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At least 379 records · Page 21

Prospects of Nanoscience with Nanocrystals: 2025 Edition

Abstract Nanocrystals (NCs) of various compositions have made important contributions to science and technology, with their impact recognized by the 2023 Nobel Prize in Chemistry for the discovery and synthesis of semiconductor quantum dots (QDs). Over four decades of research into NCs has led to numerous advancements in diverse fields, such as optoelectronics, catalysis, energy, medicine, and recently, quantum information and computing. The last 10 years since the predecessor perspective “Prospect of Nanoscience with Nanocrystals” was published in ACS Nano have seen NC research continuously evolve, yielding critical advances in fundamental understanding and practical applications. Mechanistic insights into NC formation have translated into precision control over NC size, shape, and composition. Emerging synthesis techniques have broadened the landscape of compounds obtainable in colloidal NC form. Sophistication in surface chemistry, jointly bolstered by theoretical models and experimental findings, has facilitated refined control over NC properties and represents a trusted gateway to enhanced NC stability and processability. The assembly of NCs into superlattices, along with two-dimensional (2D) photolithography and three-dimensional (3D) printing, has expanded their utility in creating materials with tailored properties. Applications of NCs are also flourishing, consolidating progress in fields targeted early on, such as optoelectronics and catalysis, and extending into areas ranging from quantum technology to phase-change memories. In this perspective, we review the extensive progress in research on NCs over the past decade and highlight key areas where future research may bring further breakthroughs.

Chemistry↗

Revealing Solvent-Assisted Li+ Transport in the Solid Electrolyte Interphase operando

The performance of energy-dense lithium metal batteries is critically influenced by the properties of the solid electrolyte interphase (SEI). Yet, progress in understanding this layer has been limited by the lack of accurate operando characterization because the SEI evolves dynamically during cycling. Here, we apply dynamic electrochemical impedance spectroscopy (dEIS) to resolve the real-time evolution of the SEI on lithium metal in ether-based electrolytes with varying degrees of fluorination. We find that faster stabilization of the compact SEI resistance correlates with improved passivation and higher Coulombic efficiency. Unexpectedly, compact SEI resistance correlates directly with Li+ solvation energy, revealing that weaker Li+ solvation increases not only bulk but also interphase resistance. These findings challenge the conventional view of the SEI as a purely solid-phase conductor and instead support a solvent-assisted Li+ transport mechanism within the compact SEI. This framework emphasizes the need to balance SEI ionic conductivity with the Li+ solvation environment to maximize lithium metal battery performance.

Sacci, Robert [ORNL] (ORCID:0000000200735221)↗

Scalable fabrication and coating methods for perovskite solar cells and solar modules

Since the report in 2012 of a solid-state perovskite solar cell (PSC) with a power-conversion efficiency (PCE) of 9.7% and a stability of 500 h, intensive efforts have been made to increase the certified PCE, reaching 25.2% in 2019. The PCE of PSCs now exceeds that of conventional thin-film solar-cell technologies, and the rate at which this increase has been achieved is unprecedented in the history of photovoltaics. Moreover, the development of moisture-stable and heat-stable materials has increased the stability of PSCs. Small-area devices (<1 cm2) are typically fabricated using a spin-coating method; however, this approach may not be suitable for the preparation of the large-area (>100 cm2) substrates required for commercialization. Thus, materials and methods need to be developed for coating large-area PSCs. In this Review, we discuss solution-based and vapour-phase coating methods for the fabrication of large-area perovskite films, examine the progress in performance and the parameters affecting the properties of large-area coatings, and provide an overview of the methodologies for achieving high-efficiency perovskite solar modules.

