Indium phosphide-based quantum dots(InP-based QDs)have emerged as promising candidates for nextgeneration display and optoelectronic technologies,offering exceptional photoluminescent(PL)properties including high effi...Indium phosphide-based quantum dots(InP-based QDs)have emerged as promising candidates for nextgeneration display and optoelectronic technologies,offering exceptional photoluminescent(PL)properties including high efficiency,narrow emission spectra,and precisely tunable wavelengths.Nevertheless,their widespread commercialization encounters substantial obstacles,primarily stemming from persistent challenges in synthetic control and material processing.Critical performance parameters—including photoluminescence quantum yield(PL QY,currently35 nm)as well as external quantum efficiency(EQE)and operational stability of device—continue to show only incremental improvements,highlighting the urgent need for fundamental breakthroughs in QDs synthesis,surface engineering and device optimization.This review systematically examines the nucleation mechanisms governing InP core formation and outlines key strategies for optimizing InP-based core/shell QDs.Furthermore,we present a comprehensive analysis of recent breakthroughs in red,green,and blue-emitting InP-based QD light-emitting diodes(QLEDs)development,focusing on modulation of charge transport engineering and suppression of charge leakage.Finally,we critically evaluate the remaining commercialization challenges and future prospects for InP-based QLEDs in next-generation display and optoelectronic technologies,outlining potential pathways for overcoming current limitations.展开更多
Photoanodic properties greatly determine the overall performance of quantum-dot-sensitized solar cells(QDSCs). In the present report, the microdynamic behaviors of carriers in the nanocomposite thin-film, a Zn Se QD...Photoanodic properties greatly determine the overall performance of quantum-dot-sensitized solar cells(QDSCs). In the present report, the microdynamic behaviors of carriers in the nanocomposite thin-film, a Zn Se QD-sensitized mesoporous La-doped nano-TiO2 thin-film, as a potential candidate for photoanode, are probed via nanosecond transient photovoltaic(TPV) spectroscopy. The results confirm that the L-Cys ligand has a dual function serving as a stabilizer and molecular linker. Large quantities of interface states are located at the energy level with a photoelectric threshold of1.58 eV and a quantum well(QW) depth of 0.67 eV. This QW depth is approximately 0.14 eV deeper than the depth of QW buried in the Zn Se QDs, and a deeper QW results in a higher quantum confinement energy. A strong quantum confinement effect of the interface state may be responsible for the excellent TPV characteristics of the photoanode. For example, the peak intensity of the TPV response of the QD-sensitized thin-film lasts a long time, from 9.40 × 10^(-7) s to 2.96 × 10^(-4) s,and the end time of the PTV response of the QD-sensitized thin-film is extended by approximately an order of magnitude compared with those of the TiO2 substrate and the QDs. The TPV characteristics of the QD-sensitized thin-film change from p-type to n-type for the QDs before and after sensitizing. These properties strongly depend on the extended diffusion length of the photogenerated carries and the reduced recombination rate of photogenerated electron-hole pairs, resulting in prolonged carrier lifetime and an increased level of electron injection into the TiO2 thin-film substrate.展开更多
In this study,a two-step method was used to synthesize highly luminescent AgGaS/ZnS/ZnS quantum dots(QDs).In the first step,an inner ZnS shell was formed via a one-pot method,which resulted in a smaller lattice mismat...In this study,a two-step method was used to synthesize highly luminescent AgGaS/ZnS/ZnS quantum dots(QDs).In the first step,an inner ZnS shell was formed via a one-pot method,which resulted in a smaller lattice mismatch between the AgGaS core and the outer ZnS shell,thereby facilitating the formation of a thick outer shell.After the two-step shelling process,the synthesized AgGaS/ZnS/ZnS QDs showed an excellent photoluminescence quantum yield(PLQY)of 96.4%with a peak wavelength of 508 nm,repre-senting the highest PLQY reported thus far for AgGaS QDs.Furthermore,the effect of halogen ions in Zn precursors on the shelling process was investigated.It was proposed that the capacity of halogen ions to coordinate with the QDs influenced the balance between Zn cation diffusion and ZnS shelling reaction.Specifically,the ZnS shelling reaction was dominant when ZnCl2was employed,while Zn cation diffusion was the dominant process under the I−-rich environment.This work provides insights into the interfacial restructuring during the ZnS shelling and offers a clear map for the tailored synthesis of core/shell QDs.展开更多
