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DOE OSTI2018

Ground and low-lying excited states of phenoxy, 1-naphthoxy, and 2-naphthoxy radicals via anion photoelectron spectroscopy

Here, we present the slow electron velocity map imaging spectroscopy of cryogenically cooled phenoxide, 1-naphthoxide, and 2-naphthoxide anions. The results allow us to examine the ground state and the lowest energy excited state in the corresponding neutral radicals. Care was taken to minimize autodetachment signals in the photoelectron spectra, allowing for more straightforward comparisons with Franck-Condon analyses. The ground states of these three aromatic oxide radicals all have the unpaired electron residing in a π orbital delocalized throughout the molecule. The electron affinity of 1-naphthoxy is measured to be 2.290(2) eV, while that of 2-naphthoxy is measured to be 2.404(2) eV, both of which are higher than that of the smaller phenoxy molecule at 2.253(1) eV. The first excited states have the unpaired electron residing in a more localized σ orbital, yielding measured term energies for the Ã state of 1.237(2) eV in 1-naphthoxy and 1.068(1) eV in 2-naphthoxy, while that of phenoxy is lower at 0.952(1) eV. The calculated Franck-Condon spectra generally showed good agreement with the experimental spectra, yielding assignments of the more active vibrations in each electronic state. Significant autodetachment signals arising from dipole bound states near the ground states of all three radicals were observed in our efforts to avoid them, and comparably less autodetachment signals were observed near the excited states. Besides this type of non-Franck-Condon intensities in the photoelectron spectra, we also observed minor features arising due to vibronic coupling in the ground states of all three radicals.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Characterization of Two Fast-Turnaround Dry Dilution Refrigerators for Scanning Probe Microscopy

Low-temperature scanning probe microscopes (SPMs) are critical for the study of quantum materials and quantum information science. Due to the rising costs of helium, cryogen-free cryostats have become increasingly desirable. However, they typically suffer from comparatively worse vibrations than cryogen-based systems, necessitating the understanding and mitigation of vibrations for SPM applications. Here, in this work, we demonstrate the construction of two cryogen-free dilution refrigerator SPMs with minimal modifications to the factory default and we systematically characterize their vibrational performance. We measure the absolute vibrations at the microscope stage with geophones and use both microwave impedance microscopy and a scanning single-electron transistor to independently measure tip-sample vibrations. Additionally, we implement customized filtering and thermal anchoring schemes and characterize the cooling power at the scanning stage and the tip electron temperature. This work serves as a reference to researchers interested in cryogen-free SPMs, as such characterization is not standardized in the literature or available from manufacturers.

36 MATERIALS SCIENCE↗

DOE OSTI2017

Magnetism out of antisite disorder in the J = 0 compound Ba 2 YIrO 6

Here, we systematically investigate the magnetic properties and local structure of Ba 2 YIrO 6 to demonstrate that Y and Ir lattice defects in the form of antiphase boundary or clusters of antisite disorder affect the magnetism observed in this 5d 4 compound. The experimental investigation involved comparison of the magnetic properties and atomic imaging of (1) a slow-cooled crystal, (2) a crystal quenched from 900°C after growth, and (3) a crystal grown using a faster cooling rate during growth than the slow-cooled one. Atomic-scale imaging by scanning transmission electron microscopy (STEM) shows that quenching from 900°C introduces Ir-rich antiphase boundaries in the crystals, and a faster cooling rate during crystal growth leads to clusters of Y and Ir antisite disorder. Compared to the slow-cooled crystals, Ba 2 YIrO 6 crystals with clusters of antisite defects have a larger effective moment and a larger saturation moment, while quenched crystals with Ir-rich antiphase boundary show a slightly suppressed moment. Our DFT and model magnetic Hamiltonian calculations suggest magnetic condensation is unlikely, as the energy to be gained from superexchange is small compared to the spin-orbit gap. However, once Y is replaced by Ir in the antisite disordered region, the picture of local nonmagnetic singlets breaks down and magnetism can be induced. This is because of (a) enhanced interactions due to increased orbital overlap and (b) increased number of orbitals mediating the interactions. Our work highlights the importance of lattice defects in understanding the experimentally observed magnetism in Ba 2 YIrO 6 and other J = 0 systems.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

