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DOE OSTI2023

Photoreactive Carbon Dioxide Capture by a Zirconium–Nanographene Metal–Organic Framework

Here, the mechanism of photochemical CO 2 reduction to formate by PCN-136, a Zr-based metal-organic framework (MOF) that incorporates light-harvesting nanographene ligands, has been investigated using steady-state and time-resolved spectroscopy and density functional theory (DFT) calculations. The catalysis was found to proceed via a "photoreactive capture" mechanism, where Zr-based nodes serve to capture CO 2 in the form of Zr- bicarbonates, while the nanographene ligands have a dual role of absorbing light and storing one-electron equivalents for catalysis. We also find that the process occurs via a "two-for-one" route, where a single photon initiates a cascade of electron/hydrogen atom transfers from the sacrificial donor to the CO 2 -bound MOF. The mechanistic findings obtained here illustrate several advantages of MOF-based architectures in molecular photocatalyst engineering and provide insights on ways to achieve high formate selectivity.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

Temperature-adaptive radiative coating for all-season household thermal regulation

The sky is a natural heat sink that has been extensively used for passive radiative cooling of households. A lot of focus has been on maximizing the radiative cooling power of roof coating in the hot daytime using static, cooling-optimized material properties. However, the resultant overcooling in cold night or winter times exacerbates the heating cost, especially in climates where heating dominates energy consumption. In this work, we approached thermal regulation from an all-season perspective by developing a mechanically flexible coating that adapts its thermal emittance to different ambient temperatures. The fabricated temperature-adaptive radiative coating (TARC) optimally absorbs the solar energy and automatically switches thermal emittance from 0.20 for ambient temperatures lower than 15°C to 0.90 for temperatures above 30°C, driven by a photonically amplified metal-insulator transition. Simulations show that this system outperforms existing roof coatings for energy saving in most climates, especially those with substantial seasonal variations.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

DOE OSTI2022

Ultrafast carrier dynamics in terahertz photoconductors and photomixers: beyond short-carrier-lifetime semiconductors

Abstract Efficient terahertz generation and detection are a key prerequisite for high performance terahertz systems. Major advancements in realizing efficient terahertz emitters and detectors were enabled through photonics-driven semiconductor devices, thanks to the extremely wide bandwidth available at optical frequencies. Through the efficient generation and ultrafast transport of charge carriers within a photo-absorbing semiconductor material, terahertz frequency components are created from the mixing products of the optical frequency components that drive the terahertz device – a process usually referred to as photomixing. The created terahertz frequency components, which are in the physical form of oscillating carrier concentrations, can feed a terahertz antenna and get radiated in case of a terahertz emitter, or mix with an incoming terahertz wave to down-convert to DC or to a low frequency photocurrent in case of a terahertz detector. Realizing terahertz photoconductors typically relies on short-carrier-lifetime semiconductors as the photo-absorbing material, where photocarriers are quickly trapped within one picosecond or less after generation, leading to ultrafast carrier dynamics that facilitates high-frequency device operation. However, while enabling broadband operation, a sub-picosecond lifetime of the photocarriers results in a substantial loss of photoconductive gain and optical responsivity. In addition, growth of short-carrier-lifetime semiconductors in many cases relies on the use of rare elements and non-standard processes with limited accessibility. Therefore, there is a strong motivation to explore and develop alternative techniques for realizing terahertz photomixers that do not rely on these defect-introduced short-carrier-lifetime semiconductors. This review will provide an overview of several promising approaches to realize terahertz emitters and detectors without short-carrier-lifetime semiconductors. These novel approaches utilize p-i-n diode junctions, plasmonic nanostructures, ultrafast spintronics, and low-dimensional materials to offer ultrafast carrier response. These innovative directions have great potentials for extending the applicability and accessibility of the terahertz spectrum for a wide range of applications.

36 MATERIALS SCIENCE↗

NASA NTRS1998

Theoretical Studies of Starburst Infrared Emission: Luminosity Indicators in Dusty Photoionized Environments

The luminosity of the central source in ionizing radiation is an essential parameter in a photoionized environment and is one of the most fundamental physical quantities one can measure. We outline a method of determining the luminosity for any emission-line region using only infrared data. In dusty environments, grains compete with hydrogen in absorbing continuum radiation. Grains produce infrared emission, and hydrogen produces recombination lines. We have computed a very large variety of photoionization models, using ranges of abundances, grain mixtures, ionizing continua, densities, and ionization parameters. The conditions were appropriate for such diverse objects as H(II) regions, planetary nebulae, starburst galaxies, and the narrow- and broad-line regions of active nuclei. The ratio of the total thermal grain emission relative to H-Beta (IR/H-Beta) is the primary indicator of whether the cloud behaves as a classical Stroemgren sphere (a hydrogen-bounded nebula) or whether grains absorb most of the incident continuum (a dust-bounded nebula). We find two global limits: when IR/H-Beta < 100, infrared recombination lines determine the source luminosity in ionizing photons; when IR/H-Beta >> 100, the grains act as a bolometer to measure the luminosity.

