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At least 433 records · Page 24

Power conversion in SnS photocathodes made by electrochemical growth is limited by recombination at (002) buried facets

Herzenbergite α-SnS is a promising p-type semiconductor for photovoltaic and solar fuel applications, but current devices are plagued by substantial photovoltage losses. Here we use vibrating Kelvin probe surface photovoltage for the first time to study the recombination losses in microcrystalline SnS photoelectrodes. α-SnS films of varied crystal orientation, size, and shape are obtained by electrochemical growth from aqueous tin( II ) chloride and sodium thiosulfate solutions near room temperature. After application of a CdS passivation layer, the films function as photocathodes for the methylviologen reduction reaction. Photoelectrochemical and surface photovoltage measurements reveal that the performance of these devices is sensitively controlled by mainly the SnS crystal orientation and to a lesser extent by the grain size. For example, the highest charge recombination rates of 8.97 × 10 14 s −1 cm −2 and lowest photocurrent (0.73 mA cm −2 ) and lowest photovoltage (0.12 V) occur for SnS films containing 500 nm crystals with irregular shapes and SnS lattices tilted away from the (001) orientation. On the other hand, the best performance (1.62 mA cm −2 , 0.16 V, 3.32 × 10 12 s −1 cm −2 ) is seen for 1100 nm fully (001) oriented SnS nanoplates. Furthermore, these findings agree with improved charge carrier mobility in the 001 direction and they also show that charge recombination in SnS films occurs mainly at dangling Sn–S bonds at buried (002) facets. Such buried interfaces need to be suppressed for optimized solar energy conversion with SnS.

Najaf, Zainab [University of California, Davis, CA↗

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]↗

Radiation Mapping UAV [Poster]

The NuMI (Neutrinos at the Main Injector) target system delivers a high-energy flux of muon-neutrinos towards a detector more than 800 km away with the goal of better understanding the origin of the universe and its evolution. The target system becomes radioactive because it is irradiated by a sub-Mega-Watt power proton beam. Radiological hazard is one of critical issues for a radiological worker which limits the iractivities near the target system; however, they often need to quantify the radiation level of the target system manually. Thus, the objective of this project is to reduce their exposure to radiation while improving the accuracy of the measurements. A quadcopter UAV fitted with a radiation dosimeter is ideal to traverse the irradiated environment as it can be deployed in any space and requires minimal hardware integration to the test room. Due to the lack of indoor GPS signal, this UAV utilizes a series of ultrasonic beacons that release several varied-frequency pulses simultaneously in order to localize the drone. The flight controller returns a 3D coordinate tied to the radiation data to understand precisely where radiation spikes are being emitted from the horn. The flight controller stores log data that can be processed into an easily interpretable map of radiation intensities. The radiation map serves as one of the primary references for planning the transportation of the NuMI horn.

43 PARTICLE ACCELERATORS↗

Simulations of Criticality Control Overpack Container Compaction at the Waste Isolation Pilot Plant

Criticality Control Overpack (CCO) containers are being considered for the disposal of defense-related nuclear waste at the Waste Isolation Pilot Plant (WIPP). At WIPP, these containers would be placed in underground disposal rooms, which will naturally close and compact the containers closer to one another over several centuries. This report details simulations to predict the final container configuration as an input to nuclear criticality assessments. Each container was discretely modeled, including the plywood and stainless steel pipe inside the 55-gallon drum, in order to capture its complex mechanical behavior. Although these high-fidelity simulations were computationally intensive, several different material models were considered in an attempt to reasonably bound the horizontal and vertical compaction percentages. When exceptionally strong materials were used for the containers, the horizontal and vertical closure respectively stabilized at 43:9 % and 93:7 %. At the other extreme, when the containers completely degraded and the clay seams between the salt layers were glued, the horizontal and vertical closure reached respective final values of 48:6 % and 100 %.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Mock-up Waveguide Loop Development toward a half-meter scale Traveling-Wave (TW) SRF cavity

