Fast Electron and Slow Hole Relaxation in InP-Based Colloidal Quantum Dots.

Autor: Richter AF; Chair for Photonics and Optoelectronics, Nano-Institute Munich, Physics Department , Ludwig-Maximilians-Universität (LMU) , Königinstr. 10 , 80539 Munich , Germany., Binder M; Chair for Photonics and Optoelectronics, Nano-Institute Munich, Physics Department , Ludwig-Maximilians-Universität (LMU) , Königinstr. 10 , 80539 Munich , Germany., Bohn BJ; Chair for Photonics and Optoelectronics, Nano-Institute Munich, Physics Department , Ludwig-Maximilians-Universität (LMU) , Königinstr. 10 , 80539 Munich , Germany., Grumbach N; Merck KGaA , Frankfurter Str. 250 , 64293 Darmstadt , Germany., Neyshtadt S; Merck KGaA , Frankfurter Str. 250 , 64293 Darmstadt , Germany., Urban AS; Nanospectroscopy Group, Nano-Institute Munich, Physics Department , Ludwig-Maximilians-Universität (LMU) , Königinstr. 10 , 80539 Munich , Germany., Feldmann J; Chair for Photonics and Optoelectronics, Nano-Institute Munich, Physics Department , Ludwig-Maximilians-Universität (LMU) , Königinstr. 10 , 80539 Munich , Germany.
Jazyk: angličtina
Zdroj: ACS nano [ACS Nano] 2019 Dec 24; Vol. 13 (12), pp. 14408-14415. Date of Electronic Publication: 2019 Dec 10.
DOI: 10.1021/acsnano.9b07969
Abstrakt: Colloidal InP-based quantum dots are a promising material for light-emitting applications as an environment friendly alternative to their Cd-containing counterparts. Especially for their use in optoelectronic devices, it is essential to understand how charge carriers relax to the emitting state after injection with excess energy and if all of them arrive at this desired state. Herein, we report time-resolved differential transmission measurements on colloidal InP/ZnS and InP/ZnSe core/shell quantum dots. By optically exciting and probing individual transitions, we are able to distinguish between electron and hole relaxation. This, in turn, allows us to determine how the initial excess energy of the charge carriers affects the relaxation processes. According to the electronic level scheme, one expects a strong phonon bottleneck for electrons, whereas holes should relax easier as their energy levels are more closely spaced. On the contrary, we find that electrons relax faster than holes. The fast electron relaxation occurs via an efficient Auger-like electron-hole scattering mechanism. On the other hand, a small wave function overlap between core and shell states slows the hole relaxation. Additionally, holes can be trapped at the core/shell interface, leading to either slow detrapping or nonradiative recombination. Overall, these results demonstrate that it is crucial to construct devices enabling the injection of charge carriers energetically close to their emitting states in order to maximize the radiative efficiency of the system.
Databáze: MEDLINE