14 SOLAR ENERGY↗

Molecular understanding of heteronuclear active sites in heme–copper oxidases, nitric oxide reductases, and sulfite reductases through biomimetic modelling

Heme-copper oxidases (HCO), nitric oxide reductases (NOR), and sulfite reductases (SiR) catalyze the multi-electron and multi-proton reductions of O 2 , NO, and SO 3 2- , respectively. Each of these reactions is important to drive cellular energy production through respiratory metabolism and HCO, NOR, and SiR evolved to contain heteronuclear active sites containing heme/copper, heme/nonheme iron, and heme-[4Fe-4S] centers, respectively. The complexity of the structures and reactions of these native enzymes, along with their large sizes and/or membrane associations, make it challenging to fully understand the crucial structural features responsible for the catalytic properties of these active sites. Here, we summarize progress that has been made to better understand these heteronuclear metalloenzymes at the molecular level though study of the native enzymes along with insights gained from biomimetic models comprising either small molecules or proteins. Further understanding the reaction selectivity of these enzymes is discussed through comparisons of their similar heteronuclear active sites, and we offer outlook for further investigations and areas of ongoing study.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Influence of processing parameters on long lasting hybrid phosphor for LED applications

Rare earth activated hybrid phosphors have made significant progress in terms of better light output, color properties and potential for long life. All these features coupled with low cost production and reduced maintenance have offered phosphor converted LEDs for diverse optoelectronic applications including signal lighting in advanced aviation. The present paper explores the effect of various processing parameters on luminescent hybrid phosphors fabricated through combustion synthesis.

36 MATERIALS SCIENCE↗

Mossbauer effect in dilute iron alloys

The effects of variable concentration, x, of Aluminum, Germanium, and Lanthanum atoms in Iron lattice on various Mossbauer parameters was studied. Dilute binary alloys of (Fe-Al), (Fe-Ge), (Fe-Al) containing up to x = 2 a/o of the dilute constituent were prepared in the form of ingots and rolled to a thickness of 0.001 in. Mossbauer spectra of these targets were then studied in transmission geometry to measure changes in the hyperfine field, peak widths isomer shifts as well as the ratio of the intensities of peaks (1,6) to the intensities of peaks (2,5). It was shown that the concept of effective hyperfine structure field in very dilute alloys provides a useful means of studying the effects of progressively increasing the solute concentration on host lattice properties.

Singh, J. J.↗

Simulation of flight-type engine fan noise in the NASA-Lewis 9 x 15 anechoic wind tunnel

A major problem in the measurement of aircraft engine fan noise is the difficulty of simulating, in a ground-based facility, the noise that occurs during flight. Flight-type noise as contrasted to the usual ground-static test noise exhibits substantial reductions in both (1) the time unsteadiness of tone noise and (2) the mean level of tones calculated to be nonpropagating or cut-off. A model fan designed with cut-off of the fundamental tone was acoustically tested in the anechoic wind tunnel under both static and tunnel flow conditions. The properties that characterize flight-type noise were progressively simulated with increasing tunnel flow. The distinctly lobed directivity pattern of propagating rotor/stator interaction modes was also observed. The results imply that the excess noise attributed to the ingestion of the flow disturbances that prevail near most static test facilities was substantially reduced with tunnel flow. The anechoic wind tunnel appears to be a useful facility for applied research on aircraft engine fan noise under conditions of simulated flight.

Heidmann, M. F.↗

Experimental simulation of impact cratering on icy satellites

Cratering processes on icy satellites were simulated in a series of 102 laboratory impact experiments involving a wide range of target materials. For impacts into homogeneous clay slurries with impact energies ranging from five million to ten billion ergs, target yield strengths ranged from 100 to 38 Pa, and apparent viscosities ranged from 8 to 200 Pa s. Bowl-shaped craters, flat-floored craters, central peak craters with high or little relief, and craters with no relief were observed. Crater diameters increased steadily as energies were raised. A similar sequence was seen for experiment in which impact energy was held constant but target viscosity and strength progressively decreases. The experiments suggest that the physical properties of the target media relative to the gravitationally induced stresses determined the final crater morphology. Crater palimpsests could form by prompt collapse of large central peak craters formed in low target strength materials. Ages estimated from crater size-frequency distributions that include these large craters may give values that are too high.

