The increasing dependence on fossil fuels and the consequent CO_(2)emissions have prompted urgent energy and environmental challenges[1,2].Solar-driven CO_(2)conversion into value-added fuels offers a sustainable and ...The increasing dependence on fossil fuels and the consequent CO_(2)emissions have prompted urgent energy and environmental challenges[1,2].Solar-driven CO_(2)conversion into value-added fuels offers a sustainable and promising solution to these issues[3].However,the practical implementation of CO_(2)photoreduction is constrained by low efficiency,primarily due to the rapid recombination of photogenerated electron-hole pairs[4].展开更多
In order to reduce deep level defects, the theory and process design of 4H-SiC homoepitaxial layer implanted by carbon ion are studied. With the Monte Carlo simulator TRIM, the ion implantation range, location of peak...In order to reduce deep level defects, the theory and process design of 4H-SiC homoepitaxial layer implanted by carbon ion are studied. With the Monte Carlo simulator TRIM, the ion implantation range, location of peak concentration and longitudinal straggling of carbon are calculated. The process for improving deep energy level in undoped 4H-SiC homoepitaxial layer by three times carbon ion-implantation is proposed, including implantation energy, dose, the SiO2 resist mask, annealing temperature, annealing time and annealing protection. The deep energy level in 4H-SiC material can be significantly improved by implantation of carbon atoms into a shallow surface layer. The damage of crystal lattice can be repaired well, and the carbon ions are effectively activated after 1 600 ℃ annealing, meanwhile, deep level defects are decreased.展开更多
Focusing on the low open circuit voltage(V_(OC))and fill factor(FF)in flexible Cu_(2)ZnSn(S,Se)_(4)(CZTSSe)solar cells,indium(In)ions are introduced into the CZTSSe absorbers near Mo foils to modify the back interface...Focusing on the low open circuit voltage(V_(OC))and fill factor(FF)in flexible Cu_(2)ZnSn(S,Se)_(4)(CZTSSe)solar cells,indium(In)ions are introduced into the CZTSSe absorbers near Mo foils to modify the back interface and passivate deep level defects in CZTSSe bulk concurrently for improving the performance of flexible device.The results show that In doping effectively inhibits the formation of secondary phase(Cu(S,Se)_(2))and VSndefects.Further studies demonstrate that the barrier height at the back interface is decreased and the deep level defects(Cu_(Sn)defects)in CZTSSe bulk are passivated.Moreover,the carrier concentration is increased and the V_(OC) deficit(V_(OC,def))is decreased significantly due to In doping.Finally,the flexible CZTSSe solar cell with 10.01%power conversion efficiency(PCE)has been obtained.The synergistic strategy of interface modification and bulk defects passivation through In incorporation provides a new thought for the fabrication of efficient flexible kesterite-based solar cells.展开更多
Understanding the defect characteristics that occur near the space-charge regions(SCRs)of kesterite(CZTSSe)solar cells is important because the recombination loss at the CZTSSe/CdS interface is considered the main cau...Understanding the defect characteristics that occur near the space-charge regions(SCRs)of kesterite(CZTSSe)solar cells is important because the recombination loss at the CZTSSe/CdS interface is considered the main cause of their low efficiency.CZTSSe surfaces with different elemental compositions were formed without polishing(C00)and with polishing for 20 s(C20)and 60 s(C60).For C60,a specific region near the SCR was excessively Cu-rich and Zn-poor compared to C00 and C20.Various charged defects formed where the elemental variation was large.As the main deep acceptor defect energy level(E_(a2))near the SCR increased,the efficiency,open-circuit voltage deficit,and current density degraded,and this phenomenon was especially rapid for large E_(a2) values.As the E_(a2) near the SCR became deep,the carrier diffusion length decreased more for the CZTSSe solar cells with a low carrier mobility than for the CuInGaSe_(2)(CIGSe)solar cells.The large amplitude of the electrostatic potential fluctuation in the CZTSSe solar cells induced a high carrier recombination and a short carrier lifetime.Consequently,the properties of the CZTSSe solar cells were more strongly degraded by defects with deep energy levels near the SCR than those of the CIGSe solar cells.展开更多
