Intrinsic (Trap-Free) Transistors Based on Epitaxial Single-Crystal Perovskites.

The first experimental realization of the intrinsic (not dominated by defects) charge conduction regime in lead-halide perovskite field-effect transistors (FETs) is reported. The advance is enabled by: i) a new vapor-phase epitaxy technique that results in large-area single-crystalline cesium lead bromide (CsPbBr3 ) films with excellent structural and surface properties, including atomically flat surface morphology, essentially free from defects and traps at the level relevant to device operation; ii) an extensive materials analysis of these films using a variety of thin-film and surface probes certifying the chemical and structural quality of the material; and iii) the fabrication of nearly ideal (trap-free) FETs with characteristics superior to any reported to date. These devices allow the investigation of the intrinsic FET and (gated) Hall-effect carrier mobilities as functions of temperature. The intrinsic mobility is found to increase on cooling from ≈30 cm2 V-1 s-1 at room temperature to ≈250 cm2 V-1 s-1 at 50 K, revealing a band transport limited by phonon scattering. Establishing the intrinsic (phonon-limited) mobility provides a solid test for theoretical descriptions of carrier transport in perovskites, reveals basic limits to the technology, and points to a path for future high-performance perovskite electronic devices.

An intra-cytoplasmic route for SARS-CoV-2 transmission unveiled by Helium-ion microscopy.

SARS-CoV-2 virions enter the host cells by docking their spike glycoproteins to the membrane-bound Angiotensin Converting Enzyme 2. After intracellular assembly, the newly formed virions are released from the infected cells to propagate the infection, using the extra-cytoplasmic ACE2 docking mechanism. However, the molecular events underpinning SARS-CoV-2 transmission between host cells are not fully understood. Here, we report the findings of a scanning Helium-ion microscopy study performed on Vero E6 cells infected with mNeonGreen-expressing SARS-CoV-2. Our data reveal, with unprecedented resolution, the presence of: (1) long tunneling nanotubes that connect two or more host cells over submillimeter distances; (2) large scale multiple cell fusion events (syncytia); and (3) abundant extracellular vesicles of various sizes. Taken together, these ultrastructural features describe a novel intra-cytoplasmic connection among SARS-CoV-2 infected cells that may act as an alternative route of viral transmission, disengaged from the well-known extra-cytoplasmic ACE2 docking mechanism. Such route may explain the elusiveness of SARS-CoV-2 to survive from the immune surveillance of the infected host.

Stimulus-responsive self-assembly of protein-based fractals by computational design.

Fractal topologies, which are statistically self-similar over multiple length scales, are pervasive in nature. The recurrence of patterns in fractal-shaped branched objects, such as trees, lungs and sponges, results in a high surface area to volume ratio, which provides key functional advantages including molecular trapping and exchange. Mimicking these topologies in designed protein-based assemblies could provide access to functional biomaterials. Here we describe a computational design approach for the reversible self-assembly of proteins into tunable supramolecular fractal-like topologies in response to phosphorylation. Guided by atomic-resolution models, we develop fusions of Src homology 2 (SH2) domain or a phosphorylatable SH2-binding peptide, respectively, to two symmetric, homo-oligomeric proteins. Mixing the two designed components resulted in a variety of dendritic, hyperbranched and sponge-like topologies that are phosphorylation-dependent and self-similar over three decades (~10 nm-10 µm) of length scale, in agreement with models from multiscale computational simulations. Designed assemblies perform efficient phosphorylation-dependent capture and release of cargo proteins.

Contactless Electrical and Structural Characterization of Semiconductor Nanowires with Axially Modulated Doping Profiles.

Efficient characterization of semiconductor nanowires having complex dopant profiles or heterostructures is critical to fully understand these materials and the devices built from them. Existing electrical characterization techniques are slow and laborious, particularly for multisegment nanowires, and impede the statistical understanding of highly variable samples. Here, it is shown that electro-orientation spectroscopy (EOS)-a high-throughput, noncontact method for statistically characterizing the electrical properties of entire nanowire ensembles-can determine the conductivity and dimensions of two distinct segments in individual Si nanowires with axially encoded dopant profiles. This analysis combines experimental measurements and computational simulations to determine the electrical conductivity of the nominally undoped segment of two-segment Si nanowires, as well as the ratio of the segment lengths. The efficacy of this approach is demonstrated by comparing results generated by EOS with conventional four-point-probe measurements. This work provides new insights into the control and variability of semiconductor nanowires for electronic applications and is a critical first step toward the high-throughput interrogation of complete nanowire-based devices.

