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At least 1,423 records · Page 79

Three-dimensional reconstruction of laser-direct-drive inertial confinement fusion hot-spot plasma from x-ray diagnostics on the OMEGA laser facility (invited)

A deep-learning convolutional neural network (CNN) is used to infer, from x-ray images along multiple lines of sight, the low-mode shape of the hot-spot emission of deuterium–tritium (DT) laser-direct-drive cryogenic implosions on OMEGA. The motivation of this approach is to develop a physics-informed 3-D reconstruction technique that can be performed within minutes to facilitate the use of the results to inform changes to the initial target and laser conditions for the subsequent implosion. The CNN is trained on a 3D radiation-hydrodynamic simulation database to relate 2D x-ray images to 3D emissivity at stagnation. The CNN accounts for the lack of an absolute spatial reference and the different bands of photon energies in the x-ray images. While previous works studied the effect of mode-1 asymmetries on implosion performance using nuclear diagnostics, this work focuses on the effect of mode 2 inferred from x-ray diagnostics on implosion performance. A current analysis of 19 DT cryogenic implosions indicates there is an upper limit of ~20% reduction in the neutron yield caused by an ℓ = 2 amplitude for ℓ 2 /ℓ 0 ≤ 0.32. Here, these conclusions are supported by 2D simulations.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

APS: High-Energy X-rays Expediting Applied and Fundamental Research

The Advanced Photon Source (APS) at Argonne National Laboratory (ANL) was designed and built as one of the first large 3rd generation synchrotrons operated at 7 GeV. The United States Department of Energy (DOE) Office of Science funded the construction and continues to fund the operation of this national facility. Furthermore, the beamlines were originally operated by Collaborative Access Teams (CAT), which allowed a strong involvement of research institutes, universities, and industry. Today 43 of 68 beamlines are operated by the X-ray Science Division (XSD) and 35 beamlines are directly funded by the DOE Office of Science. The APS became operational in 1995, and was planned right from the beginning with 4 beamlines dedicated to high-energy x-rays above 40 keV: 1-ID designed to study engineering materials science, 6-ID-D for magnetism and condensed matter research, 11-ID-B dedicated to magnetic Compton scattering using an Elliptical Multipole Wiggler, and 11-ID-C for materials science and condensed matter physics. These stations were later joined by the bending magnet beamlines 6-BM for white beam studies and 17-BM for rapid powder diffraction. CAT operated beamlines such as 15-ID for crystallography or 16-ID for high-pressure studies also use the high-energy x-ray regime frequently. The program in Compton scattering ended in 2004 and the wiggler was replaced by an undulator. 11-ID-B became the first dedicated station for Pair Distribution Function (PDF) Analysis.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Dust from early galaxies and the X-ray background radiation

The effects of the scattering of cosmic X-ray background photons by dusty foreground galaxies are explored, assuming the X-rays themselves arise in discrete sources. The effective angle of scattering is about 1-10 arcmin in the 1-3 keV band, which can lead to a decrease in the spatial fluctuations of the background observed with an IPC-like imaging device with about 1 arcmin resolution. This can reduce the number of discrete sources required to explain the smoothness of the background to values greater than about 1000/sq deg. The effect may be stronger in the direction of distant clusters of galaxies, or if distant galaxies are much dustier than assumed here.

Rudak, B.↗

Sensitivity of nulling interferometers to extra-solar zodiacal emission (EZE)

It should be possible to discover and to analyze the atmospheres of Earth-like planets of nearby stars, provided their thermal emission is not overwhelmed by a bright zodiacal cloud in the same system. Nulling interferometers in space, such as the Terrestrial Planet Finder, can efficiently suppress a stellar point source, but there is no way to suppress diffuse emission underlying the planet under study. A cloud much brighter than solar level would cause serious reduction in sensitivity, by its photon shot noise. Since some clouds have been detected that are orders of magnitude brighter, zodiacal measurements of TPF candidates to solar level are critically needed. These could be obtained relatively soon with the largest aperture ground-based interferometers observing in the 10 micron atmospheric window. A cloud would be detectable as an infrared excess, provided the stellar emission (some 10(exp 4) times brighter) is adequately suppressed by destructive interference. Ideally, the ground interferometer should have angular response similar to that of TPF, so as to measure directly the troublesome zodiacal component. The individual elements must be large, for even with approx. 8 m apertures, star cancellation and low thermal background, integration times of at least several hours will be needed to sense the clouds against shot noise from telescope thermal emission. In this paper we compare the sensitivity of TPF and ground based interferometers to a twin of the solar system at 10 pc, using Good's (1994) model of the zodiacal cloud.

