Formamidine lead triiodide(FAPbI_(3))perovskites have become the most promising photovoltaic materials for perovskite solar cells with record power conversion efficiency(PCE).However,random nucleation,phase transition...Formamidine lead triiodide(FAPbI_(3))perovskites have become the most promising photovoltaic materials for perovskite solar cells with record power conversion efficiency(PCE).However,random nucleation,phase transition,and lattice defects are still the key challenges limiting the quality of FAPbI_(3) films.Previous studies show that the introduction or adding of seeds in the precursor is effective to promote the nucleation and crystallization of perovskite films.Nevertheless,the seed-assisted approach focuses on heterogeneous seeds or hetero-composites,which inevitably induce a lattice-mismatch,the genera-tion of strain or defects,and the phase segregation in the perovskite films.Herein,we first demonstrate that high-quality perovskite films are controllably prepared using α-and δ-phases mixed FAPbI_(3) micro-crystal as the homogeneous seeds with the one-step antisolvent method.The partially dissolved seeds with suitable sizes improve the crystallinity of the perovskite flm with preferable orientation,improved carrier lifetime,and increased carrier mobility.More importantly,the α-phase-containing seeds promote the formation of α-phase FAPbI_(3) films,leading to the reduction of residual lattice strain and the suppres-sion of I-ion migration.Besides,the adding of dimethyl 2,6-pyridine dicarboxylate(DPD)into the pre-cursor further suppresses the generation of defects,contributing to the PCE of devices prepared in air ambient being significantly improved to 23.75%,among the highest PCEs for fully air-processed FAPbI_(3) solar cells.The unpackaged target devices possess a high stability,maintaining 80%of the initial PCE under simulated solar illumination exceeding 800 h.展开更多
Molten-alkali etching has been widely used to reveal dislocations in 4H silicon carbide(4H-SiC),which has promoted the identification and statistics of dislocation density in 4H-SiC single crystals.However,the etching...Molten-alkali etching has been widely used to reveal dislocations in 4H silicon carbide(4H-SiC),which has promoted the identification and statistics of dislocation density in 4H-SiC single crystals.However,the etching mechanism of 4H-SiC is limited misunderstood.In this letter,we reveal the anisotropic etching mechanism of the Si face and C face of 4H-SiC by combining molten-KOH etching,X-ray photoelectron spectroscopy(XPS)and first-principles investigations.The activation energies for the molten-KOH etching of the C face and Si face of 4H-SiC are calculated to be 25.09 and 35.75 kcal/mol,respectively.The molten-KOH etching rate of the C face is higher than the Si face.Combining XPS analysis and first-principles calculations,we find that the molten-KOH etching of 4H-SiC is proceeded by the cycling of the oxidation of 4H-SiC by the dissolved oxygen and the removal of oxides by molten KOH.The faster etching rate of the C face is caused by the fact that the oxides on the C face are unstable,and easier to be removed with molten alkali,rather than the C face being easier to be oxidized.展开更多
Discrimination of dislocations is critical to the statistics of dislocation densities in 4H silicon carbide(4H-SiC),which are routinely used to evaluate the quality of 4H-SiC single crystals and homoepitaxial layers.I...Discrimination of dislocations is critical to the statistics of dislocation densities in 4H silicon carbide(4H-SiC),which are routinely used to evaluate the quality of 4H-SiC single crystals and homoepitaxial layers.In this work,we show that the inclination angles of the etch pits of molten-alkali etched 4H-SiC can be adopted to discriminate threading screw dislocations(TSDs),threading edge dislocations(TEDs)and basal plane dislocations(BPDs)in 4H-SiC.In n-type 4H-SiC,the inclination angles of the etch pits of TSDs,TEDs and BPDs in molten-alkali etched 4H-SiC are in the ranges of 27°−35°,8°−15°and 2°−4°,respectively.In semi-insulating 4H-SiC,the inclination angles of the etch pits of TSDs and TEDs are in the ranges of 31°−34°and 21°−24°,respectively.The inclination angles of dislocation-related etch pits are independent of the etching duration,which facilitates the discrimination and statistic of dislocations in 4H-SiC.More significantly,the inclination angle of a threading mixed dislocations(TMDs)is found to consist of characteristic angles of both TEDs and TSDs.This enables to distinguish TMDs from TSDs in 4H-SiC.展开更多
