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At least 1,423 records · Page 79

Structures of the intermediates of Kok’s photosynthetic water oxidation clock

Inspired by the period-four oscillation in flash-induced oxygen evolution of photosystem II discovered by Joliot in 1969, Kok performed additional experiments and proposed a five-state kinetic model for photosynthetic oxygen evolution, known as Kok’s S-state clock or cycle. The model comprises four (meta)stable intermediates (S 0 , S 1 , S 2 and S 3 ) and one transient S 4 state, which precedes dioxygen formation occurring in a concerted reaction from two water-derived oxygens bound at an oxo-bridged tetra manganese calcium (Mn 4 CaO 5 ) cluster in the oxygen-evolving complex. This reaction is coupled to the two-step reduction and protonation of the mobile plastoquinone QB at the acceptor side of PSII. Here in this paper, using serial femtosecond X-ray crystallography and simultaneous X-ray emission spectroscopy with multi-flash visible laser excitation at room temperature, we visualize all (meta)stable states of Kok’s cycle as high-resolution structures (2.04–2.08 Å). In addition, we report structures of two transient states at 150 and 400 µs, revealing notable structural changes including the binding of one additional ‘water’, Ox, during the S 2 →S 3 state transition. Our results suggest that one water ligand to calcium (W3) is directly involved in substrate delivery. The binding of the additional oxygen Ox in the S 3 state between Ca and Mn1 supports O–O bond formation mechanisms involving O5 as one substrate, where Ox is either the other substrate oxygen or is perfectly positioned to refill the O5 position during O 2 release. Thus, our results exclude peroxo-bond formation in the S 3 state, and the nucleophilic attack of W3 onto W2 is unlikely.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

A new platform for ultra-high dose rate radiobiological research using the BELLA PW laser proton beamline

Abstract Radiotherapy is the current standard of care for more than 50% of all cancer patients. Improvements in radiotherapy (RT) technology have increased tumor targeting and normal tissue sparing. Radiations at ultra-high dose rates required for FLASH-RT effects have sparked interest in potentially providing additional differential therapeutic benefits. We present a new experimental platform that is the first one to deliver petawatt laser-driven proton pulses of 2 MeV energy at 0.2 Hz repetition rate by means of a compact, tunable active plasma lens beamline to biological samples. Cell monolayers grown over a 10 mm diameter field were exposed to clinically relevant proton doses ranging from 7 to 35 Gy at ultra-high instantaneous dose rates of 10 7 Gy/s. Dose-dependent cell survival measurements of human normal and tumor cells exposed to LD protons showed significantly higher cell survival of normal-cells compared to tumor-cells for total doses of 7 Gy and higher, which was not observed to the same extent for X-ray reference irradiations at clinical dose rates. These findings provide preliminary evidence that compact LD proton sources enable a new and promising platform for investigating the physical, chemical and biological mechanisms underlying the FLASH effect.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Triple-{alpha} reaction rate constrained by stellar evolution models

We investigate the quantitative constraint on the triple-{alpha} reaction rate based on stellar evolution theory, motivated by the recent significant revision of the rate proposed by nuclear physics calculations. Targeted stellar models were computed in order to investigate the impact of that rate in the mass range of 0.8{<=}M/M{sub Circled-Dot-Operator }{<=}25 and in the metallicity range between Z= 0 and Z= 0.02. The revised rate has a significant impact on the evolution of low-and intermediate-mass stars, while its influence on the evolution of massive stars (M > 10M{sub Circled-Dot-Operator }) is minimal. We find that employing the revised rate suppresses helium shell flashes on AGB phase for stars in the initial mass range 0.8{<=}M/M{sub Circled-Dot-Operator }{<=}6, which is contradictory to what is observed. The absence of helium shell flashes is due to the weak temperature dependence of the revised triple-{alpha} reaction cross section at the temperature involved. In our models, it is suggested that the temperature dependence of the cross section should have at least {nu} > 10 at T = 1-1.2 Multiplication-Sign 10{sup 8}K where the cross section is proportional to T{sup {nu}}. We also derive the helium ignition curve to estimate the maximum cross section to retain the low-mass first red giants. The semi-analytically derived ignition curves suggest that the reaction rate should be less than {approx} 10{sup -29} cm{sup 6} s{sup -1} mole{sup -2} at Almost-Equal-To 10{sup 7.8} K, which corresponds to about three orders of magnitude larger than that of the NACRE compilation.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Photothermally activated motion and ignition using aluminum nanoparticles

