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DOE OSTI2020

Spectral Radiative Properties of Ceramic Particles for Concentrated Solar Thermal Energy Storage Applications

This work investigates the spectral radiative properties of ceramic particles using a monochromator and a Fourier-transform infrared spectrometer (FTIR) with integrating spheres at wavelengths from 0.38 μm to 15 μm. Particles are encased between two transparent windows to obtain the directional-hemispherical reflectance of the particle bed. Two types of commercially available particles with three different sizes are examined. Integration over the solar spectrum reveals that the solar absorptance of the particle beds is between 0.940 and 0.957. The total emittance at 1000 K is also estimated by assuming the spectral emittance is independent of temperature. The optical constants of particles are modeled with effective medium approaches, considering the optical properties of individual constituent materials. The absorptance of the particle is estimated using the effective optical constants and compared with that of the particle bed from the measurement. Finally, this work facilitates the characterization of radiative properties of particles with a windowed method and provides a modeling scheme for approximating the radiative properties of composite ceramic materials.

14 SOLAR ENERGY↗

DOE OSTI2021

Effect of heterostructure engineering on electronic structure and transport properties of two-dimensional halide perovskites

Organic-inorganic halide perovskite solar cells have attracted much attention due to their low-cost fabrication, flexibility, and high-power conversion efficiency. More recent efforts show that the reduction from three- to two-dimensions (2D) of organic–inorganic halide perovskites promises an exciting opportunity to tune their electronic properties. Here, we explore the effect of reduced dimensionality and heterostructure engineering on the intrinsic material properties, such as energy stability, bandgap and transport properties of 2D hybrid organic–inorganic halide perovskites using first-principles density functional theory. We show that the energy stability of engineered perovskite heterostructures is significantly enhanced. The heterostructures with improved stability also show excellent transport properties similar to their bulk counterparts. Furthermore, these layered chemistries demonstrate the advantage of a broad range of tunable bandgaps and high-absorption coefficient in the visible spectrum. The proposed 2D heterostructured material holds potential for nano-optoelectronic devices as well as for effective photovoltaics.

36 MATERIALS SCIENCE↗

DOE OSTI2020

The Photoactive Excited State of the B 12 -Based Photoreceptor CarH

In this study we have used transient absorption spectroscopy in the UV–visible and X-ray regions to characterize the excited state of CarH, a protein photoreceptor that uses a form of B 12 , adenosylcobalamin (AdoCbl), to sense light. With visible excitation, a nanosecond-lifetime photoactive excited state is formed with unit quantum yield. The time-resolved X-ray absorption near edge structure difference spectrum of this state demonstrates that the excited state of AdoCbl in CarH undergoes only modest structural expansion around the central cobalt, a behavior similar to that observed for methylcobalamin rather than for AdoCbl free in solution. We propose a new mechanism for CarH photoreactivity involving formation of a triplet excited state. This allows the sensor to operate with high quantum efficiency and without formation of potentially dangerous side products. By stabilizing the excited electronic state, CarH controls reactivity of AdoCbl and enables slow reactions that yield nonreactive products and bypass bond homolysis and reactive radical species formation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Turning dead leaves into an active multifunctional material as evaporator, photocatalyst, and bioplastic

Large numbers of leaves fall on the earth each autumn. The current treatments of dead leaves mainly involve completely destroying the biocomponents, which causes considerable energy consumption and environmental issues. It remains a challenge to convert waste leaves into useful materials without breaking down their biocomponents. Here, we turn red maple dead leaves into an active three-component multifunctional material by exploiting the role of whewellite biomineral for binding lignin and cellulose. Owing to its intense optical absorption spanning the full solar spectrum and the heterogeneous architecture for effective charge separation, films of this material show high performance in solar water evaporation, photocatalytic hydrogen production, and photocatalytic degradation of antibiotics. Furthermore, it also acts as a bioplastic with high mechanical strength, high-temperature tolerance, and biodegradable features. These findings pave the way for the efficient utilization of waste biomass and innovations of advanced materials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Simultaneous quantification of uranium( VI ), samarium, nitric acid, and temperature with combined ensemble learning, laser fluorescence, and Raman scattering for real-time monitoring

