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At least 37 records · Page 2

Design and Optimization of Multi-Pixel Transition-Edge Sensors for X-Ray Astronomy Applications

Multi-pixel transition-edge sensors (TESs), commonly referred to as 'hydras', are a type of position sensitive micro-calorimeter that enables very large format arrays to be designed without commensurate increase in the number of readout channels and associated wiring. In the hydra design, a single TES is coupled to discrete absorbers via varied thermal links. The links act as low pass thermal filters that are tuned to give a different characteristic pulse shape for x-ray photons absorbed in each of the hydra sub pixels. In this contribution we report on the experimental results from hydras consisting of up to 20 pixels per TES. We discuss the design trade-offs between energy resolution, position discrimination and number of pixels and investigate future design optimizations specifically targeted at meeting the readout technology considered for Lynx.

Smith, Stephen J.↗

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↗

Long-Wavelength Infrared Detector

Proposed device detects infrared photons of 10- to 100-micrometer wavelength by intersubband absorption in coupled quantum wells. Based on splitting of energy level occuring when two quantum wells placed so close together wave functions of quantized energy levels overlap. Detector absorbs photons, energy which equals difference in energy between two levels resulting from split. Because degree of overlap of wave functions and, therefore, magnitude of split varied by varying width of barrier between two coupled wells, such detector, in principle, designed to operate at any desired wavelength. Restrictions on design parameters of quantum wells of proposed device less severe than single-well devices. Energy levels near tops of wells still necessary so photoexcited carriers tunnel out. Additional flexibility in design obtained by use of wells formed by barriers of different heights.

Vasquez, Richard P.↗

Current and potential productivity of wheat for a controlled environment life support system

Several determinants of crop growth are analyzed to determine theoretical and potentially achievable productivity. These include: incident photosynthetic photon flux (PPF); percent absorption of the incident PPF by photo synthetic tissue; photosynthetic efficiency; respiratory carbon use efficiency; and harvest index. The effects of optimal environmental and cultural factors on each of these determinants are also investigated. Results indicate that an increase in the percentage of absorbed photons is responsible for most of the improvement in wheat yields in an optimal controlled environment. An integrated PPF of 150 mol/sq m per d has produced 60 g/sq m per d of grain. There is almost a linear increase in wheat yields with increasing PPF. At intermediate and equal integrated daily PPF levels, photoperiod had little effect on yield per day or energy efficiency. Decreasing temperature from 23 to 17 deg increased yield per day by 20 percent but increased the life cycle from 62 to 89 days.

Bugbee, B. G.↗

Calculated quantum yield of photosynthesis of phytoplankton in the Marine Light-Mixed Layers (59 deg N, 21 deg W)

The quantum yield of photosynthesis (mol C/mol photons) was calculated at six depths for the waters of the Marine Light-Mixed Layer (MLML) cruise of May 1991. As there were photosynthetically available radiation (PAR) but no spectral irradiance measurements for the primary production incubations, three ways are presented here for the calculation of the absorbed photons (AP) by phytoplankton for the purpose of calculating phi. The first is based on a simple, nonspectral model; the second is based on a nonlinear regression using measured PAR values with depth; and the third is derived through remote sensing measurements. We show that the results of phi calculated using the nonlinear regreesion method and those using remote sensing are in good agreement with each other, and are consistent with the reported values of other studies. In deep waters, however, the simple nonspectral model may cause quantum yield values much higher than theoretically possible.