The aluminum nanoparticles (Al NPs) are demonstrated to serve as active photothermal media, to enhance and control local photothermal energy deposition via the photothermal effect activated by localized surface plasmon resonance (LSPR) and amplified by Al NPs oxidation. The activation source is a 2-AA-battery-powered xenon flash lamp. The extent of the photothermally activated movement of Al NPs can be {approx}6 mm. Ignition delay can be {approx}0.1 ms. Both scanning electron microscopy and energy-dispersive X-ray spectroscopy measurements of motion-only and after-ignition products confirm significant Al oxidation occurs through sintering and bursting after the flash exposure. Simulations suggest local heat generation is enhanced by LSPR. The positive-feedback effects from the local heat generation amplified by Al oxidation produce a large increase in local temperature and pressure, which enhances movement and accelerates ignition.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Generation of cavitation luminescence by laser-induced exothermic chemical reaction

Absorption of high power laser radiation by aqueous carbon suspensions is known to result in the formation of highly compressed bubbles of hydrogen and carbon monoxide through the endothermic carbon-steam reaction. The bubbles expand rapidly, overreaching their equilibrium diameter, and then collapse tens to hundreds of microseconds after formation to give a flash of radiation. Here we report on the effects of laser-initiated exothermic chemical reaction on cavitation luminescence. Experiments with hydrogen peroxide added to colloidal carbon suspensions show that both the time of the light flash following the laser pulse and the intensity of luminescence increase with hydrogen peroxide concentration, indicating that large, highly energetic gas bubbles are produced. Additional experiments with colloidal carbon suspensions show the effects of high pressure on the luminescent intensity and its time of appearance following firing of the laser.

36 MATERIALS SCIENCE↗

Stellar evolution and the triple-α reactions

Nuclear reaction rates play a crucial role in the evolution of stars. For low-mass stars, the triple-α reaction controls the helium burning stars in the red giant and asymptotic giant branch (AGB) phase. More importantly, the cross section of the triple-α reaction has a great impact on the helium ignition at the center of the electron degenerate helium core of red giants and on the helium shell flashes of AGB stars. It is to be noted that stellar evolution models are influenced not only by the value of the cross section, but also by the temperature dependence of the reaction rate. In this paper, I present the impact of the triple-α reaction rates on the evolution of low-mass metal-free stars and intermediate-mass AGB stars. According to the previous study, the constraint on the triple-α reaction rate is derived based on stellar evolution theory. It is found that the recent revisions of the rate proposed by nuclear physics calculations satisfy the condition for the ignition of the helium core flash in low-mass stars.

79 ASTRONOMY AND ASTROPHYSICS↗

Pre-ignition confinement and deflagration violence in LX-10 and PBX 9501

In thermal explosions of the nitramine octahydro-1,3,5,7-tetranitro-1,3,5,7-tetrazocine (HMX)-based explosives LX-10 and PBX-9501, the pre-ignition spatial and temporal heating profile defines the ignition location. The ignition location then determines the extent of inertial confinement and the violence of the resulting deflagration. In this work, we present results of experiments in which ∼23 g cylinders of LX-10 and PBX 9501 in thin-walled aluminum confinement vessels were subjected to identical heating profiles but which presented starkly different energy release signatures. Post-explosion LX-10 containment vessels were completely fragmented, while the PBX 9501 vessels were merely ruptured. Flash x-ray radiography images show that the initiation location for the LX-10 is a few mm farther from the end caps of the vessel relative to the initiation location of PBX 9501. This difference increases deflagration confinement for LX-10 at the time of ignition and extends the pressurization time during which the deflagration front propagates in the explosive. The variation in the initiation location, in turn, is determined by the thermal boundary conditions, which differ for these two explosives because of the larger coefficient of thermal expansion and greater thermal stability of the Viton binder in LX-10 relative to the estane and bis(2,2-dinitropropyl) acetal/formal binder of the PBX 9501. The thermal profile and initiation location were modeled for LX-10 using the hydrodynamics and structures code ALE3D; results indicate temperatures in the vicinity of the ignition location in excess of 274 °C near the time of ignition. The conductive burn rates for these two explosives, as determined by flash x-ray radiography, are comparable in the range 0.1–0.2 mm/μs, somewhat faster than rates observed by strand burner experiments for explosives in the temperature range 150–180 °C and pressures up to 100 MPa. The thinnest-wall aluminum containment vessels presented here rupture at lower pressures, in the range 10 MPa, suggesting that moderately higher temperatures and pressures are present near the deflagration front. For these explosives, however the most important property for determining deflagration violence is the degree of inertial confinement.

