Ion Beam Implantation for Nanofabrication and Modification.
Abstract not provided.
Bielejec, Edward S.↗
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Ion Beam Implantation for Nanofabrication and Modification.
Abstract not provided.
Bielejec, Edward S.↗
Site-Selective Modification of Lanthanum Oxychloride to Modulate Halide-Ion Conduction
Design principles for solid-state halide-ion conduction remain poorly defined despite the increasing importance of halide ions as charge carriers in a variety of energy storage and electrochemical computing technologies. Here, we employ a siteselective modification strategy in which aliovalent cations are preferentially introduced at the La 3+ crystallographic site of LaOCl in the 2c Wyckoff position, enabling controlled generation of chloride vacancies and modification of lattice dynamics to enhance chloride-ion conductivity. Aliovalent substitution of La 3+ with Mg 2+ , Ca 2+ , and Sr 2+ generates charge-compensating Cl vacancies while preserving the matlockite crystal structure. X-ray excited optical luminescence measurements with Dy 3+ as a reporter chromophore evidence vacancy-derived midgap electronic states and an extended energy range of radiation-less Auger electron emission corresponding to substantial modification of electronic structure and local electrostatic potentials. Ca alloying at 8−10 at. % increases the chloride-ion conductivity by three- to 4 orders of magnitude as compared to unalloyed LaOCl, whereas comparable amounts of Sr- and Mg-alloying in LaOCl imbue less pronounced conductivity enhancements. Temperature-dependent Raman spectroscopy measurements reveal that Ca- and Sr-alloying substantially soften the La−Cl sublattice and yield a more compliant crystal lattice that can deform to accommodate Cl-ion migration. Structure solutions derived from Rietveld refinements to powder Xray diffraction reveal larger O−La−Cl bond-angle deviations and enhanced out-of-plane cation displacements for Ca- and Sr-alloyed compositions as compared to Mg-alloyed LaOCl. Such local distortions enhance chloride-ion mobility by reshaping and flattening vacancy migration energy landscapes and by modulating lattice dynamics governing anion conduction. We further illustrate that coalloying of Ca with Mg and Sr induces a nonmonotonic conductivity−defect stoichiometry relationship that can be rationalized based on cooperative interactions. Together, these results establish site-selective aliovalent alloying of LaOCl as an effective route to halide-ion solid electrolytes and provide broadly generalizable design principles for site-selective modification to induce vacancy formation and lattice softening to engender facile anion transport
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Quantitative investigation of surface structure and interatomic potential with impact-collision ion scattering spectroscopy
Helium ion beam interactions with materials have important implications for magnetic confinement fusion, material modification, and helium ion microscopy. These interactions depend on the precise physics of how helium ions channel into the materials, which can vary greatly based on the local crystalline orientation. Here, we performed a dedicated experiment to investigate helium ion channeling in a well-characterized tungsten single crystal. Time-of-flight impact-collision ion scattering spectroscopy was used to obtain multi-angle maps of the backscattering intensity for 3 keV He + → W(111). We found that the backscattering intensity profile arising from helium ion channeling could be well described by a shadow cone analysis. This analysis revealed that subsurface W atoms as deep as the ninth monolayer contributed to the backscattering intensity profile. Binary collision approximation simulations were performed with MARLOWE to model the experimental maps with sufficient accuracy to allow for quantitative comparisons using reliability factors. These quantitative comparisons were applied to investigate how the W lattice structure and He–W interatomic potential affect the multi-angle maps.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Cross-beam energy transfer saturation by ion trapping-induced detuning
The performance of direct-drive inertial confinement fusion implosions relies critically on the coupling of laser energy to the target plasma. Cross beam energy transfer (CBET), the resonant exchange of energy between intersecting laser beams mediated by ponderomotively driven ion-acoustic waves (IAW), inhibits this coupling by scattering light into unwanted directions. Furthermore, the variety of beam intersection angles and varying plasma conditions in an implosion results in IAWs with a range of phase velocities. Here we show that CBET saturates through a resonance detuning that depends on the IAW phase velocity and that results from trapping-induced modifications to the ion distribution functions. For smaller phase velocities, the modifications to the distribution functions can rapidly thermalize in the presence of mid-Z ions, leading to a blueshift in the resonant frequency. For larger phase velocities, the modifications can persist, leading to a redshift in the resonant frequency. Ultimately, these results may reveal pathways towards CBET mitigation and inform reduced models for radiation hydrodynamics codes to improve their predictive capability.