Bottorff, Mark↗

NASA NTRS1999

Accuracy of the Independent Pixel Approximation at Absorbing Wavelengths

In order to correctly interpret shortwave cloud radiation measured by satellites and ground-based radiometers, or by two aircraft flying above and below clouds, we need to better understand interactions between inhomogeneous clouds and solar radiation. The discrepancies between shortwave absorption inferred from measurements and predicted by models, between cloud optical depths estimated from satellites and ground measurements, between single scattering albedo retrieved from in situ radiation measurements and computed from measured droplet size distribution, among others, are strongly affected by cloud horizontal inhomogeneity. Net horizontal photon transport (i. e., horizontal fluxes) are a direct consequence of the inhomoqeneity in cloud structure. Horizontal fluxes and their effect on the accuracy of the pixel-by-pixel one-dimensional (1 D) radiative transfer calculations has recently undergone close scrutiny for conservative scattering. However, the properties and magnitude of horizontal fluxes in absorbing wavelengths are still poorly understood. As far as we are aware, only Ackerman and Cox and Titov discussed correlations between horizontal fluxes at absorbing wavelengths, though these were far from comprehensive. This paper partly fills this gap. We discuss here of whether the accuracy of the Independent Pixel Approximation (IPA), a 1 D radiative transfer approximation for each pixel, is a better model for multiple scattering at conservative or at absorbing wavelengths. Issues addressed here are: (1) dependence of net horizontal fluxes on single scattering albedo; (2) connection between pixel-by-pixel accuracy of the IPA and horizontal fluxes and (3) radiative smoothing and horizontal fluxes at absorbing wavelengths. In contrast to the traditional understanding of IPA, we study IPA accuracies not only for reflectance but also for transmittance and absorptance at both conservative and absorbing wavelengths. In spite of the apparent similarity between the three processes, dependence of IPA accuracies on single-scattering albedo is completely different. As a result, cloud optical properties retrieved from high resolution satellite images and ground-based measurements using IPA at absorbing channels will have different accuracies.

Marchak, Alexander↗

DOE OSTI2021

Optimization of four terminal rear heterojunction GaAs on Si interdigitated back contact tandem solar cells

High-efficiency, four-terminal tandem solar cells composed of thin GaAs films mechanically stacked onto interdigitated back contact silicon solar cells with a glass interlayer are demonstrated. The optimal thickness of the absorber layer of a rear heterojunction GaAs subcell for use in four terminal tandem solar cells was studied. GaAs top cells with absorber layer thicknesses of 1.5, 1.9, 2.3, 2.8, and 3.5 µm were fabricated on glass and mechanically stacked onto interdigitated back-contact Si bottom cells. All tandem cells were found to have efficiencies above 30% under the AM1.5 G spectrum demonstrating a relatively weak sensitivity to thickness in the four-terminal configuration. We found the 2.8 µm absorber layer cell to have the highest top cell and tandem cell efficiency at 26.38% and 32.57%, respectively. Optical modeling with transfer matrix method for the planar top cell and Lambertian light trapping in the textured Si subcell, along with drift-diffusion Hovel equations, were used to show photon recycling enhancement to the effective diffusion length and VOC of the top cell as a result of the low-index glass interlayer.

14 SOLAR ENERGY↗

DOE OSTI2021

Violating Kirchhoff’s Law of Thermal Radiation in Semitransparent Structures

Kirchhoff’s law of thermal radiation imposes a constraint on photon-based energy harvesting processes since part of the incident energy flux is inevitably emitted back to the source. By breaking the reciprocity of the system, it is possible to overcome this restriction and improve the efficiency of energy harvesting. Here, we design and analyze a semitransparent emitter that fully absorbs normally incident energy from a given direction with zero backward and unity forward emissivity. The nearly ideal performance with wavelength-scale thickness is achieved due to the magneto-optical effect and the guided-mode resonance engineered in the emitter structure. We derive the general requirements for the nonreciprocal emitter using the temporal coupled mode theory and the symmetry considerations. As a result, we provide a realistic emitter design based on a photonic crystal slab consisting of a magnetic Weyl semimetal and silicon.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Decoupling absorption and radiative cooling in mid-wave infrared bolometric elements

