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At least 73 records · Page 4

Thiol‐Functionalized Conjugated Metal–Organic Frameworks for Stable and Efficient Perovskite Photovoltaics

Abstract Metal–organic frameworks (MOFs) have been investigated recently in perovskite photovoltaics owing to their potential to boost optoelectronic performance and device stability. However, the impact of variations in the MOF side chain on perovskite characteristics and the mechanism of MOF/perovskite film formation remains unclear. In this study, three nanoscale thiol‐functionalized UiO‐66‐type Zr‐based MOFs (UiO‐66‐(SH) 2 , UiO‐66‐MSA, and UiO‐66‐DMSA) are systematically employed and examined in perovskite solar cells (PSCs). Among these MOFs, UiO‐66‐(SH) 2 , with its rigid organic ligands, exhibited a strong interaction with perovskite materials with more efficient suppression of perovskite vacancy defects. More importantly, A detailed and in‐depth discussion is provided on the formation mechanism of UiO‐66‐(SH) 2 ‐assisted perovskite film upon in situ GIWAXS performed during the annealing process. The incorporation of UiO‐66‐(SH) 2 additives substantially facilitates the conversion of PbI 2 into the perovskite phase, prolongs the duration of stage I, and induces a delayed phase transformation pathway. Consequently, the UiO‐66‐(SH) 2 ‐assisted device demonstrates reduced defect density and superior optoelectronic properties with optimized power conversion efficiency of 24.09% and enhanced long‐term stability under ambient environment and continuous light illumination conditions. This study acts as a helpful design guide for desired MOF/perovskite structures, enabling further advancements in MOF/perovskite optoelectronic devices.

14 SOLAR ENERGY↗

Unveiling the Morphological and Physical Mechanism of Burn–in Loss Alleviation by Ternary Matrix Toward Stable and Efficient All–Polymer Solar Cells

All–polymer solar cells (All–PSCs) are considered the most promising candidate in achieving both efficient and stable organic photovoltaic devices, yet the field has rarely presented an in–depth understanding of corresponding device stability while efficiency is continuously boosted via the innovation of polymer acceptors. Herein, a ternary matrix is built for all–PSCs with optimized morphology, improved film ductility and importantly, boosted efficiency and better operational stability than its parental binary counterparts, as a platform to study the underlying mechanism. The target system PQM–Cl:PTQ10:PY–IT (0.8:0.2:1.2) exhibits an alleviated burn–in loss of morphology and efficiency under light soaking, which supports its promoted device lifetime. The comprehensive characterizations of fresh and light–soaked active layers lead to a clear illustration of opposite morphological and physical degradation direction of PQM–Cl and PTQ10, thus resulting in a delicate balance at the optimal ternary system. Specifically, the enlarging tendency of PQM–Cl and shrinking preference of PTQ10 in terms of phase separation leads to a stable morphology in their mixing phase; the hole transfer kinetics of PQM–Cl:PY–IT host is stabilized by incorporating PTQ10. Finally, this work succeeds in reaching a deep insight into all–PSC's stability promotion by a rational ternary design, which booms the prospect of gaining high–performance all–PSCs.

14 SOLAR ENERGY↗

A Flexible, Redox-Active, Aqueous Electrolyte-Based Asymmetric Supercapacitor with High Energy Density Based on Keratin-Derived Renewable Carbon

This work exploits the advantage of asymmetric configuration over symmetric supercapacitor in designing high energy density flexible devices from two active electrode materials–keratin-based renewable-resource hierarchically porous carbon and hydrous ruthenium oxide (RuO 2 ). Here, the asymmetric device exhibits significantly high capacitance. Conventional estimation of energy storage parameters, however, cannot be applied for devices with a Faradaic energy storage contribution via redox charge transfer mechanism. Therefore, this work applies a precise measurement of pseudocapacitance contribution at various scan rates to correct the device data that reveals effective capacitance of 120 F g –1 with the energy density of 37 W h kg –1 at 776 W kg –1 . It also retains excellent rate capability, >74% at high current density 25 A g –1 . The charge storage activity and device stability can be further enhanced by introducing redox-active electrolytes that improve specific capacitance, but the rate capabilities deteriorate at high current densities. Further, the principle of asymmetric electrode design is applied to fabricate a bending-tolerant, flexible device by depositing active electrode material on wire-shaped current collector followed by coupling those separated with polyvinyl alcohol gel containing redox electrolyte; it yields 36.8 mF cm –1 specific capacitance at a 0.2 mA cm –1 current density.

