Nature and Control of Shakeup Processes in Colloidal Nanoplatelets
Jordi Llusar a, Juan Ignacio Climente a
a Departament de Química Física i Analítica, Universitat Jaume I, Av. Vicent Sos Baynat, s/n, Castellón de la Plana, Spain
Proceedings of Internet NanoGe Conference on Nanocrystals (iNCNC)
Online, Spain, 2021 June 28th - July 2nd
Organizers: Maksym Kovalenko, Maria Ibáñez, Peter Reiss and Quinten Akkerman
Oral, Jordi Llusar, presentation 016
DOI: https://doi.org/10.29363/nanoge.incnc.2021.016
Publication date: 8th June 2021

To improve their quantum yield and stability, metal chalcogenide nanoplatelets (NPLs) are often synthesized as core-shell or core-crown heterostructures. Unfortunately, in doing so the emission linewidth becomes broad and asymmetric. The asymmetric linewidth has been recently ascribed to shakeup processes, a partly radiative Auger process [1,2]. Strategies are then needed for the narrowing of the emission linewidth on these colloidal materials.

In this work [3], we supply a theoretical point of view about shakeup processes in order to assess on the origin of the multi-peak emission observed on Refs [2,3}. Besides, we suggest strategies that would allow minimization of such peaks, therefore reducing the emission linewidth. The conclusions we obtain are:

(1) Shakeup processes are expected in colloidal NPLs charged with trions, unlike in strongly confined nanocrystals. Since Coulomb interactions are considerably strong one could expect sizeable radiative Auger processes.

(2) Off-centred impurities [4], reducing the system symmetry, are needed to observe shakeup processes in NPLs. This result allows us to connect the apparently different interpretations of the broadening reported in Refs [2,5], namely surface defects or shakeup processes.

(3) Multi-peaked emission in CdSe/CdS NPLs [2] cannot be explained by shakeup processes only. Therefore, we propose an alternative interpretation involving emission peaks from metastable spin triplet trion states.

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