NASA NTRS2015

ISS-CREAM Thermal and Fluid System Design and Analysis

Thermal and Fluids Analysis Workshop (TFAWS), Silver Spring MD NCTS 21070-15. The ISS-CREAM (Cosmic Ray Energetics And Mass for the International Space Station) payload is being developed by an international team and will provide significant cosmic ray characterization over a long time frame. Cold fluid provided by the ISS Exposed Facility (EF) is the primary means of cooling for 5 science instruments and over 7 electronics boxes. Thermal fluid integrated design and analysis was performed for CREAM using a Thermal Desktop model. This presentation will provide some specific design and modeling examples from the fluid cooling system, complex SCD (Silicon Charge Detector) and calorimeter hardware, and integrated payload and ISS level modeling. Features of Thermal Desktop such as CAD simplification, meshing of complex hardware, External References (Xrefs), and FloCAD modeling will be discussed.

Thermal analysis↗

DOE OSTI2018

Photoelectron spectroscopy of anthracene and fluoranthene radical anions

Here, we report the slow electron velocity map imaging spectroscopy of cryogenically cooled anthracene and fluoranthene radical anions, two similarly sized polycyclic aromatic hydrocarbon molecules. The results allow us to examine the lowest energy singlet and triplet states in the neutral molecules on equal footing from the anionic ground state. The analysis of the experimental spectra is aided by harmonic calculations and Franck-Condon simulations, which generally show good agreement with experimental values and spectra. The electron affinity of fluoranthene is measured to be 0.757(2) eV, which is larger than that of anthracene at 0.532(3) eV. The lowest energy triplet state in anthracene is observed at 1.872(3) eV above the singlet ground state, while that of fluoranthene is observed at 2.321(2) eV above its singlet ground state. Comparisons of experimental and calculated spectra show that in addition to the Franck-Condon active modes, there is a clear presence of vibrational modes that gain intensity via vibronic coupling in both the singlet and triplet states in both molecules. In addition, the triplet state generally exhibits increased vibronic coupling compared to the singlet state, with the fluoranthene triplet state exhibiting evidence of distortion from C 2v symmetry.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2017

CHROMOSPHERE TO 1 au SIMULATION OF THE 2011 MARCH 7th EVENT: A COMPREHENSIVE STUDY OF CORONAL MASS EJECTION PROPAGATION

We perform and analyze the results of a global magnetohydrodynamic simulation of the fast coronal mass ejection (CME) that occurred on 2011 March 7. The simulation is made using the newly developed Alfvén Wave Solar Model (AWSoM), which describes the background solar wind starting from the upper chromosphere and extends to 24 R {sub ⊙}. Coupling AWSoM to an inner heliosphere model with the Space Weather Modeling Framework extends the total domain beyond the orbit of Earth. Physical processes included in the model are multi-species thermodynamics, electron heat conduction (both collisional and collisionless formulations), optically thin radiative cooling, and Alfvén-wave turbulence that accelerates and heats the solar wind. The Alfvén-wave description is physically self-consistent, including non-Wentzel–Kramers–Brillouin reflection and physics-based apportioning of turbulent dissipative heating to both electrons and protons. Within this model, we initiate the CME by using the Gibson-Low analytical flux rope model and follow its evolution for days, in which time it propagates beyond STEREO A . A detailed comparison study is performed using remote as well as in situ observations. Although the flux rope structure is not compared directly due to lack of relevant ejecta observation at 1 au in this event, our results show that the new model can reproduce many of the observed features near the Sun (e.g., CME-driven extreme ultraviolet [EUV] waves, deflection of the flux rope from the coronal hole, “double-front” in the white light images) and in the heliosphere (e.g., shock propagation direction, shock properties at STEREO A ).

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2019

Microstructural and Textural Evolutions during β → α/ω Transformation in Biomedical Ti-15Mo Alloy and Its Effects on Mechanical Performance