70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
Modification of a Silicon Photomultiplier for Reduced High Temperature Dark Count Rate
In this work we present a novel method for improving the high-temperature performance of silicon photomultipliers (SiPMs) via focused ion beam (FIB) modification of individual microcells. The literature suggests that most of the dark count rate (DCR) in a SiPM is contributed by a small percentage (<5%) of microcells. By using a FIB to electrically deactivate this relatively small number of microcells, we believe we can greatly reduce the overall DCR of the SiPM at the expense of a small reduction in overall photodetection efficiency, thereby improving its high temperature performance. In this report we describe our methods for characterizing the SiPM to determine which individual microcells contribute the most to the DCR, preparing the SiPM for FIB, and modifying the SiPM using the FIB to deactivate the identified microcells.
42 ENGINEERING↗
Near-surface modification of defective KTaO 3 by ionizing ion irradiation
The synergistic effect of nuclear (S n ) and electronic (S e ) energy loss observed in some ABO 3 perovskites has attracted considerable attention due to the real possibility to modify various near-surface properties, such as the electronic and optical properties, by patterning ion tracks in the defective near-surface regions. In this study, we show that low-energy ion-induced disordering in conjunction with ionizing ion irradiation (18 MeV Si, 21 MeV Ni and 91.6 MeV Xe) is a promising approach for tailoring ion tracks in the near-surface of defective KTaO 3 . Experimental characterization and computer simulations reveal that the size of these latent ion tracks increases with S e and level of pre-existing damage. These results further reveal that the threshold S e value (S e th ) for track creation increases with decreasing pre-damage level. The values of S e th increase from 5.02 keV nm -1 , for a pre-existing fractional disorder of 0.53 in KTaO 3 , to 10.81 keV nm -1 for pristine KTaO 3 . Above these thresholds, amorphous latent tracks are produced due local melting and rapid quenching. Below a disorder fraction of 0.08 and S e ≤ 6.68 keV nm -1 , the synergistic effect is not active, and damage accumulation is suppressed due to a competing ionization-induced damage annealing process. These results indicate that, depending on S e and the amount of pre-existing damage, highly ionizing ions can either enhance or suppress damage accumulation in KTaO 3 , thus providing a pathway to tailoring defects states. Comprehending the conflicting roles of highly ionizing ions in defective ABO 3 oxides is vital for understanding and predictive modeling of ion-solid interactions in complex oxides, as well as for achieving control over ion track size in the near-surface of defective KTaO 3 .
36 MATERIALS SCIENCE↗
Graphene coating on silicon anodes enabled by thermal surface modification for high-energy lithium-ion batteries
Silicon is a high-energy density anode material for lithium-ion batteries, but it possesses shortcomings such as poor electronic conductivity, interfacial instability and mechanical fracturing that hinder its battery cycling. Carbon coating has been an important strategy for stabilizing silicon anodes, but the effects of the silicon surface properties on carbon coating morphology and the consequent silicon cycling stability have not been clearly elucidated. Herein, we find that thermal oxidation of the silicon anodes followed by chemical vapor deposition of carbonaceous precursors leads to a well-ordered graphene coating, whereas disordered graphite coating is formed on the native silicon surface. Graphene-coated silicon exhibits superior cycling performance, retaining a discharge capacity of ~1300 mAh g -1 after 300 cycles, whereas the disordered graphite-coated silicon suffers continuous degradation, retaining only~600 mAh g -1 after 300 cycles. Cryogenic electron microscopy reveals the mechanism behind the difference in cycling stabilities; graphene coated silicon is able to withstand the large mechanical strains induced during extended cycling, whereas disordered graphite coating is ruptured, exposing silicon surfaces to the electrolyte, leading to extensive buildup of SEI and poor cycling performance. Characterization of the silicon surface reveals that thermal treatment yields an oxygen-rich surface layer, which is hypothesized to play a decisive role in dictating the carbon coating. This work highlights the effect of silicon surface properties on carbon coating microstructure, and presents thermal treatment as a facile avenue to attain graphene coating on silicon anodes.
