The work unravels the previously unexplored atomic-scale mechanism involving the interaction of phonons with crystal homointerfaces. Silicon nanowires with engineered isotopic content and crystal phases were chosen for this investigation. Crystal polytypism, manifested by the presence of both diamond cubic and rhombohedral phases within the same nanowire, provided a testbed to study the impact of phase homointerfaces on phonon transport.
View Article and Find Full Text PDFThe hyperbolic dispersion relation of phonon-polaritons (PhPols) in anisotropic van der Waals materials provides high-momentum states, directional propagation, subdiffractional confinement, large optical density of states, and enhanced light-matter interactions. In this work, we use Raman spectroscopy in the convenient backscattering configuration to probe PhPol in GaSe, a 2D material presenting two hyperbolic regions separated by a double reststrahlen band. By varying the incidence angle, dispersion relations are revealed for samples with thicknesses between 200 and 750 nm.
View Article and Find Full Text PDFBlack phosphorus (BP) is unique among layered materials because of its homonuclear lattice and strong structural anisotropy. While recent investigations on few-layer BP have extensively explored the in-plane (, ) anisotropy, much less attention has been given to the out-of-plane direction (). Here, the optical response from bulk BP is probed using polarization-resolved photoluminescence (PL), photoluminescence excitation (PLE), and resonant Raman scattering along the zigzag, out-of-plane, and armchair directions.
View Article and Find Full Text PDFMotional narrowing is a phenomenon by which a quantum state can be entangled with a noisy environment and still retain its intrinsic coherence. Using two optically induced motional forces driving the environmental electrical field amplitude and fluctuations, we present a compelling illustration of the effects of motional narrowing on the energy, line shape, and line width of a single quantum emitter, a Te molecule embedded in ZnSe, subject to spectral diffusion. Motional narrowing is achieved in several regimes, irrespectively of the inhomogeneous disorder initially present and the charge reservoir state sourcing the field.
View Article and Find Full Text PDFNearshore (littoral) habitats of clear lakes with high water quality are increasingly experiencing unexplained proliferations of filamentous algae that grow on submerged surfaces. These filamentous algal blooms (FABs) are sometimes associated with nutrient pollution in groundwater, but complex changes in climate, nutrient transport, lake hydrodynamics, and food web structure may also facilitate this emerging threat to clear lakes. A coordinated effort among members of the public, managers, and scientists is needed to document the occurrence of FABs, to standardize methods for measuring their severity, to adapt existing data collection networks to include nearshore habitats, and to mitigate and reverse this profound structural change in lake ecosystems.
View Article and Find Full Text PDFIn aquatic detrital-based food webs, research suggests that autotroph-heterotroph microbial interactions exert bottom-up controls on energy and nutrient transfer. To address this emerging topic, we investigated microbial responses to nutrient and light treatments during Liriodendron tulipifera litter decomposition and fed litter to the caddisfly larvae Pycnopsyche sp. We measured litter-associated algal, fungal, and bacterial biomass and production.
View Article and Find Full Text PDFWe demonstrate a mid-infrared light-emitting diode based on the 2D semiconductor black phosphorus (BP). The device is composed of a mechanically exfoliated BP/molybdenum disulfide heterojunction. Under forward bias, it emits polarized electroluminescence at λ = 3.
View Article and Find Full Text PDF1. Well-documented in terrestrial settings, priming effects describe stimulated heterotrophic microbial activity and decomposition of recalcitrant carbon by additions of labile carbon. In aquatic settings, algae produce labile exudates which may elicit priming during organic matter decomposition, yet the directions and mechanisms of aquatic priming effects remain poorly tested.
View Article and Find Full Text PDFSecond-order Raman scattering has been extensively studied in carbon-based nanomaterials, for example, nanotube and graphene, because it activates normally forbidden Raman modes that are sensitive to crystal disorder, such as defects, dopants, strain, and so forth. The sp-hybridized carbon systems are, however, the exception among nanomaterials, where first-order Raman processes usually dominate. Here we report the identification of four second-order Raman modes, named D, D, D and D, in exfoliated black phosphorus (P(black)), an elemental direct-gap semiconductor exhibiting strong mechanical and electronic anisotropies.
View Article and Find Full Text PDFOwing to its crystallographic structure, black phosphorus is one of the few 2D materials expressing strongly anisotropic optical, transport, and mechanical properties. We report on the anisotropy of electron-phonon interactions through a polarization-resolved Raman study of the four vibrational modes of atomically thin black phosphorus (2D phosphane): the three bulk-like modes A, B, and A and the Davydov-induced mode labeled A(B). The complex Raman tensor elements reveal that the relative variation in permittivity of all A modes is irrespective of the atomic motion involved lowest along the zigzag direction, the basal anisotropy of these variations is most pronounced for A and A(B), and interlayer interactions in multilayer samples lead to reduced anisotropy.
View Article and Find Full Text PDFWe demonstrate the optical initialization of a hole-spin qubit bound to an isoelectronic center (IC) formed by a pair of Te impurities in ZnSe, an impurity-host system providing high optical homogeneity, large electric dipole moments, and potentially advantageous coherence times. The initialization scheme is based on the spin-preserving tunneling of a resonantly excited donor-bound exciton to a positively charged Te IC, thus forming a positive trion. The radiative decay of the trion within less than 50 ps leaves a heavy hole in a well-defined polarization-controlled spin state.
