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At least 811 records · Page 45

Thermomechanical response of thickly tamped targets and diamond anvil cells under pulsed hard x-ray irradiation

In the laboratory study of extreme conditions of temperature and density, the exposure of matter to high intensity radiation sources has been of central importance. Here, we interrogate the performance of multi-layered targets in experiments involving high intensity, hard x-ray irradiation, motivated by the advent of extremely high brightness hard x-ray sources, such as free electron lasers and 4th-generation synchrotron facilities. Intense hard x-ray beams can deliver significant energy in targets having thick x-ray transparent layers (tampers) around samples of interest for the study of novel states of matter and materials’ dynamics. Heated-state lifetimes in such targets can approach the microsecond level, regardless of radiation pulse duration, enabling the exploration of conditions of local thermal and thermodynamic equilibrium at extreme temperature in solid density matter. The thermal and mechanical responses of such thick layered targets following x-ray heating, including hydrodynamic relaxation and heat flow on picosecond to millisecond timescales, are modeled using radiation hydrocode simulation, finite element analysis, and thermodynamic calculations. Assessing the potential for target survival over one or more exposures and resistance to damage arising from heating and resulting mechanical stresses, this study doubles as an investigation into the performance of diamond anvil high pressure cells under high x-ray fluences. Long used in conjunction with synchrotron x-ray radiation and high power optical lasers, the strong confinement afforded by such cells suggests novel applications at emerging high intensity x-ray facilities and new routes to studying thermodynamic equilibrium states of warm, very dense matter.

Meza-Galvez, J. (ORCID:000000032699849X)↗

Reshock analysis for PMMA driven above the threshold for chemical decomposition

Polymethyl methacrylate (PMMA) is a transparent thermoplastic often used in shock compression science. Previous proceedings (AIP Conf. Proc. 845, 131 (2006)) described plate impact experiments in which PMMA was reshocked to pressures of up to ~130 GPa, well above that at which it decomposes on its principal Hugoniot. Because some of the conclusions of the original analysis were surprising, the results were reanalyzed in a later proceeding (ibid. 1426, 771 (2012)). In addition to our own reanalysis of the data, we performed hydrodynamic simulations of the experiments based on a new equation of state for PMMA shocked above its threshold for decomposition.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Ultrashort XUV pulse absorption spectroscopy of partially oxidized cobalt nanoparticles

High-order harmonic generation (HHG) based transient extreme ultraviolet (XUV) absorption spectroscopy is an emerging technique to trace photoinduced charge carrier dynamics in condensed phase materials with femtosecond and even attosecond temporal resolution and elemental specificity. However, its application to nanoparticulate samples that are relevant, for example, for novel photocatalytic light harvesting concepts, has been limited. This is in part due to the challenge to produce residual-free samples on ultrathin, XUV-transparent substrates as well as a widespread understanding that sparsely distributed nanoparticles do not provide sufficient contrast for XUV absorption measurements. Here, we present static XUV absorption spectra of partially oxidized Co nanowire-structures with diameters of approximately 4.5 nm and lengths between 10 and 40 nm, recorded with an ultrashort pulse HHG light source. Nanoparticles are synthesized by the agglomeration of Co atoms inside superfluid helium droplets, followed by surface deposition and oxidation in ambient air. The method is uniquely suited for residual-free synthesis of transition metal nanowires and their deposition on ultrathin substrates. Analysis by high-resolution transmission electron microscopy reveals the formation of CoO nanowires with regions of unoxidized Co in their interior. The nanoparticle samples are investigated in an HHG-driven ultrafast XUV absorption setup. Despite the low surface coverage of only 23%, the recorded spectrum exhibits a distinct absorption feature at the Co M 2,3 (2p) edge near 60 eV with a peak height of about 40 mOD. Finally, the results support the feasibility of table-top ultrafast transient XUV absorption studies of photoinduced dynamics in transition metal oxide nanoparticles with sub-monolayer surface coverage.

