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At least 289 records · Page 16

High yield production of ultrathin fibroid semiconducting nanowire of Ta 2 Pd 3 Se 8

Immediately after the demonstration of the high-quality electronic properties in various two dimensional (2D) van der Waals (vdW) crystals fabricated with mechanical exfoliation, many methods have been reported to explore and control large scale fabrications. Comparing with recent advancements in fabricating 2D atomic layered crystals, large scale production of one dimensional (1D) nanowires with thickness approaching molecular or atomic level still remains stagnant. Here, we demonstrate the high yield production of a 1D vdW material, semiconducting Ta 2 Pd 3 Se 8 nanowires, by means of liquid-phase exfoliation. The thinnest nanowire we have readily achieved is around 1 nm, corresponding to a bundle of one or two molecular ribbons. Transmission electron microscopy (TEM) and transport measurements reveal the as-fabricated Ta 2 Pd 3 Se 8 nanowires exhibit unexpected high crystallinity and chemical stability. Our low-frequency Raman spectroscopy reveals clear evidence of the existing of weak inter-ribbon bindings. The fabricated nanowire transistors exhibit high switching performance and promising applications for photodetectors.

1D semiconductor↗

Low temperature recovery of OFF-state stress induced degradation of AlGaN/GaN high electron mobility transistors

Thermal annealing is a widely used strategy to enhance semiconductor device performance. However, the process is complex for multi-material multi-layered semiconductor devices, where thermoelastic stresses from lattice constant and thermal expansion coefficient mismatch may create more defects than those annealed. We propose an alternate low temperature annealing technique, which utilizes the electron wind force (EWF) induced by small duty cycle high density pulsed current. To demonstrate its effectiveness, we intentionally degrade AlGaN/GaN high electron mobility transistors (HEMTs) with accelerated OFF-state stressing to increase ON-resistance ∼182.08% and reduce drain saturation current ∼85.82% of pristine condition at a gate voltage of 0 V. We then performed the EWF annealing to recover the corresponding values back to ∼122.21% and ∼93.10%, respectively. The peak transconductance, degraded to ∼76.58% of pristine at the drain voltage of 3 V, was also recovered back to ∼92.38%. This recovery of previously degraded transport properties is attributed to approximately 80% recovery of carrier mobility, which occurs during EWF annealing. We performed synchrotron differential aperture x-ray microscopy measurements to correlate these annealing effects with the lattice structural changes. We found a reduction of lattice plane spacing of (001) planes and stress within the GaN layer under the gate region after EWF annealing, suggesting a corresponding decrease in defect density. Application of this low-temperature annealing technique for in-operando recovery of degraded electronic devices is discussed.

Physics↗

Integrated Harsh Environment Gas / Temperature Wireless Microwave Acoustic Sensor System for Fossil Energy Applications

There is a significant need for sensors capable of detecting gases, such as H 2 , O 2 , NO x , SO x within harsh environments encountered in power plants, industrial manufacturing, oil and gas exploration, and aerospace applications. This project successfully demonstrated the use of wireless microwave acoustic sensor technology for the detection of gases (H 2 or O 2 ) from ambient temperatures up to 650°C. The work focused on langasite (LGS) based surface acoustic wave resonator (SAWR) sensors as the harsh-environment sensor platform and explored multiple combinations of high-temperature thin films and device structures which were used to increase the sensor platform stability and detection capability at temperatures in the operational range of 150°C to 700°C. Specific material configurations that were investigated include: yttria-stabilized-zirconia (YSZ) decorated with Pt nanoparticles, atomic layer deposited (ALD) Al 2 O 3 , palladium, and Pt/Al 2 O 3 co-deposited electrode alloys. Through the deposition of YSZ at temperatures as high as 850°C and the use of graded alloy concentrations of Pt in the fabrication of the Pt/Al 2 O 3 electrode structures, film stress problems were mitigated, and sensor operation and stability achieved. To test and evaluate SAWR sensor performance for the detection of H 2 and O 2 under the influence of temperature variations, a comprehensive gas sensor control system and test apparatus was created to operate within a laboratory box furnace-controlled environment. In addition to the advancement in thin film materials through the deposition and fabrication techniques mentioned above, the work characterized the performance of sensors containing these films in the presence of oxidizing and reducing gases between 25°C and 700°C. In particular, the work revealed that the exposure of the SAWR sensor surfaces to oxidizing environments significantly improve the sensor response to H 2 , whereas the exposure of the sensor to reducing environments at high temperatures (≈ 500°C) renders the sensor irresponsive to H 2 , requiring sensor surface treatment at high temperatures (above 500°C) to recover the responsiveness to H 2 . The SAWR sensors have been also tested for wireless operation and array operation using multiple orientations to resolve the detection of gases under temperature variations. The work developed at the University of Maine was aided by a collaboration with the NETL Research and Innovation Center, Pittsburgh, PA, where thin film materials and device structures fabricated at UMaine were tested and characterized using NETL gas reactors and surface analysis techniques. SAWR sensors fabricated at UMaine were exposed multiple times to temperatures up to 700°C and H 2 concentrations up to 100% in the NETL facilities to measure the sensor performance. Environetix Technologies Corporation, a UMaine harsh-environment sensor spin-off company, also provided support and assistance in sensor system testing and implementation. The sensor small size and configuration allows flexible sensor placement and embedding of multiple sensor arrays into a variety of components within power systems and other aerospace or industrial settings that need to be interrogated wirelessly. The SAW platform is an attractive option for high-temperature harsh-environment gas sensing applications due to its inherent features, namely small size, capability of battery-free and wireless operation, and cost effective scale production using well-established production techniques from the semiconductor industry. The research findings achieved in this work, particularly advances regarding the fabrication and performance of the SAWR gas sensor platform, can be adapted and transferred to industrial power plants and other harsh environments.

