Predicting short-range order and correlated phenomena in disordered crystalline materials
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99 GENERAL AND MISCELLANEOUS↗
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Results for “total scattering”
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Atomic-scale structure of ZrO 2 : Formation of metastable polymorphs
Metastable phases can exist within local minima in the potential energy landscape when they are kinetically “trapped” by various processing routes, such as thermal treatment, grain size reduction, chemical doping, interfacial stress, or irradiation. Despite the importance of metastable materials for many technological applications, little is known about the underlying structural mechanisms of the stabilization process and atomic-scale nature of the resulting defective metastable phase. Investigating ion-irradiated and nanocrystalline zirconia with neutron total scattering experiments, we show that metastable tetragonal ZrO 2 consists of an underlying structure of ferroelastic, orthorhombic nanoscale domains stabilized by a network of domain walls. The apparent long-range tetragonal structure that can be recovered to ambient conditions is only the configurational ensemble average of the underlying orthorhombic domains. This structural heterogeneity with a distinct short-range order is more broadly applicable to other nonequilibrium materials and provides insight into the synthesis and recovery of functional metastable phases with unique physical and chemical properties.
74 ATOMIC AND MOLECULAR PHYSICS↗
Ultrafast disordering of vanadium dimers in photoexcited VO 2
Many ultrafast solid phase transitions are treated as chemical reactions that transform the structures between two different unit cells along a reaction coordinate, but this neglects the role of disorder. Although ultrafast diffraction provides insights into atomic dynamics during such transformations, diffraction alone probes an averaged unit cell and is less sensitive to randomness in the transition pathway. Using total scattering of femtosecond x-ray pulses, we show that atomic disordering in photoexcited vanadium dioxide (VO 2 ) is central to the transition mechanism and that, after photoexcitation, the system explores a large volume of phase space on a time scale comparable to that of a single phonon oscillation. These results overturn the current understanding of an archetypal ultrafast phase transition and provide new microscopic insights into rapid evolution toward equilibrium in photoexcited matter.
36 MATERIALS SCIENCE↗
An iron evaluation story: from TALYS model parameters to validation on the ASPIS benchmark with the Monte-Carlo code TRIPOLI-4
Iron is a widespread structural material in nuclear applications. However some benchmark studies show that for many libraries, including TENDL-2019, producing good iron evaluations is still an open challenge. This work aims at improving TENDL-2019 {sup 56}Fe and {sup 54}Fe evaluations through feedbacks from experimental data and Monte Carlo results of the iron benchmark ASPIS. Part of the T6 code infrastructure was used to produce the evaluations. In the new evaluations, particular attention to resonance parameters and formalism was paid to address the importance of elastic scattering. The total inelastic scattering and inelastic continuum cross sections were shaped by modifying the input parameters of TALYS, one of the T6 codes. Additionally, it was necessary to normalise some reaction channels to those of JENDL-4.0. With the new files ASPIS results, obtained with the Monte Carlo code TRIPOLI-4, improved noticeably compared to TENDL 2019. The evaluations and parameter setting modifications are to be included into TENDL-2021. (authors)
73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
Time-dependent local and average structural evolution of δ-phase 239 Pu-Ga alloys
Here, plutonium metal is a very unusual element, exhibiting six allotropes at ambient pressure, between room temperature and its melting point, a complicated phase diagram, and a complex electronic structure. Many phases of plutonium metal are unstable with changes in temperature, pressure, chemical additions, or time. This strongly affects structure and properties, and becomes of high importance, particularly when considering effects on structural integrity over long periods of time [1]. This paper presents a time-dependent neutron total scattering study of the local and average structure of naturally aging δ-phase 239 Pu-Ga alloys, together with preliminary results on neutron tomography characterization.
