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DOE OSTI2020

Thermal kinetic inductance detectors for millimeter-wave detection

Thermal Kinetic-Inductance Detectors (TKIDs) combine the excellent noise performance of traditional bolometers with a radio frequency multiplexing architecture that enables the large detector counts needed for the next generation of millimeter-wave instruments. In this paper, we first discuss the expected noise sources in TKIDs and derive the limits where the phonon noise contribution dominates over the other detector noise terms: generation–recombination, amplifier, and two-level system noise. Second, we characterize aluminum TKIDs in a dark environment. We present measurements of TKID resonators with quality factors of about 10 5 at 80 mK. We also discuss the bolometer thermal conductance, heat capacity, and time constants. These were measured by the use of a resistor on the thermal island to excite the bolometers. These dark aluminum TKIDs demonstrate a noise equivalent power, NEP = 2 × 10 − 17 W / Hz , with a 1 / f knee at 0.1 Hz, which provides background noise limited performance for ground-based telescopes observing at 150 GHz.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2020

15.9% organic tandem solar cell with extended near-infrared absorption

Stacking single-junction organic solar cells is effective in increasing the power conversion efficiency (PCE) by reducing the thermalization loss and increasing the open circuit voltage. Current developments of non-fullerene acceptors (NFAs) offer a range of materials whose energy gaps are suited for absorbing relatively narrow slices of the solar spectrum, thus easing requirements for current balance between sub-elements in the multijunction stacks. In this report, we demonstrate a solution-processed tandem organic solar cell comprising a binary, visible-absorbing sub-cell and a ternary near-infrared (NIR) absorbing sub-cell. The ternary NIR sub-cell utilizes a narrow energy gap NFA acceptor that enables a broadened and increased absorption compared to a binary NIR sub-cell. An isopropanol surface treatment is developed to connect the hydrophilichydrophobic surfaces in the charge recombination zone (CRZ) located between the sub-cells. The nearly optically and electrically lossless CRZ combined with an anti-reflection coating results in a tandem OPV with PCE = 15.9 ± 0.2 % under AM 1.5G simulated illumination.

14 SOLAR ENERGY↗

DOE OSTI2020

Interaction of hydrogen with actinide dioxide (011) surfaces

The corrosion and oxidation of actinide metals, leading to the formation of metal-oxide surface layers with the catalytic evolution of hydrogen, impacts the management of nuclear materials. In this work, the interaction of hydrogen with actinide dioxide (AnO 2 , An = U, Np, or Pu) (011) surfaces by Hubbard corrected density functional theory (PBEsol+U) has been studied, including spin–orbit interactions and non-collinear 3k anti-ferromagnetic behavior. The actinide dioxides crystalize in the fluorite-type structure, and although the (111) surface dominates the crystal morphology, the (011) surface energetics may lead to more significant interaction with hydrogen. The dissociative adsorption of hydrogen on the UO 2 (0.44 eV), NpO 2 (-0.47 eV), and PuO 2 (-1.71 eV) (011) surfaces has been calculated. It is found that hydrogen dissociates on the PuO 2 (011) surface; however, UO 2 (011) and NpO 2 (011) surfaces are relatively inert. Recombination of hydrogen ions is likely to occur on the UO 2 (011) and NpO 2 (011) surfaces, whereas hydroxide formation is shown to occur on the PuO 2 (011) surface, which distorts the surface structure.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Dependence of the impurity transport on the dominant turbulent regime in ELM-y H-mode discharges on the DIII-D tokamak

Laser blow-off injections of aluminum and tungsten have been performed on the DIII-D tokamak to investigate the variation of impurity transport in a set of dedicated ion and electron heating scans with a fixed value of the external torque. The particle transport is quantified via the Bayesian inference method, which, constrained by a combination of a charge exchange recombination spectroscopy, soft X-ray measurements, and VUV spectroscopy provides a detailed uncertainty quantification of transport coefficients. Contrasting discharge phases with a dominant electron and ion heating reveal 3-fold drop in the impurity confinement time and order of magnitude increase in midradius impurity diffusion, when additional electron heating is applied. Further, the calculated stationary aluminum density profiles reverse from peaked in electron heated to hollow in the ion heated case, following a similar trend as electron and carbon density. Comparable values of a core diffusion have been observed for W and Al ions, while differences in the propagation dynamics of these impurities are attributed to pedestal and edge transport. Modeling of the core transport with non-linear gyrokinetics code CGYRO, significantly underpredicts the magnitude of the variation in Al transport. Diffusion increases 3-times steeper with additional electron heat flux and 10-times lower diffusion is observed in ion heated case than predicted by the modeling. Here, the CGYRO model quantitatively matches the increase of the Al diffusion when approaching the linear threshold for the transition from the ion temperature gradient (ITG) to trapped electron mode (TEM).

