Colloidal Pb Se nanocrystals(NCs)have gained considerable attention due to their efficient carrier multiplication and emissions across near-infrared and short-wavelength infrared spectral ranges.However,the fast degra...Colloidal Pb Se nanocrystals(NCs)have gained considerable attention due to their efficient carrier multiplication and emissions across near-infrared and short-wavelength infrared spectral ranges.However,the fast degradation of colloidal Pb Se NCs in ambient conditions hampers their widespread applications in infrared optoelectronics.It is well-known that the inorganic thick-shell over core improves the stability of NCs.Here,we present the synthesis of Pb Se/Pb S core/shell NCs showing wide spectral tunability,in which the molar ratio of lead(Pb)and sulfur(S)precursors,and the concentration of sulfur and Pb Se NCs in solvent have a significant effect on the efficient Pb S shell growth.The infrared light-emitting diodes(IR-LEDs)fabricated with the Pb Se/Pb S core/shell NCs exhibit an external quantum efficiency(EQE)of 1.3%at 1280 nm.The ligand exchange to optimize the distance between NCs and chloride treatment are important processes for achieving high performance on Pb Se/Pb S NC-LEDs.Our results provide evidence for the promising potential of Pb Se/Pb S NCs over the wide range of infrared optoelectronic applications.展开更多
Lead chalcohalides(PbYX,X=Cl,Br,I;Y=S,Se)is an extension of the classic Pb chalcogenides(PbY).Constructing the heterogeneous integration with PbYX and PbY material systems makes it possible to achieve significantly im...Lead chalcohalides(PbYX,X=Cl,Br,I;Y=S,Se)is an extension of the classic Pb chalcogenides(PbY).Constructing the heterogeneous integration with PbYX and PbY material systems makes it possible to achieve significantly improved optoelectronic performance.In this work,we studied the effect of introducing halogen precursors on the structure of classical PbS nanocrystals(NCs)during the synthesis process and realized the preparation of PbS/Pb3S2X2 core/shell structure for the first time.The core/shell structure can effectively improve their optical properties.Furthermore,our approach enables the synthesis of Pb3S2Br2 that had not yet been reported.Our results not only provide valuable insights into the heterogeneous integration of PbYX and PbY materials to elevate material properties but also provide an effective method for further expanding the preparation of PbYX material systems.展开更多
To enhance the reproducibility and scale up the synthesis of colloidal quantum dots(QDs),continuous flow synthesis is an appealing alternative to the widely used batch synthesis.Amongst other advantages,the strongly e...To enhance the reproducibility and scale up the synthesis of colloidal quantum dots(QDs),continuous flow synthesis is an appealing alternative to the widely used batch synthesis.Amongst other advantages,the strongly enhanced heat and mass transfer in small tubular reactors combined with controlled pressure can be cited.Nonetheless,the widespread use of this technique is hampered by special requirements such as the absence of solid or gaseous products and the room-temperature solubility of precursors.Therefore,the transfer of established reaction conditions from batch to flow is not straightforward and in most reported works the optical properties of the obtained QDs lag behind those prepared in batch reactions.This is also the case for PbS-based QDs,which are established near infrared(NIR)absorbers/emitters.Here we identified experimental conditions giving access to high-quality PbS core and PbS/CdS core/shell QDs obtained in an automated,easily scalable continuous flow synthesis.In particular,substituted thioureas have been selected as the sulfur source and ex-situ synthesized lead and cadmium oleate as the metal precursors,and appropriate solvent mixtures have been identified for each precursor.Highly luminescent PbS/CdS QDs emitting at the target wavelengths 940 and 1130 nm of special interest for NIR light-emitting diodes have been prepared,exhibiting a photoluminescence quantum yield up to 91%.展开更多
基金Project supported by the National Key Research and Development Program of China(Grant No.2016YFB0401702)the National Natural Science Foundation of China(Grant Nos.61674074 and 61405089)+6 种基金Development and Reform Commission of Shenzhen Project,China(Grant No.[2017]1395)Shenzhen Peacock Team Project,China(Grant No.KQTD2016030111203005)Shenzhen Key Laboratory for Advanced Quantum Dot Displays and Lighting,China(Grant No.ZDSYS201707281632549)Guangdong Province’s Key R&D Program:Micro-LED Display and Ultra-high Brightness Micro-display Technology,China(Grant No.2019B010925001)Guangdong University Key Laboratory for Advanced Quantum Dot Displays and Lighting,China(Grant No.2017KSYS007)Distinguished Young Scholar of National Natural Science Foundation of Guangdong,China(Grant No.2017B030306010)the start-up fund from Southern University of Science and Technology,Shenzhen,China
摘要Colloidal Pb Se nanocrystals(NCs)have gained considerable attention due to their efficient carrier multiplication and emissions across near-infrared and short-wavelength infrared spectral ranges.However,the fast degradation of colloidal Pb Se NCs in ambient conditions hampers their widespread applications in infrared optoelectronics.It is well-known that the inorganic thick-shell over core improves the stability of NCs.Here,we present the synthesis of Pb Se/Pb S core/shell NCs showing wide spectral tunability,in which the molar ratio of lead(Pb)and sulfur(S)precursors,and the concentration of sulfur and Pb Se NCs in solvent have a significant effect on the efficient Pb S shell growth.The infrared light-emitting diodes(IR-LEDs)fabricated with the Pb Se/Pb S core/shell NCs exhibit an external quantum efficiency(EQE)of 1.3%at 1280 nm.The ligand exchange to optimize the distance between NCs and chloride treatment are important processes for achieving high performance on Pb Se/Pb S NC-LEDs.Our results provide evidence for the promising potential of Pb Se/Pb S NCs over the wide range of infrared optoelectronic applications.
