University of Limerick
Browse

Localization-limited exciton oscillator strength in colloidal CdSe nanoplatelets revealed by the optically induced stark effect

Download (1.09 MB)
journal contribution
posted on 2021-08-17, 14:27 authored by Pieter Geiregat, Carmelita Rodá, Ivo Tanghe, Shalini SinghShalini Singh, Alessio Di Giacomo, Delphine Lebrun, Gianluca Grimaldi, Jorick Maes, Dries Van Thourhout, Iwan Moreels, Arjan J. Houtepen, Zeger Hens
2D materials are considered for applications that require strong light-matter interaction because of the apparently giant oscillator strength of the exciton transitions in the absorbance spectrum. Nevertheless, the effective oscillator strengths of these transitions have been scarcely reported, nor is there a consistent interpretation of the obtained values. Here, we analyse the transition dipole moment and the ensuing oscillator strength of the exciton transition in 2D CdSe nanoplatelets by means of the optically induced Stark effect (OSE). Intriguingly, we find that the exciton absorption line reacts to a high intensity optical field as a transition with an oscillator strength FStark that is 50 times smaller than expected based on the linear absorption coefficient. We propose that the pronounced exciton absorption line should be seen as the sum of multiple, low oscillator strength transitions, rather than a single high oscillator strength one, a feat we assign to strong exciton center-of-mass localization. Within the quantum mechanical description of excitons, this 50-fold difference between both oscillator strengths corresponds to the ratio between the coherence area of the exciton’s center of mass and the total area, which yields a coherence area of a mere 6.1 nm2 . Since we find that the coherence area increases with reducing temperature, we conclude that thermal effects, related to lattice vibrations, contribute to exciton localization. In further support of this localization model, we show that FStark is independent of the nanoplatelet area, correctly predicts the radiative lifetime, and lines up for strongly confined quantum dot systems.

Funding

A Study of Advection and Dispersion in the Eastern North Atlantic

Directorate for Geosciences

Find out more...

Study on Aerodynamic Characteristics Control of Slender Body Using Active Flow Control Technique

Japan Society for the Promotion of Science

Find out more...

The works of Daniel Bernoulli, Volume 5: Hydrodynamics II

Swiss National Science Foundation

Find out more...

History

Publication

Light: Science and Applications;10, 112

Publisher

Springer

Note

peer-reviewed

Other Funding information

FWO-Vlaanderen, Research Foundation Flanders, Belgium, ERC, Horizon 2020

Language

English

Usage metrics

    University of Limerick

    Categories

    No categories selected

    Exports

    RefWorks
    BibTeX
    Ref. manager
    Endnote
    DataCite
    NLM
    DC