Angel, Roger↗

Apparatus and method for creating a photonic densely-accumulated ray-point

An optical apparatus includes an optical diffraction device configured for diffracting a predetermined wavelength of incident light onto adjacent optical focal points, and a photon detector for detecting a spectral characteristic of the predetermined wavelength. One of the optical focal points is a constructive interference point and the other optical focal point is a destructive interference point. The diffraction device, which may be a micro-zone plate (MZP) of micro-ring gratings or an optical lens, generates a constructive ray point using phase-contrasting of the destructive interference point. The ray point is located between adjacent optical focal points. A method of generating a densely-accumulated ray point includes directing incident light onto the optical diffraction device, diffracting the selected wavelength onto the constructive interference focal point and the destructive interference focal point, and generating the densely-accumulated ray point in a narrow region.

Park, Yeonjoon↗

Optimizing Science Return from Plato's Observations of the Kepler Field

The Plato mission could substantially enhance its scientific yield by focusing a significant fraction of its observations with all 24 cameras viewing the Kepler Field of View (FOV). Kepler, while exceptionally productive, did not accomplish its goal of providing a direct measurement of the abundance of Earth-analog planet around sunlike stars. On this issue, Plato observations centered on the Kepler FOV would enable planet searches using the combined data sets to achieve more precise estimates of planetary occurrence rates than obtainable using data from either mission alone. The ecliptic latitude of the Kepler FOV is too low for Plato to observe with 24 cameras year-round, so current plan’s for Plato’s Northern Stare places the Kepler FOV in the periphery, reducing the number of photons collected from Kepler targets by factors of 2 or 4. We propose instead four ~6 - 8 month Plato stares with 24 cameras observing the Kepler FOV during the Plato primary mission, instead of a single 2 year stare with the Kepler FOV located to the periphery. This change would greatly increase the amount of 'Plato glass’ dedicated to the continued study of the Kepler FOV, while still enabling Plato to observe other parts of the sky during the majority of its prime mission. In addition to discovering planets below Kepler's detection threshold, this change would yield transit follow-up of thousands of known exoplanets with an effective throughput of a 0.6 m space telescope. It would also extend the observing baseline of the Kepler FOV to timescales of decades, providing key data for stellar cycles, the analysis of transit timing variations, and other decade-timescale variations. Such a campaign enhances the likelihood of the detection of true Earth-analog transiting planet candidates around sunlike stars, provide the best statistical study of exoplanet systems with transit timing variations and duration variations, and open up the study of stellar variability to new time-domains with precision on large numbers of faint targets that only 24 Plato cameras can provide.

Jack Lissauer↗

Grassland productivity responds unexpectedly to dynamic light and soil water environments induced by photovoltaic arrays

Abstract Agrivoltaic (AV) systems are designed to coproduce photovoltaic (PV) energy on lands simultaneously supporting agriculture (food/forage production). PV infrastructure in agroecosystems alters resources critical for plant growth, and water‐limited agroecosystems such as grasslands are likely to be particularly sensitive to the unique spatial and temporal patterns of incident sunlight and soil water inherent within AV systems. However, the impact of resource alteration on forage production, the primary ecosystem service from managed grasslands, is poorly resolved. Here, we evaluated seasonal patterns of soil moisture (SM) and diurnal variation in incident sunlight (photosynthetic photon flux density [PPFD]) in a single‐axis‐tracking AV system established in a formerly managed semiarid C 3 grassland in Colorado. Our goals were to (1) quantify dynamic patterns of PPFD and SM within a 1.2 MW PV array in a perennial grassland, and (2) determine how aboveground net primary production (ANPP) and photosynthetic parameters responded to the resource patterns created by the PV array. We hypothesized that spatial variability in ANPP would be strongly related to SM patterns, typical of most grasslands. We measured significant reductions in ANPP directly beneath PV panels, where SM and PPFD were both low. However, in locations with significantly increased SM from the shedding and redistribution of precipitation by PV panels, ANPP was not increased. Instead, ANPP was greatest in locations where plants were shaded in the afternoon but received high levels of PPFD in the morning hours, when air temperatures and vapor pressure deficits were relatively low. Thus, contrary to expectations, we found relatively weak relationships between SM and ANPP despite significant spatial variability in both. Further, there was little evidence that light‐saturated photosynthesis ( A sat ) and quantum yield of CO 2 assimilation (ϕCO 2 ) differed for plants growing directly beneath (lowest PPFD) versus between (highest PPFD) PV panels. Overall, the AV system established in this semiarid managed grassland did not alter patterns of ANPP in ways predictable from past studies of controls of ANPP in open grasslands. However, our results suggest that the diurnal timing of low versus high periods of PPFD incident on plants is an important determinant of productivity patterns in grasslands.