4H silicon carbide(4H-SiC)has gained a great success in high-power electronics,owing to its advantages of wide bandgap,high breakdown electric field strength,high carrier mobility,and high thermal conductivity.Conside...4H silicon carbide(4H-SiC)has gained a great success in high-power electronics,owing to its advantages of wide bandgap,high breakdown electric field strength,high carrier mobility,and high thermal conductivity.Considering the high carrier mobility and high stability of 4H-SiC,4H-SiC has great potential in the field of photoelectrochemical(PEC)water splitting.In this work,we demonstrate the irradiation-resistant PEC water splitting based on nanoporous 4H-SiC arrays.A new two-step anodizing approach is adopted to prepare 4H-SiC nanoporous arrays with different porosity,that is,a constant low-voltage etching followed by a pulsed high-voltage etching.The constant-voltage etching and pulsed-voltage etching are adopted to control the diameter of the nanopores and the depth of the nanoporous arrays,respectively.It is found that the nanoporous arrays with medium porosity has the highest PEC current,because of the enhanced light absorption and the optimized transportation of charge carriers along the walls of the nanoporous arrays.The performance of the PEC water splitting of the nanoporous arrays is stable after the electron irradiation with the dose of 800 and 1600 k Gy,which indicates that 4H-SiC nanoporous arrays has great potential in the PEC water splitting under harsh environments.展开更多
基金supported by the National Natural Science Foundation of China (61604131,62025403)the Natural Science Foundation of Zhejiang Province (LY19F040009)+1 种基金the Fundamental Research Funds of Zhejiang SciTech University (23062120-Y)the Open Project of Key Laboratory of Solar Energy Utilization and Energy Saving Technology of Zhejiang Province (ZJS-OP-2020-07)
文摘Formamidine lead triiodide(FAPbI_(3))perovskites have become the most promising photovoltaic materials for perovskite solar cells with record power conversion efficiency(PCE).However,random nucleation,phase transition,and lattice defects are still the key challenges limiting the quality of FAPbI_(3) films.Previous studies show that the introduction or adding of seeds in the precursor is effective to promote the nucleation and crystallization of perovskite films.Nevertheless,the seed-assisted approach focuses on heterogeneous seeds or hetero-composites,which inevitably induce a lattice-mismatch,the genera-tion of strain or defects,and the phase segregation in the perovskite films.Herein,we first demonstrate that high-quality perovskite films are controllably prepared using α-and δ-phases mixed FAPbI_(3) micro-crystal as the homogeneous seeds with the one-step antisolvent method.The partially dissolved seeds with suitable sizes improve the crystallinity of the perovskite flm with preferable orientation,improved carrier lifetime,and increased carrier mobility.More importantly,the α-phase-containing seeds promote the formation of α-phase FAPbI_(3) films,leading to the reduction of residual lattice strain and the suppres-sion of I-ion migration.Besides,the adding of dimethyl 2,6-pyridine dicarboxylate(DPD)into the pre-cursor further suppresses the generation of defects,contributing to the PCE of devices prepared in air ambient being significantly improved to 23.75%,among the highest PCEs for fully air-processed FAPbI_(3) solar cells.The unpackaged target devices possess a high stability,maintaining 80%of the initial PCE under simulated solar illumination exceeding 800 h.
基金This work is supported by the Natural Science Foundation of China(Grant Nos.62274143&62204216)Joint Funds of the Zhejiang Provincial Natural Science Foundation of China(Grant Nos.LHZSD24E020001)+4 种基金the“Pioneer”and“Leading Goose”R&D Program of Zhejiang(Grant Nos.2022C0102&2023C01010)Partial support was provided by the Leading Innovative and Entrepreneur Team Introduction Program of Hangzhou(Grant No.TD2022012)Fundamental Research Funds for the Central Universities(Grant No.226-2022-00200)the Natural Science Foundation of China for Innovative Research Groups(Grant No.61721005)the Open Fund of Zhejiang Provincial Key Laboratory of Wide Bandgap Semiconductors,Hangzhou Global Scientific and Technological Innovation Center,Zhejiang University.
