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Nonreciprocal Thermal Emitters Using Metasurfaces with Multiple Diffraction Channels
The emissivity and absorptivity of nonreciprocal thermal emitters are not constrained by the well-known Kirchhoff law of thermal radiation, which usually serves as the theoretical basis to characterize thermal properties. When thermal emitters are nondiffracting, which is the case in previous studies of nonreciprocal thermal emitters, the angular distribution of emissivity and absorptivity is mirror symmetric with respect to the normal direction, and the nonreciprocal effect is confined to a relatively narrow angular range. In this work, we consider nonreciprocal thermal emitters that can simultaneously couple to multiple diffraction channels. We show that the symmetry relation between absorptivity and emissivity can be broken in such multichannel emitters. The angular range in which the nonreciprocal effect is strong can also be significantly broadened. Such multichannel emitters can operate as one-way energy splitters. Our work significantly broadens the flexibility of thermal-radiation control in nonreciprocal thermal-emitter design.
Rapid thermal emittance and quantum efficiency mapping of a cesium telluride cathode in an rf photoinjector using multiple laser beamlets
Thermal emittance and quantum efficiency (QE) are key figures of merit of photocathodes, and their uniformity is critical to high-performance photoinjectors. Several QE mapping technologies have been successfully developed; however, there is still a dearth of information on thermal emittance maps. This is because of the extremely time-consuming procedure to gather measurements by scanning a small beam across the cathode with fine steps. To simplify the mapping procedure and to reduce the time required to take measurements, we propose a new method that requires only a single scan of the solenoid current to simultaneously obtain thermal emittance and QE distribution by using a pattern beam with multiple beamlets. In this paper, its feasibility has been confirmed by both beam dynamics simulation and theoretical analysis. The method has been successfully demonstrated in a proof-of-principle experiment using an L-band radio-frequency photoinjector with a cesium telluride cathode. In the experiment, seven beamlets were generated from a microlens array system and their corresponding thermal emittance and QE varied from 0.93 to 1.14 mu m/nun and from 4.6% to 8.7%, respectively. We also discuss the limitations and future improvements of the method in this paper.
Thermal emittance and lifetime of alkali-antimonide photocathodes grown on GaAs and molybdenum substrates evaluated in a –300 kV dc photogun
In this work, Cs x K y Sb photocathodes grown on GaAs and molybdenum substrates were evaluated using a –300 kV dc high voltage photogun and diagnostic beam line. Photocathodes grown on GaAs substrates, with varying antimony layer thickness (estimated range from <20 nm to >1 um), yielded similar thermal emittance per rms laser spot size values (~0.4 mmmrad=mm) but very different operating lifetime. Similar thermal emittance was obtained for a photocathode grown on a molybdenum substrate but with markedly improved lifetime. For this photocathode, no decay in quantum efficiency was measured at 4.5 mA average current and with peak current 0.55 A at the photocathode.
Angle-selective thermal emitter for directional radiative cooling and heating
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Compact source of positron beams with small thermal emittance
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Single shot cathode transverse momentum imaging in high brightness photoinjectors
In state of the art photoinjector electron sources, thermal emittance from photoemission dominates the final injector emittance. Therefore, low thermal emittance cathode developments and diagnostics are very important. Conventional thermal emittance measurements for the high gradient gun are time-consuming and thus thermal emittance is not measured as frequently as quantum efficiency during the lifetime of photocathodes, although both are important properties for the photoinjector optimizations. In this paper, a single shot measurement of photoemission transverse momentum, i.e., thermal emittance per rms laser spot size, is proposed for photocathode rf guns. By tuning the gun solenoid focusing, the electrons’ transverse momenta at the cathode are imaged to a downstream screen, which enables a single shot measurement of both the rms value and the detailed spectra of the photoelectrons’ transverse momenta. Both simulations and proof of principle experiments are reported.
High-emissivity, thermally robust emitters for high power density thermophotovoltaics
Thermal radiative energy transport is essential for high-temperature energy harvesting technologies, including thermophotovoltaics (TPVs) and grid-scale thermal energy storage. However, the inherently low emissivity of conventional high-temperature materials constrains radiative energy transfer, thereby limiting system performance and technoeconomic viability. Here, in this study, we demonstrate ultrafast femtosecond laser-material interactions to transform diverse materials into near-blackbody surfaces with broadband spectral emissivity above 0.96. This enhancement arises from hierarchically engineered light-trapping microstructures enriched with nanoscale features, effectively decoupling surface optical properties from bulk thermomechanical properties. These laser-blackened surfaces (LaBS) exhibit exceptional thermal stability, retaining high emissivity for over 100 h at temperatures exceeding 1,000°C, even in oxidizing environments. When applied as TPV thermal emitters, Ta LaBS double electrical power output from 2.19 to 4.10 W cm −2 at 2,200°C while sustaining TPV conversion efficiencies above 30%. This versatile, largely material-independent technique offers a scalable and economically viable pathway to enhance emissivity for advanced thermal energy applications.
