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Register a new userCharge transport in arrays of PbSe nanocrystals
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We report electrical transport measurements of arrays of PbSe nanocrystals forming the channels of field effect transistors. We measure the current in these devices as a function of source-drain voltage, gate voltage and temperature. Annealing is necessary to observe measurable current after which a simple model of hopping between intrinsic localized states describes the transport properties of the nanocrystal solid. We find that the majority carriers are holes, which are thermally released from acceptor states. At low source-drain voltages, the activation energy for the conductivity is given by the energy required to generate holes plus the activation over barriers resulting from site disorder. At high source-drain voltages the activation energy is given by the former only. The thermal activation energy of the zero-bias conductance indicates that the Fermi energy is close to the highest-occupied valence level, the 1Sh state, and this is confirmed by field-effect measurements, which give a density of states of approximately eight per nanocrystal as expected from the degeneracy of the 1Sh state.
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Positron annihilation lifetime spectroscopy (PALS) and positron-electron momentum density (PEMD) studies on multilayers of PbSe nanocrystals (NCs), supported by transmission electron microscopy (TEM), show that positrons are strongly trapped at NC surfaces, where they provide insight into the surface composition and electronic structure of PbSe NCs. Our analysis indicates abundant annihilation of positrons with Se electrons at the NC surfaces and with O electrons of the oleic ligands bound to Pb ad-atoms at the NC surfaces, which demonstrates that positrons can be used as a sensitive probe to investigate the surface physics and chemistry of nanocrystals inside multilayers. Ab-initio electronic structure calculations provide detailed insight in the valence and semi-core electron contributions to the positron-electron momentum density of PbSe. Both lifetime and PEMD are found to correlate with changes in the particle morphology characteristic of partial ligand removal.
The potential of semiconductors assembled from nanocrystals (NC semiconductors) has been demonstrated for a broad array of electronic and optoelectronic devices, including transistors, light emitting diodes, solar cells, photodetectors, thermoelectrics, and phase charge memory cells. Despite the commercial success of nanocrystals as optical absorbers and emitters, applications involving charge transport through NC semiconductors have eluded exploitation due to the inability for predictive control of their electronic properties. Here, we perform large-scale, ab-initio simulations to understand carrier transport, generation, and trapping in NC-based semiconductors from first principles. We use these findings to build the first predictive model for charge transport in NC semiconductors, which we validate experimentally. Our work reveals that we have been thinking about transport in NC semiconductors incorrectly. Our new insights provide a path for systematic engineering of NC semiconductors, which in fact offer previously unexplored opportunities for tunability not achievable in other semiconductor systems.
We present a theory for carrier transport in semiconducting nanoscale heterostructures that emphasizes the effects of strain at the interface between two different crystal structures. An exactly solvable model shows that the interface region, or junction, acts as a scattering potential that facilitates charge separation but also supports bound interfacial states. As a case study, we model a Type-II CdS/ZnSe heterostructure. After advancing a theory similar to that employed in model molecular conductance calculations, we calculate the electron and hole photocurrents and conductances, including non-linear effects, through the junction at steady-state.
We report electron transport measurements through nano-scale devices consisting of 1 to 3 Prussian blue analog (PBA) nanocrystals connected between two electrodes. We compare two types of cubic nanocrystals, CsCoFe (15 nm) and CsNiCr (6 nm), deposited on highly oriented pyrolytic graphite and contacted by conducting-AFM. The measured currents show an exponential dependence with the length of the PBA nano-device (up to 45 nm), with low decay factors b{eta}, in the range 0.11 - 0.18 nm-1 and 0.25 - 0.34 nm-1 for the CsCoFe and the CsNiCr nanocrystals, respectively. From the theoretical analysis of the current-voltage curve for the nano-scale device made of a single nanoparticle, we deduce that the electron transport is mediated by the localized d bands at around 0.5 eV from the electrode Fermi energy in the two cases. By comparison with previously reported ab-initio calculations, we tentatively identify the involved orbitals as the filled Fe(II)-t2g d band (HOMO) for CsCoFe and the half-filled Ni(II)-eg d band (SOMO) for CsNiCr. Conductance values measured for multi-nanoparticle nano-scale devices (2 and 3 nanocrystals between the electrodes) are consistent with a multi-step coherent tunneling in the off-resonance regime between adjacent PBAs, a simple model gives a strong coupling (around 0.1 - 0.25 eV) between the adjacent PBA nanocrystals, mediated by electrostatic interactions.
We have developed a quantitative theory of Cooper pair pumping in gated one-dimensional arrays of Josephson junctions. The pumping accuracy is limited by quantum tunneling of Cooper pairs out of the propagating potential well and by direct supercurrent flow through the array. Both corrections decrease exponentially with the number N of junctions in the array, but give a serious limitation of accuracy for any practical array. The supercurrent at resonant gate voltages decreases with N only as sin(v/N)/N, where v is the Josephson phase difference across the array.
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