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At least 397 records · Page 22

Progress toward picosecond on-chip magnetic memory

Here, we offer a perspective on the prospects of ultrafast spintronics and opto-magnetism as a pathway to high-performance, energy-efficient, and non-volatile embedded memory in digital integrated circuit applications. Conventional spintronic devices, such as spin-transfer-torque magnetic-resistive random-access memory (STT-MRAM) and spin–orbit torque MRAM, are promising due to their non-volatility, energy-efficiency, and high endurance. STT-MRAMs are now entering into the commercial market; however, they are limited in write speed to the nanosecond timescale. Improvement in the write speed of spintronic devices can significantly increase their usefulness as viable alternatives to the existing CMOS-based devices. In this article, we discuss recent studies that advance the field of ultrafast spintronics and opto-magnetism. An optimized ferromagnet–ferrimagnet exchange-coupled magnetic stack, which can serve as the free layer of a magnetic tunnel junction (MTJ), can be optically switched in as fast as ~3 ps. Integration of ultrafast magnetic switching of a similar stack into an MTJ device has enabled electrical readout of the switched state using a relatively larger tunneling magnetoresistance ratio. Purely electronic ultrafast spin–orbit torque induced switching of a ferromagnet has been demonstrated using ~6 ps long charge current pulses. We conclude our Perspective by discussing some of the challenges that remain to be addressed to accelerate ultrafast spintronics technologies toward practical implementation in high-performance digital information processing systems.

42 ENGINEERING↗

Observation of breakdown wave mechanism in avalanche ionization produced atmospheric plasma generated by a picosecond CO 2 laser

Understanding the formation and long-timescale evolution of atmospheric plasmas produced by ultrashort, long-wavelength infrared (LWIR) pulses is an important but partially understood problem. Of particular interest are plasmas produced in air with a peak laser intensity ~10 12 W/cm 2 , the so-called clamping intensity observed in LWIR atmospheric guiding experiments where tunneling and multi-photon ionization operative at near-IR or shorter wavelengths are inoperative. We find that avalanche breakdown on the surface of aerosol (dust) particles can act to seed the breakdown of air observed above the 200 GW/cm 2 threshold when a train of 3 ps 10.6 μm laser pulses separated by 18 ps is used. The breakdown first appears at the best focus but propagates backward toward the focusing optic as the plasma density approaches critical density and makes forward propagation impossible. The velocity of the backward propagating breakdown can be as high as 10 9 cm/s, an order of magnitude greater than measured with ns pulse-produced breakdown, and can be explained rather well by the so-called breakdown wave mechanism. Transverse plasma expansion with a similar velocity is assisted by UV photoionization and is observed as a secondary longitudinal breakdown mechanism in roughly 10% of the shots. When a cm-size, TW power beam is propagated, interception of aerosol particles is guaranteed and several (40 cm -3 ) breakdown sites appear, each initially producing a near-critical density plasma. On a 10 ns–1 μs timescale, shockwaves from each site expand radially and coalesce to produce a large hot gas channel. The radial velocity of the expansion agrees well with the prediction of the blast wave theory developed for ultrafast atmospheric detonations.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Constraining time-dependent ion temperature measurements in inertial confinement fusion (ICF) implosions with an intermediate distance neutron time-of-flight (nToF) detector

A concept for using an intermediate distance (0.3–3.0 m) neutron time-of-flight (nToF) to provide a constraint on the measurement of the time-dependence of ion temperature in inertial confinement fusion implosions is presented. Simulated nToF signals at different distances are generated and, with a priori knowledge of the burn-averaged quantities and burn history, analyzed to determine requirements for a future detector. Results indicate a signal-to-noise ratio >50 and time resolution <20 ps to constrain the ion temperature gradient to ∼±25% (0.5 keV/100 ps).