01 COAL, LIGNITE, AND PEAT↗

High Temperature Thick Film Sensor Development Based on Refractory Oxide Semiconductors

Solid-state, high-temperature sensing devices are required for accurate temperature, strain/stress, and failure monitoring for a range of advanced manufacturing, transportation, and military applications. High temperature conditions limit sensing strategies, where typically traditional metal and semiconductor materials are unstable, and the sensing options are limited to optical spectroscopy methods. In addition, strategies to embed the sensors directly within active components and protective thermal refractory are of interest that permit near-environment sensing which is not possible with the traditional electronic materials and components. Rare-earth chromite semiconductors exhibit some properties of interest for high temperature sensing technologies, such as: high microstructure and chemical stability, relatively high electronic conductivity at high temperatures, and relative thermal expansion coefficient matching to refractory thermal protective insulation (such as high-zirconia and -alumina ceramics). In this work, n-type and p-type doped lanthanum chromites compositions were computationally modelled and prepared, and the electrical, thermoelectric, and thermomechanical properties were measured for the obtained material systems. A few compositions were then processed into thick film health and temperature sensors and tested at high temperatures. To establish relative stability under harsh environment conditions, post- mortem microstructure and chemical composition was characterized after extended and cycle testing at high temperatures.

20 FOSSIL-FUELED POWER PLANTS↗

TCAD-Machine Learning Enabled TID Compact Model Development for Commercial SiC MOSFET

We propose a TCAD (Technology Computer Aided Design)-machine learning coupled approach that combines a TCAD tool (Charon), optimization/uncertainty quantification tool (Dakota), surrogate models, and Bayesian learning capabilities. The coupling approach is used for accurate modeling and calibration of total ionizing dose (TID) induced threshold voltage (V th ) shifts in Commercial-Off-The-Shelf (COTS) semiconductor devices and to develop physics-informed TID compact models. This versatile approach is applied to model the TID effect in an exemplar COTS 3.3 kV SiC power MOSFET (Metal-Oxide-Semiconductor Field-Effect Transistor). With the Charon-Dakota coupling, we can determine key device geometry and doping values based on device physics, which are difficult to obtain or not available for COTS devices but important for TCAD simulation; additionally, we can efficiently generate thousands of simulation results in a large parameter space, which makes it possible to develop data-driven surrogate models and perform Bayesian calibration. Utilizing the full tool-coupling approach, we achieve calibrated TCAD simulation models that accurately capture the average TID-induced V th shifts behavior with total doses and V th shifts saturation at high doses as observed in experimental data. More importantly, the calibrated TCAD simulations are obtained with determined TID model parameters (e.g., hole trap density and capture cross section) values that contain well quantified uncertainties. Furthermore, we can isolate and quantify the noises that are not captured by the TCAD models but exist in the measured data due to measurements and devices variabilities. Lastly, the calibrated surrogate models are used to develop physics-informed TID compact models. The method is generalizable to other devices and/or radiation conditions with few modifications and can provide well-determined uncertainties.

