Quantifying Blinking Suppression and Probing Its Mechanism in PPD-Treated Single Quantum Dots

Abstract

Colloidal semiconductor quantum dots (QDs) are highly promising materials for various applications, yet photoluminescence intermittency (blinking) remains a key obstacle to their practical use. While recent advances have enabled partial or complete suppression of this effect, both the degree of suppression and the mechanism by which it occurs are often difficult to establish. In the present work we analyse the blinking suppression of single CdSe/ZnS QDs after treatment with p-phenylenediamine (PPD), recently discovered by Yang et al. We revisit the blinking mechanism in this system and show that it is governed predominantly by the trapping mechanism, rather than by Auger ionization as previously proposed. For data analysis we apply a threshold-free two-dimensional criterion recently proposed by Podshivaylov and Frantsuzov. The criterion is based on the relative quantum yield estimator $\langle \hat{Q} \rangle^{(s)}$ and the decay-rate fluctuation parameter $\hatξ$. We found that PPD treatment significantly increases the relative quantum yield and leads to only a modest increase in $\hatξ$, indicating that the dominant effect of PPD is to shift the distribution of the non-radiative recombination rate toward lower values, rather than to eliminate its fluctuations. We further suggest a number of possible mechanisms of PPD-induced suppression and propose critical experiments for their verification.