We study the effect of the zero- to one-dimensional (1D) transformation on multiparticle Auger recombination using a series of elongated semiconductor nanocrystals (quantum rods). We observe a transition from the three- to two-particle recombination process as the nanocrystal aspect ratio is increased. This transition indicates that in the 1D confinement limit, Auger decay is dominated by Coulomb interactions between 1D excitons that recombine in a bimolecular fashion. One consequence of this effect is strongly reduced decay rates of higher multiparticle states that lead to increased optical-gain lifetimes and efficient light amplification due to involvement of excited electronic states.

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We perform side-by-side comparison of optical gain properties of spherical and elongated nanocrystals (quantum dots and quantum rods, respectively). This comparison indicates that elongated nanoparticles provide several features beneficial for lasing applications, such as enhanced absorption cross sections (and hence reduced lasing threshold and improved photostability), increased optical gain lifetime, and extended optical gain spectral range through the use of transitions that involve both ground and excited electronic states.

For advanced device applications, increasing the compositional abruptness of axial heterostructured and modulation doped nanowires is critical for optimizing performance. For nanowires grown from metal catalysts, the transition region width is dictated by the solute solubility within the catalyst. For example, as a result of the relatively high solubility of Si and Ge in liquid Au for vapor-liquid-solid (VLS) grown nanowires, the transition region width between an axial Si-Ge heterojunction is typically on the order of the nanowire diameter. When the solute solubility in the catalyst is lowered, the heterojunction width can be made sharper. Here we show for the first time the systematic increase in interface sharpness between axial Ge-Si heterojunction nanowires grown by the VLS growth method using a Au-Ga alloy catalyst. Through in situ tailoring of the catalyst composition using trimethylgallium, the Ge-Si heterojunction width is systematically controlled by tuning the semiconductor solubility within a metal Au-Ga alloy catalyst. The present approach of alloying to control solute solubilities in the liquid catalyst may be extended to increasing the sharpness of axial dopant profiles, for example, in Si-Ge pn-heterojunction nanowires which is important for such applications as nanowire tunnel field effect transistors or in Si pn-junction nanowires.

Discovered almost two decades ago, the solution-liquid-solid (SLS) method for semiconductor nanowire synthesis has proven to be an important route to high-quality, single-crystalline anisotropic nanomaterials. In execution, the SLS technique is similar to colloidal quantum-dot synthesis in that it entails the injection of chemical precursors into a hot surfactant solution, but mechanistically it is considered the solution-phase analogue to vapour-liquid-solid (VLS) growth. Both SLS and VLS methods make use of molten metal nanoparticles to catalyse the nucleation and elongation of single-crystalline nanowires. Significantly, however, the methods differ in how chemical precursors are introduced to the metal catalysts. In SLS, precursors are added in a one-off fashion in a flask, whereas in VLS they are carried by a flow of gas through the reaction chamber, and by-products are removed similarly. The ability to dynamically control the introduction of reactants and removal of by-products in VLS synthesis has enabled a degree of synthetic control not possible with SLS growth. We show here that SLS synthesis can be transformed into a continuous technique using a microfluidic reactor. The resulting flow-based SLS ('flow-SLS') platform allows us to slow down the synthesis of nanowires and capture mechanistic details concerning their growth in the solution phase, as well as synthesize technologically relevant axially heterostructured semiconductor nanowires, while maintaining the propensity of SLS for accessing ultrasmall diameters below 10 nm.

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Nanometric solid inclusions in diamond incorporated in garnet and zircon from felsic gneiss of the Kokchetav massif, Kazakhstan, have been examined utilizing electron microscopy and focused ion beam techniques. Host garnet and zircon contain numerous pockets of multiple inclusions, which consist of 1-3 diamond crystals intergrown with quartz, phengite, phlogopite, albite, K-feldspar, rutile, apatite, titanite, biotite, chlorite and graphite in various combinations. Recalculation of the average chemical composition of the entrapped fluid represented by multiple inclusion pockets indicates that such fluid contained a low wt% of SiO 2 , suggesting a relatively low-temperature fluid rather than a melt. Transmission electron microscopy revealed that the diamond contains abundant nanocrystalline inclusions of oxides, rare carbonates and silicates. Within the 15 diamond crystals studied, abundant inclusions were found of SiO 2 , TiO 2 , Fe x O y , Cr 2 O 3 , ZrSiO 4 , and single grains of Th x O y , BaSO 4 , MgCO 3 , FeCr 2 O 4 and a stoichiometric Fe-rich pyroxene. The diversity of trace elements within inclusions of essentially the same stoichiometry suggests that the Kokchetav diamond crystallized from a fluid containing variable amounts of Si, Fe, Ti, Cr, Zr, Ba, Mg and Th and other minor components such as K, Na, P, S, Pb, Zn, Nb, Al, Ca, Cl. Most of the components in crystals included in diamond appear to have their origin in the subducted metasediments, but some of them probably originate from the mantle. It is concluded that Kokchetav diamond most likely crystallized from a COH-rich multicomponent supercritical fluid at a relatively low temperature (hence the apparently low content of rock-forming elements), and that the diversity of major and minor components suggests interactions between subducted metasediments and mantle components.