Wide wavelength-tunable narrow-band thermal radiation from moiré patterns
Wavelength-tunable narrow-band thermal emitters are highly desired for various applications including multigas sensing. However, current thermal emitters suffer from either too broad bandwidth or too narrow tuning range. Here, based on the moiré effect, we provide a scheme of wavelength-tunable narrow-band thermal emitters with tunability over a wide wavelength range and operation at an arbitrary temperature. Thanks to the unique sensitivity of moiré patterns, our emitter achieves a tuning range to bandwidth ratio of 313, which is 68 times larger than the previous largest value ever reported.
Designing Porous Ion Emitters for Thermal Ionization Mass Spectrometry: Evaluating Metal-Organic Frameworks
In this work we describe the first exploration of metal-organic frameworks (MOFs) as ‘next generation’ ion emitters for thermal ionization mass spectrometry (TIMS). MOFs were identified as promising candidates for this application given the synthetic control over their desired structural properties. This tunability results in well-ordered, high surface area, high porosity frameworks with targeted sorption affinities. Here we explored an aluminum-based, bipyridine-containing MOF (MOF-253) with and without incorporating the high work function metal, rhenium (Re). After analysis of a Nd-bearing MOF, we hypothesized that the well-dispersed, sponge-like interconnected network of the degraded structure would enhance Nd ionization more than traditional TIMS loading activators (i.e., phosphoric acid). Compared to filaments loaded with phosphoric acid that require an additional benzene carburization step, the Nd ionization efficiencies (atoms detected relative to atoms loaded) for heated filaments loaded with MOF-253 were similar (~1%). Electron microscopy after TIMS analysis demonstrated that the MOF was retained on the filament and, as hypothesized, preserved sub-micron porosity post analysis. While these results are preliminary, they demonstrate that MOFs have potential to enhance ionization and exceed the performance of traditional loading techniques by forming nano-porous ion emitters (nano-PIEs). Thus, further experimentation is likely to exceed this performance through more specific selection of the base MOF structure and modifications to porosity and composition. This work represents a novel application of MOFs and a next step in the pursuit of advanced thermal ionization with potential to expand across the periodic table.
Enhancement of Uranium Ionization Efficiencies Using Zn-MOF-74 Derived Nanoporous Ion Emitters for Thermal Ionization Mass Spectrometry
The recent introduction of nano-porous ion emitters (nano-PIEs) formed from metal organic frameworks (MOFs) has demonstrated the potential to enhance sensitivity for thermal ionization mass spectrometry (TIMS). Nano-PIEs take advantage of the parent MOF’s chemical and structural tunability to form scaffolds for ion emitters. A study by Barpaga et al. 2023 on MOF-74 as the parent material found that with high volatility metals in their framework uranium sample utilization efficiency (SUE) increases by up to nine-fold (e.g., Zn-MOF-74) compared to that of the analyte on a bare filament (~0.05%). Here, in this study, we investigate the performance of Zn-MOF-74 to maximize uranium efficiencies at the trace level (= 10 -12 g) by altering the parent MOF morphology and chemistry (i.e., MOF crystal sizes and thermal degradation) and optimizing its integration with TIMS (i.e., MOF mass on a filament and ramp conditions). We observed improvement in SUE up to 20 times (≤1.0%) that of a bare filament load when nano-PIEs derived from nanocrystals of Zn-MOF-74 were heated under a specific current ramp condition. This demonstrates that rates of nano-PIE structural collapse during TIMS analysis and the subsequently formed nanomaterials (and their features) can be tuned to control analyte ionization.
Effects of micrometer-scale surface roughness on thermal infrared emittance spectra of silica glass
Surface roughness is known to decrease thermal infrared (TIR) absorption band intensity, but studies of the effect on geologically relevant samples are relatively limited. To determine the effect of surface roughness (with features smaller than ~2/3 of the wavelength) on TIR spectra, we investigated two glass compositions with prepared roughened surfaces: (1) high purity fused silica and (2) soda-lime glass (73 wt% SiO$_2$). We roughened the surfaces of the glasses by sandblasting and polishing with grit paper. The surfaces were characterized with scanning electron microscopy and stylus profilometry. We then analyzed the roughened glasses with TIR emittance spectroscopy. Micrometer-scale roughness causes a decrease in TIR absorption band intensity, relative to a specular surface. No significant changes in band shape or shifts in wavelength were detected. As roughness increases, empirical results show a logarithmic decrease in TIR absorption band intensity. The logarithmic trends of the two glass compositions are different; empirical roughness calibrations do not translate across different compositions. A linear, least-squares spectral deconvolution using two endmembers, specular and blackbody, predicts model spectra of roughened glass surfaces with relatively low error. This is of consequence to orbital TIR measurements of poorly constrained targets, such as the martian surface, because micrometer-scale roughness is adequately modeled by the addition of a blackbody spectrum to the deconvolution endmember matrix.
