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At least 253 records · Page 14

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DOE OSTI2020

An extended moments model of quantum efficiency for metals and semiconductors

The complexity of photocathode designs and detector materials, and the need to model their performance for short pulse durations, response to high frequency photons, presence of coatings and/or thinness of the absorptive layer, necessitates modifications to three-step and moments models of photoemission that are used in simulation codes. Here, methods to include input from computationally intensive approaches, such as density functional theory to model optical properties and transfer matrix approaches to treat emission from the surface or transport past coatings, by means of parametric models are demonstrated. First, a technique to accurately represent optical behavior so as to model reflectivity and penetration depth is given. Second, modifications to bulk models arising from the usage of thin film architectures, and a means to rapidly calculate them, is provided. Third, a parameterization to model the impact of wells associated with coatings and surface layers on the transmission probably is given. In all cases, the methods are computationally efficient and designed to allow for including input from numerically intensive approaches that would otherwise be unavailable for simulations.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2021

Probing the polar-nonpolar oxide interfaces using resonant x-ray standing wave techniques

Transition metal (TM) oxide heterostructure superlattices have attracted great attention in research communities because of their emergent interfacial phenomena that do not exist in the bulk form. In order to understand the mechanisms that cause these phenomena, it is important to use depth-resolved spectroscopies to study the electronic structure across the buried oxide interfaces. In this review, we focus on the recent applications of standing wave (SW) photoemission (SW-XPS) and resonant inelastic x-ray scattering (SW-RIXS) spectroscopy to study the depth profiles of electronic structure or carriers around the polar-nonpolar oxide interfaces. Here, using the incident photon energies near the TM x-ray absorption resonance, the created SW excitation can enhance the spectral response and certain electronic transitions, providing important insight into the interfacial electronic structure in the energy and real space regimes. Following the background introductions, we describe two SW experiments and demonstrate that the combination of SW-XPS and SW-RIXS has the potential to obtain the depth distribution of electronic/orbital states around the buried interfaces with Angstrom precision.

36 MATERIALS SCIENCE↗

DOE OSTI2026

Measurement of the Hubble constant with high-energy neutrinos

Measuring distances in the Universe is one of the hardest problems in physics and astronomy. Almost every distance probe relies on photons, whose propagation across cosmic distances introduces extinction, absorption, scattering, and radiative-transfer effects. Neutrinos suffer none of these and propagate unattenuated through dust, intergalactic medium, and dense source environments alike. We introduce a new distance-ladder method for measuring the Hubble constant $H_0$ using high-energy astrophysical neutrinos from point sources as standardizable candles, and report its first observational realization. Using 12 X-ray-selected Seyfert galaxies for which IceCube reports significant per-source neutrino excesses in its 14-year public point-source release, we exploit the disk-corona correlation $L_ν= κ\, L_X^β$ between neutrino and X-ray luminosities to construct a neutrino distance ladder anchored by non-redshift distances to NGC 1068 (Cepheid + TRGB). We find $H_0 = 49^{+40}_{-30}\,\mathrm{km\,s^{-1}\,Mpc^{-1}}$ and $β= 0.67^{+0.16}_{-0.25}$ (68% credible intervals), with the corona slope disfavoring the calorimetric limit $β= 1$ at ${\sim}2σ$. The result is consistent with existing $H_0$ determinations from Planck and SH0ES within 1$σ$. While the uncertainty on $H_0$ is large, the measurement is free of electromagnetic propagation systematics and demonstrates the viability of neutrinos as a novel cosmographical probe.

Herrera, Gonzalo [MIT, MKI; Harvard U.] (ORCID:000↗

DOE OSTI2022

Semiconductor-dielectric-metal solar absorbers with high spectral selectivity

An ideal solar thermal absorber has a sharp transition between high and low absorptance at the wavelength where the blackbody emissive power begins to exceed the solar irradiance. However, most real selective absorbers have a fairly broad transition, leading to both solar absorption and thermal emission losses. Here, we model, fabricate, and characterize a highly selective semiconductor-dielectric-metal (Ga0.46In0.54As - MgF2 - Ag) solar absorber with an extremely sharp transition from high to low absorptance. The thin semiconductor serves as a selective filter, absorbing photons with wavelengths shorter than the bandgap and transmitting those with longer wavelengths. The highly reflective dielectric-metal rear mirror allows the structure to have very low emittance for longer wavelengths. These characteristics provide the absorber with a measured solar absorptance >91% below the bandgap wavelength and infrared emittance <5% at 100 degrees C above the bandgap wavelength. This transition wavelength can be tuned by modifying the semiconductor composition, and modeling indicates that the absorber's optical properties should be stable at high temperatures, making the structure a good candidate for unconcentrated to highly concentrated solar thermal energy conversion.