The discovery of quantum dots(QDs)stands as one of the paramount technological breakthroughs of the 20th century.Their versatility spans from everyday applications to cutting-edge scientific research,encompassing area...The discovery of quantum dots(QDs)stands as one of the paramount technological breakthroughs of the 20th century.Their versatility spans from everyday applications to cutting-edge scientific research,encompassing areas such as displays,lighting,photocatalysis,bio-imaging,and photonics devices and so on.Among the myriad QDs technologies,industrially relevant CuInS2(CIS)QDs have emerged as promising alternatives to traditional Cd-and Pb-based QDs.Their tunable optoelectronic properties,high absorption coefficient,compositional flexibility,remarkable stability as well as Restriction of Hazardous Substances-compliance,with recent trends revealing a renewed interest in this material for various visible and near-infrared technological applications.This review focuses on recent advancements in CIS QDs as multidisciplinary field from its genesis in the mid-1990 to date with an emphasis on key breakthroughs in their synthesis,surface chemistry,post-synthesis modifications,and various applications.First,the comparation of properties of CIS QDs with relevant knowledge from other classes of QDs and from Ⅰ-Ⅱ-Ⅲ semiconductors as well is summarized.Second,recent advances in the synthesis methods,structure-optoelectronic properties,their defects,and passivation strategies as well as CIS-based heterostructures are discussed.Third,the state-of-the-art applications of CIS QDs ranging from solar cells,luminescence solar concentrations,photocatalysis,light emitting diodes,bioimaging and some emerging applications are summarized.Finally,we discuss open challenges and future perspectives for further advancement in this field.展开更多
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
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-pothree-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,Zn2+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
Recent progress in the field of carbon dots(CDs)has highlighted their significant potential,attributed to their exceptional optical properties and diverse applications,most notably in the realm of white lightemitting ...Recent progress in the field of carbon dots(CDs)has highlighted their significant potential,attributed to their exceptional optical properties and diverse applications,most notably in the realm of white lightemitting diodes(WLEDs).CDs are recognized for their broad spectrum of emission,adjustable fluorescence,and excellent thermal stability,making them ideal candidates for use in WLEDs.However,the challenge lies in synthesizing CDs that can emit long-wavelength,multicolor light from a single host material.This research presents a highly efficient dual-core-shell structured white-emitting phosphor,denoted as ZnS:Mn-CDs@SiO2,which has achieved an impressive photoluminescence quantum yield(PLQY)of 25.8%and an expansive full width at half maximum(FWHM)of 131 nm.The successful implementation of this novel material has led to the creation of WLEDs with Commission Internationale de l’Eclairage(CIE)coordinates at(0.32,0.38)and a correlated color temperature(CCT)of 5854.3 K,marking a significant stride in the development of high-performance WLEDs.展开更多
Blue emissive quantum dots are key materials in fabricating quantum-dot light-emitting diodes for display applications.Up to date,most of the previous blue emissive quantum dots are based on quantum dots with type-I c...Blue emissive quantum dots are key materials in fabricating quantum-dot light-emitting diodes for display applications.Up to date,most of the previous blue emissive quantum dots are based on quantum dots with type-I core-shell structure.In this work,we report pure-blue emissive ZnSe/CdxZn1-xS/ZnS quantum dots with type-II core-shell structure,which show high photoluminescence quantum yield over 90%.The type-II structure was investigated by applying time-resolved photoluminescence and transient absorption measurements,illustrating the extended photoluminescence decay lifetime of ZnSe/CdxZn1-xS quantum dots as well as the transition of bleaching peak from the valence band of ZnSe to the conduction band of CdZnS.We further fabricated ZnSe/CdxZn1-xS/ZnS quantum dots based electroluminescence devices,achieving a maximum external quantum efficiency of 6.7%and a maximum luminance of 39,766 cd·m-2.展开更多
A one-pothree-step synthetic scheme was developed for phase-pure epitaxy of CdS shells on zinc-blende CdSe nanocrystals to yield shells with up to sixteen monolayers.The key parameters for the epitaxy were identified,...A one-pothree-step synthetic scheme was developed for phase-pure epitaxy of CdS shells on zinc-blende CdSe nanocrystals to yield shells with up to sixteen monolayers.The key parameters for the epitaxy were identified,including the core nanocrystal concentration,solvent type/composition,quality of the core nanocrystals,epitaxial growth temperature,type/concentration of ligands,and composition of the precursors.Most of these key parameters were not influential when the synthetic goal was thin-shell CdSe/CdS core/shell nanocrystals.The finalized synthetic scheme was reproducible at an almost quantitative level in terms of the crystal structure,shell thickness,and optical properties.展开更多
基金support from the National Key Research and Development Program of China[Grant No.2022YFB3602901]Beijing Natural Science Foundation[Grant No.Z220007]+3 种基金the National Natural Science Foundation of China[Grant No.62574076]the National Key R&D Program of China[Grant No.2023YFE0205000]the Zhongyuan High Level Talents Special Support Plan[Grant No.244200510009]he Technological Innovation 2030-Major Projects[Grant No.2024ZD0604000].
