We present a photocurrent study of CdSe quantum dot films exhibiting unity internal quantum efficiency as a result of post-deposition treatments. While the photocurrent of untreated films is highly voltage dependent at all voltages, the treated films depend strongly on voltage at low voltage, linearly with voltage above a voltage threshold, and finally saturate at high voltage. The voltage dependence of the treated films can be reproduced with a model assuming blocking contacts and a field dependent exciton ionization efficiency that saturates to unity. The increase in exciton ionization efficiency is a result of increased surface passivation and decreased QD spacing.
Transport properties of artificial solids composed of colloidal CdSe nanocrystals (NCs) are studied from 6 K to 250 K, before and after annealing. Annealing results in greatly enhanced dark and photocurrent in NC solids, while transmission electron microscopy (TEM) micrographs show that the inter-dot separation decreases. The increased current can be attributed to the enhancement of inter-dot tunneling caused by the decreased separation between NCs and by chemical changes in their organic cap. In addition, the absorption spectra of annealed solids are slightly red-shifted and broadened. These redshifts may result from the change of the dielectric environment around the NCs. Our measurements also indicate that Coulomb interactions between charges on neighboring NCs play an important role in the tunneling current.
We present results for electronic transport measurements on large
three-dimensional arrays of CdSe nanocrystals. In response to a step in the
applied voltage, we observe a power-law decay of the current over five orders
of magnitude in time. Furthermore, we observe no steady-state dark current for
fields up to 10^6 V/cm and times as long as 2x10^4 seconds. Although the
power-law form of the decay is quite general, there are quantitative variations
with temperature, applied field, sample history, and the material parameters of
the array. Despite evidence that the charge injected into the film during the
measurement causes the decay of current, we find field-scaling of the current
at all times. The observation of extremely long-lived current transients
suggests the importance of long-range Coulomb interactions between charges on
different nanocrystals.Comment: 11 pages, 10 figure
A novel model of transport is proposed to explain power law current transients and memory phenomena observed in partially ordered arrays of semiconducting nanocrystals. The model describes electron transport by a stationary Lévy process of transmission events and thereby requires no time dependence of system properties. The waiting time distribution with a characteristic long tail gives rise to a nonstationary response in the presence of a voltage pulse. We report on noise measurements that agree well with the predicted non-Poissonian fluctuations in current, and discuss possible mechanisms leading to this behavior.
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