Brodu Annalisa, Chandrasekaran Vigneshwaran, Scarpelli Lorenzo, Buhot Jonathan, Masia Francesco, Ballottin Mariana V, Severijnen Marion, Tessier Mickaël D, Dupont Dorian, Rabouw Freddy T, Christianen Peter C M, de Mello Donega Celso, Vanmaekelbergh Daniël, Langbein Wolfgang, Hens Zeger
Debye Institute for Nanomaterials Science , Utrecht University , 3584 CC Utrecht , The Netherlands.
Physics and Chemistry of Nanostructures , Ghent University , 9000 Ghent , Belgium.
J Phys Chem Lett. 2019 Sep 19;10(18):5468-5475. doi: 10.1021/acs.jpclett.9b01824. Epub 2019 Sep 3.
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 = 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.
胶体量子点(QDs)中激子态的精细结构是由各向异性和电子-空穴交换的复合效应产生的。通过单量子点光致发光光谱,我们表明光激发的InP/ZnSe量子点的发射源于这种精细结构激子态的辐射复合。根据激发功率,我们识别出一个明亮的激子双峰、一个三重态单重态和一个双激子双峰线,它们都表现出明显的极化。InP/ZnSe量子点集合在磁场中的荧光线窄化光谱表明,明亮激子实际上由三个态组成。这些态的塞曼分裂可以用各向同性激子模型很好地描述,其中精细结构由电子-空穴交换主导,形状各向异性仅导致J = 1三重态的微小分裂。我们认为基于InP的量子点中的激子几乎是各向同性的,因为InP中轻、重空穴质量的特定比例使得激子精细结构对形状各向异性不敏感。