A pure conducting polymer (PANI-CSA) film conditioned by an electric discharge was tentatively utilized as an cathode for emitting electrons under electric fields. The emission of electrons was observed using a phos...A pure conducting polymer (PANI-CSA) film conditioned by an electric discharge was tentatively utilized as an cathode for emitting electrons under electric fields. The emission of electrons was observed using a phosphor (ZnO:Zn) screen excited by electrons from the conditioned film. The film morphology was investigated using a scanning electron microscope and it was found that undulate whisker-like sites formed on the surface. The emission was presumably due to the undulate whisker-like sites. The field enhancement factor was estimated to be as high as 1150. The electron emitting process of the PANI-CSA film conditioned by electric discharge was also discussed.展开更多
The pursuit of high-performance electrode materials is highly desired to meet the demand of batteries with high energy and power density.However,a deep understanding of the charge storage mechanism is always challengi...The pursuit of high-performance electrode materials is highly desired to meet the demand of batteries with high energy and power density.However,a deep understanding of the charge storage mechanism is always challenging,which limits the development of advanced electrode materials.Herein,high-resolution mass spectroscopy(HR-MS)is employed to detect the evolution of organic electrode materials during the redox process and reveal the charge storage mechanism,by using small molecular oxamides as an example,which have ortho-carbonyls and are therefore potential electrochemical active materials for batteries.The HR-MS results adequately proved that the oxamides could reversibly store lithium ions in the voltage window of 1.5–3.8 V.Upon deeper reduction,the oxamides would decompose due to the cleavage of the C–N bonds in oxamide structures,which could be proved by the fragments detected by HR-MS,^(1)H NMR,and the generation of NH_(3)after the reduction of oxamide by Li.This work provides a strategy to deeply understand the charge storage mechanism of organic electrode materials and will stimulate the further development of characterization techniques to reveal the charge storage mechanism for developing high-performance electrode materials.展开更多
A nonlinear optical (NLO) active alkoxysilane chromophore (SGDR1) was synthesized. A fluorinated polyimide/SGDR1 composite was prepared to improve the poor temporal stability of second-order NLO effects of the reporte...A nonlinear optical (NLO) active alkoxysilane chromophore (SGDR1) was synthesized. A fluorinated polyimide/SGDR1 composite was prepared to improve the poor temporal stability of second-order NLO effects of the reported poled sol-gel film. The poled composite film was characterized by FTIR, DSC, TGA and UV-Vis. The composite displays good hydrophobic properties, high glass transition temperature (266 ℃), and high decomposition temperature (433 ℃). The second harmonic coefficient d33 of the composite was measured to be 16.77 pm/V by using maker fringe technique. The new NLO composite exhibits 85 % of the original d33 over 720 h at 100 ℃ and possesses much better stability than the reported sol-gel film.展开更多
Since the concept of computational spectroscopy was introduced,numerous computational spectrometers have emerged.While most of the work focuses on materials,optical structures,and devices,little attention is paid to t...Since the concept of computational spectroscopy was introduced,numerous computational spectrometers have emerged.While most of the work focuses on materials,optical structures,and devices,little attention is paid to the reconstruction algorithm,thus resulting in a common issue:the effectiveness of spectral reconstruction is limited under high-level noise originating from the data acquisition process.Here,we fabricate a computational spectrometer based on a quantum dot(QD)filter array and propose what we believe is a novel algorithm,TKVA(algorithm with Tikhonov and total variation regularization,and the alternating direction method of multipliers),to suppress the impact of noise on spectral recovery.Surprisingly,the new TKVA algorithm gives rise to another advantage,i.e.,the spectral accuracy can be enhanced through interpolation of the precalibration data,providing a convenient solution for performance improvement.In addition,the accuracy of spectral recovery is also enhanced via the interpolation,highlighting its superiority in spectral reconstruction.As a result,the QD spectrometer using the TKVA algorithm shows supreme spectral recovery accuracy compared to the traditional algorithms for complex and broad spectra,a spectral accuracy as low as 0.1 nm,and a spectral resolution of 2 nm in the range of 400 to 800 nm.The new reconstruction algorithm can be applied in various computational spectrometers,facilitating the development of this kind of equipment.展开更多