Excitation of long-wavelength surface optical vibrational modes in films, cubes and film/cube composite system using an atom-sized electron beam.

Using spatially resolved Electron Energy-Loss Spectroscopy, we investigate the excitation of long-wavelength surface optical vibrational modes in elementary types of nanostructures: an amorphous SiO2 slab, an MgO cube, and in the composite cube/slab system. We find rich sets of optical vibrational modes strongly constrained by the nanoscale size and geometry. For slabs, we find two surface resonances resulting from the excitation of surface phonon polariton modes. For cubes, we obtain three main highly localized corner, edge, and face resonances. The response of those surface phonon resonances can be described in terms of eigenmodes of the cube and we show that the corresponding mode pattern is recovered in the spatially resolved EELS maps. For the composite cube/substrate system we find that interactions between the two basic structures are weak, producing minor spectral shifts and intensity variations (transparency behaviour), particularly for the MgO-derived modes.

Biological control of aragonite formation in stony corals.

Little is known about how stony corals build their calcareous skeletons. There are two prevailing hypotheses: that it is a physicochemically dominated process and that it is a biologically mediated one. Using a combination of ultrahigh-resolution three-dimensional imaging and two-dimensional solid-state nuclear magnetic resonance (NMR) spectroscopy, we show that mineral deposition is biologically driven. Randomly arranged, amorphous nanoparticles are initially deposited in microenvironments enriched in organic material; they then aggregate and form ordered aragonitic structures through crystal growth by particle attachment. Our NMR results are consistent with heterogeneous nucleation of the solid mineral phase driven by coral acid-rich proteins. Such a mechanism suggests that stony corals may be able to sustain calcification even under lower pH conditions that do not favor the inorganic precipitation of aragonite.

Mitochondria Protection after Acute Ischemia Prevents Prolonged Upregulation of IL-1ß and IL-18 and Arrests CKD.

The innate immune system has been implicated in both AKI and CKD. Damaged mitochondria release danger molecules, such as reactive oxygen species, DNA, and cardiolipin, which can cause NLRP3 inflammasome activation and upregulation of IL-18 and IL-1ß It is not known if mitochondrial damage persists long after ischemia to sustain chronic inflammasome activation. We conducted a 9-month study in Sprague-Dawley rats after 45 minutes of bilateral renal ischemia. We detected glomerular and peritubular capillary rarefaction, macrophage infiltration, and fibrosis at 1 month. Transmission electron microscopy revealed mitochondrial degeneration, mitophagy, and deformed foot processes in podocytes. These changes progressed over the study period, with a persistent increase in renal cortical expression of IL-18, IL-1ß, and TGF-ß, despite a gradual decline in TNF-α expression and macrophage infiltration. Treatment with a mitoprotective agent (SS-31; elamipretide) for 6 weeks, starting 1 month after ischemia, preserved mitochondrial integrity, ameliorated expression levels of all inflammatory markers, restored glomerular capillaries and podocyte structure, and arrested glomerulosclerosis and interstitial fibrosis. Further, helium ion microscopy vividly demonstrated the restoration of podocyte structure by SS-31. The protection by SS-31 was sustained for ≥6 months after treatment ended, with normalization of IL-18 and IL-1ß expression. These results support a role for mitochondrial damage in inflammasome activation and CKD and suggest mitochondrial protection as a novel therapeutic approach that can arrest the progression of CKD. Notably, SS-31 is effective when given long after AKI and provides persistent protection after termination of drug treatment.

High-throughput electrical measurement and microfluidic sorting of semiconductor nanowires.