14 SOLAR ENERGY↗

AI-NERD: Elucidation of relaxation dynamics beyond equilibrium through AI-informed X-ray photon correlation spectroscopy

Abstract Understanding and interpreting dynamics of functional materials in situ is a grand challenge in physics and materials science due to the difficulty of experimentally probing materials at varied length and time scales. X-ray photon correlation spectroscopy (XPCS) is uniquely well-suited for characterizing materials dynamics over wide-ranging time scales. However, spatial and temporal heterogeneity in material behavior can make interpretation of experimental XPCS data difficult. In this work, we have developed an unsupervised deep learning (DL) framework for automated classification of relaxation dynamics from experimental data without requiring any prior physical knowledge of the system. We demonstrate how this method can be used to accelerate exploration of large datasets to identify samples of interest, and we apply this approach to directly correlate microscopic dynamics with macroscopic properties of a model system. Importantly, this DL framework is material and process agnostic, marking a concrete step towards autonomous materials discovery.

36 MATERIALS SCIENCE↗

Coupled Charge and Radiation Transport Processes in Thermophotovoltaic and Thermoradiative Cells

Accurate modeling of charge transport and both thermal and luminescent radiation is crucial to the understanding and design of radiative thermal energy converters. Charge-carrier dynamics in semiconductors are well-described by the Poisson-drift-diffusion equations, and thermal radiation in emitter-absorber structures can be computed using multilayer fluctuational electrodynamics. These two types of energy flows interact through radiation absorption or luminescence and charge-carrier generation or recombination. However, past research has typically only assumed limited interaction, with thermal radiation absorption as an input for charge-carrier models to predict device performance. To examine this assumption, we develop a fully coupled iterative model of charge and radiation transport in semiconductor devices, and we use our model to analyze near-field and far-field GaSb thermophotovoltaic and thermoradiative systems. By comparing our results with past methods that do not consider cross-influences between charge and radiation transport, we find that a fully coupled approach is necessary to accurately model photon recycling and near-field enhancement of external luminescence. As these effects can substantially alter device performance, our modeling approach can aid in the design of efficient thermophotovoltaic and thermoradiative systems.

30 DIRECT ENERGY CONVERSION↗

Scintillation of liquid nitrogen

Liquid nitrogen is commonly used in cryogenic applications and is a promising medium for the direct immersion cooling of sensors used for nuclear and particle physics experiments. The scintillation properties of gaseous nitrogen are well-documented, but little is known about the scintillation of liquid nitrogen. If present, scintillation light from interactions of ambient radioactivity could produce backgrounds for rare event searches such as the direct detection of dark matter. Using a coincidence-tagged alpha decay, we demonstrate that liquid nitrogen exhibits measurable, albeit very faint, scintillation. Assuming the same scintillation wavelengths as gaseous nitrogen, we estimate a relative scintillation yield of $Y_{\liquidn}/Y^{\STP}_{\gasn} =$ \num[uncertainty-descriptors={stat,sys}]{0.0142(0.0005)(0.0030)} with respect to gaseous nitrogen at standard temperature and pressure. Considering the average scintillation yield from alpha decays in gaseous nitrogen, this implies a scintillation yield for alpha decays in liquid nitrogen of $Y_{\liquidn} = \qty[]{2.39(0.56)}{photons~per~MeV}$. To our knowledge this is the first measurement of scintillation in liquid nitrogen.

