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At least 1,009 records · Page 56

Nanorod length-dependent photodriven H2 production in 1D CdS–Pt heterostructures

Colloidal quantum confined semiconductor-metal heterostructures are promising candidates for solar energy conversion because their light absorbing semiconductor and catalytic components can be independently tuned and optimized. Although the light-to-hydrogen efficiencies of such systems have shown interesting dependences on the morphologies of the semiconductor and metal domains, the mechanisms of such dependences are poorly understood. Here, we use Pt tipped 0D CdS quantum dots (with ∼4.6 nm diameter) and 1D CdS nanorods (of ∼13.8, 27.8, 66.6, and 88.9 nm average rod lengths) as a model system to study the distance-dependence of charge separation and charge recombination times and their impacts on photo-driven H2 production. The H2 generation quantum efficiency increases from 0.2% ± 0.0% in quantum dots to 28.9% ± 0.4% at a rod length of 28 nm and shows negligible changes at longer rod lengths. The half-life time of electron transfer from CdS to Pt increases monotonically with rod length, from 0.7 ± 0.1 in quantum dots to 170.2 ± 29.5 ps in the longest rods, corresponding to a slight decrease in electron transfer quantum efficiency from 92% to 81%. The amplitude-weighted average lifetime of charge recombination of the electron in Pt with the hole in CdS increases from 4.7 ± 0.4 µs in quantum dots to 149 ± 34 µs in 28 nm nanorods, and the lifetime does not increase further in longer rods, resembling the trend in the observed H2 generation quantum efficiency. Our result suggests that the competition of the charge recombination process with the hole removal by the sacrificial electron donor plays a dominant role in the observed nanorod length dependent overall light driven H2 generation quantum efficiency.

Chemistry↗

A novel integrated time-resolved array avalanche photodiode detection system for nuclear resonant scattering measurements

Here, the nuclear resonant scattering (NRS) experiment requires photon-counting detectors with high time resolution, short dead time, large dynamic range, low noise, and large detection area. An 8-channel avalanche photodiode (APD) array detector system with high integrity, flexibility, and reliability has been developed to adapt to the demands of NRS experiments. The detector system mainly consists of four key parts: (i) an array-APD sensor, (ii) 8-channel integrated fast preamplifiers, (iii) the time-to-digital converter readout electronics, and (iv) a data acquisition system and EPICS support software. Remarkably, the system exhibits a time resolution of better than 500 ps and has a sufficiently low noise level, allowing for the lowest detection energy threshold of 4 keV. The performance of the new array-APD system as well as its real application in nuclear forward scattering (NFS) and nuclear resonant inelastic x-ray scattering (NRIXS) experiments was tested in two synchrotron facilities. With the new system, the NFS signal very close to the prompt electronic scattering signal can be extracted. Thanks to the customized EPICS-areaDetector-based control software, NRIXS spectra can be readily measured with time and energy information of the NRIXS signal stored in the raw data, which is promising for developing NRIXS data analysis in the time domain. The array-APD detector can be deployed for nuclear resonant scattering experiments at various synchrotron radiation facilities.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Silicon x-ray backlighter improvement by targets with spike-like microstructures

In order to accurately probe high energy density matter states, it is vital to create powerful x-ray backlighters. One approach to create such x-ray sources is based on the usage of short-pulse, high-energy lasers, which greatly benefits from an optimization of the laser target coupling. Here, the spectral and temporal x-ray emission profiles of structured silicon targets with micron-sized spikes on the front surface are studied at laser intensities of 10 17 W cm -2 . The laser pulse length is varied between 1 and 20 ps with an energy of up to 1 kJ. The structured targets show an up to 13× enhancement of silicon He α emission compared to flat foils with a well-defined, sharp emission pulse profile. Furthermore, the performance of the microstructured targets is compared to targets with a CH shield as well as foils irradiated with a UV prepulse.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Laser material interactions in tamped materials on picosecond time scales in aluminum