View Article and Find Full Text PDFThin layers of black phosphorus have recently raised interest owing to their two-dimensional (2D) semiconducting properties, such as tunable direct bandgap and high carrier mobilities. This lamellar crystal of phosphorus atoms can be exfoliated down to monolayer 2D-phosphane (also called phosphorene) using procedures similar to those used for graphene. Probing the properties has, however, been challenged by a fast degradation of the thinnest layers on exposure to ambient conditions.
View Article and Find Full Text PDFThe introduction of stable isotopes in the fabrication of semiconductor nanowires provides an additional degree of freedom to manipulate their basic properties, design an entirely new class of devices, and highlight subtle but important nanoscale and quantum phenomena. With this perspective, we report on phonon engineering in metal-catalyzed silicon nanowires with tailor-made isotopic compositions grown using isotopically enriched silane precursors (28)SiH4, (29)SiH4, and (30)SiH4 with purity better than 99.9%.
View Article and Find Full Text PDFIn recent years, impressive demonstrations related to quantum information processing have been realized. The scalability of quantum interactions between arbitrary qubits within an array remains however a significant hurdle to the practical realization of a quantum computer. Among the proposed ideas to achieve fully scalable quantum processing, the use of photons is appealing because they can mediate long-range quantum interactions and could serve as buses to build quantum networks.
View Article and Find Full Text PDFMicrobial communities associated with submerged detritus in aquatic ecosystems often comprise a diverse mixture of autotrophic and heterotrophic microbes, including algae, bacteria, protozoa, and fungi. Recent studies have documented increased rates of plant litter mass loss when periphytic algae are present. We conducted laboratory and field experiments to assess potential metabolic interactions between natural autotrophic and heterotrophic microbial communities inhabiting submerged decaying plant litter of Typha angustifolia and Schoenoplectus acutus.
View Article and Find Full Text PDFWe present the design of a confocal microscope adapted for optical spectroscopy and imaging at cryogenic temperatures. This system is based on the existing approach of partly inserting the optical components of the microscope inside a helium-bath cryostat. It provides a spatial resolution approaching the diffraction limit with a mechanical stability allowing uninterrupted integration times exceeding 10 h and allows keeping track of a single emitter for unlimited periods of time.
View Article and Find Full Text PDFWe examined the effect of light on extracellular enzyme activities of periphytic/endogenous microbial assemblages associated with decomposing litter of an emergent macrophyte Typha angustifolia within a small inland wetland in southeastern Michigan. Standing-dead Typha leaf litter was collected, placed into floating wire mesh litter baskets, and submerged in a wetland pool. Enzyme saturation assays were conducted on three occasions following litter submergence (days 9, 28, and 44) to generate saturation curves for the individual enzymes tested and to examine potential differences in enzyme saturation kinetics during microbial colonization and development.
View Article and Find Full Text PDFWe report a giant bowing of the spin-orbit splitting energy Delta0 in the dilute GaAs1-xBix alloy for Bi concentrations ranging from 0% to 1.8%. This is the first observation of a large relativistic correction to the host electronic band structure induced by just a few percent of isoelectronic doping in a semiconductor material.
View Article and Find Full Text PDFThe radiolabeled leucine incorporation technique for quantifying rates of bacterial production has increased in popularity since its original description for bacterioplankton communities. Prior studies addressing incorporation conditions (e.g.
View Article and Find Full Text PDFUsing optical spectroscopy with diffraction limited spatial resolution, the possibility of measuring the luminescence from single impurity centers in a semiconductor is demonstrated. Selectively studying individual centers that are formed by two neighboring nitrogen atoms in GaAs makes it possible to unveil their otherwise concealed polarization anisotropy, analyze their selection rules, identify their particular configuration, map their spatial distribution, and demonstrate the presence of a diversity of local environments. Circumventing the limitation imposed by ensemble averaging and the ability to discriminate the individual electronic responses from discrete emitters provides an unprecedented perspective on the nanoscience of impurities.
View Article and Find Full Text PDFCaspases are cysteine proteases that specifically cleave Asp-Xxx bonds. They are key agents in inflammation and apoptosis and are attractive targets for therapy against inflammation, neurodegeneration, ischemia, and cancer. Many caspase structures are known, but most involve either peptide or protein inhibitors, unattractive candidates for drug development.
View Article and Find Full Text PDFThe discovery of a series of potent, selective and reversible dipeptidyl caspase-3 inhibitors are reported. The iterative discovery process of using combinatorial chemistry, parallel synthesis, moleculare modelling and structural biology will be discussed.
View Article and Find Full Text PDFIrradiation of a solution of ethyl zinc alkoxides and CH2I2 leads to clean formation of iodomethylzinc alkoxides; these intermediates are important species generated in stereoselective cyclopropanation processes; no alkyl group exchange is observed in the absence of irradiation; the solid-state structure of (MeO)8Zn7(CH2I)6 is also reported.
View Article and Find Full Text PDF