We measure the room-temperature electron and hole field-effect mobilities (micro(FE)) of a series of alkanedithiol-treated PbSe nanocrystal (NC) films as a function of NC size and the length of the alkane chain. We find that carrier mobilities decrease exponentially with increasing ligand length according to the scaling parameter beta = 1.08-1.10 A(-1), as expected for hopping transport in granular conductors with alkane tunnel barriers. An electronic coupling energy as large as 8 meV is calculated from the mobility data. Mobilities increase by 1-2 orders of magnitude with increasing NC diameter (up to 0.07 and 0.03 cm(2) V(-1) s(-1) for electrons and holes, respectively); the electron mobility peaks at a NC size of approximately 6 nm and then decreases for larger NCs, whereas the hole mobility shows a monotonic increase. The size-mobility trends seem to be driven primarily by the smaller number of hops required for transport through arrays of larger NCs but may also reflect a systematic decrease in the depth of trap states with decreasing NC band gap. We find that carrier mobility is independent of the polydispersity of the NC samples, which can be understood if percolation networks of the larger-diameter, smaller-band-gap NCs carry most of the current in these NC solids. Our results establish a baseline for mobility trends in PbSe NC solids, with implications for fabricating high-mobility NC-based optoelectronic devices.

Iron pyrite (FeS2) is a promising earth-abundant semiconductor for thin-film solar cells. In this work, phase-pure, single-crystalline, and well-dispersed colloidal FeS2 nanocrystals (NCs) were synthesized in high yield by a simple hot-injection route in octadecylamine and then were subjected to partial ligand exchange with octadecylxanthate to yield stable pyrite NC inks. Polycrystalline pyrite thin films were fabricated by sintering layers of these NCs at 500−600 °C under a sulfur atmosphere.

The band edge optical characterization of solution-synthesized CdS nanowires (NWs) is described. Investigated wires are made through a solution−liquid–solid approach that entails the use of low-melting bimetallic catalyst particles to seed NW growth. Resulting diameters are approximately 14 nm, and lengths exceed 1 µm. Ensemble diameter distributions are ∼13%, with corresponding intrawire diameter variations of ∼5%. High-resolution transmission electron micrographs show that the wires are highly crystalline and have the wurtzite structure with growth along at least two directions: [0001] and [101̅0]. Band edge emission is observed with estimated quantum yields between ∼0.05% and 1%. Complementary photoluminescence excitation spectra show structure consistent with the linear absorption. Carrier cooling dynamics are subsequently examined through ensemble lifetime and transient differential absorption measurements. The former reveals unexpectedly long band edge decays that extend beyond tens of nanoseconds. The latter indicates rapid intraband carrier cooling on time scales of 300–400 fs. Subsequent recovery at the band edge contains significant Auger contributions at high intensities which are usurped by other, possibly surface-related, carrier relaxation pathways at lower intensities. Furthermore, an unusual intensity-dependent transient broadening is seen, connected with these long decays. The effect likely stems from band-filling on the basis of an analysis of observed spectral shifts and line widths.

We demonstrate the solution-phase synthesis of CdS/CdSe, CdSe/CdS, and CdSe/ZnTe core/shell nanowires (NWs). On the basis of bulk band offsets, type-I and type-II heterostructures are made, contributing to the further development of low-dimensional heteroassemblies using solution-phase chemistry. Core/shell wires are prepared by slowly introducing shell precursors into a solution of premade core NWs dispersed in a noncoordinating solvent at moderate temperatures (215-250 degrees C). Resulting heterostructures are characterized through low- and high-resolution transmission electron microscopy, selected area electron diffraction, and energy dispersive X-ray analysis. From these experiments, initial shell growth appears to occur through either Stranski-Krastanov or Volmer-Weber island growth. However, beyond a critical shell thickness, nucleation of randomly oriented nanocrystals results in a polycrystalline coat. In cases where overcoating has been achieved, corresponding elemental analyses show spatially varying compositions along the NW radial direction in agreement with expected element ratios. Electronic interactions between the core and shell were subsequently probed through optical studies involving UV-vis extinction spectroscopy, photoluminescence experiments, and transient differential absorption spectroscopy. In particular, transient differential absorption studies reveal unexpected shell-induced changes in core NW Auger kinetics at high carrier densities. Previously seen three-carrier Auger kinetics in CdS (bimolecular in CdSe) NWs were suppressed by the presence of a CdSe (CdS) shell. These observations suggest the ability to influence NW optical/electrical properties by coating them with a surrounding shell, a method which could be important for future NW optical studies as well as for NW-based applications.