Searcharxiv⌕ Search

arXiv subjects

Uwe R. Kortshagen

Publications and source records attributed to Uwe R. Kortshagen.

4 recordsLinked to original sources

ZnO Nanocrystal Networks Near the Insulator-Metal Transition: Tuning Contact Radius and Electron Density with Intense Pulsed Light

Networks of ligand-free semiconductor nanocrystals (NCs) offer a valuable combination of high carrier mobility and optoelectronic properties tunable via quantum confinement. In principle, maximizing carrier mobility entails crossing the insulator-metal transition (IMT), where carriers become delocalized. A recent theoretical study predicted that this transition occurs at nρ^3 ~ 0.3, where n is the carrier density and ρis the interparticle contact radius. In this work, we satisfy this criterion in networks of plasma-synthesized ZnO NCs by using intense pulsed light (IPL) annealing to tune n and ρindependently. IPL applied to as-deposited NCs increases ρby inducing sintering, and IPL applied after the NCs are coated with Al2O3 by atomic layer deposition increases n by removing electron-trapping surface hydroxyls. This procedure does not substantially alter NC size or composition and is potentially applicable to a wide variety of nanomaterials. As we increase nρ^3 to at least twice the predicted critical value, we observe conductivity scaling consistent with arrival at the critical region of a continuous quantum phase transition. This allows us to determine the critical behavior of the dielectric constant and electron localization length at the IMT. However, our samples remain on the insulating side of the critical region, which suggests that the critical value of nρ^3 may in fact be significantly higher than 0.3.

cond-mat.mtrl-sci↗

Tuning Nanocrystal Surface Depletion by Controlling Dopant Distribution as a Route Toward Enhanced Film Conductivity

Electron conduction through bare metal oxide nanocrystal (NC) films is hindered by surface depletion regions resulting from the presence of surface states. We control the radial dopant distribution in tin-doped indium oxide (ITO) NCs as a means to manipulate the NC depletion width. We find in films of ITO NCs of equal overall dopant concentration that those with dopant-enriched surfaces show decreased depletion width and increased conductivity. Variable temperature conductivity data shows electron localization length increases and associated depletion width decreases monotonically with increased density of dopants near the NC surface. We calculate band profiles for NCs of differing radial dopant distributions and, in agreement with variable temperature conductivity fits, find NCs with dopant-enriched surfaces have narrower depletion widths and longer localization lengths than those with dopant-enriched cores. Following amelioration of NC surface depletion by atomic layer deposition of alumina, all films of equal overall dopant concentration have similar conductivity. Variable temperature conductivity measurements on alumina-capped films indicate all films behave as granular metals. Herein, we conclude that dopant-enriched surfaces decrease the near-surface depletion region, which directly increases the electron localization length and conductivity of NC films.

cond-mat.mes-hall↗

Metal-insulator transition in films of doped semiconductor nanocrystals

To fully deploy the potential of semiconductor nanocrystal films as low-cost electronic materials, a better understanding of the amount of dopants required to make their conductivity metallic is needed. In bulk semiconductors, the critical concentration of electrons at the metal-insulator transition is described by the Mott criterion. Here, we theoretically derive the critical concentration $n_c$ for films of heavily doped nanocrystals devoid of ligands at their surface and in direct contact with each other. In the accompanying experiments, we investigate the conduction mechanism in films of phosphorus-doped, ligand-free silicon nanocrystals. At the largest electron concentration achieved in our samples, which is half the predicted $n_c$, we find that the localization length of hopping electrons is close to three times the nanocrystals diameter, indicating that the film approaches the metal-insulator transition.

cond-mat.mes-hall↗

Carrier Transport in Films of Alkyl-Ligand-Terminated Silicon Nanocrystals

Silicon nanocrystals (Si NCs) have shown great promise for electroluminescent and photoluminescent applications. In order to optimize the properties of Si NC devices, however, electronic transport in Si NCs films needs to be thoroughly understood. Here we present a systematic study of the temperature and electric field dependence of conductivity in films of alkyl-ligand-terminated Si NCs, which to date have shown the highest potential for device applications. Our measurements suggest that the conductivity is limited by the ionization of rare NCs containing donor impurities. At low bias, this ionization is thermally activated, with an ionization energy equal to twice the NC charging energy. As the bias is increased, the ionization energy is reduced by the electric field, as determined by the Poole-Frenkel effect. At large bias and sufficiently low temperature, we observe cold ionization of electrons from donor-containing NCs, with a characteristic tunneling length of about 1 nm. The temperature- and electric-field-dependent conductance measurements presented here provide a systematic and comprehensive picture for electron transport in lightly doped nanocrystal films.

cond-mat.mes-hall↗