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DOE OSTI2020

Materials Data on Cs(TeO3)2 by Materials Project

Cs(TeO3)2 crystallizes in the cubic Fd-3m space group. The structure is three-dimensional. Cs is bonded to six equivalent O atoms to form CsO6 octahedra that share corners with twelve equivalent TeO6 octahedra. The corner-sharing octahedral tilt angles are 69°. All Cs–O bond lengths are 3.24 Å. Te is bonded to six equivalent O atoms to form TeO6 octahedra that share corners with six equivalent CsO6 octahedra and corners with six equivalent TeO6 octahedra. The corner-sharing octahedra tilt angles range from 42–69°. All Te–O bond lengths are 2.00 Å. O is bonded in a 2-coordinate geometry to one Cs and two equivalent Te atoms.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Materials Data on Cs(AsIr)2 by Materials Project

Cs(IrAs)2 crystallizes in the tetragonal I4/mmm space group. The structure is three-dimensional. Cs is bonded in a body-centered cubic geometry to eight equivalent As atoms. All Cs–As bond lengths are 3.71 Å. Ir is bonded to four equivalent As atoms to form a mixture of distorted edge and corner-sharing IrAs4 tetrahedra. All Ir–As bond lengths are 2.47 Å. As is bonded in a 8-coordinate geometry to four equivalent Cs and four equivalent Ir atoms.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Materials Data on Cs(PIr)2 by Materials Project

Cs(IrP)2 crystallizes in the tetragonal I4/mmm space group. The structure is three-dimensional. Cs is bonded in a body-centered cubic geometry to eight equivalent P atoms. All Cs–P bond lengths are 3.67 Å. Ir is bonded to four equivalent P atoms to form a mixture of distorted corner and edge-sharing IrP4 tetrahedra. All Ir–P bond lengths are 2.36 Å. P is bonded in a 8-coordinate geometry to four equivalent Cs and four equivalent Ir atoms.

36 MATERIALS SCIENCE↗

DOE OSTI2025

U-Pu and Ba-Cs isotopic measurements on Trinitite by laser ablation sampling on the Neoma MC-ICP-MS

In this study we present the results of combined U-Pu and Ba-Cs isotope measurements obtained by laser ablation (LA) sampling of two glassy debris fragments (‘Trinitite’) from the world's first atomic bomb detonation conducted in New Mexico on July 16, 1945. Our primary goal in conducting these measurements was to understand whether examination of the U-Pu and Ba-Cs systematics by direct sampling (e.g. without any chemical separation or purification prior to isotope ratio measurement) could yield meaningful information that would differentiate the Trinitite fragments from glassy material lacking a nuclear fission signature. These measurements were conducted on a ThermoFisher Scientific Neoma multi collector – inductively coupled plasma – mass spectrometer (MC-ICP-MS), which is a relatively new MC-ICP-MS platform, so we also examine the behavior of these isotope systems in standards sampled in solution and via LA. Unsurprisingly, the measurements made on purified solutions of the U, Pu, and Ba isotopic standards produce high precision isotope ratios. Furthermore, this extends to the U-Pu measurements made by LA sampling, with the expected degradation in precision and accuracy related to matrix effects and signal intensity fluctuation. However, the Ba-Cs data acquired by LA is of low precision across all of the matrices examined and bears evidence of complex mass fractionation that will require further investigation to resolve. In total, our results indicate that the observed U-Pu isotope data are of sufficient quality to accurately constrain the U and Pu isotopic composition of glass containing sub-ppm levels of these elements which in turn could be used to differentiate glass containing anthropogenic fission products from natural glass whereas the Ba-Cs LA data cannot be used for this purpose until further methodological refinement is performed.

Ba-Cs↗

DOE OSTI2026

Uptake and Binding of At‐211 Into K‐ and Cs‐Derivatives of Alpha‐Zirconium Phosphate Nanoplatelets for Use as a Targeted Alpha Therapy Delivery Platform

The ion exchange behavior of K- and Cs-derivatives of α-zirconium phosphate, A-ZrP, with the targeted alpha therapy (TAT) radionuclide 211 At, as At + and AtO + , has been investigated. The K-ZrP shows strong affinity for both At+ and AtO + , ≥99% uptake. The affinity to Cs-ZrP was less pronounced, 87%–94% uptake, favoring At + . The binding strength was tested against several leaching solutions, including carbonate, phosphate buffered saline (PBS), 4-(2-hydroxyethyl)-1-piperazineethanesulfonic acid (HEPES) buffers, and ethylenediaminetetraacetic acid (EDTA) solutions at various concentrations (0.1–10 mM). K-ZrP retained 211 At in all buffer and EDTA solutions up to 1 mM (<0.5% leaching). The Cs-ZrP showed no leaching of At + , while AtO + leached (1%–3%) in the carbonate and HEPES buffers, along with all of the EDTA solutions, with complete retention only in the PBS buffer. In all cases, when the EDTA concentration reached 10 mM, 211 At leaching was observed. Once incorporated into the ZrP nanoplatelets, significant shielding of the α-particles was observed, not only attenuating the intensity of the emission but also reducing the energy of the α-particles themselves exiting the nanoplatelets. These properties provide the basis for K-ZrP, and to a lesser extent, Cs-ZrP to be further considered as potentially promising candidates for a delivery mechanism of 211 At for application in TAT.