Here, a 100 ps laser is used to probe the pressure generation, depth of the non-solid ablator, and the non-linear optical effects through tamper materials. Samples consisted of an aluminum ablator with tampers of sapphire and coverslip glass. In general, the sapphire tamped sample achieves higher pressures at lower laser intensities as compared to the coverslip glass tamped sample. Attempts to model the details of this set of experimental data with standard available radiation coupled hydrodynamic codes make clear that more physics is needed in these simulations to accurately predict the impact of the tamper material on the pressure generation and the depth of non-solid aluminum.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Measurement of mix at the fuel–ablator interface in indirectly driven capsule implosions on the National Ignition Facility

The interface between the capsule ablator and fuel ice layer is susceptible to hydrodynamic instabilities. The subsequent mixing of hot ablator material into the ice reduces fuel compression at stagnation and is a candidate for reduced capsule performance. The ability to diagnose ice–ablator mix is critical to understanding and improving stability at this interface. Combining the crystal backlighter imager with the single line of sight camera on the National Ignition Facility (NIF) allows direct measurement of ice–ablator mix by providing multiple quasi-monochromatic radiographs of layered capsule implosions per experiment with high spatial (∼12 μm) and temporal (∼35 ps) resolution. The narrow bandwidth of this diagnostic platform allows radiography of the inner edge of the capsule limb close to stagnation without capsule self-emission contaminating the data and removes opacity uncertainties typically associated with the spectral content of the radiograph. Analysis of radiographic data via a parameterized forward-fitting Abel inversion technique provides measurements of the distribution of mix mass inwards from the ice–ablator interface. The sensitivity of this mix measurement technique was demonstrated by applying it to layered experiments in which the stability of the ice–ablator interface was expected to vary significantly. Additional experiments suggest that high-density carbon capsules that employ a buried-layer dopant profile suffer from mixing at the innermost doped–undoped interface. Data from these experiments suggest that opacity models used in hydrodynamic simulations of NIF experiments can potentially over-predict the opacity of doped capsules. LLNL-JRNL-850535-DRAFT.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Room temperature persisting surface charge carriers driven by intense terahertz electric fields in a topological insulator Bi 2 Se 3

Topologically protected surface current is highly promising for next-generation low-dissipation and disorder-tolerant quantum electronics and computing. Yet, electric transport from the co-existing bulk state dominates the responses of the Dirac surface state, especially at elevated temperatures relevant to technological applications. Here, we present an approach that convincingly showcases the generation, disentanglement, and precise control of enduring surface charge carriers on a topological insulator, Bi 2 Se 3 , with high bulk conductivity, all achieved at room temperature. By using pump–probe modulation spectroscopy under ultrabroadband driving tunable from 4 meV to 1.55 eV, we show the terahertz (THz) field-induced surface carriers by discovering their initial temporal responses dominant over high density trivial bulk carriers. Strikingly, the response of the induced surface carrier responses persists for more than ~5 ps and is enhanced by reducing pump photon energy. The dynamics and lifetime of the distinct surface response manifest themselves as the enhanced THz pump-induced THz transmission, which directly correlates with the transient negative THz conductivity. Increasing the THz driving field reduces the induced surface carrier lifetime and identifies, particularly, an optimal pump field of E s ~ 224 kV cm -1 for generating the dominant surface response relative to the bulk. This surface carrier dominant regime is suppressed by a joint effect of enhanced surface-bulk scattering and a more rapid saturation of surface excitation compared to the bulk that sets in above E s . The controllability of room temperature topologically surface carriers through pump photon energy offer compelling possibilities for extending this approach to other topological complex materials.

36 MATERIALS SCIENCE↗

DC electrical conductivity measurements of warm dense matter using ultrafast THz radiation

We describe measurements of the DC electrical conductivity of warm dense matter using ultrafast terahertz (THz) pulses. THz fields are sufficiently slowly varying that they behave like DC fields on the timescale of electron–electron and electron–ion interactions and hence probe DC-like responses. Using a novel single-shot electro-optic sampling technique, the electrical conductivity of the laser-generated warm dense matter was determined with <1 ps temporal resolution. We present the details of the single-shot THz detection methodology as well as considerations for warm dense matter experiments. We, then, provide proof-of-concept studies on aluminum driven to the warm dense matter regime through isochoric heating and shock compression. Our results indicate a decrease in the conductivity when driven to warm dense matter conditions and provide a platform for future warm dense matter studies.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Nonlinear optical properties of lanthanum titanate glasses prepared by levitation melting

