In contrast to the traditional perspective that thermal fluctuations are insignificant in surface dynamics, here we report their influence on surface reaction dynamics. Using real-time low-energy electron microscopy imaging of NiAl(100) under both vacuum and O atmospheres, we demonstrate that transient temperature variations substantially alter the direction of atom diffusion between the surface and bulk, leading to markedly different oxidation outcomes. During heating, substantial outward diffusion of atoms from the bulk to the surface results in step growth.
View Article and Find Full Text PDFHeterostructures (HSs) formed by the transition-metal dichalcogenide materials have shown great promise in next-generation (opto)electronic applications. An artificially twisted HS allows us to manipulate the optical and electronic properties. In this work, we introduce the understanding of the energy transfer (ET) process governed by the dipolar interaction in a twisted molybdenum diselenide (MoSe) homobilayer any charge-blocking interlayer.
View Article and Find Full Text PDFMaterials with field-tunable polarization are of broad interest to condensed matter sciences and solid-state device technologies. Here, using hydrogen (H) donor doping, we modify the room temperature metallic phase of a perovskite nickelate NdNiO into an insulating phase with both metastable dipolar polarization and space-charge polarization. We then demonstrate transient negative differential capacitance in thin film capacitors.
View Article and Find Full Text PDFA key aspect of how the brain learns and enables decision-making processes is through synaptic interactions. Electrical transmission and communication in a network of synapses are modulated by extracellular fields generated by ionic chemical gradients. Emulating such spatial interactions in synthetic networks can be of potential use for neuromorphic learning and the hardware implementation of artificial intelligence.
View Article and Find Full Text PDFHigh light absorption (∼15%) and strong photoluminescence (PL) emission in monolayer (1L) transition metal dichalcogenides (TMDs) make them ideal candidates for optoelectronic device applications. Competing interlayer charge transfer (CT) and energy transfer (ET) processes control the photocarrier relaxation pathways in TMD heterostructures (HSs). In TMDs, long-distance ET can survive up to several tens of nm, unlike the CT process.
View Article and Find Full Text PDFInterlayer excitons (ILXs) - electron-hole pairs bound across two atomically thin layered semiconductors - have emerged as attractive platforms to study exciton condensation, single-photon emission and other quantum information applications. Yet, despite extensive optical spectroscopic investigations, critical information about their size, valley configuration and the influence of the moiré potential remains unknown. Here, in a WSe/MoS heterostructure, we captured images of the time-resolved and momentum-resolved distribution of both of the particles that bind to form the ILX: the electron and the hole.
View Article and Find Full Text PDFType-II heterostructures (HSs) are essential components of modern electronic and optoelectronic devices. Earlier studies have found that in type-II transition metal dichalcogenide (TMD) HSs, the dominating carrier relaxation pathway is the interlayer charge transfer (CT) mechanism. Here, this report shows that, in a type-II HS formed between monolayers of MoSe and ReS, nonradiative energy transfer (ET) from higher to lower work function material (ReS to MoSe) dominates over the traditional CT process with and a charge-blocking interlayer.
View Article and Find Full Text PDFAn exciton, a two-body composite quasiparticle formed of an electron and hole, is a fundamental optical excitation in condensed matter systems. Since its discovery nearly a century ago, a measurement of the excitonic wave function has remained beyond experimental reach. Here, we directly image the excitonic wave function in reciprocal space by measuring the momentum distribution of electrons photoemitted from excitons in monolayer tungsten diselenide.
View Article and Find Full Text PDFResolving momentum degrees of freedom of excitons, which are electron-hole pairs bound by the Coulomb attraction in a photoexcited semiconductor, has remained an elusive goal for decades. In atomically thin semiconductors, such a capability could probe the momentum-forbidden dark excitons, which critically affect proposed opto-electronic technologies but are not directly accessible using optical techniques. Here, we probed the momentum state of excitons in a tungsten diselenide monolayer by photoemitting their constituent electrons and resolving them in time, momentum, and energy.