astatine-211↗

DOE OSTI2021

Perovskite-Derived Cs 2 SnCl 6 –Silica Composites as Advanced Waste Forms for Chloride Salt Wastes

Advanced materials and processes are required to separate halides and fission products from complex salt waste streams associated with the chemical reprocessing of used nuclear fuels and molten salt reactor technologies for immobilization into chemically durable waste forms. Here, in this work, we explore an innovative concept using metal-halide perovskites as advanced host phases to incorporate Cs and Cl with very high waste loadings. Wet chemistry-synthesized Cs 2 SnCl 6 powders from CsCl salt solutions are successfully encapsulated into a silica matrix to form a composite using low-temperature spark plasma sintering with tunable Cs and Cl loadings up to 31 wt.% and 26 wt.%, respectively. Chemical durability testing of the composite waste forms by semi-dynamic leaching experiments demonstrates that incongruent leaching mechanism dominated. The metal-halide perovskite-silica composite waste forms display exceptional chemical durability with the long-term release rates of Cs and Cl comparable to or outperforming the state-of-the-art waste form materials but with significantly higher waste loadings. The scalable synthesis of the metal-halide perovskite from wet-chemistry processes opens up new opportunities in designing perovskite-glass composite waste forms for salt wastes with very high waste loadings and exceptional chemical durability for the sustainable development of advanced fuel cycles and next-generation reactor technologies.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2021

Lattice Dynamics and Optoelectronic Properties of Vacancy-Ordered Double Perovskite Cs 2 TeX 6 (X = Cl – , Br – , I – ) Single Crystals

The soft, dynamic lattice of inorganic lead halide perovskite CsPbX 3 (X = Cl ⁻ , Br ⁻ , I ⁻ ) leads to the emergence of many interesting photophysical and optoelectronic phenomena. However, probing their lattice dynamics with vibrational spectroscopy remains challenging. The influence of the fundamental octahedral building block in the perovskite lattice can be better resolved in zero-dimensional (0D) vacancy-ordered double perovskites of form A 2 BX 6 . Here we study Cs 2 TeX 6 (X = Cl ⁻ , Br ⁻ , I ⁻ ) single crystals to yield detailed insight into the fundamental octahedral building block and to explore the effect that its isolation in the crystal structure has on structural and electronic properties. The isolated [TeX 6 ] 2- octahedral units serve as the vibrational, absorbing, and emitting centers within the crystal. Serving as the vibrational centers, the isolated octahedra inform the likelihood of a random distribution of 10 octahedral symmetries within the mixed-halide spaces, as well as the presence of strong exciton-phonon coupling and anharmonic lattice dynamics. Serving as the absorbing and emitting centers, the isolated octahedra exhibit compositionally tunable absorption (1.50-3.15 eV) and emission (1.31-2.11 eV) energies. Due to greater molecular orbital overlap between neighboring octahedra with increasing halide anion size, there is a transition from a more molecule-like electronic structure in Cs 2 TeCl 6 and Cs 2 TeBr 6 -as expected from the effective 0D nature of these single crystals-to a dispersive electronic structure in Cs 2 TeI 6 , typical of three-dimensional (3D) bulk single crystals.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2026

Electron–Ion Covariance Reveals Geometry-Resolved Inner-Shell Spectra in CS 2 Photodissociation

The chemical shifts of inner-shell atomic orbitals are highly sensitive to chemical bonding and molecular structure. In evolving systems, however, the spectra of distinct molecular species and geometries overlap, obscuring the underlying chemical dynamics. Here we demonstrate the use of electron–ion covariance analysis to combine the structural sensitivity of Coulomb explosion imaging with inner-shell spectroscopy, yielding geometry-specific spectra of transient and product species. We apply this approach to the excited state dynamics of CS 2 probed by ionization above the S 2p edge. Electron–ion covariance with time- and momentum-selected S + and S 2+ ions isolates distinct S 2p photoelectron spectra for ground-state CS 2 , bent photoexcited CS 2 , the CS photoproduct, and bare atomic sulfur ─ species whose spectra overlap strongly in the channel-averaged measurement. Clear chemical shifts are observed in the covariance photoelectron spectrum for each of these species, all of which are consistent with high-level calculations. Here, by extracting the atomic S contribution to the photoelectron spectrum in a finely time-resolved manner we can disentangle this contribution to the overall time-resolved photoelectron spectrum as the photodissociation proceeds. These results demonstrate the promise of electron–ion covariance as a general approach to geometry-resolved inner-shell spectroscopy, opening a route to tracking structural evolution through chemical shifts in complex photoexcited molecules.

