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At least 181 records · Page 10

Advanced antireflection for back-illuminated silicon photomultipliers to detect faint light

Silicon photomultipliers have attracted increasing attention for detecting low-density light in both scientific research and practical applications in recent years; yet the photon losses due to reflection on the light-sensitive planar silicon surface considerably limit its photon detection efficiency. Here we demonstrate an advanced light trapping feature by developing the multi-layer antireflection coatings and the textured silicon surface with upright random nano-micro pyramids, which significantly reduces the reflection of faint light in a wide spectrum, from ultraviolet to infrared. Integrating this advanced photon confinement feature into next-generation back-illuminated silicon photomultiplier would increase the photon detection efficiency with significantly lower reflection and much more active areas. This advanced design feature offers the back-illuminated silicon photomultiplier broader application opportunities exemplified in the emerging scenarios such as nuclear medical imaging, light detection and ranging for autonomous driving, detection of scintillation light in ionizing radiation, as well as high energy physics.

42 ENGINEERING↗

Interpretative transport modeling of the WEST boundary plasma: main plasma and light impurities

Understanding impurity transport in tokamak plasmas is crucial to control radiative losses and material migration in future magnetic fusion reactors. In this work we deploy the SolEdge2D-EIRENE code to model the boundary plasma in a WEST discharge, satisfactorily reproducing measurements of both upstream and divertor plasma conditions. Additionally, the spatial distribution of oxygen, studied here as a representative light impurity, is compared to vacuum ultraviolet spectroscopy measurements acquired with an oscillating line of sight. The simulation captures a key feature of the experiment, namely a factor of sime2 higher oxygen brightness in the inner divertor region compared to the outer one. This spatial asymmetry in oxygen concentration is interpreted by analyzing the balance of friction forces and thermal gradient forces that the light impurity exchanges with the main plasma.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

All-optical single-shot complete electric field measurement of extreme ultraviolet free electron laser pulses

Recent advances in ultrafast extreme ultraviolet (EUV) and x-ray light sources provide direct access to fundamental time and length scales for biology, chemistry, and materials physics. However, such light pulses are challenging to measure due to the need for femtosecond time resolution at difficult-to-detect wavelengths. Also, single-shot measurements are needed because severe pulse-to-pulse fluctuations are common. Here we demonstrate single-shot, complete field measurements by applying a novel version of frequency resolved optical gating. An EUV free electron laser beam creates a transient grating containing the pulse’s electric field information, which is read out with a 400 nm probe pulse. By varying the time delay between two copies of the EUV pump, rather than between the pump and the probe, we separate the needed coherent wave mixing from the slow incoherent response. Because this approach uses photoionization, it should be applicable from the vacuum ultraviolet to hard x rays.

36 MATERIALS SCIENCE↗

Genetic Fusion of Thermoresponsive Polypeptides with UCST‐type Behavior Mediates 1D Assembly of Coiled‐Coil Bundlemers

Abstract Thermoresponsive resilin‐like polypeptides (RLPs) of various lengths were genetically fused to two different computationally designed coiled coil‐forming peptides with distinct thermal stability, to develop new strategies to assemble coiled coil peptides via temperature‐triggered phase separation of the RLP units. Their successful production in bacterial expression hosts was verified via gel electrophoresis, mass spectrometry, and amino acid analysis. Circular dichroism (CD) spectroscopy, ultraviolet‐visible (UV/Vis) turbidimetry, and dynamic light scattering (DLS) measurements confirmed the stability of the coiled coils and showed that the thermosensitive phase behavior of the RLPs was preserved in the genetically fused hybrid polypeptides. Cryogenic‐transmission electron microscopy and coarse‐grained modeling revealed that functionalizing the coiled coils with thermoresponsive RLPs leads to their thermally triggered noncovalent assembly into nanofibrillar assemblies.

Patkar, Sai S.↗

Genetic Fusion of Thermoresponsive Polypeptides with UCST–type Behavior Mediates 1D Assembly of Coiled–Coil Bundlemers

Thermoresponsive resilin-like polypeptides (RLPs) of various lengths were genetically fused to two different computationally designed coiled coil-forming peptides with distinct thermal stability, to develop new strategies to assemble coiled coil peptides via temperature-triggered phase separation of the RLP units. Furthermore, their successful production in bacterial expression hosts was verified via gel electrophoresis, mass spectrometry, and amino acid analysis. Circular dichroism (CD) spectroscopy, ultraviolet-visible (UV/Vis) turbidimetry, and dynamic light scattering (DLS) measurements confirmed the stability of the coiled coils and showed that the thermosensitive phase behavior of the RLPs was preserved in the genetically fused hybrid polypeptides. Cryogenic-transmission electron microscopy and coarse-grained modeling revealed that functionalizing the coiled coils with thermoresponsive RLPs leads to their thermally triggered noncovalent assembly into nanofibrillar assemblies.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Quantification of Key Peroxy and Hydroperoxide Intermediates in the Low-Temperature Oxidation of Dimethyl Ether