74 ATOMIC AND MOLECULAR PHYSICS↗

The role of water vapor during the synthesis of hydrogen doped In 2 O 3

Hydrogen-doped In 2 O 3 synthesized using magnetron sputtering or atomic layer deposition in the presence of water vapor has high transparency in the near infra-red region and mobility values that are almost three to four times of those in commercially used In 2 O 3 :Sn at a much lower carrier concentration. However, simple questions like what happens when water molecules enter In 2 O 3 or why the dominant charge carrier changes from an oxygen vacancy in In 2 O 3 :Sn to H + in In 2 O 3 are not clear. Using hybrid functional based density functional theory calculations, in this study we show that water molecules spontaneously split into H + and OH – . The H + interstitial bonds with an oxygen in In 2 O 3 , and the OH – interstitial occupies a vacant lattice site or is trapped by an oxygen vacancy. Thus, in agreement with experimental findings, our results suggest that the concentration of oxygen vacancies decreases as the partial pressure of water increases. The charge transition level, ϵ ( – / + ) , of a hydrogen interstitial and the Fermi level at which the formation energies of OH – and H + are equal lie above the conduction band minimum, suggesting that the H + interstitial has a lower formation energy. In addition, water molecules do not exhibit any propensity to form clusters, meaning that H + ions can diffuse and remain spatially separated from each other.

36 MATERIALS SCIENCE↗

A high-pressure flow through test vessel for neutron imaging and neutron diffraction-based strain measurement of geological materials

Neutron scattering and neutron imaging have emerged as powerful methods for experimentally investigating material deformation and fluid flow in the interior of otherwise inaccessible or opaque structures. This paper describes the design and provides example uses of a pressure cell developed for investigating such behaviors within geological materials. The cell can accommodate cylindrical samples with diameters up to 38.1 mm and lengths up to 154 mm. Additionally, ports in the cell and a pressure isolating sleeve around the sample allow the independent application of confining pressure up to 69 MPa and axial pressure up to 34.5 MPa. Furthermore, two material versions of the cell have been manufactured and used to date. An aluminum version is typically used for temperatures below 40 °C, because of its relative transparency to neutrons, while a titanium version, which is comparatively more neutron attenuating, is used for experiments requiring triaxial pressurization under conditions up to 350 °C. The pressure cells were commissioned at the VULCAN engineering diffractometer at the Oak Ridge National Laboratory (ORNL), Spallation Neutron Source, and have since been used at the ORNL high flux isotope reactor CG1-D imaging beamline, National Institute of Standard and Technology (NIST) BT-2, and NIST NG6 imaging beamlines.

47 OTHER INSTRUMENTATION↗

False metals, real insulators, and degenerate gapped metals

This paper deals with a significant family of compounds predicted by simplistic electronic structure theory to be metals but are, in fact, insulators. This false metallic state has been traditionally attributed in the literature to reflect the absence of proper treatment of electron-electron correlation (“Mott insulators”) whereas, in fact, even mean-field like density functional theory describes the insulating phase correctly if the restrictions posed on the simplistic theory are avoided. Such unwarranted restrictions included different forms of disallowing symmetry breaking described in this article. As the science and technology of conductors have transitioned from studying simple elemental metals such as Al or Cu to compound conductors such as binary or ternary oxides and pnictides, a special class of degenerate but gapped metals has been noticed. Their presumed electronic configurations show the Fermi level inside the conduction band or valence band, yet there is an “internal band gap” between the principal band edges. The significance of this electronic configuration is that it might be unstable toward the formation of states inside the internal band gap when the formation of such states costs less energy than the energy gained by transferring carriers from the conduction band to these lower energy acceptor states, changing the original (false) metal to an insulator. The analogous process also exists for degenerate but gapped metals with the Fermi level inside the valence band, where the energy gain is defined by transfer of electrons from the donor level to the unoccupied part of the valence band. We focus here on the fact that numerous electronic structure methodologies have overlooked some physical factors that could stabilize the insulating alternative, predicting instead false metals that do not really exist (note that this is in general not a physical phase transition, but a correction of a previous error in theory that led to a false prediction of a metal). Such errors include: (i) ignoring spin symmetry breaking, such as disallowing magnetic spin ordering in CuBi2O4 or disallowing the formation of polymorphous spin networks in paramagnetic LaTiO 3 and YTiO 3 ; (ii) ignoring structural symmetry breaking, e.g., not enabling energy-lowering bond disproportionation (Li-doped TiO 2 , SrBiO 3 , and rare-earth nickelates), or not exploring pseudo-Jahn–Teller-like distortions in LaMnO 3 , or disallowing spontaneous formation of ordered vacancy compounds in Ba 4 As 3 and Ag 3 Al 22 O 34 ; and (iii) ignoring spin–orbit coupling forcing false metallic states in CaIrO 3 and Sr 2 IrO 4 . The distinction between false metals vs real insulators is important because (a) predicting theoretically that a given compound is metal even though it is found to be an insulator often creates the temptation to invoke high order novel physical effects (such as correlation in d-electron Mott insulators) to explain what was in effect caused by a more mundane artifact in a lower-level mean-field band theory, (b) recent prediction of exotic physical effects such as topological semimetals were unfortunately based on the above compounds that were misconstrued by theory to be metal, but are now recognized to be stable insulators not hosting exotic effects, and (c) practical technological applications based on stable degenerate but gapped metals such as transparent conductors or electrides for catalysis must rely on the systematically correct and reliable theoretical classification of metals vs insulators.

