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Efficient Inverse Auger Recombination at Threshold in CdSe Nanocrystals

TLDR
In this article, the authors apply the semi-empirical nonlocal pseudopotential method to the investigation of prospects for direct carrier multiplication (DCM) in neutral and negatively charged CdSe nanocrystals.
Abstract
We apply the semiempirical nonlocal pseudopotential method to the investigation of prospects for direct carrier multiplication (DCM) in neutral and negatively charged CdSe nanocrystals In this process, known in the bulk as impact ionization, a highly excited carrier transfers, upon relaxation to the band edge, its excess energy Δ to a valence electron, promoting it across the band gap and thus creating two excitons from one For excess energies just a few meV above the energy gap Eg (the DCM threshold), we find the following: (i) DCM is much more efficient in quantum dots than in bulk materials, with rates of the order of 1010 s-1 In conventional bulk solids, comparable rates are obtained only for excess energies about 1 eV above Eg (ii) Unlike the case in the bulk, in both neutral and charged nanocrystals the DCM rate is not an increasing function of the excess energy but oscillates as Δ moves in and out of resonance with the energy of the discrete spectrum of these 0D systems, (iii) The main contribution to the DCM rates is found to come from the dot surface, as in the case of Auger multiexciton recombination rates, (iv) Direct radiative recombination of excited electron-hole pairs and phonon-assisted decay are slower than DCM, but (v) the rate of Auger cooling (where the relaxation energy of an excited electron is used to excite a hole into deeper levels) can be of the same order of magnitude as that of the DCM process Furthermore, for excess energies well above the DCM threshold, the presence of an energy gap within the hole manifold considerably slows DCM compared to Auger cooling (AC), which is not affected by it Achieving competitive DCM processes will, therefore, require the suppression of Auger cooling, for example, by removing the hole from the dot or by trapping it at the surface

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eprints@whiterose.ac.uk
Universities of Leeds, Sheffield and York
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This is the author’s version of an article published in Nano Letters
White Rose Research Online URL for this paper:
http://eprints.whiterose.ac.uk/id/eprint/75642
Published article:
Califano, M, Zunger, A and Franceschetti, A (2004) Efficient inverse Auger
recombination at threshold in CdSe nanocrystals. Nano Letters, 4 (3). 525 - 531 .
ISSN 1530-6984
http://dx.doi.org/10.1021/nl049869w

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Citations
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Journal ArticleDOI

Quantum Dot Solar Cells. Semiconductor Nanocrystals as Light Harvesters

TL;DR: In this paper, three major ways to utilize semiconductor dots in solar cell include (i) metal−semiconductor or Schottky junction photovoltaic cell, (ii) polymer−smiconductor hybrid solar cell, and (iii) quantum dot sensitized solar cell.
Journal ArticleDOI

Meeting the Clean Energy Demand: Nanostructure Architectures for Solar Energy Conversion

TL;DR: In this article, three major ways to utilize nanostructures for the design of solar energy conversion devices are discussed: (i) mimicking photosynthesis with donor−acceptor molecular assemblies or clusters, (ii) semiconductor assisted photocatalysis to produce fuels such as hydrogen, and (iii) nanostructure semiconductor based solar cells.
Journal ArticleDOI

Quantum dot solar cells. harvesting light energy with CdSe nanocrystals molecularly linked to mesoscopic TiO2 films.

TL;DR: By using bifunctional surface modifiers (SH-R-COOH), CdSe quantum dots (QDs) have been assembled onto mesoscopic TiO(2) films and exhibits a photon-to-charge carrier generation efficiency of 12%.
Journal ArticleDOI

Quantum Dot Solar Cells. Tuning Photoresponse through Size and Shape Control of CdSe−TiO2 Architecture

TL;DR: Two major findings are highlighted: ability to tune the photoelectrochemical response and photoconversion efficiency via size control of CdSe quantum dots and improvement in the photoconversions efficiency by facilitating the charge transport through TiO2 nanotube architecture.
Journal ArticleDOI

Spectral and Dynamical Properties of Multiexcitons in Semiconductor Nanocrystals

TL;DR: The specific topics discussed here include the structure of NC electronic states, spectral signatures of multiexcitons in transient absorption and photoluminescence, exciton-exciton interaction energies, Auger recombination, and carrier multiplication.
References
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Journal ArticleDOI

Detailed Balance Limit of Efficiency of p‐n Junction Solar Cells

TL;DR: In this article, an upper theoretical limit for the efficiency of p−n junction solar energy converters, called the detailed balance limit of efficiency, has been calculated for an ideal case in which the only recombination mechanism of holeelectron pairs is radiative as required by the principle of detailed balance.
Journal ArticleDOI

Synthesis and characterization of nearly monodisperse CdE (E = sulfur, selenium, tellurium) semiconductor nanocrystallites

TL;DR: In this paper, a simple route to the production of high-quality CdE (E=S, Se, Te) semiconductor nanocrystallites is presented, based on pyrolysis of organometallic reagents by injection into a hot coordinating solvent.
Journal ArticleDOI

Quantum dot solar cells

TL;DR: In this article, three QD solar cell configurations are described: (1) photoelectrodes comprising QD arrays, (2) QD-sensitized nanocrystalline TiO 2, and (3) QDs dispersed in a blend of electron- and hole-conducting polymers.
Journal ArticleDOI

Quantization of multiparticle auger rates in semiconductor quantum dots

TL;DR: It is observed that in the quantum-confined regime, the Auger constant is strongly size-dependent and decreases with decreasing the quantum dot size as the radius cubed.
Journal ArticleDOI

Bandgap Dependence and Related Features of Radiation Ionization Energies in Semiconductors

TL;DR: In this article, the authors developed a simple phenomenological model capable of describing the present experimental situation from the standpoint of yield, variance, and bandgap dependence, based on the premise that e, the average amount of radiation energy consumed per pair, can be accounted for by a sum of three contributions: the intrinsic bandgap (EG), optical phonon losses r(ℏωR), and the residual kinetic energy (9/5) EG.
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