36 MATERIALS SCIENCE↗
Report on Advanced Detector Development
Neutron, gamma and charged particle detection improvements are key to supporting many of the foreseen measurements and systems envisioned in the R&D programs and the future fuel cycle requirements, such as basic nuclear physics and data, modeling and simulation, reactor instrumentation, criticality safety, materials management and safeguards. This task will focus on the developmental needs of the FCR&D experimental programs, such as elastic/inelastic scattering, total cross sections and fission neutron spectra measurements, and will leverage a number of existing neutron detector development efforts and programs, such as those at LANL, PNNL, INL, and IAC as well as those at many universities, some of whom are funded under NE grants and contracts. Novel materials and fabrication processes combined with state-of-the-art electronics and computing provide new opportunities for revolutionary detector systems that will be able to meet the high precision needs of the program. This work will be closely coordinated with the Nuclear Data Crosscut. The Advanced Detector Development effort is a broadly-focused activity that supports the development of improved nuclear data measurements and improved detection of nuclear reactions and reactor conditions. This work supports the design and construction of large-scale, multiple component detectors to provide nuclear reaction data of unprecedented quality and precision. Examples include the Time Projection Chamber (TPC) and the DANCE detector at LANL. This work also supports the fabrication and end-user application of novel scintillator materials detection and monitoring.
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
Introduction to Pair Distribution Function Analysis
By collecting a total scattering pattern, subtracting the non-sample background, applying corrections, and taking the Fourier transform, the real space pair distribution function can be obtained. A PDF gives the distribution of inter-atomic distances in a material and is an excellent probe of short and intermediate range structure. RMC refinements using multiple data types are an excellent method for multi-scale modeling, including the mesoscale range.
36 MATERIALS SCIENCE↗
Negative Ion Formation in Complex Heavy Systems
The project’s primary objective is to gain a fundamental theoretical understanding of the near-threshold electron attachment mechanism in low energy electron elastic scattering from complex heavy systems through the calculation of integral and differential cross sections and extract reliable electron affinities (EAs). The complex angular momentum (CAM), also known as Regge-pole methodology wherein is fully embedded the crucial electron-electron correlations and the core polarization interaction, is used for the investigations. Regge trajectories allow us to probe electron attachment at the fundamental level near threshold, thereby uncovering new manifestations, including the mechanism of nanocatalysis, and determine reliable EAs. Low-energy electron elastic scattering total cross sections (TCSs) for the lanthanide and actinide atoms and the fullerene molecules are calculated. From the TCSs ground, metastable and excited states anionic binding energies (BEs) are extracted and compared with the available measured and/or calculated EAs. Significantly, our calculated ground state anionic BEs correspond to the theoretically challenging to calculate EAs and they are used to assess the reliability of existing EAs. Doubly charged negative ions of atoms and molecules are proposed as novel tunable catalysts and demonstrated in the oxidation of water into peroxide. Negatively charged fullerene molecules are used to catalyze water oxidation to peroxide and water synthesis from H 2 and O 2 as well. Violation of time-reversal and particle-hole symmetries in strongly correlated Fermi systems are reviewed with the collaboration involving the International Laboratory of Fermi Condensation.
74 ATOMIC AND MOLECULAR PHYSICS↗
Ab-initio molecular dynamics study of eutectic chloride salt: MgCl2–NaCl–KCl
Ionic liquid materials are viable candidates as a heat transfer fluid (HTF) in a wide range of applications, notably within concentrated solar power (CSP) technology and molten salt reactors (MSRs). For next-generation CSP and MSR technologies that strive for higher power generation efficiency, a HTF with wide liquid phase range and energy storage capabilities is crucial. Studies have shown that eutectic chloride salts exhibit thermal stability at high temperatures, high heat storage capacity, and are less expensive than nitrate and carbonate salts. However, the experimental data needed to fully evaluate the potential of eutectic chloride salts as a HTF contender are scarce and entail large uncertainties. Considering the high cost and potential hazards associated with the experimental methods used to determine the properties of ionic liquids, molecular modeling can be used as a viable alternative resource. In this study, the eutectic ternary chloride salt MgCl 2 –NaCl–KCl is modeled using ab-initio molecular dynamics simulations (AIMDs) in the liquid phase. Using the simulated data, the thermophysical and transport properties of eutectic chloride salt can be calculated: density, viscosity, heat capacity, diffusion coefficient, and ionic conductivity. For an initial model validation, experimental pair-distribution function data were obtained from X-ray total scattering techniques and compared to the theoretical pair-distribution function. Additionally, theoretical viscosity values are compared to experimental viscosity values for a similar system. The results provide a starting foundation for a MgCl 2 –NaCl–KCl model that can be extended to predict other fundamental properties.
