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At least 829 records · Page 46

Efficient First-Principles Methodology for the Calculation of the All-Phonon Inelastic Scattering in Solids

Inelastic scattering experiments are key methods for mapping the full dispersion of fundamental excitations of solids in the ground as well as nonequilibrium states. A quantitative analysis of inelastic scattering in terms of phonon excitations requires identifying the role of multiphonon processes. Here, we develop an efficient first-principles methodology for calculating the all-phonon quantum mechanical structure factor of solids. We demonstrate our method by obtaining excellent agreement between measurements and calculations of the diffuse scattering patterns of black phosphorus, showing that multiphonon processes play a substantial role. The present approach constitutes a step towards the interpretation of static and time-resolved electron, x-ray, and neutron inelastic scattering data.

36 MATERIALS SCIENCE↗

Scattering off molecules far from equilibrium

We report that pump-probe gas phase X-ray scattering experiments, enabled by the development of X-ray free electron lasers, have advanced to reveal scattering patterns of molecules far from their equilibrium geometry. While dynamic displacements reflecting the motion of wavepackets can probe deeply into the reaction dynamics, in many systems, the thermal excitation embedded in the molecules upon optical excitation and energy randomization can create systems that encompass structures far from the ground state geometry. For polyatomic molecular systems, large amplitude vibrational motions are associated with anharmonicity and shifts of interatomic distances, making analytical solutions using traditional harmonic approximations inapplicable. More generally, the interatomic distances in a polyatomic molecule are not independent and the traditional equations commonly used to interpret the data may give unphysical results. Here, we introduce a novel method based on molecular dynamic trajectories and illustrate it on two examples of hot, vibrating molecules at thermal equilibrium. When excited at 200 nm, 1,3-cyclohexadiene (CHD) relaxes on a subpicosecond time scale back to the reactant molecule, the dominant pathway, and to various forms of 1,3,5-hexatriene (HT). With internal energies of about 6 eV, the energy thermalizes quickly, leading to structure distributions that deviate significantly from their vibrationless equilibrium. The experimental and theoretical results are in excellent agreement and reveal that a significant contribution to the scattering signal arises from transition state structures near the inversion barrier of CHD. In HT, our analysis clarifies that previous inconsistent structural parameters determined by electron diffraction were artifacts that might have resulted from the use of inapplicable analytical equations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

On the Formation of Phantom Electron Phase Space Density Peaks in Single Spacecraft Radiation Belt Data

This study examines the rapid losses and acceleration of trapped relativistic and ultrarelativistic electron populations in the Van Allen radiation belt during the September 7–9, 2017 geomagnetic storm. By analyzing the dynamics of the last closed drift shell (LCDS), and the electron flux and phase space density (PSD), we show that the electron dropouts are consistent with magnetopause shadowing and outward radial diffusion to the compressed LCDS. During the recovery phase, an in-bound pass of Van Allen Probe A shows an apparent local peak in PSD, which does not exist in reality. Here, a careful analysis of the multipoint measurements by the Van Allen Probes reveals instead how the apparent PSD peak arises from aliasing monotonic PSD profiles which are rapidly increasing due to acceleration from very fast inwards radial diffusion. In the absence of such multisatellite conjunctions during fast acceleration events, such peaks might otherwise be associated with local acceleration processes.

79 ASTRONOMY AND ASTROPHYSICS↗

Exploring Anomalous Polarization Dynamics in Organometallic Halide Perovskites

Organometallic halide perovskites (OMHPs) have attracted broad attention as prospective materials for optoelectronic applications. Among the many anomalous properties of these materials, of special interest are the ferroelectric properties including both classical and relaxor-like components, as a potential origin of slow dynamics, field enhancement, and anomalous mobilities. Here, ferroelectric properties of the three representative OMHPs are explored, including FAPb x Sn 1–x I 3 (x = 0, x = 0.85) and FA 0.85 MA 0.15 PbI 3 using band excitation piezoresponse force microscopy and contact mode Kelvin probe force microscopy, providing insight into long- and short-range dipole and charge dynamics in these materials and probing ferroelectric density of states. Furthermore, second-harmonic generation in thin films of OMHPs is observed, providing a direct information on the noncentrosymmetric polarization in such materials. Overall, the data provide strong evidence for the presence of ferroelectric domains in these systems; however, the domain dynamics is suppressed by fast ion dynamics. These materials hence present the limit of ferroelectric materials with spontaneous polarization dynamically screened by ionic and electronic carriers.

