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Additional Trials & Tribulations in Synthesizing a Sulfide Standard

Well-characterized sulfide reference materials that can serve as matrix-matched calibrants for in-situ trace element analyses via laser ablation inductively coupled plasma mass spectrometry (LA-ICP-MS) remain elusive. Here, we describe the creation an in-house sulfide standard at NASA JSC that will be used to measure siderophile and chalcophile trace elements in low pressure experimental products, specifically pentlandite ([FeNi]9S8) and pyrrhotite ([FeNi]1-xS), as well as natural sulfides in terrestrial and meteoritic mineral assemblages. Recent methods in creating a homogenous sulfide standard include pressed pellets, synthesized chips, or fused glass [e.g. 1-3]. Other studies, however, have had success in forming homogenous FeS standards via synthesization methods [e.g. 4-6]. We present a variation of the method described in [4], in which we create a pyrrhotite standard doped with a variety of trace elements (Zn, As, Se, Mo, Ru, Rh, Pd, Sn, Sb, Te, W, Os, Ir, Pt, Au) at ~10-40 ppm and Cu at ~200 ppm. Sulfide compositions were constructed using Fe and Ni metal and elemental sulfur powders. Trace elements were added to elemental sulfur from Atomic Absorption Spectroscopy (AAS) elemental standards as either nitrate or chloride solutions to prevent oxidation of the metal powders. The dried sulfur mixture was mixed with Fe and Ni powders and mechanically mixed before two aliquots were placed in separate SiO2 tubes. Each tube was held under vacuum for ~30 minutes, sealed under vacuum, and then heated at 800C for 48 hours. Like [4], the synthesis products were composed of pourous sulfide crystals. Major element analyses of both experimental aliquots, collected using an Electron Probe Microanalyser (EPMA), yield indistinguishable major element compositions (uncertainties in 2SE & 2RSE[%]), with an average of 57.90  0.09 (0.16 %), 4.95  0.03 (0.55 %), and 39.70  0.14 (0.34 %), for Fe, Ni, and S, respectively. Trace element data were measured using a Photon Machines 193nm laser ablation system coupled to a Thermo-Scientific Element-XR ICP-MS. Spot sizes were limited to 50 μm due to the porous nature of the sulfide target material. Trace element abundances, normalized to Fe as an internal standard, were also found to be homogenous between the two aliquots, with weighted mean 2RSE (%) values of <3.0 for all trace elements. Synthesized products were re-powdered and absolute concentrations measured via solution ICP-MS. Although the sulfide appears to be homogenous, sintering experiments will be performed to more closely match the standard density to natural sulfides and minimize differences in ablation behavior. Improved density also allows for higher sensitivity (i.e. more compact target material) and larger spot sizes or traverses, as void space is eliminated. Additional major and trace element analyses on the products of the sintering experiments will be undertaken.

Jacob B Setera↗
DOE OSTI2023

Simulating lossy Gaussian boson sampling with matrix-product operators

Gaussian boson sampling, a computational model that is widely believed to admit quantum supremacy, has already been experimentally demonstrated and is claimed to surpass the classical simulation capabilities of even the most powerful supercomputers today. However, whether the current approach limited by photon loss and noise in such experiments prescribes a scalable path to quantum advantage is an open question. Here, to understand the effect of photon loss on the scalability of Gaussian boson sampling, we analytically derive the asymptotic operator entanglement entropy scaling, which relates to the simulation complexity. As a result, we observe that efficient tensor network simulations are likely possible under the N out ∝ √N scaling of the number of surviving photons N out in the number of input photons N. We numerically verify this result using a tensor network algorithm with U⁡(1) symmetry, and we overcome previous challenges due to the large local Hilbert-space dimensions in Gaussian boson sampling with hardware acceleration. Additionally, we observe that increasing the photon number through larger squeezing does not increase the entanglement entropy significantly. Finally, we numerically find the bond dimension necessary for fixed accuracy simulations, providing more direct evidence for the complexity of tensor networks.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2025

