A long-standing issue regarding the local and long-range structure of V(2)O(5)*nH(2)O xerogel has been successfully addressed. The full three-dimensional structure of the lamellar turbostratic V(2)O(5)*nH(2)O xerogel was determined by the atomic pair distribution function technique. We show that on the atomic scale the slabs of the xerogel can be described well as almost perfect pairs (i.e., bilayers) of single V(2)O(5) layers made of square pyramidal VO(5) units. These slabs are separated by water molecules and stack along the z-axis of a monoclinic unit cell (space group C2/m) with parameters a = 11.722(3) A, b = 3.570(3) A, c = 11.520(3) A, and beta = 88.65 degrees. The stacking sequence shows signatures of turbostratic disorder and a structural coherence limited to 50 A.
The molecular building block approach was employed effectively to construct a series of novel isoreticular, highly porous and stable, aluminum-based metal–organic frameworks with soc topology. From this platform, three compounds were experimentally isolated and fully characterized: namely, the parent Al-soc-MOF-1 and its naphthalene and anthracene analogues. Al-soc-MOF-1 exhibits outstanding gravimetric methane uptake (total and working capacity). It is shown experimentally, for the first time, that the Al-soc-MOF platform can address the challenging Department of Energy dual target of 0.5 g/g (gravimetric) and 264 cm3 (STP)/cm3 (volumetric) methane storage. Furthermore, Al-soc-MOF exhibited the highest total gravimetric and volumetric uptake for carbon dioxide and the utmost total and deliverable uptake for oxygen at relatively high pressures among all microporous MOFs. In order to correlate the MOF pore structure and functionality to the gas storage properties, to better understand the structure–property relationship, we performed a molecular simulation study and evaluated the methane storage performance of the Al-soc-MOF platform using diverse organic linkers. It was found that shortening the parent Al-soc-MOF-1 linker resulted in a noticeable enhancement in the working volumetric capacity at specific temperatures and pressures with amply conserved gravimetric uptake/working capacity. In contrast, further expansion of the organic linker (branches and/or core) led to isostructural Al-soc-MOFs with enhanced gravimetric uptake but noticeably lower volumetric capacity. The collective experimental and simulation studies indicated that the parent Al-soc-MOF-1 exhibits the best compromise between the volumetric and gravimetric total and working uptakes under a wide range of pressure and temperature conditions.
tors (17). The resulting density matrix has only positive eigenvalues, and hence it represents a physically possible state. Its fidelity with respect to the expected Bell state, |Y -〉 from Eq. 2, is F = 86.0(4)%, with 0.5 < F ≤ 1 proving entanglement (18). From the density matrix, following (16), we derive a concurrence of C = 0.73(7), with 0 < C ≤ 1 also proving entanglement. Because of technical imperfections, e.g., of polarizers in the detection setups, the observed fidelity/concurrence sets a lower bound for both the atom-photon and photon-photon entanglement achieved. The same measurements were done for B = −0.13 G and t S = 2.8 ms for which the atomic superposition state accumulates a p phase shift (compare to Fig. 3). Therefore, a density matrix corresponding to the Bell stateis expected. This is indeed observed (Fig. 4B) with a fidelity of F = 82.9(6)% and a concurrence of C = 0.72(13). The state evolves between the two photon detections as a result of the constant magnetic field.Future experiments could produce a timeindependent |Y + 〉 Bell state by applying a pulsed magnetic field to the atom between entanglement generation and state mapping. Moreover, partial driving of the Raman transition in combination with atomic state manipulation should allow production of highly entangled multiphoton states (12). Our technique applied to a quasi-permanently trapped intracavity atom (3, 19) will push the probability of success even further, making the scheme truly deterministic. Two (or more) such systems operated in parallel are perfectly suited for teleportation and entanglement experiments in a quantum network (20)(21)(22) or quantum gate operations in a distributed and, hence, scalable quantum computer (23, 24). Inorganic porous materials are being developed for use as molecular sieves, ion exchangers, and catalysts, but most are oxides. We show that various sulfide and selenide clusters, when bound to metal ions, yield gels having porous frameworks. These gels are transformed to aerogels after supercritical drying with carbon dioxide. The aerogels have high internal surface area (up to 327 square meters per gram) and broad pore size distribution, depending on the precursors used. The pores of these sulfide and selenide materials preferentially absorb heavy metals. These materials have narrow energy gaps (between 0.2 and 2.0 electron volts) and low densities, and they may be useful in optoelectronics, as photocatalysts, or in the removal of heavy metals from water.
If the full scientific and technological potential of mesostructured materials is to be achieved, systems with continuous domains in the form of single crystals or films must be prepared. Here we report a reliable and facile system for making large single-crystal particles of chalcogenido mesostructured materials with a highly organized cubic structure, accessible pore structure, and semiconducting properties. Building blocks with square planar bonding topology, Pt(2+) and [Sn(2)Se(6)](4)(-), in combination with long-chain pyridinium surfactants (C(n)PyBr, n = 18, 20) favor faceted single-crystal particles with the highest possible space group symmetry Ia3d. This is an important step toward developing large single-domain crystalline mesostructured semiconductors and usable natural self-assembled antidot array systems. The tendency toward cubic symmetry is so strong that the materials assemble readily under experimental conditions that can tolerate considerable variation and form micrometer-sized rhombic dodecahedral cubosome particles. The c-C(n)PyPtSnSe materials are the first to exhibit reversible ion-exchange properties. The surfactant molecules can be ion-exchanged reversibly and without loss of the cubic structure and particle morphology. The cubosomes possess a three-dimensional open Pt-Sn-Se framework with a low-energy band gap of approximately 1.7 eV.