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2020

Simulations of divertor plasmas with inverse sheaths

The effect of strong electron emission from material surfaces has been proposed to form an “inverse sheath”: a region with a positive potential relative to the near-wall plasma which prevents the flow of ions to the wall [M. D. Campanell, “Negative plasma potential relative to electronemitting surfaces,” Phys. Rev. E. 88, 033103 (2013); M. D. Campanell and M. V. Umansky, “Strongly emitting surfaces unable to float below plasma potential,” Phys. Rev. Lett. 116, 1–5 (2016); M. D. Campanell and G. R. Johnson, “Thermionic cooling of the target plasma to a sub-ev temperature,” Phys. Rev. Lett. 122, 1–5 (2019)]. We assess the viability of this regime in a tokamak device using the 2D edge plasma transport code UEDGE [T. Rognlien et al ., “A fully implicit, time dependent 2-D fluid code for modeling tokamak edge plasmas,” J. Nucl. Mater. 196–198, 347–351 (1992)]. Since the UEDGE code does not consider the sheath region directly, we apply boundary conditions at the divertor targets which emulate the physics of both “standard” and “inverse” sheath regimes [R. Masline et al ., “Influence of the inverse sheath on divertor plasma performance in tokamak edge plasma simulations,” Contrib. Plasma Phys. 60, e201900097 (2020)]. Using these boundary conditions, we perform scoping studies to assess plasma parameters near the target by varying the density at the core-edge interface. We observe a smooth transition in the resultant profiles of plasma parameters for the standard sheath, and a bifurcation across the simulation set for plasmas with an inverse sheath. The cause of this bifurcation is assessed by performing the parameter scan both with and without impurity radiation; we observe that the bifurcation persists in both cases, indicating that this bifurcation is caused by plasma recombination.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2020

Defect filtering for thermal expansion induced dislocations in III–V lasers on silicon

Epitaxially integrated III–V semiconductor lasers for silicon photonics have the potential to dramatically transform information networks, but currently, dislocations limit performance and reliability even in defect-tolerant InAs quantum dot (QD)-based lasers. Despite being below the critical thickness, QD layers in these devices contain previously unexplained misfit dislocations, which facilitate non-radiative recombination. We demonstrate here that these misfit dislocations form during post-growth cooldown due to the combined effects of (1) thermal-expansion mismatch between the III–V layers and silicon and (2) mechanical hardening in the active region. By incorporating an additional sub-critical thickness, indium-alloyed “misfit dislocation trapping layer,” we leverage these mechanical hardening effects to our advantage, displacing 95% of misfit dislocations from the QD layer in model structures. Unlike conventional dislocation mitigation strategies, the trapping layer reduces neither the number of threading dislocations nor the number of misfit dislocations. It simply shifts the position of misfit dislocations away from the QD layer, reducing the defects' impact on luminescence. In full lasers, adding a misfit dislocation trapping layer both above and below the QD active region displaces misfit dislocations and substantially improves performance: we measure a twofold reduction in lasing threshold currents and a greater than threefold increase in output power. Overall, our results suggest that devices employing both traditional threading dislocation reduction techniques and optimized misfit dislocation trapping layers may finally lead to fully integrated, commercially viable silicon-based photonic integrated circuits.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Cryogenic spatial–temporal imaging of surface photocarrier dynamics in MAPbI 3 films at the single grain level

We use cryogenic spatial–temporal photoluminescence (PL) imaging measurements down to 10 K and with short-wavelength, 405 nm laser excitation to study surface charge generation, trapping, and recombination at single bright and dark grains as well as their boundaries in model methylammonium lead iodide (MAPbI 3 ) polycrystalline thin films. These salient conditions are shown to be critical for identifying both the detrimental and cooperative roles of grain microstructures where the dark grains serve as the PL quenching center, while the grain boundaries are largely benign and may promote electron–hole separation.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Optimized continuum x-ray emission from laser-generated plasma

