The presence of SnZn-related defects in Cu_(2)ZnSn(S,Se)_(4)(CZTSSe)absorber results in large irreversible energy loss and extra irreversible electron-hole non-radiative recombination,thus hindering the efficiency enh...The presence of SnZn-related defects in Cu_(2)ZnSn(S,Se)_(4)(CZTSSe)absorber results in large irreversible energy loss and extra irreversible electron-hole non-radiative recombination,thus hindering the efficiency enhancement of CZTSSe devices.Although the incorporation of Ag in CZTSSe can effectively suppress the SnZn-related defects and significantly improve the resulting cell performance,an excellent efficiency has not been achieved to date primarily owing to the poor electrical-conductivity and the low carrier density of the CZTSSe film induced by Ag substitution.Herein,this study exquisitely devises an Ag/H co-doping strategy in CZTSSe absorber via Ag substitution programs followed by hydrogen-plasma treatment procedure to suppress SnZn defects for achieving efficient CZTSSe devices.In-depth investigation results demonstrate that the incorporation of H in Ag-based CZTSSe absorber is expected to improve the poor electrical-conductivity and the low carrier density caused by Ag substitution.Importantly,the C=O and O-H functional groups induced by hydrogen incorporation,serving as an electron donor,can interact with under-coordinated cations in CZTSSe material,effectively passivating the SnZn-related defects.Consequently,the incorporation of an appropriate amount of Ag/H in CZTSSe mitigates carrier non-radiative recombination,prolongs minority carrier lifetime,and thus yields a champion efficiency of 14.74%,showing its promising application in kesterite-based CZTSSe devices.展开更多
Metal halide perovskites,particularly the quasi-two-dimensional perovskite subclass,have exhibited considerable potential for next-generation electroluminescent materials for lighting and display.Nevertheless,the pres...Metal halide perovskites,particularly the quasi-two-dimensional perovskite subclass,have exhibited considerable potential for next-generation electroluminescent materials for lighting and display.Nevertheless,the presence of defects within these perovskites has a substantial influence on the emission efficiency and durability of the devices.In this study,we revealed a synergistic passivation mechanism on perovskite films by using a dual-functional compound of potassium bromide.The dual functional potassium bromide on the one hand can passivate the defects of halide vacancies with bromine anions and,on the other hand,can screen the charged defects at the grain boundaries with potassium cations.This approach effectively reduces the probability of carriers quenching resulting from charged defects capture and consequently enhances the radiative recombination efficiency of perovskite thin films,leading to a significant enhancement of photoluminescence quantum yield to near-unity values(95%).Meanwhile,the potassium bromide treatment promoted the growth of homogeneous and smooth film,facilitating the charge carrier injection in the devices.Consequently,the perovskite light-emitting diodes based on this strategy achieve a maximum external quantum efficiency of~21%and maximum luminance of~60,000 cd m^(-2).This work provides a deeper insight into the passivation mechanism of ionic compound additives in perovskite with the solution method.展开更多
The function of solid electrolytes and the composition of solid electrolyte interphase(SEI)are highly significant for inhibiting the growth of Li dendrites.Herein,we report an in-situ interfacial passivation combined ...The function of solid electrolytes and the composition of solid electrolyte interphase(SEI)are highly significant for inhibiting the growth of Li dendrites.Herein,we report an in-situ interfacial passivation combined with self-adaptability strategy to reinforce Li_(0.33)La_(0.557)TiO_(3)(LLTO)-based solid-state batteries.Specifically,a functional SEI enriched with LiF/Li_(3)PO_(4) is formed by in-situ electrochemical conversion,which is greatly beneficial to improving interface compatibility and enhancing ion transport.While the polarized dielectric BaTiO_(3)-polyamic acid(BTO-PAA,BP)film greatly improves the Li-ion transport kinetics and homogenizes the Li deposition.As expected,the resulting electrolyte offers considerable ionic conductivity at room temperature(4.3 x 10~(-4)S cm^(-1))and appreciable electrochemical decomposition voltage(5.23 V)after electrochemical passivation.For Li-LiFePO_(4) batteries,it shows a high specific capacity of 153 mA h g^(-1)at 0.2C after 100 cycles and a long-term durability of 115 mA h g^(-1)at 1.0 C after 800 cycles.Additionally,a stable Li plating/stripping can be achieved for more than 900 h at 0.5 mA cm^(-2).The stabilization mechanisms are elucidated by ex-situ XRD,ex-situ XPS,and ex-situ FTIR techniques,and the corresponding results reveal that the interfacial passivation combined with polarization effect is an effective strategy for improving the electrochemical performance.The present study provides a deeper insight into the dynamic adjustment of electrode-electrolyte interfacial for solid-state lithium batteries.展开更多
