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At least 1,081 records · Page 60

Assessment of Low-Level Pu Isotope Ratio Measurements Using Multicollector Inductively Coupled Plasma Mass Spectrometry (MC-ICP-MS/MS) Equipped with a Pre-Mass Filter

We present an initial investigation into the performance of a multicollector inductively coupled plasmamass spectrometer equipped with a pre-mass filter (Neoma MC-ICP-MS/MS) for making plutonium (Pu) isotope ratio measurements on solutions containing low level (i.e., pg mL –1 ) Pu concentrations. This assessment was achieved by comparison of the 240 Pu/ 239 Pu, 241 Pu/ 239 Pu, and 242 Pu/ 239 Pu ratios attained over a one month period on the MC-ICP-MS/MS with the long-term (∼1 year) performance observed on the predecessor MC-ICP-MS (Neptune Plus) instrument each equipped with an equipped with an APEXΩ desolvating nebulizer for repeated measurements of certified reference materials from New Brunswick Program Office (NBL PO) CRM 136a and CRM 137. The MC-ICP-MS/MS performance of repeated measurement of CRM 136a (n = 20) resulted in mean values of 240 Pu/ 239 Pu = 0.1448 ± 0.0006, 241 Pu/ 239 Pu = 0.00371 ± 0.00006, and 242 Pu/ 239 Pu = 0.00682 ± 0.00006 (k = 2). The CRM 137 (n = 20), analyzed during the same analytical sessions, produced mean values for 240 Pu/ 239 Pu = 0.2414 ± 0.0006, 241 Pu/ 239 Pu = 0.00464 ± 0.00007, and 242 Pu/ 239 Pu = 0.0157 ± 0.0001 (k = 2). These results closely align with the certificate values for CRM 136a and CRM 137 and are within the k = 2 envelopes defined by the long-term performance of the traditional MC-ICP-MS approach (Neptune Plus). Examination of the performance of the various Pu isotope ratios as a function of total Pu content revealed accurate results (<3% relative difference, or RD) above ∼50 fg total Pu. The results presented here demonstrate the capability of the MC-ICP-MS/MS making accurate and precise low level Pu isotopic measurements. While the intent of this work was not to investigate the functionality of the collision cell, the pre-mass filter was employed. Future studies are warranted to investigate the entire capability of the MC-ICP-MS/MS collision cell and pre-cell mass filter optimization for performing low level Pu isotope measurements, even in mixed matrix samples.

CRM↗

Depth-resolved sagebrush root metabolomics, rhizosphere microbial communities, and geochemistry at the East River Watershed

This data set consists of results from soil nutrient profile, untargeted metabolomics, mass spec imaging, and amplicon sequencing. Data for soil nutrient profile includes common cations (Ca, Mg, Na, and K etc.) extracted from 3 digesting steps – ammonia acetate (for exchangeable cations), nitric acid (for acid dissolved fraction), and hydrofluoric acid/perchloric acid (HF/HClO4) for whole soil digestion. It also includes concentration of organic carbon, inorganic nitrogen (ammonia and nitrate) and phosphorus (Bray-1 P and nitric acid extract), and total nitrogen and phosphorus. Data for untargeted metabolomics includes metabolomic profile for root exudate/tissues and soil extracts from depths at surface soil to saprolite, that were measured using gas chromatography – mass spectrometry (GC-MS), and liquid chromatography – tandem mass spectrometry (LC-MS/MS). Data for mass spec imaging includes spatial distribution of metabolites that were detected and annotated with Fourier transformation ion cyclotron resonance mass spectrometer (FTICR-MS). Data for amplicon sequencing includes the base paired 16S and ITS ribosomal RNA sequences from Miseq Illumina sequencing. All samples were collected from 2 sampling campaign October 2022 and June 2023. Collectively, these datasets enable a mechanistic evaluation of how nutrient acquisition, especially nitrogen and phosphorus, differs between shallow roots operating in soil and deep roots functioning within the fractured bedrock zone. All files are provided as comma-separated values (CSV) fies (.csv) and (GZIP) file (.gz). The compressed .gz FASTQ files can be read directly in R using the dada2 package as part of the amplicon sequence analysis workflow. This work was supported by the Watershed Function Science Focus Area at Lawrence Berkeley National Laboratory funded by the US Department of Energy, Office of Science, Biological and Environmental Research under Contract No. DE-AC02-05CH11231. This research was performed on a project award 60563 (https://dx.doi.org/10.46936/expl.proj.2022.60563/60008727) from the Environmental Molecular Sciences Laboratory, a DOE Office of Science User Facility sponsored by the Biological and Environmental Research program under Contract No. DE-AC05-76RL01830.

