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Arjan J Houtepen

Publications and source records attributed to Arjan J Houtepen.

3 recordsLinked to original sources

The hidden role of acetate in the PbSe nanocrystal synthesis.

Monodisperse spherical, star-shaped, and octahedral PbSe nanocrystals were synthesized via a hot injection method. We show that the shape and size of the colloidal PbSe nanocrystals are determined by the concentration of acetate and that only acetate-free reaction mixtures result in spherical nanocrystals. The presence of acetate leads to efficient oriented attachment of smaller PbSe nanoparticles along the 100 crystal axis. Comparing different synthesis procedures from the recent literature with our observations, we propose that the acetate, naturally present in insufficiently dried reaction mixtures, is responsible for many of the PbSe crystal shapes reported in the literature. In addition we show that it is possible to synthesize these star-shaped nanocrystals so monodisperse that they form ordered monolayers with crystal alignment.

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Orbital occupation in electron-charged CdSe quantum-dot solids.

We have prepared high-quality assemblies of monodisperse CdSe quantum dots and employed a combination of electrochemical gating and electrical and optical techniques to study orbital occupation in these quantum-dot solids. Electron occupation in localized states is important in some cases and can be unambiguously distinguished from occupation of the nanocrystal eigenstates. In addition, all excitonic transitions show a red-shift in the transition energy, due to the presence of electron charge. We infer that the energy of the S electrons is determined by the quantum-confinement energy and by Coulomb repulsions of the S electron with all other electrons in the assembly. By using a simple electron-repulsion model, we explain observed differences in the electron-addition energy for different samples, the broadening of the electron occupation as a function of electrochemical potential, and the strong dependence of the electron-addition energy on nanocrystal diameter.

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Electron-conducting quantum-dot solids with ionic charge compensation.

Electron-conducting quantum-dot solids can be prepared on the basis of assemblies of colloidal insulating nanocrystals if electrons can be injected in the delocalized conduction orbitals. We discuss the energetics of electron injection in such an artificial solid consisting of weakly coupled quantum dots. We show that quantum confinement and electron electron repulsion determine the charging characteristics. The electron electron repulsion energy can be screened by three-dimensional charge compensation from trapped holes or positive inert ions inserted in the assembly. We present experimental results on the electron storage and long-range transport in assemblies of ZnO nanocrystals in which the electron charge is compensated by positive ions. The electron electron repulsion energy in assemblies permeated with an aqueous electrolyte solution is strongly screened. In contrast, the repulsion energy is about 100 meV in aprotic solvents; the repulsion energy strongly influences electron storage and the characteristics of long-range electron transport.

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