Low Electron Flux Research Articles

Modeling the Global Distribution of Chorus Wave Induced Relativistic Microburst Spatial Characteristics

AbstractThe full spatiotemporal distribution of chorus wave‐induced relativistic electron microburst is modeled for chorus waves originated from different L shells and MLTs, based on the newly developed numerical precipitation model (Kang et al., 2022, https://doi.org/10.1029/2022gl100841). The wave‐particle interaction process that induces each microburst is analyzed in detail, and its relation to the chorus wave propagation effects is explained. The global distribution of maximum precipitation fluxes and scale sizes of relativistic microbursts is then obtained by modeling chorus waves at different L‐shells and local times. The characteristics of dawn and midnight sector microbursts have little difference, but the noon sector has much larger maximum flux and much smaller full width at half maximum, which may be due to dayside's low electron flux in the Landau resonance range. This suggests the controlling effect of keV electrons on the MeV electron precipitation intensity and properties and the overall relativistic electron loss in the outer radiation belt.

Goethite Mineral Dissolution to Probe the Chemistry of Radiolytic Water in Liquid-Phase Transmission Electron Microscopy.

Liquid-Phase Transmission Electron Microscopy (LP-TEM) enables in situ observations of the dynamic behavior of materials in liquids at high spatial and temporal resolution. During LP-TEM, incident electrons decompose water molecules into highly reactive species. Consequently, the chemistry of the irradiated aqueous solution is strongly altered, impacting the reactions to be observed. However, the short lifetime of these reactive species prevent their direct study. Here, the morphological changes of goethite during its dissolution are used as a marker system to evaluate the influence of radiation on the changes in solution chemistry. At low electron flux density, the morphological changes are equivalent to those observed under bulk acidic conditions, but the rate of dissolution is higher. On the contrary, at higher electron fluxes, the morphological evolution does not correspond to a unique acidic dissolution process. Combined with kinetic simulations of the steady state concentrations of generated reactive species in the aqueous medium, the results provide a unique insight into the redox and acidity interplay during radiation induced chemical changes in LP-TEM. The results not only reveal beam-induced radiation chemistry via a nanoparticle indicator, but also open up new perspectives in the study of the dissolution process in industrial or natural settings.

Ligand Size and Carbon-Chain Length Study of Silver Carboxylates in Focused Electron-Beam-Induced Deposition.

Gas-assisted focused electron-beam-induced deposition is a versatile tool for the direct writing of complex-shaped nanostructures with unprecedented shape fidelity and resolution. While the technique is well-established for various materials, the direct electron beam writing of silver is still in its infancy. Here, we examine and compare five different silver carboxylates, three perfluorinated: [Ag2(µ-O2CCF3)2], [Ag2(µ-O2CC2F5)2], and [Ag2(µ-O2CC3F7)2], and two containing branched substituents: [Ag2(µ-O2CCMe2Et)2] and [Ag2(µ-O2CtBu)2], as potential precursors for focused electron-beam-induced deposition. All of the compounds show high sensitivity to electron dissociation and efficient dissociation of Ag-O bonds. The as-deposited materials have silver contents from 42 at.% to above 70 at.% and are composed of silver nano-crystals with impurities of carbon and fluorine between them. Precursors with the shortest carbon-fluorine chain ligands yield the highest silver contents. In addition, the deposited silver content depends on the balance of electron-induced ligand co-deposition and ligand desorption. For all of the tested compounds, low electron flux was related to high silver content. Our findings demonstrate that silver carboxylates constitute a promising group of precursors for gas-assisted focused electron beam writing of high silver content materials.

Maximizing electron flux, microbial diversity and gene abundance in MFC powered electro-Fenton system by optimizing co-addition of lysozyme and 2-bromoethanesulfonate