Carder, K. L.↗

Optical Probe of the Superconducting Normal Mixed State in a Magnetic Penetration Thermometer

Using ultraviolet photon pulses, we have probed the internal behavior of a molybdenum-gold Magnetic Penetration Thermometer (MPT) that we designed for x-ray microcalorimetry. In this low-temperature detector, the diamagnetic response of a superconducting MoAu bilayer is used to sense temperature changes in response to absorbed photons. We have previously described an approximate model that explains the high responsivity of the detector to temperature changes as a consequence of a Meissner transition of the molybdenum-gold film in the magnetic field applied by the superconducting circuit used to bias the detector. We compare measurements of MPT heat capacity and thermal conductance, derived from UV photon pulse data, to our model predictions for the thermodynamic properties of the sensor and for the electron cooling obtained by quasiparticle recombination. Our data on electron cooling power is also relevant to the operation of other superconducting detectors, such as Microwave Kinetic Inductance Detectors.

superconductivity↗

Coated fiber optic chemical and radiation sensors

Distributed fiber optic chemical and radiation sensors formed by coating the fibers with certain types of response materials are provided. For distributed chemical sensors, the coatings are reactive with the targets; the heat absorbed or released during a reaction will cause a local temperature change on the fiber. For distributed radiation sensors, coating a fiber with a scintillator enhances sensitivity toward thermal neutrons, for example, by injecting light into the fiber. The luminescent components in these materials are taken from conjugated polymeric and oligomeric dyes, metal organic frameworks with sorbed dyes, and two-photon-absorbing semiconductors. The compositions may exhibit strong gamma rejection. Other scintillators combining luminescent materials with neutron converters are available. With a multiple-layer coating, it may be possible to identify the presence of both neutrons and gamma rays, for example. Coatings may be applied during manufacture or in the field.

Lamberti, Vincent E.↗

Discussion of Yellow Starthistle Response to Photosynthetic Irradiance, Photoperiod, and CO2

Yellow Starthistle (Centaurea solstitialis) is a native annual weed of Eurasia and since introduction into the United STates has become an invasive and noxious weed. It grows in a rosette habit during the vegetative state and usually bolts in summer to produce a large and branched flowering stem. Time to flowering in Yellow Starthistle has been attributed to photoperiod, nitrogen nutrition, temperature, and water stress. We executed a series of studies to investigate the role of light, both photoperiod and photosynthetic photon flux, on flowering and development in Yellow Starthistle. Treatments were presented in 4 ways: 1) varying day length with constant photosynthetic photon flus (PPF) providing increasing daily integrated Photosynthetic Photon (PP) exposure with longer day lengths 2) varying day length while adjusting PPF to maintain daily PP exposure for all treatments 3) extending photoperiod treatments beyond common 12-h photosynthetic period with low light levels to maintain both PPF and daily PP across all treatments4)reciprocal exchange of plant among photoperiod treatments Yellow Starthistle appears to be a long-day plant with a critical day length requirement between 14-h and 16-h to induce transition from vegetative to floral stages in development. PPF and daily absorbed photons did not affect time to vegetative floral stage transition, but did affect factors such as biomass accumulation and canopy parameters such as specific leaf mass. Reciprocal exchange of plants between floral inducing and inhibiting photoperiod treatments, starting at 2-weeks post germination, had no effect on to flower. Flowering was determined by photoperiod experienced during the first 2-weeks (or less) post germination.Yellow Starthistle net photosynthetic response to elevated atmospheric CO2 concentrations over a range of photosynthetically active radiation flux rates and temperatures will also be presented and discussed.