42 ENGINEERING↗

Light desorption from an yttrium neutralizer for Rb and Fr magneto-optical trap loading

We present here the first evidence of photodesorption induced by low-intensity non-resonant light from an yttrium thin foil, which works as a neutralizer for Rb and Fr ions beam. Neutral atoms are suddenly ejected from the metal surface in a pulsed regime upon illumination with a broadband flash light and then released in the free volume of a pyrex cells. Here atoms are captured by a Magneto-Optical Trap (MOT), which is effectively loaded by the photodesorption. Loading times of the order of the flash rise time are measured. Desorption is also obtained in the continuous regime, by exploiting CW visible illumination of the metallic neutralizer surface. We demonstrate that at lower CW light intensities vacuum conditions are not perturbed by the photodesorption and hence the MOT dynamics remains unaffected, while the trap population increases thanks to the incoming desorbed atoms flux. Even with the Y foil at room temperature and hence with no trapped atoms, upon visible illumination, the number of trapped atoms reaches 10{sup 5}. The experimental data are then analyzed by means of an analytical rate equation model, which allows the analysis of this phenomenon and its dynamics and allows the determination of critical experimental parameters and the test of the procedure in the framework of radioactive Francium trapping. In this view, together with an extensive investigation of the phenomenon with {sup 85}Rb, the first demonstration of the photodesorption-aided loading of a {sup 210}Fr MOT is shown.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Effect of the light spectrum of various substrates for inkjet printed conductive structures sintered with intense pulsed light

In this work, the novel method of intense pulsed light (IPL) sintering of a nanoparticle silver ink is presented. Various patterns are printed with the Inkjet technology on two flexible foils with different light spectra. One is a clear Polyethylenterephthalat [PET] foil and the second is a light brownish Polyimide [PI] foil. The samples are flashed with different parameters regarding to pulse intensity and pulse length. Microscopic images are indicating the impact of the flashing parameters and the different light spectra of the substrates on the sintered structures. Sheet and line resistance are measured and the conductivity is calculated. A high influence of the property of the substrate with respect to light absorption and thermal conductivity on the functionality of printed conductive structures could be presented. With this new method of IPL sintering, highly conductive inkjet printed silver patterns could be manufactured within milliseconds on flexible polymeric foils without damaging the substrate.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Spectrometer for shot-to-shot photon energy characterization in the multi-bunch mode of the free electron laser at Hamburg

The setup and first results from commissioning of a fast online photon energy spectrometer for the vacuum ultraviolet free electron laser at Hamburg (FLASH) at DESY are presented. With the use of the latest advances in detector development, the presented spectrometer reaches readout frequencies up to 1 MHz. In this paper, we demonstrate the ability to record online photon energy spectra on a shot-to-shot base in the multi-bunch mode of FLASH. Clearly resolved shifts in the mean wavelength over the pulse train as well as shot-to-shot wavelength fluctuations arising from the statistical nature of the photon generating self-amplified spontaneous emission process have been observed. In addition to an online tool for beam calibration and photon diagnostics, the spectrometer enables the determination and selection of spectral data taken with a transparent experiment up front over the photon energy of every shot. This leads to higher spectral resolutions without the loss of efficiency or photon flux by using single-bunch mode or monochromators.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

High order magnetic optics for high dynamic range proton radiography at a kinetic energy of 800 MeV