In this study, a microbial fuel cell powered electro-Fenton system (MFCⓅEFs) was established in order to overcome the shortcomings of low electron flux and unexpected methane production, while simultaneously treating excess sludge (ES, substrate) and refractory syringic acid (SA). A strategy of co-adding lysozyme (LZ, as ES degradation catalyst) and 2-bromoethanesulfonate (BES, as methane inhibitor) into ES was optimized in MFCⓅEFs to maximize electron flux, microbial community diversity and functional gene abundance. The removal of sludge total chemical oxygen demand (TCOD) achieved 81.69% in 25 d under an optimal co-addition strategy (40.41 mg/gSS of LZ, 27.03 mmol/L of BES, adding on 22.8 h of the7th day), with a simultaneous high degradation of SA (99.30% in 25 h). Correspondingly, a maximum power density of 3.35 W/m3 was achieved (only 0.62 W/m3 from the control), which effectively realizes in-situ micro-electricity generation and utilization for bioelectric Fenton processes. Moreover, 42.25% of the total charges were employed for bio-electricity generation. The electricigens of Pseudomonas, Acinetobacter and Chlorobium showed effective enrichment, while the abundance of methanogenesis archaea was extremely decreased. Functional genes associated with methanogenesis including mtaA, hdra, and mcrA were effectively inhibited. The life cycle assessment along with an optimized co-addition strategy illustrated a beneficial environmental effect, particularly in terms of ecosystem quality and climate change. Above all, an enhanced synchronous degradation of excess sludge and refractory pollutants had been realized in a green and environmentally friendly way.

In situ STEM analysis of electron beam induced chemical etching of an ultra-thin amorphous carbon foil by oxygen during high resolution scanning

Support foils for (scanning) transmission electron microscopy ((S)TEM) samples are commonly amorphous carbon foils. State of the art (S)TEM high resolution imaging methods use ultra-thin carbon foils of only a few nm thickness, especially for imaging beam sensitive materials with low acceleration voltages and electron fluxes. In this study we analyze in situ the effect of chemical etching on a 2 nm amorphous carbon foil due to residual oxygen and by leaking in oxygen into the microscope column. We vary the vacuum level on a Nion UltraStem 100 between ultra high vacuum and that typical in TEM. This enables us to carry out a systematic investigation of chemical etching as function of both, oxygen pressure and electron flux. In addition the results of chemical etching are compared with those of sputtering from knock-on damage leading to the conclusion that chemical etching is the important cause for carbon removal from an amorphous foil at low oxygen pressures and low electron fluxes. We observe that the electron flux dependency using high resolution scanning conditions differs from the case of a resting electron beam. To interpret the results of chemical etching a scanning etching model is proposed that takes care of the specific conditions of STEM.

The 600 keV electron injections in the Earth’s outer radiation belt: A statistical study

Relativistic electron injections are one of the mechanisms of relativistic (≥0.5 MeV) electron enhancements in the Earth’s outer radiation belt. In this study, we present a statistical observation of 600 keV electron injections in the outer radiation belt by using data from the Van Allen Probes. On the basis of the characteristics of different injections, 600 keV electron injections in the outer radiation belt were divided into pulsed electron injections and nonpulsed electron injections. The 600 keV electron injections were observed at 4.5 &lt; <i>L</i> &lt; 6.4 under the geomagnetic conditions of 450 nT &lt; <i>AE</i> &lt; 1,450 nT. An <i>L</i> of ~4.5 is an inward limit for 600 keV electron injections. Before the electron injections, a flux negative<i> L</i> shell gradient for ≤0.6 MeV electrons or low electron fluxes in the injected region were observed. For 600 keV electron injections at different <i>L</i> shells, the source populations from the Earth’s plasma sheet were different. For 600 keV electron injections at higher <i>L</i> shells, the source populations were higher energy electrons (~200 keV at <i>X</i> ~ –9 <i>R</i>_E), whereas the source populations for 600 keV electron injections at lower <i>L</i> shells were lower energy electrons (~80 keV at <i>X</i> ~ –9 <i>R</i>_E). These results are important to further our understanding of electron injections and rapid enhancements of 600 keV electrons in the Earth’s outer radiation belt.

Beam-induced heating at low electron fluxes during liquid phase transmission electron microscopy

Beam-induced heating at low electron fluxes during liquid phase transmission electron microscopy

Reconstruction of the Radiation Belts for Solar Cycles 17–24 (1933–2017)