In this work, laser-induced fluorescence spectroscopy (LIFS), Raman spectroscopy, and a stacked regression ensemble was developed for near real-time quantification of uranium(VI) (1–100 μg mL –1 ), samarium (0–200 μg mL –1 ) and nitric acid (0.1–4 M) with varying temperature (20 °C–45 °C). LIFS applications range from fundamental lab-scale studies to real-time process monitoring at industrial levels, such as nuclear reprocessing applications, provided the phenomena affecting the fluorescence spectrum are accounted for (e.g., absorption, quenching, complexation). Multiple chemometric models were examined and compared to a more traditional multivariate regression approach called partial least squares (PLS). Results obtained on synthetic samples selected using D-optimal experimental design indicated that a stacked regression method, which included ridge regression, random forest, PLS, and an eXtreme gradient boost algorithm, successfully measured uranium(VI) concentrations directly in nitric acid without measuring luminescence lifetimes or standard addition. The top model resulted in percent root-mean-square error of prediction values of 5.2, 1.9, 3.0, and 2.3% for U(VI), Sm 3+ , HNO 3 , and temperature, respectively. The approach may be useful for quantifying fluorescent fission products (e.g., Sm 3+ ) to provide information on burnup of irradiated nuclear fuel. This novel framework reinforces the applicability of LIFS for real-time applications in nuclear fuel cycle applications.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

DOE OSTI2024

Design and characterization of the time-resolved opacity spectrometer (OpSpecTR) for the NIF iron opacity campaign

A new time-resolved opacity spectrometer (OpSpecTR) is currently under development for the National Ignition Facility (NIF) opacity campaign. Here, the spectrometer utilizes Icarus version 2 (IV2) hybridized complementary metal–oxide–semiconductor sensors to collect gated data at the time of the opacity transmission signal, unlocking the ability to collect higher-temperature measurements on NIF. Experimental conditions to achieve higher temperatures are feasible; however, backgrounds will dominate the data collected by the current time-integrating opacity spectrometer. The shortest available OpSpecTR integration time of ~2 ns is predicted to reduce self-emission and other late-time backgrounds by up to 80%. Initially, three Icarus sensors will be used to collect data in the self-emission, backlighter, and absorption regions of the transmission spectrum, with plans to upgrade to five Daedalus sensors in future implementations with integration times of ~1.3 ns. We present the details of the diagnostic design along with recent characterization results of the IV2 sensors.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2024

1.1 eV GaInAs Cell Development for Dual-Use Solar and 1070 nm Laser Power Converters

Dual-use power converter cells can receive solar and laser power simultaneously to generate current, an application relevant to space and terrestrial industries. This study investigates two concepts of solar cells optimized for dual-use 1070 nm laser and solar power conversion, a single-junction and triple-junction cell. Because it is bandgap-tuned for a 1070 nm laser, the 1.1 eV junction is incorporated into each of the two designs, making its development key to the success of both concepts. Efficiency data for a one junction GaInAs cell demonstrates a laser conversion efficiency of 38% at 1070nm wavelength without an anti-reflection coating. However, the single-junction device requires optimization to reduce short wavelength absorption of the broad solar spectrum. In both devices, the graded buffer layers in the GaInAs cell affects the cell's performance by reducing threading dislocations in the active junction. However, the buffer in the three-junction device also acts as a lateral transport layer and so affects the fill factor depending on its sheet resistance. By varying the buffer thickness, we demonstrate a direct relationship between buffer thickness and sheet resistance reduction, while considering implications to open-circuit voltages. We also performed resistance modeling to determine the optimal grid spacing and thickness of the grid fingers to minimize losses due to sheet resistance and grid shading.