Dimethyl ether (DME) oxidation is a model chemical system with a small number of prototypical reaction intermediates that also has practical importance for low-carbon transportation. Although it has been studied experimentally and theoretically, ambiguity remains in the relative importance of competing DME oxidation pathways in the low-temperature autoignition regime. To focus on the primary reactions in DME autoignition, we measured the time-resolved concentration of five intermediates, CH 3 OCH 2 OO (ROO), OOCH 2 OCH 2 OOH (OOQOOH), HOOCH 2 OCHO (hydroperoxymethyl formate, HPMF), CH 2 O, and CH 3 OCHO (methyl formate, MF), from photolytically initiated experiments. We performed these studies at P = 10 bar and T = 450-575 K, using a high-pressure photolysis reactor coupled to a time-of-flight mass spectrometer with tunable vacuum-ultraviolet synchrotron ionization at the Advanced Light Source. Our measurements reveal that the timescale of ROO decay and product formation is much shorter than predicted by current DME combustion models. The models also strongly underpredict the observed yields of CH 2 O and MF and do not capture the temperature dependence of OOQOOH and HPMF yields. Adding the ROO + OH $\rightarrow$ RO + HO 2 reaction to the chemical mechanism (with a rate coefficient approximated from similar reactions) improves the prediction of MF. Increasing the rate coefficients of ROO ↔ QOOH and QOOH + O 2 ↔ OOQOOH reactions brings the model predictions closer to experimental observations for OOQOOH and HPMF, while increasing the rate coefficient for the QOOH $\rightarrow$ 2 CH 2 O + OH reaction is needed to improve the predictions of formaldehyde. In conclusion, to aid future quantification of DME oxidation intermediates by photoionization mass spectrometry, we report experimentally determined ionization cross-sections for ROO, OOQOOH, and HPMF.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Investigation of O( 3 P) Initiated Oxidation Products of 2,3-Dimethylfuran Using Synchrotron Photoionization

Biofuels are an appealing alternative to augment conventional fossil fuels, given that traditional fossil fuels are finite in nature despite being the highest-consumed energy source. Furans have been studied as potential biofuels due to their renewability, high energy density, and ability to both blend with existing fossil fuels and serve as a stand-alone fuel. Although promising, more research efforts on the combustion of furan-based biofuels are needed. Here, in this study, the oxidation of 2,3-dimethylfuran (2,3-DMF) initiated by O( 3 P) was investigated using vacuum-ultraviolet synchrotron radiation from the Advanced Light Source at the Lawrence Berkeley National Laboratory. The reaction was studied at 550 K and 7 Torr. Major reaction products include 3-methyl-3-buten-2-one, 4,5-dimethyl-3(2H)-furanone, and 3-methyl-4-oxo-2(Z)-pentenal, with 3-methyl-3-buten-2-one being the most abundant.

CBS-QB3↗

Theoretical and experimental study on the O( 3 P) + 2,5-dimethylfuran reaction in the gas phase

In this work we report a joint experimental and computational study on the 2,5-dimethylfuran oxidation reaction in the gas phase initiated by atomic oxygen O( 3 P). The experiments have been performed by using vacuum-ultraviolet synchrotron radiation at the Advanced Light Source (ALS) of the Lawrence Berkeley National Laboratory (LBNL), at a temperature of 550 K and a pressure of 8 Torr. The experimental data were supported by quantum-chemical calculations along with a kinetic model, also taking into account the possible involvement of different magnetic states, performed in the framework of the RRKM theory. Propyne, acetaldehyde, methylglyoxal, dimethylglyoxal, 3-penten-2-one, 2,5-dimethylfuran-3(2 H )-one, and 1,2-diacetyl ethylene have been identified as the main primary products arising under the conditions of the experiment. Our computational model suggests that these species can be formed at the concentration and branching ratio experimentally observed only in the presence of a non-negligible fraction of non-thermalized intermediates.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Neural Density Estimation and Uncertainty Quantification for ChemCam Spectra [Slides]

