Semiconductor nanoplatelets (NPLs), with their large exciton binding energy, narrow photoluminescence (PL), and absence of dielectric screening for photons emitted normal to the NPL surface, could be expected to become the fastest luminophores amongst all colloidal nanostructures. However, super-fast emission is suppressed by a dark (optically passive) exciton ground state, substantially split from a higher-lying bright (optically active) state. Here, the exciton fine structure in 2-8 monolayer (ML) thick Cs n − 1 Pb n Br 3n + 1 NPLs is revealed by merging temperature-resolved PL spectra and time-resolved PL decay with an effective mass model taking quantum confinement and dielectric confinement anisotropy into account. This approach exposes a thickness-dependent bright-dark exciton splitting reaching 32.3 meV for the 2 ML NPLs. The model also reveals a 5-16 meV splitting of the bright exciton states with transition dipoles polarized parallel and perpendicular to the NPL surfaces, the order of which is reversed for the thinnest NPLs, as confirmed by TR-PL measurements. Accordingly, the individual bright states must be taken into account, while the dark exciton state strongly affects the optical properties of the thinnest NPLs even at room temperature. Significantly, the derived model can be generalized for any isotropically or anisotropically confined nanostructure.
Controlling electronic population through chemical doping is one way to tip the balance between competing phases in materials with strong electronic correlations. Vanadium dioxide exhibits a first-order phase transition at around 338 K between a high-temperature, tetragonal, metallic state (T) and a low-temperature, monoclinic, insulating state (M1), driven by electron-electron and electron-lattice interactions. Intercalation of VO2 with atomic hydrogen has been demonstrated, with evidence that this doping suppresses the transition. However, the detailed effects of intercalated H on the crystal and electronic structure of the resulting hydride have not been previously reported. Here we present synchrotron and neutron diffraction studies of this material system, mapping out the structural phase diagram as a function of temperature and hydrogen content. In addition to the original T and M1 phases, we find two orthorhombic phases, O1 and O2, which are stabilized at higher hydrogen content. We present density functional calculations that confirm the metallicity of these states and discuss the physical basis by which hydrogen stabilizes conducting phases, in the context of the metal-insulator transition.
We report measurements of the diffusion of atomic hydrogen in single crystalline VO 2 micro/nanobeams by direct exposure to atomic hydrogen, without catalyst. The atomic hydrogen is generated by a hot filament, and the doping process takes place at moderate temperature (373 K). Undoped VO 2 has a metal-to-insulator phase transition at ~340 K between a high -temperature, rutile, metallic phase and a low-temperature, monoclinic, insulating phase with a resistance exhibiting a semiconductor-like temperature dependence.Atomic hydrogenation results in stabilization of the metallic phase of VO 2 micro/nanobeam down to 2 K, the lowest point we could reach in our measurement setup. Optical characterization shows that hydrogen atoms prefer to diffuse along the c-axis of rutile (a-axis of monoclinic) VO 2 , along the oxygen "channels". Based on observing the movement of the hydrogen diffusion front in single crystalline VO 2 beams, we estimate the diffusion constant
We investigate "Posner molecules", calcium phosphate clusters with chemical formula Ca9(PO4)6. Originally identified in hydroxyapatite, Posner molecules have also been observed as free-floating molecules in vitro. The formation and aggregation of Posner molecules have important implications for bone growth, and may also play a role in other biological processes such as the modulation of calcium and phosphate ion concentrations within the mitochondrial matrix. In this work, we use a first-principles computational methodology to study the structure of Posner molecules, their vibrational spectra, their interactions with other cations, and the process of pairwise bonding. Additionally, we show that the Posner molecule provides an ideal environment for the six constituent 31P nuclear spins to obtain very long spin coherence times. In vitro, the spins could provide a platform for liquid-state nuclear magnetic resonance quantum computation. In vivo, the spins may have medical imaging applications. The spins have also been suggested as "neural qubits" in a proposed mechanism for quantum processing in the brain.
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