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DOE OSTI2020

Templated epitaxy of TiO 2 (B) on a perovskite

The bronze-phase TiO 2 (B) has an open atomic framework that makes it a good candidate for applications in photochemical and electrochemical conversion of energy. However, the synthesis of bronze-phase TiO 2 (B) thin films on perovskite substrates, such as SrTiO 3 (STO), which is one of the most conventional versatile substrates for oxide epitaxy, has been extremely challenging owing to the preferential formation of the anatase TiO 2 over TiO 2 (B). The main reason is that the anatase TiO 2 has not only a smaller lattice mismatch than TiO 2 (B), but also a better structural symmetry match when grown on STO. Here, we demonstrate a way to circumventing this problem by using a VO 2 (B) buffer layer, yielding the growth of a high-quality single crystalline TiO 2 (B) film on a (001)-oriented STO substrate. Finally, from the resulting TiO 2 (B) film, we found that this film has a large optical bandgap of ~3.6 eV, which is close to the known theoretical value, the largest among TiO 2 polymorphs, and useful for developing high-power energy devices.

36 MATERIALS SCIENCE↗

NASA NTRS2022

Orbiting Laser Configuration and Sky Coverage: Coherent Reference for Breakthrough Starshot Ground-based Laser Array

We present the concept of using an orbiting laser as a coherent optical reference to phase a several kilometer diameter array of ground-based lasers designed to accelerate interstellar nano-spacecraft to 20% light-speed using laser propulsion. We investigate the geometrical and temporal constraints for the initial case of the target star Proxima b in the Alpha Centauri system using a laser ground site in the southern hemisphere. Based on these constraints, we detail requirements for the mission architecture for an orbiting laser to be used as an optical reference. We then present two orbits that can meet all given requirements and represent a range of engagement times and days between engagements. We also present a range of orbits with periods from 3 to 4 days and engagement times from 660 to 800 s. If desired, the orbit can be matched to the sidereal day, so each orbit period, the beacon can align with the ground station and the same target star without maneuvers. A discussion of the tradeoff between the Earth-based site latitude, time on engagement, and days between engagements is presented.

Breakthrough Starshot; interstellar spacecraft; co↗

DOE OSTI2021

Multi-octave-spanning supercontinuum generation through high-energy laser filaments in YAG and ZnSe pumped by a 2.4 μm femtosecond Cr:ZnSe laser

Abstract We present experimental and numerical investigations of high-energy mid-infrared filamentation with multi-octave-spanning supercontinuum generation (SCG), pumped by a 2.4 μm, 250 fs Cr:ZnSe chirped-pulse laser amplifier. The SCG is demonstrated in both anomalous and normal dispersion regimes with YAG and polycrystalline ZnSe, respectively. The formation of stable and robust single filaments along with the visible-to-mid-infrared SCG is obtained with a pump energy of up to 100 μJ in a 6-mm-long YAG medium. To the best of the authors’ knowledge, this is the highest-energy multi-octave-spanning SCG from a laser filament in a solid. On the other hand, the SCG and even-harmonic generation based on random quasi-phase matching (RQPM) are simultaneously observed from the single filaments in a 6-mm-long polycrystalline ZnSe medium with a pump energy of up to 15 μJ. The numerical simulations based on unidirectional pulse propagation equation and RQPM show excellent agreement with the measured multi-octave-spanning SCG and even-harmonic generation. They also reveal the temporal structure of mid-infrared filaments, such as soliton-like self-compression in YAG and pulse broadening in ZnSe.