COTS↗

Thallium Bromide Semiconductor Radiation Materials and Detectors Characterization Studies

Two overarching requirements of crucial importance for the commercial and scientific establishment of semiconductor radiation detectors are: (1) exceptionally high-purity crystals with impurity concentrations less than 1 part-per-billion and (2) single crystals that are relatively free from subgrain boundaries, secondary phases, dislocations, and other electrically-active defects. We investigated the properties of thallium bromide (TlBr) material that affect its performance with the goal of increasing the material's commercial viability for radiation detection applications. For this purpose, we used beamlines at the National Synchrotron Light Source (NSLS) at Brookhaven National Laboratory (BNL), performing Micron-scale X-ray Detector Mapping, White Beam X-ray Diffraction Topography, and Micron-scale X-ray Fluorescence. These characterization methods improve the industry's understanding of TlBr and lead to the production of improved instrumentation. In this particular study we report electro-migration measurements of positive-ion Cu, Ag, and Au impurities in TlBr detectors under electric field strengths typically used for device operation. BNL improved TlBr detectors with an electrode design that corrects the response non-uniformities caused by crystal defects. This design can achieve improved energy resolution while using typical-grade, commercial crystals with relaxed quality requirements, thus reducing the overall cost of detectors. Additional characterization will be necessary to fully understand the structure and performance of TlBr with the ultimate goal to achieve the highest energy resolution. Our findings from past work will be presented along with our recommendations for additional investigation.

36 MATERIALS SCIENCE↗

Optoelectronic and structural characterization of trapezoidal defects in 4H-SiC epilayers and the effect on MOSFET reliability

To this day, trapezoidal defects are found in clusters and high counts in wafers representing the industry standard in terms of material quality being produced. This study sheds light on the nature, origin, behavior, and impact of this defect on device yield and reliability. Trapezoidal defects in 4H-SiC epitaxial layers were investigated by photoluminescence (PL) imaging, scanning electron microscopy (SEM), cathodoluminescence spectrum imaging (CLSI), SEM electron beam induced current (EBIC) imaging, and by transmission electron microscopy (TEM) observation. The bar-shaped stacking faults were identified by the PL and CL measurements with a peak emission wavelength of 420 and 450 nm. An optoelectronic behavioral study based on the recombination enhanced dislocation glide mechanism revealed how expanding dislocations and stacking faults interact with each other. Combining the luminescence and microscopy results, the nature of the stacking faults was identified as being a combination of Shockley-type and Frank-type stacking faults. The TEM analysis showed that these defects originate from the substrate and the stacking sequences of some of the faults were determined as (…2, 4, 2…) and (…2, 3, 2…) in the Zhdanov's notation by high-resolution TEM. The origin of this defect is speculated based on our results and previous reports. The EBIC imaging showed that the high density of SFs in these towers is a strong site of carrier recombination, which presumably has an impact on the transfer characteristics of SiC devices. Furthermore, these defects have shown to impact metal oxide semiconductor field effect transistors electrical performance via an increase in the on-state resistance depending on the coverage percentage of the tower of defects in the active area of the device.

4H-SiC↗

Interdigitated electrode geometry variation and external quantum efficiency of GaN/AlGaN-based metal-semiconductor-metal UV photodetectors

Aluminum gallium-nitride (Al x Ga 1–x N)-based metal–semiconductor–metal (MSM) ultraviolet photodetectors photodetectors (PD’s) have been successfully designed and fabricated using conventional photolithography techniques and tested experimentally to study their spectral sensitivity across different Al content, x, with x varying from 0 to 0.3. (Al)GaN-based UV PD’s have wide and tunable direct band gaps. The ability to easily select the photodetected wavelength by simply varying the aluminum content of GaN thin film (Al x Ga 1–x N) is a significant advantage of these group III–V compounds. Typically, MSM PD’s grown on (Al)GaN thin films result in ultrafast photodetection because of their highly mobile carriers. These devices are limited by the carrier transit time due to the negligible capacitance presented by the interdigitated fingers. Various electrode geometries were fabricated to investigate the influence of metal contact shapes on the devices’ performance indices with emphasis on the response speed and bias-voltage–independent efficiency. Here, coupled with the independently measured Hall mobility and electric field, we computed the carrier transit time of the devices to be as short as 1.31 ps and the bias-voltage–independent external quantum efficiencies were as high as 70% at 60 V for n-doped and intrinsic devices when operated in the reverse bias regime. Here, (Al x )Ga 1–x N photodetectors were designed to explore spectral sensitivity by altering x from 0 to 0.3.