Pagani, Luca (ORCID:0000000234692581)↗

Testing the Solar Probe Cup, An Instrument Designed to Touch The Sun

Abstract: Solar Probe Plus will be the first, fastest, and closest mission to the Sun, providing the first direct sampling of the sub-Alfvénic corona. The Solar Probe Cup (SPC) is a unique re-imagining of the traditional Faraday Cup design and materials for immersion in this high temperature environment. Sending an instrument of this type into a never-seen particle environment requires extensive characterization prior to launch to establish sufficient measurement accuracy and instrument response. To reach this end, a slew of tests are created for allowing SPC to see ranges of appropriate ions and electrons, as well as a facility that reproduces solar photon spectra and fluxes for this mission. Having already tested the SPC at flight-like temperatures with no significant modification of the noise floor, we recently completed a round of particle testing to see if the deviations in Faraday Cup design fundamentally change the operation of the instrument. Results and implications from these tests will be presented, as well as performance comparisons to cousin instruments such as those on the WIND spacecraft.

solar physics↗

Airborne Measurements of CO2 Column Concentration and Range Using a Pulsed Direct-Detection IPDA Lidar

We have previously demonstrated a pulsed direct detection IPDA lidar to measure range and the column concentration of atmospheric CO2. The lidar measures the atmospheric backscatter profiles and samples the shape of the 1,572.33 nm CO2 absorption line. We participated in the ASCENDS science flights on the NASA DC-8 aircraft during August 2011 and report here lidar measurements made on four flights over a variety of surface and cloud conditions near the US. These included over a stratus cloud deck over the Pacific Ocean, to a dry lake bed surrounded by mountains in Nevada, to a desert area with a coal-fired power plant, and from the Rocky Mountains to Iowa, with segments with both cumulus and cirrus clouds. Most flights were to altitudes >12 km and had 5-6 altitude steps. Analyses show the retrievals of lidar range, CO2 column absorption, and CO2 mixing ratio worked well when measuring over topography with rapidly changing height and reflectivity, through thin clouds, between cumulus clouds, and to stratus cloud tops. The retrievals shows the decrease in column CO2 due to growing vegetation when flying over Iowa cropland as well as a sudden increase in CO2 concentration near a coal-fired power plant. For regions where the CO2 concentration was relatively constant, the measured CO2 absorption lineshape (averaged for 50 s) matched the predicted shapes to better than 1% RMS error. For 10 s averaging, the scatter in the retrievals was typically 2-3 ppm and was limited by the received signal photon count. Retrievals were made using atmospheric parameters from both an atmospheric model and from in situ temperature and pressure from the aircraft. The retrievals had no free parameters and did not use empirical adjustments, and >70% of the measurements passed screening and were used in analysis. The differences between the lidar-measured retrievals and in situ measured average CO2 column concentrations were <1.4 ppm for flight measurement altitudes >6 km.

Lidar↗

Reprocessing Microflare Data

The report concerns work on detecting and cataloging solar microflares using an automated. An accompanying figure represents the solar microflare distribution during the period of April 1991 to November 1992, the height of solar activity after the launch of CGRO. It also shows the distribution extending below the distribution obtained at GSFC by manual means. We have implemented significant refinements in the search algorithm. The algorithm in its simplest form searches for transient events and based upon the distribution of the signal among the different BATSE detectors, we can assign it to be of solar origin if the signal distribution conforms to what one expects from a burst or transient from that direction. One of the major problems in an earlier effort was to search for microflares and large flares simultaneously. The requirement for a dynamic range of almost 10(exp 4) resulted in ambiguous identifications at the low side of the distribution. We have since restricted the search to events with peak count rates under 2000/s. Larger events are easily identified in the manual search, so we have chosen not to duplicate that work. The second problem was that missing counts existed below channel 0 in the BATSE Large Area Detector (LAD) data. These have been recovered and are now included in the search process. This provides data below 20 keV, and as we get closer to the thermal part of the spectrum, it provides greater sensitivity. The third problem was that too many BATSE detectors were used in the search. Detectors with pointing directions far from the Sun, although detecting the event, had poorly known responses. Detectors greater than approximately 60 degrees off the Sun are no longer included in the search process. By reducing the systematic errors with the large off-axis detectors we can conduct more rigorous statistical tests of a candidate event to ascertain whether it originated from the solar direction. We have reprocessed the period in the early mission that covers solar maximum and constructed the microflare distribution shown in the figure. The results of the automated search start to deviate from the manual search results below about 1000/s. Not only do we now have this distribution but we have a database of solar microflares that was used to construct the distribution. This database contains the signal at higher energy channels as well as that in channel zero (and below). From this one can, using software at GSFC, construct a photon spectrum for some of the larger microflares. It can also be used in other solar studies, especially those that correlate the X-ray flux with emission at other wavelengths. With some additional effort we hope to integrate this database into the corresponding one residing at the Solar Data Analysis Center at GSFC. The entire CGRO mission's data can now be reprocessed to obtain the microflare distribution at all phases of the solar cycle. This work is in progress. The results of this work will be presented in forthcoming scientific workshops and conferences.