14 SOLAR ENERGY↗

DOE OSTI2023

One dimensional temperature measurements by resonantly ionized photoemission thermometry of molecular nitrogen

This paper presents an extensive parameter study of a non-intrusive and non-seeded laser diagnostic method for measuring one dimensional (1D) rotational temperature of molecular nitrogen (N 2 ) at 165 - 450 K. Compared to previous efforts using molecular oxygen, here resonantly ionized and photoelectron induced fluorescence of molecular nitrogen for thermometry (N 2 RIPT) was demonstrated. The RIPT signal is generated by directly probing various rotational levels within the rovibrational absorption band of N 2 , corresponding to the 3-photon transition of N 2 ( X 1 Σ g + , v =0→ b 1 Π u , v ′ =6) near 285 nm, without involving collisional effects of molecular oxygen and nitrogen. The photoionized N 2 produces strong first negative band of N 2 + ( B 2 Σ u + − X 2 Σ g + ) near 390 nm, 420 nm, and 425 nm. Boltzmann analyses of various discrete fluorescence emission lines yield rotational temperatures of molecular nitrogen. By empirically choosing multiple rotational levels within the absorption band, non-scanning thermometry can be accurately achieved for molecular nitrogen. It is demonstrated that the N 2 RIPT technique can measure 1D temperature profile up to ∼5 cm in length within a pure N 2 environment. Multiple wavelengths are thoroughly analyzed and listed that are accurate for RIPT for various temperature ranges.

McCord, Walker (ORCID:0000000179747550)↗

DOE OSTI2024

Argon metastable density and temperature of a 94 GHz microplasma

Laser diode absorption spectroscopy is used to experimentally measure Ar(1s 5 ) metastable density and translational gas temperature within a 94 GHz microplasma. A square two-dimensional photonic crystal (PhC) at this resonance frequency serves to ignite and sustain the plasma from 20 to 200 Torr (2.7 × 10 3 –2.7 × 10 4 Pa) by using millimeter wave power from 300 to 1000 mW. Metastable density within the plasma is estimated from the absorption line shape of the laser traversing the PhC. The metastable density reaches an order of 10 19 m –3 at lower pressure and decreases as pressure increases. From the Lorentzian line shape of the absorption profile at 811.53 nm, the gas temperature is extracted and found to increase from 500 K at 20 Torr to 1300 K at 200 Torr. Furthermore, these data are analyzed and compared with a zero-dimensional plasma model and with previous experimental plasma results at 43 GHz.

42 ENGINEERING↗

DOE OSTI2021

Unraveling the intrinsic atomic physics behind x-ray absorption line shifts in warm dense silicon plasmas

Here, we present a novel free-energy density functional theory (DFT)-based methodology for optical property calculations of warm dense matter to cover a wide range of thermodynamic conditions and photon energies including the entire x-ray range. It uses Mermin–Kohn–Sham density functional theory with exchange-correlation (XC) thermal effects taken into account via a fully temperature dependent generalized gradient approximation XC functional. The methodology incorporates a combination of the ab initio molecular dynamics (AIMD) snapshotted Kubo–Greenwood optic data with a single-atom in simulation cell calculations to close the photon energy gap between the L and K edges and extend the K-edge tail toward many-keV photon energies. This gap arises in the standard scheme due to a prohibitively large number of bands required for the Kubo–Greenwood calculations with AIMD snapshots. Kubo–Greenwood data on snapshots provide an accurate description of optic properties at low photon frequencies slightly beyond the L-edge and x-ray absorption near edges structure (XANES) spectra, while data from periodic calculations with single atoms cover the tail regions beyond the edges. To demonstrate its applicability to mid-Z materials where the standard DFT-based approach is not computationally feasible, we have applied it to opacity calculations of warm dense silicon plasmas. These first-principles calculations revealed a very interesting phenomon of red-to-blue shift in K–L (1s → 2p) and K-edge absorptions along both isotherm and isochore, which are absent in most continuum-lowering models of traditional plasma physics. This new physics phenomenon can be attributed to the underlying competition between the screening of deeply bound core electrons and the screening of outer-shell electrons caused by warm-dense-plasma conditions. We further demonstrate that the ratio of 1s → 2p to the K-edge x-ray absorptions can be used to characterize warm-dense-plasma conditions. Eventually, based on our absorption calculations, we have established a first-principles opacity table (FPOT) for silicon in a wide range of material densities and temperatures.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2023