42 ENGINEERING↗

Polarization-induced 2D electron gases in N-polar AlGaN/AlN heterostructures on single-crystal AlN substrates

Polarization-induced carriers play an important role in achieving high electrical conductivity in ultrawide bandgap semiconductor AlGaN, which is essential for various applications ranging from radio frequency and power electronics to deep UV photonics. Despite significant scientific and technological interest, studies on polarization-induced carriers in N-polar AlGaN are rare. We report the observation and properties of polarization-induced two-dimensional electron gases (2DEGs) in N-polar AlGaN/AlN heterostructures on single-crystal AlN substrates by systematically varying the Al content in the 8 nm top layers from x = 0 to x = 0.6, spanning energy bandgaps from 3.56 to 4.77 eV. The 2DEG density drops monotonically with increasing Al content, from 3.8 × 1013/cm2 in the GaN channel, down to no measurable conductivity for x = 0.6. Alloy scattering limits the 2DEG mobility to below 50 cm2/V s for x = 0.49. These results provide valuable insights for designing N-polar AlGaN channel high electron mobility transistors on AlN for extreme electronics at high voltages and high temperatures, and for UV photonic devices.

Physics↗

Highly efficient photoelectric effect in halide perovskites for regenerative electron sources

Electron sources are a critical component in a wide range of applications such as electron-beam accelerator facilities, photomultipliers, and image intensifiers for night vision. We report efficient, regenerative and low-cost electron sources based on solution-processed halide perovskites thin films when they are excited with light with energy equal to or above their bandgap. We measure a quantum efficiency up to 2.2% and a lifetime of more than 25 h. Importantly, even after degradation, the electron emission can be completely regenerated to its maximum efficiency by deposition of a monolayer of Cs. The electron emission from halide perovskites can be tuned over the visible and ultraviolet spectrum, and operates at vacuum levels with pressures at least two-orders higher than in state-of-the-art semiconductor electron sources.

36 MATERIALS SCIENCE↗

Monocrystalline 1.7-eV MgCdTe solar cells

Monocrystalline 1.7-eV Mg 0.13 Cd 0.87 Te/Mg x Cd 1-x Te (x > 0.13) double-heterostructure (DH) solar cells with varying Mg composition in the barrier layers are grown by molecular beam epitaxy. Furthermore, a Mg 0.13 Cd 0.87 Te/Mg 0.37 Cd 0.63 Te DH solar cell featuring abrupt interfaces between barriers and absorber and the addition of a SiO 2 anti-reflective coating demonstrates open-circuit voltage (V OC ), short-circuit current density (J SC ), fill factor (FF), and device active-area efficiencies up to 1.129 V, 17.3 mA/cm 2 , 77.7% and 15.2%, respectively. The V OC and FF vary oppositely with the Mg x Cd 1-x Te barrier height indicating an optimal design of the MgCdTe DHs as a tradeoff between carrier confinement and carrier transport. Temperature-dependent V OC measurements reveal the majority of carrier recombination in the devices occurs outside the DHs, in the a-Si:H hole-contact layer and at the interface between the a-Si:H layer and the Mg x Cd 1-x Te top barrier at room temperature. Simulation results for the device with the highest efficiency show that the p-type a-Si:H layer and Mg 0.37 Cd 0.63 Te top barrier contribute 1.3 mA/cm 2 and 2.4 mA/cm 2 J SC loss, respectively.

14 SOLAR ENERGY↗

Rashba splitting in organic–inorganic lead–halide perovskites revealed through two-photon absorption spectroscopy

Abstract The Rashba splitting in hybrid organic–inorganic lead–halide perovskites (HOIP) is particularly promising and yet controversial, due to questions surrounding the presence or absence of inversion symmetry. Here we utilize two-photon absorption spectroscopy to study inversion symmetry breaking in different phases of these materials. This is an all-optical technique to observe and quantify the Rashba effect as it probes the bulk of the materials. In particular, we measure two-photon excitation spectra of the photoluminescence in 2D, 3D, and anionic mixed HOIP crystals, and show that an additional band above, but close to the optical gap is the signature of new two-photon transition channels that originate from the Rashba splitting. The inversion symmetry breaking is believed to arise from ionic impurities that induce local electric fields. The observation of the Rashba splitting in the bulk of HOIP has significant implications for the understanding of their spintronic and optoelectronic device properties.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Solution-Grown Ternary Semiconductors: Nanostructuring and Stereoelectronic Lone Pair Distortions in I–V–VI 2 Materials