Lead sulfide(PbS)colloidal quantum dot(CQD)photodiodes integrated with silicon-based readout integrated circuits(ROICs)offer a promising solution for the next-generation short-wave infrared(SWIR)imaging technology.Des...Lead sulfide(PbS)colloidal quantum dot(CQD)photodiodes integrated with silicon-based readout integrated circuits(ROICs)offer a promising solution for the next-generation short-wave infrared(SWIR)imaging technology.Despite their potential,large-size CQD photodiodes pose a challenge due to high dark currents resulting from surface states on nonpassivated(100)facets and trap states generated by CQD fusion.In this work,we present a novel approach to address this issue by introducing double-ended ligands that supplementally passivate(100)facets of halidecapped large-size CQDs,leading to suppressed bandtail states and reduced defect concentration.Our results demonstrate that the dark current density is highly suppressed by about an order of magnitude to 9.6 nA cm^(2) at -10 mV,which is among the lowest reported for PbS CQD photodiodes.Furthermore,the performance of the photodiodes is exemplary,yielding an external quantum efficiency of 50.8%(which corresponds to a responsivity of 0.532 A W^(-1))and a specific detectivity of 2.5×10^(12) Jones at 1300 nm.By integrating CQD photodiodes with CMOS ROICs,the CQD imager provides high-resolution(640×512)SWIR imaging for infrared penetration and material discrimination.展开更多
Infrared solar cells are more efective than normal bandgap solar cells at reducing the spectral loss in the near-infrared region,thus also at broadening the absorption spectra and improving power conversion efciency.P...Infrared solar cells are more efective than normal bandgap solar cells at reducing the spectral loss in the near-infrared region,thus also at broadening the absorption spectra and improving power conversion efciency.PbS colloidal quantum dots(QDs)with tunable bandgap are ideal infrared photovoltaic materials.However,QD solar cell production sufers from small-areabased spin-coating fabrication methods and unstable QD ink.Herein,the QD ink stability mechanism was fully investigated according to Lewis acid–base theory and colloid stability theory.We further studied a mixed solvent system using dimethylformamide and butylamine,compatible with the scalable manufacture of method-blade coating.Based on the ink system,100 cm2 of uniform and dense near-infrared PbS QDs(~0.96 eV)flm was successfully prepared by blade coating.The average efciencies of above absorber-based devices reached 11.14%under AM1.5G illumination,and the 800 nm-fltered efciency achieved 4.28%.Both were the top values among blade coating method based devices.The newly developed ink showed excellent stability,and the device performance based on the ink stored for 7 h was similar to that of fresh ink.The matched solvent system for stable PbS QD ink represents a crucial step toward large area blade coating photoelectric devices.展开更多
As promising optoelectronic materials,lead sulfide quantum dots(PbS QDs)have attracted great attention.However,their applications are substantially limited by the QD quality and/or complicated synthesis.Herein,a facil...As promising optoelectronic materials,lead sulfide quantum dots(PbS QDs)have attracted great attention.However,their applications are substantially limited by the QD quality and/or complicated synthesis.Herein,a facile new synthesis is developed for highly monodisperse and halide passivated PbS QDs.The new synthesis is based on a heterogeneous system containing a PbCl_(2)-Pb(OA)_(2)solid-liquid precursor solution.The solid PbCl_(2)inhibits the diffusion of monomers and maintains a high oversaturation condition for the growth of PbS QDs,resulting in high monodispersities.In addition,the PbCl_(2)gives rise to halide passivation on the PbS QDs,showing excellent stability in air.The high monodispersity and good passivation endow these PbS QDs with outstanding optoelectronic properties,demonstrated by a 9.43%power conversion efficiency of PbS QD solar cells with a bandgap of~0.95 eV(1,300 nm).We believe that this heterogeneous strategy opens up a new avenue optimizing for the synthesis and applications of QDs.展开更多
Infrared(IR)solar cells are promising devices for improving the power conversion efficiency(PCE)of conventional solar cells by expanding the utilization region of the sunlight spectrum to near-infrared range.IR solar ...Infrared(IR)solar cells are promising devices for improving the power conversion efficiency(PCE)of conventional solar cells by expanding the utilization region of the sunlight spectrum to near-infrared range.IR solar cells based on colloidal quantum dots(QDs)have attracted extensive attention due to the widely tunable absorption spectrum controlled by dot size and the unique solution processibility.However,the trade-off in QD solar cells between light absorption and photo-generated carrier collection has limited the further improvement of PCE.Here,we present high-performance PbS QD IR solar cells resulting from the combination of boosted light absorption and optimized carrier extraction.By constructing an optical resonance cavity,the light absorption is significantly enhanced in the range of 1,150–1,300 nm at a relatively thin photoactive layer.Meanwhile,the thin photoactive layer facilitates efficient carrier extraction.Consequently,the PbS QD IR solar cells exhibit a highly efficient photoelectric conversion in the IR region,resulting in a high IR PCE of 1.3%which is comparable to the highest value of solution-processed IR solar cells based on PbSe QDs.These results demonstrate that constructing an optical resonance cavity is a reasonable strategy for effective conversion of photons in the devices aiming at light in a relatively narrow wavelength range,such as IR solar cells and narrow band photodetectors.展开更多
基金This work was supported by the Key Project of Chinese Ministry of Education (No. 104208)the National Natural Science Foundation of China under grant No. 50573024.