36 MATERIALS SCIENCE↗

Trimerized small-molecule acceptors enable high-performance organic solar cells with high open-circuit voltage and prolonged life-time

Although the recent development of Y-series small-molecule acceptors (SMAs) has led to a dramatic increase in the power conversion efficiency (PCE) of organic solar cells (OSCs), the operational stability (device lifetime) of OSCs is inadequate for commercialization. In this study, we develop a new trimer acceptor (TYT), consisting of three Y-based molecules linked by electron-donating spacers, to realize an OSC with high-performance (PCE > 18%) and -stability (t 80% lifetime > 8000 h under 1 sun illumination, in which t 80% lifetime is the time required for the PCE of the OSC to reach 80% of its initial value). We demonstrate that the trimerization approach affords an acceptor, TYT, with an upshifted lowest unoccupied molecular orbital energy level, which, in turn, affords an efficient OSC with a high open-circuit voltage (0.964 V). In addition, the glass-transition temperature (T g ) of TYT (217 °C) is significantly higher than those of monomer (MYT, T g = 80 °C) and dimer (DYT, T g = 127 °C) acceptors, which effectively suppresses the molecular diffusion of TYT in a blend film with a polymer donor. Accordingly, a TYT-based OSC demonstrates a high PCE (18.2%) and long t 80% lifetime under 1 sun illumination (8454 h), outperforming MYT- and DYT-based OSCs that exhibit PCEs and t 80% lifetimes of 16.4% and 35 h, and 17.3% and 2551 h, respectively. Therefore, this study provides important guidelines for the design of electron acceptors in achieving OSCs with high performance and stability close to a commercial level.

14 SOLAR ENERGY↗

External Radiation and Magnetic-Field Effects on the Coherence and Stability of Transmon Qubits

Superconducting transmon qubits are a central building block of modern quantum computing architectures, yet their coherence properties remain sensitive to external influences that can limit performance or introduce temporal instabilities. In this talk, I will discuss two experimental studies aimed at quantifying these effects. First, I will examine how ionizing radiation impacts qubit relaxation. Using the same transmon device operated at two locations with dramatically different radiation backgrounds—the above-ground SQMS facility at Fermilab (USA) and the deep-underground Gran Sasso Laboratory (Italy)—we observe a higher rate of radiation-induced decay events above ground, even though intrinsic noise remains the dominant source of single-shot errors. I will also discuss the detection efficiency of a radiation detector made using such a device. Second, I will present results on how small magnetic fields, applied either during cooldown or at millikelvin temperatures, influence device stability. We find that fixed-frequency transmons maintain robust coherence up to approximately 600 mG of trapped out-of-plane field, and that controlled application of magnetic field can reduce temporal fluctuations in T1. Together, these studies provide insight into how external environments shape transmon coherence and offer potential pathways for improving qubit stability in scalable quantum processors.

Roy, Tanay [Fermilab]↗

Performance characterization of 5×5×12 mm 3 virtual Frisch-grid TlBr detectors

Thallium bromide (TlBr) is a promising material for semiconductor gamma-ray detectors due to its high atomic number (Tl = 81, Br = 35), high density (7.56 g/cm 3 ), and relatively low melting point (460 °C). These properties give TlBr several competitive features, including high detection efficiency, good energy resolution, and lower fabrication costs, making it suitable for applications requiring compact, highly sensitive gamma-ray detection systems. Recent developments of TlBr detectors have progressed toward thicker crystals, up to 10–20 mm, configured as pixelated or virtual Frisch-grid (VFG) devices with volumes >1 cm 3 . Despite these advances, challenges remain in practical implementation, including material and fabrication issues that affect energy resolution, device stability, performance, and longevity. These challenges are similar to those faced by HgI 2 and lead-halide perovskite detectors. Here, this study presents results from characterizing over 100 position-sensitive 5×5×12 mm 3 virtual Frisch-grid detectors fabricated by Radiation Monitoring Devices Inc. For a prototype Radioisotope Identification Device (RIID). The work identified factors limiting the performance and longevity of TlBr detectors, including stochastic response variations that limit the energy resolution to 2–3 % (at 662 keV) for most devices, performance degradation associated with defect decoration, and contact delamination. Addressing these issues advances the use of TlBr and similar materials for reliable, high-resolution gamma-ray spectroscopy.