25 ENERGY STORAGE↗
Interplay Between Stereochemically Active Lone Pair Repulsions, Sigma Hole Interactions, and Delocalized Redox Processes in Topochemical Fluoride‐Ion Insertion
Topochemical insertion/extraction of cations has emerged as a generalizable strategy for modulating the crystal and electronic structure of periodic solids. In contrast, strategies for topochemical anion insertion are poorly explored and fundamental principles for designing insertion hosts to accommodate anions remain scarce. Here, we observe reversible room-temperature fluoride-ion insertion within tunnels of Sn 2 TiO 4 defined by the stereochemical expression of Sn 5 s 2 lone pairs. X-ray scattering studies of fluoride-ion-insertion-induced crystal structure modulation and X-ray absorption/emission spectroscopy probes of electronic structure along with magnetic susceptibility measurements and first-principles calculations are used to decipher design principles underpinning reversible fluoride-ion insertion and bulk diffusion. Fluoride-ion insertion is enabled by a combination of a large, polarizable tunnel, delocalized redox at Ti─O─Sn centers, inherent repulsion between the fluoride-ion and Sn 5 s 2 electron lone pairs, and the formation of dative interactions between Sn-centered σ-holes and fluoride-ions, yielding a reversible capacity of 0.5 fluoride-ions per Sn 2 TiO 4 formula unit. Our results demonstrate that the complex interplay between dative interactions and stereochemically active lone pair repulsions is critical to defining the thermodynamics and kinetics controlling fluoride-ion insertion and diffusion. As such, the design of fluoride-ion insertion hosts for anion batteries requires site-selective modification to modulate lattice—ion interactions.
36 MATERIALS SCIENCE↗
Polyphosphonates as ionic conducting polymers
Polyphosphonates, a class of polymers with the generic formula –[P(R)(X)–OR'O] n –, exhibit a high degree of modularity due to the range of R, R', and X groups that can be incorporated. As such, these polymers may be designed with a polyethylene oxide (PEO) backbone (R' group) and employed as solid polymer electrolytes (SPEs). Two PEO-containing polyphosphonate analogs (R = Ph; X = S or Se) were doped with LiPF 6 and their conductivities were measured. Conductivities were similar (X = S) to or exceeding (X = Se) those of standard PEO systems (just below 10 -4 S/cm at 100°C). Binding models for Li + were generated using 31 P{ 1 H}NMR titration experiments. Binding of Li + by these polyphosphonates followed a positive cooperativity model, and varying the X group (S or Se) affected the observed cooperativity (Hill coefficient = 1.73 and 4.16, respectively). The presence of Se also leads to an increase in conductivity as temperature is raised above the T g , which is likely an effect of reduced Columbic interactions. Finally, because of their modularity and ease with which cation binding can be evaluated using 31 P{ 1 H} NMR titration experiments, polyphosphonates offer a unique approach for the modification of Li + ion battery technology.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Relationship between ZSM-5 pore modifications and gallium proximity and liquid hydrocarbon number distribution from ethanol oligomerization
Effect of ZSM-5 pore modification and gallium ions proximity inside the zeolite channels on ethanol conversion to liquid hydrocarbon yields.