Optics↗

DOE OSTI2025

Production, quality assurance and quality control of the SiPM Tiles for the DarkSide-20k Time Projection Chamber

The DarkSide-20k dark matter direct detection experiment will employ a 21 m 2 silicon photomultiplier (SiPM) array, instrumenting a dual-phase 50 tonnes liquid argon Time Projection Chamber (TPC). SiPMs are arranged into modular photosensors called Tiles, each integrating 24 SiPMs onto a printed circuit board (PCB) that provides signal amplification, power distribution, and a single-ended output for simplified readout. Tiles are further grouped into Photo-Detector Units (PDUs). This paper details the production of the Tiles and the Quality Assurance and Quality Control (QA-QC) protocol established to ensure their performance and uniformity. The production and QA-QC of the Tiles are carried out at Nuova Officina Assergi (NOA), an ISO-6 clean room facility at LNGS. This process includes wafer-level cryogenic characterisation, precision die attaching, wire bonding, and extensive electrical and optical validation of each Tile. The overall production yield exceeds 83.5%, matching the requirements of the DarkSide-20k production plan. These results validate the robustness of the Tile design and its suitability for operation in a cryogenic environment.

Acerbi, F. [Fondazione Bruno Kessler]↗

NASA NTRS1991

Optical phase-locked loop (OPLL) for free-space laser communications with heterodyne detection

Several advantages of coherent free-space optical communications are outlined. Theoretical analysis is formulated for an OPLL disturbed by shot noise, modulation noise, and frequency noise consisting of a white component, a 1/f component, and a 1/f-squared component. Each of the noise components is characterized by its associated power spectral density. It is shown that the effect of modulation depends only on the ratio of loop bandwidth and data rate, and is negligible for an OPLL with loop bandwidth smaller than one fourth the data rate. Total phase error variance as a function of loop bandwidth is displayed for several values of carrier signal to noise ratio. Optimal loop bandwidth is also calculated as a function of carrier signal to noise ratio. An OPLL experiment is performed, where it is shown that the measured phase error variance closely matches the theoretical predictions.

Win, Moe Z.↗

DOE OSTI2020

Structural Evolution of Layered Hybrid Lead Iodide Perovskites in Colloidal Dispersions

Controlling the structure of layered hybrid metal halide perovskites, such as the Ruddlesden-Popper (R-P) phases, is challenging because of their tendency to form mixtures of varying composition. Colloidal growth techniques, such as antisolvent precipitation, forms colloidal dispersions with properties that match bulk layered R-P phases, but controlling the composition of these particles remains challenging. Here, we explore the microstructure of particles of R-P phases of methylammonium lead iodide prepared by antisolvent precipitation from ternary mixtures of alkylammonium cations, where one cation can form perovskite phases (CH 3 NH 3 + ) and the other two promote layered structures as spacers (e.g. C 4 H 9 NH 3 + and C 12 H 25 NH 3 + ). We determine that alkylammonium spacers pack with constant methylene density in the R-P interlayer, and exclude interlayer solvent in dispersed colloids, regardless of length or branching. Using this result, we illustrate how the competition between cations that act as spacers between layers, or as grain- terminating ligands, determines the colloidal microstructure of layered R-P crystallites in solution. Optical measurements reveal that quantum well dimensions can be tuned by engineering the ternary cation composition. Transmission synchrotron wide-angle X-ray scattering and small angle neutron scattering reveal changes in the structure of colloids in solvent and after deposition into thin films. In particular, we find that spacers can alloy between R-P layers if they share common steric arrangements, but tend to segregate into polydisperse R-P phases if they do not mix. In conclusion, this study provides a framework to compare the microstructure of colloidal layered perovskites and suggests clear avenues to control phase and colloidal morphology.

14 SOLAR ENERGY↗

NASA NTRS1992

Electro-optic resonant phase modulator

An electro-optic resonant cavity is used to achieve phase modulation with lower driving voltages. Laser damage thresholds are inherently higher than with previously used integrated optics due to the utilization of bulk optics. Phase modulation is achieved at higher speeds with lower driving voltages than previously obtained with non-resonant electro-optic phase modulators. The instant scheme uses a data locking dither approach as opposed to the conventional sinusoidal locking schemes. In accordance with a disclosed embodiment, a resonant cavity modulator has been designed to operate at a data rate in excess of 100 megabits per sec. By carefully choosing the cavity finesse and its dimension, it is possible to control the pulse switching time to within 4 nano-sec. and to limit the required switching voltage to within 10 V. This cavity locking scheme can be applied by using only the random data sequence, and without the need of dithering of the cavity. Compared to waveguide modulators, the resonant cavity has a comparable modulating voltage requirement. Because of its bulk geometry, the resonant cavity modulator has the potential of accommodating higher throughput power. Mode matching into the bulk device is easier and typically can be achieved with higher efficiency. An additional control loop is incorporated into the modulator to maintain the cavity on resonance.