View Article and Find Full Text PDFWe report on the evolution of the thickness-dependent electronic band structure of the two-dimensional layered-dichalcogenide molybdenum disulfide (MoS2). Micrometer-scale angle-resolved photoemission spectroscopy of mechanically exfoliated and chemical-vapor-deposition-grown crystals provides direct evidence for the shifting of the valence band maximum from Γ to K, for the case of MoS2 having more than one layer, to the case of single-layer MoS2, as predicted by density functional theory. This evolution of the electronic structure from bulk to few-layer to monolayer MoS2 had earlier been predicted to arise from quantum confinement.
View Article and Find Full Text PDFThe oxidation of CO is the archetypal heterogeneous catalytic reaction and plays a central role in the advancement of fundamental studies, the control of automobile emissions, and industrial oxidation reactions. Copper-based catalysts were the first catalysts that were reported to enable the oxidation of CO at room temperature, but a lack of stability at the elevated reaction temperatures that are used in automobile catalytic converters, in particular the loss of the most reactive Cu(+) cations, leads to their deactivation. Using a combined experimental and theoretical approach, it is shown how the incorporation of titanium cations in a Cu2O film leads to the formation of a stable mixed-metal oxide with a Cu(+) terminated surface that is highly active for CO oxidation.
View Article and Find Full Text PDFSubstrate engineering is a key factor in the synthesis of new complex materials. The substrate surface has to be conditioned in order to minimize the energy threshold for the formation of the desired phase or to enhance the catalytic activity of the substrate. The mechanism of the substrate activity, especially of technologically relevant oxide surfaces, is poorly understood.
View Article and Find Full Text PDFFruit growth is a coordinated, complex interaction of cell division, differentiation and expansion. Gibberellin (GA) involvement in the reproductive events is an important aspect of GA effects. Perennial fruit-trees such as plum (Prunus salicina L.
View Article and Find Full Text PDFPhotosystem II (PSII) of photosynthesis has the unique ability to photochemically oxidize water. Recently an engineered bacterioferritin photochemical 'reaction centre' (BFR-RC) using a zinc chlorin pigment (ZnCe6) in place of its native heme has been shown to photo-oxidize bound manganese ions through a tyrosine residue, thus mimicking two of the key reactions on the electron donor side of PSII. To understand the mechanism of tyrosine oxidation in BFR-RCs, and explore the possibility of water oxidation in such a system we have built an atomic-level model of the BFR-RC using ONIOM methodology.
View Article and Find Full Text PDFDoping catalytically inactive materials with dispersed atoms of an active species is a promising route toward realizing ultradilute binary catalyst systems. Beyond catalysis, strategically placed metal atoms can accelerate a wide range of solid-state reactions, particularly in hydrogen storage processes. Here we analyze the role of atomic Ti catalysts in the hydrogenation of Al-based hydrogen storage materials.
View Article and Find Full Text PDFThe absorption and energy transfer properties of photosynthetic pigments are strongly influenced by their local environment or "site." Local electrostatic fields vary in time with protein and chromophore molecular movement and thus transiently influence the excited state transition properties of individual chromophores. Site-specific information is experimentally inaccessible in many light-harvesting pigment-proteins due to multiple chromophores with overlapping spectra.
View Article and Find Full Text PDFThe CaMn(4) cluster of the oxygen-evolving complex (OEC) of photosynthesis catalyzes the light-driven splitting of water into molecular oxygen, protons, and electrons. The OEC is buried within photosystem II (PSII), a multisubunit integral membrane protein complex, and water must find its way to the CaMn(4) cluster by moving through protein. Channels for water entrance, and proton and oxygen exit, have previously been proposed following the analysis of cavities found within X-ray structures of PSII.
View Article and Find Full Text PDFSuppression of nucleation around a gold electrode during pentacene growth on a SiO2 channel is found by photoemission electron microscopy. Mass flow is driven by the difference between the molecular orientations on SiO2 and gold. The poor connectivity at the channel/electrode boundary causes degradation in the performance of a field-effect transistor, which is found to be improved by self-assembled monolayer treatment on the electrode (see figure; thickness in monolayers (ML)).
View Article and Find Full Text PDFOn 24 July 2005, six members of a single family were admitted to the Medicine and Pediatrics Department of Khulna Medical College Hospital, Khulna, Bangladesh, with a history of ingestion of puffer fish. All patients developed toxic manifestations. The cases were clinically analysed with successful outcomes.
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