36 MATERIALS SCIENCE↗

Langmuir probe surveys of an arcjet exhaust

Electrostatic (Langmuir) probes of both spherical and cylindrical geometry have been used to obtain electron number density and temperature in the exhaust of a laboratory arcjet. The arcjet thruster operated on nitrogen and hydrogen mixtures to simulate fully decomposed hydrazine in a vacuum environment with background pressures less than 0.05 Pa. The exhaust appears to be only slightly ionized (less than 1 percent) with local plasma potentials near facility ground. The current-voltage characteristics of the probes indicate a Maxwellian temperature distribution. Plume data are presented as a function of arcjet operating conditions and also position in the exhaust.

Zana, Lynnette M.↗

Langmuir probe surveys of an arcjet exhaust

Electrostatic (Langmuir) probes of both spherical and cylindrical geometry have been used to obtain electron number density and temperature in the exhaust of a laboratory arcjet. The arcjet thruster operated on nitrogen and hydrogen mixtures to simulate fully decomposed hydrazine in a vacuum environment with background pressures less than 0.05 Pa. The exhaust appears to be only slightly ionized (less than 1 percent) with local plasma potentials near facility ground. The current-voltage characteristics of the probes indicate a Maxwellian temperature distribution. Plume data are presented as a function of arcjet operating conditions and also position in the exhaust.

Zana, Lynnette M.↗

Magnetic Field Measurement and Analysis for the Muon g-2 Experiment

The Muon g-2 Experiment (E989) at Fermilab measures the muon magnetic anomaly, aiming to resolve the greater than 3$\sigma$ discrepancy between the previous measurement and the Standard Model calculation with an improved precision of 140 part-per-billion (ppb). In E989, the muon beam is stored in a ring magnet. The spin precession frequency $\omega_{a}$ is measured by counting the decay positrons in 24 calorimeters, and the magnetic field is measured by nuclear magnet resonance (NMR) probes. An in-vacuum field scanning system consisting of NMR probes and read-out electronics has been implemented to measure the magnetic field applied to the muon beam. An additional 378 NMR probes, placed at fixed locations outside the vacuum chamber, monitor the field drift in between field scans. A high-accuracy probe was designed for calibrating the probes in the scanner. In this presentation, the magnetic field measurement hardware system and analysis methods will be described in detail. The progress of the Run-1 data analysis and improvements in Run-2 will be presented as well.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Demonstration of femtosecond X-ray pump X-ray probe diffraction on protein crystals

The development of X-ray free-electron lasers (XFELs) has opened the possibility to investigate the ultrafast dynamics of biomacromolecules using X-ray diffraction. Whereas an increasing number of structures solved by means of serial femtosecond crystallography at XFELs is available, the effect of radiation damage on protein crystals during ultrafast exposures has remained an open question. We used a split-and-delay line based on diffractive X-ray optics at the Linac Coherent Light Source XFEL to investigate the time dependence of X-ray radiation damage to lysozyme crystals. For these tests, crystals were delivered to the X-ray beam using a fixed-target approach. The presented experiments provide probe signals at eight different delay times between 19 and 213 femtoseconds after a single pump event, thereby covering the time-scales relevant for femtosecond serial crystallography. Even though significant impact on the crystals was observed at long time scales after exposure with a single X-ray pulse, the collected diffraction data did not show significant signal reduction that could be assigned to beam damage on the crystals in the sampled time window and resolution range. This observation is in agreement with estimations of the applied radiation dose, which in our experiment was clearly below the values expected to cause damage on the femtosecond time scale. The experiments presented here demonstrate the feasibility of time-resolved pump-multiprobe X-ray diffraction experiments on protein crystals.