Photosynthetic↗

Discussion of Yellow Starthistle Response to Irradiance, Photoperiod, and CO2

Yellow Starthistle (Centaurea solstitialis) is a native annual weed of Eurasia and since introduction into the US has become an invasive and noxious weed. It grows in a rosette habit during the vegetative state and usually bolts in summer to produce a large and branched flowering stem. Time to flowering in Yellow Starthistle has been attributed to photoperiod, nitrogen nutrition, temperature, and water stress. We executed a series of studies to investigate the role of light, both photoperiod and photosynthetic photon flux, on flowering and development in Yellow Starthistle. Treatments were presented in 4 ways: (1) Varying day length with constant photosynthetic photon flus (PPF) - providing increasing daily integrated Photosynthetic Photon (PP) exposure with longer day lengths, (2) Varying day length while adjusting PPF to maintain daily PP exposure for all treatments, (3) Extending photoperiod treatments beyond common 12-h photosynthetic period with low light levels to maintain both PPF and daily PP across all treatments; and (4) Reciprocal exchange of plant among photoperiod treatments. Yellow Starthistle appears to be a long-day plant with a critical day length requirement between 14-h and 16-h to induce transition from vegetative to floral stages in development. PPF and daily absorbed photons did not affect time to vegetative / floral stage transition, but did affect factors such as biomass accumulation and canopy parameters such as specific leaf mass. Reciprocal exchange of plants between floral inducing and inhibiting photoperiod treatments, starting at 2-weeks post germination, had no effect on to flower. Flowering was determined by photoperiod experienced during the first 2-weeks (or less) post germination. Yellow Starthistle net photosynthetic response to elevated atmospheric CO2 concentrations over a range of photosynthetically active radiation flux rates and temperatures will also be presented and discussed.

Photons↗

Two-photon or higher-order absorbing optical materials and methods of use

Compositions capable of simultaneous two-photon absorption and higher order absorptivities are disclosed. Many of these compositions are compounds satisfying the formulae D-.PI.-D, A-.PI.-A, D-A-D and A-D-A, wherein D is an electron donor group, A is an electron acceptor group and .PI. comprises a bridge of .pi.-conjugated bonds connecting the electron donor groups and electron acceptor groups. In A-D-A and D-A-D compounds, the .pi. bridge is substituted with electron donor groups and electron acceptor groups, respectively. Also disclosed are methods that generate an electronically excited state of a compound, including those satisfying one of these formulae. The electronically excited state is achieved in a method that includes irradiating the compound with light. Then, the compound is converted to a multi-photon electronically excited state upon simultaneous absorption of at least two photons of light. The sum of the energies of all of the absorbed photons is greater than or equal to the transition energy from a ground state of the compound to the multi-photon excited state. The energy of each absorbed photon is less than the transition energy between the ground state and the lowest single-photon excited state of the compound is less than the transition energy between the multi-photon excited state and the ground state.

Marder, Seth↗

Coupling of Infrared Active Colloidal Quantum Dots and Amorphous Selenium for Fast and Sensitive Photodetection

Colloidal quantum dot (CQD) based infrared (IR) photodetectors offer facile wavelength tunability in the IR and low-cost fabrication. However, owing to their large surface areas, CQDs intrinsically have significant surface traps critically affecting the speed of CQD photodetectors, typically mediated through tedious surface passivation efforts. In this report, an alternative strategy involving coupling of near-IR photoactive lead sulfide CQDs with a thermally evaporated amorphous selenium (a-Se) hole transport layer is proposed. By separating the detector into a photon absorbing CQD region and a charge transport a-Se region, the study takes advantage of the extremely low noise, predominantly hole-only transport process in a-Se. Here, a high 3 dB bandwidth of 2.5 MHz and a competitive specific detectivity of 2.5 × 10 11 Jones at room temperature are demonstrated at 980 nm. This report serves as a first demonstration of strong coupling between an IR active CQD absorber and a-Se, which paves the path to obtain fast and highly photoresponsive IR photodetection in the future.

36 MATERIALS SCIENCE↗

Direct Exciton Harvesting from a Bound Triplet Pair

Abstract Singlet fission is commonly defined as the generation of two triplet excitons from a single absorbed photon. However, ambiguities within this definition arise due to the complexity of the various double triplet states that exist in SF chromophores and the corresponding interconversion processes. To clarify this process, singlet fission is frequently depicted as sequential two‐step conversion in which a singlet exciton decays into a bound triplet‐pair biexciton state that dissociates into two “free” triplet excitons. However, this model discounts the potential for direct harvesting from the coupled biexciton state. Here, it is demonstrated that individual triplet excitons can be extracted directly from a bound triplet pair. It is demonstrated that due to the requirement for geminate triplet–triplet annihilation in intramolecular singlet fission compounds, unique spectral and kinetic signatures can be used to quantify triplet‐pair harvesting yields. An internal quantum efficiency for triplet exciton transfer from the triplet pair of >50%, limited only by the solubility of the compounds is achieved. The harvesting process is not dependent on the net multiplicity of the triplet‐pair state, suggesting that an explicit, independent dissociation step is not a requirement for using triplet pairs to do chemical or electrical work.

