ABSTRACT:We dope CdSe nanocrystals with Ag impurities and investigate their optical and electrical properties. Doping leads not only to dramatic changes but surprising complexity. The addition of just a few Ag atoms per nanocrystal causes a large enhancement in the fluorescence, reaching efficiencies comparable to core−shell nanocrystals. While Ag was expected to be a substitutional acceptor, nonmonotonic trends in the fluorescence and Fermi level suggest that Ag changes from an interstitial (ntype) to a substitutional (p-type) impurity with increased doping.
Electrical transport in films of CdSe nanocrystals with diameters varying from 2.9 to 5.1 nm was examined over 233-300 K by employing electrolyte gating to control the electron density. The transport parameters varied strongly and systematically with nanocrystal diameter. First, a strong correlation was observed between the device turn-on voltage and the size-dependent position of the lowest unoccupied electronic states of the nanocrystals. Second, the electron mobility increased with increasing particle diameter and reached a high value of 0.6 cm 2 /(V s) for films with 5.1 nm nanocrystals. Third, the charge transport could be described in terms of the nearest-neighbor-hopping mechanism with a size-dependent activation energy and a pre-exponential factor for mobility. The activation energy can be viewed as a size-dependent charging energy of an individual nanocrystal. Collectively, the combination of size-and temperature-dependent measurements provides a powerful approach to understanding electrical transport in nanocrystal films.
We report the size- and temperature-dependence of electron transport in thin films of PbSe nanocrystals. Upon increasing temperature over the range 28-200 K, the electron transport underwent a transition in mechanism from Efros-Shklovskii-variable-range-hopping (ES-VRH) to nearest-neighbor-hopping (NNH). The transition occurred at higher temperatures for films with smaller particles. The electron localization length, estimated from the ES-VRH model, was comparable to the nanocrystal size and scaled systematically with nanocrystal diameter. The activation energy from the NNH regime was also size-dependent, which is attributed both to size-dependent Coulomb effects and the size-distribution of nanocrystals.
A general, one-pot, single-step method for producing colloidal silver chalcogenide (Ag(2)E; E = Se, S, Te) nanocrystals is presented, with an emphasis on Ag(2)Se. The method avoids exotic chemicals, high temperatures, and high pressures and requires only a few minutes of reaction time. While Ag(2)S and Ag(2)Te are formed in their low-temperature monoclinic phases, Ag(2)Se is obtained in a metastable tetragonal phase not observed in the bulk.
We prepare Ag(2)Se nanocrystals with average diameters between 2.7 and 10.4 nm that exhibit narrow optical absorption features in the near to mid infrared. We demonstrate that these features are broadly tunable due to quantum confinement. They provide the longest wavelength absorption peaks (6.5 μm) yet reported for colloidal nanocrystals.
PSS-Te nanowires. This technique is shown to provide tunability of thermoelectric and electronic properties, providing up to 22% enhancement of the system's power factor in the low-doping regime, consistent with preferential scattering of low energy carriers. This work provides an exciting platform for rational design of multiphase nanocomposites and highlights the potential for engineering of carrier filtering within hybrid thermoelectrics via introduction of interfaces with controlled structural and energetic properties.
Nanocrystals are known to alter the relative stability of bulk solid phases. Here we test the limits of this effect on Ag2Se nanocrystals, a promising new electronic and infrared material. In the bulk, Ag2Se exhibits a solid-solid phase transition to a superionic conducting phase at moderate temperatures. We map this phase transition as a function of size, temperature, and surface treatment in Ag2Se core-only and core-shell nanocrystals. We show that the transition can be tuned not just below but also above the bulk phase-transition temperature. This phase flexibility has implications for applications in optoelectronic and phase-memory devices.
Silicon wafers are commonly etched in potassium hydroxide solutions to form highly symmetric surface structures. These arise when slow-etching {111} atomic planes are exposed on standard low-index surfaces. However, the ability of nonstandard high-index wafers to provide more complex structures by tilting the {111} planes has not been fully appreciated. We demonstrate the power of this approach by creating chiral surface structures and nanoparticles of a specific handedness from gold. When the nanoparticles are dispersed in liquids, gold colloids exhibiting record molar circular dichroism (>5 × 10(9) M(-1) cm(-1)) at red wavelengths are obtained. The nanoparticles also present chiral pockets for binding.
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