Flash radiography with 800 MeV kinetic energy protons at Los Alamos National Laboratory is an important experimental tool for investigations of dynamic material behavior driven by high explosives or pulsed power. The extraction of quantitative information about density fields in a dynamic experiment from proton generated images requires a high fidelity model of the proton imaging process. It is shown that accurate calculations of the transmission through the magnetic lens system require terms beyond second order for protons far from the tune energy. The approach used integrates the correlated multiple Coulomb scattering distribution simultaneously over the collimator and the image plane. Comparison with a series of static calibration images demonstrates the model’s accurate reproduction of both the transmission and blur over a wide range of tune energies in an inverse identity lens that consists of four quadrupole electromagnets.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Design of a new turbulent dynamo experiment on the OMEGA-EP

Turbulent dynamos that exponentially amplify initially small, seed magnetic fields are crucial in magnetizing the Galaxy and beyond. Until now, the ideal environment for turbulent dynamos to grow has been difficult to recreate. In a new approach, we leverage the long pulse capability of the OMEGA-EP laser to recreate the highly conductive and inviscid (Rem∼5500, Prm≳1) growth environment of the turbulent dynamo within the magnetized plasma jet ablated from a simple cone target of CH plastic. In 3-D FLASH simulations of our scheme, we find that the ideal dynamo environment is a typically ∼1 mm3, ≳1.5 keV hot spot where the laser beams intersect to produce maximum direct heating of the jet plasma. The dynamo environment is maintained from the onset of steady flows through the ∼10 ns length of the laser pulse. For a plasma vorticity of 0.3–3.0 ns–1 and a dynamo active over ∼5 ns, the magnetic energy increases on an exponential trajectory by more than a decade. Fourier analysis reveals that the dynamo progressively saturates up to EB/EK∼20% from small scales k≳30 cm−1 to large in the time it is sustained. We find robust agreement between the evolution of magnetic energy spectra extracted from the FLASH physics simulation and that derived from synthetic sheath-accelerated proton deflectometry images, thereby demonstrating that the dynamo activity can be quantified in a real experiment.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Aerosol jet printed 3 omega sensors for thermal conductivity measurement

The 3 omega (3ω) method is a trusted technique for measuring thermal conductivity—a fundamental material property of critical importance in a broad range of applications. However, traditional 3ω sensor processing requires some form of physical vapor deposition, such as metal evaporation or sputtering. These 3ω sensor deposition techniques limit the materials and sample sizes applicable to the 3ω method. This work demonstrates an aerosol jet printing method to directly print silver 3ω sensors that yield accurate temperature-dependent measurement up to 300 °C on materials with thermal conductivity ranging from 1 to 150 W/m K. The interrelationship between printed sensor geometry, sensor thermal stability, and applicability to the 3ω method is examined. Thermal conductivity measurement with 3ω sensors conventionally sintered at 300 °C agrees to independent laser flash measurement within 4% from room temperature to 150 °C. An unconventional rapid high-temperature sintering method is shown to produce sensors that agree within 3% of the laser flash measurements from room temperature to 300 °C. The rapid sintering profiles also reduced the sensor–substrate thermal boundary resistance of the printed sensors by as much as 88%. The direct printing of 3ω sensors creates opportunities for measurement of thermal transport properties in applications previously inapplicable to the 3ω method.

47 OTHER INSTRUMENTATION↗

Deceleration-stage Rayleigh–Taylor growth in a background magnetic field studied in cylindrical and Cartesian geometries

Experiments have identified the Rayleigh–Taylor (RT) instability as one of the greatest obstacles to achieving inertial confinement fusion. Consequently, mitigation strategies to reduce RT growth and fuel–ablator mixing in the hotspot during the deceleration phase of the implosion are of great interest. In this work, the effect of seed magnetic fields on deceleration-phase RT growth are studied in planar and cylindrical geometries under conditions relevant to the National Ignition Facility (NIF) and Omega experiments. The magnetohydrodynamic (MHD) and resistive-MHD capabilities of the FLASH code are used to model imploding cylinders and planar blast-wave-driven targets. Realistic target and laser parameters are presented that suggest the occurrence of morphological differences in late-time RT evolution in the cylindrical NIF case and a measurable difference in spike height of single-mode growth in the planar NIF case. The results of this study indicate the need for target designs to utilize an RT-unstable foam–foam interface in order to achieve sufficient magnetic field amplification to alter RT evolution. Benchmarked FLASH simulations are used to study these magnetic field effects in both resistive and ideal MHD.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Thermal conductivity evaluation of ion irradiated Si 3 N 4 and ZrN ceramics using spatial domain thermoreflectance