Lanthanum titanate glasses (17 La 2 O 3 -83 TiO 2 ) are fabricated via aerodynamic levitation melting. Here, nonlinear refraction and absorption were measured with the Z scan technique using ps optical pulses at 532 nm wavelength with peak intensities in the range of 0.25–2.5 GW/cm 2 . The two-photon absorption coefficient (β) and the effective nonlinear refraction coefficient (⁠$n^{eff}_{2}$) are found to be, respectively, 2.19 cm/GW and 152 × 10 -16 cm 2 /W (85 × 10 -13 esu). The Raman gain is measured to be 106 × 10 -11 cm/W. The nonlinearity strength is found to be nearly 60 times larger in lanthanum titanate glasses relative to silica.

36 MATERIALS SCIENCE↗

Review and meta-analysis of electron temperatures from high-intensity laser–solid interactions

The accelerated electron spectrum from high-intensity laser–solid interaction is often conveniently described using a Boltzmann distribution, whose temperature is known within the field as the hot-electron temperature. The importance of the electron temperature is highlighted by the sheer number of experimental and simulation studies on the subject over the past three decades. Recently, multi-kJ, multi-ps pulses have yielded electron spectra with temperatures far beyond the expected ponderomotive result. Expressions that predict the electron temperature considering laser parameters beyond intensity and wavelength have been developed, albeit using small datasets. In this review, we present what is, to the best of our knowledge, the largest dataset of electron temperatures gathered from experimental measurements and particle-in-cell simulations. This dataset allows us to compare existing analytical and empirical hot-electron temperature scaling models over a wide parameter range. We also develop new scaling models that incorporate the laser pulse duration of the laser and the plasma scale length. Three models that include pulse-duration and scale length dependence are especially successful at predicting both simulated and experimental data. The dataset will soon be made publicly available to encourage further investigation.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Iron dopant energy levels in β-Ga 2 O 3

The energetic positions of the two Fe dopant levels in the bandgap of β-Ga 2 O 3 are determined to be at 3.05(±0.05) and 3.85(±0.05) eV below the conduction band minimum from transmission measurements employing a sub-picosecond tunable ultraviolet laser radiation source. A further measurement of the quantum efficiency of photoelectron emission from the Fe:Ga 2 O 3 (010) photocathode is consistent with the obtained absorption data and a dominant optical phonon assisted Franck–Condon emission mechanism, while also providing an estimate of 100 ps for the conduction band electron lifetime.

24 POWER TRANSMISSION AND DISTRIBUTION↗

Electrical design of the flexible imaging diffraction diagnostic for laser experiments (FIDDLE) at the National Ignition Facility (NIF)—Requirements, design, and performance

The Flexible Imaging Diffraction Diagnostic for Laser Experiments (FIDDLE) is a newly developed diagnostic for imaging time resolved diffraction in experiments at the National Ignition Facility (NIF). It builds on the successes of its predecessor, the Gated Diffraction Development Diagnostic (G3D). The FIDDLE was designed to support eight Daedalus version 2 sensors (six more hCMOS sensors than any other hCMOS-based diagnostic in NIF to date) and an integrated streak camera. We will review the electrical requirements, design, and performance of the electrical subsystems that were created to support this large number of cameras in the FIDDLE. The analysis of the data that the FIDDLE is intended to collect relies heavily on the accurate and well-understood timing of each sensor. We report camera-to-camera timing jitter of less than 100 ps rms and sensor integration times of 2.2 ns FWHM in 2-2 timing mode. Additionally, diffraction experiments on the NIF produce electric fields (EMI) on the order of 1 kV/m, which have been observed to negatively impact the performance of some electrical components of the FIDDLE. We report on the results of testing hCMOS camera electronics in a similar EMI environment generated in an offline lab. In addition, we also summarize the use of a novel approach to using a vector network analyzer as an EMI leak detector to understand and reduce the negative impacts of EMI on the FIDDLE.