Chen, Chien-Chung↗

DOE OSTI2026

Quantum Theory of Surface Lattice Resonances

The collective interactions of nanoparticles arranged in periodic structures give rise to high‐ in‐plane diffractive modes known as surface lattice resonances. Although these resonances and their broader implications have been extensively studied within the framework of classical electrodynamics and linear response theory, a quantum optical theory capable of describing the dynamics of these structures, especially in the presence of material nonlinearities beyond ad hoc few‐mode approximations, is largely missing. To this end, we consider a lattice of metallic nanoparticles coupled to the electromagnetic field and derive the quantum input–output relations within the electric dipole approximation. As applications, we analyze coupling between the nanoparticle array and external quantum emitters, and show how the formalism extends to molecular optomechanics, where the high ‐factors of SLRs enable coupling to collective vibrational modes. We further consider arrays composed of saturable excitonic emitters, demonstrating how emitter nonlinearities can be used to switch the SLR condition between electronic transitions. Using a perturbative approach that accounts for population dynamics, we show how these effects can be probed in pump–probe experiments and give rise to nonlinear phase‐matching phenomena. Our work provides a microscopic framework for modeling SLRs interacting with quantum emitters without phenomenological descriptions of the electromagnetic environment.

molecular optomechanics↗

DOE OSTI2025

High-throughput micro-scale bandgap mapping for perovskite-inspired materials with complex composition space

Abstract To realize the full promise of high-throughput experimental workflows, the rate of sample synthesis must be matched by that of characterization. Of growing interest are contactless optical techniques that can rapidly measure material homogeneity and properties. Here, we present a hyperspectral imaging method to measure local optical bandgap distributions within samples, utilizing spatially-resolved reflectance spectra coupled with automated data analysis. We collect approximately one million optical bandgap data across the compositional space of Cs 3 (Bi x Sb 1-x ) 2 (Br y I 1-y ) 9 perovskite-inspired materials. Our results show non-monotonic bandgap variations (i.e., bandgap bowing) along six composition gradient sequences, in addition to identifying samples with multiple bandgaps in statistics. High-throughput transient absorption spectroscopy reveals that within these compositions, the depletion of the ground state carriers to excited states occurred at discrete energy levels with independent carrier dynamics, consistent with the bandgap observation and indicative of phase separation. This work demonstrates the potential for rapid optical measurements to assess material quality and homogeneity in a high-throughput experimental setting, supporting screening and recipe optimization of optoelectronic material candidates with desired carrier dynamics and optical properties.

Science & Technology - Other Topics↗

DOE OSTI2024

Symmetric second-harmonic generation in sub-wavelength periodically poled thin film lithium niobate

Second-harmonic generation (SHG) extensively employs periodically poled nonlinear crystals through forward quasi-phase-matching to achieve efficient frequency conversion. As poling periods approach sub-micrometers, backward quasi-phase-matching has also been demonstrated, albeit by utilizing pulsed laser drives. The realization of symmetric second-harmonic generation, characterized by counterpropagating pumps, however, has remained elusive despite theoretical predictions. The main challenge lies in achieving strong nonlinear coupling with the poling period below half the wavelength of the second-harmonic light. The recent emergence of high-quality ferroelectric lithium niobate thin films provides an opportunity for achieving precise domain control at submicron dimensions. In this paper, we demonstrate reliable control of ferroelectric domains in a thin film lithium niobate waveguide with a poling period down to 370 nm, thereby realizing highly efficient continuous-wave pumped symmetric SHG. This demonstration not only validates the feasibility of achieving subwavelength periodic poling on waveguides but could also enable submicron ferrolectric domain structures to be leveraged in integrated photonics and nonlinear optics research.