基金supported by the National Key Research and Development Program of China(Grant No.2022YFE0110300)the National Natural Science Foundation of China(Grant Nos.52372215,92163114,and 52202274)+5 种基金the Natural Science Foundation of Jiangsu Province of China(Grant No.BK20230504)the Special Fund for the"Dual Carbon"Science and Technology Innovation of Jiangsu province(Industrial Prospect and Key Technology Research program)(Grant Nos.BE2022023 and BE2022021)the Natural Science Foundation of the Jiangsu Higher Education Institutions of China(Grant No.21KJA430004)Gusu Innovation and Entre preneurship Leading Talent Program(Grant No.ZXL2022451)the China Postdoctoral Science Foundation(Grant No.2023M732523)supported by Suzhou Key Laboratory of Functional Nano&Soft Materials,Collaborative Innovation Center of Suzhou Nano Science&Technology,the 111 Project.
摘要Lead chalcohalides(PbYX,X=Cl,Br,I;Y=S,Se)is an extension of the classic Pb chalcogenides(PbY).Constructing the heterogeneous integration with PbYX and PbY material systems makes it possible to achieve significantly improved optoelectronic performance.In this work,we studied the effect of introducing halogen precursors on the structure of classical PbS nanocrystals(NCs)during the synthesis process and realized the preparation of PbS/Pb3S2X2 core/shell structure for the first time.The core/shell structure can effectively improve their optical properties.Furthermore,our approach enables the synthesis of Pb3S2Br2 that had not yet been reported.Our results not only provide valuable insights into the heterogeneous integration of PbYX and PbY materials to elevate material properties but also provide an effective method for further expanding the preparation of PbYX material systems.
基金platforms of the Grenoble Instruct-ERIC center(ISBGUAR 3518 CNRSCEA-UGA-EMBL)within the Grenoble Partnership for Structural Biology(PSB)+1 种基金supported by FRISBI(ANR-10-INBS-0005-02)financed within the University Grenoble Alpes graduate school(Ecoles Universitaires de Recherche)CBH-EUR-GS(ANR-17-EURE-0003).
摘要To enhance the reproducibility and scale up the synthesis of colloidal quantum dots(QDs),continuous flow synthesis is an appealing alternative to the widely used batch synthesis.Amongst other advantages,the strongly enhanced heat and mass transfer in small tubular reactors combined with controlled pressure can be cited.Nonetheless,the widespread use of this technique is hampered by special requirements such as the absence of solid or gaseous products and the room-temperature solubility of precursors.Therefore,the transfer of established reaction conditions from batch to flow is not straightforward and in most reported works the optical properties of the obtained QDs lag behind those prepared in batch reactions.This is also the case for PbS-based QDs,which are established near infrared(NIR)absorbers/emitters.Here we identified experimental conditions giving access to high-quality PbS core and PbS/CdS core/shell QDs obtained in an automated,easily scalable continuous flow synthesis.In particular,substituted thioureas have been selected as the sulfur source and ex-situ synthesized lead and cadmium oleate as the metal precursors,and appropriate solvent mixtures have been identified for each precursor.Highly luminescent PbS/CdS QDs emitting at the target wavelengths 940 and 1130 nm of special interest for NIR light-emitting diodes have been prepared,exhibiting a photoluminescence quantum yield up to 91%.