Traveling-Wave (TW) technology can push the accelera-tor field gradient of niobium SRF cavity to 70MV/m or higher beyond the fundamental limit of 50~60MV/m in Standing-Wave regime. The success of TW resonance excitation in a proof-of-principle 3-cell SRF cavity in 2K liquid helium encouraged to advance TW technologies necessary more for future accelerator-scale one. Fermilab has proposed a preliminary RF design of a half-meter scale TW cavity by considering the physical dimensions of existing SRF facilities and the lessons learned from the 3-cell. It consists of a 7-cell structure and a power feed-back waveguide (WG) loop with new TW excitation and control schemes such as, double directional coupler and two WG tuners. Mock-up waveguide loop development was launched under Fermilab LDRD program to demon-strate those new RF schemes at a room temperature. Fab-rication drawings of a mock-up loop were completed. Here details and plans of the development are reported.

Furuta, F. [Fermilab] (ORCID:0009000072218576)↗

Relating Texture and Thermomechanical Processing Variables in Mg–Zn–Ca Alloys

It is well known that the strong basal texture commonly produced in magnesium alloy sheets leads to poor formability at room temperature. A sizable body of work has explored how changing the alloy composition and rolling conditions can yield more desirable textures; however important thermomechanical variables, such as the feed rate during rolling, are often not included in the literature, making it difficult to correlate how changes in processing affect the final crystallographic texture. This work explores the texture evolution and grain refinement in Mg-Zn-Ca alloys during plane strain compression (PSC) using a Gleeble thermomechanical simulator. This instrument allows for precise control and capture of the thermomechanical history of the sample. The texture and grain morphology of the compressed samples were characterized using Electron Backscatter Diffraction (EBSD). The texture results will be used to identify which alloys and processing conditions should be scaled up for future rolling studies.

36 MATERIALS SCIENCE↗

Anti-reflection coating with mullite and Duroid for large-diameter cryogenic sapphire and alumina optics

We developed a broadband two-layer anti-reflection (AR) coating for use on a sapphire half-wave plate (HWP) and an alumina infrared (IR) filter for the cosmic microwave background (CMB) polarimetry. Measuring the faint CMB B-mode signals requires maximizing the number of photons reaching the detectors and minimizing spurious polarization due to reflection with an off-axis incident angle. Sapphire and alumina have high refractive indices of 3.1 and are highly reflective without an AR coating. This paper presents the design, fabrication, quality control, and measured performance of an AR coating using thermally sprayed mullite and Duroid 5880LZ. This technology enables large optical elements with diameters of 600 mm. We also present a thermography-based nondestructive quality control technique, which is key to assuring good adhesion and preventing delamination when thermal cycling. We demonstrate the average reflectance of about 2.6% (0.9%) for two observing bands centered at 90/150 (220/280) GHz. At room temperature, the average transmittance of a 105 mm square test sample at 220/280 GHz is 83%, and it will increase to 90% at 100 K, attributed to reduced absorption losses. Therefore, our developed layering technique has proved effective for 220/280 GHz applications, particularly in addressing dielectric loss concerns. This AR coating technology has been deployed in the cryogenic HWP and IR filters of the Simons Array and the Simons observatory experiments and applies to future experiments such as CMB-S4.

Sakaguri, Kana (ORCID:0000000156678118)↗

Temporal and spatial tuning of optical constants in praseodymium doped ceria by electrochemical means

Abstract Temporal and spatial tuning of the refractive index of optical thin films is desired for flat optics applications. The redistribution of mobile ions in mixed ionic-electronic conductors (MIEC) has been demonstrated to serve as a viable means for achieving optical tuning down to the nanoscale. Here we studied the dynamic range of the optical tuning achievable in the refractive index, in the MIEC oxide – Pr x Ce 1− x O 2− δ (PCO), for x = 0.1, 0.2 and 0.4, at 500 °C, by in-situ spectrophotometry. Significant increases in the modulation of both the imaginary and real optical constants in the visible and the adjacent spectra were obtained for increased doping levels. Device employing an electrochemical titration method was implemented to modulate the oxygen concentration, and thereby the optical transmission of PCO. Incorporation of a patterned top electrode allowed for the demonstration of spatial control of PCO thin film properties by in-situ video imaging of the optical switching process. The electrochemically induced optical state is shown to remain non-volatile upon quenching the device to room temperature under applied bias.