Seemala, Bhogeswararao↗
Improved interfacial li-ion transport in composite polymer electrolytes via surface modification of LLZO
Composite polymer electrolytes that incorporate ceramic fillers in a polymer matrix offer mechanical strength and flexibility as solid electrolytes for lithium metal batteries. However, fast Li + transport between polymer and Li + -conductive filler phases is not a simple achievement due to high barriers for Li + exchange across the interphase. This study demonstrates how modification of Li 7 La 3 Zr 2 O 12 (LLZO) nanofiller surfaces with silane chemistries influences Li + transport at local and global electrolyte scales. Anhydrous reactions covalently link amine-functionalized silanes [(3-aminopropyl)triethoxysilane (APTES)] to LLZO nanoparticles, which protects LLZO in air. APTES functionalization lowers the poly (ethylene oxide) (PEO)-LLZO interphase resistance to half that of unmodified LLZO and increases effective Li + transference number, while insulating Al 2 O 3 completely blocks ion exchange and lowers transference number and conductivity in PEO-lithium bis(trifluoromethanesulfonyl)imide (LiTFSI)-LLZO composites. Modeling an inner resistive interphase between LLZO and PEO surrounded by an outer conductive interphase explains non-linear conductivity trends. Solid-state 7 Li & 6 Li nuclear magnetic resonance shows Li + only exchanges between PEO-LiTFSI and some LLZO interphase, with no appreciable Li + transport through bulk LLZO. Surface functionalization is a promising path toward lowering the polymer-ceramic interphase resistance. This work demonstrates that local changes in Li + transport affect macroscopic performance, highlighting the intricate relationships between all interfaces in inherently heterogeneous composite polymer electrolytes.
25 ENERGY STORAGE↗
Erratum to: Soft- and reactive landing of ions onto surfaces: concepts and applications
Soft- and reactive landing of mass-selected ions is gaining attention as a promising approach for the precisely-controlled preparation of materials on surfaces that are not amenable to deposition using conventional methods. A broad range of ionization sources and mass filters are available that make ion soft-landing a versatile tool for surface modification using beams of hyperthermal (<100?eV) ions. The ability to select the mass-to-charge ratio of the ion, its kinetic energy and charge state, along with precise control of the size, shape, and position of the ion beam on the deposition target distinguishes ion soft landing from other surface modification techniques. Soft- and reactive landing have been used to prepare interfaces for practical applications as well as precisely-defined model surfaces for fundamental investigations in chemistry, physics, and materials science. For instance, soft- and reactive landing have been applied to study the surface chemistry of ions isolated in the gas-phase, prepare arrays of proteins for high-throughput biological screening, produce novel carbon-based and polymer materials, enrich the secondary structure of peptides and the chirality of organic molecules, immobilize electrochemically-active proteins and organometallics on electrodes, create thin films of complex molecules, and immobilize catalytically active organometallics as well as ligated metal clusters. In addition, soft landing has enabled investigation of the size-dependent behavior of bare metal clusters in the critical subnanometer size regime where chemical and physical properties do not scale predictably with size. The morphology, aggregation, and immobilization of larger bare metal nanoparticles, which are directly relevant to the design of catalysts as well as improved memory and electronic devices, have also been studied using ion soft landing. This review article begins in section 1 with a brief introduction to the existing applications of ion soft- and reactive landing. Section 2 provides an overview of the ionization sources and mass filters that have been used to date for soft landing of mass-selected ions. A discussion of the competing processes that occur during ion deposition as well as the types of ions and surfaces that have been investigated follows in section 3. Section 4 discusses the physical phenomena that occur during and after ion soft landing, including retention and reduction of ionic charge along with factors that impact the efficiency of ion deposition. The influence of soft landing on the secondary structure and biological activity of complex ions is addressed in section 5. Lastly, an overview of the structure and mobility as well as the catalytic, optical, magnetic, and redox properties of bare ionic clusters and nanoparticles deposited onto surfaces is presented in section 6. © 2015 Wiley Periodicals, Inc. Mass Spec Rev 35:439–479, 2016.