Moore, A. S. (ORCID:0000000221258882)↗

Tracking structural solvent reorganization and recombination dynamics following e – photoabstraction from aqueous I – with femtosecond x-ray spectroscopy and scattering

Here we present a sub-picosecond resolved investigation of the structural solvent reorganization and geminate recombination dynamics following 400 nm two-photon excitation and photodetachment of a valence p electron from the aqueous atomic solute, I–(aq). The measurements utilized time-resolved X-ray Absorption Near Edge Structure (TR-XANES) spectroscopy and X-ray Solution Scattering (TR-XSS) at the Linac Coherent Light Source x-ray free electron laser in a laser pump/x-ray probe experiment. The XANES measurements around the L 1 -edge of the generated nascent iodine atoms (I 0 ) yield an average electron ejection distance from the iodine parent of 7.4 ± 1.5 Å with an excitation yield of about 1/3 of the 0.1M NaI aqueous solution. The kinetic traces of the XANES measurement are in agreement with a purely diffusion-driven geminate iodine–electron recombination model without the need for a long-lived (I 0 :e–) contact pair. Nonequilibrium classical molecular dynamics simulations indicate a delayed response of the caging H 2 O solvent shell and this is supported by the structural analysis of the XSS data: We identify a two-step process exhibiting a 0.1 ps delayed solvent shell reorganization time within the tight H-bond network and a 0.3 ps time constant for the mean iodine–oxygen distance changes. The results indicate that most of the reorganization can be explained classically by a transition from a hydrophilic cavity with a well-ordered first solvation shell (hydrogens pointing toward I–) to an expanded cavity around I 0 with a more random orientation of the H 2 O molecules in a broadened first solvation shell.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Investigation of the significance of excited species in wave-heated dense non-ideal microplasmas using particle-in-cell Monte Carlo-collision modeling

A computational model for the interaction of a high-pressure microplasma with an electromagnetic wave is presented. A one-dimensional particle-in-cell Monte Carlo collision model is used to investigate the plasma non-ideality effects in a second-stage laser-heated xenon plasma with a comprehensive chemistry mechanism, including excited species. A xenon microplasma at a temperature of 300 K and pressure of 10 bar becomes non-ideal after the laser heating stage with lower ionization and electronic excitation barriers, which makes the presence of excited species important to the plasma generation process. For these conditions, two-step ionization via excited species becomes a major contributor to plasma ionization. We find that full ionization of the plasma is obtained in ~2 ps when excited species are included in the chemistry model, as opposed to ~2.5 ps for a chemistry mechanism that does not consider their effect. With excited species, the ionization mode transitions from direct ionization via electron-neutral collisions to direct and stepwise ionization as the plasma generation progresses.

36 MATERIALS SCIENCE↗

Effect of Mg doping on carrier recombination in GaN

Time-resolved photoluminescence measurements have been performed on Mg-doped GaN for Mg concentrations in the low- to mid-10 19 cm -3 . As-grown and annealed (600–675 °C) samples were studied. In the as-grown samples, the nonradiative carrier lifetime was found to be about 200 ps and nearly independent of the Mg concentration. Upon annealing, the carrier lifetimes shorten to ~150 ps but, again, show little dependence on the annealing temperature. The analysis of possible Shockley–Read–Hall recombination centers and their behavior during doping and annealing suggests that the main nonradiative recombination center is the Mg–nitrogen vacancy complex. The weak dependence of the PL decay times on temperature indicates that carrier capture into this center has a very low potential barrier, and the nonradiative recombination dominates even at low temperatures.