Nitride ceramics have been investigated for different applications in the nuclear industry, such as space nuclear power, fusion reactor diagnostics and plasma heating, inert matrix fuels, and accident tolerant fuels. Although thermal conductivity remains one of the most important properties to track following irradiation, traditional techniques such as laser flash and xenon flash are limited to bulk sample characterization, which requires lengthy and cost-consuming neutron irradiation. This work used spatial domain thermoreflectance (SDTR) for the micrometer-scale measurement of thermal conductivity in 15 MeV Ni ion-irradiated silicon nitride and zirconium nitride from 1 to 50 dpa and 300 to 700 °C. Here, the SDTR-measured unirradiated thermal conductivity was found to be consistent with the published data on bulk samples. Electrically conductive ZrN exhibits modest reduction after irradiation which is minimal at the highest irradiation temperatures. In electrically insulating Si 3 N 4 , the reduction is more significant and unlike ZrN, the reduction remains significant even at a higher irradiation temperature. The thermal resistance evolution following irradiation was compared with lattice swelling, which was determined using grazing incidence x-ray diffraction, and radiation-induced defects were observed using transmission electron microscopy. A saturation value was observed between 15 and 50 dpa for thermal conductivity degradation in both nitride ceramics and a direct correlation with high-temperature defect recombination was observed, as well as the potential presence of additional carrier scattering mechanisms.

36 MATERIALS SCIENCE↗

Heat capacity of microgram oxide samples by fast scanning calorimetry

Quantitative scanning calorimetry on microgram-sized samples opens a broad, new range of opportunities for studying the thermodynamic properties of quantity-limited materials, including those produced under extreme conditions or found as rare accessory minerals in nature. We calibrated the Mettler Toledo Flash DSC 2+ calorimeter to obtain quantitative heat capacities in the range 200–350 °C, using samples weighing between 2 and 11.5 μg. Our technique is applied to a new set of oxide materials to which it has never been used before, without the need for melting, glass transitions, or phase transformations. Heat capacity data were obtained for silica in the high pressure stishovite (rutile) structure, dense post-stishovite glass, standard fused quartz, and for TiO2 rutile. These heat capacities agree within 5%–15% with the literature values reported for rutile, stishovite, and fused SiO2 glass. The heat capacity of post-stishovite glass, made by heating stishovite to 1000 °C, is a newly reported value. After accurate calibrations, measured heat capacities were then used to calculate masses for samples in the microgram range, a substantial improvement over measurement in conventional microbalances, which have uncertainties approaching 50%–100% for such small samples. Since the typical uncertainty of heat capacities measured on 10–100 mg samples in conventional differential scanning calorimetry is typically 7% (1%–5% with careful work), flash differential scanning calorimetry, using samples a factor of 1000 smaller, increases the uncertainty of heat capacity measurements by a factor of <3, opening the door for meaningful measurements on ultra-small, high-pressure samples and other quantity-limited materials.

Instruments & Instrumentation↗

Simulations of three-layer Richtmyer–Meshkov mixing in a shock tube

Here, the Richtmyer–Meshkov instability causes perturbations to grow after a shock traverses a fluid density interface. This increases the mixing rate between fluid from either side of the interface. We use the Flash Eulerian hydrodynamic code to investigate alterations when a thin third layer of intermediate density is placed along the interface, effectively creating two adjacent unstable interfaces. This is a common occurrence in engineering applications where a thin barrier initially separates two materials. We find that the width of the mixing layer is similar or slightly reduced; however, the total mass of mixed material can actually increase. The mixing layer becomes more compact and efficient. However, the normalized mixed mass decreases, meaning that finger entrainment becomes more important than in the simple two-layer case. The effect of adding the central layer appears to decrease when the Atwood number is decreased. The Flash results are also benchmarked against two-layer experimental data from a shock tube at the University of Arizona.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