EARTH SCIENCE > AGRICULTURE > SOILS > CARBON↗

Understanding the Role of Hydroxyl Functionalization in Linear Poly(Ethylenimine) for Oxidation‐Resistant Direct Air Capture of CO 2

Aminopolymer-based adsorbents are a prominent class of materials being used for direct air capture of CO 2 at the industrial scale. However, improving their working lifetime, specifically by increasing their resilience to oxidative degradation, remains an ongoing challenge. Toward this end, functionalization of aminopolymers with non-amine functionalities such as hydroxyls has emerged in recent years as a promising strategy toward improving adsorbent lifetime. Although there is a growing body of work demonstrating the effectiveness of this approach and investigating the origin of this improved stability, studies to date have primarily focused on branched aminopolymer systems such as branched poly(ethylenimine). In this work, hydroxyl-functionalized linear poly(ethylenimine) is used to continue to probe the underlying protective mechanism of this strategy. A combination of thermogravimetric analysis, NMR relaxometry, differential scanning calorimetry, and computational simulations is used to better understand the relationship between the extent of chemical functionalization, physical properties, and adsorbent performance.

amine-based adsorbent↗

Cardiac myosin activation with 2-deoxy-ATP via increased electrostatic interactions with actin

The naturally occurring nucleotide 2-deoxy-adenosine 5'-triphosphate (dATP) can be used by cardiac muscle as an alternative energy substrate for myosin chemomechanical activity. We and others have previously shown that dATP increases contractile force in normal hearts and models of depressed systolic function, but the structural basis of these effects has remained unresolved. In this work, we combine multiple techniques to provide structural and functional information at the angstrom-nanometer and millisecond time scales, demonstrating the ability to make both structural measurements and quantitative kinetic estimates of weak actin–myosin interactions that underpin sarcomere dynamics. Exploiting dATP as a molecular probe, we assess how small changes in myosin structure translate to electrostatic-based changes in sarcomere function to augment contractility in cardiac muscle. Through Brownian dynamics simulation and computational structural analysis, we found that deoxy-hydrolysis products [2-deoxy-adenosine 5&prime;-diphosphate (dADP) and inorganic phosphate (Pi)] bound to prepowerstroke myosin induce an allosteric restructuring of the actin-binding surface on myosin to increase the rate of cross-bridge formation. We then show experimentally that this predicted effect translates into increased electrostatic interactions between actin and cardiac myosin in vitro. Finally, using small-angle X-ray diffraction analysis of sarcomere structure, we demonstrate that the proposed increased electrostatic affinity of myosin for actin causes a disruption of the resting conformation of myosin motors, resulting in their repositioning toward the thin filament before activation. The dATP-mediated structural alterations in myosin reported here may provide insight into an improved criterion for the design or selection of small molecules to be developed as therapeutic agents to treat systolic dysfunction.

59 BASIC BIOLOGICAL SCIENCES↗

Domain Wall Patterning and Giant Response Functions in Ferrimagnetic Spinels

Abstract The manipulation of mesoscale domain wall phenomena has emerged as a powerful strategy for designing ferroelectric responses in functional devices, but its full potential is not yet realized in the field of magnetism. This work shows a direct connection between magnetic response functions in mechanically strained samples of Mn 3 O 4 and MnV 2 O 4 and stripe‐like patternings of the bulk magnetization which appear below known magnetostructural transitions. Building off previous magnetic force microscopy data, a small‐angle neutron scattering is used to show that these patterns represent distinctive magnetic phenomena which extend throughout the bulk of two separate materials, and further are controllable via applied magnetic field and mechanical stress. These results are unambiguously connected to the anomalously large magnetoelastic and magnetodielectric response functions reported for these materials, by performing susceptibility measurements on the same crystals and directly correlating local and macroscopic data.

