Theoretical characterisation of spheroidal PbSe/PbS Core/Shell colloidal quantum dot heterostructures

Walsh, TM 2016, Theoretical characterisation of spheroidal PbSe/PbS Core/Shell colloidal quantum dot heterostructures , PhD thesis, University of Salford.

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Abstract

Nanocrystal quantum dots (NQDs) show great promise in the advancement of the field of photovoltaics. While the maximum efficiency of conventional solar cell (SC) devices is limited to ∼ 31% (Shockley-Queisser limit), devices based on NQDs may attain a maximal thermodynamic efficiency of 42% through the exploitation of multiple exciton generation (MEG). In this process, several electron- hole pairs are created by the absorption of a single high energy photon, as opposed to the single excitons created in conventional solar cell devices. IV-VI semiconductor nanocrystals (PbS, PbSe) are of particular interest as candidates for the exploitation of MEG due to the narrow band gap, high confinement energies, and long radiative carrier lifetimes observed in these systems. In order to realise the full potential of MEG devices, full characterisation of the optoelectronic properties of the underlying nanoparticles is desirable. While the size-dependent properties of NQDs are well understood, the effects of NQD shape are less so. This thesis investigates the effect of ellipticity on the optoelectronic properties associated with spheroidal NQDs. To this end, a four-band, anisotropic, and radially variant k · p system Hamiltonian is expanded in a planewave basis in order to calculate single-particle eigenenergies and eigenfunctions of colloidal PbSe/PbS core/shell heterogeneous NQDs of varying ellipticity. Many-body effects are accounted for via a full configuration interaction (CI) Hamiltonian, the basis of which is comprised of the single-particle states. Exci- tonic and bi-excitonic corrections are then found by mixing of the basis states. In this manner, such diverse electronic and optical properties as quasi-particle binding energies, momentum matrix elements, and charge carrier lifetimes, both radiative and non-radiative, may be predicted.

Item Type: Thesis (PhD)
Schools: Schools > School of Computing, Science and Engineering
Funders: Engineering and Physical Sciences Research Council (EPSRC)
Depositing User: Thomas Mathew Walsh
Date Deposited: 11 Jan 2018 13:45
Last Modified: 11 Jan 2018 13:45
URI: http://usir.salford.ac.uk/id/eprint/41075

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