Alkali pnictogen dichalcogenides–I–V–VI 2 or APnCh 2 –have been identified as promising semiconducting materials for energy conversion devices. However, the controlled nanoscale synthesis and our understanding of the effects of cation ordering and stereochemically active lone pairs on the structures of these ternary compounds remain underdeveloped. Here, we use solution-phase chemistry to synthesize a family of APnCh 2 materials, including LiSbSe 2 , NaSbS 2 , NaSbSe 2 , NaBiS 2 , and NaBiSe 2 . Our approach utilizes alkali metal hydrides (AH) or carboxylates, A(O 2 CR), PnPh 3 , and elemental chalcogens as synthetic precursors and oleylamine or 1-octadecene as solvents. Synthetic manipulation via fine-tuning of reaction temperature enables control over the degree of ordering caused by the Sb 5s 2 lone pair-induced distortions in NaSbS 2 . Pair distribution function analysis demonstrates that the structure of the Sb-containing phases deviates much more from a disordered rock salt structure than that of the Bi-containing phases. This local distortion, induced by the Sb lone pair, leads to a previously unreported noncentrosymmetric NaSbS 2 crystal structure, which is additionally supported by second-harmonic generation measurements. Infrared and multinuclear solid-state NMR spectroscopies show that oleylamine or chelating carboxylates and, in some cases, unreacted precursors (LiH and PnPh 3 ) remain bound to the nanocrystalline surfaces. Further, a deeper understanding of the local atomic environment, long-range ordering, surface chemistry, and optoelectronic properties of these materials may speed up their fundamental study and application.

36 MATERIALS SCIENCE↗

Direct Optoelectronic Imaging of 2D Semiconductor–3D Metal Buried Interfaces

The semiconductor-metal junction is one of the most critical factors for high performance electronic devices. In two-dimensional (2D) semiconductor devices, minimizing voltage drop at this junction is of particularly challenging and important. Despite numerous studies on contact resistance in 2D semiconductors, the exact nature of the buried interface under a 3D metal remains elusive and unclear. Herein, we report the direct observation of 2D semiconductor-metal buried interface using recently developed metal-assisted transfer technique to expose the buried interface which is then directly investigated using scanning probe techniques. We characterize the spatially varying electronic and optical properties of this buried interface with < 20 nm resolution. To be specific, potential, conductance and photoluminescence at the buried metal/MoS 2 interface are correlated under variety of metal deposition conditions as well as type of metal contacts. We observe that direct evaporation of Au on MoS 2 induces large strain of ~5% in the MoS 2 which coupled with charge transfer leads to degenerate doping of the MoS 2 underneath the contact. These factors lead to improvement of contact resistance to record values of 138 kΩ μm measured using local conductance probes. This approach was adopted to investigate MoS 2 -In/Au alloy interface, which records lowest contact resistance of 63 kΩ μm. Overall, our results highlight that the MoS 2 /Metal interface is very sensitive to method of contact making and provides a universal strategy to characterize buried contact interfaces involving 2D semiconductors.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

High broadband photoconductivity of few-layered MoS 2 field-effect transistors measured using multi-terminal methods: effects of contact resistance

Among the layered two dimensional semiconductors, molybdenum disulfide (MoS 2 ) is considered to be an excellent candidate for applications in optoelectronics and integrated circuits due to its layer-dependent tunable bandgap in the visible region, high ON/OFF current ratio in field-effect transistors (FET) and strong light–matter interaction properties. In this study, using multi-terminal measurements, we report high broadband photocurrent response ( R ) and external quantum efficiency (EQE) of few-atomic layered MoS 2 phototransistors fabricated on a SiO 2 dielectric substrate and encapsulated with a thin transparent polymer film of Cytop. The photocurrent response was measured using a white light source as well as a monochromatic light of wavelength λ = 400 nm–900 nm. We measured responsivity using a 2-terminal configuration as high as R = 1 × 10 3 A W -1 under white light illumination with an optical power P opt = 0.02 nW. The R value increased to 3.5 × 10 3 A W -1 when measured using a 4-terminal configuration. Using monochromatic light on the same device, the measured values of R were 10 3 and 6 × 10 3 A W -1 under illumination of λ = 400 nm when measured using 2- and 4-terminal methods, respectively. The highest EQE values obtained using λ = 400 nm were 10 5 % and 10 6 % measured using 2- and 4-terminal configurations, respectively. The wavelength dependent responsivity decreased from 400 nm to the near-IR region at 900 nm. The observed photoresponse, photocurrent–dark current ratio (PDCR), detectivity as a function of applied gate voltage, optical power, contact resistances and wavelength were measured and are discussed in detail. The observed responsivity is also thoroughly studied as a function of contact resistance of the device.