Dirhodium(II,II) Complexes as Panchromatic Single-Molecule Photocatalysts for Hydrogen Evolution

The growing global energy demand and climate change have prompted a shift from carbon-based fuels to sustainable energy sources. Hydrogen production by harnessing solar energy and using abundant proton sources represents an attractive approach to addressing this crisis. Single-molecule single-chromophore photocatalysts, capable of both absorbing the incident photon and catalyzing the chemical transformation, are able to circumvent energy losses present in multicomponent systems that require a photosensitizer and a catalyst, often employing additional redox relay molecules. Here, the series of complexes derived from cis-[Rh 2 (μ-DPhF) 2 (μ-bncn) 2 ] 2+ (1; DPhF = N,N′-diphenylformamidinate, bncn = benzo[c]cinnoline) discussed in this Account presents robust and air-stable single-molecule photocatalysts with panchromatic absorption from the ultraviolet spectral region to the near-infrared (NIR), with high turnover frequencies of ∼20 to 30 h –1 under red light irradiation. For comparison, other single-molecule hydrogen-evolving photocatalysts reported to date exhibit low photocatalytic efficiency, are not operable in the visible or NIR regions, and are unstable under an ambient atmosphere.

Absorption↗
DOE OSTI2022

Selected topics in diffraction with protons and nuclei: past, present, and future

Here, we review a broad range of phenomena in diffraction in the context of hadron–hadron, hadron–nucleus collisions and deep inelastic lepton–proton/nucleus scattering focusing on the interplay between the perturbative QCD and non-perturbative models. We discuss inclusive diffraction in DIS, phenomenology of dipole models, resummation and parton saturation at low x , hard diffractive production of vector mesons, inelastic diffraction in hadron–hadron scattering, formalism of color fluctuations, inclusive coherent and incoherent diffraction as well as soft and hard diffraction phenomena in hadron–hadron/nucleus and photon–nucleus collisions. For each topic we review key results from the past and present experiments including HERA and the LHC. Finally, we identify the remaining open questions, which could be addressed in the continuing experiments, in particular in photon-induced reactions at the LHC and the future electron–ion collider in the US, large hadron electron collider and future circular collider at CERN.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2023

Prospects and applications of on-chip lasers

Abstract Integrated silicon photonics has sparked a significant ramp-up of investment in both academia and industry as a scalable, power-efficient, and eco-friendly solution. At the heart of this platform is the light source, which in itself, has been the focus of research and development extensively. This paper sheds light and conveys our perspective on the current state-of-the-art in different aspects of application-driven on-chip silicon lasers. We tackle this from two perspectives: device-level and system-wide points of view. In the former, the different routes taken in integrating on-chip lasers are explored from different material systems to the chosen integration methodologies. Then, the discussion focus is shifted towards system-wide applications that show great prospects in incorporating photonic integrated circuits (PIC) with on-chip lasers and active devices, namely, optical communications and interconnects, optical phased array-based LiDAR, sensors for chemical and biological analysis, integrated quantum technologies, and finally, optical computing. By leveraging the myriad inherent attractive features of integrated silicon photonics, this paper aims to inspire further development in incorporating PICs with on-chip lasers in, but not limited to, these applications for substantial performance gains, green solutions, and mass production.

Zhou, Zhican↗
NASA NTRS1979

Pulsar magnetospheres

The structure of both the interior and exterior pulsar magnetosphere depends upon the strength of its plasma source near the surface of the star. We review magnetospheric models in the light of a vacuum pair-production source model proposed by Sturrock, and Ruderman and Sutherland. This model predicts the existence of a cutoff, determined by the neutron star's spin rate and magnetic field strength, beyond which coherent radio emission is no longer possible. The observed distribution of pulsar spin periods and period derivatives, and the distribution of pulsars with missing radio pulses, is quantitatively consistent with the pair production threshold, when its variation of neutron star radius and moment of inertia with mass is taken into account. All neutron stars observed as pulsars can have relativistic magnetohydrodynamic wind exterior magnetospheres. The properties of the wind can be directly related to those of the pair production source. Radio pulsars cannot have relativistic plasma wave exterior magnetospheres. On the other hand, most erstwhile pulsars in the galaxy are probably halo objects that emit weak fluxes of energetic photons that can have relativistic wave exterior magnetospheres. Extinct pulsars have not been yet observed.