36 MATERIALS SCIENCE↗

Enhancement of the spin–orbit torque efficiency in W/Cu/CoFeB heterostructures via interface engineering

Here, the spin-torque ferromagnetic resonance signal and the spin Hall magnetoresistance induced by the spin Hall effect of W/Cu/CoFeB heterostructures with different Cu layer thicknesses (t Cu ) have been systemically studied. The effective spin mixing conductance $g^{↑↓}_{eff}$, the interfacial spin transparency T, and the real spin–orbit torque efficiency ( J s J c ) real show a significant increase compared to the W/CoFeB heterostructure. ( J s J c ) real reaches its maximum of ~0.54, increased up to ~50% at the optimized tCu ~ 0.52 nm according to our theoretical prediction. More importantly, the intrinsic spin Hall angle of W, $θ^{int}_{SH}$ ~ 0.79 ± 0.20, has also been obtained after the correction of the inverse spin Hall effect and T. This suggests that the Cu insertion improves the interface quality and, therefore, assists the spin transport in the heterostructures, which potentially improves the performance of next-generation spintronic devices.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Observation of interacting polaronic gas behavior in Ta-doped TiO 2 thin films via terahertz time-domain spectroscopy

Transparent conductive oxides (TCOs)—materials that have the twin desirable features of high optical transmission and electrical conductivity—play an increasingly significant role in the fields of photovoltaics and information technology. As an excellent TCO, Ta-doped anatase TiO 2 shows great promise for a wide range of applications. Here, terahertz time-domain spectroscopy is used to study the complex optical conductivity $\tilde{σ}$ (ω) of the TCO—heavily Ta-doped TiO 2 thin films with different Ta-doping concentrations, in the frequency range of 0.3–2.7 THz and the temperature range of 10–300 K. Fitting the complex optical conductivity to a Drude-like behavior allows us to extract the temperature dependence of the effective mass, which suggests the existence of many-body large polarons. Moreover, the carrier scattering rate of Ta-doped TiO 2 with different carrier concentrations agrees with the interacting polaron gas theory. Our results suggest that with increasing electron density in TiO 2 , the interaction between polarons is larger and electron–phonon coupling is smaller, which is beneficial for achieving high mobility and conductivity in TiO 2 .

36 MATERIALS SCIENCE↗

Drive-pressure optimization in ramp-wave compression experiments through differential evolution

Ramp-wave dynamic-compression experiments are used to examine quasi-isentropic loading paths in materials. The gradual and continuous increase in pressure created by ramp waves make these types of experiments ideal for studying nonequilibrium material behavior, such as solidification kinetics. In ramp-wave compression experiments, the input drive pressure to the experimental setup may be exerted through one of a number of different mechanisms (e.g., magnetic fields, gas-gun-driven impactors, or high-energy lasers) and is generally required for simulating such experiments. Yet, regardless of the specific mechanism, this drive pressure cannot be measured directly (measurements are generally taken at a location near the back of the experimental setup through a transparent window), leading to an inverse problem where one must determine the drive pressure at the front of the experimental setup (i.e., the input) that corresponds to the particle velocity (the output) measured near the back of the experimental setup. Furthermore, we solve this inverse problem using a heuristic optimization algorithm, known as differential evolution, coupled with a multiphysics, hydrodynamics code that simulates the compression of the experimental setup. By running many rounds of forward simulations of the experimental setup, our optimization process iteratively searches for a drive pressure that is optimized to closely reproduce the experimentally measured particle velocity near the back of the experimental setup. While our optimization methodology requires a significant number of hydrodynamics simulations to be conducted, many of these can be performed in parallel, which greatly reduces the time cost of our methodology. One novel aspect of our method for determining the drive pressure is that it does not require physical modeling of the drive mechanism and can thus be broadly applied to many types of ramp-compression experiments, regardless of the drive mechanism.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Solvent influence on non-adiabatic interfacial electron transfer at conductive oxide electrolyte interfaces