AbstractWe present a reconstruction of the dynamics of the radiation belts from solar cycles 17 to 24 which allows us to study how radiation belt activity has varied between the different solar cycles. The radiation belt simulations are produced using the Versatile Electron Radiation Belt (VERB)‐3D code. The VERB‐3D code simulations incorporate radial, energy, and pitch angle diffusion to reproduce the radiation belts. Our simulations use the historical measurements of Kp (available since solar cycle 17, i.e., 1933) to model the evolution radiation belt dynamics between L* = 1–6.6. A nonlinear auto regressive network with exogenous inputs (NARX) neural network was trained off GOES 15 measurements (January 2011–March 2014) and used to supply the upper boundary condition (L* = 6.6) over the course of solar cycles 17–24 (i.e., 1933–2017). Comparison of the model with long term observations of the Van Allen Probes and CRRES demonstrates that our model, driven by the NARX boundary, can reconstruct the general evolution of the radiation belt fluxes. Solar cycle 24 (January 2008–2017) has been the least active of the considered solar cycles which resulted in unusually low electron fluxes. Our results show that solar cycle 24 should not be used as a representative solar cycle for developing long term environment models. The developed reconstruction of fluxes can be used to develop or improve empirical models of the radiation belts.

Mapping Grains, Boundaries, and Defects in 2D Covalent Organic Framework Thin Films.

To improve their synthesis and ultimately realize the technical promise of two-dimensional covalent organic frameworks (2D COFs), it is imperative that a robust understanding of their structure be developed. However, high-resolution transmission electron microscopy (HR-TEM) imaging of such beam-sensitive materials is an outstanding characterization challenge. Here, we overcome this challenge by leveraging low electron flux imaging conditions and high-speed direct electron counting detectors to acquire high-resolution images of 2D COF films. We developed a Fourier mapping technique to rapidly extract nanoscale structural information from these TEM images. This postprocessing script analyzes the evolution of 2D Fourier transforms across a TEM image, which yields information about polycrystalline domain orientations and enables quantification of average domain sizes. Moreover, this approach provides information about several types of defects present in a film, such as overlapping grains and various types of grain boundaries. We also find that the pre-eminent origin of defects in COF-5 films, a prototypical boronate ester-linked COF, arises as a consequence of broken B-O bonds formed during polymerization. These results suggest that the nanoscale features observed are a direct consequence of chemical phenomena. Taken together, this mapping approach provides information about the fundamental microstructure and crystallographic underpinnings of 2D COF films, which will guide the development of future 2D polymerization strategies and help realize the goal of using 2D COFs in a host of thin-film device architectures.

Unhindered Brownian Motion of Individual Nanoparticles in Liquid-Phase Scanning Transmission Electron Microscopy.

Liquid-phase transmission electron microscopy (LPTEM) offers label-free imaging of nanoparticle (NP) processes in liquid with sub-nanometer spatial and millisecond temporal resolution. However, LPTEM studies have reported only on NPs moving orders of magnitude slower than expected from bulk aqueous liquid conditions, likely due to strong interactions with the LPTEM liquid-enclosing membranes. We demonstrate how scanning transmission electron microscope (STEM) imaging can be used to measure the motion of individual NPs and agglomerates, which are not hindered by such interactions. Only at low electron flux do we find that individual NPs exhibit Brownian motion consistent with optical control experiments and theoretical predictions for unhindered passive diffusive motion in bulk liquids. For increasing electron flux, we find increasingly faster than passive motion that still appears effectively Brownian. We discuss the possible origins of this beam-sample interaction. This establishes conditions for the use of STEM as a reliable tool for imaging nanoscale hydrodynamics in situ TEM.

Solar activity phase dependence of the magnetospheric processes and relativistic electron flux at geostationary orbit