Kennel, C. F.↗
NASA NTRS1982

Development of the cosmic ray techniques

It has been found that most advances of cosmic-ray physics have been directly related to the development of observational techniques. The history of observational techniques is discussed, taking into account ionization chambers, refinements applied to ionization chambers to make them suitable for an effective use in the study of cosmic radiation, the Wulf-type electrometer, the electrometer designed by Millikan and Neher, the Geiger-Mueller counter, the experiment of Bothe and Kolhoerster, the coincidence circuit, and a cosmic-ray 'telescope'. Attention is given to a magnetic lens for cosmic rays, a triangular arrangement of Geiger-Mueller counters used to demonstrate the production of a secondary radiation, a stereoscopic cloud-chamber photograph of showers, the cloud-chamber picture which provided the first evidence of the positive electron, and arrangements for studying photon components, mu-mesons, and air showers.

Rossi, B.↗
NASA NTRS1995

Study of the rotational-level and temperature dependence of the quenching rate of OH fluorescence due to collisions with water molecules

The importance of the OH radical as an intermediate in many combustion reactions and in atmospheric photochemistry has led many researchers to use it as a diagnostic tool in these processes. The amount of data that has been acquired over the years for this radical is quite considerable. However, the quenching rate of OH with water molecules as a function of temperature and the rotational level of the excited state is not very well understood. The motivation of the studies undertaken is to bridge the gap between the low temperature measurements and the high temperature ones reported in the literature. The technique generally employed in these diagnostics is laser-induced fluorescence (LIF), through which rotational state selective excitation of the radical is possible. Furthermore, in a combustion medium, water is produced in abundance so that knowledge of the quenching rate of OH due to water molecules plays a crucial role in interpreting the data. In general, the precursor to an understanding of the collisional quenching rates of OH involves a characterization of the mode in which the radical is produced; the resulting rotational and translational distribution, followed by a measurement of the OH temperature; and ultimately obtaining the rate constants from the pressure dependence of the fluorescence signal. The experimental implementation of these measurements therefore involved, as a first step, the production of the OH radicals in a microwave discharge cell using water vapor as the source, wherein a hydrogen atom is abstracted from H2O. The second step involved the absorption of photons from the frequency-doubled output of a pulsed amplified, single-frequency cw ring dye laser. By tuning the laser to the peak of the transition and observing the fluorescence decay after the laser pulse, the lifetime of the OH in a particular rotational electronic state was determined (tau = 1.4 microseconds for Q(sub 1)(3)). Knowledge of this parameter led to a determination of the quenching rate. By varying the water vapor pressure in the cell and measuring the lifetime as a function of pressure a linear plot of the quenching rate as a function of pressure was obtained. Using this plot, the quenching cross section was deduced. It has therefore been possible to measure the local translational temperature and the quenching cross section with one laser system.