Chemistry↗

Tuning Intermediate Bands of Protective Coatings to Reach the Bulk-Recombination Limit of Stable Water-Oxidation GaP Photoanodes

Stable photoelectrochemical solar fuel production requires protective coatings to achieve effective charge separation, transport, and injection at the semiconductor–liquid interfaces, implying that the coating should energetically align its intermediate band (IB) with both the photoabsorber's band edge and co-catalyst's potentials. Yet approaches to adjust coating IB positions to accommodate various semiconductor light absorbers for constructing efficient and stable photoelectrodes have not been developed. In this report, three types of transition metal (M = Mn 2+ , Mn 3+ , and Cr 3+ ions) alloyed TiO2 coatings are discovered using atomic layer deposition (ALD). The IB energetics of these coatings are characterized by X-ray photoelectron spectroscopy and are found to be tunable inside the TiO 2 bandgap, through varying ALD growth conditions. By applying these coatings to n-type GaP and integrating with IrO x co-catalysts, the water-oxidation J–E performance is comparable to an uncoated corroding GaP photoanode. It reaches the bulk recombination limit of the GaP and achieves ≈28% absorbed photon to current efficiency under 475-nm light excitation (6.48 mW cm -2 ) and 100-h stable water oxidation. The outstanding performance and stability are attributed to the efficient charge separation and hole transport, as allowed by the energy alignment of the coating IB and the GaP valence band edge.

36 MATERIALS SCIENCE↗

Observation of Long-Lived UV-Induced Fluorescence from Environmental Materials Using the HVeV Detector as Developed for SuperCDMS

Here, we describe recent experiments using a SuperCDMS HVeV single-charge sensitive detector illuminated with an ultraviolet LED (275 nm) and a monochromatic laser(650 nm) using a dual fiber optic system installed in a small dilution refrigerator at Stanford University. We observed a population of fluorescence background events after UV exposure but not after exposure to the laser source. The fluorescence was likely due to scattered UV photons absorbed outside the detector. We discuss the possibility of fluorescence being a contributor to the low energy excess background observed in above-ground Dark Matter experiments.

36 MATERIALS SCIENCE↗

Surface and interface structures of epitaxial Sb 2 Se 3 on mica

Sb 2 Se 3 thin film is an emerging photon absorber used in solar cells. We report the study of surface and interface structures of Sb2Se3(1 2 0) film grown on mica substrate by a high-rate vapor transport method. The interface epitaxial relationship between Sb 2 Se 3 and mica examined by the cross- sectional TEM images and diffraction patterns along the [0 0 1] and [10] directions of Sb 2 Se 3 reveal a rectangular structure with lengths of 4.03 ± 0.1 Å and 5.29 ± 0.1 Å, consistent with the [1 2 0] out-of-plane direction of Sb 2 Se 3 bulk lattice parameters. In contrast, the two-dimensional reciprocal space map (2D map) constructed from azimuthal reflection high-energy electron diffraction (ARHEED) patterns from the surface exhibits a decorated hexagonal structure. This surface structure emerges from six epitaxial orientation domains/rods and each domain has a rectangular unit mesh of 3.94 ± 0.09 Å and 26.95 ± 1.16 Å along the [0 0 1] and [10] directions. The 26.95 Å is consistent with the unit mesh of the outermost layer of the Sb 2 Se 3 (1 2 0) domains/rods. Overall, our 2D map reveals surface information that are not easily observed by other diffraction techniques.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Photoinduced Charge Carrier Dynamics and Electron Injection Efficiencies in Au Nanoparticle-Sensitized TiO 2 Determined with Picosecond Time-Resolved X-ray Photoelectron Spectroscopy