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
Lattice Distortion and Phase Stability of Pd-Doped NiCoFeCr Solid-Solution Alloys
In the present study, we have revealed that (NiCoFeCr)100−xPdx (x= 1, 3, 5, 20 atom%) high-entropy alloys (HEAs) have both local- and long-range lattice distortions by utilizing X-ray total scattering, X-ray diffraction, and extended X-ray absorption fine structure methods. The local lattice distortion determined by the lattice constant difference between the local and average structures was found to be proportional to the Pd content. A small amount of Pd-doping (1 atom%) yields long-range lattice distortion, which is demonstrated by a larger (200) lattice plane spacing than the expected value from an average structure, however, the degree of long-range lattice distortion is not sensitive to the Pd concentration. The structural stability of these distorted HEAs under high-pressure was also examined. The experimental results indicate that doping with a small amount of Pd significantly enhances the stability of the fcc phase by increasing the fcc-to-hcp transformation pressure from ~13.0 GPa in NiCoFeCr to 20–26 GPa in the Pd-doped HEAs and NiCoFeCrPd maintains its fcc lattice up to 74 GPa, the maximum pressure that the current experiments have reached.
36 MATERIALS SCIENCE↗
Fullerene Negative Ions: Formation and Catalysis
We first explore negative-ion formation in fullerenes C 44 to C 136 through low-energy electron elastic scattering total cross sections calculations using our Regge-pole methodology. Then, the formed negative ions C 44 – to C 136 – are used to investigate the catalysis of water oxidation to peroxide and water synthesis from H 2 and O 2 . The exploited fundamental mechanism underlying negative-ion catalysis involves hydrogen bond strength-weakening/breaking in the transition state. Density Functional Theory transition state calculations found C 60 – optimal for both water and peroxide synthesis, C 100 – increases the energy barrier the most, and C 136 – the most effective catalyst in both water synthesis and oxidation to H 2 O 2 .
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Surfactant-free syntheses and pair distribution function analysis of osmium nanoparticles
A surfactant-free synthesis of precious metal nanoparticles (NPs) performed in alkaline low-boiling-point solvents has been recently reported. Monoalcohols are here investigated as solvents and reducing agents to obtain colloidal Os nanoparticles by using low-temperature (<100 °C) surfactant-free syntheses. The effect of the precursor (OsCl 3 or H 2 OsCl 6 ), precursor concentration (up to 100 mM), solvent (methanol or ethanol), presence or absence of a base (NaOH), and addition of water (0 to 100 vol %) on the resulting nanomaterials is discussed. It is found that no base is required to obtain Os nanoparticles as opposed to the case of Pt or Ir NPs. The robustness of the synthesis for a precursor concentration up to 100 mM allows for the performance of X-ray total scattering with pair distribution function (PDF) analysis, which shows that 1–2 nm hexagonal close packed (hcp) NPs are formed from chain-like [OsO x Cl y ] complexes.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
A Comet Active Beyond the Crystallization Zone
We present observations showing inbound long-period comet C/2017 K2 (PANSTARRS) to be active at a record heliocentric distance. Nucleus temperatures are too low (60–70 K) either for water ice to sublimate or for amorphous ice to crystallize, requiring another source for the observed activity. Using the Hubble Space Telescope we find a sharply bounded, circularly symmetric dust coma 10{sup 5} km in radius, with a total scattering cross-section of ∼10{sup 5} km{sup 2}. The coma has a logarithmic surface brightness gradient −1 over much of its surface, indicating sustained, steady-state dust production. A lack of clear evidence for the action of solar radiation pressure suggests that the dust particles are large, with a mean size ≳0.1 mm. Using a coma convolution model, we find a limit to the apparent magnitude of the nucleus V>25.2 (absolute magnitude H>12.9). With assumed geometric albedo p {sub V} = 0.04, the limit to the nucleus circular equivalent radius is <9 km. Prediscovery observations from 2013 show that the comet was also active at 23.7 au heliocentric distance. While neither water ice sublimation nor exothermic crystallization can account for the observed distant activity, the measured properties are consistent with activity driven by sublimating supervolatile ices such as CO{sub 2}, CO, O{sub 2}, and N{sub 2}. Survival of supervolatiles at the nucleus surface is likely a result of the comet’s recent arrival from the frigid Oort Cloud.
