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Secondary electron emission yield measurements of dielectrics based on a novel collector-only method
The total electron-induced Secondary Electron Yield (SEY) of alkali-free glass has been determined by a novel technique which is solely based on the use of a collector electrode and of two interchangeable dielectric samples. The current from a charge-saturated sample provides a direct measure of the primary beam current. The SEY from the (uncharged) sample under investigation can then be determined simply as the ratio between the collector currents measured at the same electron energy from both samples. We further apply a low-current, short-pulse procedure to limit sample charging, needed to mitigate distortion of the SEY by charging effects. The potential build-up during the experiment could be reconstructed based on the primary electron currents and the measured SEY. This strategy permitted us to measure a 6-point SEY curve, without the need for intermediate discharging of the sample, as the total induced surface potential rise could be kept below +2.55 V
Microscopic Proof of Photoluminescence from Mechanochemically Synthesized 1-Octene-Capped Quantum-Confined Silicon Nanoparticles: Implications for Light-Emission Applications
Silicon nanoparticles (SiNPs) have been explored intensively for their use in applications requiring efficient fluorescence for LEDs, lasers, displays, photovoltaic spectral-shifting filters, and biomedical applications. High radiative rates are essential for such applications, and theoretically these could be achieved via quantum confinement and/or straining. Wet-chemical methods used to synthesize SiNPs are under scrutiny because of reported contamination by fluorescent carbon species. To develop a cleaner method, we utilize a specially designed attritor type high-energy ball-mill and use a high-purity (99.999%) Si microparticle precursor. The mechanochemical process is used under a continuous nitrogen gas atmosphere to avoid oxidation of the particles. We confirm the presence of quantum-confined NPs (<5 nm) using atomic force microscopy (AFM). Microphotoluminescence (PL) spectroscopy coupled to AFM confirms quantum-confined tunable red/near-infrared PL emission in SiNPs capped with an organic ligand (1-octene). Using micro-Raman-PL spectroscopy, we confirm SiNPs as the origin of the emission. These results demonstrate a facile and potentially scalable mechanochemical method of synthesis for contamination-free SiNPs
Avoiding Shading Losses in Concentrator Photovoltaics Using a Soft-Imprinted Cloaking Geometry
Shading losses are a longstanding obstacle in photovoltaic devices, particularly in concentrator photovoltaics, where the tradeoff between shading and resistive losses limits the concentration at which the highest power conversion efficiency is achieved to values far below the capabilities of concentrator optics. Here, we demonstrate a simple and scalable fabrication method that enables large front metal coverage while keeping shading losses to a minimum. Soft-imprint lithography is used to create trenches in a transparent polymer above the metal contacts, enabling cloaking via refraction at a range of angles near normal incidence. Using optical characterization techniques, we first confirm that the metal contacts are indeed optically cloaked. We then demonstrate an increase in short-circuit current density from 29.95 to 39.12 mA/cm2 for a Si solar cell with 25% front metal coverage before and after patterning, respectively. We investigate the angular performance of the trench pattern and further demonstrate how such a cloaking strategy could be implemented in concentrator photovoltaics to enable efficiency peaks at concentrations beyond 1000 suns
Holistic Determination of Optoelectronic Properties using High-Throughput Spectroscopy of Surface-Guided CsPbBr3 Nanowires
Optoelectronic micro- and nanostructures have a vast parameter space to explore for modification and optimization of their functional performance. This paper reports on a data-led approach using high-throughput single nanostructure spectroscopy to probe >8000 structures, allowing for holistic analysis of multiple material and optoelectronic parameters with statistical confidence. The methodology is applied to surface-guided CsPbBr3 nanowires, which have complex and interrelated geometric, structural, and electronic properties. Photoluminescence-based measurements, studying both the surface and embedded interfaces, exploits the natural inter nanowire geometric variation to show that increasing the nanowire width reduces the optical bandgap, increases the recombination rate in the nanowire bulk, and reduces the rate at the surface interface. A model of carrier recombination and diffusion ascribes these trends to carrier density and strain effects at the interfaces and self-consistently retrieves values for carrier mobility, trap densities, bandgap, diffusion length, and internal quantum efficiency. The model predicts parameter trends, such as the variation of internal quantum efficiency with width, which is confirmed by experimental verification. As this approach requires minimal a priori information, it is widely applicable to nano- and microscale materials
Avoiding Shading Losses in Concentrator Photovoltaics Using a Soft-Imprinted Cloaking Geometry
Shading losses are a longstanding obstacle in photovoltaic devices, particularly in concentrator photovoltaics, where the tradeoff between shading and resistive losses limits the concentration at which the highest power conversion efficiency is achieved to values far below the capabilities of concentrator optics. Here, we demonstrate a simple and scalable fabrication method that enables large front metal coverage while keeping shading losses to a minimum. Soft-imprint lithography is used to create trenches in a transparent polymer above the metal contacts, enabling cloaking via refraction at a range of angles near normal incidence. Using optical characterization techniques, we first confirm that the metal contacts are indeed optically cloaked. We then demonstrate an increase in short-circuit current density from 29.95 to 39.12 mA/cm2 for a Si solar cell with 25% front metal coverage before and after patterning, respectively. We investigate the angular performance of the trench pattern and further demonstrate how such a cloaking strategy could be implemented in concentrator photovoltaics to enable efficiency peaks at concentrations beyond 1000 suns
Contraction and expansion of nanocomposites during ion exchange reactions
The next generation of advanced functional materials can greatly benefit from methods for realizing the
right chemical composition at the right place. Nanocomposites of amorphous silica and metal carbonate nanocrystals
(BaCO3/SiO2) form an attractive starting point as they can straightforwardly be assembled in different controllable
three-dimensional (3D) shapes, while the chemical composition of the nanocrystals can be completely converted via
ion-exchange. Nevertheless, it is still unknown—let alone predictable—how nanoscopic changes in the lattice volume
of the nanocrystals translate to changes in the microscopic dimensions of the 3D BaCO3/SiO2 structures during
ion-exchange. Here we demonstrate that the microscopic shape adapts to contraction and expansion of the atomic
spacing of nanocrystals. Starting from BaCO3/SiO2, we systematically decrease and increase lattice volumes by converting
the BaCO3 nanocrystals into a range of chalcogenides and perovskites. Based on geometrical analysis, we
obtain a precise prediction for how the microscopic nanocomposite volume follows the change in nanoscopic crystal
volume. The silica matrix facilitates mechanical flexibility to adapt to nanoscopic volume changes, while preserving
the 3D morphology and fine details of the original composite with high fidelity. The versatility and predictability of
shape-preserving conversion reactions open up exciting opportunities for using nanocomposites as functional components.
