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Ultrathin semiconductor nanocrystals (NCs) with at least one dimension belowtheir exciton Bohr radius receive a rapidly increasing attention due to theirunique physicochemical properties such as strong quantum confinement, largesurface-to-volume ratio, and giant oscillator strength. These superiorproperties highly depend on the shape and crystal phase of semiconductor NCs.Slight changes in the shape and phase of NCs can cause significant changes intheir properties. Therefore, it is crucial to controllably synthesizesemiconductor NCs. Here, we demonstrate not only the synthesis of robustwell-defined ultrathin ZnS nanoplatelets (NPLs) with excitonic absorption andemission, but also the precise shape and phase control of ZnS NCs based on asoft template strategy. The key feature of our approach is the tuning of thesulfur precursor amount, resulting in a simultaneous shape/phase transformationbetween wurtzite (WZ) ZnS NPLs and zinc blende (ZB) ZnS nanorods (NRs) atmoderate temperatures (150 degree). UV-vis absorption and photoluminescence(PL) spectra reveal very distinct optical properties between WZ-ZnS NPLs andZB-ZnS NRs. UV-vis absorption spectra of WZ-ZnS NPLs clearly exhibit a sharpexcitonic peak that is not observed in ZB-ZnS NRs. Besides, the PLcharacterization shows that WZ-ZnS NPLs have a narrow excitonic emission peak(292 nm), while the ZB-ZnS NRs exhibit a broad collective emission bandconsisting of four emission peaks (335, 359, 395, and 468 nm). The appearanceof excitonic features in the absorption spectra of ZnS NPLs is explained byinterband electronic transitions, which is simulated in the framework ofdensity functional theory (DFT). The presented simple and effective syntheticstrategy opens a new path to synthesize further NCs with shape and phasecontrol for advanced applications in electronics and photonics.

From wurtzite nanoplatelets to zinc blende nanorods: Simultaneous control of shape and phase in ultrathin ZnS nanocrystals