47 OTHER INSTRUMENTATION↗

Evidence of non-isentropic release from high residual temperatures in shocked metals measured with ultrafast x-ray diffraction

Shock experiments are widely used to understand the mechanical and electronic properties of matter under extreme conditions. However, after shock loading to a Hugoniot state, a clear description of the post-shock thermal state and its impacts on materials is still lacking. We used diffraction patterns from 100-fs x-ray pulses to investigate the temperature evolution of laser-shocked Al–Zr metal film composites at time delays ranging from 5 to 75 ns driven by a 120-ps short-pulse laser. We found significant heating of both Al and Zr after shock release, which can be attributed to heat generated by inelastic deformation. A conventional hydrodynamic model that employs (i) typical descriptions of Al and Zr mechanical strength and (ii) elevated strength responses (which might be attributed to an unknown strain rate dependence) did not fully account for the measured temperature increase, which suggests that other strength-related mechanisms (such as fine-scale void growth) could play an important role in thermal responses under shock wave loading/unloading cycles. Our results suggest that a significant portion of the total shock energy delivered by lasers becomes heat due to defect-facilitated plastic work, leaving less converted to kinetic energy. This heating effect may be common in laser-shocked experiments but has not been well acknowledged. High post-shock temperatures may induce phase transformation of materials during shock release. Another implication for the study is the preservability of magnetic records from planetary surfaces that have a shock history from frequent impact events.

42 ENGINEERING↗

Ultra-fast single-crystal CVD diamonds in the particle time-of-flight (PTOF) detector for low yield burn-history measurements on the NIF (invited)

The Particle Time of Flight (PTOF) diagnostic is a chemical vapor deposition diamond-based detector and is the only diagnostic for measuring nuclear bang times of low yield (<1013) shots on the National Ignition Facility. Recently, a comprehensive study of detector impulse responses revealed certain detectors with very fast and consistent impulse responses with a rise time of <50 ps, enabling low yield burn history measurements. At the current standoff of 50 cm, this measurement is possible with fast 14 MeV neutrons from deuterium–tritium (DT) fusion plasmas. PTOF-inferred DT burn width numbers compare well with widths inferred from the gamma reaction history diagnostic on mid-yield (1013–1015) shots, where both systems are capable of making this measurement. These new capabilities could be extended to 2.5 MeV deuterium–deuterium neutrons from D plasmas and to even lower yield by reducing the detector standoff distance to 10 cm; a design for this is also presented.

42 ENGINEERING↗

Ultrafast photoinduced charge carrier dynamics of L-cysteine and oleylamine stabilized CsPbBr3 perovskite quantum dots coupled with gold nanoparticles

We have synthesized L-cysteine and oleylamine stabilized CsPbBr3 perovskite quantum dots (PQDs) and coupled them with gold nanoparticles (AuNPs). The PQDs and AuNPs, as well as their hybrid nanostructures (HNS), were characterized using UV–visible (UV–vis) and photoluminescence (PL) spectroscopy. The UV–vis spectra show absorption bands of the HNS at 503 and 520 nm, attributed mainly to PQDs and AuNPs, respectively. The PQDs show a strong excitonic PL band peaked at 513 nm from PQDs. The HR-TEM results show the formation of hybrid structures between PQDs and AuNPs, which is also supported by the PL quenching of the PQDs by the coupled AuNPs. Ultrafast dynamics of the exciton and charge carriers in the HNS and pristine PQD were studied using femtosecond transient absorption. Multiexponential fitting of the dynamic data revealed the existence of shallow and deep trap states in pristine PQDs and ultrafast electron transfer from PQDs to AuNPs in the HNS. A kinetic model was proposed to account for the key dynamic processes involved and to extract the time for electron transfer from PQDs to AuNPs in the HNS, found to be ∼2 ps. Dynamic processes in pristine PQDs are largely unchanged by HNS formation with AuNPs.