摘要Indium phosphide-based quantum dots(InP-based QDs)have emerged as promising candidates for nextgeneration display and optoelectronic technologies,offering exceptional photoluminescent(PL)properties including high efficiency,narrow emission spectra,and precisely tunable wavelengths.Nevertheless,their widespread commercialization encounters substantial obstacles,primarily stemming from persistent challenges in synthetic control and material processing.Critical performance parameters—including photoluminescence quantum yield(PL QY,currently35 nm)as well as external quantum efficiency(EQE)and operational stability of device—continue to show only incremental improvements,highlighting the urgent need for fundamental breakthroughs in QDs synthesis,surface engineering and device optimization.This review systematically examines the nucleation mechanisms governing InP core formation and outlines key strategies for optimizing InP-based core/shell QDs.Furthermore,we present a comprehensive analysis of recent breakthroughs in red,green,and blue-emitting InP-based QD light-emitting diodes(QLEDs)development,focusing on modulation of charge transport engineering and suppression of charge leakage.Finally,we critically evaluate the remaining commercialization challenges and future prospects for InP-based QLEDs in next-generation display and optoelectronic technologies,outlining potential pathways for overcoming current limitations.
基金supported by the Natural Science Foundation of Hebei Province,China(Grant Nos.E2013203296 and E2017203029)
摘要Photoanodic properties greatly determine the overall performance of quantum-dot-sensitized solar cells(QDSCs). In the present report, the microdynamic behaviors of carriers in the nanocomposite thin-film, a Zn Se QD-sensitized mesoporous La-doped nano-TiO2 thin-film, as a potential candidate for photoanode, are probed via nanosecond transient photovoltaic(TPV) spectroscopy. The results confirm that the L-Cys ligand has a dual function serving as a stabilizer and molecular linker. Large quantities of interface states are located at the energy level with a photoelectric threshold of1.58 eV and a quantum well(QW) depth of 0.67 eV. This QW depth is approximately 0.14 eV deeper than the depth of QW buried in the Zn Se QDs, and a deeper QW results in a higher quantum confinement energy. A strong quantum confinement effect of the interface state may be responsible for the excellent TPV characteristics of the photoanode. For example, the peak intensity of the TPV response of the QD-sensitized thin-film lasts a long time, from 9.40 × 10^(-7) s to 2.96 × 10^(-4) s,and the end time of the PTV response of the QD-sensitized thin-film is extended by approximately an order of magnitude compared with those of the TiO2 substrate and the QDs. The TPV characteristics of the QD-sensitized thin-film change from p-type to n-type for the QDs before and after sensitizing. These properties strongly depend on the extended diffusion length of the photogenerated carries and the reduced recombination rate of photogenerated electron-hole pairs, resulting in prolonged carrier lifetime and an increased level of electron injection into the TiO2 thin-film substrate.
基金supported by the National Natural Science Foun-dation of China(No.62074044)Zhongshan-Fudan Joint Innova-tion Center,Jihua Laboratory Projects of Guangdong Province(No.X190111UZ190)+1 种基金Shanghai Post-doctoral Excellence Program(No.2021016)Shanghai Rising-Star program(No.22YF1402000).
摘要In this study,a two-step method was used to synthesize highly luminescent AgGaS/ZnS/ZnS quantum dots(QDs).In the first step,an inner ZnS shell was formed via a one-pot method,which resulted in a smaller lattice mismatch between the AgGaS core and the outer ZnS shell,thereby facilitating the formation of a thick outer shell.After the two-step shelling process,the synthesized AgGaS/ZnS/ZnS QDs showed an excellent photoluminescence quantum yield(PLQY)of 96.4%with a peak wavelength of 508 nm,repre-senting the highest PLQY reported thus far for AgGaS QDs.Furthermore,the effect of halogen ions in Zn precursors on the shelling process was investigated.It was proposed that the capacity of halogen ions to coordinate with the QDs influenced the balance between Zn cation diffusion and ZnS shelling reaction.Specifically,the ZnS shelling reaction was dominant when ZnCl2was employed,while Zn cation diffusion was the dominant process under the I−-rich environment.This work provides insights into the interfacial restructuring during the ZnS shelling and offers a clear map for the tailored synthesis of core/shell QDs.
基金X.H.acknowledges the financial support by Australian Research Council(ARC)Future Fellowship(FT190100756)M.P.S.gratefully acknowledges the support by the ARC under Discovery Early Career Researcher Award(DECRA)(DE210101565)and Discovery Project(DP230101676).