Koker, Edmond B.↗
NASA NTRS2023

Development of a Photoacoustic Formaldehyde Monitor

Key indoor air quality pollutant formaldehyde (H2CO) is tracked on International Space Station (ISS) using passive badges returned to the ground periodically for analysis. The process is time-consuming both in preparation and for analysis upon return 6-12 months later. Badges also require precious crew time for deploy, retrieval and stow. As NASA’s focus in space exploration shifts to the Moon and Mars, archival sample return becomes increasingly impractical, so the aim of this project is to develop a highly reliable real-time analyzer for H2CO at low concentrations with data downlinked. Potential sources of H2CO include materials off gassing, use of formalin as a tissue fixative in biological payloads and overheating of acetal polymers. The Spacecraft Maximum Allowable Concentration (SMAC) for H2CO is 100 ppb for exposures of 7 days or longer. ISS concentrations recently run only 10 - 30 ppb but have spiked as high as 60 ppb in the past. Gateway real time monitoring requirements call for a range of 8 - 140 ppb. For this project, a concentration range of 5 - 500 ppb H2CO is targeted. The core tunable diode laser spectroscopy (TDLS) technology was developed by Vista Photonics through the NASA and US Navy Small Business Innovation Research (SBIR) programs. Monitors based on this technology have been demonstrated on ISS, trialed on a nuclear submarine and are in production as Anomaly Gas Analyzers for both ISS and Orion. Initially, direct absorption TDLS was used exclusively in these monitors, however, the H2CO target concentration is much lower, and a longer wavelength required, so a photoacoustic spectroscopy (PAS) technique was adapted, where the laser excitation is detected by a sensitive microphone vs. a conventional photodetector. This paper will discuss the results of NASA-JSC laboratory testing of a prototype PAS based formaldehyde monitor and explore potential adaptations for Gateway missions and beyond.

Paul D Mudgett↗
DOE OSTI2026

Axion-like particle at the 10 GeV scale: Higgs decays to wide jets and photons

If axion-like particles (ALPs) exist, they may have renormalizable couplings only to the Higgs boson ($h^0$) or to fields beyond the Standard Model. An ALP $A_h$ lighter than about 60 GeV would allow the $h^0 \to A_h A_h$ decay, with a branching fraction determined by the explicit global symmetry breaking responsible for the main contributions to the $A_h$ mass ($M_A$). New heavy fields that carry color and electric charge, such as squarks, can mediate $A_h$ decays at one loop mostly into gluons, but also into photons. Exploring LHC sensitivity to $A_h$, we show that the $h^0 \to A_h A_h \to (gg)(γγ)$ channel leads to a diphoton resonance at $M_A$ whose production rate is consistent with a $3.5σ$ excess reported by a CMS search at $M_A \approx 13.6$ GeV. For $M_A$ of order 10 GeV, the $h^0 \to A_h A_h \to 4g$ cascade decay leads to two wide jets (each with 2-prong substructure) that form a resonance at 125 GeV.

Dobrescu, Bogdan A. [Fermilab] (ORCID:000000034291↗
DOE OSTI2020

C HIMERA : A Massively Parallel Code for Core-collapse Supernova Simulations

Herein we provide a detailed description of the C HIMERA code, a code developed to model core collapse supernovae (CCSNe) in multiple spatial dimensions. The CCSN explosion mechanism remains the subject of intense research. Progress to date demonstrates that it involves a complex interplay of neutrino production, transport, and interaction in the stellar core, three-dimensional stellar core fluid dynamics and its associated instabilities, nuclear burning, and the fundamental physics of the neutrino–stellar core weak interactions and the equations of state of all stellar core constituents—particularly, the nuclear equation of state associated with core nucleons, both free and bound in nuclei. C HIMERA , by incorporating detailed neutrino transport, realistic neutrino–matter interactions, three-dimensional hydrodynamics, realistic nuclear, leptonic, and photonic equations of state, and a nuclear reaction network, along with other refinements, can be used to study the role of neutrino radiation, hydrodynamic instabilities, and a variety of input physics in the explosion mechanism itself. It can also be used to compute observables such as neutrino signatures, gravitational radiation, and the products of nucleosynthesis associated with CCSNe. The code contains modules for neutrino transport, multidimensional compressible hydrodynamics, nuclear reactions, a variety of neutrino interactions, equations of state, and modules to provide data for post-processing observables such as the products of nucleosynthesis, and gravitational radiation. C HIMERA is an evolving code, being updated periodically with improved input physics and numerical refinements. We detail here the current version of the code, from which future improvements will stem, which can in turn be described as needed in future publications.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2026