36 MATERIALS SCIENCE↗

Structures reveal opening of the store-operated calcium channel Orai

The store-operated calcium (Ca2+) channel Orai governs Ca2+ influx through the plasma membrane of many non-excitable cells in metazoans. The channel opens in response to the depletion of Ca2+ stored in the endoplasmic reticulum (ER). Loss- and gain-of-function mutants of Orai cause disease. Our previous work revealed the structure of Orai with a closed pore. Here, using a gain-of-function mutation that constitutively activates the channel, we present an X-ray structure of Drosophila melanogaster Orai in an open conformation. Well-defined electron density maps reveal that the pore is dramatically dilated on its cytosolic side in comparison to the slender closed pore. Cations and anions bind in different regions of the open pore, informing mechanisms for ion permeation and Ca2+ selectivity. Opening of the pore requires the release of cytosolic latches. Together with additional X-ray structures of an unlatched-but-closed conformation, we propose a sequence for store-operated activation.

Hou, Xiaowei↗

Smart Meters Enabling Voltage Monitoring and Control Functionalities: The Last-Mile Voltage Stability Issue

It is a demanding yet challenging task to design the next generation of smart meters. This work investigates the new voltage monitoring and control function for the next-generation smart meters, and identifies its added values for power system voltage stability issues. In terms of voltage monitoring, the risk benefit analysis for adding voltage magnitudes to smart meter measurements is presented, and the risk mitigation strategies along with the co-simulation validation via GridLAB-D and NS-3 are proposed, all providing insight into the new function evaluation. In terms of voltage control, a new voltage stability control scheme is developed, which uses voltage measurements from smart meters and utilizes the observability and controllability of distributed energy resources and controllable loads. Different from traditional voltage control schemes focusing on voltage regulation and power quality monitoring from the utility perspective, the proposed control scheme can achieve the maximum real power transfer margin at the end user side, enabling the voltage stability issues being solved at the grid edge, i.e. the last-mile segment. It is the first work that considers voltage monitoring and control collectively for smart meter investment. It can help power engineering community supplement smart meter applications and shape the next-generation smart meters.

42 ENGINEERING↗

Charge transport in nanostructured materials: Implementation and verification of constrained density functional theory

The in silico design of novel complex materials for energy conversion requires accurate, ab initio simulation of charge transport. In this work, we present an implementation of constrained density functional theory (CDFT) for the calculation of parameters for charge transport in the hopping regime. We verify our implementation against literature results for molecular systems, and we discuss the dependence of results on numerical parameters and the choice of localization potentials. In addition, we compare CDFT results with those of other commonly used methods for simulating charge transport between nanoscale building blocks. As a result, we show that some of these methods give unphysical results for thermally disordered configurations, while CDFT proves to be a viable and robust approach.

36 MATERIALS SCIENCE↗

The 3D printing and modeling of functionally graded Kelvin foams for controlling crushing performance

Mechanical impact protection is an important consideration in many applications, ranging from product transportation to sports. Cellular materials are typically used due to their desirable energy absorption properties and light weight. However, their large deformation and rate dependent responses (especially of polymer foams) are challenging to consider in design. Additionally, the use of foams with uniform properties, such as uniform density and uniform stiffness, often restricts the designed foams to only be suitable for a narrow range of mechanical impact conditions whereas real applications commonly face unpredictable situations. 3D printing offers fabrication flexibility and thus opens the door to create foams with tailored properties. In this work, we investigate the feasibility of using 3D printing for functionally graded foams (FGFs) that are optimal over a broad range of mechanical environments. The foams are fabricated by the recently developed grayscale digital light processing (g-DLP) method which can print parts with locally designed properties. These foams are tested under drop test conditions and with slower displacement control. We also model the large deformation behavior of FGFs using finite element analysis in which we account for the different viscoelastic behaviors of the distinct grayscale regions. We then use the model to examine the impact mitigation capabilities of FGFs in different loading scenarios. Finally, we show how FGFs can be used to satisfy real-world design goals using the case study of a motorcycle helmet. In contrast to prior work, we investigate continuous, functionally graded foams of a single density that differ in their viscoelastic responses. This work provides further insight into the benefits of viscoelastic properties and modulus graded foams and presents a manufacturing approach that can be used to produce the next generation of flexible lattice foams as mechanical absorbers.