Ryan, James M.↗

Rossi X-Ray Timing Explorer Observations of the Gamma-Ray Blazar PKS 2155-304

PKS 2155-304 is the archetypical X-ray-selected BL Lac object (XBL). It is one of the brightest BL Lacs at x-ray through optical wavelengths where it has a relatively featureless continuum and displays rapid, large amplitude variability. This continuum is thought to be direct synchrotron emission from a distribution of ultra-relativistic electrons which extends to unusually high energies (Edelson et al. 1995). The gamma-ray emission from PKS 2155-304 constitutes a second, separate, spectral component. Observations with the EGRET telescope aboard the Compton Gamma Ray Observatory (CGRO) show that the spectral energy distribution of this gamma-ray component must peak at energies above 10 GeV (Vestrand et al. 1995). This, plus the realization that the extension of the synchrotron component into the x-ray band meant that ambient photons would be scattered to TeV energies, led to predictions that PKS 2155-304 would be a detectable TeV gamma ray source (Vestrand et al. 1995; Stecker et al. 1996). The University of Durham group has recently reported the discovery of TeV gamma ray emission from PKS 2155-304 (Chadwick et al. 1998, 1999) . The TeV emission was detected in 1996 September and 1997 October/November, with the largest fluxes being measured in 1997 November. During 1997 November, we detected a record high GeV gamma-ray flux from PKS 2155-304 with CGRO/EGRET (Sreekumar and Vestrand 1997) and subsequently very high x-ray fluxes were measured with BeppoSAX (Chiapeeti et al. 1997). Here we report on the record x-ray fluxes measured with the Rossi X-Ray Timing Explorer (RXTE) during the GeV/TeV outburst.

Vestrand, W. Thomas↗

Two-Photon Fluorescence Microscope for Microgravity Research

A two-photon fluorescence microscope has been developed for the study of biophysical phenomena. Two-photon microscopy is a novel form of laser-based scanning microscopy that enables three-dimensional imaging without many of the problems inherent in confocal microscopy. Unlike one-photon optical microscopy, two-photon microscopy utilizes the simultaneous nonlinear absorption of two near-infrared photons. However, the efficiency of two-photon absorption is much lower than that of one-photon absorption, so an ultra-fast pulsed laser source is typically employed. On the other hand, the critical energy threshold for two-photon absorption leads to fluorophore excitation that is intrinsically localized to the focal volume. Consequently, two-photon microscopy enables optical sectioning and confocal performance without the need for a signal-limiting pinhole. In addition, there is a reduction (relative to one-photon optical microscopy) in photon-induced damage because of the longer excitation wavelength. This reduction is especially advantageous for in vivo studies. Relative to confocal microscopy, there is also a reduction in background fluorescence, and, because of a reduction in Rayleigh scattering, there is a 4 increase of penetration depth. The prohibitive cost of a commercial two-photon fluorescence-microscope system, as well as a need for modularity, has led to the construction of a custom-built system (see Figure 1). This system includes a coherent mode-locked titanium: sapphire laser emitting 120-fs-duration pulses at a repetition rate of 80 MHz. The pulsed laser has an average output power of 800 mW and a wavelength tuning range of 700 to 980 nm, enabling the excitation of a variety of targeted fluorophores. The output from the laser is attenuated, spatially filtered, and then directed into a confocal scanning head that has been modified to provide for side entry of the laser beam. The laser output coupler has been replaced with a dichroic filter that reflects the longer-wavelength excitation light and passes the shorter-wavelength fluorescence light. Also, the confocal pinhole has been removed to increase the signal strength. The laser beam is scanned by a twoperpendicular- axis pair of galvanometer mirrors through a pupil transfer lens into the side port of an inverted microscope. Finally, the beam is focused by a 63-magnification, 1.3-numerical- aperture oil-immersion objective lens onto a specimen. The pupil transfer lens serves to match the intermediate image planes of the scanning head and the microscope, and its location is critical. In order to maximize the quality of the image, (that is, the point spread function of the objective lens for all scan positions), the entire system was modeled in optical-design software, and the various free design parameters (the parameters of the spatial-filter components as well as the separations of all of the system components) were determined through an iterative optimization process. A modular design was chosen to facilitate access to the optical train for future fluorescence correlation spectroscopy and fluorescence-lifetime experiments.