43 PARTICLE ACCELERATORS↗

Optical interference effect in strong-field electronic coherence spectroscopy

Here, we investigate strong-field-induced electronic coherences in argon and molecular nitrogen ions created by high-intensity, few-cycle infrared laser pulses. This is a step toward the long-sought goal of strong-field coherent control in molecular chemistry. We employ high-intensity, few-cycle infrared laser pulses in a pump-probe setup to investigate a recent prediction that electronic coherences in nitrogen molecules change the ion yields versus pump-probe delay. [Yuen et al., Phys. Rev. A 109, L011101 (2024)]. The predicted coherence signals in molecular nitrogen could not be resolved above the optical interference of the pump and probe pulses; a simultaneous measurement clearly resolved the induced cation fine-structure coherence in strong-field-ionized argon. The results of our comparison with simulations suggest that optical interference effects manifest differently in each ionic species and must be carefully accounted for when interpreting experimental data. We find that nonsequential double ionization in the low-intensity region of the focal volume can reduce the visibility of coherence generated by two-pulse sequential ionization, and we quantify the importance of pulse shape and spectral characteristics for isolating the desired coherence signals.

charge migration↗

Quantitative examination of carbide and sulphide precipitates in chemically complex steels processed by direct strip casting

A high strength low alloy steel composition has been melted and processed by two different routes: simulated direct strip casting and slow cooled ingot casting. The microstructures were examined with scanning and transmission electron microscopy, atom probe tomography and small angle neutron scattering (SANS). The formation of cementite (Fe{sub 3}C), manganese sulphides (MnS) and niobium carbo-nitrides (Nb(C,N)) was investigated in both casting conditions. The sulphides were found to be significantly refined by the higher cooling rate, and developed an average diameter of only 100 nm for the fast cooled sample, and a diameter too large to be measured with SANS in the slow cooled condition (> 1.1 μm). Slow cooling resulted in the development of classical Nb(C,N) precipitation, with an average diameter of 7.2 nm. However, after rapid cooling both the SANS and atom probe tomography data indicated that the Nb was retained in the matrix as a random solid solution. There was also some evidence that O, N and S are also retained in solid solution in levels not found during conventional processing. - Highlights: • The influence of cooling rate on microstructure is investigated in a HSLA steel. • SANS, TEM and APT are used to characterise the sulphides and Nb(C,N) precipitates. • The slow cooling rate result in the formation of Nb(C,N) precipitates. • The fast cooling rate results in a microstructure supersaturated in Nb, C and N. • The sulphides are 100 nm in the fast cooled sample and > 1 μm in the slow cooled one.

36 MATERIALS SCIENCE↗

Defect chemistry and high-temperature transport in SrFe{sub 1−x}Sn{sub x}O{sub 3–δ}

The electrical conductivity of SrFe{sub 1–x}Sn{sub x}O{sub 3–δ} (x=0.05, 0.10, 017) was measured by a four-probe dc technique in the partial oxygen pressure range of 10{sup –18}–0.5 atm at temperatures between 800 °Ð ÐŽ and 950 °Ð ÐŽ. The oxygen content in these oxides was measured under the same ambient conditions by means of coulometric titration. The thermodynamic analysis of oxygen nonstoichiometry data was carried out to determine the equilibrium constants for defect-formation reactions and to calculate the concentrations of ion and electron charge carriers. The partial contributions of oxygen ions, electrons and holes to charge transport were assessed, and the mobility of respective carriers was evaluated by an integral examination of the electrical conductivity and oxygen nonstoichiometry data. It has been found that the mobility of holes in SrFe{sub 1−x}Sn{sub x}O{sub 3−δ} varies in the range of ~0.005–0.04 cm{sup 2} V{sup −1} s{sup −1}, linearly increasing with the oxygen content and decreasing with increased tin concentration. The mobility of electron carriers was shown to be independent of the oxygen content. The average migration energy of an electron was estimated to be ~0.45 eV, with that of a hole being ~0.3 eV. - Highlights: • The conductivity and oxygen nonstoichiometry in SrFe{sub 1−x}Sn{sub x}O{sub 3−δ} were measured. • Tin substitution was found to affect insignificantly defect formation reactions. • The hole mobility was found to increase linearly with the oxygen content. • The hole mobility was found to be much higher than the electron mobility.