3D printing↗

Attaining regularization length insensitivity in phase-field models of ductile failure

In this work, a cohesive phase-field model of ductile fracture in a finite-deformation setting is presented. The model is based on a free-energy function in which both elastic and plastic work contributions are coupled to damage. Using a strictly variational framework, the field evolution equations, damage kinetics, and flow rule are jointly derived from a scalar least-action principle. Particular emphasis is placed on the use of a rational function for the stress degradation that maintains a fixed effective strength with decreasing regularization length. The model is employed to examine crack growth in pure mode-I problems through the generation of crack growth resistance (J-R) curves. In contrast to alternative models, the current formulation gives rise to J-R curves that are insensitive to the regularization length. Numerical evidence suggests convergence of local fields with respect to diminishing regularization length as well.

42 ENGINEERING↗

Electron Transfer Theory Elucidates the Hidden Role Played by Triethylamine and Triethanolamine during Photocatalysis

Triethylamine (TEA) and triethanolamine (TEOA) are renowned, in part, for their ability to reductively quench excited states by outer-sphere electron transfer with vast and still growing applications as sacrificial electron donors for photocatalytic systems. Upon amine oxidation, the resulting TEA •+ and TEOA •+ radical cations undergo proton transfer (or hydrogen atom transfer), resulting in the formation of a chemical reductant that has an α-carbon centered radical adjacent to the nitrogen center (TEA • and TEOA • ). In this contribution, we have electrochemically and spectroscopically characterized a set of electron acceptors which, upon accepting an electron, are a series of photocatalysts, [ReCl(R 1 R 2 -bpy)(CO) 3 ] •– , where R 1 and R 2 are electron-donating and electron-withdrawing groups in the 4,4′- and 5,5′-positions on the bipyridyl ligand. Here, we substantiated the formation of the electron donors, TE(O)A • , by spin trapping electron paramagnetic resonance spectroscopy, where TE(O)A • reacts with 2,4,6-tri-tert-butylnitrosobenzene to generate N-centered and O-centered radical adducts. Having established the chemical behaviors of the electron acceptors and donors individually, the electron transfer rate constants were determined across a 1.43 V range in driving force. The redox potential of TEA • was benchmarked to within ±80 mV on an absolute scale in V vs Fc + /Fc in CH 3 CN by using an empirical rate vs free-energy correlation, electron transfer theory, and density functional theory calculations. The equilibrium potentials for TEA • and TEOA • were determined to be −1.98 V and −1.76 V, respectively. Based on the kinetic and thermochemical analysis presented for TEA • and TEOA • , these transient radicals can be broadly considered strong homogeneous chemical reductants within the wider context of photoredox potentials. Thus, this work clarifies a frequently unnoticed secondary function for these sacrificial electron donors during photocatalysis and rationalizes the possibility of a one-photon/two-electron conversion process that is dependent on the free-energy exchange between TE(O)A • and photocatalysts.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Calibration of energy density functionals with deformed nuclei

Nuclear density functional theory is the prevalent theoretical framework for accurately describing nuclear properties at the scale of the entire chart of nuclides. Given an energy functional and a many-body scheme (e.g., single- or multireference level), the predictive power of the theory depends strongly on how the parameters of the energy functionals have been calibrated with experimental data. Expanded algorithms and computing power have enabled recent optimization protocols to include data in deformed nuclei in order to optimize the coupling constants of the energy functional. The primary motivation of this work is to test the robustness of such protocols with respect to some of the technical and numerical details of the underlying calculations, especially when the calibration explores a large parameter space. To this end, we quantify the effect of these uncertainties on both the optimization and statistical emulation of composite objective functions. We also emphasize that Bayesian calibration can provide better estimates of the theoretical errors used to define objective functions.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Nuclear Computational Low Energy Initiative (NUCLEI)