Johnson, Grant E.↗
Synthesis of magnesiowüstite nanocrystallites embedded in an amorphous silicate matrix via low energy multiple ion implantations
The synthesis process is presented for experimentally simulating modifications in cosmic dust grains using sequential ion implantations or irradiations followed by thermal annealing. Cosmic silicate dust analogues were prepared via implantation of 20–80 keV Fe - , Mg - , and O - ions into commercially available p-type silicon (100)wafers. The as-implanted analogues are amorphous with a Mg/(Fe+Mg) ratio of 0.5 tailored to match theoretical abundances in circumstellar dusts. Before the ion implantations were performed, Monte-Carlo-based ion-solid interaction codes were used to model the dynamic redistribution of the implanted atoms in the silicon substrate. 600 keV helium ion irradiation was performed on one of the samples before thermal annealing. Two samples were thermally annealed at a temperature appropriate for an M-class stellar wind, 1000 K, for 8.3 h in a vacuum chamber with a pressure of 1 x 10 -7 torr. The elemental depth profiles were extracted utilizing Rutherford Backscattering Spectrometry (RBS) in the samples before and after thermal annealing. X-ray diffraction (XRD)analysis was employed for the identification of various phases in crystalline minerals in the annealed analogues. Transmission electron microscopy (TEM) analysis was utilized to identify specific crystal structures. RBS analysis shows redistribution of the implanted Fe, Mg, and O after thermal annealing due to incorporation into the crystal structures for each sample type. XRD patterns along with TEM analysis showed nanocrystalline Mg and Fe oxides with possible incorporation of additional silicate minerals.
79 ASTRONOMY AND ASTROPHYSICS↗
Modification of Z0 leptonic invariant mass in ultrarelativistic heavy ion collisions as a measure of the electromagnetic field
Not Available
72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
A simple model for jet quenching in Heavy Ion Physics
This is a simple python code to calculate jet quenching for nuclear modification factors in relativistic heavy-ion collisions. This code can be used to generate all results specified in RR0010127, to be submitted to Physical Review C.
Soltz, Ron↗
Observation of nuclear modification of energy-energy correlators inside jets in heavy ion collisions
Energy-energy correlators are constructed by averaging the number of charged particle pairs within jets, weighted by the product of their transverse momenta, as a function of the angular separation of the particles within a pair. They are sensitive to a multitude of perturbative and nonperturbative quantum chromodynamics phenomena in high-energy particle collisions. Using lead-lead data recorded with the CMS detector, energy-energy correlators inside high transverse momentum jets are measured in heavy ion collisions for the first time. The data are obtained at a nucleon-nucleon center-of-mass energy of 5.02 TeV and correspond to an integrated luminosity of 1.70 nb −1 . A similar analysis is done for proton-proton collisions at the same center-of-mass energy to establish a reference. The ratio of lead-lead to proton-proton energy-energy correlators reveals significant jet substructure modifications in the quark-gluon plasma. The results are compared to different models that incorporate either color coherence or medium response effects, where the two effects predict similar substructure modifications.
72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
Jet charge modification in dense QCD matter
In these proceedings we report a recent calculation of the jet charge modification in heavy-ion relative to proton collisions at the LHC. Jets have played an essential role in constraining theories of in-medium parton shower evolution and in determining the properties of the quark-gluon plasma created in ultra-relativistic nuclear reactions. It is important to extend these studies to flavor-tagged jets and explore observables that are sensitive to their partonic origin. The average jet charge, introduced early on in the history of quantum chromodynamics, is a proxy for the electric charge of the quark or gluon that initiates the jet. In the framework of soft-collinear effective theory, we show how to evaluate the jet charge in a dense strongly-interacting matter environments. We identify observables that can isolate the contribution of in-medium branching from isospin effects and present predictions for the transverse momentum dependence of the jet charge distribution in nucleus-nucleus collisions and its modification relative to the proton case.
72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