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 ZnCl_(2)was 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
CdS and CdS/ZnS quantum dots were synthesized by the microemulsion method in sulfosuccinic acid bis(2-ethylhexyl)ester sodium salt(AOT) surfactant reverse micelles containing water.The products were characterized by U...CdS and CdS/ZnS quantum dots were synthesized by the microemulsion method in sulfosuccinic acid bis(2-ethylhexyl)ester sodium salt(AOT) surfactant reverse micelles containing water.The products were characterized by UV-Vis spectrometer,transmission electronmicroscopy(TEM),energy dispersive X-ray spectroscope(EDX)and photoluminescence(PL) spectroscope.The diameter of CdS/ZnS nanoparticle was obvious larger than that of CdS nanoparticle.The diameter of the nanoparticle was estimated,which was confirmed by the images of TEM.The existence of core-shell structure was established by the result of energy dispersive X-ray analysis.PL studies of the samples showed that the luminescence from CdS was enhanced by the ZnS shell.A possible reason was that the ZnS shell reduced the number of defects on the surface of CdS quantum dots,which were assumed to act as centers for radiation-free recombination.展开更多
基金supported by the Natural Science Foundation of Hebei Province,China(Grant Nos.E2013203296 and E2017203029)
文摘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).
文摘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 ZnCl_(2)was 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.
文摘纳米技术研究体系中量子点是重要的研究模块之一,量子点尺寸非常小,具有独特的光物理特性。该文旨通过实验进行分析,实验过程选择99%纯度硼氢化钠、99%纯度硫酸锌、S212恒速搅拌器、TG16-WS高速离心机、0.310 mL巯基乙酸等,制备0.4565 g CdCl_(2)·2.5H_(2)O混合液,当样本溶液呈现橙色时,表明CdTe核已制备完成。实验结果显示:单脉冲能量增加时,τ_(-rise)与τ_(2)有所降低,τ_(1)数值增加,τ_(-rise)与壳层厚度呈正比关系。通过对量子点荧光特性的分析,有利于促进核壳结构量子点的制备。
文摘CdS and CdS/ZnS quantum dots were synthesized by the microemulsion method in sulfosuccinic acid bis(2-ethylhexyl)ester sodium salt(AOT) surfactant reverse micelles containing water.The products were characterized by UV-Vis spectrometer,transmission electronmicroscopy(TEM),energy dispersive X-ray spectroscope(EDX)and photoluminescence(PL) spectroscope.The diameter of CdS/ZnS nanoparticle was obvious larger than that of CdS nanoparticle.The diameter of the nanoparticle was estimated,which was confirmed by the images of TEM.The existence of core-shell structure was established by the result of energy dispersive X-ray analysis.PL studies of the samples showed that the luminescence from CdS was enhanced by the ZnS shell.A possible reason was that the ZnS shell reduced the number of defects on the surface of CdS quantum dots,which were assumed to act as centers for radiation-free recombination.