36 MATERIALS SCIENCE↗

Control of microphonics for a superconducting radio-frequency photo-injector cryomodule

A superconducting radio-frequency photo-injector cryomodule is being developed for the high-energy upgrade of the Linac Coherent Light Source (LCLS-II-HE). This effort is a collaboration between the Facility for Rare Isotope Beams at Michigan State University (MSU), Argonne National Laboratory, Helmholtz-Zentrum Dresden-Rossendorf, and SLAC National Accelerator Laboratory. The cryomodule features a 185.7 MHz superconducting quarter-wave resonator (QWR) designed to operate with an RF electric field of 30 MV/m at the photo-cathode. Mechanical vibrations must be controlled for operation with stable amplitude and phase. The first prototype cryomodule was cold-tested at MSU with a QWR, fundamental power coupler, tuner, and cathode stalk. In the cold test, we observed microphonics that made it difficult to control the RF phase at high gradient. The cryogenic circuit was identified as a likely culprit. This paper presents our studies of microphonics during the cryomodule cold test and follow-up investigations at room temperature. Our findings provided valuable feedback for modifications to the cryogenic circuit and a successful second cold test of the cryomodule.

Accelerator Physics↗

Optical-Gating of Spin-based Quantum States (Final Report)

This project developed a generalizable strategy for optical control of spin-based quantum states through the Photoisomerization-Induced Spin–Charge Excited State (PISCES) process, in which a photochromic spirooxazine ligand bound to an electronically bistable metal complex enables reversible, room-temperature optical switching of spin states in both dilute matrices and the solid state. A multidisciplinary team integrated synthesis, spectroscopy, theory, and surface science to establish design principles for opto-spintronic quantum materials. Systematic structure–property studies across four spirooxazine series revealed that donor–π–acceptor interactions govern thermal isomerization, which proceeds via a rotational pathway. Pulsed EPR measurements demonstrated millisecond-scale coherence times in cobalt-dioxolene-spirooxazine complexes, establishing their promise as optically addressable molecular qubits; the approach was extended to Cu(II), Ni(II), and lanthanide complexes, including optical modulation of zero-field splittings and clock transitions. Two-dimensional IR spectroscopy resolved picosecond ground-state population exchange dynamics, while ab initio calculations elucidated photoisomerization mechanisms and parametrized Hamiltonians for spin relaxation and decoherence. Toward device integration, the team fabricated 2D polymer scaffolds for covalent qubit organization, developed tip-enhanced Raman imaging of molecular monolayers, and demonstrated optical gating of gate voltage in spirooxazine-graphene field-effect transistors. The project produced numerous publications, dissertations, and presentations, and trained over 30 researchers.

2D polymers↗

A new dynamic zOnal model with air-diffuser (DOMA) - Application to thermal comfort prediction

A new Dynamic zOnal Model with Air-diffuser (DOMA) was developed. Several case studies were investigated and tested to evaluate and validate this program using measurement data. This new model was integrated into a TRaNsient SYstems Simulation program library and coupled with the multi-zone thermal model. The DOMA/TRNSYS coupled model was then used to predict room temperature distribution over an entire day of a single-zone building. The results show that increasing the heating outputs of the electric floor system, for example, from 75 to 200 W/m 2 , would not effectively improve the indoor thermal comfort, since the thermostat will reach the set point first and then turn off the system before the room gets enough heat and reach a comfortable level. This indicates the importance of selecting an appropriate location and set point for the thermostat when using a floor heating system. This potential thermal comfort issue can only be identified through the two-node model with a dynamic zonal model rather than the conventional PMV model, which thus suggests that for optimizing indoor thermal comfort of a building equipped with a time-sensitive control strategy and/or HVAC system, the TSENS results obtained from the two-node model integrated with DOMA are more appropriate than PMVs.