79 ASTRONOMY AND ASTROPHYSICS↗
On the Crystal Structure of Colloidally Prepared Metastable Ag2Se Nanocrystals
Structural polymorphism is known for many bulk materials; however, on the nanoscale metastable polymorphs tend to form more readily than in the bulk, and with more structural variety. One such metastable polymorph observed for colloidal Ag2Se nanocrystals has traditionally been referred to as the “tetragonal” phase of Ag2Se. While there are reports on the chemistry and properties of this metastable polymorph, its crystal structure, and therefore electronic structure, has yet to be determined. We report that an anti-PbCl2-like structure type (space group P21/n) accurately describes the powder X-ray diffraction and X-ray total scattering patterns of colloidal Ag2Se nanocrystals prepared by several different methods. Density functional theory (DFT) calculations indicate that the anti-PbCl2-like Ag2Se polymorph is a dynamically stable, narrow-band gap semiconductor. DFT results reveal a dense theoretical Ag2Se phase space with many low-energy polymorphs, which helps explain the large number of polymorphs reported in the literature. Analysis and calculation data are stored in the zip archive. The `ag2se-calcs.aiida.` contains the provenance of the calculations and can be imported into an AiiDA database instance. The antiPbCl2like_Ag2Se_laboratory.cif file is the Reitveld refined Ag2Se structure starting from the PbCl2 structure.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
aosnephwet (c1)
The nephelometer measures the total scattering and hemispheric backscattering of aerosol. Nephelometers are deployed in pairs, with one measuring the ambient conditions and the other measuring the scattering as a function of slowly increasing or decreasing relative humidity (RH). The combination can then be used to derive the hygroscopic growth factor as a function of RH: f(RH). The nephelometer is part of the aerosol observing system (AOS).
54 ENVIRONMENTAL SCIENCES↗
aosnephdry (c1)
The nephelometer measures the total scattering and hemispheric backscattering of aerosol. Nephelometers are deployed in pairs, with one measuring the ambient conditions and the other measuring the scattering as a function of slowly increasing or decreasing relative humidity (RH). The combination can then be used to derive the hygroscopic growth factor as a function of RH: f(RH). The nephelometer is part of the aerosol observing system (AOS).
54 ENVIRONMENTAL SCIENCES↗
Pressure Induced Topological Quantum Phase Transition in Weyl Semimetal T d -MoTe 2
In this paper, we report the temperature and pressure (p max ≃1.5 GPa) evolution of the crystal structure of the Weyl semimetal T d -MoTe 2 by combination of neutron diffraction and the X-ray total scattering experiments. We find that the fundamental non-centrosymmetric structure T d is fully suppressed and transforms into a centrosymmertic 1T' structure at a critical pressure of p cr ~ 1.2–1.4 GPa. This is strong evidence for a pressure induced quantum phase transition (QPT) between topological to a trivial electronic state. Although the topological QPT has strong effect on magnetoresistance, it is interesting that the superconducting (SC) critical temperature T c , the superfluid density, and the SC gap all change smoothly and continuously across p cr and no sudden effects are seen concomitantly with the suppression of the T d structure. This implies that the T c , and thus the SC pairing strength, is unaffected by the topological QPT. However, the QPT requires the change in the SC gap symmetry from non-trivial s +- to a trivial s ++ state, which we discuss in this work. Our systematic characterizations of the structure and SC properties associated with the topological QPT provide deep insight into the pressure induced phase diagram in this topological quantum material.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Cesium-cesium cross section and the lennard- jones parameters.
Cesium-cesium total scattering cross section computed by Lennard-Jones parameter for cesium vapor transport properties
SCATTERING CROSS SECTION↗