The CsSnI perovskite and the corresponding SnF-containing material with nominal composition CsSnIF were synthesized by solid-state reactions and structurally characterized by powder X-ray diffraction. Both materials undergo rapid phase transformation upon exposure to air from the black orthorhombic phase (B-γ-CsSnI) to the yellow orthorhombic phase (Y-CsSnI), followed by irreversible oxidation into CsSnI within several hours. The phase transition occurs at a significantly lower rate in the SnF-containing material rather than in the pure perovskite. The high hole-carrier concentration of the materials prohibits the detection of Raman signals for B-γ-CsSnI and induces a very strong plasmonic reflectance in the far-IR. In contrast, far-IR phonon bands and a rich Raman spectrum are observed for the Y-CsSnI modification below 140 cm with weak frequency shift gradients versus temperatures between -95 and +170 °C. Above 170 °C, the signal is lost due to B-α-CsSnI re-formation. The photoluminescence spectra exhibit residual blue shifts and broadening as a sign of structural transformation initiation.
Open framework metal chalcogenide solids, with pore sizes in the nano- and mesoscale, are of potentially broad technological and fundamental interest in research areas ranging from optoelectronics to the physics of quantum confinement. Although there have been significant advances in the design and synthesis of mesostructured silicas, the construction of their non-oxidic analogues still remains a challenge. Here we describe a synthetic strategy that allows the preparation of a large class of mesoporous materials based on supramolecular assembly of tetrahedral Zintl anions [SnSe4]4- with transition metals in the presence of cetylpyridinium (CP) surfactant molecules. These mesostructured semiconducting selenide materials are of the general formulae (CP)4-2xMxSnSe4 (where 1.0 < x < 1.3; M=Mn, Fe, Co, Zn, Cd, Hg). The resulting materials are open framework chalcogenides and form mesophases with uniform pore size (with spacings between 35 and 40 A). The pore arrangement depends on the synthetic conditions and metal used, and include disordered wormhole, hexagonal and even cubic phases. All compounds are medium bandgap semiconductors (varying between 1.4 and 2.5 eV). We expect that such semiconducting porous networks could be used for optoelectronic, photosynthetic and photocatalytic applications.
Superconducting low dimensional systems are the natural choice for fast and sensitive infrared detection, because of their quantum nature and the low-noise, cryogenic operation environment. On the other hand, monochromatic and coherent electron beams, emitted from superconductors and carbon-based nanostructured materials, respectively, are significant for the development of electron optical systems such as electron microscopes and electron-beam nanofabrication systems. Here we describe for the first time a simple method which yields carbon nanotubes encapsulating single crystalline superconducting tin nanowires by employing the catalytic chemical vapor deposition method over solid tin dioxide. The superconducting tin nanowires, with diameters 15-35 nm, are covered with well-graphitized carbon walls and show, due to their reduced diameters, a critical magnetic field (Hc) more than 30 times higher than the value of bulk metallic tin.
Flame-melting rapid-cooling reactions were used to synthesize a number of pure phases of the Cs2MIIMIV 3Q8 family (MII = Mg, Zn, Cd, Hg; MIV = Ge, Sn; Q = S, Se, Te) whereas the more toxic members were synthesized using a traditional tube furnace synthesis. All Cs2MIIMIV 3Q8 compounds presented here crystallize in the noncentrosymmetric space group P212121, except for Cs2ZnGe3S8, which crystallizes in the centrosymmetric space group P21/n. The structures contain chains of corner-sharing MIIQ4 and MIVQ4 tetrahedra linked by edge-sharing MIV 2Q6 dimers to give a two-dimensional structure. All phases are structurally similar to the AMIIIMIVQ4 (A = alkali metal, Tl; MIII = Al, Ga, In; MIV = Si, Ge, Sn; Q = S, Se) phases; however, the members of this family have completely ordered MII and MIV sites as opposed to the occupational disorder of MIII and MIV over all tetrahedral sites present in AMIIIMIVQ4. The structural trends of the Cs2MIIMIV 3Q8 family are discussed, along with a systematic study of their optical properties. Density functional theory (DFT) electronic structure calculations were performed using the projector augmented wave method to further investigate the trends in the band gaps of the Cs2MIIMIV 3Se8 (MII = Mg, Zn; MIV = Ge, Sn) compounds. The experimental diffuse reflectance UV–vis spectroscopy results show that the Mg compounds have smaller band gaps than those containing Zn for both the Ge and the Sn families whereas the DFT calculations show the opposite trend. Cs2HgSn3Se8 was studied as a representative example of this family using differential thermal analysis and melts congruently at 595 °C. Crystal growth of this compound using the Bridgman method resulted in a polycrystalline ingot from which plate crystals ∼2 mm × 3 mm could be cleaved. The band gap of the compounds varies from a narrow 1.07 eV for Cs2ZnGe3Te8 to a wide 3.3 eV for Cs2ZnGe3S8 and Cs2CdGe3S8 making this family a potentially useful source of materials for a variety of electronic applications. Cs2HgSn3Se8 crystals exhibit photoconductivity response where the photoexcited electron and hole show mobility-lifetime products on the order of 3.69 × 10–5 cm2/V and (μτ)h∥ = 7.78 × 10–5 cm2/V, respectively.
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