文摘A pure conducting polymer (PANI-CSA) film conditioned by an electric discharge was tentatively utilized as an cathode for emitting electrons under electric fields. The emission of electrons was observed using a phosphor (ZnO:Zn) screen excited by electrons from the conditioned film. The film morphology was investigated using a scanning electron microscope and it was found that undulate whisker-like sites formed on the surface. The emission was presumably due to the undulate whisker-like sites. The field enhancement factor was estimated to be as high as 1150. The electron emitting process of the PANI-CSA film conditioned by electric discharge was also discussed.
基金financialy supported by the National Natural Science Foundation of China(52173163,22279038,and 22205069)the National 1000-Talents Program,the Innovation Fund of WNLO,the Open Fund of the State Key Laboratory of Integrated Optoelectronics(IOSKL2020KF02)+1 种基金Wenzhou Science&Technology Bureau(ZG2022020,G20220022,and G20220026)the China Postdoctoral Science Foundation(2021TQ0115,2021 M701302,and 2020 M672323)
文摘The pursuit of high-performance electrode materials is highly desired to meet the demand of batteries with high energy and power density.However,a deep understanding of the charge storage mechanism is always challenging,which limits the development of advanced electrode materials.Herein,high-resolution mass spectroscopy(HR-MS)is employed to detect the evolution of organic electrode materials during the redox process and reveal the charge storage mechanism,by using small molecular oxamides as an example,which have ortho-carbonyls and are therefore potential electrochemical active materials for batteries.The HR-MS results adequately proved that the oxamides could reversibly store lithium ions in the voltage window of 1.5–3.8 V.Upon deeper reduction,the oxamides would decompose due to the cleavage of the C–N bonds in oxamide structures,which could be proved by the fragments detected by HR-MS,^(1)H NMR,and the generation of NH_(3)after the reduction of oxamide by Li.This work provides a strategy to deeply understand the charge storage mechanism of organic electrode materials and will stimulate the further development of characterization techniques to reveal the charge storage mechanism for developing high-performance electrode materials.
文摘A nonlinear optical (NLO) active alkoxysilane chromophore (SGDR1) was synthesized. A fluorinated polyimide/SGDR1 composite was prepared to improve the poor temporal stability of second-order NLO effects of the reported poled sol-gel film. The poled composite film was characterized by FTIR, DSC, TGA and UV-Vis. The composite displays good hydrophobic properties, high glass transition temperature (266 ℃), and high decomposition temperature (433 ℃). The second harmonic coefficient d33 of the composite was measured to be 16.77 pm/V by using maker fringe technique. The new NLO composite exhibits 85 % of the original d33 over 720 h at 100 ℃ and possesses much better stability than the reported sol-gel film.
基金supported by the National Key Research and Development Program of China(Grant No.2021YFA0715502)the National Natural Science Foundation of China(Grant Nos.61974052,U22A2083,62204091,62374068,and 62304085)+3 种基金the Scientific Research Project of Wenzhou(Grant No.G2023025)the Innovation Project of Optics Valley Laboratory(Grant No.OVL2023ZD002)the Exploration Project of Natural Science Foundation of Zhejiang Province(Grant No.LY23F040005)the Fund from Science,Technology,and Innovation Commission of Shenzhen Municipality(Grant Nos.GJHZ20210705142540010 and GJHZ20220913143403007).
