Impurity doping of ultrasmall nanoscale (usn) silicon (Si) currently used in ultralarge scale integration (ULSI) faces serious miniaturization challenges below the 14 nm technology node such as dopant out-diffusion and inactivation by clustering in Si-based field-effect transistors (FETs). Moreover, self-purification and massively increased ionization energy cause doping to fail for Si nano-crystals (NCs) showing quantum confinement. To introduce electron- (n-) or hole- (p-) type conductivity, usn-Si may not require doping, but an energy shift of electronic states with respect to the vacuum energy between different regions of usn-Si. We show in theory and experiment that usn-Si can experience a considerable energy offset of electronic states by embedding it in silicon dioxide (SiO2) or silicon nitride (Si3N4), whereby a few monolayers (MLs) of SiO2 or Si3N4 are enough to achieve these offsets. Our findings present an alternative to conventional impurity doping for ULSI, provide new opportunities for ultralow power electronics and open a whole new vista on the introduction of p- and n-type conductivity into usn-Si.
A hexagonal phase in the ternary Ge-Se-Te system with an approximate composition of GeSe Te has been known since the 1960s but its structure has remained unknown. We have succeeded in growing single crystals by chemical transport as a prerequisite to solve and refine the Ge Se Te structure. It consists of layers that are held together by van der Waals type weak chalcogenide-chalcogenide interactions but also display unexpected Ge-Ge contacts, as confirmed by electron microscopy analysis. The nature of the electronic structure of Ge Se Te was characterized by chemical bonding analysis, in particular by the newly introduced density of energy (DOE) function. The Ge-Ge bonding interactions serve to hold electrons that would otherwise go into antibonding Ge-Te contacts.
Controlling a state of material between its crystalline and glassy phase has fostered many real-world applications. Nevertheless, design rules for crystallization and vitrification kinetics still lack predictive power. Here, we identify stoichiometry trends for these processes in phase change materials, i.e. along the GeTe-GeSe, GeTe-SnTe, and GeTe-Sb2Te3 pseudo-binary lines employing a pump-probe laser setup and calorimetry. We discover a clear stoichiometry dependence of crystallization speed along a line connecting regions characterized by two fundamental bonding types, metallic and covalent bonding. Increasing covalency slows down crystallization by six orders of magnitude and promotes vitrification. The stoichiometry dependence is correlated with material properties, such as the optical properties of the crystalline phase and a bond indicator, the number of electrons shared between adjacent atoms. A quantum-chemical map explains these trends and provides a blueprint to design crystallization kinetics.
Impurity doping in silicon (Si) ultra-large-scale integration is one of the key challenges which prevent further device miniaturization. Using ultraviolet photoelectron spectroscopy and X-ray absorption spectroscopy in the total fluorescence yield mode, we show that the lowest unoccupied and highest occupied electronic states of ≤3 nm thick SiO2-coated Si nanowells shift by up to 0.2 eV below the conduction band and ca. 0.7 eV below the valence band edge of bulk silicon, respectively. This nanoscale electronic structure shift induced by anions at surfaces (NESSIAS) provides the means for low-nanoscale intrinsic Si (i-Si) to be flooded by electrons from an external (bigger, metallic) reservoir, thereby getting highly electron- (n-) conductive. While our findings deviate from the behavior commonly believed to govern the properties of silicon nanowells, they are further confirmed by the fundamental energy gap as per nanowell thickness when compared against published experimental data. Supporting our findings further with hybrid density functional theory calculations, we show that other group IV semiconductors (diamond, Ge) do respond to the NESSIAS effect in accord with Si. We predict adequate nanowire cross-sections (X-sections) from experimental nanowell data with a recently established crystallographic analysis, paving the way to undoped ultrasmall silicon electronic devices with significantly reduced gate lengths, using complementary metal–oxide–semiconductor-compatible materials.
Hybrid sol-gel catalysts of zinc hexacyanocobaltate and SiO 2 were prepared by co-precipitation of the double metal cyanide with silica. Hybrid catalysts prepared at moderately acidic conditions showed the best performance with respect to activity, selectivity and stability. The hybrid sol-gel materials displayed high catalytic activity for the copolymerisation of styrene oxide and carbon dioxide (up to 650 mol SO (mol Zn h) −1 ) and high productivity (575 g Polymer g Catalyst −1 ). They also displayed good selectivity to the polymeric product (80-87%), while only little cyclic styrene carbonate was formed as side product. A detailed electron microscopy study of the hybrid sol-gel materials showed that the active phase consisted of thin platelets containing the metals in a molar ratio n Zn /n Co = 2.1, whereby the double metal cyanide was closely associated with silica.
Alloys of sulphur, selenium and tellurium, often referred to as chalcogenide semiconductors offer a highly versatile, compositionally-controllable material platform for a variety of passive and active photonic applications. They are optically nonlinear, photoconductive materials with wide transmission windows that present various high- and low-index dielectric, low-epsilon and plasmonic properties across ultra-violet, visible and infrared frequencies, in addition to an ultra-fast, non-volatile, electrically-/optically-induced switching capability between phase states with markedly different electromagnetic properties. This roadmap collection presents an in-depth account of the critical role that chalcogenide semiconductors play within various traditional and emerging photonic technology platforms. The potential of this field going forward is demonstrated by presenting context and outlook on selected socioeconomically important research streams utilizing chalcogenide semiconductors. To this end, this roadmap encompasses selected topics that range from systematic design of material properties and switching kinetics to device level nanostructuring and integration within various photonic system architectures.
Chalcogenides possess interesting optical properties, which are attractive for a variety of applications such as data storage, neuromorphic computing, and photonic switches. Lately a group of covalently bonded chalcogenides including Sb2Se3 and Sb2S3 has moved into the focus of interest for such photonic applications, where high optical contrast as well as reliable and fast switching is of crucial importance. Here, these properties of Sb2Se3 are examined and compared with typical phase change materials such as GeSb2Te4 and Ge2Sb2Te5. Sb2Se3 is favorable for many photonic applications due to its larger band gap, yet, the maximum optical contrast achievable is smaller than for GeTe and Ge2Sb2Te5. Furthermore, crystallization needs significantly longer and exhibits a distinctively wider stochastic distribution of reflectances after crystallization, which provides challenges for the usage in photonic applications. At the same time, the glassy/amorphous state of Sb2Se3 is more stable. These differences can be attributed to differences in bonding of the crystalline state, which is more covalent for Sb2Se3. A quantum‐chemical map can help to understand and explain these trends and facilitates the design of tailored materials for photonic applications.
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