36 MATERIALS SCIENCE↗

n–Doping of a Low–Electron–Affinity Polymer Used as an Electron–Transport Layer in Organic Light–Emitting Diodes

n-Doping electron-transport layers (ETLs) increases their conductivity and improves electron injection into organic light-emitting diodes (OLEDs). Because of the low electron affinity and large bandgaps of ETLs used in green and blue OLEDs, n-doping has been notoriously more difficult for these materials. In this work, n-doping of the polymer poly[(9,9-dioctylfluorene-2,7-diyl)-alt-(benzo[2,1,3]thiadiazol-4,7-diyl)] (F8BT) is demonstrated via solution processing, using the air-stable n-dopant (pentamethylcyclopentadienyl)(1,3,5-trimethylbenzene)ruthenium dimer [RuCp*Mes] 2 . Undoped and doped F8BT films are characterized using ultraviolet and inverse photoelectron spectroscopy. The ionization energy and electron affinity of the undoped F8BT are found to be 5.8 and 2.8 eV, respectively. Upon doping F8BT with [RuCp*Mes] 2 , the Fermi level shifts to within 0.25 eV of the F8BT lowest unoccupied molecular orbital, which is indicative of n-doping. Conductivity measurements reveal a four orders of magnitude increase in the conductivity upon doping and irradiation with ultraviolet light. Here, the [RuCp*Mes] 2 -doped F8BT films are incorporated as an ETL into phosphorescent green OLEDs, and the luminance is improved by three orders of magnitude when compared to identical devices with an undoped F8BT ETL.

36 MATERIALS SCIENCE↗

Atomically Precise Graphene Nanoribbon Transistors with Long-Term Stability and Reliability

Atomically precise graphene nanoribbons (GNRs) synthesized from the bottom-up exhibit promising electronic properties for high-performance field-effect transistors (FETs). The feasibility of fabricating FETs with GNRs (GNRFETs) has been demonstrated, with ongoing efforts aimed at further improving their performance. However, their long-term stability and reliability remain unexplored, which is as important as their performance for practical applications. In this work, we fabricated short-channel FETs with nine-atom-wide armchair GNRs (9-AGNRFETs). We revealed that the on-state (/ ON ) current performance of the 9-AGNRFETs deteriorates significantly over consecutive full transistor on and off logic cycles, which has neither been demonstrated nor previously considered. To address this issue, we deposited a thin ~10 nm thick atomic layer deposition (ALD) layer of aluminum oxide (Al 2 O 3 ) directly on these devices. The integrity, compatibility, electrical performance, stability, and reliability, of the GNRFETs before and/or after Al 2 O 3 deposition were comprehensively studied. The results indicate that the observed decline in electrical device performance is most likely due to the degradation of contact resistance over multiple measurement cycles. We successfully demonstrated that the devices with the Al 2 O 3 layer operate well up to several thousand continuous full cycles without any degradation. Our study offers valuable insights into the stability and reliability of GNR transistors, which could facilitate their large-scale integration into practical applications.

36 MATERIALS SCIENCE↗

Near-field imaging of plasmonic nanopatch antennas with integrated semiconductor quantum dots

Plasmonic nanopatch antennas that incorporate dielectric gaps hundreds of picometers to several nanometers thick have drawn increasing attention over the past decade because they confine electromagnetic fields to grossly sub-diffraction-limited volumes. Substantial control over the optical properties of excitons and color centers confined within these plasmonic cavities has already been demonstrated with far-field optical spectroscopies, but near-field optical spectroscopies are essential for an improved understanding of the plasmon–emitter interaction at the nanoscale. Here, we characterize the intensity and phase-resolved plasmonic response of isolated nanopatch antennas by cathodoluminescence microscopy. Furthermore, we explore the distinction between optical and electron beam spectroscopies of coupled plasmon–exciton heterostructures to identify constraints and opportunities for future nanoscale characterization and control of hybrid nanophotonic structures. While we observe substantial Purcell enhancement in time-resolved photoluminescence spectroscopies, negligible Purcell enhancement is observed in cathodoluminescence spectroscopies of hybrid nanophotonic structures. The substantial differences in measured Purcell enhancement for electron beam and laser excitation can be understood as a result of the different selection rules for these complementary experiments. Overall, these results provide a fundamentally new understanding of near-field plasmon–exciton interactions in nanopatch antennas, which is essential for myriad emerging quantum photonic devices.

36 MATERIALS SCIENCE↗