We present a spectrally selective, passively cooled mid-wave infrared bolometric absorber engineered to spatially and spectrally decouple infrared absorption and thermal emission. The structure leverages an antenna-coupled metal–insulator–metal resonance for mid-wave infrared normal incidence photon absorption and a long-wave infrared optical phonon absorption feature, aligned closer to peak room temperature thermal emission. The phonon-mediated resonant absorption enables a strong long-wave infrared thermal emission feature limited to grazing angles, leaving the mid-wave infrared absorption feature undisturbed. The two independently controlled absorption/emission phenomena demonstrate decoupling of the photon detection mechanism from radiative cooling and offer a new design approach enabling ultra-thin, passively cooled mid-wave infrared bolometers.

Ware, Alexander (ORCID:0009000256937727)↗

NASA NTRS2013

An Archival Chandra and XMM-Newton Survey of Type 2 Quasars

In order to investigate obscuration in high-luminosity type 2 active galactic nuclei (AGNs), we analyzed Chandra and XMM-Newton archival observations for 71 type 2 quasars detected at 0.05 < z < 0.73, which were selected based on their [O III] lambda5007 emission lines. For 54 objects with good spectral fits, the observed hard X-ray luminosity ranges from 2 × 10(exp 41) to 5.3 × 10(exp 44) erg s(exp −1), with a median of 1.1 × 10(exp 43) erg s(exp −1). We find that the means of the column density and photon index of our sample are log N(sub H) = 22.9 cm(exp −2) and gamma = 1.87, respectively. From simulations using a more physically realistic model, we find that the absorbing column density estimates based on simple power-law models significantly underestimate the actual absorption in approximately half of the sources. Eleven sources show a prominent Fe K alpha emission line (EW>100 eV in the rest frame) and we detect this line in the other sources through a joint fit (spectral stacking). The correlation between the Fe K alpha and [O III] fluxes and the inverse correlation of the equivalent width of the Fe Kα line with the ratio of hard X-ray and [O III] fluxes is consistent with previous results for lower luminosity Seyfert 2 galaxies. We conclude that obscuration is the cause of the weak hard X-ray emission rather than intrinsically low X-ray luminosities. We find that about half of the population of optically selected type 2 quasars are likely to be Compton thick. We also find no evidence that the amount of X-ray obscuration depends on the AGN luminosity (over a range of more than three orders of magnitude in luminosity).

quasars: general↗

NASA NTRS2018

Lyman-Alpha Comes of Age

The Lyman-alpha (Lyα) line is the strongest recombination line of hydrogen, which constitutes the dominant share of normal matter in the Universe. Fifty-one years ago, it was predicted that Lyα emission should appear prominently in the spectra of young primordial galaxies. For the next 30 years, this prediction was tested by many surveys, but none found the predicted galaxies at the predicted luminosities. The blame for these non-detections was squarely cast on the resonant nature of the Lyα line, which requires Lyα photons to scatter off many hydrogen atoms before escaping from a galaxy. This can hugely increase the path that they traverse, and consequently also the probability that they will be absorbed by dust. This remained the dominant explanation of the missing high-redshift lines for decades, despite some dissenting opinions about the effect of dust. The spectra of nearby galaxies from the International Ultraviolet Explorer are inconclusive about what allows galaxies to be Lyα emitters. The ‘missing’ lines were finally detected 20 years ago, at flux levels much below the original predictions - a difference that we understand to be predominantly due to the hierarchical growth of galaxies, such that star-forming objects at high redshift are much less massive than anticipated in the original prediction. The discovery and study of Lyα galaxies has blossomed into an invaluable method for understanding the youngest stages of galaxy formation, the circumgalactic medium, and ultimately the epoch of reionization. The high equivalent widths of Lyα galaxies from the earliest high-redshift surveys show that they are low-mass galaxies dominated by young stellar populations. The Sakura CLAW workshop (which used the Twitter hashtag #SakuraCLAW) gathered more than 110 participants (Fig. 1) who showcased progress that pushed the frontiers of Lyα galaxy science in sample size, sensitivity, redshifts and physical understanding..