A new photocatalyst,PdS@NH_(2)-MIL-125(Ti)@ZnS(PdS/M125/ZnS)heterojunction is fabricated for photo-catalytic H_(2)generation for the first time,where PdS nanoparticles are anchored in the pore of M125 by utilizing its...A new photocatalyst,PdS@NH_(2)-MIL-125(Ti)@ZnS(PdS/M125/ZnS)heterojunction is fabricated for photo-catalytic H_(2)generation for the first time,where PdS nanoparticles are anchored in the pore of M125 by utilizing its confinement effect,and the ZnS is closely wrapped on the surfaces of the MOFs.The optimal photocatalyst exhibits a significantly enhanced H_(2)generation rate of 1164.2μmol/g/h,while the pure M125 only displays a H_(2)generation rate of 16.7μmol/g/h.The resultant improvement can be ascribed to the following comprehensive advantages.The hierarchical structure built by PdS,M125,and ZnS can form lots of intimate interfaces,offer abundant sites for reaction,and smooth channels for charge carri-ers due to the porous characteristics of MOFs.Moreover,M125 and ZnS with inner defect levels form an analogous type-II heterojunction assisted by PdS co-catalyst,which greatly promotes charge separation.This work may supply a new avenue to design MOFs photocatalysts for energy conversion.展开更多
The intrinsic defect of cadmium vacancy （Vcd） in cadmium telluride （CdTe） has been studied by first-principles cal- culations using potentials with both the screened hybrid functional of Heyd, Scuseria, and Ernzer...The intrinsic defect of cadmium vacancy （Vcd） in cadmium telluride （CdTe） has been studied by first-principles cal- culations using potentials with both the screened hybrid functional of Heyd, Scuseria, and Ernzerhof （HSE） approximation and the generalized gradient approximation of the Perdew-Burke-Ernzerhof form （PBE-GGA）. Both results show that the Ta structure of the Vctl defect for different charges is the most stable structure as compared with the distorted C3v structure with one hole localized at one of the four nearest Te atoms. This indicates that the John-Teller distortion （C3v） structure may be unstable in bulk CdTe crystal. The reason likely lies in the delocalized resonance nature of the t2 state of the Vcd defect. Moreover, the formation energy obtained by the HSE method is about 0.6-0.8 eV larger than that obtained by the PBE method. The transition levels calculated by the PBE method and the HSE method are similar and well consistent with the experimental results.展开更多
TiO 2 films have been deposited on glass substrates using DC reactive magnetron sputtering at different oxygen partial pressures from 0.10Pa to 0.65Pa.The transmittance (UV vis) and photoluminescence (PL) spectra of...TiO 2 films have been deposited on glass substrates using DC reactive magnetron sputtering at different oxygen partial pressures from 0.10Pa to 0.65Pa.The transmittance (UV vis) and photoluminescence (PL) spectra of the films were recorded.The results of the UV vis spectra show that the deposition rate of the films decreased at oxygen partial pressure P(O 2)≥0.15Pa,the band gap increased from 3.48eV to 3.68eV for direct transition and from 3.27eV to 3.34eV for indirect transition with increasing the oxygen partial pressure.The PL spectra show convincingly that the transtion for films was indirect,and there were some oxygen defect energy levels at the band gap of the films.With increasing the O 2 partial pressure,the defect energy levels decreased.For the films sputtered at 0.35 and 0.65Pa there were two defect energy levels at 2.63eV and 2.41eV,corresponding to 0.72eV and 0.94eV below the conduction band for a band gap of 3.35eV,respectively.For the films sputtered at 0.10Pa and 0.15Pa,there was an energy band formed between 3.12eV and 2.06eV,corresponding to 0.23eV and 1.29eV below the conduction band.展开更多
Secondary electron emission(SEE)induced by the positive ion is an essential physical process to influence the dynamics of gas discharge which relies on the specific surface material.Surface charging has a significant ...Secondary electron emission(SEE)induced by the positive ion is an essential physical process to influence the dynamics of gas discharge which relies on the specific surface material.Surface charging has a significant impact on the material properties,thereby affecting the SEE in the plasma-surface interactions.However,it does not attract enough attention in the previous studies.In this paper,SEE dependent on the charged surface of specific materials is described with the computational method combining a density functional theory(DFT)model from the first-principle theory and the theory of Auger neutralization.The effect ofκ-Al2O3 surface charge,as an example,on the ion-induced secondary electron emission coefficient(SEEC)is investigated by analyzing the defect energy level and band structure on the charged surface.Simulation results indicate that,with the surface charge from negative to positive,the SEEC of a part of low ionization energy ions(such as Ei=12.6 eV)increases first and then decreases,exhibiting a nonlinear