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Characterizing and manipulating the circular polarization of light is central to numerous emerging technologies, including spintronics and quantum computing. Separately, monolayer tungsten disulfide (WS2) is a versatile material that has demonstrated promise in a variety of applications, including single photon emitters and valleytronics. Here, we demonstrate a method to tune the photoluminescence (PL) intensity (factor of x161), peak position (38.4meV range), circular polarization (39.4% range), and valley polarization of a Bi2Se3-WS2 2D heterostructure using a low-power laser (0.762uW) in ambient. Changes are spatially confined to the laser spot, enabling submicron (814nm) features, and are long-term stable (>334 days). PL and valley polarization changes can be controllably reversed through laser exposure in vacuum, allowing the material to be erased and reused. Atmospheric experiments and first-principles calculations indicate oxygen diffusion modulates the exciton radiative vs. non-radiative recombination pathways, where oxygen absorption leads to brightening, and desorption to darkening., Published: ACS Appl. Mater. Interfaces 2022

Nanocrystals of doped semiconductors, such as Cu_(2-x)S, hold much promise for near infrared active devices because, unlike in noble metals, their tunable infrared plasmon can exist in nanocrystals with diameters

Nanocrystallization has been an important approach for reducing thermal conductivity in thermoelectric materials due to limits on phonon mean-free path imposed by the characteristic structural size. We report on thermal conductivity as low as 0.3 Wm−1K−1 of nanocrystalline silicon thin films prepared by plasma-enhanced chemical-vapor deposition as grain size is reduced to 2.8 nm by controlling hydrogen dilution of silane gas during growth. A multilayered film composed by alternating growth conditions, with layer thicknesses of 3.6 nm, is measured to have a thermal conductivity 30% and 15% lower than its two constituents. Our quantitative analysis attributes the strong reduction of thermal conductivity with decreasing grain size to the magnifying effect of porosity which occurs concomitantly due to increased mass density fluctuations. Our results demonstrate that ultrasmall grain sizes, multilayering, and porosity, all at a similar nanometer-size scale, may be a promising way to engineer thermoelectric materials. Thermoelectric materials convert heat into electricity and their performance is determined by their figure of merit ZT, which is generally too small in many materials for practical applications. Here, the authors demonstrate that a reduction in grain size for nanocrystalline Si can reduce thermal conductivity and potentially be used as a method to engineer greater ZT in Si for thermoelectric applications.

Batteries that offer high specific energy and energy density coupled with improved safety and lower cost will affect applications ranging from electric vehicles, portable electronic devices, and grid-level energy storage. Alkaline nickel–zinc (Ni–Zn) batteries use nonflammable aqueous electrolyte and nonstrategic, low-cost electrode materials; however with a two-electron anode, a cathode that stores more than one electron per Ni atom would increase energy density. Herein, we report the effect of substituting metal ions (aluminium, cobalt, manganese, or zinc) into α-Ni(OH)2, a phase that can accommodate more than one-electron charge storage, but which typically converts to lower-capacity β-Ni(OH)2 upon cycling in alkaline electrolytes. We adapt a microwave-assisted process that expresses α-Ni(OH)2 as a high surface-area nanosheet morphology and find that we retain this morphology with all metal-ion substituents. The series is characterized using scanning electron microscopy, transmission electron microscopy, X-ray diffraction, and Raman spectroscopy. Metal-ion substitution influences aggregate growth, interlayer distance, and vibrational frequencies. We test powder-composite cathodes prepared using the substituted α-Ni(OH)2 series versus zinc sponge anodes in alkaline electrolyte under device-relevant mass loadings and using an intentionally aggressive charging protocol to determine onset voltage for oxygen evolution. The electrochemical charge-storage behaviour is established using galvanostatic cycling and differential capacity analysis. The substituents significantly influence both Ni-centred redox and oxygen-evolution voltages (vs. Zn/Zn2+). The incorporation of Al3+ within α-Ni(OH)2 nanosheets provides higher capacity and phase stability compared to the divalent substituents and unsubstituted α-Ni(OH)2. The presence of ordered free nitrates in the interlayer of Al3+-substituted α-Ni(OH)2, not seen with Co2+ or Mn2+ substituents, correlates with the improved electrochemical performance.

We determine the activity of catalytic carbon monoxide (CO) oxidation as a function of the size of gold nanoparticles (Au NP), their weight loading, and their interfacial intimacy with similarly si...