Electro- and photoproduction of muon pairs with $$\mu $$CLAS12: double deeply virtual compton scattering, timelike compton scattering, and $$J/\psi $$ production

The CEBAF Large Acceptance Spectrometer for operation at 12 GeV (CLAS12) at the Thomas Jefferson National Accelerator Facility has played a central role in advancing the understanding of nucleon and nuclear structure. As increasingly precise data become available, new physics opportunities emerge that extend beyond the current capabilities of CLAS12. In this article, a program to explore the quark and gluon structure of the nucleon through di-muon electro- and photoproduction is presented. Its primary focus is the measurement of beam-spin asymmetries in Double Deeply Virtual Compton Scattering, . By independently varying the incoming and outgoing photon virtualities and momentum transfer, the DDVCS measurement provides access to the Generalized Parton Distributions over their full three-dimensional phase space, extending beyond the kinematic constraints of Deeply Virtual Compton Scattering and Timelike Compton Scattering. In addition, the large acceptance and high luminosity of the CLAS12 experiment will enable precision measurements of near-threshold production and high-statistics studies of Timelike Compton Scattering.

Alvarado, J. S.↗
DOE OSTI2025

Role of Metal Cocatalysts in the Photocatalytic Production of Hydrogen from Water Revisited

The use of photocatalysts to promote the production of molecular hydrogen from water, following the so-called water splitting reaction, continues to be a promising route for the green production of fuels. The molecular basis of this photocatalysis is the photoexcitation of electrons from the valence band of semiconductors to their conduction band, from which they can be transferred to chemical reactants, protons in the case of water, to promote a reduction reaction. The mechanism by which such a process takes place has been studied extensively using titanium oxide, a simple material that fulfills most requirements for water splitting. However, photocatalysis with TiO 2 tends to be highly inefficient; a cocatalyst, commonly a late transition metal (Au, Pt) in nanoparticle form, needs to be added to facilitate the production of H 2 . The metal is widely believed to help with the scavenging of the excited electrons from the conduction band of the semiconductor in order to prevent their recombination with the accompanying hole formed in the valence band, a step that cancels the initial photon absorption and competes with the photolytic chemical reduction. Here we review and analyze the molecular basis for that mechanism and argue for an alternative explanation, that the role of the metal is to help with the recombination of the atomic hydrogen atoms produced by proton reduction on the semiconductor surface instead. First, we summarize what is known about the electronic structure of these photocatalysts and how the electronic levels need to line up for the reduction of protons in water to be feasible. Next, we review the current understanding of the dynamics of the steps associated with the absorption of photons, the de-excitation via electron–hole pair recombination and fluorescence decay, and the electronic transitions that lead to proton reduction, and contrast those with the rates of the chemical steps required to produce molecular hydrogen. The following section addresses the changes introduced by the addition of the metal cocatalyst, comparatively evaluating its role as either an electron scavenger or a promoter of the recombination of hydrogen atoms. A discussion of the viable chemical mechanisms for the latter pathway is included. Finally, we briefly mention other associated aspects of this photocatalysis, including the possible promotion of H 2 production with visible light via resonant excitation of the surface plasmon of Au nanoparticles, the use of single-metal (Au, Pt) atom catalysts and of yolk–shell nanostructures, and the reduction of organic molecules. We end with a brief personal perspective on the possible generality of the concepts introduced in this Critical Review.