Fischer, David G.↗

Development of Position-Sensitive Magnetic Calorimeters for X-Ray Astronomy

Metallic magnetic calorimeters (MMC) are one of the most promising devices to provide very high energy resolution needed for future astronomical x-ray spectroscopy. MMC detectors can be built to large detector arrays having thousands of pixels. Position-sensitive magnetic (PoSM) microcalorimeters consist of multiple absorbers thermally coupled to one magnetic micro calorimeter. Each absorber element has a different thermal coupling to the MMC, resulting in a distribution of different pulse shapes and enabling position discrimination between the absorber elements. PoSMs therefore achieve the large focal plane area with fewer number of readout channels without compromising spatial sampling. Excellent performance of PoSMs was achieved by optimizing the designs of key parameters such as the thermal conductance among the absorbers, magnetic sensor, and heat sink, as well as the absorber heat capacities. Micro fab ri - cation techniques were developed to construct four-absorber PoSMs, in which each absorber consists of a two-layer composite of bismuth and gold. The energy resolution (FWHM full width at half maximum) was measured to be better than 5 eV at 6 keV x-rays for all four absorbers. Position determination was demonstrated with pulse-shape discrimination, as well as with pulse rise time. X-ray microcalorimeters are usually designed to thermalize as quickly as possible to avoid degradation in energy resolution from position dependence to the pulse shapes. Each pixel consists of an absorber and a temperature sensor, both decoupled from the cold bath through a weak thermal link. Each pixel requires a separate readout channel; for instance, with a SQUID (superconducting quantum interference device). For future astronomy missions where thousands to millions of resolution elements are required, having an individual SQUID readout channel for each pixel becomes difficult. One route to attaining these goals is a position-sensitive detector in which a large continuous or pixilated array of x-ray absorbers shares fewer numbers of temperature sensors. A means of discriminating the signals from different absorber positions, however, needs to be built into the device for each sensor. The design concept for the device is such that the shape of the temperature pulse with time depends on the location of the absorber. This inherent position sensitivity of the signal is then analyzed to determine the location of the event precisely, effectively yielding one device with many sub-pixels. With such devices, the total number of electronic channels required to read out a given number of pixels is significantly reduced. PoSMs were developed that consist of four discrete absorbers connected to a single magnetic sensor. The design concept can be extended to more than four absorbers per sensor. The thermal conductance between the sensor and each absorber is different by design and consequently, the pulse shapes are different depending upon which absorber the xrays are received, allowing position discrimination. A magnetic sensor was used in which a paramagnetic Au:Er temperature-sensitive material is located in a weak magnetic field. Deposition of energy from an x-ray photon causes an increase in temperature, which leads to a change of magnetization of the paramagnetic sensor, which is subsequently read out using a low noise dc-SQUID. The PoSM microcalorimeters are fully microfabricated: the Au:Er sensor is located above the meander, with a thin insulation gap in between. For this position-sensitive device, four electroplated absorbers are thermally linked to the sensor via heat links of different thermal conductance. One pixel is identical to that of a single-pixel design, consisting of an overhanging absorber fabricated directly on top of the sensor. It is therefore very strongly thermally coupled to it. The three other absorbers are supported directly on a silicon-nitride membrane. These absorbers are thermally coupled to the sensor via Ti (5 nm)/Au250 nm) metal links. The strength of the links is parameterized by the number of gold squares making up the link. For detector performance, experimentally different pulse-shapes were demonstrated with 6 keV x-rays, which clearly show different rise times for different absorber positions. For energy resolution measurement, the PoSM was operated at 32 mK with an applied field that was generated using a persistent current of 50 mA. Over the four pixels, energy resolution ranges from 4.4 to 4.7 eV were demonstrated.