47 OTHER INSTRUMENTATION↗

Stability of Cu(In x Ga 1− x )Se 2 Solar Cells Utilizing RbF Postdeposition Treatment under a Sulfur Atmosphere

Alkali halide postdeposition treatments (PDTs) have become a key tool to maximize efficiency in Cu(In x Ga 1− x )Se 2 (CIGS) photovoltaics. RbF PDTs have emerged as an alternative to the more common Na‐ and K‐based techniques. This study utilizes temperature‐dependent current–voltage ( JVT ) measurements to study a unique RbF PDT performed in a S atmosphere. The samples are measured before and after 6 months in a desiccator to study device stability. Both samples contain Na and K which diffuse from the soda–lime glass substrate. A reference sample and a RbF + S PDT sample both show the development of a rear contact barrier after aging. The contact barrier is higher for the RbF + S PDT sample, leading to decreased current in forward bias. Series resistance is also higher in the RbF + S PDT device which leads to lower fill factor. However, after aging the reference sample has a larger decrease in open‐circuit voltage ( V OC ). Ideality factor measurements suggest Shockley–Read–Hall recombination dominates both samples. V OC versus temperature and a temperature‐dependent activation energy model are used to calculate diode activation energies for each sample condition. Both techniques produce similar values that indicate recombination primarily occurs within the bulk absorber.

14 SOLAR ENERGY↗

Exploring Local Ionic Motion in Perovskite Solar Cells at Nanoscale through Scanning Thermo-Ionic Microscopy

We investigate the local ionic motion in the absorber layer of perovskite solar cells using scanning thermo-ionic microscopy (STIM). STIM images of perovskite films show higher STIM amplitude at most of the grain boundaries due to higher ionic motion at those regions. The perovskite absorber layer of devices aged under blue (450 nm) light soaking shows higher amplitude in STIM signal compared to controls kept in dark storage. Such enhancement of STIM amplitude upon aging under light implies an increased concentration or diffusivity (or both) of mobile ionic species in stressed devices. Our results demonstrate the utilization of the STIM technique to assess and understand the intrinsic local ionic motion in perovskite absorbers for further advancement in device stability and functionality.

aging↗

Cooperative control of a DNA origami force sensor

Abstract Biomolecular systems are dependent on a complex interplay of forces. Modern force spectroscopy techniques provide means of interrogating these forces, but they are not optimized for studies in constrained environments as they require attachment to micron-scale probes such as beads or cantilevers. Nanomechanical devices are a promising alternative, but this requires versatile designs that can be tuned to respond to a wide range of forces. We investigate the properties of a nanoscale force sensitive DNA origami device which is highly customizable in geometry, functionalization, and mechanical properties. The device, referred to as the NanoDyn, has a binary (open or closed) response to an applied force by undergoing a reversible structural transition. The transition force is tuned with minor alterations of 1 to 3 DNA oligonucleotides and spans tens of picoNewtons (pN). The DNA oligonucleotide design parameters also strongly influence the efficiency of resetting the initial state, with higher stability devices (≳10 pN) resetting more reliably during repeated force-loading cycles. Finally, we show the opening force is tunable in real time by adding a single DNA oligonucleotide. These results establish the potential of the NanoDyn as a versatile force sensor and provide fundamental insights into how design parameters modulate mechanical and dynamic properties.