Construction & Building Technology↗

The Driving Force Controls Charge Separation Distance in Solid-State Organic Donor/Acceptors

In this work, charge pairs of varying separation distance are interpreted from photoinduced absorption detected magnetic resonance (PADMR) spectroscopy of organic, small molecule dilute donor/acceptor thin films. We report that a donor/acceptor film that generates few free charges at room temperature yet has a relatively large, calculated driving force for electron transfer generates a large concentration of tightly bound CT states when measured with PADMR. These states are markedly absent in films with smaller driving forces yet higher free charge yields which instead only show charge-separated state signals with weaker spin coupling. We interpret this result to be in support of a hypothesis where a larger reorganization energy associated with charge transfer to tightly bound CT states means that they are primarily generated in systems far from the Marcus optimum for free charge yield. And the highest free charge yielding systems instead predominantly undergo long-range charge separation into the acceptor host.

charge separation↗

Discovery and Characterization of a Metastable Cubic Interstitial Nickel–Carbon System with an Expanded Lattice

Metastable, i.e., kinetically favored but thermodynamically not stable, interstitial solid solutions of carbon in iron are well-understood. Carbon can occupy the interstitial atoms of the host metal, altering its properties. Alloying of the host metal results in the stabilization of the FeC x phases, widening its application. Pure nickel finds niche applications, mainly focusing on catalysis, while nickel alloys are widely applied, e.g., in gas turbines, reactors, and seawater piping. Nickel carbide (Ni 3 C) is the well-known stable Ni–C system displaying a rhombohedral (R3̅c) crystal structure. Some reports describe an elusive cubic Ni–C system, observed during certain catalytic reactions occurring on nickel and formed by the occupation of the interstitials of the metal with carbon: to date, the stabilization and characterization of this phase have not been accomplished. Hereby, we report on the synthesis of a cubic metastable NiC x phase using chemical vapor deposition of methane on supported nickel nanoparticles. The structure was predicted by DFT/ReaxFF, synthesized and monitored with in situ time-resolved synchrotron XRD, and experimentally confirmed by Rietveld refinement and (S)TEM-EELS under ambient conditions. The results show an Fm3̅m phase with a lattice parameter of a = 3.749 ± 0.037 Å at room temperature, with the highest ever reported atomic percentage of carbon occupying the octahedral interstices of 23.1%, resulting in a NiC 0.3 phase. The degree of occupation of the interstitial voids by carbon can be controlled, enabling the tuning of the host metal’s d-spacing and composition, highlighting the applicability of this synthesis route for catalytic nanoparticle preparation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Flat epitaxial quasi-1D phosphorene chains

The emergence of peculiar phenomena in 1D phosphorene chains (P chains) has been proposed in theoretical studies, notably the Stark and Seebeck effects, room temperature magnetism, and topological phase transitions. Attempts so far to fabricate P chains, using the top-down approach starting from a few layers of bulk black phosphorus, have failed to produce reliably precise control of P chains. We show that molecular beam epitaxy gives a controllable bottom-up approach to grow atomically thin, crystalline 1D flat P chains on a Ag(111) substrate. Scanning tunneling microscopy, angle-resolved photoemission spectroscopy, and density functional theory calculations reveal that the armchair-shaped chains are semiconducting with an intrinsic 1.80 ± 0.20 eV band gap. This could make these P chains an ideal material for opto-electronic devices.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Optoelectronic memristor devices including one or more solid electrolytes with electrically controllable optical properties