We study continuum x-ray emission from hot plasma at the National Ignition Facility (NIF). We find that the x-ray yield in the multi-keV photon energy range is larger in Ti than in Ag or Au. This apparent paradox is due to Ti K-shell vacancies generated by the extraordinary energy density achieved by the NIF lasers. This is supported by direct observations of large continuum enhancement above the Ti K-series limit due to both free–bound (recombination) emission and strong Ly α (H-like) emission. Detailed calculations agree well with our measurements and support our conclusions.  X-ray emission from matter pervades the universe and plays an important role in the high-energy density (HED) regime (~10 5 J/cm 3 ). For example, the emission and absorption of x-rays controls the thermal state and evolution of stellar interiors.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2021

Single photon sources with near unity collection efficiencies by deterministic placement of quantum dots in nanoantennas

Deterministic coupling between photonic nodes in a quantum network is an essential step toward implementing various quantum technologies. The omnidirectionality of free-standing emitters, however, makes this coupling highly inefficient, in particular if the distant nodes are coupled via low numerical aperture (NA) channels such as optical fibers. This limitation requires placing quantum emitters in nanoantennas that can direct the photons into the channels with very high efficiency. Moreover, to be able to scale such technologies to a large number of channels, the placing of the emitters should be deterministic. In this work, we present a method for directly locating single free-standing quantum emitters with high spatial accuracy at the center of highly directional bullseye metal–dielectric nanoantennas. We further employ non-blinking, high quantum yield colloidal quantum dots for on-demand single-photon emission that is uncompromised by instabilities or non-radiative exciton recombination processes. Taken together, this approach results in a record-high collection efficiency of 85% of the single photons into a low NA of 0.5, setting the stage for efficient coupling between on-chip, room temperature nanoantenna-emitter devices and a fiber or a remote free-space node without the need for additional optics.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Efficient excimer-based white OLEDs with reduced efficiency roll-off

A tetradentate Pt(II) complex, Pt2O2-p2m, which exhibits both efficient monomer and excimer emission, was synthesized. Through rational device design to broaden the recombination zone, an OLED device employing Pt2O2-p2m demonstrated an impressively high peak external quantum efficiency (EQE) of 21.5% and a warm white emission with a color rendering index of 71 and Commission Internationale de L'Eclairage coordinates of (0.409, 0.458). Moreover, a reduced efficiency roll-off was also observed to retain high EQE values of 20% EQE at 1000 cd/m 2 and 17% EQE at 5000 cd/m 2 , and an LT70 (time to 70% initial luminance) was estimated to be over 150 h at 1000 cd/m2 under constant operation at accelerated driving conditions.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Efficiency of bulk perovskite-sensitized upconversion: Illuminating matters

Photon upconversion via triplet–triplet annihilation could allow for the existing efficiency limit of single junction solar cells to be surpassed. Indeed, efficient upconversion at subsolar fluences has been realized in bulk perovskite-sensitized systems. Many questions have remained unanswered, in particular, regarding their behavior under photovoltaic operating conditions. Here, we investigate the impact of repeated and continuous illumination on bilayer perovskite/rubrene upconversion devices. We find that variations of the underlying perovskite carrier recombination dynamics greatly impact the upconversion process. Trap filling and triplet sensitization are in direct competition: more saturated trap states in the perovskite and, thus, longer underlying perovskite photoluminescence lifetimes allow for an increased number of carriers to diffuse to the perovskite/rubrene interface and undergo charge extraction to the triplet state of rubrene. As a result, the upconversion efficiency is greatly influenced by the underlying trap density: the upconverted photoluminescence intensity increases by two orders of magnitude under continuous illumination for 4 h. This shows that the upconversion efficiency is difficult to define for this system. Importantly, these results indicate that perovskite-sensitized upconversion devices exhibit peak performance under continuous illumination, which is a requirement for their successful integration into photovoltaics to help overcome the Shockley–Queisser limit in single junction solar cells.

VanOrman, Zachary A. (ORCID:000000027773012X)↗

DOE OSTI2021

Experimental study of atmospheric pressure single-pulse nanosecond discharge in pin-to-pin configuration