This study investigated the precipitation behaviors and mechanical performance of Ti-15Mo alloy subjected to different treatment conditions. The microstructures were analyzed via scanning electron microscopy and transmission electron microscopy. The tensile properties and resultant fracture surfaces were investigated to determine the relationship between the phase transformation and mechanical performance. The Ti-15Mo alloy had a notable elongation due to no observable precipitation during solution treatment plus quenching (STQ). A high ultimate tensile strength (UTS) was obtained with a considerable amount of ω precipitates transformed during air cooling after solution treatment (ST). The coarse precipitates and additional precipitation free zones in the Ti-15Mo alloy treated with furnace cooling (FC) after ST induced a decrease in UTS. Furthermore, the absence of a continuous grain boundary α phase resulted in a lower strength in the specimen annealed at 600 °C after hot rolling. The alloy iso-aged after STQ exhibited good tensile properties with a UTS of 920 MPa and an elongation of 15%. The texture and variant relationship of the precipitates was analyzed with x-ray diffraction and electron backscatter diffraction. The common variants of the β matrix influenced the nucleation of precipitates in the Ti-15Mo alloy annealed after hot rolling, and the precipitates showed an obvious {01-10}α main texture. The variant selection of α precipitates at the grain boundary was caused by the two adjacent β grains in the alloy treated by FC after ST.

36 MATERIALS SCIENCE↗

DOE OSTI2015

Influence of cooling rate on the precipitation behavior in Ti–Nb–Mo microalloyed steels during continuous cooling and relationship to strength

In this study we elucidate carbide precipitation at varied cooling rates in Ti–Nb–Mo microalloyed steels during continuous cooling. The study suggests that increasing the cooling rate prevents precipitate formation in the ferrite phase during continuous cooling after finish rolling at 850 °C. At a lower cooling rate of 0.5 °C/s, the microhardness of ferrite grains exhibited maxima because of high volume fraction of fine carbides. A high density of nanoscale carbides with similar precipitation characteristics, including interphase precipitates, was observed at cooling rates of 0.5 and 1 °C/s, but the carbides were marginally larger and the spacing between them was increased with cooling rate. Additionally, carbide precipitation at a high cooling rate was associated with strain-induced precipitation. Through the analysis of selection area electron diffraction patterns and high-resolution transmission electron microscopy, lattice imaging, the fine spherical-shaped carbides of size ~ 6–10 nm were identified as MC-type carbides of the type (Ti,Nb,Mo)C and NbC. - Highlights: • We model three cooling rates which have indicated different precipitation behaviors. • We find two types of precipitates including NbC and (Ti,Nb,Mo)C based on HRTEM study. • Increasing cooling rate will decrease volume fraction and size of the precipitates. • There is no absence of interphase precipitation when the cooling rate increases to 5 °C/s.

36 MATERIALS SCIENCE↗

DOE OSTI2015

Auger-Limited Carrier Recombination and Relaxation in CdSe Colloidal Quantum Wells

Using time-resolved photoluminescence spectroscopy, we show that two-exciton Auger recombination dominates carrier recombination and cooling dynamics in CdSe nanoplatelets, or colloidal quantum wells. The electron-hole recombination rate depends only on the number of electron-hole pairs present in each nanoplatelet, and is consistent with a twoexciton recombination process over a wide range of exciton densities. The carrier relaxation rate within the conduction and valence bands also depends only on the number of electron-hole pairs present, apart from an initial rapid decay, and is consistent with the cooling rate being limited by reheating due to Auger recombination processes. These Auger-limited recombination and relaxation dynamics are qualitatively different from the carrier dynamics in either colloidal quantum dots or epitaxial quantum wells. TOC FIGURE:

Auger Recombination↗

DOE OSTI2023

Understanding and Controlling Photothermal Responses in MXenes

MXenes have the potential for efficient light-to-heat conversion in photothermal applications. To effectively utilize MXenes in such applications, it is important to understand the underlying nonequilibrium processes, including electron–phonon and phonon–phonon couplings. Here, we use transient electron and X-ray diffraction to investigate the heating and cooling of photoexcited MXenes at femtosecond to nanosecond time scales. Our results show extremely strong electron–phonon coupling in Ti 3 C 2 -based MXenes, resulting in lattice heating within a few hundred femtoseconds. We also systematically study heat dissipation in MXenes with varying film thicknesses, chemical surface terminations, flake sizes, and annealing conditions. We find that the thermal boundary conductance (TBC) governs the thermal relaxation in films thinner than the optical penetration depth. In conclusion, we achieve a 2-fold enhancement of the TBC, reaching 20 MW m –2 K –1 , by controlling the flake size or chemical surface termination, which is promising for engineering heat dissipation in photothermal and thermoelectric applications of the MXenes.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