文摘Molten-alkali etching has been widely used to reveal dislocations in 4H silicon carbide(4H-SiC),which has promoted the identification and statistics of dislocation density in 4H-SiC single crystals.However,the etching mechanism of 4H-SiC is limited misunderstood.In this letter,we reveal the anisotropic etching mechanism of the Si face and C face of 4H-SiC by combining molten-KOH etching,X-ray photoelectron spectroscopy(XPS)and first-principles investigations.The activation energies for the molten-KOH etching of the C face and Si face of 4H-SiC are calculated to be 25.09 and 35.75 kcal/mol,respectively.The molten-KOH etching rate of the C face is higher than the Si face.Combining XPS analysis and first-principles calculations,we find that the molten-KOH etching of 4H-SiC is proceeded by the cycling of the oxidation of 4H-SiC by the dissolved oxygen and the removal of oxides by molten KOH.The faster etching rate of the C face is caused by the fact that the oxides on the C face are unstable,and easier to be removed with molten alkali,rather than the C face being easier to be oxidized.
基金supported by“Pioneer”and“Leading Goose”R&D Program of Zhejiang(Grant No.2022C01021)National Key Research and Development Program of China(Grant Nos.2018YFB2200101)+3 种基金Natural Science Foundation of China(Grant Nos.61774133)Fundamental Research Funds for the Central Universities(Grant No.2018XZZX003-02)Natural Science Foundation of China for Innovative Research Groups(Grant No.61721005)Zhejiang University Education Foundation Global Partnership Fund.
文摘Discrimination of dislocations is critical to the statistics of dislocation densities in 4H silicon carbide(4H-SiC),which are routinely used to evaluate the quality of 4H-SiC single crystals and homoepitaxial layers.In this work,we show that the inclination angles of the etch pits of molten-alkali etched 4H-SiC can be adopted to discriminate threading screw dislocations(TSDs),threading edge dislocations(TEDs)and basal plane dislocations(BPDs)in 4H-SiC.In n-type 4H-SiC,the inclination angles of the etch pits of TSDs,TEDs and BPDs in molten-alkali etched 4H-SiC are in the ranges of 27°−35°,8°−15°and 2°−4°,respectively.In semi-insulating 4H-SiC,the inclination angles of the etch pits of TSDs and TEDs are in the ranges of 31°−34°and 21°−24°,respectively.The inclination angles of dislocation-related etch pits are independent of the etching duration,which facilitates the discrimination and statistic of dislocations in 4H-SiC.More significantly,the inclination angle of a threading mixed dislocations(TMDs)is found to consist of characteristic angles of both TEDs and TSDs.This enables to distinguish TMDs from TSDs in 4H-SiC.
基金supported by National Natural Science Foundation of China(Grant Nos.62274143 and U22A2075)Hangzhou Joint Funds of the Zhejiang Provincial Natural Science Foundation of China(Grant No.LHZSD24E020001)+3 种基金Partial support was provided by Leading Innovative and Entrepreneur Team Introduction Program of Hangzhou(Grant No.TD2022012)Fundamental Research Funds for the Central Universities(Grant No.226-2022-00200)Natural Science Foundation of China for Innovative Research Groups(Grant No.61721005)the Open Fund of Zhejiang Provincial Key Laboratory of Wide Bandgap Semiconductors。
文摘4H silicon carbide(4H-SiC)has gained a great success in high-power electronics,owing to its advantages of wide bandgap,high breakdown electric field strength,high carrier mobility,and high thermal conductivity.Considering the high carrier mobility and high stability of 4H-SiC,4H-SiC has great potential in the field of photoelectrochemical(PEC)water splitting.In this work,we demonstrate the irradiation-resistant PEC water splitting based on nanoporous 4H-SiC arrays.A new two-step anodizing approach is adopted to prepare 4H-SiC nanoporous arrays with different porosity,that is,a constant low-voltage etching followed by a pulsed high-voltage etching.The constant-voltage etching and pulsed-voltage etching are adopted to control the diameter of the nanopores and the depth of the nanoporous arrays,respectively.It is found that the nanoporous arrays with medium porosity has the highest PEC current,because of the enhanced light absorption and the optimized transportation of charge carriers along the walls of the nanoporous arrays.The performance of the PEC water splitting of the nanoporous arrays is stable after the electron irradiation with the dose of 800 and 1600 k Gy,which indicates that 4H-SiC nanoporous arrays has great potential in the PEC water splitting under harsh environments.
