Up-conversion lasing actions are normally difficult to realize in light-emitting materials due to small multi-photon absorp-tion cross section and fast dephasing of excited states during multi-photon excitation.This p...Up-conversion lasing actions are normally difficult to realize in light-emitting materials due to small multi-photon absorp-tion cross section and fast dephasing of excited states during multi-photon excitation.This paper reports an easily ac-cessible up-conversion amplified spontaneous emission(ASE)in organic-inorganic hybrid perovskites(MAPbBr3)films by optically exciting broad gap states with sub-bandgap laser excitation.The broad absorption was optimized by adjust-ing the grain sizes in the MAPbBr3 films.At low sub-bandgap pumping intensities,directly exciting the gap states leads to 2-photon,3-photon,and 4-photon up-conversion spontaneous emission,revealing a large optical cross section of multi-photon excitation occurring in such hybrid perovskite films.At moderate pumping intensity(1.19 mJ/cm2)of 700 nm laser excitation,a significant spectral narrowing phenomenon was observed with the full width at half maximum(FWHM)de-creasing from 18 nm to 4 nm at the peak wavelength of 550 nm,simultaneously with a nonlinear increase on spectral peak intensity,showing an up-conversion ASE realized at low threshold pumping fluence.More interestingly,the up-con-version ASE demonstrated a giant magnetic field effect,leading to a magneto-ASE reaching 120%.In contrast,the up-conversion photoluminescence(PL)showed a negligible magnetic field effect(<1%).This observation provides an evid-ence to indicate that the light-emitting states responsible for up-conversion ASE are essentially formed as spatially exten-ded states.The angular dependent spectrum results further verify the existence of spatially extended states which are polarized to develop coherent in-phase interaction.Clearly,using broad gap states with spatially extended light-emitting states presents a new approach to develop up-conversion ASE in organic-inorganic hybrid perovskites.展开更多
An ultra-thin molybdenum(VI)oxide(MoO3)modification layer can significantly improve hole injection from an electrode even though the MoO3 layer does not contact the electrode.We find that as the thickness of the organ...An ultra-thin molybdenum(VI)oxide(MoO3)modification layer can significantly improve hole injection from an electrode even though the MoO3 layer does not contact the electrode.We find that as the thickness of the organic layer between MoO3 and the electrode increases,the hole injection first increases and it then decreases.The optimum thickness of 5 nm corresponds to the best current improvement 70%,higher than that in the device where MoO3 directly contacts the Al electrode.According to the 4,4-bis[N-(1-naphthyl)-N-phenyl-amino]biphenyl(NPB)/MoO3 interface charge transfer mechanism and the present experimental results,we propose a mechanism that mobile carriers generated at the interface and accumulated inside the device change the distribution of electric field inside the device,resulting in an increase of the probability of hole tunneling through the injection barrier from the electrode,which also explains the phenomenon of hole injection enhanced by MoO3/NPB/Al composite anode.Based on this mechanism,different organic materials other than NPB were applied to form the composite electrode with MoO3.Similar current enhancement effects are also observed.展开更多
Perovskite light-emitting diodes(PeLEDs)exhibit remarkable potential in the field of displays and solidstate lighting.However,blue PeLEDs,a key element for practical applications,still lag behind their green and red c...Perovskite light-emitting diodes(PeLEDs)exhibit remarkable potential in the field of displays and solidstate lighting.However,blue PeLEDs,a key element for practical applications,still lag behind their green and red counterparts,due to a combination of strong nonradiative recombination losses and unoptimized device structures.In this report,we propose a buried interface modification strategy to address these challenges by focusing on the bottom-hole transport layer(HTL)of the PeLEDs.On the one hand,a multifunctional molecule,aminoacetic acid hydrochloride(AACl),is introduced to modify the HTL/perovskite interface to regulate the perovskite crystallization.Experimental investigations and theoretical calculations demonstrate that AACl can effectively reduce the nonradiative recombination losses in bulk perovskites by