quantum Dots - Experiment and Theory

Here the relationship between emission and ligand restriction of a series of ZnSe/ZnS quantum dots (QDs) encapsulated in nanoparticles is investigated systematically via experiments and quantum theory. The QDs have a ZnSe core and a ZnS shell, capped with hydrophobic ligands (triotylphosphine oxide/hexadecylamine), allowing them to be entrapped in a model biomembrane, bicelle, made of zwitterionic dipalmitoyl and dihexanoyl phosphatidylcholines and charged dipalmitoyl phosphatidylglycerol. Enhanced photoluminescence is observed upon encapsulation, depending on the QD-to-lipid ratio. Transmission electron microscopy and small-angle X-ray scattering confirm that QDs are preferably situated at the rim of bicellar discs. A simplified quantum dissipation heat-bath theory is proposed to correlate the enhancement with slower nonradiative processes caused by the restriction-in-motion (RIM) of the surface ligands. However, Fõrster resonance energy transfer due to QD aggregation counteracts the effect.

36 MATERIALS SCIENCE↗

Ferromagnetic Insulator to Metal Transition in Noncentrosymmetric Graphene Nanoribbons

Engineering sublattice imbalance within the unit cell of bottom-up synthesized graphene nanoribbons (GNRs) represents a versatile tool for realizing custom-tailored quantum nanomaterials. The interaction between low-energy zero-modes (ZMs) not only contributes to frontier bands but can form the basis for magnetically ordered phases. Here, we present the bottom-up synthesis of a noncentrosymmetric GNR that places all ZMs on the majority sublattice sites. Scanning tunneling microscopy and spectroscopy reveal that strong electron–electron correlations, leading to the Stoner magnetic instability, drive the system into a ferromagnetically ordered insulating ground state featuring a sizable band gap of E g ∼1.2 eV. At higher temperatures, a chemical transformation induces an insulator-to-metal transition that quenches the ferromagnetic order. Tight-binding (TB), density functional theory, and GW calculations corroborate our experimental observations. Furthermore, this work showcases how control over molecular symmetry, sublattice polarization, and ZM hybridization in bottom-up synthesized nanographenes can open a path to the exploration of many-body physics in rationally designed quantum materials.

Band structure↗

Leveraging lifetime information to perform real-time 3D single-particle tracking in noisy environments

A microscopy platform that leverages the arrival time of individual photons to enable 3D single-particle tracking of fast-moving (translational diffusion coefficient of ≃ 3.3 µm 2 /s) particles in high-background environments is reported here. It combines a hardware-based time-gating module, which enables the rate of photon processing to be as high as 100 MHz, with a two-photon excited 3D single-particle tracking confocal microscope to enable high sample penetration depth. Proof-of-principle experiments where single quantum dots are tracked in solutions containing dye-stained cellulose are shown, with tracking performance markedly improved using the hardware-based time-gating module. Furthermore, such a microscope design is anticipated to be of use to a variety of communities who wish to track single-particles in cellular environments, which commonly have high fluorescence and scattering background.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Structural and optical properties of cubic GaN on U-grooved Si (100)

Cubic GaN epitaxy on large-area U-grooved silicon (100) dies is demonstrated by metalorganic chemical vapor deposition, and its structural and optical properties are reported. Scanning electron, atomic force, and transmission electron microscopy studies reveal that cubic GaN shows no discernible threading dislocations and a low stacking fault density of 3.27 ± 0.18 × 10 4 cm –1 . Temperature-dependent photoluminescence studies reveal as-grown cubic GaN band edge emission internal quantum efficiency as 25.6% ± 0.9%. Selective etching of the low-temperature AlN buffer layer, SiO 2 sidewalls, and hexagonal-phase GaN is demonstrated, which increases the cubic GaN band edge emission internal quantum efficiency to 31.6% ± 0.8%. This increase is attributed to the decrease in the radiative recombination lifetime via the removal of defective hexagonal-phase GaN. Altogether, cubic GaN on U-grooved silicon with high structural and optical quality is reported, promising its suitability for next-generation devices.