Optics↗

NASA NTRS2001

X-Ray Spectral Study of a Newly Ginga-Detected DQ Her

The goal of this proposal was to observe with ASCA, YY Dra, a DQ Her objected identified using archival Ginga data, in order to complete a high quality ASCA study of Ginga-detected DQ Her stars. There are relatively few DQ Her objects characterized by X-ray pulsations at the white dwarf spin period and optical pulsations at the orbital period and extremely complex X-ray spectra. The ASCA study included seven DQ Her objects. ASCA is able to resolve separate components of the Fe K emission and to set constraints on temperatures in the accretion column, and the mass of the white dwarf. The 40ksec observation, corresponding to roughly three orbital cycles, allowed the study of continuum changes with spin and orbital phase. The ASCA spectrum can be modelled as a bremsstrahlung with evidence for cold, helium-like and hydrogen-like iron emission, and helium-like argon emission. The lines yield a plasma temperature that is compatible with that from the continuum modelling (10-20 keV). The X-ray light-curve clearly shows sinusoidal variation from the spin pulse and shallow absorption dips at the orbital cycle. The derived parameters match well with the -accretion curtain, model for intermediate polars. The results will be presented together with the seven other DQ Her type sources observed with ASCA.

Vrtilek, S.↗

NASA NTRS2014

Structural Characterization of Lateral-grown 6H-SiC am-plane Seed Crystals by Hot Wall CVD Epitaxy

The performance of commercially available silicon carbide (SiC) power devices is limited due to inherently high density of screw dislocations (SD), which are necessary for maintaining polytype during boule growth and commercially viable growth rates. The NASA Glenn Research Center (GRC) has recently proposed a new bulk growth process based on axial fiber growth (parallel to the c-axis) followed by lateral expansion (perpendicular to the c-axis) for producing multi-faceted m-plane SiC boules that can potentially produce wafers with as few as one SD per wafer. In order to implement this novel growth technique, the lateral homoepitaxial growth expansion of a SiC fiber without introducing a significant number of additional defects is critical. Lateral expansion is being investigated by hot wall chemical vapor deposition (HWCVD) growth of 6H-SiC am-plane seed crystals (0.8mm x 0.5mm x 15mm) designed to replicate axially grown SiC single crystal fibers. The post-growth crystals exhibit hexagonal morphology with approximately 1500 m (1.5 mm) of total lateral expansion. Preliminary analysis by synchrotron white beam x-ray topography (SWBXT) confirms that the growth was homoepitaxial, matching the polytype of the respective underlying region of the seed crystal. Axial and transverse sections from the as grown crystal samples were characterized in detail by a combination of SWBXT, transmission electron microscopy (TEM) and Raman spectroscopy to map defect types and distribution. X-ray diffraction analysis indicates the seed crystal contained stacking disorders and this appears to have been reproduced in the lateral growth sections. Analysis of the relative intensity for folded transverse acoustic (FTA) and optical (FTO) modes on the Raman spectra indicate the existence of stacking faults. Further, the density of stacking faults is higher in the seed than in the grown crystal. Bundles of dislocations are observed propagating from the seed in m-axis lateral directions. Contrast extinction analysis of these dislocation lines reveals they are edge type basal plane dislocations that track the growth direction. Polytype phase transition and stacking faults were observed by high-resolution TEM (HRTEM), in agreement with SWBXT and Raman scattering.