Splitting photons: Singlet fission in nanocrystal-molecule hybrid structures

The goal of this research is to enable all the energy contained in sunlight to be harvested by making full use of the energy contained in the blue and green wavelengths of light. Current systems are unable to extract all of the energy available from photons in this wavelength range due to rapid relaxation processes that dissipate a fraction of the energy as heat. In this work, inexpensive, earth-abundant components capable of supporting multi-excitonic processes involving more than one tightly bound excited state are investigated as a way to exceed the Shockley-Queisser limit. This research will examine hybrid organic-inorganic nanostructures capable of singlet fission, a process by which one high-energy spin-singlet state is converted into two lower-energy spin-triplet states, and subsequent triplet exciton transfer. Specifically, the organic molecules diphenylhexatriene and tetracene that maximally absorb blue light and are known to exhibit singlet fission will be bound to lead chalcogenide nanocrystals. A variety of steady-state and time-resolved spectroscopic techniques will be used to study the transfer of energy from spin-triplet excitons that are created in the organic molecules to the nanoparticle acceptors. The hybrid nanostructures here will be fully characterized both in solution or thin film via electronic absorption and photoluminescence spectroscopy, nuclear magnetic resonance spectroscopy, high-resolution mass spectrometry, transmission electron microscopy, photoelectron spectroscopy, time correlated single photon counting and transient absorption experiments. The effect of molecular and nanocrystal structure on the electronic coupling between the hybrid components will be examined to establish fundamental relationships between structure and triplet energy transfer efficiency. The findings will be directly applicable to a potential tetracene-silicon platform that may ultimately enhance the power conversion efficiency of silicon solar cells.

30 DIRECT ENERGY CONVERSION↗

DOE OSTI2024

Broadband nonreciprocal thermal emissivity and absorptivity

A body that violates Kirchhoff’s law of thermal radiation exhibits an inequality in its spectral directional absorptivity and emissivity. Achieving such an inequality is of fundamental interest as well as a prerequisite for achieving thermodynamic limits in photonic energy conversion and radiative cooling. Thus far, inequalities in the spectral directional emissivity and absorptivity have been limited to narrow spectral resonances, or wavelengths well beyond the infrared regime4. Bridging the gap from basic demonstrations to practical applications requires control over a broad spectral range of the unequal spectral directional absorptivity and emissivity. In this work, we demonstrate broadband nonreciprocal thermal emissivity and absorptivity by measuring the thermal emissivity and absorptivity of gradient epsilon-near-zero InAs layers of subwavelength thicknesses (50 nm and 150 nm) with an external magnetic field. The effect occurs in a spectral range (12.5–16 μm) that overlaps with the infrared transparency window and is observed at moderate (1 T) magnetic fields.

42 ENGINEERING↗

DOE OSTI2021

Simulating 50 keV X-ray Photon Detection in Silicon with a Down-Conversion Layer

Simulation results are presented that explore an innovative, new design for X-ray detection in the 20–50 keV range that is an alternative to traditional direct and indirect detection methods. Typical indirect detection using a scintillator must trade-off between absorption efficiency and spatial resolution. With a high-Z layer that down-converts incident photons on top of a silicon detector, this design has increased absorption efficiency without sacrificing spatial resolution. Simulation results elucidate the relationship between the thickness of each layer and the number of photoelectrons generated. Further, the physics behind the production of electron-hole pairs in the silicon layer is studied via a second model to shed more light on the detector’s functionality. Together, the two models provide a greater understanding of this detector and reveal the potential of this novel form of X-ray detection.

