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| 1 | Rationally designed synthesis of bright AgInS2/ZnS quantum dots with emission control显示文摘In the blossoming field of Cd-free semiconductor quantum dots(QDs),ternary Ⅰ-Ⅲ-VI QDs have received increasing attention due to the ease of the environmentally friendly synthesis of high-quality materials in water,their high photoluminescence(PL)quantum yields(QYs)in the red and near infrared(NIR)region,and their inherently low toxicity.Moreover,their oxygen-insensitive long PL lifetimes of up to several hundreds of nanoseconds close a gap for applications exploiting the compound-specific parameter PL lifetime.To overcome the lack of reproducible synthetic methodologies and to enable a design-based control of their PL properties,we assessed and modelled the synthesis of high-quality MPA-capped AglnS2/ZnS(AlS/ZnS)QDs.Systematically refined parameters included reaction time,temperature,Ag:In ratio,S:In ratio,Zn:In ratio,MPA:ln ratio,and pH using a design-of-experiment approach.Guidance for the optimization was provided by mathematical models developed for the application-relevant PL parameters,maximum PL wavelength,QY,and PL lifetime as well as the elemental composition in terms of Ag:ln:Zn ratio.With these experimental data-based models,MPA:ln and Ag:ln ratios and pH values were identified as the most important synthesis parameters for PL control and an insight into the connection of these parameters could be gained.Subsequently,the experimental conditions to synthetize QDs with tunable emission and high QY were predicted.The excellent agreement between the predicted and experimentally found PL features confirmed the reliability of our methodology for the rational design of high quality AlS/ZnS QDs with defined PL features.This approach can be straightforwardly extended to other ternary and quaternary QDs and to doped QDs. | Jose X.Soares K.David Wegner David S.M.Ribeiro Armindo Melo Ines Hausler Joao L.M.Santos Ute Resch-Genger | 2020 | Nano Research2020，13，9： | 2 |
| 2 | Size focusing of colloidal quantum dots under high monomer concentration显示文摘The diffusion-controlled growth mode is widely used to narrow the size distribution of colloidal quantum dots.However,this growth mode always suffers from size broadening at the later growth stage.By monitoring the growth process of CdS colloidal quantum dots,we show the size broadening is a result of different growth rates of CdS colloidal quantum dots(CQDs)with different morphologies.Monomer concentration-dependent growth experiments demonstrate the different growth rates are caused by the different ligand permeabilities of CdS CQDs.The cubic ones have lower ligand permeability but higher saturated surface reaction rate than the noncubic ones,leading to unexpected narrower size distribution under higher monomer concentration.More efficient narrowing can be obtained by the addition of chloride ions,which can increase the ligand permeability of all CdS CQDs,as well as the opposite discrepancies in ligand permeability and surface reaction between cubic and noncubic CdS CQDs.The photoluminescence(PL)full width at half maximum(FWHM)of CdS CQDs can be narrowed down to below 80 meV for PL peaks from 430 to 500 nm.Given the inevitable usage of the ligands in the solution synthesis of colloidal nanocrystals,the influence of morphology difference on growth rate should be common.Our results can provide an alternative solution to realize size focusing for the synthesis of colloidal nanocrystals. | Huiyan Liu Zhi Liu Chaodan Pu | 2022 | Nano Research2022，15，8： | 0 |
| 3 | AgAuSe quantum dots with absolute photoluminescence quantum yield of 87.2%:The effect of capping ligand chain length显示文摘Surface ligands of colloidal quantum dots(QDs)have a profound influence on their surface states,which has been verified in the studies of the effect of ligand head groups on the photoluminescence(PL)properties of QDs.However,the investigation of the ligand chain length is limited.Here,we systematically explored the effect of chain length on the Ag_(2)Se QDs by selecting three ligands,1-octanethiol(OTT),1-dodecanethiol(DDT),and 1-hexadecanethiol(HDT),with diverse chain lengths.We found that the PL intensity of Ag_(2)Se QDs increased with the decrease of the ligand chain length due to the enhanced passivation of surface defects emerging from the robust QD-ligand interface binding affinity and the weaker hydrophobic chain–chain interaction.Subsequently,AgAuSe QDs terminated with OTT were obtained by alloying parent OTT-Ag_(2)Se QDs with Au precursor with a record absolute PL quantum yield(PLQY)of 87.2%at 970 nm,facilitating ultrasensitive in vivo angiography imaging in a nude mouse model.We expect that our finding of the important role of the ligand chain length on the optical properties of QDs will be suggestive to the design and synthesis of high-quality QDs,and also look forward to the clinical applications of the ultra-bright AgAuSe QDs. | Ziqiang Sun Cheng Liu Hongchao Yang Xiaohu Yang Yejun Zhang Hongzhen Lin Youyong Li Qiangbin Wang | 2022 | Nano Research2022，15，9： | 0 |
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