摘要The discovery of quantum dots(QDs)stands as one of the paramount technological breakthroughs of the 20th century.Their versatility spans from everyday applications to cutting-edge scientific research,encompassing areas such as displays,lighting,photocatalysis,bio-imaging,and photonics devices and so on.Among the myriad QDs technologies,industrially relevant CuInS2(CIS)QDs have emerged as promising alternatives to traditional Cd-and Pb-based QDs.Their tunable optoelectronic properties,high absorption coefficient,compositional flexibility,remarkable stability as well as Restriction of Hazardous Substances-compliance,with recent trends revealing a renewed interest in this material for various visible and near-infrared technological applications.This review focuses on recent advancements in CIS QDs as multidisciplinary field from its genesis in the mid-1990 to date with an emphasis on key breakthroughs in their synthesis,surface chemistry,post-synthesis modifications,and various applications.First,the comparation of properties of CIS QDs with relevant knowledge from other classes of QDs and from Ⅰ-Ⅱ-Ⅲ semiconductors as well is summarized.Second,recent advances in the synthesis methods,structure-optoelectronic properties,their defects,and passivation strategies as well as CIS-based heterostructures are discussed.Third,the state-of-the-art applications of CIS QDs ranging from solar cells,luminescence solar concentrations,photocatalysis,light emitting diodes,bioimaging and some emerging applications are summarized.Finally,we discuss open challenges and future perspectives for further advancement in this field.
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Fund Project for Transformation of Scientific and Technological Achievements of Jiangsu Province of China(BA2023020)。
摘要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-pothree-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,Zn2+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.
基金the Recruitment Program of Global Experts,National Natural Science Foundation of China(Grant No.62175033 and 61775040)the Fujian Science&Technology Innovation Laboratory for Optoelectronic Information(Grant No.2021ZZ126)Fuzhou University for the financial support.
摘要Recent progress in the field of carbon dots(CDs)has highlighted their significant potential,attributed to their exceptional optical properties and diverse applications,most notably in the realm of white lightemitting diodes(WLEDs).CDs are recognized for their broad spectrum of emission,adjustable fluorescence,and excellent thermal stability,making them ideal candidates for use in WLEDs.However,the challenge lies in synthesizing CDs that can emit long-wavelength,multicolor light from a single host material.This research presents a highly efficient dual-core-shell structured white-emitting phosphor,denoted as ZnS:Mn-CDs@SiO2,which has achieved an impressive photoluminescence quantum yield(PLQY)of 25.8%and an expansive full width at half maximum(FWHM)of 131 nm.The successful implementation of this novel material has led to the creation of WLEDs with Commission Internationale de l’Eclairage(CIE)coordinates at(0.32,0.38)and a correlated color temperature(CCT)of 5854.3 K,marking a significant stride in the development of high-performance WLEDs.
基金granted by National Natural Science Foundation of China(No.U23B20683)the Natural Science Foundation of Beijing Municipality(No.Z210018).
摘要Blue emissive quantum dots are key materials in fabricating quantum-dot light-emitting diodes for display applications.Up to date,most of the previous blue emissive quantum dots are based on quantum dots with type-I core-shell structure.In this work,we report pure-blue emissive ZnSe/CdxZn1-xS/ZnS quantum dots with type-II core-shell structure,which show high photoluminescence quantum yield over 90%.The type-II structure was investigated by applying time-resolved photoluminescence and transient absorption measurements,illustrating the extended photoluminescence decay lifetime of ZnSe/CdxZn1-xS quantum dots as well as the transition of bleaching peak from the valence band of ZnSe to the conduction band of CdZnS.We further fabricated ZnSe/CdxZn1-xS/ZnS quantum dots based electroluminescence devices,achieving a maximum external quantum efficiency of 6.7%and a maximum luminance of 39,766 cd·m-2.
基金The financial support from the National Natural Science Foundation of China(Nos.21233005 and 91433204)is acknowledged.
摘要A one-pothree-step synthetic scheme was developed for phase-pure epitaxy of CdS shells on zinc-blende CdSe nanocrystals to yield shells with up to sixteen monolayers.The key parameters for the epitaxy were identified,including the core nanocrystal concentration,solvent type/composition,quality of the core nanocrystals,epitaxial growth temperature,type/concentration of ligands,and composition of the precursors.Most of these key parameters were not influential when the synthetic goal was thin-shell CdSe/CdS core/shell nanocrystals.The finalized synthetic scheme was reproducible at an almost quantitative level in terms of the crystal structure,shell thickness,and optical properties.