We present an experimental study of nanosecond high-voltage discharges in a pin-to-pin electrode configuration at atmospheric conditions operating in single-pulse mode (no memory effects). Discharge parameters were measured using microwave Rayleigh scattering, laser Rayleigh scattering, optical emission spectroscopy enhanced with a nanosecond probing pulse, and fast photography. Spark and corona discharge regimes were studied for electrode gap sizes 2-10 mm and discharge pulse duration of 90 ns. The spark regime was observed for gaps < 6 mm using discharge pulse energies of 0.6-1 mJ per mm of the gap length. Higher electron number densities, total electron number per gap length, discharge currents, and gas temperatures were observed for smaller electrode gaps and larger pulse energies, reaching maximal values of about 7.5 x 10 15 cm -3 , 3.5 x 10 11 electrons per mm, 22 A, and 4,000 K (at 10 microseconds after the discharge), respectively, for a 2 mm gap and 1 mJ/mm discharge pulse energy. Initial breakdown was followed by a secondary breakdown occurring about 30-70 ns later and was associated with ignition of a cathode spot and transition to cathodic arc. Here, a majority of the discharge pulse energy was deposited into the gas before the secondary breakdown (85-89%). The electron number density after the ns-discharge pulse decayed with a characteristic time scale of 150 ns governed by dissociative recombination and electron attachment to oxygen mechanisms. For the corona regime, substantially lower pulse energies (~0.1 mJ/mm), peak conduction current (1-2 A), and electron numbers (3-5 x 10 10 electrons per mm), and gas temperatures (360 K) were observed.

42 ENGINEERING↗

DOE OSTI2021

Inverted metamorphic GaInAs solar cell grown by dynamic hydride vapor phase epitaxy

We present an inverted metamorphic rear heterojunction ~1.0 eV GaInAs solar cell deposited by dynamic hydride vapor phase epitaxy (D-HVPE) with high growth rate. This device uses a Ga 1-x In x P compositionally graded buffer (CGB) to bridge the lattice constant gap between the GaAs substrate and the Ga0.71In0.29As emitter layer. High-resolution x-ray diffraction and transmission electron microscopy confirm that the Ga 0.71 In 0.29 As emitter is grown lattice-matched to the in-plane lattice constant of the CGB with minimal generation of defects at the GaInAs/GaInP interface. The device contains a threading dislocation density of 2.3 × 10 6 cm -2 , a level that enables high-performance minority carrier devices and is comparable to previously demonstrated GaInP CGBs grown by D-HVPE. The device exhibits an open-circuit voltage of 0.589 V under a one-sun AM1.5G illumination condition and a bandgap-voltage offset of 0.407 V, indicating metamorphic epitaxial performance nearly equal to state-of-the-art devices. We analyze the dark current of the device and determine that reducing recombination in the depletion region, which can be achieved by reducing the threading dislocation density and optimizing the device doping density, will improve the device performance. Furthermore, the CGB and device layers, comprising ~8 µm of thickness, are grown in under 10 min, highlighting the ability of D-HVPE to produce high-quality metamorphic devices of all types with the potential for dramatically higher throughput compared to present technology.

14 SOLAR ENERGY↗

DOE OSTI2022

Role of ripples in altering the electronic and chemical properties of graphene

Ripples of graphene are known to manipulate electronic and hydrogenation properties of graphitic materials. More detailed work is needed to elucidate the structure–property relationship of these systems. In this work, the density functional theory is used to compute the energy and electronic structure of the graphene models with respect to variable curvatures and hydrogen adsorption sites. The magnitude of finite bandgap opening depends on the orientation of ripples, and the hydrogen adsorption energy depends on the local curvature of graphene. An adsorbed hydrogen alters the local curvature, resulting in relatively weakened adsorption on the neighboring three sites, which gives a rationale to experimentally observed dynamic equilibrium stoichiometry (H:C = 1:4) of hydrogenated graphene. The surface diffusion transition state energy of adsorbed hydrogen is computed, which indicates that the Eley–Rideal surface recombination mechanism may be important to establish the dynamic equilibrium, instead of the commonly assumed Langmuir–Hinshelwood mechanism.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

Reduction of efficiency droop in c -plane InGaN/GaN light-emitting diodes using a thick single quantum well with doped barriers

We report on c-plane InGaN/GaN single quantum well (QW) light-emitting diodes (LEDs) of different well widths (3 or 9 nm) with and without doped barriers. QW barriers were doped with the aim of reducing the internal electric field (F QW ) in the QW to increase the electron-hole overlap, therefore increasing the recombination rates and resulting in the reduction of the efficiency droop. We, indeed, observed, through biased photocurrent spectroscopy, a reduction in F QW with doped barriers, with F QW being in the same direction of the p-n junction field at zero bias as opposed to the junction field for LEDs without doped barriers. Even with the improvement in the ground state wavefunction overlap, the ground state transition rate remains low for thick QWs. Transitions through excited states were observed for both thick QW LEDs with and without doped barriers. Here, the thick QW LED without doped barriers displayed low external quantum efficiency (EQE), likely as a result of the carrier overflow due to the poor confinement of carriers in the excited states. On the other hand, for LEDs with doped barriers, the flatter band in the QW resulting from the lower F QW reduces the energy separation between the eigenstates, leading to better confinement of carriers in the excited states. With doped barriers, we demonstrated a low efficiency droop 9-nm-thick single QW LED with a peak EQE of 42% at 40 A/cm 2 and an EQE of 36% at 400 A/cm 2 .