Introductio
Profusion of transition pathways for interacting hysterons
The response, pathways, and memory effects of cyclically driven complex media can be captured by hysteretic elements called hysterons. Here we demonstrate the profound impact of hysteron interactions on pathways and memory. Specifically, while the Preisach model of independent hysterons features a restricted class of pathways which always satisfy return point memory, we show that three interacting hysterons generate more than 15 000 transition graphs, with most violating return point memory and having features completely distinct from the Preisach model. Exploring these opens a route to designer pathways and information processing in complex matter
Pseudochirality at exceptional rings of optical metasurfaces
Non-Hermitian optical metasurfaces have recently attracted interest as a platform for controlling light in amplitude, phase, and polarization. Here we predict that breaking parity-time symmetry in honeycomblike active plasmonic metasurfaces can lead to nonunitary circular dichroism at oblique incidence. This extraordinary chiroptical response is achieved through band folding that enables coupling of incident light to spin-polarized flat bands surrounded by exceptional rings, formed at Dirac points of plasmonic lattice resonances. The reported spin polarization differs from previously reported chiral and pseudochiral phenomena in that it solely emerges from spatial distribution of gain and loss and at the same time it does not involve the inherent chirality of isolated exceptional points, but instead it can be considered as a non-Hermitian counterpart of spin polarization of K-point valleys. Our findings may become useful in designing and realizing novel polarization-controlling optical elements and spin-polarized exceptional ring lasers
Photon Statistics of Incoherent Cathodoluminescence with Continuous and Pulsed Electron Beams
Photon bunching in incoherent cathodoluminescence (CL) spectroscopy originates from the fact that a single high-energy electron can generate multiple photons when interacting with a material, thus, revealing key properties of electron–matter excitation. Contrary to previous works based on Monte Carlo modeling, here we present a fully analytical model describing the amplitude and shape of the second order autocorrelation function (g(2)(τ)) for continuous and pulsed electron beams. Moreover, we extend the analysis of photon bunching to ultrashort electron pulses, in which up to 500 electrons per pulse excite the sample within a few picoseconds. We obtain a simple equation relating the bunching strength (g(2)(0)) to the electron beam current, emitter decay lifetime, pulse duration, in the case of pulsed electron beams, and electron excitation efficiency (γ), defined as the probability that an electron creates at least one interaction with the emitter. The analytical model shows good agreement with the experimental data obtained on InGaN/GaN quantum wells using continuous, ns-pulsed (using beam blanker) and ultrashort ps-pulsed (using photoemission) electron beams. We extract excitation efficiencies of 0.13 and 0.05 for 10 and 8 keV electron beams, respectively, and we observe that nonlinear effects play no compelling role, even after excitation with ultrashort and dense electron cascades in the quantum wells
Ion Imaging of Native Protein Complexes Using Orthogonal Time-of-Flight Mass Spectrometry and a Timepix Detector
Native mass spectrometry (native MS) has emerged as a powerful technique to study the structure and stoichiometry of large protein complexes. Traditionally, native MS has been performed on modified time-of-flight (TOF) systems combined with detectors that do not provide information on the arrival coordinates of each ion at the detector. In this study, we describe the implementation of a Timepix (TPX) pixelated detector on a modified orthogonal TOF (O-TOF) mass spectrometer for the analysis and imaging of native protein complexes. In this unique experimental setup, we have used the impact positions of the ions at the detector to visualize the effects of various ion optical parameters on the flight path of ions. We also demonstrate the ability to unambiguously detect and image individual ion events, providing the first report of single-ion imaging of protein complexes in native MS. Furthermore, the simultaneous space- and time-sensitive nature of the TPX detector was critical in the identification of the origin of an unexpected TOF signal. A signal that could easily be mistaken as a fragment of the protein complex was explicitly identified as a secondary electron signal arising from ion-surface collisions inside the TOF housing. This work significantly extends the mass range previously detected with the TPX and exemplifies the value of simultaneous space- and time-resolved detection in the study of ion optical processes and ion trajectories in TOF mass spectrometers