DOE OSTI2016

Plant model of KIPT neutron source facility simulator

Argonne National Laboratory (ANL) of the United States and Kharkov Institute of Physics and Technology (KIPT) of Ukraine are collaborating on constructing a neutron source facility at KIPT, Kharkov, Ukraine. The facility has 100-kW electron beam driving a subcritical assembly (SCA). The electron beam interacts with a natural uranium target or a tungsten target to generate neutrons, and deposits its power in the target zone. The total fission power generated in SCA is about 300 kW. Two primary cooling loops are designed to remove 100-kW and 300-kW from the target zone and the SCA, respectively. A secondary cooling system is coupled with the primary cooling system to dispose of the generated heat outside the facility buildings to the atmosphere. In addition, the electron accelerator has a low efficiency for generating the electron beam, which uses another secondary cooling loop to remove the generated heat from the accelerator primary cooling loop. One of the main functions the KIPT neutron source facility is to train young nuclear specialists; therefore, ANL has developed the KIPT Neutron Source Facility Simulator for this function. In this simulator, a Plant Control System and a Plant Protection System were developed to perform proper control and to provide automatic protection against unsafe and improper operation of the facility during the steady-state and the transient states using a facility plant model. This report focuses on describing the physics of the plant model and provides several test cases to demonstrate its capabilities. The plant facility model uses the PYTHON script language. It is consistent with the computer language of the plant control system. It is easy to integrate with the simulator without an additional interface, and it is able to simulate the transients of the cooling systems with system control variables changing on real-time.

43 PARTICLE ACCELERATORS↗

DOE OSTI2019

Optical Stochastic Cooling Program at Fermilab's Integrable Optics Test Accelerator

Beam cooling enables an increase of peak and average luminosities and significantly expands the discovery potential of colliders. Optical Stochastic Cooling (OSC) is a high-bandwidth cooling technique that will advance the present state-of-the-art, stochastic-cooling rate by more than three orders of magnitude. A proof-of-principle demonstration with protons or heavy ions involves prohibitive costs, risks and technological challenges; however, exploration of OSC with electrons is a cost-effective alternative for studying the beam-cooling physics, optical systems and diagnostics. The ability to demonstrate OSC was a key requirement in the design of Fermilab's Integrable Optics Test Accelerator (IOTA) ring. The IOTA program will explore the physics and technology of OSC in amplified and non-amplified configurations. We also plan to investigate the cooling and manipulation of a single electron stored in the ring. The OSC apparatus is currently being fabricated, and installation will begin in the fall of 2019. In this contribution, we will describe the IOTA OSC program, the upcoming passive-OSC experimental runs and ongoing preparations for an amplified-OSC experiment

43 PARTICLE ACCELERATORS↗

DOE OSTI2019

Optical Stochastic Cooling Program at Fermilab's Integrable Optics Test Accelerator

43 PARTICLE ACCELERATORS↗

DOE OSTI2016

THE LAUNCHING OF COLD CLOUDS BY GALAXY OUTFLOWS. II. THE ROLE OF THERMAL CONDUCTION

We explore the impact of electron thermal conduction on the evolution of radiatively cooled cold clouds embedded in flows of hot and fast material as it occurs in outflowing galaxies. Performing a parameter study of three-dimensional adaptive mesh refinement hydrodynamical simulations, we show that electron thermal conduction causes cold clouds to evaporate, but it can also extend their lifetimes by compressing them into dense filaments. We distinguish between low column-density clouds, which are disrupted on very short times, and high-column density clouds with much longer disruption times that are set by a balance between impinging thermal energy and evaporation. We provide fits to the cloud lifetimes and velocities that can be used in galaxy-scale simulations of outflows in which the evolution of individual clouds cannot be modeled with the required resolution. Moreover, we show that the clouds are only accelerated to a small fraction of the ambient velocity because compression by evaporation causes the clouds to present a small cross-section to the ambient flow. This means that either magnetic fields must suppress thermal conduction, or that the cold clouds observed in galaxy outflows are not formed of cold material carried out from the galaxy.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2016

Thermal evolution of antiferromagnetic correlations and tetrahedral bond angles in superconducting FeTe 1-x Se x