47 OTHER INSTRUMENTATION↗

DOE OSTI2025

Fast superconducting qubit control with subharmonic drives

Increasing the fidelity of single-qubit gates requires a combination of faster pulses and increased qubit coherence. However, these requirements can be contradictory. Additionally, increasing the drive power can heat the qubit’s environment and degrade coherence. In this work, we circumvent this issue and achieve rapid gates by pumping a transmon’s native Kerr at approximately one third of the qubit’s resonant frequency. The subharmonic Rabi rate of the process is proportional to applied drive amplitude cubed, allowing for rapid gates. In addition, we demonstrate that filtering can be used to protect the qubit’s coherence while performing rapid gates. Single qubit gates as short as 37.4 ns are demonstrated with fidelity of 99.91%. We present theoretical calculations indicating that drive induced multi-photon decay will not limit qubit lifetime; calculated power absorption also indicates that this technique could reduce cryostat heating for fast gates, a vital requirement for large-scale quantum computers.

Xia, Mingkang [Univ. of Pittsburgh, PA (United Sta↗

DOE OSTI2019

Exploring itinerant states in divalent hexaborides using rare-earth L edge resonant inelastic x-ray scattering

We present a study of resonant inelastic x-ray scattering (RIXS) spectra collected at the rare-earth L edges of divalent hexaborides YbB 6 and EuB 6 . In both systems, RIXS-active features are observed at two distinct resonances separated by ~10 eV in incident energy, with angle-dependence suggestive of distinct photon scattering processes. RIXS spectra collected at the divalent absorption peak resemble the unoccupied 5d density of states calculated using density functional theory. We discuss possible origins of this correspondence including a scenario which changes the 4f valence. In addition, anomalous resonant scattering is observed at higher incident energy, where no corresponding absorption feature is present. Our results demonstrate the potential for L-edge RIXS to assess the itinerant-state properties of -electron materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2020

Revisiting supernova constraints on a light CP-even scalar

A light CP-even Standard Model (SM) gauge-singlet scalar S can be produced abundantly in the supernova core, via the nucleon bremsstrahlung process NN → NNS, due to its mixing with the SM Higgs boson. Including the effective S coupling to both nucleons and the pion mediators, we evaluate the production amplitude for the S particle and point out a key difference with the well-known light CP-odd scalar (axion) and vector boson (dark photon) cases. Taking the subsequent decay and re-absorption of S into account, we present a complete calculation of the energy loss rate for the S particle. We then use the SN1987A luminosity constraints to derive updated supernova limits on the mixing of the scalar S with the SM Higgs boson. We find that the mixing angle sin θ with the SM Higgs is excluded only in the narrow range of 3.9 × 10 -7 to 7.0 × 10 -6 , depending on the scalar mass up to about 147 MeV, beyond which the supernova limit disappears.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2023

Time-Resolved Radioluminescence of the Polynuclear Copper(I) Phosphor Cu4I6²–. Different Temporal responses to Photo, X-Ray, β-Ray and α-Particle Excitation

Described for the first time are the time-resolved radioluminescence (TRRL) properties of the highly luminescent copper(I) cluster Cu4I62– using X-ray, b-ray and a-particle excitation. The copper(I) phosphors are two crystalline salts of this anion, [Na2(18-crown-6)2(H2O)3][Cu4I6] (I) and [Li(benzo-15-crown-5)2(H2O)]2[Cu4I6] (II), that had been shown to display strong photoluminescence (PL) when excited with ultraviolet light. The integrated radioluminescence (RL) spectra observed when pulsed X-rays were used as the excitation source are virtually the same as the PL spectra under comparable conditions. These temporal RL spectra are invariant at all observation times indicating that the observed scintillation occurs from a common excited state (or set of excited states). When the TRRL is collected from excitation with a pulsed X-ray source, b-ray decay from 90Sr or a-decay from 244Cm, the longer components (>2 μs) of the TRRL displayed (in each case) lifetimes comparable to those of the strictly exponential PL decays recorded under pulsed laser UV excitation. However, at shorter observation times (< 500 ns), the RL decay deviated from the exponential model, indicating a markedly different temporal luminescence behavior when these materials were excited with pulsed high energy radiation. Furthermore, this effect was the most pronounced for the a-particle excitation. These results suggest that the absorption of a very high energy X-ray photon, b-ray or a-particle at a site within the crystalline solid leads to a high local density of electronic excited states and that coupling between these states provides an alternative channel for excited state decay. Given that the patterns observed