This study aims to investigate the effects of the solar activity phases on the magnetospheric processes in relation to daily relativistic electron ($E>2$ MeV) dynamics at geosynchronous orbit (GEO) during Solar Cycles 23–24. GOES observations indicate that in the descending phase the electron fluxes are seasonally dependent with largest flux in equinoctial periods, relatively high, and 27-day recurrent, while in the maximum phases they are relatively low and nonrecurrent. The electron fluxes are relatively low and partially recurrent in the ascending phases. The cross correlation coefficients (c.c.s) of daily $K_{\textrm{p}}$–$V_{\textrm{sw}}$, $K_{\textrm{p}}$–$AE$, $K_{\textrm{p}}$–$AL$ evolve in the similar trend for both solar cycles: highest during the descending phases, lower in the ascending phases, and lowest in the maximum and minimum phases. The correlation of $K_{\textrm{p}}$–viscous term is strongest during descending phases and weakest around the maximum phases. The correlation of $K_{\textrm{p}}$–merging term slightly varies in a chaotic way from one solar phase to another, but drops to its lowest value in the solar minimum. The correlation analysis results signify the role of the solar activity in controlling the solar wind–magnetosphere couplings. Two case studies during maximum (2000) and descending (2017) phases indicate that the solar activity dependence of the magnetospheric processes and relativistic electrons is characterized by substorm activity and solar wind drivers. Most of the substorms induced by coronal mass ejections in the maximum phase exhibit strong but short and non-repetitive features that associate with low electron fluxes at GEO. In contrast, high intensity, prolonged, and repetitive substorm activities induced by high-speed solar winds are the main cause of the relativistic electron enhancements during the descending phases. The enhancements strongly depend on $V_{\textrm{sw}}$ and $\Sigma K_{\textrm{p}}$ in which only appropriate $V_{\textrm{sw}}$ and $\Sigma K_{\textrm{p}}$ are required. In the descending phase, the requirements for the flux enhancements to $\geq 10^{3}$ cm−2 sr−1 s−1 are the simultaneity of $V_{\textrm{sw}}>500$ km/s and the prolongation of $\Sigma K_{\textrm{p}}>220$ and to $\geq 10^{4}$ cm−2 sr−1 s−1 when $V_{\textrm{sw}}\geq 630$ km/s and $\Sigma K_{\textrm{p}}>227$. Furthermore, the correlations of $\Sigma K_{\textrm{p}}$ and log-electron fluxes are stronger in the descending/ascending phases than in the maximum phase, while the time lag between them is longer in the maximum phase. The remarkable correlations of $V_{\textrm{sw}}$–$K_{\textrm{p}}$ and in the descending phase indicate appropriate magnetospheric convection in association with the repetitive substorms that can effectively trigger the stochastic mechanisms of electron acceleration. The results are extensively discussed in the light of observations and current theories of radiation belt dynamics.

Forecasting Megaelectron‐Volt Electrons Inside Earth's Outer Radiation Belt: PreMevE 2.0 Based on Supervised Machine Learning Algorithms

AbstractWe present the recent progress in upgrading a predictive model for megaelectron‐volt (MeV) electrons inside the Earth's outer Van Allen belt. This updated model, called PreMevE 2.0, provides improved forecasts, particularly at outer L‐shells, by adding upstream solar wind speeds to the model's input parameter list that originally includes precipitating electrons observed at low Earth orbits and MeV electron fluxes in situ measured by a geosynchronous satellite. Furthermore, based on several kinds of linear and artificial neural networks algorithms, a list of models was constructed, trained, validated, and tested with 42‐month MeV electron observations from Van Allen Probes. Out‐of‐sample test results from these models show that, with optimized model hyperparameters and input parameter combinations, the top performer from each category of models has the similar capability of making reliable 1‐day (2‐day) forecasts of 1‐MeV electron flux distributions with performance efficiency values ~0.87 (~0.82) averaged over the L‐shell range of 2.8–6.6, significantly outperforming the previous version of PreMevE particularly at L‐shells &gt; ~4.5. Interestingly, the linear regression model is often the most successful when compared to other models, which suggests the relationship between dynamics of trapped 1‐MeV electrons and precipitating electrons is dominated by linear components. Results also show that PreMevE 2.0 can reasonably well predict the onsets of MeV electron events in 2‐day forecasts. PreMevE 2.0 is designed to be driven by observations from longstanding space infrastructure to make high‐fidelity forecasts for MeV electrons, thus can be an invaluable space weather forecasting tool for the future.

Experimental and Numerical Study of Internal Charging on Spacecraft and Risks of Discharge on Floating Metallic Elements

Space system design rules and manufacturing processes may sometimes lead to the use of floating conductors in internal subsystems. This configuration promotes charge accumulation and increases the risk of electrostatic discharges (ESDs). This article presents an experimental and numerical study on this issue. We have selected and tested a Sub-D connector that is susceptible to internal charging because it may contain ungrounded conductors. We assessed its charging behavior and the risk of discharges induced by floating pins. For this purpose, the connector is tested in different configurations. It is irradiated using monoenergetic electron beams, carried out in the GEODUR irradiation facility installed at ONERA, Toulouse, France. Electric currents and potentials induced within the irradiated connector have been measured and correlated with simulation performed with the SPIS-IC code. Experiments confirmed that the connector’s charging behavior is directly influenced by the energy of the involved particles. The sample could present fast charging kinetics after exposure for a few hours at relatively low electron fluxes. ESDs, intense enough to damage sensitive electronic components, have also been observed. We have shown that the discharge risk is mainly related to the connector wiring.