Greeley, R.↗

Atomic oxygen effects on materials

Understanding of the basic processes of atomic oxygen interaction is currently at a very elementary level. However, measurement of erosion yields, surface morphology, and optical properties for low fluences have brought about much progress in the past decade. Understanding the mechanisms and those factors that are important for proper simulation of low Earth orbit is at a much lower level of understanding. The ability to use laboratory simulations with confidence to quantifiably address the functional performance and durability of materials in low Earth orbit will be necessary to assure long-term survivability to the natural space environment.

Banks, Bruce A.↗

Structural behavior of composites with progressive fracture

The objective of the study is to unify several computational tools developed for the prediction of progressive damage and fracture with efforts for the prediction of the overall response of damaged composite structures. In particular, a computational finite element model for the damaged structure is developed using a computer program as a byproduct of the analysis of progressive damage and fracture. Thus, a single computational investigation can predict progressive fracture and the resulting variation in structural properties of angleplied composites.

Minnetyan, L.↗

A review of solar wind ion and electron plasma distribution functions: Present understanding and Ulysses results

Our present understanding of the distribution functions of the solar wind ion and electron thermal/suprathermal populations will be reviewed covering selected theoretical and observational topics. Roughly half the review will be devoted to recent discoveries (since Solar Wind 7). Among recent results are those of the Ulysses mission. The SWICS experiment observed pick-up protons and alpha particles, and acceleration of these particles at interplanetary shocks. Positive ion phenomena observed by SWOOPS include enhanced proton-alpha particle differential streaming both: (1) at high latitudes; and (2) in the ecliptic beyond 1 AU in the vicinity of shocks. The SWOOPS positive ion observations also demonstrate relative constancy of the entropy per proton at high latitudes beyond about 2.5 AU. Double beaming in both protons and alphas is observed by SWOOPS on either side of the current sheet, but not within; a possible explanation is reconnection at the edge of the current sheet. SWOOPS observed bi-directional streaming of electrons beyond 2 AU not only within Coronal Mass Ejections, but also upstream of corotating interplanetary shocks. Latitudinal and radial gradients of Ulysses electron core and halo temperatures will be discussed, as will work in progress on the three dimensional (in velocity space) properties of ion distributions.

Goldstein, B. E.↗

Dependence of the Element Patterns of HYDROSTAR on Mutual Coupling

HYDROSTAR is a hybrid synthesis radiometer, intended for spaceborne applications, which employs a real aperture (waveguide stick antenna) for resolution along track and employs aperture synthesis to obtain resolution across track. This L-band system is an extension of the successful aircraft prototype, the Electronically Steered Thinned Array Radiometer (ESTAR). A proof-of-concept, full size system was constructed (45 wavelength in the synthesis direction) and subjected to extensive antenna pattern and associated microwave component measurements in an outdoor antenna test facility. HYDROSTAR employs a thinned array of 16 elements each 5.8 inches long in the along track dimension and spanning 9.5 inches across track. Each element is a narrow-wall shunt slot array with 36 slots. The polarization is linear (along-track). In the across track dimension, the antennas are deployed in a minimum redundancy array which has 90 independent baselines spaced in integer multiples of half a wavelength. The closest spacings used are for the first three elements at each end, which are spaced by only one-half wavelength. This study was intended to assess how closely each of 16 stick element patterns compare with their nominal values (as an individual, isolated radiator), when installed in their intended composite thinned array configuration. Extensive pattern measurements of the 16 elements that constitute the HYDROSTAR antenna subsystem were conducted to observe their relative features along the synthesis plane. Data was also collected for the mutual coupling between pairs of selected antennas. All antenna patterns had features different from that of an isolated element indicating some level of interaction among neighboring radiators. Those elements which had nearest neighbors at least five wavelengths away were located near the middle of the array. Their radiation patterns displayed sonic small, symmetric ripple across their full azimuth range. The patterns of elements that lie within 2.5 wavelengths of their neighbors showed stronger and asymmetric features. These are believed to be caused by mutual coupling among these structures. Evidence for this was seen when an antenna position was displaced by 0.05 wavelengths, Its pattern and those of its near neighbors were seen to change. Displacement within the plane of the array were observed to have different effects than displacements out-of-plane. A program of data analysis and theoretical development is in progress to provide a physical interpretation of the properties of these antenna patterns and to develop methods which can optimize the performance of this synthetic aperture imaging system. This includes compensation for pattern asymmetries and element position perturbation.