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

DOE OSTI2021

Near-field photonic thermal diode based on hBN and InSb films

A thermal diode is a two-terminal device that allows heat to transfer more easily in one direction (forward bias) than in the opposite direction (reverse bias). A photonic thermal diode operates in a contactless mode and may afford a large operating temperature range. Here, a near-field photonic thermal diode based on hexagonal boron nitride (hBN) and indium antimonide (InSb) films is theoretically demonstrated. In this work, the temperature dependence of the interband absorption of InSb is used to couple (or decouple) with the hyperbolic phonon polaritons in hBN. The numerical analysis predicts a rectification ratio greater than 17 for a 10 nm vacuum gap, when operating at an average temperature of 300 K and a temperature difference of 200 K. The calculated rectification ratio exceeds 35 at higher average temperatures with larger temperature differences.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

DOE OSTI2020

Hard X-ray Fluorescence measurements with TESs at the Advanced Photon Source

Transition Edge Sensor (TES) spectrometers for hard X-ray beamline science will enable improved X-ray emission and absorption spectroscopy in the information-rich 2 to 20keV energy range. We are building a TES-based instrument for time Advanced Photon Source (APS) synchrotron, to be made available to beamline users. 24-pixel prototype arrays have recently been fabricated and tested. the first, spectroscopy measurements using these arrays are promising, with a best single-pixel energy resolution of 11.2 eV and saturation energy > 20 keV. We present a series of recent X-ray Fluorescence measurements involving transition metal elements and multi-element samples with closely spaced emission lines, in particular a Cu-Ni-Co thin film and a foil of Cu and Hf, The TES-measured spectra are directly compared to spectra measured with silicon drift detectors at an APS beamline, demonstrating the improved X-ray science made possible by TES spectrometers.

Guruswamy, Tejas↗

DOE OSTI2026

Dehydration Pathway Study of Ultrathin Ni (OH) 2 Probed via In Situ X-Ray Photoelectron Spectromicroscopy

In this work, the conversion of ultrathin 2D-Ni (OH) 2 to NiO is studied using in situ X-ray absorption near edge spectroscopy at the Ni L 3 and O K edges and using variable photon energy X-ray photoelectron spectroscopy at the Ni 2p 3/2 and O 1s edges. The Ni L 3 X-ray absorption spectroscopy and corresponding 2p 3/2 X-ray photoelectron spectroscopy show the oxidation state of the Ni atom to be Ni 2+ in the course of the reaction; however, the film surface and oxygen defect structure show the presence of a large metallic Ni component before the complete disappearance of the hydroxide phase indicating oxygen vacancy formation before the completion of water desorption. O 1s spectral changes during heat treatment under ultrahigh vacuum, O 2 dosing, and H 2 O dosing suggest the spectral features are due to water desorption and adsorption. Furthermore, by comparing the relative probe depths of X-ray photoelectron spectroscopy and X-ray absorption spectroscopy, it is determined that the surface, at each step in the dehydration process, consists of a combination of Ni, NiO, and Ni (OH) 2 phases, which each contain a mixture of adsorbed hydroxyl groups. Repeated dosing with H 2 O, studied with O 1s X-ray photoelectron spectroscopy, suggests that the dissociation of water facilitates the formation of oxygen vacancies.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Beating absorption in solid-state high harmonics

Since the new millennium coherent extreme ultra-violet and soft x-ray radiation has revolutionized the understanding of dynamical physical, chemical and biological systems at the electron’s natural timescale. Unfortunately, coherent laser-based upconversion of infrared photons to vacuum-ultraviolet and soft x-ray high-order harmonics in gaseous, liquid and solid targets is notoriously inefficient. In dense nonlinear media, the limiting factor is strong re-absorption of the generated high-energy photons. Here we overcome this limitation by generating high-order harmonics from a periodic array of thin one-dimensional crystalline silicon ridge waveguides. Adding vacuum gaps between the ridges avoids the high absorption loss of the bulk and results in a ~ 100-fold increase of the extraction depth. As the grating period is varied, each high harmonic shows a different and marked modulation, indicating their waveguiding in the vacuum slots with reduced absorption. Looking ahead, our results enable bright on-chip coherent short-wavelength sources and may extend the usable spectral range of traditional nonlinear crystals to their absorption windows. Potential applications include on-chip chemically-sensitive spectro-nanoscopy.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