08 HYDROGEN↗
DOE OSTI2023

Depletion Chain Simplification With Pseudo-Nuclides to Model Decay Effects

This work introduces the novel usage of pseudo-nuclides to model decay effects which are otherwise absent from simplified depletion libraries. Pseudo-nuclides are artificial nuclides which, when added to a simplified depletion library, can preserve quantities of interest such as decay energy release or decay photon activity which are otherwise significantly under-predicted by simplified libraries. Several dozen pseudo-nuclides are capable of accurately modeling decay effects of hundreds of short-lived radionuclides. The computational resources needed to model the decay effects in depletion systems with simplified depletion libraries with pseudo-nuclides are significantly less than those needed when using simplified depletion libraries without pseudo-nuclides. When compared to the similar method of decay heat precursors for a given system, pseudo-nuclides allow for smaller depletion libraries to be generated because of their ability to more accurately model the fission product irradiation effect on decay heat.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2023

Model-independent search for the presence of new physics in events including H → γγ with $\sqrt{s}$ = 13 TeV pp data recorded by the ATLAS detector at the LHC

A model-independent search for new physics leading to final states containing a Higgs boson, with a mass of 125.09 GeV, decaying to a pair of photons is performed with 139 fb -1 of $\sqrt{s}$ = 13 TeV $pp$ collision data recorded by the ATLAS detector at the Large Hadron Collider at CERN. This search examines 22 final states categorized by the objects that are produced in association with the Higgs boson. These objects include isolated electrons or muons, hadronically decaying $τ$-leptons, additional photons, missing transverse momentum, and hadronic jets, as well as jets that are tagged as containing a $b$-hadron. No significant excesses above Standard Model expectations are observed and limits on the production cross section at 95% confidence level are set. Detector efficiencies are reported for all 22 signal regions, which can be used to convert detector-level cross-section limits reported in this paper to particle-level cross-section constraints.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2022

CGC for ultra-peripheral Pb+Pb collisions at the Large Hadron Collider: a more realistic calculation

We provide the first calculation of two-gluon production at mid-rapidity in ultra-peripheral collisions in the Color Glass Condensate framework. To estimate systematic uncertainty associated with poor understanding of the wave function of the nearly real photon, we consider two diametrically different models: the dilute quark-antiquark dipole approximation and a vector meson, in which color charge density is approximated by McLerran-Venugopalan model. In the experimentally relevant range, the target nucleus can be faithfully approximated by a highly saturated state. This simplification enables us to perform efficient numerical simulations and extract the two-gluon correlation functions and the associated azimuthal harmonics.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2025

Exciton fission enhanced silicon solar cell

While silicon solar cells dominate global photovoltaic energy production, their continued improvement is hindered by the single-junction limit. One possible solution is to use molecular singlet exciton fission to generate two electrons from each absorbed high-energy photon. We demonstrate that the long-standing challenge of coupling molecular excited states to silicon solar cells can be overcome using sequential charge transfer. Combining zinc phthalocyanine, aluminum oxide, and a shallow junction crystalline silicon microwire solar cell, the peak charge generation efficiency per photon absorbed in tetracene is (138% ± 6%), comfortably surpassing the quantum efficiency limit for conventional silicon solar cells and establishing a new, scalable approach to low-cost, high-efficiency photovoltaics.

14 SOLAR ENERGY↗
DOE OSTI2022

Nonadiabatic dissociation of molecular Bose-Einstein condensates: Competition between chemical reactions

Here, we provide a framework to solve generic models describing the dissociation of multiple molecular Bose Einstein condensates in a nonadiabatic regime. The competition between individual chemical reactions can lead to non-trivial dependence on critical components such as path interference and symmetries, thus, affecting the final distribution of atomic population. We find an analytical solution for an illustrative example model involving four atomic modes. When the system parameters satisfy CPT symmetry, where C is charge conjugation, P is parity, and T is time-reversal symmetry, our solution predicts a population imbalance between atomic modes that is exponentially sensitive to system parameters. However, a weakly broken symmetry alters the population in each atomic mode and can reverse the population imbalance. Our solution also demonstrates a strong quantum correlation between atomic modes that leads to the spontaneous production of atoms in a multi-mode squeezed state. Moreover, in our framework, a time-dependent non-Hermitian quantum mechanics naturally manifests which can alternatively be realized experimentally in photonic systems.

74 ATOMIC AND MOLECULAR PHYSICS↗