Modifying Cytochrome c Maturation Can Increase the Bioelectronic Performance of Engineered Escherichia coli.

Genetic circuits that encode extracellular electron transfer (EET) pathways allow the intracellular state of Escherichia coli to be electronically monitored and controlled. However, relatively low electron flux flows through these pathways, limiting the degree of control by these circuits. Since the EET pathway is composed of multiple multiheme cytochromes c (cyts c) from Shewanella oneidensis MR-1, we hypothesized that lower expression levels of cyt c may explain this low EET flux and may be caused by the differences in the cyt c maturation (ccm) machinery between these two species. Here, we constructed random mutations within ccmH by error-prone PCR and screened for increased cyt c production. We identified two ccmH mutants, ccmH-132 and ccmH-195, that exhibited increased heterologous cyt c expression, but had different effects on EET. The ccmH-132 strain reduced WO3 nanoparticles faster than the parental control, whereas the ccmH-195 strain reduced more slowly. The same trend is reflected in electrical current generation: ccmH-132, which has only a single mutation from WT, drastically increased current production by 77%. The percentage of different cyt c proteins in these two mutants suggests that the stoichiometry of the S. oneidensis cyts c is a key determinant of current production by Mtr-expressing E. coli. Thus, we conclude that modulating cyt c maturation effectively improves genetic circuits governing EET in engineered biological systems, enabling better bioelectronic control of E. coli.

Considerations for imaging thick, low contrast, and beam sensitive samples with liquid cell transmission electron microscopy

Transmission electron microscopy of whole cells is hindered by the inherently large thickness and low atomic contrast intrinsic of cellular material. Liquid cell transmission electron microscopy allows samples to remain in their native hydrated state and may permit visualizing cellular dynamics in-situ. However, imaging biological cells with this approach remains challenging and identifying an optimal imaging regime using empirical data would help foster new advancements in the field. Recent questions about the role of the electron beam inducing morphological changes or damaging cellular structure and function necessitates further investigation of electron beam-cell interactions, but such comparisons are complicated by variability in imaging techniques used across various studies currently present in literature. The necessity for using low electron fluxes while imaging biological samples requires finding an imaging strategy which produces the strongest contrast and signal to noise ratio for the electron flux used. Here, we experimentally measure and evaluate signal to noise ratios and damage mechanisms between liquid and cryogenic samples of intact cells using multiple electron imaging modalities all on the same instrument and with equivalent beam parameters to standardize the comparison. We also discuss considerations for optimal electron microscopy imaging conditions for future studies on whole cells within liquid environments.

New low electron flux facility in the 0–3.5 MeV range for the study of induced signal in JUICE instruments: UVS and MAJIS measurements

We designed and built a new test facility to investigate signal induced by electrons in the 0–3.5 MeV in the JUICE UVS and MAJIS instruments. The facility uses radioisotopes sources to produce low flux of electrons (<6000 electrons/cm2.s). We present the facility, its capabilities and the results of measurements on UVS and MAJIS.

Direct Electron Beam Writing of Silver-Based Nanostructures

Direct writing utilizing a focused electron beam constitutes an interesting alternative to resist-based techniques, as it allows for precise and flexible growth onto any conductive substrate in a single-step process. One important challenge, however, is the identification of appropriate precursors which allow for deposition of the material of choice, e.g., for envisaged applications in nano-optics. In this regard the coinage metal silver is of particular interest since it shows a relatively high plasma frequency and, thus, excellent plasmonic properties in the visible range. By utilizing the precursor compound AgO2Me2Bu, direct writing of silver-based nanostructures via local electron beam induced deposition could be realized for the first time. Interestingly, the silver deposition was strongly dependent on electron dose; at low doses of 30 nC/μm2 a dominant formation of pure silver crystals was observed, while at higher electron doses around 104 nC/μm2 large carbon contents were measured. A scheme for the enhanced silver deposition under low electron fluxes by an electronic activation of precursor dissociation below thermal CVD temperature is proposed and validated using material characterization techniques. Finally, the knowledge gained was employed to fabricate well-defined two-dimensional deposits with maximized silver content approaching 75 at. %, which was achieved by proper adjustment of the deposition parameters. The corresponding deposits consist of plasmonically active silver crystallites and demonstrate a pronounced Raman signal enhancement of the carbonaceous matrix.

