American Chemical Society
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Fine Structure of Nearly Isotropic Bright Excitons in InP/ZnSe Colloidal Quantum Dots

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journal contribution
posted on 2019-09-03, 17:19 authored by Annalisa Brodu, Vigneshwaran Chandrasekaran, Lorenzo Scarpelli, Jonathan Buhot, Francesco Masia, Mariana V. Ballottin, Marion Severijnen, Mickaël D. Tessier, Dorian Dupont, Freddy T. Rabouw, Peter C. M. Christianen, Celso de Mello Donega, Daniël Vanmaekelbergh, Wolfgang Langbein, Zeger Hens
The fine structure of exciton states in colloidal quantum dots (QDs) results from the compound effect of anisotropy and electron–hole exchange. By means of single-dot photoluminescence spectroscopy, we show that the emission of photoexcited InP/ZnSe QDs originates from radiative recombination of such fine structure exciton states. Depending on the excitation power, we identify a bright exciton doublet, a trion singlet, and a biexciton doublet line that all show pronounced polarization. Fluorescence line narrowing spectra of an ensemble of InP/ZnSe QDs in magnetic fields demonstrate that the bright exciton effectively consists of three states. The Zeeman splitting of these states is well described by an isotropic exciton model, where the fine structure is dominated by electron–hole exchange and shape anisotropy leads to only a minor splitting of the F = 1 triplet. We argue that excitons in InP-based QDs are nearly isotropic because the particular ratio of light and heavy hole masses in InP makes the exciton fine structure insensitive to shape anisotropy.