59 BASIC BIOLOGICAL SCIENCES↗

Oxidative instability of ionomers in hydroxide-exchange-membrane water electrolyzers

Hydroxide-exchange membrane (HEM) electrolyzers can produce green H 2 with only earth-abundant catalysts and electrolyte-free (nominally pure) water feed, significantly decreasing system cost and complexity. However, HEM technology suffers from short lifetimes, attributed in part to poor stability of anion-exchange polymers used in the membrane and catalyst layers. We use electrochemical analysis and ex situ characterization techniques to study anion-exchange-polymer degradation in electrolyzers. Using multiple ionomers, catalyst-layer additives, and electrolyte feed, we show how anode-ionomer oxidation is the dominant degradation mechanism for all HEM-based electrolyzer cells tested. Here, we find improved device stability using oxidation-resistant catalyst-layer binders and propose new design strategies for advanced ionomer and catalyst-layer development.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Defect engineering in wide-bandgap perovskites for efficient perovskite–silicon tandem solar cells

Wide-bandgap (WBG) mixed-halide perovskites show promise of realizing efficient tandem solar cells but at present suffer from large open-circuit voltage loss and the mechanism is still unclear. Here we show that WBG perovskites with iodide–bromide compositions have an increased concentration of deep traps induced by iodide interstitials, which limits performance of WBG perovskite cells. We employ tribromide ions to suppress the iodide interstitial formation and thus reduce charge recombination in bladed WBG perovskite films of Cs 0.1 FA 0.2 MA 0.7 Pb(I 0.85 Br 0.15 )3. The 1-µm-thick opaque WBG perovskite solar cells have an efficiency of 21.9%, a small open-circuit voltage deficit of 0.40 V and a large fill factor of 83%. The efficiency of the best-performing monolithic perovskite–silicon tandem cell using this perovskite reaches 28.6%. Furthermore, the tribromide addition also suppresses light-induced phase segregation in WBG perovskites and thus enhance device stability. Encapsulated tandem cells maintain 93% of their initial efficiency after operation for 550 h.

14 SOLAR ENERGY↗

Electro-Thermal Simulation Studies of SiC Junction Diodes Containing Screw Dislocations Under High Reverse-Bias Operation

The objective of this work was to conduct a modeling study of SiC P-N junction diodes operating under high reverse biased conditions. Analytical models and numerical simulation capabilities were to be developed for self-consistent electro-thermal analysis of the diode current-voltage (I-V) characteristics. Data from GRC indicate that screw dislocations are unavoidable in large area SiC devices, and lead to changes in the SiC diode electrical response characteristics under high field conditions. For example, device instability and failures linked to internal current filamentation have been observed. The physical origin of these processes is not well understood, and quantitative projections of the electrical behavior under high field and temperature conditions are lacking. Thermal calculations for SiC devices have not been reported in the literature either. So estimates or projections of peak device temperatures and power limitations do not exist. This numerical study and simulation analysis was aimed at resolving some of the above issues. The following tasks were successfully accomplished: (1) Development of physically based models using one- and two-dimensional drift-diffusion theory for the transport behavior and I-V characteristics; (2) One- and two-dimensional heat flow to account for internal device heating. This led to calculations of the internal temperature profiles, which in turn, were used to update the electrical transport parameters for a self-consistent analysis. The temperature profiles and the peak values were thus obtainable for a given device operating condition; (3) Inclusion of traps assumed to model the presence of internal screw dislocations running along the longitudinal direction; (4) Predictions of the operating characteristics with and without heating as a function of applied bias with and without traps. Both one and two-dimensional cases were implemented; (5) Assessment of device stability based on the operating characteristics. The presence of internal non-uniformities, particularly filamentary structures, was probed and demonstrated; (6) Cause and physical origins of filamentary behavior and unstable I-V characteristics were made transparent; (7) It was demonstrated that diodes containing defects would be more prone to thermal breakdown associated with the temperature dependent decrease in the thermal conductivity; and (8) Finally, negative differential resistance (S-shaped NDR) which can potential lead to device instability and filamentary behavior was shown to occur for diodes containing a line of defects such as could be associated with a screw dislocation line.

Joshi, R. P.↗

A thermotropic liquid crystal enables efficient and stable perovskite solar modules

Perovskite solar cells have seen impressive progress in performance and stability, yet maintaining efficiency while scaling area remains a challenge. Here we find that additives commonly used to passivate large-area perovskite films often co-precipitate during perovskite crystallization and aggregate at interfaces, contributing to defects and to spatial inhomogeneity. Here we develop design criteria for additives to prevent their evaporative precipitation and enable uniform passivation of defects. We explored liquid crystals with melting point below the perovskite processing temperature, functionalization for defect passivation and hydrophobicity to improve device stability. We find that thermotropic liquid crystals such as 3,4,5-trifluoro-4'-(trans-4-propylcyclohexyl)biphenyl enable large-area perovskite films that are uniform, low in defects and stable against environmental stress factors. We demonstrate modules with a certified stabilized efficiency of 21.1% at an aperture area of 31 cm 2 and enhanced stability under damp-heat conditions (ISOS-D-3, 85% relative humidity, 85 °C) with T 86 (the duration for the efficiency to decay to 86% of the initial value) of 1,200 h, and reverse bias with (ISOS-V-1, negative maximum-power-point voltage) and without bypass diodes.