36 MATERIALS SCIENCE↗

Observation of laser ablation of silicon as a function of pulse length at constant fluence via time-resolved x-ray spectroscopy

We investigate the ablation of silicon as a function of laser pulse length at a constant fluence using time-resolved x-ray spectroscopy data obtained from OMEGA EP experiments at the University of Rochester's Laboratory for Laser Energetics. Our targets consisted of three-layer planar structures composed of Si (50 μm), Cu (25 μm), and SiO 2 (500 μm) layers. The Si layer was irradiated by a 351-nm laser with varying pulse widths of 250 ps, 500 ps, 1 ns, and 10 ns while maintaining a constant fluence of ~27.9 kJ/cm 2 . Electron temperatures and densities of the ablated plasma were determined by analyzing the time-resolved x-ray spectroscopy data through a comparison of experimental measurements with synthetic results obtained from Si atomic calculations in a steady state and non-local thermodynamic equilibrium. These calculations were computed using PrismSPECT. Additionally, radiation-hydrodynamics simulations with FLASH are used to generate simulated plasma-density and plasma-temperature profiles, which are then compared with the experimental measurements. Our analyses reveal that increasing the laser pulse length at a constant fluence results in a decrease in electron temperatures and densities. Furthermore, the longer pulses with lower intensities lead to deeper ablation regions before reaching the peak ablation but lower ionization balances in the silicon layer. Furthermore, these findings emphasize the critical role of laser pulse length in plasma ablation and shock generation for laser-impulse studies.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Reactivity of radiolytically and photochemically generated tertiary amine radicals towards a CO 2 reduction catalyst

Homogeneous solar fuels photocatalytic systems often require several additives in solution with the catalyst to operate, such as a photosensitizer (PS), Brønsted acid/base, and a sacrificial electron donor (SED). Tertiary amines, in particular triethylamine (TEA) and triethanolamine (TEOA), are ubiquitously deployed in photocatalysis applications as SEDs and are capable of reductively quenching the PS’s excited state. Upon oxidation, TEA and TEOA form TEA •+ and TEOA •+ radical cations, respectively, which decay by proton transfer to generate redox non-innocent transient radicals, TEA • and TEOA • , respectively, with redox potentials that allow them to participate in an additional electron transfer step, thus resulting in net one-photon/two-electron donation. However, the properties of the TEA • and TEOA • radicals are not well understood, including their reducing powers and kinetics of electron transfer to catalysts. Herein, we have used both pulse radiolysis and laser flash photolysis to generate TEA • and TEOA • radicals in CH 3 CN, and combined with UV/Vis transient absorption and time-resolved mid-infrared spectroscopies, we have probed the kinetics of reduction of the well-established CO 2 reduction photocatalyst, fac-ReCl(bpy)(CO) 3 (bpy = 2,2'-bipyridine), by these radicals [k TEA• = (4.4 ± 0.3) × 10 9 M –1 s –1 and k TEOA• = (9.3 ± 0.6) × 10 7 M –1 s –1 ]. The ~50× smaller rate constant for TEOA • indicates, that in contrast to a previous assumption, TEA • is a more potent reductant than TEOA • (by ~0.2 V, as estimated using the Marcus cross relation). This knowledge will aid in the design of photocatalytic systems involving SEDs. Furthermore, we also show that TEA can be a useful radiolytic solvent radical scavenger for pulse radiolysis experiments in CH 3 CN, effectively converting unwanted oxidizing radicals into useful reducing equivalents in the form of TEA • radicals.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Interface-modulated kinetic differentials in electron and hole transfer rates as a key design principle for redox photocatalysis by Sb2VO5/QD heterostructures

The efficient conversion of solar energy to chemical energy represents a critical bottleneck to the energy transition. Photocatalytic splitting of water to generate solar fuels is a promising solution. Semiconductor quantum dots (QDs) are prime candidates for light-harvesting components of photocatalytic heterostructures, given their size-dependent photophysical properties and band-edge energies. A promising series of heterostructured photocatalysts interface QDs with transition-metal oxides which embed midgap electronic states derived from the stereochemically active electron lone pairs of p-block cations. Here, we examine the thermodynamic driving forces and dynamics of charge separation in Sb2VO5/CdSe QD heterostructures, wherein a high density of Sb 5s2-derived midgap states are prospective acceptors for photogenerated holes. Hard-x-ray valence band photoemission spectroscopy measurements of Sb2VO5/CdSe QD heterostructures were used to deduce thermodynamic driving forces for charge separation. Interfacial charge transfer dynamics in the heterostructures were examined as a function of the mode of interfacial connectivity, contrasting heterostructures with direct interfaces assembled by successive ion layer adsorption and reaction (SILAR) and interfaces comprising molecular bridges assembled by linker-assisted assembly (LAA). Transient absorption spectroscopy measurements indicate ultrafast (<2 ps) electron and hole transfer in SILAR-derived heterostructures, whereas LAA-derived heterostructures show orders of magnitude differentials in the kinetics of hole (<100 ps) and electron (∼1 ns) transfer. The interface-modulated kinetic differentials in electron and hole transfer rates underpin the more effective charge separation, reduced charge recombination, and greater photocatalytic efficiency observed for the LAA-derived Sb2VO5/CdSe QD heterostructures.

