As the properties of a semiconductor material depend on the fate of the excitons, manipulating exciton behavior is the primary objective of nanomaterials. Although nanocrystals exhibit unusual excitonic characteristics owing to strong spatial confinement, studying the interactions between excitons in a single nanoparticle remains challenging due to the rapidly vanishing multiexciton species. Here, a platform for exciton tailoring using a straightforward strategy of shape-tuning of single-crystalline nanocrystals is presented. Spectroscopic and theoretical studies reveal a systematic transition of exciton confinement orientation from 3D to 2D, which is solely tuned by the geometric shape of material. Such a precise shape-effect triggers a multiphoton emission in single nanotetrapods with arms longer than the exciton Bohr radius of material. In consequence, the unique interplay between the multiple quantum states allows a geometric modulation of the quantum-confined Stark effect and nanocrystal memory effect in single nanotetrapods. These results provide a useful metric in designing nanomaterials for future photonic applications.
Keywords: exciton confinement; exciton-exciton interactions; multiphoton emission; nanotetrapods; single-crystalline tetrapods; single-dot spectroscopy; time-resolved spectroscopy.
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