This is the Final Report for Ohio State University for the NUCLEI SciDAC­3 project. In addition to the local OSU summary given here, we have attached a global NUCLEI summary and a list of papers and talks by the full collaboration, with OSU contributions marked in red. The NUCLEI project, as defined by the scope of work, developed, implemented and ran codes for large­scale computations of many topics in low­energy nuclear physics. Physics studied included the properties of nuclei and nuclear decays, nuclear structure and reactions, and the properties of nuclear matter. The computational techniques used included Quantum Monte Carlo, Configuration Interaction, Coupled Cluster, In­Medium SRG, and Density Functional methods. The research program emphasized areas of high interest to current and possible future DOE nuclear physics facilities, including ATLAS and FRIB (nuclear structure and reactions, and nuclear astrophysics), TJNAF (neutron distributions in nuclei, few body systems, and electroweak processes), NIF (thermonuclear reactions), MAJORANA and FNPB (neutrinoless double­beta decay and physics beyond the Standard Model), and LANSCE (fission studies). Research at Ohio State University played an integral role in NUCLEI by providing input microscopic interactions and operators needed for ab initio structure and reaction calculations including uncertainty quantification, independent ab initio calculations using the in­medium similarity renormalization group (IM­SRG), and developing microscopic constraints for the next­generation energy density functionals (EDF). Much of the theoretical work at OSU was closely coordinated with the theory team at Michigan State University. Although the OSU group did not usually directly develop codes for the highest performance computing components of NUCLEI, we provided needed inputs for much of the effort. In particular, our work contributes to the “Validated Nuclear Interactions” task as well as to both of the “Structure and Reactions” tasks.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Trigonometric continuous-variable gates and hybrid quantum simulations of the sine-Gordon model

Hybrid qubit-qumode quantum computing platforms provide a natural setting for simulating interacting bosonic quantum field theories. However, existing continuous-variable gate constructions rely predominantly on polynomial functions of canonical quadratures. In this work, we introduce a complementary universality paradigm based on trigonometric continuous-variable gates, which enable a Fourier-like representation of bosonic operators and are particularly well suited for periodic and non-perturbative interactions. We present an ancilla-based framework for implementing trigonometric gates with arguments given by arbitrary Hermitian functions of qumode quadratures. The protocol yields unitary gates deterministically, and non-unitary gates through probabilistic post-selection. As a concrete application, we develop a hybrid qubit-qumode quantum simulation of the lattice sine-Gordon model. Using these gates, we prepare ground states via quantum imaginary-time evolution, simulate real-time dynamics, compute time-dependent vertex two-point correlation functions, and extract quantum kink profiles under topological boundary conditions. Our results demonstrate that trigonometric continuous-variable gates provide a physically natural framework for simulating interacting field theories on near-term hybrid quantum hardware, while establishing a parallel route to universality beyond polynomial gate constructions. We expect that the trigonometric gates introduced here to find broader applications, including quantum simulations of condensed matter systems, quantum chemistry, and biological models.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

A bi-functional ferroelectric Pb(Zr0.52Ti0.48)O3 films: Energy storage properties and ferroelectric photovoltaic effects

Highlights: • PZT films by sol-gel method exhibited a higher energy densities (∼11.2 J/cm{sup 3}) and energy conversion efficiency (∼68%). • Pt/PZT/Pt devices showed the higher open circuit voltage (V{sub oc} ∼1 V), larger short circuit current (J{sub sc} ∼0.1 mA/cm{sup 2}). • Pt/PZT/Pt devices might improve the properties of energy storage and photovoltage in ferroelectric films. - Abstract: In this work, we reported a bi-functional ferroelectric Pb(Zr{sub 0.52}Ti{sub 0.48})O{sub 3} (PZT) films which show energy storage properties and photovoltaic effects. The PZT films were crystallized into pure pseudo-cubic structure with the (001) preferred orientation. The polarization characterizations revealed a large recoverable energy storage density (∼11.2 J/cm{sup 3}) and a high energy conversion efficiency (∼68%) with good thermal stability (25 °C–100 °C) and fast response (>10 Hz). Meanwhile, the Pt/PZT/Pt capacitor presented a significant photovoltaic effect. The open circuit voltage and the short circuit current were -0.92 V and 139 μA/cm{sup 2} at original state, respectively, while they were slightly increased to -1.01 V and 155 μA/cm{sup 2} in polarization-up state, and slightly decreased to -0.77 V and 90 μA/cm{sup 2} in polarization-down state. The maximum power conversion efficiency was enhanced one order of magnitude than that of polycrystalline PZT film reported elsewhere. Our study opens up a pathway toward developing bi-functional ferroelectric devices with simultaneously high energy storage density and high photovoltaic performance.

