As an essential candidate for environment-friendly luminescent quantum dots(QDs),CuInS-based QDs have attracted more attention in recent years.However,several drawbacks still hamper their industrial applications,such ...As an essential candidate for environment-friendly luminescent quantum dots(QDs),CuInS-based QDs have attracted more attention in recent years.However,several drawbacks still hamper their industrial applications,such as lower photoluminescence quantum yield(PLQY),complex synthetic pathways,uncontrollable emission spectra,and insufficient photostability.In this study,CuInZnS@ZnS core/shell QDs was prepared via a one-pot/three-step synthetic scheme with accurate and tunable control of PL spectra.Then their ensemble spectroscopic properties during nucleation formation,alloying,and ZnS shell growth processes were systematically investigated.PL peaks of these QDs can be precisely manipulated from 530 to 850 nm by controlling the stoichiometric ratio of Cu/In,Zn^(2+)doping and ZnS shell growth.In particular,CuInZnS@ZnS QDs possess a significantly long emission lifetime(up to 750 ns),high PLQY(up to 85%),and excellent crystallinity.Their spectroscopic evolution is well validated by Cu-deficient related intragap emission model.By controlling the stoichiometric ratio of Cu/In,two distinct Cu-deficient related emission pathways are established based on the differing oxidation states of Cu defects.Therefore,this work provides deeper insights for fabricating high luminescent ternary or quaternary-alloyed QDs.展开更多
基金Fund Project for Transformation of Scientific and Technological Achievements of Jiangsu Province of China(BA2023020)。
文摘As an essential candidate for environment-friendly luminescent quantum dots(QDs),CuInS-based QDs have attracted more attention in recent years.However,several drawbacks still hamper their industrial applications,such as lower photoluminescence quantum yield(PLQY),complex synthetic pathways,uncontrollable emission spectra,and insufficient photostability.In this study,CuInZnS@ZnS core/shell QDs was prepared via a one-pot/three-step synthetic scheme with accurate and tunable control of PL spectra.Then their ensemble spectroscopic properties during nucleation formation,alloying,and ZnS shell growth processes were systematically investigated.PL peaks of these QDs can be precisely manipulated from 530 to 850 nm by controlling the stoichiometric ratio of Cu/In,Zn^(2+)doping and ZnS shell growth.In particular,CuInZnS@ZnS QDs possess a significantly long emission lifetime(up to 750 ns),high PLQY(up to 85%),and excellent crystallinity.Their spectroscopic evolution is well validated by Cu-deficient related intragap emission model.By controlling the stoichiometric ratio of Cu/In,two distinct Cu-deficient related emission pathways are established based on the differing oxidation states of Cu defects.Therefore,this work provides deeper insights for fabricating high luminescent ternary or quaternary-alloyed QDs.