14 SOLAR ENERGY↗

Reconfiguring the band-edge states of photovoltaic perovskites by conjugated organic cations

The band edges of metal-halide perovskites with a general chemical structure of ABX 3 (A, usually a monovalent organic cation; B, a divalent cation; and X, a halide anion) are constructed mainly of the orbitals from B and X sites. Hence, the structural and compositional varieties of the inorganic B–X framework are primarily responsible for regulating their electronic properties, whereas A-site cations are thought to only help stabilize the lattice and not to directly contribute to near-edge states. We report a π-conjugation–induced extension of electronic states of A-site cations that affects perovskite frontier orbitals. The π-conjugated pyrene-containing A-site cations electronically contribute to the surface band edges and influence the carrier dynamics, with a properly tailored intercalation distance between layers of the inorganic framework. Lastly, the ethylammonium pyrene increased hole mobilities, improved power conversion efficiencies relative to that of a reference perovskite, and enhanced device stability.

36 MATERIALS SCIENCE↗

Accelerated Selectrion of Optimal Perovskite Alloys for Solar PV using a Combined Quantum and Machine Learning Hierachiral Approach

The project aims to: (i) accelerate the discovery of “Missing HP alloys” by combining quantum mechanics and artificial intelligence machine learning approaches, and (ii) analyze the stabilities of candidate alloys, including those that do not pass selection filters (and are thus expected to degrade over time) to decipher the nature of the instabilities to guide the development of durable solar cell materials. Successful candidates will be subjected to validation experiments at NREL's state-of-the-art facilities. The discoveries this effort will provide will be directly testable and implementable and will greatly impact U.S. progress in HP PV as they will provide clear direction and motivation for experimental studies including specific material synthetic targets, device optimization, and device stability protocols. A key advantage of this effort is the feedback and guidance provided by the Industry Collaborative Work Group that we established to coordinate academic and national lab research with industry needs. The proposed work will provide a basis for and direct the development of robust and reliable HP PV. It will also provide a timely, valuable and extensive roadmap to the experimental HP PV community to enable it to focus its efforts on improving and fine-tuning promising HP compositions that this effort predicts will likely be the best performers rather than wandering in the vast chemical space for decades spending enormous resources mostly evaluating unpromising candidate materials.

14 SOLAR ENERGY↗

Recent advances of two-dimensional material additives in hybrid perovskite solar cells

Perovskite solar cells (PSCs) have become one of the state-of-the-art photovoltaic technologies due to their facile solution-based fabrication processes combined with extremely high photovoltaic performance originating from excellent optoelectronic properties such as strong light absorption, high charge mobility, long free charge carrier diffusion length, and tunable direct bandgap. However, the poor intrinsic stability of hybrid perovskites under environmental stresses including light, heat, and moisture, which is often associated with high defect density in the perovskite, has limited the large-scale commercialization and deployment of PSCs. The use of process additives, which can be included in various subcomponent layers in the PSC, has been identified as one of the effective approaches that can address these issues and improve the photovoltaic performance. Among various additives that have been explored, two-dimensional (2D) materials have emerged recently due to their unique structures and properties that can enhance the photovoltaic performance and device stability by improving perovskite crystallization, defect passivation, and charge transport. In this work, we provide a review of the recent progresses in 2D material additives for improving the PSC performance based on key representative 2D material systems, including graphene and its derivatives, transitional metal dichalcogenides, and black phosphorous, providing a useful guideline for further exploiting unique nanomaterial additives for more efficient and stable PSCs in the near future.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Regiospecific Incorporation of Acetylene Linker in High‐Electron Mobility Dimerized Acceptors for Organic Solar Cells with High Efficiency (18.8%) and Long 1‐Sun Lifetime (> 5000 h)