Ionization↗

DOE OSTI2024

Local A-Site Phase Segregation Leads to Cs-Rich Regions Showing Accelerated Photodegradation in Mixed-Cation Perovskite Semiconductor Films

We use hyperspectral photoluminescence microscopy to study compositional heterogeneity and its influence on the stability of mixed-cation (formamindinium (FA) and cesium) FA 1-x Cs x Pb(I 0.9 Br 0.1 ) 3 lead halide perovskites with different Cs contents. We observe substantial microscale heterogeneity in the photoluminescence. By correlating photoluminescence maps with time-of-flight secondary ion mass spectrometry (ToF-SIMS) imaging, we show that the redder-photoluminescence regions of the perovskite film are associated with Cs-rich compositions. X-ray diffraction measurement and confocal Raman spectroscopy provide evidence for the presence of d-phase CsPbI x Br 3-x in these regions. Photo-aging tests show that these Cs-rich clusters undergo faster photoluminescence decay than the rest of the film. These observations highlight the importance of local heterogeneities and their influence on the stability of halide perovskite semiconductors being studied for optoelectronics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Operation of Cs–Sb–O activated GaAs in a high voltage DC electron gun at high average current

Negative Electron Affinity (NEA) activated GaAs photocathodes are the most popular option for generating a high current (>1 mA) spin-polarized electron beam. Despite its popularity, a short operational lifetime is the main drawback of this material. Recent works have shown that the lifetime can be improved by using a robust Cs–Sb–O NEA layer with minimal adverse effects. In this work, we operate GaAs photocathodes with this new activation method in a high voltage environment to extract a high current. We demonstrate that improved chemical resistance of Cs–Sb–O activated GaAs photocathodes allowed them to survive a day-long transport process from a separate vacuum system using a vacuum suitcase. During beam running, we observed spectral dependence on lifetime improvement. In particular, we saw a 45% increase in the lifetime at 780 nm on average for Cs–Sb–O activated GaAs compared to Cs–O activated GaAs.

47 OTHER INSTRUMENTATION↗

DOE OSTI2024

Synthesis and structural characterization of a hydrated sodium–caesium tetracosatungstate(VI), Na 5 Cs 19 [W 24 O 84 ]·21H 2 O

Crystal formation of pentasodium nonadecacesium tetracosatungstate(VI) heneikosahydrate, Na 5 Cs 19 [W 24 O 84 ]·21H 2 O, was successfully achieved by the conversion of [H 2 W 12 O 42 ] 10– through the addition of excess Cs + . The crystal structure comprising the toroidal isopolyoxidometalate is presented, as well as its Raman spectrum. Na 5 Cs 19 (H 2 O) 21 W 24 O 84 crystallizes in the rhombohedral space group R$\overline{3}$ with an obverse centering. The title compound represents the addition of a new member to the isopolytungstate family with mixed alkali counter-ions and contains rarely observed five-coordinate tungsten(VI) atoms in the [W 24 O 84 ] 24– anion (site symmetry C 3i ) arising from the conversion mediated by Cs + counter-ions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Carbon Storage Planning Inquiry Tool (CS PlanIT)

The CS PlanIT provides stakeholders with easy access to geographically explore, query, and evaluate multiple data layers for a user-defined area of interest, with the goal to accelerate carbon storage resource, feasibility assessments, and planning efforts. The data within CS PlanIT are arranged and categorized to assess each stage of the Carbon Capture and Storage supply chain, from CO2 (Carbon Dioxide) emission sources, critical energy infrastructure (including transport), to CO2 geologic storage and sink locations. Furthermore, stakeholders can gain insights into community and environmental impacts, as CS PlanIT leverages Environmental Justice and Social Justice (EJSJ) and natural hazard datasets. Additionally, documentation in the form of an interactive ArcGIS story map and data catalog are included within the EDX publication to provide user’s information to better understand and explain CS PlanIT’s layout, functions, and associated data sets.

Justman, Devin M.↗

NASA NTRS1982

Production of CS and S in Comet Bradfield /1979 X/

High and low resolution ultraviolet spectra of carbon monosulfide (CS) in Comet Bradfield (1979 X) were obtained with the IUE satellite. The high resolution rotational profile of the (0, 0) band at 257.5 nm can be fitted with a theoretical profile derived assuming a Boltzmann temperature of 70 K. Spatial plots of the low resolution data for both S and CS show that these emissions are concentrated toward the cometary nucleus. The results that have been obtained are consistent with a Haser model for CS and S where the parent molecule is CS2. A very rapid variation of CS brightness with heliocentric distance is found.