14 SOLAR ENERGY↗

The 2.4 μ m Galaxy Luminosity Function as Measured Using WISE . III. Measurement Results

The Widefield Infrared Survey Explorer (WISE) satellite surveyed the entire sky multiple times in four infrared wavelengths (3.4, 4.6, 12, and 22 μm). The unprecedented combination of coverage area and depth gives us the opportunity to measure the luminosity function (LF) of galaxies, one of the fundamental quantities in the study of them, at 2.4 μm to an unparalleled level of formal statistical accuracy in the near-infrared. The big advantage of measuring LFs at wavelengths in the window of ≈2–3.5 μm is that it correlates more closely to the total stellar mass in galaxies than others. In this paper we report on the parameters of the 2.4 μm LF of galaxies obtained from applying the spectro-luminosity-functional-based methods to datasets from the previous papers in this series using the mean and covariance of 2.4 μm normalized spectral energy distributions (SEDs) from our previous work. In terms of the single Schechter function parameters evaluated at the present epoch, the combined result is: ${\phi }_{\star }=5.8\,\pm [{0.3}_{\mathrm{stat}},{0.4}_{\mathrm{sys}}]\times {10}^{-3}\,{\mathrm{Mpc}}^{-3}$, ${L}_{\star }=6.4\pm [{0.1}_{\mathrm{stat}},{0.3}_{\mathrm{sys}}]\times {10}^{10}\,{L}_{2.4\mu {\rm{m}}\odot }$ (M$_{\star}$ = -21.67 ± [0.02 stat , 0.05 sys ] AB mag), and $α$ = -1.050 ± [0.004 stat , 0.04 sys ]. The high statistical accuracy comes from combining public redshift surveys with the wide coverage from WISE, and the unevenness in statistical accuracy is a result of our efforts to work around biases of uncertain origin that affect resolved and marginally resolved galaxies. With further refinements, the techniques applied in this work promise to advance the study of the SED of the universe.

79 ASTRONOMY AND ASTROPHYSICS↗

Addressing Function Allocation for the Digital Transformation of Existing Nuclear Power Plants

The existing nuclear power plants in the United States (U.S.) have a vital role in providing carbon-free electricity. For the existing nuclear power plant fleet to remain economically viable, a significant digital transformation that fundamentally changes the way in which these plants are operated, maintained, and supported ought to be seriously considered. Safe and reliable automation is needed. This work describes important considerations and challenges that come with function allocation for the adoption of new automation at existing nuclear power plants. Specifically, this work reviews the state-of-the-art in function allocation guidance and highlights how it can be used within the U.S. nuclear industry. An objective of this work is to present the current challenges and proposed approaches to the human factors community to support future research and development that ultimately supports the effective use of function allocation in the digital transformation of existing nuclear power plants.

99 GENERAL AND MISCELLANEOUS↗

pwv_kpno: A Python Package for Modeling the Atmospheric Transmission Function Due to Precipitable Water Vapor

In this work, we present a Python package, pwv_kpno, which provides models for the atmospheric transmission due to precipitable water vapor (PWV) at user-specified sites. Using the package, ground-based photometric observations taken between 3000 and 12,000 Å can be corrected for atmospheric effects due to PWV. Atmospheric transmission in the optical and near-infrared is highly dependent on the PWV column density along the line of sight. By measuring the delay of dual-band GPS signals through the atmosphere, the SuomiNet project provides accurate PWV measurements for hundreds of locations around the world. The pwv_kpno package uses published SuomiNet data in conjunction with MODTRAN models to determine the modeled, time-dependent atmospheric transmission. A dual-band GPS system was installed at Kitt Peak National Observatory (KPNO) in the spring of 2015. Using measurements from this receiver we demonstrate that we can successfully predict the PWV at KPNO from nearby dual-band GPS stations on the surrounding desert floor. The pwv_kpno package can thus provide atmospheric transmission functions for observations taken before the KPNO receiver was installed. Using PWV measurements from the desert floor, we correctly model PWV absorption features present in spectra taken at KPNO. Finally, we also demonstrate how to configure the package for use at other observatories.

79 ASTRONOMY AND ASTROPHYSICS↗