Chemistry↗

Formation of the oxyl’s potential energy surface by the spectral kinetics of a vibrational mode

One of the most reactive intermediates for oxidative reactions is the oxyl radical, an electron-deficient oxygen atom. The discovery of a new vibration upon photoexcitation of the oxygen evolution catalysis detected the oxyl radical at the SrTiO3 surface. The vibration was assigned to a motion of the sub-surface oxygen underneath the titanium oxyl (Ti–O●−) created upon hole transfer to (or electron extraction from) a hydroxylated surface site. Evidence for such an interfacial mode is derived from its spectral shape, which exhibited a Fano resonance—a coupling of a sharp normal mode to continuum excitations. Here, this Fano resonance is utilized to derive precise formation kinetics of the oxyl radical and its associated potential energy surface (PES). From the Fano lineshape, the formation kinetics are obtained from the anti-resonance (the kinetics of the coupling factor), the resonance (the kinetics of the coupled continuum excitations), and the frequency integrated spectrum (the kinetics of the normal mode’s cross-section). All three perspectives yield logistic function growth with a half-rise of 2.3 ± 0.3 ps and a time constant of 0.48 ± 0.09 ps. A non-equilibrium transient associated with photoexcitation is separated from the rise of the equilibrated PES. The logistic function characterizes the oxyl coverage at the very initial stages (t ∼ 0) to have an exponential growth rate that quickly decreases toward zero as a limiting coverage is reached. Such time-dependent reaction kinetics identify a dynamic activation barrier associated with the formation of a PES and quantify it for oxyl radical coverage.

Chemistry↗

Inferring fusion nuclear burnwidths with low gain photomultiplier impulse response functions

When an inertial confinement fusion implosion is compressed, it maintains thermonuclear density and temperatures for a very short time scale, about 100 ps. The Gamma Reaction History diagnostic measures the time evolution of the fusion burn, but its temporal resolution is limited by the use of a photomultiplier tube (PMT) to amplify the photon signal. Multichannel plate-based PMTs have a fast (~120 ps) full-width at half-max impulse response function (IRF), but the time scale is similar to the incoming physics signal. An analysis routine is used to remove the effect of the PMT IRF and infer the incident fusion burnwidth. With the National Ignition Facility achieving ignition and creating much brighter signals, the PMTs are run at gains three orders of magnitude lower than nominal operation. Calibration at these settings shows the PMT IRFs get ~15% wider. Taking the gain-dependent IRF can affect the inferred nuclear burnwidths by up to ~15%.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Toward an integrated multi-gigahertz ionizing particle diagnostic

Needs arising at both current and future accelerator facilities call for the development of radiation-hardened position-sensing diagnostics that can operate with multi-GHz repetition rates. Such instruments are likely to also have applications in the diagnosis of rapid plasma behavior. Here, building on the recent work of our Advanced Accelerator Diagnostics Collaboration, we are exploring the development of integrated multi-GHz ionizing particle detection systems based on chemical-vapor deposition diamond sensors, with the initial goal of producing a quadrant detector that can determine the intensity and centroid position of a particle beam at a repetition rate between 5 and 10 GHz. Results from our initial high-speed characterization work are presented, including those from a single-channel sensor with a GHz response. Approaches to achieving multi-GHz (5–10 GHz) rate capability, including the design of a dedicated Application Specific Integrated Circuit and the use of 3D RF-solver computer aided design software, are presented and discussed in more detail. 3D RF simulations suggest clean pulses of duration less than 250 ps (FWHM less than 125 ps) can be achieved with the approaches developed by this work.