文摘Since the concept of computational spectroscopy was introduced,numerous computational spectrometers have emerged.While most of the work focuses on materials,optical structures,and devices,little attention is paid to the reconstruction algorithm,thus resulting in a common issue:the effectiveness of spectral reconstruction is limited under high-level noise originating from the data acquisition process.Here,we fabricate a computational spectrometer based on a quantum dot(QD)filter array and propose what we believe is a novel algorithm,TKVA(algorithm with Tikhonov and total variation regularization,and the alternating direction method of multipliers),to suppress the impact of noise on spectral recovery.Surprisingly,the new TKVA algorithm gives rise to another advantage,i.e.,the spectral accuracy can be enhanced through interpolation of the precalibration data,providing a convenient solution for performance improvement.In addition,the accuracy of spectral recovery is also enhanced via the interpolation,highlighting its superiority in spectral reconstruction.As a result,the QD spectrometer using the TKVA algorithm shows supreme spectral recovery accuracy compared to the traditional algorithms for complex and broad spectra,a spectral accuracy as low as 0.1 nm,and a spectral resolution of 2 nm in the range of 400 to 800 nm.The new reconstruction algorithm can be applied in various computational spectrometers,facilitating the development of this kind of equipment.
基金National Natural Science Foundation of China,Grant/Award Numbers:U22A2083,62204091,62374068National Key Research and Development Program of China,Grant/Award Number:2021YFA0715502+5 种基金Key R&D program of Hubei Province,Grant/Award Number:2021BAA014Innovation Project of Optics Valley Laboratory,Grant/Award Numbers:OVL2021BG009,OVL2023ZD002Exploration Project of Natural Science Foundation of Zhejiang Province,Grant/Award Number:LY23F040005Fund for Innovative Research Groups of the Natural Science Foundation of Hubei Province,Grant/Award Number:2020CFA034Fund from Science,Technology and Innovation Commission of Shenzhen Municipality,Grant/Award Numbers:GJHZ20210705142540010,GJHZ20220913143403007China Postdoctoral Science Foundation,Grant/Award Numbers:2021M691118,2022M711237,2022M721243,2023T160244。
文摘Lead sulfide(PbS)colloidal quantum dot(CQD)photodiodes integrated with silicon-based readout integrated circuits(ROICs)offer a promising solution for the next-generation short-wave infrared(SWIR)imaging technology.Despite their potential,large-size CQD photodiodes pose a challenge due to high dark currents resulting from surface states on nonpassivated(100)facets and trap states generated by CQD fusion.In this work,we present a novel approach to address this issue by introducing double-ended ligands that supplementally passivate(100)facets of halidecapped large-size CQDs,leading to suppressed bandtail states and reduced defect concentration.Our results demonstrate that the dark current density is highly suppressed by about an order of magnitude to 9.6 nA cm^(2) at -10 mV,which is among the lowest reported for PbS CQD photodiodes.Furthermore,the performance of the photodiodes is exemplary,yielding an external quantum efficiency of 50.8%(which corresponds to a responsivity of 0.532 A W^(-1))and a specific detectivity of 2.5×10^(12) Jones at 1300 nm.By integrating CQD photodiodes with CMOS ROICs,the CQD imager provides high-resolution(640×512)SWIR imaging for infrared penetration and material discrimination.
基金HS acknowledges the financial support from the National Natural Science Foundation of China(Grant No.62374065)the Interdisciplinary Research promotion of HUST(No.2023JCYJ040)+4 种基金the Innovation Project of Optics Valley Laboratory(No.OVL2021BG008)the Program of Science Technology of Wenzhou City(No.G20210011)HH acknowledges the fnancial support from the Innovation and Technology Commission(No.MHP/104/21)the Shenzhen Science Technology and Innovation Commission(No.JCYJ20210324125612035)the City University of Hong Kong(Nos.9360140,7005720,9667229,9680331,7005580,and 9678291)。
文摘Infrared solar cells are more efective than normal bandgap solar cells at reducing the spectral loss in the near-infrared region,thus also at broadening the absorption spectra and improving power conversion efciency.PbS colloidal quantum dots(QDs)with tunable bandgap are ideal infrared photovoltaic materials.However,QD solar cell production sufers from small-areabased spin-coating fabrication methods and unstable QD ink.Herein,the QD ink stability mechanism was fully investigated according to Lewis acid–base theory and colloid stability theory.We further studied a mixed solvent system using dimethylformamide and butylamine,compatible with the scalable manufacture of method-blade coating.Based on the ink system,100 cm2 of uniform and dense near-infrared PbS QDs(~0.96 eV)flm was successfully prepared by blade coating.The average efciencies of above absorber-based devices reached 11.14%under AM1.5G illumination,and the 800 nm-fltered efciency achieved 4.28%.Both were the top values among blade coating method based devices.The newly developed ink showed excellent stability,and the device performance based on the ink stored for 7 h was similar to that of fresh ink.The matched solvent system for stable PbS QD ink represents a crucial step toward large area blade coating photoelectric devices.
