This talk describes the use of excited-state quantum chemistry techniques to investigate the intraband absorption of doped semiconductor nanoparticles as a function of doping density, nanoparticle radius, and material properties, where the excess electrons are modeled as interacting electrons confined to a sphere. The excitation evolves from single-particle to plasmonic with increasing number of electrons at fixed density, and the threshold number of electrons to produce a plasmon increases with density due to quantum confinement and electron–hole attraction. In addition, the excitation passes through an intermediate regime where it is best characterized as an intraband exciton. We compare equation-of- motion coupled-cluster theory with those of more affordable single-excitation theories and identify the inclusion of electron–hole interactions as essential to describing the evolution of the excitation. Despite the simplicity of the model, the results are in reasonable agreement with the experimental spectra of doped ZnO nanoparticles at a doping density of 1.4 × 10<sup>20</sup> cm<sup>−3</sup>.

Optical properties of doped quantum dots from quantum chemistry

ACS Spring Meeting 2021

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