junctions↗

DOE OSTI2025

1.1 eV GaInAs Cell Development for Dual-Use Solar and 1070 nm Laser Power Converters

Dual-use photovoltaic cells can receive solar and laser power simultaneously to generate current, an application relevant to space and terrestrial industries. This study investigates two concepts of solar cells optimized for dual-use 1070 nm laser and solar power conversion, a single-junction and triple-junction cell. The cell designs are based upon the 3- junction inverted metamorphic solar cell, previously shown highly efficient for solar conversion. Because it is closely bandgap-tuned for a 1070 nm laser, the 1 eV bottom junction is incorporated into each of the two designs, making its development key to the success of both concepts. However, each design requires some modification for efficient dual use. The single-junction device requires optimization to reduce short wavelength absorption of the broad solar spectrum. In both devices, the graded buffer layers in the GaInAs cell affect the cell's performance by reducing threading dislocations in the active junction. However, the buffer in the three-junction device also acts as a lateral transport layer and so affects the fill factor depending on its sheet resistance. By varying the buffer thickness, we demonstrate a direct relationship between buffer thickness and sheet resistance reduction, while considering implications to open-circuit voltages. We also performed resistance modeling to determine the optimal grid spacing and thickness of the grid fingers to minimize losses due to sheet resistance and grid shading. Efficiency data for a one junction GaInAs cell demonstrates a laser conversion efficiency of 38% at 1070 nm wavelength without an anti-reflection coating.

dual-use↗

DOE OSTI2020

ARES. III. Unveiling the Two Faces of KELT-7 b with HST WFC3

We present the analysis of the hot-Jupiter KELT-7 b using transmission and emission spectroscopy from the Hubble Space Telescope, both taken with the Wide Field Camera 3. Our study uncovers a rich transmission spectrum that is consistent with a cloud-free atmosphere and suggests the presence of H{sub 2}O and H{sup −}. In contrast, the extracted emission spectrum does not contain strong absorption features and, although it is not consistent with a simple blackbody, it can be explained by a varying temperature–pressure profile, collision induced absorption, and H{sup −}. KELT-7 b had also been studied with other space-based instruments and we explore the effects of introducing these additional data sets. Further observations with Hubble, or the next generation of space-based telescopes, are needed to allow for the optical opacity source in transmission to be confirmed and for molecular features to be disentangled in emission.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2022

Record Efficiency Multijunction Solar Cells with Strain-Balanced Quantum Well Superlattices

The absorption edge of a GaAs solar cell can be tuned to longer wavelengths with strain-balanced quantum wells, as an alternative to metamorphic epitaxy. For one-sun photovoltaic applications, an optimum bandgap for both single and multijunction solar cells is near the broad water absorption peak at 930 nm and can be accessed by a Ga0.9In0.1As alloy. This alloy is strained with respect to the GaAs substrate, and so only very thin ~10 nm layers can be grown without relaxation via dislocation formation. However, solar cells require significant thickness for complete absorption of the incoming solar spectrum, requiring many such layers. We have designed quantum well superlattices with up to 300 sets of carefully tuned strain-balanced GaInAs/GaAsP pairs by limiting composition modulation and material degradation. We have incorporated quantum well solar cells into multijunction devices to achieve record 32.9% two-junction and 39.5% three-junction solar cells under standard one-sun illumination. We will describe the physics of the quantum well devices and the growth conditions that lead to sharp interfaces and good material quality, as well as the characterization of the efficiencies.