Existing nanowire electrical characterization tools not only are expensive and require sophisticated facilities, but are far too slow to enable statistical characterization of highly variable samples. They are also generally not compatible with further sorting and processing of nanowires. Here, we demonstrate a high-throughput, solution-based electro-orientation-spectroscopy (EOS) method, which is capable of automated electrical characterization of individual nanowires by direct optical visualization of their alignment behavior under spatially uniform electric fields of different frequencies. We demonstrate that EOS can quantitatively characterize the electrical conductivities of nanowires over a 6-order-of-magnitude range (10(-5) to 10 S m(-1), corresponding to typical carrier densities of 10(10)-10(16) cm(-3)), with different fluids used to suspend the nanowires. By implementing EOS in a simple microfluidic device, continuous electrical characterization is achieved, and the sorting of nanowires is demonstrated as a proof-of-concept. With measurement speeds two orders of magnitude faster than direct-contact methods, the automated EOS instrument enables for the first time the statistical characterization of highly variable 1D nanomaterials.

Contactless Determination of Electrical Conductivity of One-Dimensional Nanomaterials by Solution-Based Electro-orientation Spectroscopy.

Nanowires of the same composition, and even fabricated within the same batch, often exhibit electrical conductivities that can vary by orders of magnitude. Unfortunately, existing electrical characterization methods are time-consuming, making the statistical survey of highly variable samples essentially impractical. Here, we demonstrate a contactless, solution-based method to efficiently measure the electrical conductivity of 1D nanomaterials based on their transient alignment behavior in ac electric fields of different frequencies. Comparison with direct transport measurements by probe-based scanning tunneling microscopy shows that electro-orientation spectroscopy can quantitatively measure nanowire conductivity over a 5-order-of-magnitude range, 10(-5)-1 Ω(-1) m(-1) (corresponding to resistivities in the range 10(2)-10(7) Ω·cm). With this method, we statistically characterize the conductivity of a variety of nanowires and find significant variability in silicon nanowires grown by metal-assisted chemical etching from the same wafer. We also find that the active carrier concentration of n-type silicon nanowires is greatly reduced by surface traps and that surface passivation increases the effective conductivity by an order of magnitude. This simple method makes electrical characterization of insulating and semiconducting 1D nanomaterials far more efficient and accessible to more researchers than current approaches. Electro-orientation spectroscopy also has the potential to be integrated with other solution-based methods for the high-throughput sorting and manipulation of 1D nanomaterials for postgrowth device assembly.

Oxygen incorporation in rubrene single crystals.

Single crystal rubrene is a model organic electronic material showing high carrier mobility and long exciton lifetime. These properties are detrimentally affected when rubrene is exposed to intense light under ambient conditions for prolonged periods of time, possibly due to oxygen up-take. Using photoelectron, scanning probe and ion-based methods, combined with an isotopic oxygen exposure, we present direct evidence of the light-induced reaction of molecular oxygen with single crystal rubrene. Without a significant exposure to light, there is no reaction of oxygen with rubrene for periods of greater than a year; the crystal's surface (and bulk) morphology and chemical composition remain essentially oxygen-free. Grand canonical Monte Carlo computations show no sorbtion of gases into the bulk of rubrene crystal. A mechanism for photo-induced oxygen inclusion is proposed.

Chemical properties of oxidized silicon carbide surfaces upon etching in hydrofluoric acid.

Hydrogen termination of oxidized silicon in hydrofluoric acid results from an etching process that is now well understood and accepted. This surface has become a standard for studies of surface science and an important component in silicon device processing for microelectronics, energy, and sensor applications. The present work shows that HF etching of oxidized silicon carbide (SiC) leads to a very different surface termination, whether the surface is carbon or silicon terminated. Specifically, the silicon carbide surfaces are hydrophilic with hydroxyl termination, resulting from the inability of HF to remove the last oxygen layer at the oxide/SiC interface. The final surface chemistry and stability critically depend on the crystal face and surface stoichiometry. These surface properties affect the ability to chemically functionalize the surface and therefore impact how SiC can be used for biomedical applications.

Confocal Raman microscopy across the metal-insulator transition of single vanadium dioxide nanoparticles.