Progress in the development of plasmon-enabled light-harvesting technologies requires a better understanding of their fundamental operating principles and current limitations. In this work, we employ picosecond time-resolved X-ray photoemission spectroscopy to investigate photoinduced electron transfer in a plasmonic model system composed of 20 nm sized gold nanoparticles (NPs) attached to a nanoporous film of TiO 2 . The measurement provides direct, quantitative access to transient local charge distributions from the perspectives of the electron donor (AuNP) and the electron acceptor (TiO 2 ). On average, approximately two electrons are injected per NP, corresponding to an electron injection yield per absorbed photon of 0.1%. Back electron transfer from the perspective of the electron donor is dominated by a fast recombination channel proceeding on a time scale of 60 ± 10 ps and a minor contribution that is completed after ~1 ns. The findings provide a detailed picture of photoinduced charge carrier generation in this NP–semiconductor junction, with important implications for understanding achievable overall photon-to-charge conversion efficiencies.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Uncovering the Role of Hole Traps in Promoting Hole Transfer from Multiexcitonic Quantum Dots to Molecular Acceptors

The understanding of electronic dynamics in multiexcitonic quantum dots (QDs) is important for designing efficient systems useful in high power scenarios, such as solar concentrators and multielectron charge transfer. The multiple charge carriers within a QD can undergo undesired Auger recombination events, which rapidly annihilate carriers on picosecond time scales and generate heat from absorbed photons instead of useful work. Compared to the transfer of multiple electrons, the transfer of multiple holes has proven to be more difficult due to slower hole transfer rates. To probe the competition between Auger recombination and hole transfer in CdSe, CdS, and CdSe/CdS QDs of varying sizes, we synthesized a phenothiazine derivative with optimized functionalities for binding to QDs as a hole accepting ligand and for spectroscopic observation of hole transfer. Transient absorption spectroscopy was used to monitor the photoinduced absorption features from both trapped holes and oxidized ligands under excitation fluences where the averaged initial number of excitons in a QD ranged from ~1 to 19. We observed fluence-dependent hole transfer kinetics that last around 100 ps longer than the predicted Auger recombination lifetimes, and the transfer of up to 3 holes per QD. Theoretical modeling of the kinetics suggests that binding of hole acceptors introduces trapping states significantly different from those in native QDs passivated with oleate ligands. Holes in these modified trap states have prolonged lifetimes, which promotes the hole transfer efficiency. These results highlight the beneficial role of hole-trapping states in devising hole transfer pathways in QD-based systems under multiexcitonic conditions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

A Nanocrystal Catalyst Incorporating a Surface Bound Transition Metal to Induce Photocatalytic Sequential Electron Transfer Events

Heterogeneous photocatalysis is less common but can provide unique avenues for inducing novel chemical transformations and can also be utilized for energy transductions, i.e., the energy in the photons can be captured in chemical bonds. Here, we developed a novel heterogeneous photocatalytic system that employs a lead-halide perovskite nanocrystal (NC) to capture photons and direct photogenerated holes to a surface bound transition metal Cu-site, resulting in a N–N heterocyclization reaction. The reaction starts from surface coordinated diamine substrates and requires two subsequent photo-oxidation events per reaction cycle. We establish a photocatalytic pathway that incorporates sequential inner sphere electron transfer events, photons absorbed by the NC generate holes that are sequentially funneled to the Cu-surface site to perform the reaction. The photocatalyst is readily prepared via a controlled cation-exchange reaction and provides new opportunities in photodriven heterogeneous catalysis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