36 MATERIALS SCIENCE↗

Cryogenic Correlative Single‐Particle Photoluminescence Spectroscopy and Electron Tomography for Investigation of Nanomaterials

Abstract Cryogenic single‐particle photoluminescence (PL) spectroscopy has been used with great success to directly observe the heterogeneous photophysical states present in a population of luminescent particles. Cryogenic electron tomography provides complementary nanometer scale structural information to PL spectroscopy, but the two techniques have not been correlated due to technical challenges. Here, we present a method for correlating single‐particle information from these two powerful microscopy modalities. We simultaneously observe PL brightness, emission spectrum, and in‐plane excitation dipole orientation of CdSSe/ZnS quantum dots suspended in vitreous ice. Stable and fluctuating emitters were observed, as well as a surprising splitting of the PL spectrum into two bands with an average energy separation of 80 meV. In some cases, the onset of the splitting corresponded to changes in the in‐plane excitation dipole orientation. These dynamics were assigned to structures of individual quantum dots and the excitation dipoles were visualized in the context of structural features.

Dahlberg, Peter D.↗

Electric Field Control of Magnetic Skyrmion Helicity in a Centrosymmetric 2D van der Waals Magnet

Two-dimensional van der Waals magnets hosting topological magnetic textures, such as skyrmions, show promise for spintronics and quantum computing. Electrical control of these topological spin textures is crucial for enhancing operational performance and functionality. Here, using electron microscopy combined with in situ electric and magnetic biasing, we show that the skyrmion helicity in insulating Cr 2 Ge 2 Te 6 can be controlled by the direction of the external electric field applied during the field cooling process. The electric field-tuned helicity remains stable at low temperature, even amid variations in magnetic and electric fields. Our theoretical investigation reveals that nonzero Dzyaloshinskii-Moriya interactions between nearest neighbors, induced by the electric field, change their sign upon reversing the electric field direction, thereby facilitating helicity selection. The electrical control of magnetic helicity demonstrated in this study can be extended to other centrosymmetric skyrmion-hosting magnets, paving the way for future device designs in topological spintronics and quantum computing.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Edge-Confined Excitons in Monolayer Black Phosphorus

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. Here 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.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Robust estimation of charge carrier diffusivity using transient photoluminescence microscopy

Transient microscopy has emerged as a powerful tool for imaging the diffusion of excitons and free charge carriers in optoelectronic materials. In many excitonic materials, extraction of diffusion coefficients can be simplified because of the linear relationship between signal intensity and local excited state population. However, in materials where transport is dominated by free charge carriers, extracting diffusivities accurately from multidimensional data is complicated by the nonlinear dependence of the measured signal on the local charge carrier density. To obtain accurate estimates of charge carrier diffusivity from transient microscopy data, statistically robust fitting algorithms coupled to efficient 3D numerical solvers that faithfully relate local carrier dynamics to raw experimental measurables are sometimes needed. Here, we provide a detailed numerical framework for modeling the spatiotemporal dynamics of free charge carriers in bulk semiconductors with significant solving speed reduction and for simulating the corresponding transient photoluminescence microscopy data. To demonstrate the utility of this approach, we apply a fitting algorithm using a Markov chain Monte Carlo sampler to experimental data on bulk CdS and methylammonium lead bromide (MAPbBr 3 ) crystals. Parameter analyses reveal that transient photoluminescence microscopy can be used to obtain robust estimates of charge carrier diffusivities in optoelectronic materials of interest, but that other experimental approaches should be used for obtaining carrier recombination constants. Additionally, simplifications can be made to the fitting model depending on the experimental conditions and material systems studied. Our open-source simulation code and fitting algorithm are made freely available to the scientific community.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

CP2 skyrmions and skyrmion crystals in realistic quantum magnets

Abstract Magnetic skyrmions are nanoscale topological textures that have been recently observed in different families of quantum magnets. These objects are called CP 1 skyrmions because they are built from dipoles—the target manifold is the 1D complex projective space, CP 1 ≅ S 2 . Here we report the emergence of magnetic CP 2 skyrmions in a realistic spin-1 model, which includes both dipole and quadrupole moments. Unlike CP 1 skyrmions, CP 2 skyrmions can also arise as metastable textures of quantum paramagnets, opening a new road to discover emergent topological solitons in non-magnetic materials. The quantum phase diagram of the spin-1 model also includes magnetic field-induced CP 2 skyrmion crystals that can be detected with regular momentum- (diffraction) and real-space (Lorentz transmission electron microscopy) experimental techniques.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