suppressing the growth of low-n perovskite phases and also the losses at the bottom interface by passivating interfacial defects.On the other hand,a self-assembly nanomesh structure is ingeniously developed within the HTLs.This nanomesh structure is meticulously crafted through the blending of poly-(9,9-dioctyl-fluorene-co-N-(4-butyl phenyl)diphenylamine)and poly(n-vinyl carbazole),significantly enhancing the light outcoupling efficiency in PeLEDs.As a result,our blue PeLEDs achieve remarkable external quantum efficiencies,20.4%at 487 nm and 12.5%at 470 nm,which are among the highest reported values.Our results offer valuable insights and effective methods for achieving high-performance blue PeLEDs.展开更多
Although perovskite light-emitting diodes(PeLEDs)have seen unprecedented development in device efciency over the past decade,they sufer signifcantly from poor operational stability.This is especially true for blue PeL...Although perovskite light-emitting diodes(PeLEDs)have seen unprecedented development in device efciency over the past decade,they sufer signifcantly from poor operational stability.This is especially true for blue PeLEDs,whose operational lifetime remains orders of magnitude behind their green and red counterparts.Here,we systematically investigate this efciency-stability discrepancy in a series of green-to blue-emitting PeLEDs based on mixed Br/Cl-perovskites.We fnd that chloride incorporation,while having only a limited impact on efciency,detrimentally afects device stability even in small amounts.Device lifetime drops exponentially with increasing Cl-content,accompanied by an increased rate of change in electrical properties during operation.We ascribe this phenomenon to an increased mobility of halogen ions in the mixed-halide lattice due to an increased chemically and structurally disordered landscape with reduced migration barriers.Our results indicate that the stability enhancement for PeLEDs might require diferent strategies from those used for improving efciency.展开更多
The photovoltaic performance of perovskite solar cell is determined by multiple interrelated factors,such as perovskite compositions,electronic properties of each transport layer and fabrication parameters,which makes...The photovoltaic performance of perovskite solar cell is determined by multiple interrelated factors,such as perovskite compositions,electronic properties of each transport layer and fabrication parameters,which makes it rather challenging for optimization of device performances and discovery of underlying mechanisms.Here,we propose and realize a novel machine learning approach based on forward-reverse framework to establish the relationship between key parameters and photovoltaic performance in high-profile MASnxPb1-xI3 perovskite materials.The proposed method establishes the asymmetrically bowing relationship between band gap and Sn composition,which is precisely verified by our experiments.Based on the analysis of structural evolution and SHAP library,the rapid-change region and low-bandgap plateau region for small and large Sn composition are explained,respectively.By establishing the models for photovoltaic parameters of working photovoltaic devices,the deviation of short-circuit current and open-circuit voltage with band gap in defective-zone and low-bandgap-plateau regions from Shockley-Queisser theory is captured by our models,and the former is due to the deep-level traps formed by crystallographic distortion and the latter is due to the enhanced susceptibility by increased Sn4+content.The more difficulty for hole extraction than electron is also concluded in the models and the prediction curve of power conversion efficiency is in a good agreement with Shockley-Queisser limit.With the help of search and optimization algorithms,an optimized Sn:Pb composition ratio near 0.6 is finally obtained for high-performance perovskite solar cells,then verified by our experiments.Our constructive method could also be applicable to other material optimization and efficient device development.展开更多
基金This work was supported by the 973 Program and China National Key Basic Research Program(2016YFA0301100,2016YFA0302000,and 2018YFA0306201)National Science Foundation of China(11774063 and 11727811)+2 种基金Science and Technology Commission of Shanghai Municipality(19XD1434600,2019SHZDZX01 and 19DZ2253000)Air Force Office of Scientific Research(AFOSR)under the grant number FA 9550-15-1-0064,AOARD(FA2386-15-1-4104)National Science Foundation(NSF-1911659).