Single Crystal↗

DOE OSTI2025

Crystalline Organic Compounds as Effective Nuclei in Contact Efflorescence of Ammonium Sulfate

Contact nucleation is believed to play a role in liquid-to-solid phase transitions in the atmosphere including ice nucleation and salt efflorescence. Here, for this work, contact efflorescence of optically levitated ammonium sulfate droplets by collisions with organic particles is probed using a long working-distance optical trap. Two highly viscous water-soluble organic compounds (d-(+)-raffinose and citric acid), and two insoluble highly surface-active organic compounds (stearic acid and cis-pinonic acid) were probed for their ability to induce efflorescence upon contact. While three of the organics showed minimal effectiveness as contact nuclei, cis-pinonic acid showed a remarkable ability to initiate contact efflorescence of ammonium sulfate, occurring near ammonium sulfate’s deliquescence relative humidity. Further analysis of cis-pinonic acid using bright-field microscopy in an electrodynamic balance provided evidence that the cis-pinonic acid particles are crystalline under the laboratory conditions. We suggest that the close lattice match between crystalline ammonium sulfate and crystalline cis-pinonic acid may account for the observed effectiveness in initiating contact efflorescence of ammonium sulfate. In contrast, tests of contact nucleation between cis-pinonic acid and sodium chloride, a pair with a poor lattice match, did not result in efflorescence. These findings suggest that crystalline organic compounds in the atmosphere could act as effective nuclei for contact efflorescence of atmospherically relevant salts, provided they share a compatible lattice structure.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS1982

Mode characteristics of nonplanar double-heterojunction and large-optical-cavity laser structures

Mode behavior of nonplanar double-heterojunction (DH) and large-optical-cavity (LOC) lasers is investigated using the effective index method to model the lateral field distribution. The thickness variations of various layers for the devices discussed are correlated with the growth characteristics of liquid-phase epitaxy over topographical features (channels, mesas) etched into the substrate. The effective dielectric profiles of constricted double-heterojunction (CDH)-LOC lasers show a strong influence on transverse mode operation: the fundamental transverse mode (i.e., in the plane perpendicular to the junction) may be laterally index-guided, while the first (high)-order mode is laterally index-antiguided. The analytical model developed uses a smoothly varying hyperbolic cosine distribution to characterize lateral index variations. The waveguide model is applied to several lasers to illustrate conditions necessary to convert leaky modes to trapped ones via the active-region gain distribution. Theoretical radiation patterns are calculated using model parameters, and matched to an experimental far-field pattern.

Butler, J. K.↗

NASA NTRS1995

Observational studies of the clearing phase in proto-planetary disk systems

Progress in this study is summarized for its second year. An extensive program of high dispersion UV spectral studies using the IUE (International Ultraviolet Explorer) has resulted in acquisition of 40 Herbig Ae/Be star and related object spectra. We find that accreting, circumstellar gas is detected with velocities consistent with material in free-fall toward the stars in approximately 38% of the sample. With acquisition of optical measurements of the projected stellar rotational velocities, we find that the systems with accreting gas exhibit systematically higher projected rotational velocities than the systems showing signatures of outflowing material only. When combined with polarimetric and photometric data, the IUE spectra for these stars indicate that accretion in intermediate-mass pre-main sequence stars is confined to the plane of the circumstellar dust disk. This is in contrast to lower-mass PMS stars where accretion, persumably along magnetic field lines, is seen at polar latitudes. Our data also support significant clearing of the central regions of these circumstellar disks, as originally suggested. The model which most closely matches the observational data is accretion from a disk envelope, as developed by Calvet et al. (1994).