The ChemCam instrument of Curiosity uses laser-induced breakdown spectroscopy (LIBS). It fires a laser at target and vaporizes rock surfaces, creating a plasma. Three spectrographs divide the plasma light into wavelengths for chemical analysis: ultraviolet, violet, and visible near-infrared. Regression methods (SVR, PCR, CNN) have been employed for calibration (prediction of the elemental composition of samples); however, labeled ChemCam samples are limited. Here, we focus on unsupervised learning and employ generative models from ChemCam analysis. Further, we use labels (supervised) in combination to the generative model to compute uncertainties related to predictions. We report generative modeling can be successfully applied to model real-world data. Normalizing flow models can be efficiently constructed on latent spaces for fast downstream inference. Unsupervised and supervised learning can be combined to form an uncertainty quantification framework.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Initial Benchmarks of UV LEDs and Comparisons with White LEDs

The primary goal of this report is to benchmark the initial level of performance of a selection of commercial UV LEDs across all three bands (i.e., UV-A, UV-B, UV-C). To provide the initial performance benchmarks, a test matrix containing 13 different UV LED products was created in association with the LED Systems Reliability Consortium (LSRC). The products in this test matrix were all commercially available as of June 2021, and at least 22 samples of each product were tested. In addition, two common, commercial white LEDs were tested to provide a benchmark against blue-pumped white LEDs. Testing of the samples included electrical performance testing (e.g., current-voltage measurements) and photometric testing in a calibrated integrating sphere capable of measuring devices in the UV-A, UV-B, and UV-C bands. The electrical testing provided insights into the performance of the semiconductor layers in the LEDs, allowing parameters such as the threshold voltage (V th ) and serial resistance (R serial ) of each sample to be determined. The photometric testing provided insights into emission wavelengths, peak shapes, and radiant efficiencies for each sample. Combined, the information from these tests permits the overall device efficiencies to be compared and provides insights into the electrical and optical performance of the technology.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

Silver Nanoparticles Functionalized Nanosilica Grown over Graphene Oxide for Enhancing Antibacterial Effect

The continuous growth of multidrug-resistant bacteria due to the overuse of antibiotics and antibacterial agents poses a threat to human health. Silver nanoparticles, silica-based materials, and graphene-based materials have become potential antibacterial candidates. In this study, we developed an effective method of enhancing the antibacterial property of graphene oxide (GO) by growing nanosilica (NS) of approximately 50 nm on the graphene oxide (GO) surface. The structures and compositions of the materials were characterized through powdered X-ray diffraction (P-XRD), transmission electron microscopy (TEM), scanning electron microscopy coupled with energy dispersive X-ray spectroscopy (SEM-EDS), ultraviolet–visible spectroscopy (UV–VIS), dynamic light scattering (DLS), Raman spectroscopy (RM), Fourier-transform infrared spectroscopy (FTIR), Brunauer–Emmet–Teller (BET) surface area, and pore size determination. The silver nanoparticles (AgNPs) with an average diameter of 26 nm were functionalized on the nanosilica (NS) surface. The composite contained approximately 3% of silver nanoparticles. The silver nanoparticles on nanosilica supported over graphene oxide (GO/NS/AgNPs) exhibited a 7-log reduction of Escherichia coli and a 5.2-log reduction of Bacillus subtilis within one hour of exposure. Both GO/NS and GO/NS/AgNPs exhibited substantial antimicrobial effects against E. coli and B. subtilis.

36 MATERIALS SCIENCE↗

Tantalum pentoxide: a new material platform for high-performance dielectric metasurface optics in the ultraviolet and visible region

Dielectric metasurfaces, composed of planar arrays of subwavelength dielectric structures that collectively mimic the operation of conventional bulk optical elements, have revolutionized the field of optics by their potential in constructing high-efficiency and multi-functional optoelectronic systems on chip. The performance of a dielectric metasurface is largely determined by its constituent material, which is highly desired to have a high refractive index, low optical loss and wide bandgap, and at the same time, be fabrication friendly. Here, we present a new material platform based on tantalum pentoxide (Ta 2 O 5 ) for implementing high-performance dielectric metasurface optics over the ultraviolet and visible spectral region. This wide-bandgap dielectric, exhibiting a high refractive index exceeding 2.1 and negligible extinction coefficient across a broad spectrum, can be easily deposited over large areas with good quality using straightforward physical vapor deposition, and patterned into high-aspect-ratio subwavelength nanostructures through commonly-available fluorine-gas-based reactive ion etching. We implement a series of high-efficiency ultraviolet and visible metasurfaces with representative light-field modulation functionalities including polarization-independent high-numerical-aperture lensing, spin-selective hologram projection, and vivid structural color generation, and the devices exhibit operational efficiencies up to 80%. Our work overcomes limitations faced by scalability of commonly-employed metasurface dielectrics and their operation into the visible and ultraviolet spectral range, and provides a novel route towards realization of high-performance, robust and foundry-manufacturable metasurface optics.