Weissman, David E.↗

Initial Results from the Bloomsburg University Goniometer Laboratory

The Bloomsburg University Goniometer Laboratory (B.U.G. Lab) consists of three systems for studying the photometric properties of samples. The primary system is an automated goniometer capable of measuring the entire bi-directional reflectance distribution function (BRDF) of samples. Secondary systems include a reflectance spectrometer and digital video camera with macro zoom lens for characterizing and documenting other physical properties of measured samples. Works completed or in progress include the characterization of the BRDF of calibration surfaces for the 2003 Mars Exploration Rovers (MER03), Martian analog soils including JSC-Mars-1, and tests of photometric models.

Shepard, M. K.↗

Smart Coating for Corrosion Indication and Prevention: Recent Progress

The authors are developing a smart coating system based on pH-triggered release microcapsules. These microcapsules can be incorporated into various coating systems for corrosion detection, protection and self-repair of mechanical coating damage. This paper will present the results from progress made to date in the controlled release properties of these microcapsules as well as in their corrosion indication and corrosion inhibition function.

Li, Wenyan↗

Towards Co-evolution of Membranes and Metabolism

Conceptually, the most robust way to explain how primitive cell-like structures acquired and increased their capabilities is on the basis of Darwinian evolution. A population of protocells containing material that produced more environmentally fit progeny would increase in time at the expense of other protocells. In this scenario, protocellular boundaries were inextricably connected to the metabolism they encapsulated: to be inheritable, early metabolism must have led to an increased rate of growth and division of vesicles and, similarly, transport through vesicle boundaries must have supported the evolution of metabolism. Everything that could not be delivered from the environment had to be produced and retained inside protocells. Despite their importance to the understanding of the origin of life, only a few cases of coupling between metabolism and membrane-related processes have been identified so far. For example, reactions inside fatty-acid vesicles have been linked to their competitive growth and division, and mechanisms by which membrane permeability might have coupled to information polymers have been proposed and explained. Most recently, it has been shown that a dipeptide inside fatty-acid vesicles catalyzes the formation of another dipeptide that binds to vesicle walls and, by doing so, promotes their growth at the expense of other vesicles, thus demonstrating evolutionary advantage of small, membrane-bound peptides. It has been shown that the appearance of phospholipids imparted selective advantage to protocells bound by phospholipid-containing membranes, eventually driving fatty-acid vesicles to extinction. Phospholipid membranes, however, are nearly impermeable to charged species. Yet, the ability to transport ions across membranes was vital for regulating cellular volume, pH homeostasis, generating energy and sensing the environment. To account for this, evolutionary scenarios for the emergence of simple ion channels, protein structures surrounding water-filled pores in the membrane that facilitate ion transport, have been developed. We will review recent progress in experimental and theoretical studies on coupling properties of membranes to metabolism, with the focus on how they impose constraints on scenarios for the origin of life, and discuss how these studies form the basis for future work on this topic.

metabolism↗

Correlated Spatio-temporal Evolution of Extreme-Ultraviolet Ribbons and Hard X-Rays in a Solar Flare