The kinetics for interfacial electron transfer (ET) from a transparent conductive oxide (tin-doped indium oxide, ITO, Sn:In 2 O 3 ) to molecular acceptors 4-[N,N-di(p-tolyl)amino]benzylphosphonic acid, TPA, and [Ru II (bpy) 2 (4,4' -(PO 3 H 2 ) 2 -bpy)] 2+ , RuP, positioned at variable distances within and beyond the electric double layer (EDL), were quantified in benzonitrile and methanol by nanosecond absorption spectroscopy as a function of the thermodynamic driving force, -ΔG ° . Relevant ET parameters such as the rate constant, k et , reorganization energy, λ, and electronic coupling, Hab, were extracted from the kinetic data. Overall, k et increased as the distance between the molecular acceptor and the conductor decreased. For redox active molecules within the Helmholtz planes of the EDL, k et was nearly independent of -ΔG° , consistent with a negligibly small λ value. Rips–Jortner analysis revealed a non-adiabatic electron transfer mechanism consistent with H ab < 1 cm -1 . The data indicate that the barrier for electron transfer is greatly diminished at the conductor–electrolyte interface.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Experiments and simulations of isochorically heated warm dense carbon foam at the Texas Petawatt Laser

An experimental and simulation study of warm dense carbon foams at ambient density (n e ~10 21 cm –3 ) is presented. This study of isochorically heated foams is motivated by their potential application in carbon-atmosphere white-dwarf envelopes, where there are modeling uncertainties due to the equation of state. The foams are heated on an approximately picosecond time scale with a laser-accelerated proton beam. The cooling and expansion of the heated foams can be modeled with appropriately initialized radiation-hydrodynamics codes; xRAGE code is used in this work. The primary experimental diagnostic is the streaked optical pyrometer, which images a narrow band of radiation from the rear surface of the heated material. Presented are xRAGE modeling results for both solid aluminum targets and carbonized resorcinol-formaldehyde foam targets, showing that the foam appears to cool slowly on the pyrometer because of partial transparency. So that simulations of cooling foam are processed properly, it is necessary to account for finite optical depth in the photosphere calculation, and the methods for performing that calculation are presented in depth.

36 MATERIALS SCIENCE↗

Polyvinyl acetate-based polymer host for optical and far-infrared spectroscopy of individualized nanoparticles

Preparation techniques for producing films of individualized solution-dispersed nanoparticles (NPs) for optical spectroscopy are frequently technically challenging and tailored for a specific NP system. In this work, we present a rapid, easy, and economical technique for producing polyvinyl acetate (PVAc)-based NP-polymer films on the order of 100’s of micrometers thick that exhibit high uniformity, low aggregation, excellent optical transparency, and low terahertz absorption. In addition, we find that these films are robust at cryogenic temperatures and have a high laser damage threshold of 0.3 TW cm –2 , which make them suitable for pulsed laser measurements. We show that free-standing, flexible, PVAc films can incorporate both one-dimensional single-wall carbon nanotubes (SWCNTs) and zero-dimensional Au NPs. Using absorbance, Raman scattering, and photoluminescence excitation spectroscopy, we observe that SWCNT individualization is maintained, and minimized polymer strain imposed, when the nanotubes are transitioned from the solution to the polymer host. This PVAc-based polymer host presents researchers with a straightforward method for producing free-standing and flexible NP films with low aggregation.

36 MATERIALS SCIENCE↗

A patterned phase-changing vanadium dioxide film stacking with VO 2 nanoparticle matrix for high performance energy-efficient smart window applications

A vanadium dioxide (VO 2 ) based solid-to-solid phased changing material has been attracting great interest in smart window applications. However, achieving high solar modulation and high transparency simultaneously in visible light is the major challenge for the practical application of this smart material. To resolve this issue, in this paper, a smart film composed of a VO 2 nanoparticle matrix and a patterned VO 2 film is presented. Furthermore, numerical modeling and electromagnetic simulation are carried out to characterize the performance in terms of solar modulation and luminous transmittance, and a parametric study is carried out to optimize the proposed smart window film. Compared with the VO 2 nanoparticle matrix, the proposed structure can obtain 23% solar modulation and 57% luminous transmittance but with a much thinner thickness, which will significantly reduce the cost and fabrication complexity and extend the environment stability.