42 ENGINEERING↗

DOE OSTI2021

Charge collection and trapping mechanisms in hexagonal boron nitride epilayers

Understanding charge collection and trapping mechanisms is crucial for using hexagonal boron nitride (h-BN) as active layers for many photonic and electronic devices such as deep UV detectors and emitters, neutron detectors, and single photon emitters. Charge collection and trapping mechanisms in h-BN epilayers have been investigated by probing impurity related optical emissions under an applied electrical field. Our results suggested that the existence of oxygen impurities affects the charge collection efficiency and results in an additional emission peak at 3.75 eV, corresponding to a donor-acceptor pair (DAP) recombination involving O N (oxygen residing on the nitrogen site) donors and the V B -H (boron vacancy bonded with hydrogen complex) deep level acceptors. Experimental results further revealed that the applied electric field induces an anti-correlation between the emission intensity of the DAP transition and the charge collection efficiency from which it was shown that it is possible to find an expression to quantitatively measure the maximum charge collection efficiency in h-BN. The results introduce not only a coherent picture for the relationship between common impurities in h-BN and charge collection and trapping mechanisms but also useful insights into possible approaches to improve the quality, purity, and charge collection of the h-BN epilayers.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2021

Ultra-wide bandgap β-Ga 2 O 3 films: Optical, phonon, and temperature response properties

Optical and phonon interactions of Ga 2 O 3 thin films with nanocrystalline morphology were studied at extreme temperatures. The films were grown using a sputtering technique and analyzed via temperature response transmission, Raman scattering, and high-resolution deep-UV photoluminescence (PL). Raman modes indicated that the structure corresponds to the β-phase. The optical-gap at the range of 77–620 K exhibited a redshift of ~200 meV, with a temperature coefficient of ~0.4 meV/K. The optical-gap at room-temperature is 4.85 eV. The electron–phonon interaction model at that temperature range pointed to a low energy phonon, ~31 meV, that is involved in the thermal properties of the optical-gap. Detailed Urbach energy analysis indicated that defects are the dominant mechanism controlling the band-edge characteristics even at an elevated temperature regime where phonon dominance is usually expected. Defects are attributed to the disordered forms of graphite that were detected via Raman scattering and to the granular morphology of the film. A deep-UV laser with an above bandgap exaction line of 5.1 eV was employed to map the PL of the films. The highly resolved spectra, even at room-temperature, show a strong emission of ~3.56 eV attributed to self-trapped holes (STHs). The STH is discussed and modeled in terms of the self-trapped exciton. Moreover, a very distinct but low-intensity emission was found at 4.85 eV that agrees with the value of the optical-gap and is attributed to bandgap recombination. The intensity ratio between the STH and that of the bandgap was found to be 6:1.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Quantum efficiency of InGaN–GaN multi-quantum well solar cells: Experimental characterization and modeling

InGaN-based multi-quantum well (MQW) solar cells are promising devices for photovoltaics (e.g., for tandem solar cells and concentrator systems), space applications, and wireless power transfer. In order to improve the efficiency of these devices, the factors limiting their efficiency and stability must be investigated in detail. Due to the complexity of a MQW structure, compared with a simple pn junction, modeling the spectral response of these solar cells is not straightforward, and ad hoc methodologies must be implemented. In this paper, we propose a model, based on material parameters and closed-formula equations, that describes the shape of the quantum efficiency of InGaN/GaN MQW solar cells, by taking into account the layer thickness, the temperature dependence of the absorption coefficient, and quantum confinement effects. We demonstrate (i) that the proposed model can effectively reproduce the spectral response of the cells; in addition, (ii) we prove that the bulk p-GaN layer absorbs radiation, but the carriers photogenerated in this region do not significantly contribute to device current. Finally, we show that (iii) by increasing the temperature, there is a redshift of the absorption edge due to bandgap narrowing, which can be described by Varshni law and is taken into account by the model, and a lowering in the extraction efficiency due to the increase in recombination (mostly Shockley–Read–Hall) inside the quantum wells, which is also visible by decreasing light intensity.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