36 MATERIALS SCIENCE↗

Open-source simulation program for extreme ultraviolet and soft x-ray sources based on high-harmonic generation

Light sources based on high-harmonic generation (HHG) underpin ultrafast spectroscopy experiments across a large range of photon energies, spanning from the extreme ultraviolet to the soft x-ray. To this day, their design, implementation, and improvement presens unique challenges, but can be aided by numerical tools. Here we present a new simulation program designed for this purpose, which takes both macroscopic and microscopic aspects of high-harmonic generation into account and is therefore applicable across the broad range of parameters which HHG based light sources are today utilized. The program is validated by comparison with published experimental results and by calculating harmonic emission in four common experimental configurations.

Femtosecond lasers↗

Measurement of the liquid argon scintillation pulse shape using differentiable simulation in the coherent CAPTAIN-Mills experiment

The coherent CAPTAIN-Mills (CCM) experiment is a liquid argon (LAr) light collection detector searching for MeV-scale neutrino and beyond Standard Model physics signatures. Two hundred eight-inch photomultiplier tubes instrument the seven-ton fiducial volume with 50% photocathode coverage to detect light produced by charged particles. CCM’s light-based approach reduces requirements of LAr purity, compared to other detection technologies, such that sub-MeV particles can be reliably detected without additional LAr filtration and with 𝒪⁡(1) parts per million of common contaminants. We present a measurement of LAr light production and propagation parameters, with uncertainties, obtained from a sample of MeV-scale electromagnetic events. The optimization of this high-dimensional parameter space was facilitated by a differentiable optical photon Monte Carlo simulation and detailed photomultiplier tube response characterization. This result accurately predicts the timing and spatial distribution of light due to scintillation and Cherenkov emission in the detector. This is the first description of photon propagation in LAr to include several effects, including anomalous dispersion of the index of refraction near the ultraviolet resonance, Mie scattering from impurities, and Cherenkov light production.

Cherenkov detectors↗

Pre-Ionization Controlled Laser Plasma Formation for Ignition Applications (Final Scientific/Technical Report)

This report consists of three grand funded papers. Abstracts for each follow. 1) In this work, we present experimental and modeling studies of air pre-ionization using ultraviolet (UV) laser pulses and its effect on laser breakdown of an overlapped near-infrared (NIR) pulse. Experimental studies are conducted with a 266 nm beam (fourth harmonic of Nd:YAG) for UV pre-ionization and an overlapped 1064 nm NIR beam (fundamental of Nd:YAG), both having pulse duration of 10 ns. Results show that the UV beam produces a pre-ionized volume which assists in breakdown of the NIR beam, leading to reduction in NIR breakdown threshold by factor of >2. Numerical modeling is performed to examine the ionization and breakdown of both beams. The modeled breakdown threshold of the NIR, including assist by pre-ionization, is in reasonable agreement with the experimental results. 2) The present contribution compares the energy absorption, optical emission, temperature, and fluid dynamics of ultraviolet (UV) λ = 266 nm and near infrared (NIR) λ = 1064 nm nanosecond laser induced plasmas in ambient air. For UV pulses at the conditions studied, energy absorption by the plasmas increases relatively gradually with laser pulse energy starting at delivered energy of E~8 mJ. Corresponding measurements of plasma luminosity show that the absorption of UV radiation does not necessarily result in visible plasma emission. For the NIR induced plasmas, the energy absorption profile is far more abrupt and begins at ~55 mJ. In contrast with UV, the absorption of NIR radiation is always accompanied by intense optical emission. The temperatures of both types of plasma have been measured with Rayleigh scattering thermometry (at times after the Thomson signal sufficiently diminishes). The UV plasmas can attain a wider range of temperatures, including lower temperatures, depending on the pulse energy (e.g., T ~400–2000K for E ~7–35 mJ at Δt = 10 μs after the pulse) while the NIR plasmas show only hotter temperatures (e.g., T ~ 12 000 K for E = 75 mJ at Δt = 10 μs after the pulse) as is consistent with the literature. Differences in the fluid dynamics for UV versus NIR pulses are shown with Schlieren imaging. In this work, the contrast in the UV and NIR plasma threshold behavior is attributed to differing roles of avalanche ionization and multiphoton ionization as is also illustrated by a simple numerical model. 3) The present contribution examines the impact of plasma dynamics and plasma-driven fluid dynamics on the flame growth of laser ignited mixtures and shows that a new dual-pulse scheme can be used to control the kernel formation process in ways that extend the lean ignition limit. We perform a comparative study between (conventional) single-pulse laser ignition (λ = 1064 nm) and a novel dual-pulse method based on combining an ultraviolet (UV) pre-ionization pulse (λ = 266 nm) with an overlapped near-infrared (NIR) energy addition pulse (λ = 1064 nm). We employ OH* chemiluminescence to visualize the evolution of the early flame kernel. For single-pulse laser ignition at lean conditions, the flame kernel separates through third lobe detachment, corresponding to high strain rates that extinguish the flame. In this work, we investigate the capabilities of the dual-pulse to control the plasma-driven fluid dynamics by adjusting the axial offset of the two focal points. In particular, we find there exists a beam waist offset whereby the resulting vorticity suppresses formation of the third lobe, consequently reducing flame stretch. With this approach, we demonstrate that the dual-pulse method enables reduced flame speeds (at early times), an extended lean limit, increased combustion efficiency, and decreased laser energy requirements.