Malhotra, Sangeeta↗

DOE OSTI2020

Synchrotron characterization of high-Z, current-mode x-ray detectors

Fast x-ray detectors are critical tools in pulsed power and fusion applications, where detector impulse response of a nanosecond or better is often required. Semiconductor detectors can create fast, sensitive devices with extensive operational flexibility. There is typically a trade-off between detector sensitivity and speed, but higher atomic number absorbers can increase hard x-ray absorption without increasing the charge collection time, provided carriers achieve high velocity. This paper presents x-ray pulse characterization conducted at the Advanced Photon Source of x-ray absorption efficiency and temporal impulse response of current-mode semiconductor x-ray detectors composed of Si, GaAs, and CdTe.

47 OTHER INSTRUMENTATION↗

NASA NTRS2006

Long-Wavelength Infrared (LWIR) Quantum Dot Infrared Photodetector (QDIP) Focal Plane Array

We have exploited the artificial atomlike properties of epitaxially self-assembled quantum dots for the development of high operating temperature long wavelength infrared (LWIR) focal plane arrays. Quantum dots are nanometer-scale islands that form spontaneously on a semiconductor substrate due to lattice mismatch. QDIPs are expected to outperform quantum well infrared detectors (QWIPs) and are expected to offer significant advantages over II-VI material based focal plane arrays. QDIPs are fabricated using robust wide bandgap III-V materials which are well suited to the production of highly uniform LWIR arrays. We have used molecular beam epitaxy (MBE) technology to grow multi-layer LWIR quantum dot structures based on the InAs/InGaAs/GaAs material system. JPL is building on its significant QWIP experience and is basically building a Dot-in-the-Well (DWELL) device design by embedding InAs quantum dots in a QWIP structure. This hybrid quantum dot/quantum well device offers additional control in wavelength tuning via control of dot-size and/or quantum well sizes. In addition the quantum wells can trap electrons and aide in ground state refilling. Recent measurements have shown a 10 times higher photoconductive gain than the typical QWIP device, which indirectly confirms the lower relaxation rate of excited electrons (photon bottleneck) in QDPs. Subsequent material and device improvements have demonstrated an absorption quantum efficiency (QE) of approx. 3%. Dot-in-the-well (DWELL) QDIPs were also experimentally shown to absorb both 45 deg. and normally incident light. Thus we have employed a reflection grating structure to further enhance the quantum efficiency. JPL has demonstrated wavelength control by progressively growing material and fabricating devices structures that have continuously increased in LWIR response. The most recent devices exhibit peak responsivity out to 8.1 microns. Peak detectivity of the 8.1 micrometer devices has reached approx. 1 x 10(exp 10) Jones at 77 K. Furthermore, we have fabricated the first long-wavelength 640x512 pixels QDP focal plane array. This QDIP focal plane may has produced excellent infrared imagery with noise equivalent temperature difference of 40 mK at 60K operating temperature. In addition, we have managed to increase the quantum efficiency of these devices from 0.1% (according to the data published in literature) to 20% in discrete devices. This is a factor of 200 increase in quantum efficiency. With these excellent results, for the first time QDIP performance has surpassed the QWIP performance. Our goal is to operate these long-wavelength detectors at much higher operating temperature than 77K which can be passively achieved in space. This will be a huge leap in high performance infrared detectors specifically applicable to space science instruments.

infrared imaging↗

NASA NTRS1990

The transfer of resonance-line radiation in static astrophysical media

An analytic solution is derived for the mean intensity of resonance-line radiation within an absorbing medium of large scattering optical depth but low density. The line profile, the mean number of scatterings before absorption or escape, the mean path length traveled, and the fraction of the photons which escape the medium are derived. Approximate methods are also developed which permit the treatment of media of intermediate optical depth, where scattering takes place in the Doppler core. Astrophysical applications include the absorption of H Ly-alpha radiation by stellar dust, the pumping of H2 Lyman band lines by H Ly-alpha and the Bowen fluorescence.

Neufeld, David A.↗

NASA NTRS1992

The ionosphere as a gamma ray burst detector

Unlike all man made detectors, which are only sensitive to relative narrow regions of the electromagnetic spectrum, the ionosphere is practically a perfect detector for high energy radiation because it absorbs all radiation from the far-ultraviolet to the higher energy gamma-rays. Therefore, it may be possible to employ the terrestrial atmosphere as a detector of high energy celestial photons. As early as the 1940's solar flares were detected by the disturbance they caused to the ionosphere. The VLF (3 - 30 kHz) approach for detecting ionospheric disturbances is based on the following physical circumstance: celestial high energy radiation ionizes the atoms of the earth's ionosphere leading to the production of free electrons. These free electrons influence the propagation of electromagnetic waves. By studying the phase and amplitude changes of VLF radio wave propagating in the earth-ionosphere waveguide, it was hoped to ascertain the electron density in these regions and draw conclusions about the celestial radiation which caused them. To detect gamma-ray bursts, two conditions for the optimal detection are: (1) large zenith angle; and (2) alignment of burst and propagation path.