42 ENGINEERING↗

A transmitted-beam diagnostic for the wavelength-tunable UV drive beam on OMEGA

A transmitted-beam diagnostic (P9TBD) was developed as part of a new experimental platform used to study laser–plasma interactions on OMEGA. Located in the opposing port to the wavelength-tunable (350 nm to 353 nm) UV drive beam, the P9TBD characterizes the beam after it propagates through an undersense plasma. The instrument consists of a large-aperture window that allows light to exit the target chamber and project onto a thin sheet of semi-transparent diffuser material. Light transmitted through the diffuser is recorded using a time-integrated camera and a fiber-optically coupled streaked spectrometer, providing measurements of the energy, power, fluence, polarization, and spectrum of the transmitted beam. Here, the diagnostic enables direct observation of a variety of cross-beam energy transfer phenomena, such as wavelength detuning, polarization effects, and gain saturation.

47 OTHER INSTRUMENTATION↗

One-dimensional edge contact to encapsulated MoS 2 with a superconductor

Establishing ohmic contact to van der Waals semiconductors such as MoS 2 is crucial to unlocking their full potential in next-generation electronic devices. Encapsulation of few layer MoS 2 with hBN preserves the material’s electronic properties but makes electrical contacts more challenging. Progress toward high quality edge contact to encapsulated MoS 2 has been recently reported. Here, we evaluate a contact methodology using sputtered MoRe, a type II superconductor with a relatively high critical field and temperature commonly used to induce superconductivity in graphene. We find that the contact transparency is poor and that the devices do not support a measurable supercurrent down to 3 K, which has ramifications for future fabrication recipes.

2D materials↗

Efficient and tunable blue light generation using lithium niobate nonlinear photonics

Thin-film lithium niobate (LN) has recently emerged as a playground for chip-scale nonlinear optics and leads to efficient frequency conversions from near-infrared to near-visible bands. For many nonlinear and quantum photonics applications, it is desirable to operate deep into the visible band within LN's transparency window. However, the strong material dispersion at short wavelengths makes phase-matching difficult, necessitating sub-micrometer scale control of domain structures for efficient phase-matching. Here, we report the operation of thin film LN in the blue wavelength and high fidelity poling of the thin-film LN waveguide to this regime. As a result, quasi-phase matching is realized between IR (871 nm) and blue (435.5 nm) wavelengths in a straight waveguide and prompts strong blue light generation with a conversion efficiency (1040% ± 140%/W). This blue second harmonic generator exhibits stable temperature tunability, which is important for applications that require precise frequency alignment, such as atomic clocks.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Topological field theory with Haagerup symmetry

Here, we construct a (1 + 1)d topological field theory (TFT) whose topological defect lines (TDLs) realize the transparent Haagerup $\mathscr{H}$ 3 fusion category. This TFT has six vacua, and each of the three non-invertible simple TDLs hosts three defect operators, giving rise to a total of 15 point-like operators. The TFT data, including the three-point coefficients and lasso diagrams, are determined by solving all the sphere four-point crossing equations and torus one-point modular invariance equations. We further verify that the Cardy states furnish a non-negative integer matrix representation under TDL fusion. While many of the constraints we derive are not limited to this particular TFT with six vacua, we leave open the construction of TFTs with two or four vacua. Finally, TFTs realizing the Haagerup $\mathscr{H}$ 1 and $\mathscr{H}$ 2 fusion categories can be obtained by gauging algebra objects. This article makes a modest offering in our pursuit of exotica and the quest for their eventual conformity.

97 MATHEMATICS AND COMPUTING↗

Few-cycle optical field breakdown and damage of gallium oxide and gallium nitride

Both gallium oxide and gallium nitride have great potential for use as high power transparent conducting oxide materials for a wide range of optoelectronic applications. It is, therefore, important to determine the dynamic optical field breakdown for these materials. Here, we report laser damage thresholds for Ga 2 O 3 and GaN using 9 fs few-cycle pulses with a center wavelength near 760 nm. We determine laser-induced damage thresholds (LIDTs) for both single pulse and multi-pulse exposures, with multi-pulse LIDT showing significant reduction compared to single pulse LIDT (in some cases, >50%), possibly due to laser-induced defects. We show that Ga 2 O 3 and GaN have an ultrafast optical field breakdown of 23 and 18 GV/m when nearly polarized along their [010] and [111] planes, respectively, extending their suitability for high power applications to the ultrashort pulse regime. To accurately characterize the excited carrier density criteria in which apparent laser damage occurs, carrier excitation dynamics for the entire laser pulse interaction were simulated using a modified Keldysh ionization model. For the measured single-shot threshold fluences, the plasma critical density was surpassed by 2 orders of magnitude and 2D finite-difference time-domain simulations were employed to understand the pulse interaction near the surface.

Tripepi, Michael↗