Rational interface engineering is essential for minimizing interfacial nonradiative recombination losses and enhancing device performance.Herein,we report the use of bidentate diphenoxybenzene(DPOB)isomers as surface ...Rational interface engineering is essential for minimizing interfacial nonradiative recombination losses and enhancing device performance.Herein,we report the use of bidentate diphenoxybenzene(DPOB)isomers as surface modifiers for perovskite films.The DPOB molecules,which contain two oxygen(O)atoms,chemically bond with undercoordinated Pb^(2+) on the surface of perovskite films,resulting in compression of the perovskite lattice.This chemical interaction,along with physical regulations,leads to the formation of high-quality perovskite films with compressive strain and fewer defects.This compressive strain-induced band bending promotes hole extraction and transport,while inhibiting charge recombination at the interfaces.Furthermore,the addition of DPOB will reduce the zero-dimensional(OD) Cs_4PbBr_6 phase and produce the two-dimensional(2D) CsPb_(2)Br_5 phase,which is also conducive to the improvement of device performance.Ultimately,the resulting perovskite films,which are strain-released and defect-passivated,exhibit exceptional device efficiency,reaching 10.87% for carbon-based CsPbBr_(3) device,14.86% for carbon-based CsPbI_(2)Br device,22,02% for FA_(0.97)Cs_(0.03)PbI_(3) device,respectively.Moreover,the unencapsulated CsPbBr_(3) PSC exhibits excellent stability under persistent exposure to humidity(80%) and heat(80℃) for over 50 days.展开更多
Printable mesoscopic perovskite solar cells(PM-PSCs)possess notable merits in terms of cost-effectiveness,easy manufacturing,and large scale applications.Nevertheless,the absence of a hole transport layer contributes ...Printable mesoscopic perovskite solar cells(PM-PSCs)possess notable merits in terms of cost-effectiveness,easy manufacturing,and large scale applications.Nevertheless,the absence of a hole transport layer contributes to the exacerbation of carrier recombination,and the defects between the perovskite and electron transport layer(ETL)interfaces significantly decrease the efficiency of the devices.In this study,a bifunctional surface passivation approach is proposed by applying a thioacetamide(TAA)surfactant on the mesoporous TiO_(2)interface.The results demonstrate that TAA molecules could interact with TiO_(2),thereby diminishing the oxygen vacancy defects.Additionally,the amino group and sulfur atoms in TAA molecules act as Lewis base to effectively passivate the uncoordinated Pb^(2+)in perovskite and improve the morphology of perovskite,and decrease the trap-state density of perovskite.The TAA passivation mechanism improves the alignment of energy levels between TiO_(2)and perovskite,facilitating electron transport and reducing carrier recombination.Consequently,the TAA-passivated device achieved a champion power conversion efficiency(PCE)of 17.86%with a high fill factor(FF)of 79.16%and an open-circuit voltage(V_(OC))of 0.971 V.This investigation presents a feasible strategy for interfacial passivation of the ETL to further improve the efficiency of PM-PSCs.展开更多
Inverted perovskite solar cells have gained prominence in industrial advancement due to their easy fabrication,low hysteresis effects,and high stability.Despite these advantages,their efficiency is currently limited b...Inverted perovskite solar cells have gained prominence in industrial advancement due to their easy fabrication,low hysteresis effects,and high stability.Despite these advantages,their efficiency is currently limited by excessive defects and poor carrier transport at the perovskite-electrode interface,particularly at the buried interface between the perovskite and transparent conductive oxide(TCO).Recent efforts in the perovskite community have focused on designing novel self-assembled molecules(SAMs)to improve the quality of the buried interface.However,a notable gap remains in understanding the regulation of atomic-scale interfacial properties of SAMs between the perovskite and TCO interfaces.This understanding is crucial,particularly in terms of identifying chemically active anchoring groups.In this study,we used the star SAM([2-(9H-carbazol-9-yl)ethyl]phosphonic acid)as the base structure to investigate the defect passivation effects of eight common anchoring groups at the perovskite-TCO interface.Our findings indicate that the phosphonic and boric acid groups exhibit notable advantages.These groups fulfill three key criteria:they provide the greatest potential for defect passivation,exhibit stable adsorption with defects,and exert significant regulatory effects on interface dipoles.Ionized anchoring groups exhibit enhanced passivation capabilities for defect energy levels due to their superior Lewis base properties,which effectively neutralize local charges near defects.Among various defect types,iodine vacancies are the easiest to passivate,whereas iodine-substituted lead defects are the most challenging to passivate.Our study provides comprehensive theoretical insights and inspiration for the design of anchoring groups in SAMs,contributing to the ongoing development of more efficient inverted perovskite solar cells.展开更多