Chemistry↗

MeV x-ray production from a petawatt laser in the regime of a relativistically transparent preplasma, with applications to radiography

Bright sources of mega-electron volt (MeV) x-rays have many unique applications, including nuclear physics, radiation oncology, and imaging high areal density systems. High intensity lasers (>1018 W cm−2) incident on mm-thick metal targets can deliver MeV x-rays via the bremsstrahlung process, providing sources with ultrashort duration (∼ps) and small source size (∼100 μm). Here, we report on a reproducible regime of laser-driven MeV x-ray sources, where the x-ray dose can be further increased by 60% by coating the metal target with micrometers of plastic. High fidelity numerical simulations indicate that the interaction is a result of relativistic transparency in the preplasma. Though relativistic transparency is present in both cases, the greater sound speed and smaller ion inertia of the plastic target allow the laser to more deeply penetrate and couple more efficiently to electrons. Radiography with this system demonstrates a resolving power < 300 μm, important for imaging applications.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Development and characterization of a laser-gated, high resolution x-ray radiography platform for high energy density experiments using toroidally bent crystals

Bent crystal x-ray imagers are a well-established diagnostic tool to study high energy density (HED) objects by acquiring two-dimensional x-ray radiographs. Often, studying these HED objects requires very high spatial resolution, which is limited by astigmatism when using spherically bent crystals. By using toroidal-shaped crystals instead, astigmatism can be reduced and the overall spatial resolution of the instrument improved. Here, the development and characterization of a laser-gated x-ray radiography platform at the National Ignition Facility using a toroidal crystal is presented. This includes measurements of the spatial and temporal profile, which is determined by the x-ray source. In conclusion, to properly validate the reduced astigmatism, a new multi-plane grid approach was implemented, which, for the first time, allows a depth of field measurement, alignment verification and x-ray source size estimate in a single shot, demonstrating the current platform’s capability to provide sub-10 μm resolution over a 0.9 mm depth of field with a temporal resolution of 110 ps.

Crystal optics↗

Iodine recombination in xenon solvent: Clusters in the gas to liquid-like state transition

Supercritical fluids (SCFs) have attracted significant attention as solvents for chemical reactions due to their unique properties, such as high diffusivity, low viscosity, and tunable solvation properties. These properties profoundly influence reaction kinetics and are often attributed to the formation of molecular clusters within SCFs. To study the effect of supercritical solvent on chemical reactivity and dynamics of reactions, one needs to understand the dynamics of clusters in supercritical fluid. Extensive experiments on the photodissociation and recombination of iodine in supercritical fluids served as a model system for understanding these effects. Experimental studies have been complemented by theoretical and computational investigations, which mostly employ Monte Carlo or empirical molecular dynamics simulations. However, computational studies using non-reactive force fields and ab initio approaches present challenges in capturing reactive processes at larger scales within supercritical fluids. Here, in this work, we developed the ReaxFF parameters by training against quantum mechanics data. ReaxFF reactive force field based molecular dynamics simulations were performed, studying the dynamics of a xenon solvent and cage effect at different thermodynamic conditions for the iodine recombination reaction. We show that the conditions near the critical point are the optimal conditions to study the cage effect. We show that the average lifetime of xenon clusters ranging between 5 and 11 ps is comparable to iodine geminate recombination. Our simulation results of iodine recombination in xenon solvent demonstrate the higher probability of iodine molecule formation in the presence of xenon clusters. Finally, we show that the supercritical condition exhibits the highest recombination rate for iodine atoms.

Cage effect↗

Increased electron, positron, and x-ray production from high intensity laser interactions using micro-wire targets

We report increases in energetic electrons, positrons, and x-rays emitted from high-intensity laser interactions (10 18−20 W/cm 2 ) with structured silicon micro-wires on the surface of a 1 mm gold converter target using a 10 ps laser pulse. A total of four different wire configurations are tested, where the gaps (7–28 μm) between the wires and the thicknesses (3–6 μm) of the wires are varied, while the height remains constant (⁠ ~25 μm). We observe the largest enhancement in electrons, positrons, and x-rays with the sparsest wire configurations. The electron temperature (T e ≈6 MeV) remains consistent across all shots, regardless of whether wires or planar targets are used. This suggests that the observed enhancement is due to increased laser light absorption by the accelerated electrons over a long scale length. Two-dimensional particle-in-cell simulations confirm that absorption is significantly enhanced with the wire target. Additionally, specific simulations examining laser pointing on different parts of the wire structure reveal that, while the final electron spectrum remains largely insensitive, the angular distribution is highly sensitive to these variations.

Bremsstrahlung↗