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Influence of Surfactants and Charges on CdSe Quantum Dots

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Abstract

Surface effects significantly influence the functionality of semiconductor nanocrystals. High quality nanocrystals can be achieved with good control of surface passivation by various hydrophobic ligands. In this work, the chemistry between CdSe quantum dots and common surface capping ligands is investigated using density functional theory (DFT). We discuss the electronic structures and optical properties of small CdSe clusters controlled by their size of particle, self-organization, capping ligands, and positive charges. The chosen model ligands reproduce good structural and energetic description of the interactions between the ligands and quantum dots. In order to capture the chemical nature and energetics of the interactions between the capping ligands and CdSe quantum dots, we found that PMe3 is needed to adequately model trioctylphosphine (TOP), NH3 is sufficient for amines, while OPH2Me could be used to model trioctylphosphine oxide. The relative binding interaction strength between ligands was found to decrease in order Cd–O > Cd–N > Cd–P with average binding energy per ligand being −25 kcal/mol for OPH2Me, −20 kcal/mol for NH3 and −10 kcal/mol for PMe3. Charges on studied stoichiometric clusters were found to have a significant effect on their structures, binding energies, and optical properties.

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Acknowledgments

PY acknowledges support from Environmental Molecular Sciences Laboratory (a national scientific user facility sponsored by the U.S. Department of Energy’s Office of Biological and Environmental Research) located at Pacific North-west National Laboratory and operated for the DOE by Battelle. ST acknowledges support of the Center for Advanced Solar Photophysics (CASP), an Energy Frontier Research Center funded by the U.S. Department of Energy (DOE). We acknowledge support of Center for Integrated Nanotechnology (CINT) and Center for Nonlinear Studies (CNLS). Los Alamos National Laboratory is operated by Los Alamos National Security, LLC, for the National Nuclear Security Administration of the U.S. Department of Energy under contract DE-AC52-06NA25396.

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  1. Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, 902 Battlelle Boulevard, Richland, WA, 99352, USA

    Ping Yang

  2. Center for Integrated Nanotechnologies (CINT), Los Alamos National Laboratory, Los Alamos, NM, 87545, USA

    Sergei Tretiak & Sergei Ivanov

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  1. Ping Yang
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Yang, P., Tretiak, S. & Ivanov, S. Influence of Surfactants and Charges on CdSe Quantum Dots. J Clust Sci 22, 405–431 (2011). https://doi.org/10.1007/s10876-011-0398-y

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