36 MATERIALS SCIENCE↗

Probing the CP nature of the top–Higgs Yukawa coupling in t t ¯ H and tH events with H → b b ¯ decays using the ATLAS detector at the LHC

The CP properties of the coupling between the Higgs boson and the top quark are investigated using 139 fb−1 of proton–proton collision data recorded by the ATLAS experiment at the LHC at a centre-of-mass energy of s=13 TeV. The CP structure of the top quark–Higgs boson Yukawa coupling is probed in events with a Higgs boson decaying into a pair of b-quarks and produced in association with either a pair of top quarks, tt¯H, or a single top quark, tH. Events containing one or two electrons or muons are used for the measurement. Multivariate techniques are used to select regions enriched in tt¯H and tH events, where dedicated CP-sensitive observables are exploited. In an extension of the Standard Model (SM) with a CP-odd admixture in the top–Higgs Yukawa coupling, the mixing angle between CP-even and CP-odd couplings is measured to be α=11−73∘∘+52∘, compatible with the SM prediction corresponding to α=0.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Electron drift and longitudinal diffusion in high pressure xenon-helium gas mixtures

We report new measurements of the drift velocity and longitudinal diffusion coefficients of electrons in pure xenon gas and in xenon-helium gas mixtures at 1-9 bar and electric field strengths of 50-300 V/cm. In pure xenon we find excellent agreement with world data at all E/P, for both drift velocity and diffusion coefficients. However, a larger value of the longitudinal diffusion coefficient than theoretical predictions is found at low E/P in pure xenon, below the range of reduced fields usually probed by TPC experiments. A similar effect is observed in xenon-helium gas mixtures at somewhat larger E/P. Drift velocities in xenon-helium mixtures are found to be theoretically well predicted. Although longitudinal diffusion in xenon-helium mixtures is found to be larger than anticipated, extrapolation based on the measured longitudinal diffusion coefficients suggest that the use of helium additives to reduce transverse diffusion in xenon gas remains a promising prospect.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Measurement of ambient radon progeny decay rates and energy spectra in liquid argon using the MicroBooNE detector

We report measurements of radon progeny in liquid argon within the MicroBooNE time projection chamber (LArTPC). The presence of specific radon daughters in MicroBooNE’s 85 metric tons of active liquid argon bulk is probed with newly developed charge-based low-energy reconstruction tools and analysis techniques to detect correlated Bi 214 − Po 214 radioactive decays. Special datasets taken during periods of active radon doping enable new demonstrations of the calorimetric capabilities of single-phase neutrino LArTPCs for β and α particles with electron-equivalent energies ranging from 0.1 to 3.0 MeV. By applying Bi 214 − Po 214 detection algorithms to data recorded over a 46-day period, no statistically significant presence of radioactive Bi 214 is detected, and a limit on the activity is placed at < 0.35 mBq / kg at the 95% confidence level. This bulk Bi 214 radiopurity limit—the first ever reported for a liquid argon detector incorporating liquid-phase purification—is then further discussed in relation to the targeted upper limit of 1 mBq / kg on bulk Rn 222 activity for the DUNE neutrino detector. Published by the American Physical Society 2024

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Pioneer 10 and 11 ultraviolet photometer observations of the Jovian satellites

The Pioneer 10 and 11 Jupiter probes have provided several opportunities for observation of the Jovian satellites J I through J V. From these data, a tenuous atmosphere of hydrogen for Io has been identified. In the present work, an additional short-wavelength (less than 800 A) emission associated with an extended cloud centered on Io is reported and interpreted as arising from the radiative decay of excited atomic ions. Characteristic X-rays produced by electron bombardment of Io's surface may also contribute to the signal. Emission features associated with Amalthea (J V) and Europa (J II) are also observed. Signals apparently associated with J V occur in the long-wavelength channel, while emissions were observed in the short-wavelength channel during J II observations. The data of the long-wavelength channel are interpreted as arising from atomic hydrogen Lyman-alpha emission in all cases. The source species for the short-wavelength emissions cannot at this time be unambiguously determined, but the wavelength range of the signals is well established.