Bandler, SImon↗

Forming Perchlorates on Mars Through Plasma Chemistry During Dust Events

We report experimental evidences to support a new formation mechanism, multiphase redox plasma chemistry, for perchlorate on Mars observed during the Phoenix mission, whose high concentrations and high ClO4/Cl ratio cannot be fully interpreted by photochemistry. This chemical reaction occurs between Cl-bearing minerals on the Mars surface and free radicals generated by electrostatic discharge (ESD) during Mars dust events (dust storms, dust devils, and grain saltation). We conducted simulated ESD experiments in a Mars chamber with pure CO2, CO2+H2O(g), and Mars Simulate Gas Mixture at Martian atmospheric pressure. We directly observed (1) the instantaneous generation of atmospheric free radicals CO2+, CO+, OI, HIII, HII, OH, ArI, N2, and N2+in normal glow discharge (NGD), detected by in situ plasma emission spectroscopy, and O3by UV and Mid-IR spectroscopy; (2) the fast transformation of NaCl to NaClO3and NaClO4detected by laser Raman spectroscopy, with oxychlorine enrichment at the sample surfaces confirmed by ion chromatography. Through two sets of experimental comparison, we found that the oxidation power of ESD-electron is three orders of magnitude higher than that of UVC-photon. We scaled our experimental results to the modeled ESD in Mars dust events and Mars surface UV radiation level, and concluded that plasma chemistry occurred during Mars dust events can be an additional important formation mechanism for the large amounts of perchlorates observed during various missions to Mars.

Wu, Zhongchen↗

Integrating computation and experiment to investigate photoelectrodes for solar water splitting at the microscopic scale.

CONSPECTUS: Photoelectrochemical water-splitting is a promising and sustainable way to store the energy of the sun in chemical bonds and use it to produce hydrogen gas, a clean fuel. The key components in photoelectrochemical cells (PECs) are photoelectrodes, including a photocathode that reduces water to hydrogen gas and a photoanode that oxidizes water to oxygen gas. Materials used in photoelectrodes for PECs must effectively absorb sunlight, yield photogenerated carriers, and exhibit electronic properties that enable the efficient shuttling of carriers to the surface to participate in relevant water-splitting reactions. Discovering and understanding the key characteristics of optimal photoelectrode materials is paramount to the realization of PEC technologies. Oxide-based photoelectrodes can satisfy many of these materials requirements, including stability in aqueous environments, band edges with reasonable alignment with the redox potentials for water splitting, and ease of synthesis. However, oxide photoelectrodes generally suffer from poor charge transport properties and considerable bulk electron-hole separation, and they have relatively large band gaps. Numerous strategies have been proposed to improve these aspects and understand how these improvements are reflected in the photoelectrochemical performance. Unfortunately, the structural and compositional complexity of multinary oxides accompanied by the inherent complexity of photoelectrochemical processes makes it challenging to understand the individual effects of composition, structure, and defects in the bulk and on the surface on a material's photoelectrochemical properties. The integration of experiment and theory has great potential to increase our atomic-level understanding of structure-composition-property relationships in oxide photoelectrodes. In this Account, we describe how integrating experiment and theory is beneficial for achieving scientific insights at the microscopic scale. We highlight studies focused on understanding the role of (i) bulk composition via solid-state solutions, intercalation, and comparison with isoelectronic compounds, (ii) dopants for both the anion and cation and their interactions with oxygen vacancies, and (iii) surface/interface structure in the photocurrent generation and photoelectrochemical performance in oxide photoelectrodes. In each instance, we outline strategies and considerations for integrating experiment and theory and describe how this integration led to valuable insights and new directions in uncovering structure-composition-property relationships. Our aim is to demonstrate the unique value of combining experiment and theory in studying photoelectrodes and to encourage the continued effort to bring experiment and theory in closer step with each other.

Wang, Wennie↗