Mcgruder, Charles H., III↗

NASA NTRS2011

Ultrasensitive Superconducting Transition Edge Sensors Based On Electron-Phonon Decoupling

We have successfully fabricated the superconducting transition edge sensor (TES), bolometer technology that centers on the use of electron-phonon decoupling (EPD) to thermally isolate the bolometer. Along with material characterization for large format antenna coupled bolometer arrays, we present the initial test results of bolometer based on EPD designed for THz detection. We have selected a design approach that separates the two functions of photon absorption and temperature measurement, allowing separate optimization of the performance of each element. We have integrated Molybdenum/Gold (Mo/Au) bilayer TES and ion assisted thermally evaporated (IAE) Bismuth (Bi) films as radiation absorber coupled to a low-loss microstripline from Niobium (Nb) ground plane to a twin-slot antenna structure. The thermal conductance and the time constant of these devices have been measured, and are consistent with our calculations. The device exhibits a single time constant at 0.1 K of approx.160 IlS, which is compatible with readout by a high-bandwidth single SQUID or a time domain SQUID multiplexer. The effects of thermal conductance and electrothermal feedback are major determinants of the time constant, but the electronic heat capacity also plays a major role. The NEP achieved in the device described above is 2.5x10(exp -17)W(gamma)Hz. Our plan is to demonstrate a reduction of the volume in the superconducting element to 5 microns x 5 microns in films of half the thickness at Tc = 60mK. By calculation, this new geometry corresponds to an NEP reduction of two orders of magnitude to 2.5x10(exp -19)W/(gamma)Hz, with a time constant of ~130/ls.

Jethava, Nikhil↗

DOE OSTI2023

Low Catalyst Loading Enhances Charge Accumulation for Photoelectrochemical Water Splitting

Abstract Solar water oxidation is a critical step in artificial photosynthesis. Successful completion of the process requires four holes and releases four protons. It depends on the consecutive accumulation of charges at the active site. While recent research has shown an obvious dependence of the reaction kinetics on the hole concentrations on the surface of heterogeneous (photo)electrodes, little is known about how the catalyst density impacts the reaction rate. Using atomically dispersed Ir catalysts on hematite, we report a study on how the interplay between the catalyst density and the surface hole concentration influences the reaction kinetics. At low photon flux, where surface hole concentrations are low, faster charge transfer was observed on photoelectrodes with low catalyst density compared to high catalyst density; at high photon flux and high applied potentials, where surface hole concentrations are moderate or high, slower surface charge recombination was afforded by low‐density catalysts. The results support that charge transfer between the light absorber and the catalyst is reversible; they reveal the unexpected benefits of low‐density catalyst loading in facilitating forward charge transfer for desired chemical reactions. It is implied that for practical solar water splitting devices, a suitable catalyst loading is important for maximized performance.

Liu, Tianying↗

DOE OSTI2023

Low Catalyst Loading Enhances Charge Accumulation for Photoelectrochemical Water Splitting

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS2004

NGC 4388- Spectral Studies of the First Seyfert 2 Seen by INTEGRAL

We present first INTEGRAL and XMM-Newton ob- servations of a Seyfert galaxy, the type 2 AGN NGC 4388. Several INTEGRAL observations performed in 2003 allow us to study the spectrum in the 20 - 300 keV range. In addition two XMM-Newton observations give detailed insight into the 0.2 - 10 keV emission. Comparison with previous observations by BeppoSAX, SIGMA and CGROIOSSE show that the overall spectrum for soft X-rays up to the gamma-rays can be described by a highly absorbed and variable non-thermal component in addition to constant non-absorbed thermal emission of low abundance (2 - 5%Za), plus a constant Fe K alpha line. The hard X-ray component is well described by a simple power law with a mean photon index of 1 = 1.7. During the INTEGRAL observations the flux at 100 keV increased by a factor of 1.5. The analysis of XMM-Newton data implies that the emission below 3 keV is decoupled from the AGN and probably due to extended emission as seen in Chandra observations. The constant iron line emission is apparently also decoupled from the direct emission of the central engine and likely to be generated in the obscuring material, e.g. in the molecular torus or even further away.

Beckman, V.↗