It has recently been demonstrated that dynamical magnetic correlations measured by neutron scattering in iron chalcogenides can be described with models of short-range correlations characterized by particular choices of four-spin plaquettes, where the appropriate choice changes as the parent material is doped towards superconductivity. Here we apply such models to describe measured maps of magnetic scattering as a function of two-dimensional wave vectors obtained for optimally superconducting crystals of FeTe 1–x Se x . We show that the characteristic antiferromagnetic wave vector evolves from that of the bicollinear structure found in underdoped chalcogenides (at high temperature) to that associated with the stripe structure of antiferromagnetic iron arsenides (at low temperature); these can both be described with the same local plaquette, but with different interplaquette correlations. While the magnitude of the low-energy magnetic spectral weight is substantial at all temperatures, it actually weakens somewhat at low temperature, where the charge carriers become more itinerant. The observed change in spin correlations is correlated with the dramatic drop in the electronic scattering rate and the growth of the bulk nematic response upon cooling. Lastly, we also present powder neutron diffraction results for lattice parameters in FeTe 1–x Se x indicating that the tetrahedral bond angle tends to increase towards the ideal value upon cooling, in agreement with the increased screening of the crystal field by more itinerant electrons and the correspondingly smaller splitting of the Fe 3d orbitals.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2017

Rapid Tooling for Functional Prototype of Metal Mold Processes Final Report CRADA No. TC-1032-98

Production inserts for die-casting were generally fabricated from materials with sufficient strength and· good wear properties at casting temperatures for long life. Frequently tool steels were used and machining was done with a combination of. conventional and Electric Discharge Machining (EDM) with some handwork, an expensive and time consuming process, partilly for prototype work. We proposed electron beam physical vapor deposition (EBPVD) as a process for rapid fabrication of dies. Metals, ranging from low melting point to refractory metals (Ta, Mo, etc.), would be evaporated and deposited at high rates (-2mm/hr.). Alloys could be easily evaporated and deposited if their constituent vapor pressures were similar and with more difficulty if they were not. Of course, layering of different materials was possible if required for a specific application. For example, a hard surface layer followed by a tough steel and backed by a high thermal conductivity (possibly cooled) copper layer could be fabricated. Electron-beam deposits exhibited 100% density and lull strength when deposited at a substrate (mandrel) temperature that was a substantial fraction of the deposited material's melting point. There were several materials that could have the required high temperature properties and ease of fabrication required for such a mandrel. We had successfully used graphite, machined from free formed objects with a replicator, to produce aluminum-bronze test molds. There were several parting layer materials of interest, but the ideal material depended upon the specific application.

36 MATERIALS SCIENCE↗

DOE OSTI2016

Thermal Performance Benchmarking

The goal for this project is to thoroughly characterize the thermal performance of state-of-the-art (SOA) in-production automotive power electronics and electric motor thermal management systems. Information obtained from these studies will be used to: evaluate advantages and disadvantages of different thermal management strategies; establish baseline metrics for the thermal management systems; identify methods of improvement to advance the SOA; increase the publicly available information related to automotive traction-drive thermal management systems; help guide future electric drive technologies (EDT) research and development (R&D) efforts. The thermal performance results combined with component efficiency and heat generation information obtained by Oak Ridge National Laboratory (ORNL) may then be used to determine the operating temperatures for the EDT components under drive-cycle conditions. In FY16, the 2012 Nissan LEAF power electronics and 2014 Honda Accord Hybrid power electronics thermal management system were characterized. Comparison of the two power electronics thermal management systems was also conducted to provide insight into the various cooling strategies to understand the current SOA in thermal management for automotive power electronics and electric motors.

33 ADVANCED PROPULSION SYSTEMS↗

NASA NTRS1992

Of narrow lines and beaming in the strong-field SSC emission model

The synchrotron self-Compton (SSC) emission model for gamma-ray bursts is capable of producing narrow line features for a variety of modelled field strengths, primary electron injection distributions and burst luminosities. Multiple resonant scattering with synchrotron continuum photons efficiently traps and cools pairs in the ground state to an average energy where the Compton energy loss rate is zero. Annihilation between pairs in these cooled distributions can be very efficient. For isotropic injection of primary electrons, there is an anti-correlation of the intensity of the angular-binned emission between the portions of the continuum spectrum below the cyclotron peak and above the annihilation line feature. Small-angle emission dominates the continuum above the annihilation line feature and is smooth through the line up to the pair production cut-off, which can be above several MeV for small enough angles. The angle-averaged annihilation line is made of components which can have peak emission centered at energies away from 511 keV, due to Doppler shifting. For beamed injection,the annihilation line breaks up into relatively narrow components in the angular emission, which sum into a broad feature in the angle-averaged emission.

Preece, Robert D.↗