We analyze the structure and evolution of ribbons from the M7.3 SOL2014-04-18T13 flare using ultraviolet images from the Interface Region Imaging Spectrograph and the Solar Dynamics Observatory (SDO)/Atmospheric Imaging Assembly (AIA), magnetic data from the SDO/Helioseismic and Magnetic Imager, hard X-ray (HXR) images from the Reuven Ramaty High Energy Solar Spectroscopic Imager, and light curves from the Fermi/Gamma-ray Burst Monitor, in order to infer properties of coronal magnetic reconnection. As the event progresses, two flare ribbons spread away from the magnetic polarity inversion line. The width of the newly brightened front along the extension of the ribbon is highly intermittent in both space and time, presumably reflecting nonuniformities in the structure and/or dynamics of the flare current sheet. Furthermore, the ribbon width grows most rapidly in regions exhibiting concentrated nonthermal HXR emission, with sharp increases slightly preceding the HXR bursts. The light curve of the ultraviolet emission matches the HXR light curve at photon energies above 25 keV. In other regions the ribbon-width evolution and light curves do not temporally correlate with the HXR emission. This indicates that the production of nonthermal electrons is highly nonuniform within the flare current sheet. Our results suggest a strong connection between the production of nonthermal electrons and the locally enhanced perpendicular extent of flare ribbon fronts, which in turn reflects the inhomogeneous structure and/or reconnection dynamics of the current sheet. Despite this variability, the ribbon fronts remain nearly continuous, quasi-one-dimensional features. Thus, although the reconnecting coronal current sheets are highly structured, they remain quasi-two-dimensional and the magnetic energy release occurs systematically, rather than stochastically, through the volume of the reconnecting magnetic flux.

S. J. Naus↗

Sharp Transition from Nonmetallic Au 246 to Metallic Au 279 with Nascent Surface Plasmon Resonance

Here, the optical properties of metal nanoparticles have attracted wide interest. Recent progress in controlling nanoparticles with atomic precision (often called nanoclusters) provide new opportunities for investigating many fundamental questions, such as the transition from excitonic to plasmonic state, which is a central question in metal nanoparticle research because it provides insights into the origin of surface plasmon resonance (SPR) as well as the formation of metallic bond. However, this question still remains elusive because of the extreme difficulty in preparing atomically precise nanoparticles larger than 2 nm. Here we report the synthesis and optical properties of an atomically precise Au 279 (SR) 84 nanocluster. Femtosecond transient absorption spectroscopic analysis reveals that the Au 279 nanocluster shows a laser power dependence in its excited state lifetime, indicating metallic state of the particle, in contrast with the nonmetallic electronic structure of the Au 246 (SR) 80 nanocluster. Steady-state absorption spectra reveal that the nascent plasmon band of Au 279 at 506 nm shows no peak shift even down to 60 K, consistent with plasmon behavior. The sharp transition from nonmetallic Au 246 to metallic Au 279 is surprising and will stimulate future theoretical work on the transition and many other relevant issues.

36 MATERIALS SCIENCE↗

Influence of Rare Earth Ce Additions on Microstructure and Mechanical Properties of Experimental Pipeline Steels

Herein, the effect of Ce additions ranging from 57 to 263 ppm is evaluated for an experimental pipeline steel. Compared to the Ce-free steel, progressive Ce additions result in a slightly refined microstructure, significantly improve transverse impact properties, and slightly increase strength. All these observations can be attributed to the gradual transformation of Mn sulfide and Mn–Si–Al oxide inclusions to Ce-containing oxide/sulfides. In particular, the inclusions consist exclusively of sub-5 μm spherical Ce 2 O 2 S particles upon near-stoichiometric additions of Ce, considering the oxygen and sulfur impurity level of the steel. In conclusion, the results suggest that Ce is a potentially promising alloying addition for next-generation pipeline steels by replacing overtly deleterious inclusions with potentially beneficial ones.

36 MATERIALS SCIENCE↗