Mechanical engineering↗

Synchrotron Photoionization Study of the Diisopropyl Ether Oxidation

Abstract Scientific evidence has shown oxygenates help to reduce dangerous pollutants arising from burning fossil fuel in the automotive sector. For this reason, their use as additives has spread widely. The aim of this work consists in providing a comprehensive identification of the main primary oxidation products of diisopropyl ether (DIPE), one of the most promising among etheric oxygenates. The Cl‐initiated oxidation of DIPE is examinated by using a vacuum ultraviolet (VUV) synchrotron radiation at the Advanced Light Source (ALS) of the Lawrence Berkeley National Laboratory (LBNL). Products are identified on the basis of their mass‐to‐charge ratio, shape of photoionization spectra, adiabatic ionization energies, and chemical kinetic profiles, at three different temperatures (298, 550, and 650 K). Acetone, propanal, propene, and isopropyl acetate have been identified as major reaction products. Acetone is the main primary product. Theoretical calculations using the composite CBS‐QB3 method provided useful tools to validate the postulated reaction mechanisms leading to experimentally observed species. The formation of other species is also discussed.

Giustini, Andrea↗

Time-resolved quantification of key species and mechanistic insights in low-temperature tetrahydrofuran oxidation

Here, we investigate the kinetics and report the time-resolved concentrations of key chemical species in the oxidation of tetrahydrofuran (THF) at 7500 torr and 450–675 K. Experiments are carried out using high-pressure multiplexed photoionization mass spectrometry (MPIMS) combined with tunable vacuum ultraviolet radiation from the Berkely Lab Advanced Light Source. Intermediates and products are quantified using reference photoionization (PI) cross sections, when available, and constrained by a global carbon balance tracking approach at all experimental temperatures simultaneously for the species without reference cross sections. From carbon balancing, we determine time-resolved concentrations for the ROO˙ and ˙OOQOOH radical intermediates, butanedial, and the combined concentration of ketohydroperoxide (KHP) and unsaturated hydroperoxide (UHP) products stemming from the ˙QOOH + O 2 reaction. Furthermore, we quantify a product that we tentatively assign as fumaraldehyde, which arises from UHP decomposition via H 2 O or ˙OH + H loss. The experimentally derived species concentrations are compared with model predictions using the most recent literature THF oxidation mechanism of Fenard et al., (Combust. Flame, 2018, 191, 252–269). Our results indicate that the literature mechanism significantly overestimates THF consumption and the UHP + KHP concentration at our conditions. The model predictions are sensitive to the rate coefficient for the ROO˙ isomerization to ˙QOOH, which is the gateway for radical chain propagating and branching pathways. Comparisons with our recent results for cyclopentane (Demireva et al., Combust. Flame, 2023, 257, 112506) provide insights into the effect of the ether group on reactivity and highlight the need to determine accurate rate coefficients of ROO˙ isomerization and subsequent reactions.

Demireva, Maria↗

Imaging plasma formation in isolated nanoparticles with ultrafast resonant scattering

We have recorded the diffraction patterns from individual xenon clusters irradiated with intense extreme ultraviolet pulses to investigate the influence of light-induced electronic changes on the scattering response. The clusters were irradiated with short wavelength pulses in the wavelength regime of different 4d inner-shell resonances of neutral and ionic xenon, resulting in distinctly different optical properties from areas in the clusters with lower or higher charge states. The data show the emergence of a transient structure with a spatial extension of tens of nanometers within the otherwise homogeneous sample. Simulations indicate that ionization and nanoplasma formation result in a light-induced outer shell in the cluster with a strongly altered refractive index. The presented resonant scattering approach enables imaging of ultrafast electron dynamics on their natural timescale.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