Judge, D. L.↗

From Chaos to Clarity: Autonomous Materials Discovery for Extreme Environments

The pursuit of advanced functional materials for energy applications demands an understanding of their behavior under the most challenging conditions. Extreme environments, characterized by intense radiation, high temperatures, and corrosive chemistries, push materials to their limits, often revealing unexpected behaviors and degradation pathways. Traditional materials research approaches, relying on trial-and-error experimentation, are often slow and resource-intensive, ill-suited to the complexities of extreme environments. This talk will explore the transformative potential of autonomous materials science in revolutionizing our understanding of materials synthesis and degradation in extreme environments. By integrating advanced microscopy techniques, artificial intelligence, and robotic experimentation, we can accelerate the discovery and design of resilient materials for a sustainable future. The presentation will highlight recent breakthroughs in autonomous microscopy, computer vision, and machine learning, showcasing their ability to unravel complex material transformations at the atomic scale. The talk will also delve into the challenges and opportunities associated with deploying autonomous systems to probe extreme environments, emphasizing the importance of robust algorithms, real-time data analysis, and adaptive experimentation. Our ultimate goal is to empower scientists with unprecedented capabilities to explore, understand, and engineer materials that can withstand the harshest conditions, paving the way for innovations in energy, aerospace, and beyond.

artificial intelligence↗

Two cubic phases in kimzeyite garnet from the type locality Magnet Cove, Arkansas

The crystal structure of an optically anisotropic kimzeyite garnet from Magnet Cove, Arkansas, USA, where it was first discovered, was refined with the Rietveld method, cubic space group, Ia\overline 3 d, and monochromatic [λ = 0.41422 (2) Å] synchrotron high-resolution powder X-ray diffraction (HRPXRD) data. The Rietveld refinement reduced χ 2 and overall R ( F 2 ) values are 1.840 and 0.0647, respectively. The sample, with the general garnet formula [8] X 3 [6] Y 2 [4] Z 3 [4] O 12 , contains an intergrowth of two cubic phases that occur initially as oscillatory growth zoning, and patchy intergrowths arise later from fluid-enhanced dissolution and re-precipitation. The two compositions obtained with electron-probe microanalyses (EPMA) are Ca 3.00 (Zr 1.31 Ti 4+ 0.46 Fe 3+ 0.22 Mn 3+ 0.01 ) Σ2 [Al 0.76 Fe 3+ 1.01 Si 1.23 ] Σ3 O 12 for phase 1 a and Ca 2.99 (Zr 1.48 Ti 4+ 0.37 Fe 3+ 0.15 ) Σ2 [Al 0.87 Fe 3+ 0.98 Si 1.15 ] Σ3 O 12 for phase 1 b . The weight percentage, unit-cell parameter (Å), distances (Å), and site occupancy factors (s.o.f.s) for phase 1 a are as follows: 42.6 (2)%, a = 12.46553 (3) Å, average < X —O> = 2.482, Y —O = 2.059 (2), Z —O = 1.761 (2) Å, Ca ( X s.o.f.) = 0.960 (4), Zr ( Y s.o.f.) = 0.809 (3), and Fe ( Z s.o.f.) = 0.623 (2). The corresponding values for phase 1 b are 57.4 (2)%, a = 12.47691 (2) Å, average < X —O> = 2.482, Y —O = 2.062 (1), Z —O = 1.762 (1) Å, Ca ( X s.o.f.) = 0.957 (3), Zr ( Y s.o.f.) = 0.828 (2) and Fe ( Z s.o.f.) = 0.617 (2). The main structural differences between the two phases are in the unit-cell parameter, Δ a = 0.01138 Å, Y (s.o.f.), and Y —O distance. Structural mismatch between the two cubic phases in a crystal gives rise to strain-induced optical anisotropy.

36 MATERIALS SCIENCE↗

Shock-tube studies of atomic silicon emission in the spectral range 180 to 300 nm

Emission spectroscopy of shock-heated atomic silicon was performed in the spectral range 180 to 300 nm, in an environment simulating the ablation layer expected around a Jovian entry probe with a silica heat shield. From the spectra obtained at temperatures from 6000 to 10,000 K and electron number densities from 1 quadrillion to 100 quadrillion per cu cm, the Lorentzian line-widths were determined. The results showed that silicon lines are broadened significantly by both electrons (Stark broadening) and hydrogen atoms (Van der Waals broadening), and the combined line-widths are much larger than previously assumed. From the data, the Stark and the Van der Waals line-widths were determined for 34 silicon lines. Radiative transport through a typical shock layer was computed using the new line-width data. The computations showed that silicon emission in the hot region is large, but it is mostly absorbed in the colder region adjacent to the wall.

Prakash, S. G.↗