We built a collector to filter interplanetary dust particles (IDPs) larger than 5 μm from the clean air at the Amundsen Scott South Pole station. Our sampling strategy used long duration, continuous dry filtering of near‐surface air in place of short duration, high‐speed impact collection on flags flown in the stratosphere. We filtered ~10\(^7\) m\(^3\) of clean Antarctic air through 20 cm diameter, 3 µm filters coupled to a suction blower of modest power consumption (5–6 kW). Our collector ran continuously for 2 years and yielded 41 filters for analyses. Based on stratospheric concentrations, we predicted that each month’s collection would provide 300–900 IDPs for analysis. We identified 19 extraterrestrial (ET) particles on the 66 cm\(^2\) of filter examined, which represented ~0.5% of the exposed filter surfaces. The 11 ET particles larger than 5 µm yield about a fifth of the expected flux based on >5 µm stratospheric ET particle flux. Of the 19 ET particles identified, four were chondritic porous IDPs, seven were FeNiS beads, two were FeNi grains, and six were chondritic material with FeNiS components. Most were

We demonstrate that unstained DNA nanostructures can be chemically mapped by using aberration-corrected scanning transmission electron microscopy (STEM) with energy-dispersive spectroscopy (EDS). Key to this measurement is the use of graphene supports whose reduced background scattering compared to thicker carbon supports allows EDS to image phosphorus and other elements in the DNA (or in attachments to the DNA) as well as to see the divalent cations used to stabilize the nanostructure. In addition, unlike in other EDS analyses, the chemical maps we obtain can be made quantitative in an absolute sense because each individual DNA nanostructure is in effect a very large macromolecule (∼4.7 MDa) with a known chemical composition. In this way, not only can STEM/EDS serve DNA nanotechnology as a characterization tool but also the DNA structures can function as molecular standards for improving mesoscale EDS techniques.

Here we report the relative degrees of thermal metamorphism for five Antarctic Ornans-like carbonaceous (CO) chondrites, including Dominion Range (DOM) 08006, as determined from the Cr-content of their FeO-rich (ferroan) olivine. These five CO3 chondrites complete the previously poorly-defined CO3.00 to 3.2 chondrite metamorphic trend. DOM 08006 appears to be a highly primitive CO chondrite of petrologic type 3.00. We report the detailed mineralogy and petrography of DOM 08006 using a coordinated, multi-technique approach. The interchondrule matrix in DOM 08006 consists of unequilibrated mixtures of silicate, metal, and sulfide minerals and lacks Fe-rich rims on silicates indicating that DOM 08006 has only experienced minimal, if any, thermal metamorphism. This is also reflected by the Co/Ni ratios of Ni-rich and Ni-poor metal, a sensitive indicator of thermal metamorphism, and the presence of euhedral chrome-spinel grains, which typically become subhedral to anhedral during progressive metamorphism. DOM 08006 matrix shows minor evidence for aqueous alteration and while the presence of magnetite surrounding metal in chondrules indicates that there has been some interaction with fluid, much metal remains and none of the sulfides analyzed show evidence of being formed by aqueous alteration. Furthermore, the plagioclase of ∼50% of chondrules analyzed show resolvable excess silica indicating that these chondrules have experienced minimal, if any, reprocessing in the CO parent body. Noble gas data for DOM 08006 show that it contains the highest concentrations of trapped 36Ar and 132Xe of all CO chondrites analyzed to date, further indicating that DOM 08006 is the most primitive CO chondrite known. The cosmic ray exposure age of DOM 08006 is estimated to be ∼19 Ma. The minimally altered nature of DOM 08006 demonstrates that it is an extremely important sample for providing valuable insight into early Solar System conditions. At a total weight of 667 g, a significant amount of material is available for a wide array of future studies.

Samples from asteroid 25143 Itokawa returned by the Hayabusa mission have been identified as LL4-6 ordinary chondrite materials and have shown it to be a rubble pile that aggregated after break-up of a parent body. Here we investigate particle RB-CV-0038 from the Itokawa regolith using scanning and transmission electron microscopy and energy dispersive spectroscopy. We identify a cubanite-chalcopyrite-troilite-pyrrhotite assemblage, the phases and structure of which are indicative of low-temperature, aqueous alteration. Cubanite is stable only at temperatures below around 250 °C and has thus far only been identified in CI carbonaceous chondrites and the comet 81P/Wild2 sample suite. Chalcopyrite is also very rare in the meteorite record and is found mostly in R chondrites and some CK chondrites. Because the Itokawa parent body experienced significant thermal alteration with little evidence of low-temperature equilibration or aqueous alteration, we propose that the assemblage we identify is most likely exogenous and represents a component of an impacting body. Cubanite and chalcopyrite identified in regolith grains returned from the Itokawa asteroid by the Hayabusa mission likely represent part of an exogenous mineral assemblage with a carbonaceous chondrite or cometary origin