43 PARTICLE ACCELERATORS↗

A novel high frequency, high bandwidth, three phase Mach–Zehnder optical data link

In inertial confinement fusion, hydrogen isotopes are fused together under high pressures and temperatures. Typically, the duration of these experiments is incredibly short, on the order of around 60–150 ps. Due to the high radiation environment, a detector’s signal is typically data linked far distances to a protected location. The diagnostic challenge for fusion reaction history measurements is to measure signals of interest maximizing dynamic range while also maintaining time resolution on the order of 10 ps. In this work, we present a new experimental optical data link used to efficiently transport diagnostic signals over great distances to the recording system while not restricting the dynamic range. The concept of a three phase Mach–Zehnder modulator system is introduced as well as a description of the physical prototype. The initial results from testing at the OMEGA facility show that this system is a viable method for signal transportation.

47 OTHER INSTRUMENTATION↗

Efficient generation and extreme compression of multidimensional solitary states in molecular gas-filled hollow-core fibers driven by picosecond Yb lasers

We present an in-depth study on the impact of spatiotemporal Raman enhancement in molecular gas-filled hollow-core fibers (HCFs), demonstrating the efficient generation and post-compression of multidimensional solitary states (MDSS). Through different experimental scenarios—employing large-core HCFs filled with molecular gases (N 2 and N 2 O) and driven by high energy, sub-picosecond and picosecond Fourier transform-limited ytterbium laser pulses—this work leverages multimode propagation and enhanced spatiotemporal interactions to achieve significant spectral broadening and asymmetric redshift, contrasting sharply with self-phase modulation. Our findings reveal that, beyond the regime of maximum nonadiabatic molecular alignment, spatiotemporal nonlinear enhancement primarily governs spectral broadening for input pulse durations up to 1 ps. The process shows limited sensitivity to input pulse duration and the two investigated molecular gases (N 2 and N 2 O), with only subtle differences in broadening arising from their distinct Raman spectroscopic properties. Furthermore, post-compression of MDSS was achieved in various cases. Notably, using 7 mJ, 1 ps laser pulses, we generated 22 fs pulses with a 47% energy conversion efficiency of the input pulse energy. These results position MDSS as a powerful platform for generating high-energy, ultrashort pulses with tunable wavelengths, offering a robust solution for applications such as high harmonic generation.

47 OTHER INSTRUMENTATION↗

Resolving discrepancies in bang-time predictions for indirect-drive ICF experiments on the NIF: Insights from the Build-A-Hohlraum campaign

This study investigated discrepancies between measured and simulated x-ray drive in Indirect-Drive Inertial Confinement Fusion (ID-ICF) hohlraums at the National Ignition Facility. Despite advances in radiation-hydrodynamic simulations, a consistent “drive deficit” remains. Experimentally measured ID-ICF capsule bang-times are systematically 400–700 ps later than simulations predict. The Build-A-Hohlraum (BAH) campaign explored potential causes for this discrepancy by systematically varying hohlraum features, including laser entrance hole (LEH) windows, capsules, and gas fills. Overall, the agreement between simulated and experimental x-ray drive was found to be largely unaffected by these changes. The data allow us to exclude some hypotheses put forward to potentially explain the discrepancy. Errors in the local thermodynamic equilibrium (LTE) atomic modeling, errors in the modeling of LEH closure, and errors due to a lack of plasma species mix physics in simulations are shown to be inconsistent with our measurements. Instead, the data support the hypothesis that errors in NLTE emission modeling are a significant contributor to the discrepancy. X-ray emission in the 2–4 keV range is found to be approximately 30% lower than in simulations. This is accompanied by higher than predicted electron temperatures in the gold bubble region, pointing to errors in non-LTE modeling. Introducing an opacity multiplier of 0.87 on energy groups above 1.8 keV improves agreement with experimental data, reducing the bang-time discrepancy from 300 to 100 ps. These results underscore the need for refined NLTE opacity models to enhance the predictive power of hohlraum simulations.