GaAs↗

DOE OSTI2024

1.1 eV GaInAs Cell Development for Dual-Use Solar and 1075 nm Laser Power Converters

Dual-use power converter cells can receive solar and laser power simultaneously to generate current, an application relevant to space and terrestrial industries. This study investigates two concepts of solar cells optimized for dual- use 1070 nm laser and solar power conversion, a single-junction and triple-junction cell. Because it is bandgap-tuned for a 1070 nm laser, the 1.1 eV junction is incorporated into each of the two designs, making its development key to the success of both concepts. Efficiency data for a one junction GaInAs cell demonstrates a laser conversion efficiency of 38% at 1070nm wavelength without an anti-reflection coating. However, the single-junction device requires optimization to reduce short wavelength absorption of the broad solar spectrum. In both devices, the graded buffer layers in the GaInAs cell affects the cell's performance by reducing threading dislocations in the active junction. However, the buffer in the three-junction device also acts as a lateral transport layer and so affects the fill factor depending on its sheet resistance. By varying the buffer thickness, we demonstrate a direct relationship between buffer thickness and sheet resistance reduction, while considering implications to open-circuit voltages. We also performed resistance modeling to determine the optimal grid spacing and thickness of the grid fingers to minimize losses due to sheet resistance and grid shading.

dual-use↗

DOE OSTI2023

Optical spectral observations of three binary millisecond pulsars

We present the results of optical spectroscopy of stellar companions to three binary millisecond pulsars, PSRs J0621+2514, J2317+1439, and J2302+4442, obtained with the Gran Telescopio Canarias. The spectrum of the J0621+2514 companion shows a blue continuum and prominent Balmer absorption lines. The latter are also resolved in the spectrum of the J2317+1439 companion, showing that both are DA-type white dwarfs. No spectral features are detected for the J2302+4442 companion; however, its broad-band magnitudes and the spectral shape of the continuum emission imply that this is also a DA-type white dwarf. Based on the spectral analyses, we conclude that the companions of J0621+2514 and J2317+1439 are relatively hot, with effective temperatures T eff = 8600 ± 200 and 9600 ± 2000 K, respectively, while the J2302+4442 companion is significantly cooler, T eff <6000 K. We also estimated the distance to J0621+2514 of 1.1 ± 0.3 kpc and argue that its companion and the companion of J2317+1439 are He-core white dwarfs providing constraints on their cooling ages of $\lesssim$2 Gyr.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2022

Autodifferentiable Spectrum Model for High-dispersion Characterization of Exoplanets and Brown Dwarfs

We present an autodifferentiable spectral modeling of exoplanets and brown dwarfs. This model enables a fully Bayesian inference of the high-dispersion data to fit the ab initio line-by-line spectral computation to the observed spectrum by combining it with the Hamiltonian Monte Carlo in recent probabilistic programming languages. An open-source code, ExoJAX, developed in this study, was written in Python using the GPU/TPU compatible package for automatic differentiation and accelerated linear algebra, JAX. We validated the model by comparing it with existing opacity calculators and a radiative transfer code and found reasonable agreements for the output. As a demonstration, we analyzed the high-dispersion spectrum of a nearby brown dwarf, Luhman 16 A, and found that a model including water, carbon monoxide, and H 2 /He collision-induced absorption was well fitted to the observed spectrum (R = 10 5 and 2.28-2.30 μm). As a result, we found that T0 = 1295$^{-32}_{+35}$ K at 1 bar and C/O = 0.62 ± 0.03, which is slightly higher than the solar value. This work demonstrates the potential of a full Bayesian analysis of brown dwarfs and exoplanets as observed by high-dispersion spectrographs and also directly imaged exoplanets as observed by high-dispersion coronagraphy.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2020

The 1.66 μm spectrum of the ethynyl radical, CCH

Frequency-modulated diode laser transient absorption spectra of the ethynyl radical have been recorded at wavelengths close to 1.66 μm. The observed spectrum includes strong, regular, line patterns. The two main bands observed originate in the ground $\tilde{χ}$ 2 Σ + state and its first excited bending vibrational level of 2 $Π$ symmetry. The upper states, of 2 Σ + symmetry at 6055.6 cm -1 and 2 $Π$ symmetry at 6413.5 cm -1 , respectively, had not previously been observed and the data were analyzed in terms of an effective Hamiltonian representing their rotational and fine structure levels to derive parameters which can be used to calculate rotational levels up to J = 37/2 for the 2 $Π$ level and J = 29/2 for the 2 Σ one. Additionally, a weaker series of lines have been assigned to absorption from the second excited bending, (0 2 0), level of 2 Σ symmetry, to a previously observed state of 2 $Π$ symmetry near 6819 cm -1 . These strong absorption bands at convenient near-IR laser wavelengths will be useful for monitoring CCH radicals in chemical systems.