An optoelectronic memristor includes a first electrode, a second electrode, and a solid electrolyte in between that is in electrical communication with the first electrode and the second electrode. The solid electrolyte has an electronic conductivity of about 10 −10 Siemens/cm to about 10 −4 Siemens/cm at room temperature. The first electrode, and optionally the second electrode, can be optically transparent at a specific wavelength and/or a wavelength range. A direct current (DC) voltage source is employed to apply an electric field across the solid electrolyte, which induces a spatial redistribution of ionic defects in the solid electrolyte. In turn, this causes a change in electrical resistance of the solid electrolyte. The application of the electric field can also cause a change in an optical property of the solid electrolyte at the specific wavelength, and/or at the wavelength range (or a portion thereof).

Defferriere, Thomas↗

Toward Full Configuration Interaction for Transition-Metal Complexes

In this work, an efficacious approximation to full configuration interaction (FCI) is adapted to calculate singlet-triplet gaps for transition-metal complexes. This strategy, incremental FCI (iFCI), uses a many-body expansion to systematically add correlation to a simple reference wave function and therefore achieves greatly reduced computational costs compared to FCI. iFCI through the 3-body expansion is demonstrated on four model transition-metal complexes involving the metals Zn, V, and Cu. Screening techniques to increase the computational efficiency of iFCI are proposed and tested, showing reduction in the number of 3-body terms by more than 90% with controlled errors. The largest complex treated by iFCI has 142 valence electrons, all of which are correlated among the full set of 444 active orbitals. Computed spin gaps approach experimental results for the four complexes, though room for improvement remains.

74 ATOMIC AND MOLECULAR PHYSICS↗

Chemical instability at chalcogenide surfaces impacts chalcopyrite devices well beyond the surface

The electrical and optoelectronic properties of materials are determined by the chemical potentials of their constituents. The relative density of point defects is thus controlled, allowing to craft microstructure, trap densities and doping levels. Here, we show that the chemical potentials of chalcogenide materials near the edge of their existence region are not only determined during growth but also at room temperature by post-processing. In particular, we study the generation of anion vacancies, which are critical defects in chalcogenide semiconductors and topological insulators. The example of CuInSe 2 photovoltaic semiconductor reveals that single phase material crosses the phase boundary and forms surface secondary phases upon oxidation, thereby creating anion vacancies. The arising metastable point defect population explains a common root cause of performance losses. This study shows how selective defect annihilation is attained with tailored chemical treatments that mitigate anion vacancy formation and improve the performance of CuInSe 2 solar cells.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

High-frequency electrical behavior in V 3 O 5 thin films

Vanadium oxides are known for their metal–insulator transition (MIT), with V 3 O 5 being notable for its transition temperature exceeding room temperature. At about 430 K, this material shows a change in crystal symmetry accompanied with one order of magnitude increase in its electrical conductivity and alterations in its optical properties. Although the property changes during the MIT in V 3 O 5 are less pronounced than those observed in VO 2 , its transition temperature is 90 K higher, making it appealing for applications requiring elevated temperatures. In this article, the high-frequency characteristics were determined in a V 3 O 5 two-terminal device in the range from 5 to 35 GHz. The S-parameters showed that the return loss at room temperature was close to −1.5 dB, and the isolation between ports was approximately −50 dB. At temperatures above the metal–insulator transition, the isolation decreased to around −40 dB at 35 GHz. For S11 and S22, similar behavior was observed at room temperature, with a notable change in the S-parameter phase of the device. This behavior suggests that V 3 O 5 may function well as a capacitor because the considerable change in phase could control the flow of electrical signals in devices. This property also may be used for matching purposes, especially considering its response to temperature changes. Additionally, conductivity calculation from S-parameters shows a decrease of approximately two orders of magnitude at 500 K and one order of magnitude at 300 K compared to DC values. These findings highlight V 3 O 5 potential for integration into radio frequency devices that demand consistent performance in high-temperature environments.

36 MATERIALS SCIENCE↗