Grady, Carol A.↗

NASA NTRS2007

Remote and Ground Truth Spectral Measurement Comparisons

FORMOSAT III are a set of six research satellites from Taiwan that were launched in April 2006. The satellites are in 800 km, 71 degree inclination orbits and separated by 24 degrees in ascending node. Ground truth spectral measurements were taken of outer surface materials on FORMOSAT III. From those measurements, a computer model was built to predict the spectral reflectance, which included phase angle and orientation of the spacecraft relative to the observer. However, materials exposed to the space environment have exhibited spectral changes including a darkening and a reddening of the spectra. This reddening was seen as an increase in slope of the reflectance as the wavelength increases. Therefore, the model of pristine materials was augmented to include the space weathering effects. Remote data were collected on two of the six FORMOSAT satellites using the 1.6 meter telescope at AMOS (Air Force Maui Optical and Supercomputing) site with the Spica spectrometer. Due to the separation in ascending node, observations were made on whichever one of the six satellites was visible on that specific night. Three nights of data were collected using the red (6000 9500 angstroms) filter and two nights of data were collected using the blue (3200 -6600 angstroms) filter. A comparison of the data showed a good match to the pristine model for the blue filter region. The absorption feature near 5500 angstroms due to the copper colored Kapton multi-layer insulation (MLI) was very apparent in the remote samples and a good fit to the data was seen in both satellites observed. The features in the red filter regime agreed with the pristine model up through 7000 angstroms where the reddening begins and the slope of the remote sample increases. A comparison of the two satellites showed similar features in the red and blue filter regions, i.e. the satellites were aging at the same rate. A comparison of the pristine model to the first month of remote measurements showed the amount by which the satellite had reddened. This information was used in the space weathered model to predict the second month s reflectance measurement. The results showed that the reddening did not increase from the first month of observations to the second. A third month of data will be necessary to determine if the reddening occurs instantly and then stabilizes with time or if the effect continues to increase with time.

Abercromby, Kira Jorgensen↗

DOE OSTI2021

Production and Performance of High Sulfur Concentration Waste Glasses (FY21)

In FY21 Savannah River National Laboratory (SRNL) was tasked to investigate the practical aspects of low activity waste (LAW) glass production with high sulfur loading for the Office of River Protection (ORP). Relationships between sulfur solubility, retention, and melter resonance need to be evaluated to refine waste loading limits and the super saturated melting (triple melt, grind, and wash) methodology. The impact of high sulfur concentration on durability and phase stability (crystallization and liquid-liquid immiscibility) during slow cooling also needs to be further evaluated. To accomplish this, SRNL proposed scaled melter testing using simulants with matched physicochemical properties to melter feed, as opposed to laboratory reagents. This type of testing is expected to validate applicability to design parameters and functional criteria expected during unit operations. This work was expected to commence in FY21, with the first melter tests being performed near the end of the FY. However, reduced access to Savannah River Site and personnel availability during the COVID-19 pandemic significantly reduced the amount of time and resources available to perform the task. This report documents the experimental plan and progress towards this task. The following is a summarized list of scheduled testing that will be performed on feed, condensate, cold cap and glass: 1) Melter runs; 2) Product consistency test (PCT); 3) Inductively coupled plasma optical emission spectroscopy (ICP-OES); and 4) Optical (OM) and scanning electron microscopy (SEM).

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2025

Tunable coherent mixed-dimensional perovskite heterojunctions and quantum wells grown from solution

Coherent heterojunctions, quantum wells and multiple quantum wells are needed for high-performance devices; these are generally grown via a dedicated vapour phase epitaxy process. Here we demonstrate the growth of coherent perovskite heterojunctions and quantum wells made of mixed-dimensional perovskites using a solution process. By exploiting the solubility difference of methylammonium (MA + ) and 4-(aminomethyl)piperidinium (4AMP 2+ ), we assemble layered perovskites with different layer numbers. The resulting 4AMP-MA n–1 Pb n I 3n+1 materials each with different layer numbers or bandgaps form quantum wells. Heterojunctions and quantum wells made of 4AMP-MA 2 Pb 3 I 10 (n = 3) and 4AMP-MAPb 2 I 7 (n = 2) with various barrier thickness are tailored by the solution temperature profile during crystal growth. Multiple quantum wells have been formed by cycling temperature profiles. The planar heterojunction and quantum wells have lattice matching without interfacial defects, and exhibit strong thermal stability. Type I band alignment at the n = 2/n = 3 heterojunction is confirmed by both computation and optical studies. In conclusion, this study opens a new direction for the development of sophisticated perovskite heterojunction and quantum well devices.

77 NANOSCIENCE AND NANOTECHNOLOGY↗