We report thermoelectric measurements over a temperature range of 80 K to 300 K of heavily boron-doped nanocrystalline silicon films prepared by hot-wire and plasma-enhanced chemical-vapor depositions. The nanocrystalline silicon films were doped by either gaseous deposition precursors or post-deposition ion implantation, resulting in boron concentrations ranging from 1–2×1020 cm−3 to 3 × 1021 cm−3. Reasonable values of the Seebeck coefficient and electrical conductivity were obtained at 300 K, comparable to many other research work. We also report thermal conductivity measurements on these films before doping, which we use to estimate their prospective thermoelectric efficiency. These measurements show values as low as 0.76 W/mK at 300 K which depend highly upon the grain sizes of the nc-Si films. We find that post-deposition doping by ion-implantation is more effective at enhancing the power factor than gaseous doping, and the power factor is only weakly dependent upon doping concentration for the films doped by ion implantation. We conclude that improvements of the thermoelectric efficiency of nc-Si films may depend more on a reduction of their thermal conductivity than doping optimization. The small grain sizes and the low thermal conductivity of the undoped nc-Si films accomplished in this work are therefore encouraging developments.

Meteorites originating from primitive C-type asteroids are composed of materials from the Sun’s protoplanetary disk, including up to a few per cent organic carbon. In contrast, some interplanetary dust particles and micrometeorites have much higher carbon contents, up to >90%, and are thought to originate from icy outer Solar System bodies and comets. Here we report an approximately 100-µm-diameter very carbon-rich clast, with highly primitive characteristics, in the matrix of a CR2 chondrite, LaPaz Icefield 02342. The clast may represent a cometary building block, largely unsampled in meteorite collections, that was captured by a C-type asteroid during the early stages of planet formation. The existence of this cometary microxenolith supports the idea of a radially inward transport of materials from the outer protoplanetary disk into the CR chondrite reservoir during the formation of planetesimals. Moreover, the H-isotopic composition of the clast is suggestive of a temporal evolution of organic isotopic compositions in the comet-forming region of the disk. The composition and characteristics of a C-rich clast within the LaPaz Icefield 02342 meteorite suggests that the clast is composed of materials related to comets and icy bodies. The clast probably formed in the outer Solar System, was transported inward and finally accreted into LaPaz’s parent body.

Geobacter sulfurreducens is of interest for the highest efficiency of power generation and extremely long extracellular electron transfer (EET) between the bacterium and electrodes. Despite more than 15 years of intensive molecular biological research, there is still no clear answer which molecules are responsible for these processes. In the present work, we look at the problem from another (atomic) perspective and identify the location and shape of the compounds that are known to be conductive, particularly those containing Fe atoms. By using highly sophisticated energy dispersive X-ray spectroscopy combined with high-angle annular dark-field transmission electron microscopy enabling detection, identification, and localization of chemical compounds on the surface at nearly atomic spatial resolution, we analyze Fe spatial distribution within the G. sulfurreducens community. We discover the presence of small Fe-containing particles on the surface of the bacterium cells. The size of the particles (diameter 5.6 nm) is highly reproducible and comparable with the size of a single protein. The particles cover about 2% of the cell surface, which is similar to that expected for molecular conductors responsible for electron transfer through the bacterium cell wall. We find that G. sulfurreducens filaments ("bacterial molecular wires") also contain Fe atoms in their bundles. We observe that the bacterium enable changing the distance between the Fe-containing bundles in the filaments from separated to attached (the latter is needed for the efficient electron transfer between the Fe-containing particles), depending on the bacterium metabolic activity and attachment to extracellular substrates. These results are consistent with the recently published research about the role of Fe atoms in protein molecular conductance ( Phys. Chem. Chem. Phys. , 2018 , 20 , 14072 - 14081 ) and show what type of Fe-containing particles are involved in the bacterial extracellular communication. They can be used for the design and construction of artificial biomolecular wires and bioinorganic interfaces.

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An ultrafast laser (λ=1030 nm, ~160 fs) was used to synthesize nanodiamonds directly from ethanol liquid (sans target) through the process of laser filamentation. The laser parameters (such as energy, repetition rate, irradiation time) for nanodiamond synthesis were optimized and characterized with their UV-VIS absorbance, optical emission spectra, Raman, and TEM (transmission electron microscopy) analysis. TEM analysis showed the synthesized nanodiamonds were 2-5 nm size with little or no aggregation and had visible lattice fringes of 2.07 A corresponding to diamond (111). Methods of doping the nanodiamonds with nitrogen or other species during laser synthesis will also be presented.