基金supported by the National Key R&D Program of China(Nos.2021YFA0715502 and 2021YFA0715500)the National Natural Science Foundation of China(Nos.61974052 and 61904065),the Innovation Project of Optics Valley Laboratory(No.OVL2021BG009)+2 种基金the Fund from Science,Technology and Innovation Commission of Shenzhen Municipality(No.GJHZ20210705142540010)the Key R&D Program of Hubei Province(No.2021BAA014)the International Science and Technology Cooperation Project of Hubei Province(No.2021EHB010).
文摘As promising optoelectronic materials,lead sulfide quantum dots(PbS QDs)have attracted great attention.However,their applications are substantially limited by the QD quality and/or complicated synthesis.Herein,a facile new synthesis is developed for highly monodisperse and halide passivated PbS QDs.The new synthesis is based on a heterogeneous system containing a PbCl_(2)-Pb(OA)_(2)solid-liquid precursor solution.The solid PbCl_(2)inhibits the diffusion of monomers and maintains a high oversaturation condition for the growth of PbS QDs,resulting in high monodispersities.In addition,the PbCl_(2)gives rise to halide passivation on the PbS QDs,showing excellent stability in air.The high monodispersity and good passivation endow these PbS QDs with outstanding optoelectronic properties,demonstrated by a 9.43%power conversion efficiency of PbS QD solar cells with a bandgap of~0.95 eV(1,300 nm).We believe that this heterogeneous strategy opens up a new avenue optimizing for the synthesis and applications of QDs.
基金supported by the National Key R&D Program of China(No.2021YFA0715502)the National Natural Science Foundation of China(Nos.61974052,and 61904065)+2 种基金the Innovation Project of Optics Valley Laboratory(No.OVL2021BG009)the Fund from Science,Technology and Innovation Commission of Shenzhen Municipality(No.GJHZ20210705142540010)the Fundamental Research Funds for the Central Universities(WUT:2022IVA055).
文摘Infrared(IR)solar cells are promising devices for improving the power conversion efficiency(PCE)of conventional solar cells by expanding the utilization region of the sunlight spectrum to near-infrared range.IR solar cells based on colloidal quantum dots(QDs)have attracted extensive attention due to the widely tunable absorption spectrum controlled by dot size and the unique solution processibility.However,the trade-off in QD solar cells between light absorption and photo-generated carrier collection has limited the further improvement of PCE.Here,we present high-performance PbS QD IR solar cells resulting from the combination of boosted light absorption and optimized carrier extraction.By constructing an optical resonance cavity,the light absorption is significantly enhanced in the range of 1,150–1,300 nm at a relatively thin photoactive layer.Meanwhile,the thin photoactive layer facilitates efficient carrier extraction.Consequently,the PbS QD IR solar cells exhibit a highly efficient photoelectric conversion in the IR region,resulting in a high IR PCE of 1.3%which is comparable to the highest value of solution-processed IR solar cells based on PbSe QDs.These results demonstrate that constructing an optical resonance cavity is a reasonable strategy for effective conversion of photons in the devices aiming at light in a relatively narrow wavelength range,such as IR solar cells and narrow band photodetectors.
基金This work was supported by the National Key Research and Development Program of China(2021YFA0715502)the National Natural Science Foundation of China(61904065,61974052,and 62204091)+5 种基金Key R&D Program of Hubei Province(2021BAA014)International Science and Technology Cooperation Project of Hubei Province(2021EHB010)the fund for Innovative Research Groups of the Natural Science Foundation of Hubei Province(2020CFA034)Scientific Research Project of Wenzhou(G20210013)the China Postdoctoral Science Foundation(2021M691118,and 2022M711237)the Fund from Science,Technology and Innovation Commission of Shenzhen Municipality(GJHZ20210705142540010).