High temperature selective emitters via critical coupling of weak absorbers
Tailoring the emission spectra of a solar thermophotovoltaic emitter away from that of a blackbody, thereby minimizing transmission and thermalization loss in the energy receiver, is a viable approach to circumventing the Shockley-Queisser limit to single junction solar energy conversion. Embodiments allow for radically tuned selective thermal emission that leverages the interplay between two resonant phenomena in a simple planar structure—absorption in weakly-absorbing thin films and reflection in multi-layer dielectric stacks. A virtual screening approach is employed based on Pareto optimality to identify a small number of promising structures for a selective thermal emitter from a search space of millions, several of which approach the ideal values of a step-function selective thermal emitter.
Fractal Nanostructured Solar Selective Surfaces for Next Gen Concentrating Solar Power (Final Report)
This project reports a novel coating with enhanced solar absorptance and reduced thermal emittance with high efficiency at elevated temperature for next-generation concentrated solar power (CSP) plants, with targeted operating temperatures around 750°C. Highly textured single and multimetallic oxide coatings were electrodeposited onto Inconel substrate by systematically varying the composition and process parameters. The optimized coating exhibited micro-to-nano structures designed to match the wavelengths in the visible region of the solar spectrum. These structures facilitate resonant absorption of solar radiation, significantly boosting solar absorption and accommodating thermal stress during high temperature exposure. A high solar absorptance exceeding 0.985 and a low thermal emittance below 0.5, yielding a thermal efficiency near 95%, was achieved for the optimized coatings without any anti-reflective overcoat, that remained robust after 750 h of isothermal exposure to 750°C in air. The coatings are also robust to severe mechanical and environmental stressors. The innovative approach presented in this study demonstrates the potential for tailoring air-stable solar absorber coatings to achieve high absorption, low emittance, and excellent high-temperature endurance, meeting the rigorous demands of next-generation CSP systems. A technoeconomic analysis reveals the economic advantage of the coatings for Gen3 CSP installations in different geographical zones globally.
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.
Influence of Tabula Rasa on Process- and Light-Induced Degradation of Solar Cells Fabricated From Czochralski Silicon
Monocrystalline Si solar cells are fabricated from Czochralski (Cz) Si, which contains 10 17 –10 18 cm -3 oxygen atoms. Cz Si undergoes degradation during high-temperature thermal processing steps, such as dopant diffusion to form the p - n junction. This degradation in the bulk minority carrier lifetime can be related to the formation of oxygen precipitates. We found that a high-temperature annealing process known as tabula rasa (TR) not only mitigates process-induced degradation via oxygen precipitate nuclei dissolution, but also modifies subsequent light-induced degradation. We report on the bulk carrier lifetime of n - and p -type Cz Si after TR, which homogenizes the interstitial oxygen in the bulk Si to its monoatomic form in either an N 2 or O 2 environment. A control sample, which was not subjected to a TR processing step, experienced severe process-induced degradation during a boron emitter thermal budget as oxygen precipitates were formed in the Si bulk. These precipitates could be imaged using photoluminescence. Additionally, samples that underwent a TR processing step prior to the boron emitter thermal budget show efficient gettering of metallic impurities compared to the control sample, which showed a decline in the implied open-circuit voltage after the gettering step. Furthermore, modification of the interstitial oxygen bonding by TR had a strong effect on the light-induced degradation kinetics. Instead of a typically observed monotonic decrease, minority carrier lifetime increases first, followed by a nonmonotonic decrease over a ~20 h period. Finally, we conclude that by modifying the interstitial oxygen bonding via TR pretreatment, p -type Cz Si wafers become substantially resistant to harsh solar cell processes and strongly modified light-induced degradation, which would open alternative ways to mitigate this degradation mechanism.
Role of Transition Metals in Metal–Organic Frameworks as Nanoporous Ion Emitters for Thermal Ionization Mass Spectrometry
Thermal ionization mass spectroscopy (TIMS) is a powerful analytical technique that allows for precise determination of isotopic ratios. Analysis on low abundance samples, however, can be limited by the ionization efficiency. Following an investigation into a new type of metal-organic hybrid material devised to promote the emission of analyte ions (nano-PIES) and reduce traditional sample loading problems, this work probes the impact that changing the metal in the material has on the ionization of Uranium-238. Being derived from metal-organic frameworks (MOFs), nano-PIEs inherit the tunability of the parent MOFs; the MOF-74 series has been well studied for probing the impact various framework metals (i.e., Mg, Mn, Co, Ni, Cu, Zn, and Cd) have on material properties, and thus, a series of nano-PIEs with different metals were derived from an isoreticular MOF-74 series. In conclusion, trends in ionization efficiency were studied as a function of ionization potential, volatility, and work function of the framework metals as well as the mechanism of ionization.