Jackson, W. M.↗

NASA NTRS1985

Theoretical transition probabilities between the lowest 2S, 2P and 2D states of Na, K, Rb and Cs

Theoretical transition probabilities between the lowest 2S, 2P and 2D states of the alkali atoms Na through Cs have been computed using near Hartree-Fock quality Slater basis sets. The important core-valence correlation effects are incorporated explicitly by a configuration-interaction procedure. For Cs, the calculations were repeated using a Gaussian basis set so that relativistic effects could be incorporated through an effective core potential procedure. The best calculated electric quadrupole Einstein coefficients are Na(196.3/s), K(103.6/s), Rb(72.4/s) and Cs(19.7/s). Core-valence effects become increasingly important down the column, and reduce the quadrupole transition strengths to about the same degree as for the 2P-2S and 2D-2P dipole-allowed transitions. Relativistic effects increase the quadrupole moment of Cs, but less so than in Ba, presumably because the alkali 2D states are more diffuse.

Langhoff, S. R.↗

NASA NTRS1986

A CS J = 2 1 survey of the galactic center region

A CS map of the galactic center region is presented consisting of 15,000 spectra covering -1 deg. less than 3. deg. 6 min., -0 deg.4 min. less than b less than 0 deg. 4 min., each having an rms noise of 0.15 K in 1 MHz filters. CS is a high-excitation molecule, meaning that it is excited into emission only when the ambient density is less than n much greater than or approx. 2 x 10 to the 4th power/cu cm CS emission in the inner 2 deg. of the galaxy is nearly as pervasive as CO emission, in stark contrast to the outer galaxy where CS emission is confined to cloud cores. Galactic center clouds are on average much more dense than outer Galaxy clouds. This can be understood as a necessary consequence of the strong tidal stresses in the inner galaxy.

Stark, A. A.↗

NASA NTRS1990

CS in nearby galaxies: Distribution, kinematics, and multilevel studies

As a result of observations at the Institute for Radio Astronomy in the Millimeter Range (IRAM) 30-m telescope, maps of the distribution of the J = 2-1 transition of CS toward the galaxies IC 342 and NGC 253 are presented. The distribution of the CS emission from NGC 253 is consistent with the CO 1-0 line. The distribution of the CS emission from IC 342, however, resembles more that seen in the CO 3-2 line. For the first time, the detection of the isotopic substitution C-34S is reported toward an external galaxy: The C-34S 2-1 line has been detected toward NGC 253 and M 82 and the C-34S line has been detected tentatively toward M 82. Also for the first time, extragalactic CS has been observed in the 3-2 (toward NGC 253, IC 342 and M 82) and 5-4 (NGC 253 and IC 342) transitions.

Mauersberger, R.↗

NASA NTRS1992

Chemistry in circumstellar disks - CS toward HL Tauri

High spatial and spectral resolution dust continuum and CS line-emission maps of the material immediately surrounding HL Tauri are presented. The 3.06-thermal dust map gives an upper limit to the source size of roughly 200 AU. When combined with previous millimeter continuum measurements, a beta value of 1.2 +/-0.3 is derived along with a disk mass of 0.1 solar mass, in agreement with previous disk radiative transfer models of the IR and submillimeter flux from HL Tau. The low dust emissivity index as compared to particles in the diffuse ISM is best explained by grain growth or composition evolution. The present observations of the CS and CO emission lines forming the molecular cloud surrounding HL Tauri are consistent with the 'canonical' temperatures, densities, and abundances derived in other Taurus cloud cores. In contrast, the CS emission in aperture synthesis maps at 650-AU spatial resolution is most consistent with CS/CO ratios at least 25-50 times lower in the gas immediately surrounding HL Tauri if the CS emission is optically thin. The continuum and spectral line results obtained are strong indicators of conditions thought to be similar to those in the presolar nebula some 4.5 AE ago.

Blake, Geoffrey A.↗

NASA NTRS2010

Transport of Cs-137 from Boreal Biomass Burning in Summer of 2010

The summer of 2010 was a severe fire season in western Russia. Wildfires were detected in the Bryansk region, raising concerns that radionuclide contamination from the Chernobyl accident could be resuspended in the atmosphere. We simulate the transport of passive and particulate tracers of biomass burning from this region using the GEOS5 GOCART model driven by assimilated meteorology. Biomass burning emissions are based on MODIS fire detections. We validate the model against aerosol optical depth from MODIS. Using a range of estimates for Cs-137 emissions during wildfires, we estimate the downwind concentration and deposition of Cs-137 based on the emission ratios of Cs-137 to the simulated tracers. We discuss the sensitivity of our results to the location of the fires and the fraction of Cs-137 resuspended.

Strode, Sarah↗