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2021

Optimal 1D Ly α forest power spectrum estimation – II. KODIAQ, SQUAD, and XQ-100

ABSTRACT We measure the 1D Ly α power spectrum P1D from Keck Observatory Database of Ionized Absorption toward Quasars (KODIAQ), The Spectral Quasar Absorption Database (SQUAD), and XQ-100 quasars using the optimal quadratic estimator. We combine KODIAQ and SQUAD at the spectrum level, but perform a separate XQ-100 estimation to control its large resolution corrections in check. Our final analysis measures P1D at scales k < 0.1 s km−1 between redshifts $z$ = 2.0–4.6 using 538 quasars. This sample provides the largest number of high-resolution, high-S/N observations; and combined with the power of optimal estimator it provides exceptional precision at small scales. These small-scale modes (k ≳ 0.02 s km−1), unavailable in Sloan Digital Sky Survey and Dark Energy Spectroscopic Instrument analyses, are sensitive to the thermal state and reionization history of the intergalactic medium, as well as the nature of dark matter. As an example, a simple Fisher forecast analysis estimates that our results can improve small-scale cut-off sensitivity by more than a factor of 2.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2024

Impact of Self-shielding Minihalos on the Lyα Forest at High Redshift

Abstract Dense gas in minihalos with masses of 10 6 −10 8 M ⊙ can shield themselves from reionization for ∼100 Myr after being exposed to the UV background. These self-shielded systems, often unresolved in cosmological simulations, can introduce strong absorption in quasar spectra. This paper is the first systematic study on the impact of these systems on the Ly α forest. We first derive the H i column density profile of photoevaporating minihalos by conducting 1D radiation–hydrodynamics simulations. We utilize these results to estimate the Ly α opacity from minihalos in a large-scale simulation that cannot resolve self-shielding. When the ionization rate of the background radiation is 0.03 × 10 −12 s −1 , as expected near the end of reionization at z ∼ 5.5, we find that the incidence rate of damped Ly α absorbers increases by a factor of ∼2−4 compared to at z = 4.5. The Ly α flux is, on average, suppressed by ∼3% of its mean due to minihalos. The absorption features enhance the 1D power spectrum up to ∼5% at k ∼ 0.1 h Mpc −1 (or 10 −3 km −1 s), which is comparable to the enhancement caused by inhomogeneous reionization. The flux is particularly suppressed in the vicinity of large halos along the line-of-sight direction at separations of up to 10 h −1 Mpc at r ⊥ ≲ 2 h −1 Mpc. However, these effects become much smaller for higher ionizing rates (≳0.3 × 10 −12 s −1 ) expected in the post-reionization Universe. Our findings highlight the need to consider minihalo absorption when interpreting the Ly α forest at z ≳ 5.5. Moreover, the sensitivity of these quantities to the ionizing background intensity can be exploited to constrain the intensity itself.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2022

Systems and methods for radiative cooling and heating

Systems and methods for radiative cooling and heating are provided. For example, systems for radiative cooling can include a top layer including one or more polymers, where the top layer has high emissivity in at least a portion of the thermal spectrum and an electromagnetic extinction coefficient of approximately zero, absorptivity of approximately zero, and high transmittance in at least a portion of the solar spectrum, and further include a reflective layer including one or more metals, where the reflective layer has high reflectivity in at least a portion of the solar spectrum.

Yu, Nanfang↗

DOE OSTI2023

Systems and methods for radiative cooling and heating

Yu, Nanfang↗