changing trend.This is quite different from the monotonic decreasing tendency observed in the previous model which simplifies the electronic structure.This irregular increase of the SEEC can be attributed to the lower escaped probability of orbital energy.The results further illustrate that the excessive charge could cause the bottom of the conduction band close to the valence band,thus leading to the decrease of the orbital energy occupied by the excited electrons.The nonlinear change of SEEC demonstrates a more realistic situation of how the electronic structure of material surface influences the SEE process.This work provides an accurate method of calculating SEEC from specific materials,which is urgent in widespread physical scenarios sensitive to surface materials,such as increasingly growing practical applications concerning plasma-surface interactions.展开更多
Unintentionally doped 4H-SiC homoepitaxial layers grown by hot-wall chemical vapor deposition （HWCVD） have been studied using photoluminescence （PL） technique in the temperature range of 10 to 240 K. A broadband g...Unintentionally doped 4H-SiC homoepitaxial layers grown by hot-wall chemical vapor deposition （HWCVD） have been studied using photoluminescence （PL） technique in the temperature range of 10 to 240 K. A broadband green luminescence has been observed. Vacancies of carbon （Vc） are revealed by electron spin resonance （ESR） technique at 110 K. The results strongly suggest that the green band luminescence, as shallow donor-deep accepter emission, is attributed to the vacancies of C and the extended defects. The broadband green luminescence spectrum can be fitted by the two Gauss-type spectra using nonlinear optimization technique. It shows that the broad-band green luminescence originates from the combination of two independent radiative transitions. The centers of two energy levels are located 2.378 and 2.130 eV below the conduction band, respectively, and the ends of two energy levels are expanded and superimposed each other.展开更多
All-inorganic perovskites are advantageous in terms of improved thermal stability compared to organic-inorganic counterparts.However,the ion migration-induced hysteresis significantly undermines the long-term operatio...All-inorganic perovskites are advantageous in terms of improved thermal stability compared to organic-inorganic counterparts.However,the ion migration-induced hysteresis significantly undermines the long-term operational stability of all-inorganic perovskite solar cells(PSCs),particularly in mixed halide perovskites.Herein,we report that tin-lead(Sn-Pb)alloying for all-inorganic mixed halide perovskites can effectively inhibit the ion migration behavior,as comprehensively revealed by the time-of-flight secondary ion mass spectrometry(TOF-SIMS),optical microscopy and galvanostatic measurements.On one hand,the small-sized Sn2+cations can tighten the lattice structure to enhance the Pb/Sn-X(X=I and Br)ionic bonds,thereby effectively immobilizing the halide ions.On the other hand,Sn substitution can significantly reduce anti-site defects,such as I_(Cs)and I_(Pb),which are considered potential pathways for ion migration.With these advantages,ion migration is greatly suppressed in Sn-Pb alloyed inorganic perovskites,resulting in reduced hysteresis and improved operational stability of PSC devices.展开更多
The transition among multiple charging states of a semiconductor＇s localized intrinsic/impurity defects is considered as phase transitions, and the concept of transition Gibbs free energy level （TGFEL） is proposed....The transition among multiple charging states of a semiconductor＇s localized intrinsic/impurity defects is considered as phase transitions, and the concept of transition Gibbs free energy level （TGFEL） is proposed. Dependence of the cross section of TGFEL on its charge state is discussed. Introduction of TGFEL to replace acti- vation energy has fundamentally important consequences for semiconductor physics and devices. TGFEL involves entropy. What is to be included and not included in the entropy term consistently for all defect levels is an unre- solved open question, related to correct interpretation of various experimental data associated with various defect levels. This work is a first step towards resolving this question.展开更多
文摘The increasing dependence on fossil fuels and the consequent CO_(2)emissions have prompted urgent energy and environmental challenges[1,2].Solar-driven CO_(2)conversion into value-added fuels offers a sustainable and promising solution to these issues[3].However,the practical implementation of CO_(2)photoreduction is constrained by low efficiency,primarily due to the rapid recombination of photogenerated electron-hole pairs[4].