Abstract The commercialization of organic solar cells (OSCs) requires both high power conversion efficiency (PCE) and long‐term stability. However, the lifetime of the OSCs containing small‐molecule acceptors (SMA) should be significantly enhanced. In this study, a series of planarity‐controlled is developed, high electron mobility dimerized SMAs (DSMAs) and realize OSCs with high‐performance (PCE = 18.8%) and high‐stability ( t 80% lifetime = 5380 h under 1‐Sun illumination). An acetylene linker with a planar triple bond is designed for dimerization of SMA units to afford the high backbone planarity necessary to achieve high crystallinity and electron mobility. To further engineer the molecular conformation and electron mobility of the DSMAs, different regioisomers of a Y‐based SMA are dimerized to yield three regioisomerically distinct DSMAs, denoted as DYA‐I, DYA‐IO, and DYA‐O, respectively. It is found that the crystallinity, electron mobility, and glass transition temperature of the DSMAs gradually increase in the order of DYA‐O, DYA‐IO, and DYA‐I, which, in turn, enhance the PCE and device stability of the resulting OSCs; DYA‐O (PCE = 16.45% and t 80% lifetime = 3337 h) < DYA‐IO (PCE = 17.54% and t 80% lifetime = 4255 h) < DYA‐I (PCE = 18.83% and t 80% lifetime = 5380 h).

Chemistry↗

Effects of Replacing Treadmill Running with Alternative Exercise Countermeasures During Long-Duration Spaceflight

Introduction: Current exercise countermeasures on the International Space Station (ISS), including treadmill running, cycle ergometry, and resistive exercise, are used to protect crewmember health and performance during long-duration spaceflight. However, exploration vehicles for Artemis and beyond will have volume and power restrictions, requiring exercise hardware to have a smaller footprint and use fewer resources. Thus, recent efforts have focused on developing exercise devices that provide both aerobic and resistive training on one platform without including a treadmill, such as the European Enhanced Exploration Exercise Device (E4D). It is critical to validate the efficacy of exploration-focused exercise modalities to preserve muscle strength, aerobic fitness, bone density, and sensorimotor performance. Thus, the aim of this study is to determine the physiological effects of spaceflight that occur with nominal ISS exercise prescriptions compared to exploration-forward exercise modalities to determine if a treadmill is required to maintain current levels of protection during long-duration missions. Methods: Crewmembers will be assigned to one of three groups: 1) Control Group (n ≥ 40) who will partake in nominal exercise on the ISS, including running on the treadmill with vibration isolation system 2 (T2), ergometry on the cycle ergometer with vibration isolation and stabilization device (CEVIS), and strength training on the advanced resistive exercise device (ARED); 2) Active Group 1, who will partake in CEVIS and ARED exercise only (n = 8); and 3) Active Group 2, who will partake in aerobic and resistive exercise on the E4D only (n = 8). For Active Group 1, nominal aerobic exercise on T2 will be replaced with corresponding exercise on CEVIS. For Active Group 2, a dedicated exercise prescription will be designed to maximize the capabilities of the E4D to include resistive exercise, cycle ergometry, rowing, and rope pulling. Crewmembers in both active groups will not be permitted to perform treadmill exercise. Health and performance markers including bone mineral density (dual-energy x-ray absorptiometry [DXA]), body composition (DXA), cardiovascular fitness (cycle VO2peak), muscle strength and endurance (isometric/isokinetic testing, power endurance testing), sensorimotor performance (sit-to-stand, obstacle course), postural control (computerized dynamic posturography), and blood and urine biochemical markers of bone metabolism will be assessed before, during, and following spaceflight. Results: Data collection for this study is currently in progress. Conclusions: This study will assess the efficacy of exploration exercise modalities, including the effects of removing the treadmill exercise capability or of exclusively using the E4D, compared to nominal ISS exercise across an entire mission on bone, muscle, aerobic, and sensorimotor health and performance. Findings from this study will help provide a recommendation on whether these exploration exercise modalities can sufficiently protect against physiological deconditioning during spaceflight or whether a treadmill may be required to maintain current levels of protection during future exploration class spaceflight missions.

A.N. Varanoske↗