posted on 2021-08-17, 14:27authored byPieter 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