基金Supported by the National Natural Science Foundation of China (No. 61006008)Xi'an Applied Materials Innovation Fund (No. XA-AM-200607)
文摘In order to reduce deep level defects, the theory and process design of 4H-SiC homoepitaxial layer implanted by carbon ion are studied. With the Monte Carlo simulator TRIM, the ion implantation range, location of peak concentration and longitudinal straggling of carbon are calculated. The process for improving deep energy level in undoped 4H-SiC homoepitaxial layer by three times carbon ion-implantation is proposed, including implantation energy, dose, the SiO2 resist mask, annealing temperature, annealing time and annealing protection. The deep energy level in 4H-SiC material can be significantly improved by implantation of carbon atoms into a shallow surface layer. The damage of crystal lattice can be repaired well, and the carbon ions are effectively activated after 1 600 ℃ annealing, meanwhile, deep level defects are decreased.
基金supported by the National Natural Science Foundation of China(62074037)the Science and Technology Department of Fujian Province(2020I0006)the Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China(2021ZZ124)。
文摘Focusing on the low open circuit voltage(V_(OC))and fill factor(FF)in flexible Cu_(2)ZnSn(S,Se)_(4)(CZTSSe)solar cells,indium(In)ions are introduced into the CZTSSe absorbers near Mo foils to modify the back interface and passivate deep level defects in CZTSSe bulk concurrently for improving the performance of flexible device.The results show that In doping effectively inhibits the formation of secondary phase(Cu(S,Se)_(2))and VSndefects.Further studies demonstrate that the barrier height at the back interface is decreased and the deep level defects(Cu_(Sn)defects)in CZTSSe bulk are passivated.Moreover,the carrier concentration is increased and the V_(OC) deficit(V_(OC,def))is decreased significantly due to In doping.Finally,the flexible CZTSSe solar cell with 10.01%power conversion efficiency(PCE)has been obtained.The synergistic strategy of interface modification and bulk defects passivation through In incorporation provides a new thought for the fabrication of efficient flexible kesterite-based solar cells.
基金the National Research Foundation of Korea(NRF)grant funded by the Ministry of Science and ICT(No.2022M3J1A1085371)the DGIST R&D programs of the Ministry of Science and ICT(23-ET-08 and 23-CoE-ET-01)the National Research Foundation of Korea(NRF),funded by the Korean Government(NRF-2021R1A2C1008598).
文摘Understanding the defect characteristics that occur near the space-charge regions(SCRs)of kesterite(CZTSSe)solar cells is important because the recombination loss at the CZTSSe/CdS interface is considered the main cause of their low efficiency.CZTSSe surfaces with different elemental compositions were formed without polishing(C00)and with polishing for 20 s(C20)and 60 s(C60).For C60,a specific region near the SCR was excessively Cu-rich and Zn-poor compared to C00 and C20.Various charged defects formed where the elemental variation was large.As the main deep acceptor defect energy level(E_(a2))near the SCR increased,the efficiency,open-circuit voltage deficit,and current density degraded,and this phenomenon was especially rapid for large E_(a2) values.As the E_(a2) near the SCR became deep,the carrier diffusion length decreased more for the CZTSSe solar cells with a low carrier mobility than for the CuInGaSe_(2)(CIGSe)solar cells.The large amplitude of the electrostatic potential fluctuation in the CZTSSe solar cells induced a high carrier recombination and a short carrier lifetime.Consequently,the properties of the CZTSSe solar cells were more strongly degraded by defects with deep energy levels near the SCR than those of the CIGSe solar cells.