Band emission↗

Multiframe X-ray diffraction on the OMEGA EP laser

A method of measuring multiple temporally resolved powder x-ray diffraction measurements during a single dynamic compression laser experiment has been demonstrated on the OMEGA EP laser. Up to four time-gated snapshots of the x-ray diffraction pattern are collected on an ultrafast x-ray framing camera with a 2θ scattering angle coverage of 48°–65° and 400-ps temporal resolution with the potential for 10°–160° and 200-ps resolution. X-ray diffraction snapshots capture the transformation to a high-pressure β phase in ramp-compressed Zr, constraining the atomic structure and pressure–density equation-of-state in a single shot. Here, this platform will be used to constrain transition pressures, understand the role of kinetics, and verify the existence of hysteresis and metastability on phase transformations at the lattice level under single-shot dynamic compression.

47 OTHER INSTRUMENTATION↗

Ytterbium laser system for studying parametric amplification of femtosecond pulses with a centre wavelength of ∼2 μm

A laser system is developed with an optical synchronisation of a femtosecond signal with a pump channel. The signal of a driving ytterbium fibre laser with a 60 MHz repetition rate of stretched femtosecond pulses is amplified in energy from several nanojoules to 0.4 mJ at a pulse repetition rate of 3 kHz in a wideband amplifier and then is compressed in time to 250 fs. The obtained radiation is used for generating femtosecond laser pulses with a centre wavelength of ∼2 μm, pulse energy of above 20 μJ, duration of several field oscillations, and phase stabilisation between the electromagnetic field and envelope. The other pulse of the driving fibre laser provides optical synchronisation and a minimal time delay and is directed to a regenerative Yb : YAG disk amplifier for amplification to an energy of 4 mJ at a pulse repetition rate of 3 kHz and duration of 20 ps. A multipass disk amplifier is developed for further increasing the energy of pump chirped pulses to an energy of 70 mJ at a pulse repetition rate of 10 Hz and duration of 400 ps for studying parametric amplification under sub-nanosecond pumping. (paper)

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Untangling the sequence of events during the S 2 → S 3 transition in photosystem II and implications for the water oxidation mechanism

In oxygenic photosynthesis, light-driven oxidation of water to molecular oxygen is carried out by the oxygen-evolving complex (OEC) in photosystem II (PS II). Recently, we reported the room-temperature structures of PS II in the four (semi)stable S-states, S 1 , S 2 , S 3 , and S 0 , showing that a water molecule is inserted during the S 2 → S 3 transition, as a new bridging O(H)-ligand between Mn1 and Ca. To understand the sequence of events leading to the formation of this last stable intermediate state before O 2 formation, we recorded diffraction and Mn X-ray emission spectroscopy (XES) data at several time points during the S 2 → S 3 transition. At the electron acceptor site, changes due to the two-electron redox chemistry at the quinones, Q A and Q B , are observed. At the donor site, tyrosine Y Z and His190 H-bonded to it move by 50 µs after the second flash, and Glu189 moves away from Ca. This is followed by Mn1 and Mn4 moving apart, and the insertion of O X (H) at the open coordination site of Mn1. This water, possibly a ligand of Ca, could be supplied via a “water wheel”-like arrangement of five waters next to the OEC that is connected by a large channel to the bulk solvent. XES spectra show that Mn oxidation (τ of ∼350 µs) during the S 2 → S 3 transition mirrors the appearance of O X electron density. This indicates that the oxidation state change and the insertion of water as a bridging atom between Mn1 and Ca are highly correlated.

59 BASIC BIOLOGICAL SCIENCES↗