We present the first Raman scattering measurements on nanoparticulate vanadium dioxide (VO(2)), as well as the first observations of the temperature-induced phase transition in individual VO(2) nanoparticles (NPs). We compare the Raman response of two VO(2) NPs and a companion VO(2) film undergoing their monoclinic-tetragonal-monoclinic transformations and offer qualitative explanations for the large observed differences in hysteresis width. While bulk crystals and contiguous films contain numerous nucleation sites, individual NPs likely harbor only a few, which may make it possible to correlate detectable defects (e.g., grain boundaries and dislocations) with the "ease" of switching phases, as quantified by the width of the thermal hysteresis.

Experimental characterization of a metal-oxide-semiconductor field-effect transistor-based Coulter counter.

We report the detailed characterization of an ultrasensitive microfluidic device used to detect the translocation of small particles through a sensing microchannel. The device connects a fluidic circuit to the gate of a metal-oxide-semiconductor field-effect transistor (MOSFET) and detects particles by monitoring the MOSFET drain current modulation instead of the modulation in the ionic current through the sensing channel. The minimum volume ratio of the particle to the sensing channel detected is 0.006%, which is about ten times smaller than the lowest detected volume ratio previously reported in the literature. This volume ratio is detected at a noise level of about 0.6% of the baseline MOSFET drain current, clearly showing the amplification effects from the fluidic circuits and the MOSFETs. We characterize the device sensitivity as a function of the MOSFET gate potential and show that its sensitivity is higher when the MOSFET is operating below its threshold gate voltage than when it is operating above the threshold voltage. In addition, we demonstrate that the device sensitivity linearly increases with the applied electrical bias across the fluidic circuit. Finally, we show that polystyrene beads and glass beads with similar sizes can be distinguished from each other based on their different translocation times, and the size distribution of microbeads can be obtained with accuracy comparable to that of direct scanning electron microscopy measurements.

Synthesis, Surface Studies, Composition and Structural Characterization of CdSe, Core/Shell, and Biologically Active Nanocrystals.

Nanostructures, with their very large surface to volume ratio and their non-planar geometry, present an important challenge to surface scientists. New issues arise as to surface characterization, quantification and interface formation. This review summarizes the current state of the art in the synthesis, composition, surface and interface control of CdSe nanocrystal systems, one of the most studied and useful nanostructures.

Homogeneously alloyed CdSxSe1-x nanocrystals: synthesis, characterization, and composition/size-dependent band gap.

Alloy nanocrystals provide an additional degree of freedom in selecting desirable properties for nanoscale engineering because their physical and optical properties depend on both size and composition. We report the pyrolytic synthesis of homogeneously alloyed CdS(x)Se(1-x) nanocrystals in all proportions. The nanocrystals are characterized using UV-visible absorption spectroscopy, transmission electron microscopy, X-ray diffractrometry, and Rutherford backscattering spectrometry to determine precisely structure, size, and composition. The dependence of band gap on nanocrystal size and composition is elucidated, yielding a bowing constant of 0.29, in agreement with bulk values. In addition, the morphology of the resultant nanocrystals can be altered by changing the reaction conditions, generating structures ranging from homogeneous, spherical nanocrystals to one-dimensional gradient nanorods.

Photoinduced phase transition in VO2 nanocrystals: ultrafast control of surface-plasmon resonance.

We study the ultrafast insulator-to-metal transition in nanoparticles of VO2, obtained by ion implantation and self-assembly in silica. The nonmagnetic, strongly correlated compound VO2 undergoes a reversible phase transition, which can be photoinduced on an ultrafast time scale. In the nanoparticles, prompt formation of the metallic state results in the appearance of surface-plasmon resonance. We achieve large, ultrafast enhancement of optical absorption in the near-infrared spectral region that encompasses the wavelength range for optical-fiber communications. One can further tailor the response of the nanoparticles by controlling their shape.

Dynamic scaling, island size distribution, and morphology in the aggregation regime of submonolayer pentacene films.

Scaling behavior of the island size distribution through a universal scaling function f(u) is demonstrated for submonolayer pentacene islands in the aggregation regime (0.1