基金This work was financially supported by the Guangdong Basic and Applied Basic Research Foundation(No.207079374034)the State Key Laboratory of Solidification Processing(No.2021-BJ-04)the State Key Laboratory for Mechanical Behavior of Materials(No.20222421)。
文摘A new photocatalyst,PdS@NH_(2)-MIL-125(Ti)@ZnS(PdS/M125/ZnS)heterojunction is fabricated for photo-catalytic H_(2)generation for the first time,where PdS nanoparticles are anchored in the pore of M125 by utilizing its confinement effect,and the ZnS is closely wrapped on the surfaces of the MOFs.The optimal photocatalyst exhibits a significantly enhanced H_(2)generation rate of 1164.2μmol/g/h,while the pure M125 only displays a H_(2)generation rate of 16.7μmol/g/h.The resultant improvement can be ascribed to the following comprehensive advantages.The hierarchical structure built by PdS,M125,and ZnS can form lots of intimate interfaces,offer abundant sites for reaction,and smooth channels for charge carri-ers due to the porous characteristics of MOFs.Moreover,M125 and ZnS with inner defect levels form an analogous type-II heterojunction assisted by PdS co-catalyst,which greatly promotes charge separation.This work may supply a new avenue to design MOFs photocatalysts for energy conversion.
基金supported by the National Natural Science Foundation of China(Grant No.A050506)the Innovation Program of Shanghai Municipal Education Commission,China(Grant No.12ZZ096)+1 种基金the Shanghai Leading Academic Disciplines,China(Grant No.S30107)the Science and Technology Commissionof Shanghai,China(Grant No.11530500200)
文摘The intrinsic defect of cadmium vacancy （Vcd） in cadmium telluride （CdTe） has been studied by first-principles cal- culations using potentials with both the screened hybrid functional of Heyd, Scuseria, and Ernzerhof （HSE） approximation and the generalized gradient approximation of the Perdew-Burke-Ernzerhof form （PBE-GGA）. Both results show that the Ta structure of the Vctl defect for different charges is the most stable structure as compared with the distorted C3v structure with one hole localized at one of the four nearest Te atoms. This indicates that the John-Teller distortion （C3v） structure may be unstable in bulk CdTe crystal. The reason likely lies in the delocalized resonance nature of the t2 state of the Vcd defect. Moreover, the formation energy obtained by the HSE method is about 0.6-0.8 eV larger than that obtained by the PBE method. The transition levels calculated by the PBE method and the HSE method are similar and well consistent with the experimental results.
文摘TiO 2 films have been deposited on glass substrates using DC reactive magnetron sputtering at different oxygen partial pressures from 0.10Pa to 0.65Pa.The transmittance (UV vis) and photoluminescence (PL) spectra of the films were recorded.The results of the UV vis spectra show that the deposition rate of the films decreased at oxygen partial pressure P(O 2)≥0.15Pa,the band gap increased from 3.48eV to 3.68eV for direct transition and from 3.27eV to 3.34eV for indirect transition with increasing the oxygen partial pressure.The PL spectra show convincingly that the transtion for films was indirect,and there were some oxygen defect energy levels at the band gap of the films.With increasing the O 2 partial pressure,the defect energy levels decreased.For the films sputtered at 0.35 and 0.65Pa there were two defect energy levels at 2.63eV and 2.41eV,corresponding to 0.72eV and 0.94eV below the conduction band for a band gap of 3.35eV,respectively.For the films sputtered at 0.10Pa and 0.15Pa,there was an energy band formed between 3.12eV and 2.06eV,corresponding to 0.23eV and 1.29eV below the conduction band.
基金supported by the National Key Research and Development Plan of China(No.2021YFE0114700)National Natural Science Foundation of China(No.52377145).