文摘Up-conversion lasing actions are normally difficult to realize in light-emitting materials due to small multi-photon absorp-tion cross section and fast dephasing of excited states during multi-photon excitation.This paper reports an easily ac-cessible up-conversion amplified spontaneous emission(ASE)in organic-inorganic hybrid perovskites(MAPbBr3)films by optically exciting broad gap states with sub-bandgap laser excitation.The broad absorption was optimized by adjust-ing the grain sizes in the MAPbBr3 films.At low sub-bandgap pumping intensities,directly exciting the gap states leads to 2-photon,3-photon,and 4-photon up-conversion spontaneous emission,revealing a large optical cross section of multi-photon excitation occurring in such hybrid perovskite films.At moderate pumping intensity(1.19 mJ/cm2)of 700 nm laser excitation,a significant spectral narrowing phenomenon was observed with the full width at half maximum(FWHM)de-creasing from 18 nm to 4 nm at the peak wavelength of 550 nm,simultaneously with a nonlinear increase on spectral peak intensity,showing an up-conversion ASE realized at low threshold pumping fluence.More interestingly,the up-con-version ASE demonstrated a giant magnetic field effect,leading to a magneto-ASE reaching 120%.In contrast,the up-conversion photoluminescence(PL)showed a negligible magnetic field effect(<1%).This observation provides an evid-ence to indicate that the light-emitting states responsible for up-conversion ASE are essentially formed as spatially exten-ded states.The angular dependent spectrum results further verify the existence of spatially extended states which are polarized to develop coherent in-phase interaction.Clearly,using broad gap states with spatially extended light-emitting states presents a new approach to develop up-conversion ASE in organic-inorganic hybrid perovskites.
基金Supported by the National Natural Science Foundation of China under Grant Nos 11874007 and 11574049
文摘An ultra-thin molybdenum(VI)oxide(MoO3)modification layer can significantly improve hole injection from an electrode even though the MoO3 layer does not contact the electrode.We find that as the thickness of the organic layer between MoO3 and the electrode increases,the hole injection first increases and it then decreases.The optimum thickness of 5 nm corresponds to the best current improvement 70%,higher than that in the device where MoO3 directly contacts the Al electrode.According to the 4,4-bis[N-(1-naphthyl)-N-phenyl-amino]biphenyl(NPB)/MoO3 interface charge transfer mechanism and the present experimental results,we propose a mechanism that mobile carriers generated at the interface and accumulated inside the device change the distribution of electric field inside the device,resulting in an increase of the probability of hole tunneling through the injection barrier from the electrode,which also explains the phenomenon of hole injection enhanced by MoO3/NPB/Al composite anode.Based on this mechanism,different organic materials other than NPB were applied to form the composite electrode with MoO3.Similar current enhancement effects are also observed.
基金supported by the National Natural Science Foundation of China(12134010,62074117,and 12174290)the support of the Key R&D program from Hubei Province(2023BAB102)+1 种基金ERC Consolidator Grant(LEAP,101045098)the Swedish Government Strategic Research Area in Materials Science on Functional Materials at Link?ping University(Faculty Grant SFO–Mat–LiU No.2009–00971)。
文摘Perovskite light-emitting diodes(PeLEDs)exhibit remarkable potential in the field of displays and solidstate lighting.However,blue PeLEDs,a key element for practical applications,still lag behind their green and red counterparts,due to a combination of strong nonradiative recombination losses and unoptimized device structures.In this report,we propose a buried interface modification strategy to address these challenges by focusing on the bottom-hole transport layer(HTL)of the PeLEDs.On the one hand,a multifunctional molecule,aminoacetic acid hydrochloride(AACl),is introduced to modify the HTL/perovskite interface to regulate the perovskite crystallization.Experimental investigations and theoretical calculations demonstrate that AACl can effectively reduce the nonradiative recombination losses in bulk perovskites by suppressing the growth of low-n perovskite phases and also the losses at the bottom interface by passivating interfacial defects.On the other hand,a self-assembly nanomesh structure is ingeniously developed within the HTLs.This nanomesh structure is meticulously crafted through the blending of poly-(9,9-dioctyl-fluorene-co-N-(4-butyl phenyl)diphenylamine)and poly(n-vinyl carbazole),significantly enhancing the light outcoupling efficiency in PeLEDs.As a result,our blue PeLEDs achieve remarkable external quantum efficiencies,20.4%at 487 nm and 12.5%at 470 nm,which are among the highest reported values.Our results offer valuable insights and effective methods for achieving high-performance blue PeLEDs.