Dynamic responses of the Earth's radiation belts during periods of solar wind dynamic pressure pulse based on normalized superposed epoch analysis

AbstractUsing the electron flux measurements obtained from five satellites (GOES 15 and POES 15, 16, 18, and 19), we investigate the flux variations of radiation belt electrons during forty solar wind dynamic pressure pulses identified between September 2012 and December 2014. By utilizing the mean duration of the pressure pulses as the epoch timeline and stretching or compressing the time phases of individual events to normalize the duration by means of linear interpolation, we have performed normalized superposed epoch analysis to evaluate the dynamic responses of radiation belt energetic electrons corresponding to various groups of solar wind and magnetospheric conditions in association with solar wind dynamic pressure pulses. Our results indicate that by adopting the timeline normalization we can reproduce the typical response of the electron radiation belts to pressure pulses. Radiation belt electron fluxes exhibit large depletions right after the Pdyn peak during the periods of northward interplanetary magnetic field (IMF) Bz and are more likely to occur during the Pdyn pulse under southward IMF Bz conditions. For the pulse events with large negative values of (Dst)min, radiation belt electrons respond in a manner similar to those with southward IMF Bz, and the corresponding postpulse recovery can extend to L ~ 3 and exceed the prepulse flux levels. Triggered by the solar wind pressure enhancements, deeper earthward magnetopause erosion provides favorable conditions for the prompt electron flux dropouts that extend down to L ~ 5, and the pressure pulses with longer duration tend to produce quicker and stronger electron flux decay. In addition, the events with high electron fluxes before the Pdyn pulse tend to experience more severe electron flux dropouts during the course of the pulse, while the largest rate of electron flux increase before and after the pulse occurs under the preconditioned low electron fluxes. These new results help us understand how electron fluxes respond to solar wind dynamic pressure pulses and how these responses depend on the solar wind and geomagnetic conditions and on the preconditions in the electron radiation belts.

Particle Flux Effects on Physicochemical Polymer Degradations

Particle flux effects on polymer physicochemical degradations were investigated. Different polymers were studied depending on application: silicone, fluoropolymer, acrylic, epoxy, polyimide, polyurethane, etc. Polymers with surface functional properties (paint, coating, etc.) were dissociated from polymers with bulk properties (potting, cable, etc.). Surface materials were exposed to protons, and bulk materials were exposed to electron radiations. Two fluxes were used: and for electrons and and for protons. The total dose was fixed at 500 Mrad for electron radiations and 1 Grad for proton radiations. Functional properties (thermo-optical and mechanical) depending on material application were measured before and after irradiation exposure. Chemical structure modifications were also investigated. From all combined results, no global tendency was evidenced. The study shows that low or high irradiation flux induces more or less degradations according to polymer type, the composition of the polymer, and functional properties of concern. Flux effects can also depend on particle nature (electron or proton). The last point was highlighted by silicone polymer degradations; high proton flux caused more damage than low flux. On the contrary, low electron flux induced more degradations than high flux.

Investigation of phase separation in InGaN alloys by plasmon loss spectroscopy in a TEM

ABSTRACTPhase separation of InxGa1-xN alloys into Ga-rich and In-rich regions was observed by a number of research groups for samples grown with high indium content, x. Due to the radiation sensitivity of InGaN to beam damage by fast electrons, high-resolution imaging in transmission electron microscopy (TEM) or core-loss electron energy-loss spectroscopy (EELS) may lead to erroneous results. Low-loss EELS can yield spectra of the plasmon loss regions at much lower electron fluxes. Unfortunately, due to their delayed edge onset, the low energetic core losses of Ga and In partially overlap with the plasmon peaks, all of which shift with indium content.Here we demonstrate a method to quantify phase separation in InGaN thin films from the low-loss region in EELS by simultaneously fitting both plasmon and core losses over the energy range of 13-30eV. Phase separation is shown to lead to a broadening of the plasmon peak and the overlapping core losses, resulting in an unreliable determination of the indium concentration from analyzing the plasmon peak position alone if phase separation is present. For x=0.3 and x=0.59, the relative contributions of the binary compounds are negligibly small and indicate random alloys. For xnom.=0.62 we observed strong broadening, indicating phase separation.