文摘Secondary electron emission(SEE)induced by the positive ion is an essential physical process to influence the dynamics of gas discharge which relies on the specific surface material.Surface charging has a significant impact on the material properties,thereby affecting the SEE in the plasma-surface interactions.However,it does not attract enough attention in the previous studies.In this paper,SEE dependent on the charged surface of specific materials is described with the computational method combining a density functional theory(DFT)model from the first-principle theory and the theory of Auger neutralization.The effect ofκ-Al2O3 surface charge,as an example,on the ion-induced secondary electron emission coefficient(SEEC)is investigated by analyzing the defect energy level and band structure on the charged surface.Simulation results indicate that,with the surface charge from negative to positive,the SEEC of a part of low ionization energy ions(such as Ei=12.6 eV)increases first and then decreases,exhibiting a nonlinear changing trend.This is quite different from the monotonic decreasing tendency observed in the previous model which simplifies the electronic structure.This irregular increase of the SEEC can be attributed to the lower escaped probability of orbital energy.The results further illustrate that the excessive charge could cause the bottom of the conduction band close to the valence band,thus leading to the decrease of the orbital energy occupied by the excited electrons.The nonlinear change of SEEC demonstrates a more realistic situation of how the electronic structure of material surface influences the SEE process.This work provides an accurate method of calculating SEEC from specific materials,which is urgent in widespread physical scenarios sensitive to surface materials,such as increasingly growing practical applications concerning plasma-surface interactions.
基金supported by the State Key Development Program for Basic Research of China (No. 51327020202)the Key Fund of the Ministryof Education of China (No. 106150)the Xi’an Applied Materials Innovation Fund (No. XA-AM-200607).
文摘Unintentionally doped 4H-SiC homoepitaxial layers grown by hot-wall chemical vapor deposition （HWCVD） have been studied using photoluminescence （PL） technique in the temperature range of 10 to 240 K. A broadband green luminescence has been observed. Vacancies of carbon （Vc） are revealed by electron spin resonance （ESR） technique at 110 K. The results strongly suggest that the green band luminescence, as shallow donor-deep accepter emission, is attributed to the vacancies of C and the extended defects. The broadband green luminescence spectrum can be fitted by the two Gauss-type spectra using nonlinear optimization technique. It shows that the broad-band green luminescence originates from the combination of two independent radiative transitions. The centers of two energy levels are located 2.378 and 2.130 eV below the conduction band, respectively, and the ends of two energy levels are expanded and superimposed each other.
基金supported by National Natural Science Foundation of China(Nos.51925206 and 52461160328)the Strategic Priority Research Program of the Chinese Academy of Sciences(XDB0450301)the Fundamental Research Funds for the Central Universities(20720220009,WK2490000002).
文摘All-inorganic perovskites are advantageous in terms of improved thermal stability compared to organic-inorganic counterparts.However,the ion migration-induced hysteresis significantly undermines the long-term operational stability of all-inorganic perovskite solar cells(PSCs),particularly in mixed halide perovskites.Herein,we report that tin-lead(Sn-Pb)alloying for all-inorganic mixed halide perovskites can effectively inhibit the ion migration behavior,as comprehensively revealed by the time-of-flight secondary ion mass spectrometry(TOF-SIMS),optical microscopy and galvanostatic measurements.On one hand,the small-sized Sn2+cations can tighten the lattice structure to enhance the Pb/Sn-X(X=I and Br)ionic bonds,thereby effectively immobilizing the halide ions.On the other hand,Sn substitution can significantly reduce anti-site defects,such as I_(Cs)and I_(Pb),which are considered potential pathways for ion migration.With these advantages,ion migration is greatly suppressed in Sn-Pb alloyed inorganic perovskites,resulting in reduced hysteresis and improved operational stability of PSC devices.
基金support from CNBM (China National Building Materials) Group for its partial financial support of the work
文摘The transition among multiple charging states of a semiconductor＇s localized intrinsic/impurity defects is considered as phase transitions, and the concept of transition Gibbs free energy level （TGFEL） is proposed. Dependence of the cross section of TGFEL on its charge state is discussed. Introduction of TGFEL to replace acti- vation energy has fundamentally important consequences for semiconductor physics and devices. TGFEL involves entropy. What is to be included and not included in the entropy term consistently for all defect levels is an unre- solved open question, related to correct interpretation of various experimental data associated with various defect levels. This work is a first step towards resolving this question.