基金supported by the National Natural Science Foundation of China(Grant Nos.62274135,52250060,and 62288102)supported by the Swedish Energy Agency Energimyndigheten(Nos.P2019-48758 and P2022-00394)+2 种基金the Göran Gustafsson Foundation for Research in Natural Sciences and Medicine and the Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linköping University(Faculty Grant SFO-Mat-LiU No.2009-00971)support from China Scholarship Council(No.202006210284)and Tsinghua Scholarship for short-term overseas graduate studiesby resources provided by the National Academic Infrastructure for Supercomputing in Sweden(NAISS)and the Swedish National Infrastructure for Computing(SNIC)at the National Supercomputer Centre(NSC)and the PDC Center for High Performance Computing partially funded by the Swedish Research Council through grant agreements no.2022-06725 and no.2018-05973.
文摘Although perovskite light-emitting diodes(PeLEDs)have seen unprecedented development in device efciency over the past decade,they sufer signifcantly from poor operational stability.This is especially true for blue PeLEDs,whose operational lifetime remains orders of magnitude behind their green and red counterparts.Here,we systematically investigate this efciency-stability discrepancy in a series of green-to blue-emitting PeLEDs based on mixed Br/Cl-perovskites.We fnd that chloride incorporation,while having only a limited impact on efciency,detrimentally afects device stability even in small amounts.Device lifetime drops exponentially with increasing Cl-content,accompanied by an increased rate of change in electrical properties during operation.We ascribe this phenomenon to an increased mobility of halogen ions in the mixed-halide lattice due to an increased chemically and structurally disordered landscape with reduced migration barriers.Our results indicate that the stability enhancement for PeLEDs might require diferent strategies from those used for improving efciency.
基金supported by the National Natural Science Foundation of China(grant numbers 61774046 and 11374063),and by Shanghai Municipal Natural Science Foundation under Grant Nos.19ZR1402900.
文摘The photovoltaic performance of perovskite solar cell is determined by multiple interrelated factors,such as perovskite compositions,electronic properties of each transport layer and fabrication parameters,which makes it rather challenging for optimization of device performances and discovery of underlying mechanisms.Here,we propose and realize a novel machine learning approach based on forward-reverse framework to establish the relationship between key parameters and photovoltaic performance in high-profile MASnxPb1-xI3 perovskite materials.The proposed method establishes the asymmetrically bowing relationship between band gap and Sn composition,which is precisely verified by our experiments.Based on the analysis of structural evolution and SHAP library,the rapid-change region and low-bandgap plateau region for small and large Sn composition are explained,respectively.By establishing the models for photovoltaic parameters of working photovoltaic devices,the deviation of short-circuit current and open-circuit voltage with band gap in defective-zone and low-bandgap-plateau regions from Shockley-Queisser theory is captured by our models,and the former is due to the deep-level traps formed by crystallographic distortion and the latter is due to the enhanced susceptibility by increased Sn4+content.The more difficulty for hole extraction than electron is also concluded in the models and the prediction curve of power conversion efficiency is in a good agreement with Shockley-Queisser limit.With the help of search and optimization algorithms,an optimized Sn:Pb composition ratio near 0.6 is finally obtained for high-performance perovskite solar cells,then verified by our experiments.Our constructive method could also be applicable to other material optimization and efficient device development.