Electron-hole correlations govern Auger recombination in nanostructures

Abstract

The fast nonradiative decay of multiexcitonic states via Auger recombination is a fundamental process affecting a variety of applications based on semiconductor nanostructures. From a theoretical perspective, the description of Auger recombination in confined semiconductor nanostructures is a challenging task due to the large number of valance electrons and exponentially growing number of excited excitonic and biexcitonic states that are coupled by the Coulomb interaction. These challenges have restricted the treatment of Auger recombination to simple, noninteracting electron-hole models. Herein we present a novel approach for calculating Auger recombination lifetimes in confined nanostructures having thousands to tens of thousands of electrons, explicitly including electron-hole interactions. We demonstrate that the inclusion of electron-hole correlations are imperative to capture the correct scaling of the Auger recombination lifetime with the size and shape of the nanostructure. In addition, correlation effects are required to obtain quantitatively accurate lifetimes even for systems smaller than the exciton Bohr radius. Neglecting such correlations can result in lifetimes that are 2 orders of magnitude too long. We establish the utility of the new approach for CdSe quantum dots of varying sizes and for CdSe nanorods of varying diameters and lengths. Our new approach is the first theoretical method to postdict the experimentally known universal volume scaling law for quantum dots and makes novel predictions for the scaling of the Auger recombination lifetimes in nanorods.

References in corpus (7)

• 1D Exciton Spectroscopy of Semiconductor Nanorods
• The Electronic Structure of CdSe/CdS Core/Shell Seeded Nanorods: Type-I or Quasi-Type-II?
• A pseudopotential study of electron-hole excitations in colloidal, free-standing InAs quantum dots
• Theory of multiexciton generation in semiconductor nanocrystals
• Origins of singlet fission in solid pentacene from an ab initio Green's-function approach
• Theory of highly excited semiconductor nanostructures including Auger coupling: exciton-bi-exciton mixing in CdSe nanocrystals
• Biexciton generation rates in CdSe nanorods are length independent

Cited by in corpus (10)

• Electrical control of single-photon emission in highly-charged individual colloidal quantum dots
• Thickness-Dependence of Exciton-Exciton Annihilation in Halide Perovskite Nanoplatelets
• Simulations of nonradiative processes in semiconductor nanocrystals
• Nonadiabatic to Adiabatic Transition of Electron Transfer in Colloidal Quantum Dot Molecules
• Negative diffusion of excitons in quasi-two-dimensional systems
• Room temperature single-photon superfluorescence from a single epitaxial cuboid nano-heterostructure
• Ab Initio Modeling of Phonon-Assisted Relaxation of Electrons and Excitons in Semiconductor Nanocrystals for Multiexciton Generation
• Microscopic Theory of Exciton-Exciton Annihilation in Two-Dimensional Semiconductors
• Renormalization of excitonic properties by polar phonons
• Spin-Dependent Transport Through a Colloidal Quantum Dot: The Role of Exchange Interactions