Phenyl-C_(61)-butyric acid methyl ester(PCBM) serves as a common electron transport layer(ETL) in inverted p-i-n structure perovskite solar cells(IPSCs),yet energy barriers and insufficient passivation at the PCBM-per...Phenyl-C_(61)-butyric acid methyl ester(PCBM) serves as a common electron transport layer(ETL) in inverted p-i-n structure perovskite solar cells(IPSCs),yet energy barriers and insufficient passivation at the PCBM-perovskite interface hinder device effectiveness and durability.In this study,we present a series of novel Fullerene Phenylacid Ester Derivatives(FPEDs:FPP,FTPP,FDPP) incorporated into PCBM.Our investigations illustrate that FPEDs effectively act to passivate the perovskite surface by forming robust interactions with uncoordinated Pb^(2+) ions via the phosphine oxide groups present in their molecular structures,thereby enhancing the stability of the devices.Moreover,these additives elevate the energy level of the lowest unoccupied molecular orbital(LUMO) of ETL,diminish the electron injection barrier,and enhance the efficiency of interlayer electron transport.Incorporating FPEDs enhances ETL coverage on the perovskite layer,reducing leakage current significantly.Notably,Devices with PCBM/FTPP achieved a peak PCE of 23.62% and showed superior stability,maintaining 96,8% of the initial PCE after 500 h,while control devices retained merely 80.7% over the same period.展开更多
Ag substitution in Cu_(2)ZnSn(S,Se)_(4)(CZTSSe)is a promising way to mitigate Cu/Zn related defects,electrostatic fluctuations and Shockley-Read-Hall(SRH)recombination centers.However,high performance ACZTSSe solar ce...Ag substitution in Cu_(2)ZnSn(S,Se)_(4)(CZTSSe)is a promising way to mitigate Cu/Zn related defects,electrostatic fluctuations and Shockley-Read-Hall(SRH)recombination centers.However,high performance ACZTSSe solar cells are generally demonstrated with more Ag amounts and strenuous fabrication processes,which are not ideal when using cheap constituent materials CZTSSe.To reduce the Ag amount(2%-3%),local Ag substitutions into CZTSSe at front(F),back(B)and dual front/back(FB)were proposed.Experimental results revealed that F-passivation effectively reduced the Cu/Zn related defects and further limits the interface/bulk recombination whereas B-passivation improved the grain growth at the back interface and further allows enhanced transport of charge carriers.By employing the dual Agpassivation approach,the final ACZTSSe device parameters were significantly improved and remarkable power conversion efficiency(PCE)of 12.43%was achieved with eco-friendly aqueous solution process.展开更多
Defect-induced charge carrier recombination at the interfaces between perovskite and adjacent charge transport layers restricts further improvements in the device performance of perovskite solar cells(PSCs).Defect pas...Defect-induced charge carrier recombination at the interfaces between perovskite and adjacent charge transport layers restricts further improvements in the device performance of perovskite solar cells(PSCs).Defect passivation at these interfaces can reduce trap states and inhibit the induced nonradiative recombination.Herein,we report a double-sided interfacial passivation via simply evaporating potassium chloride(DIP-KCl)at both the hole transport layer(HTL)/perovskite and perovskite/electron transport layer(ETL)interfaces in inverted planar PSCs.We demonstrate that the bottom KCl layer at the HTL/perovskite interface not only reduces the interfacial defects and improves the interfacial contact,but also leads to increased perovskite crystallinity,while the top KCl layer at the perovskite/ETL interface efficiently passivates the perovskite top surface defects and facilitates electron extraction at this interface.Thus,suppressed nonradiative recombination and faster charge extraction at both interfaces close to the perovskite layer can be achieved by using our DIP-KCl strategy.As a result,inverted PSCs based on DIP-KCl present an increased efficiency from 17.1% to 19.2% and enhanced stability,retaining over 90% of their initial efficiency after aging at maximum power point tracking for 1000 h.This work provides a simple and efficient way for defect passivation to further increase the efficiency and stability of PSCs.展开更多
Organic cation and halide anion defects are omnipresent in the perovskite films,which will destroy perovskite electronic structure and downgrade the properties of devices.Defect passivation in halide perovskites is cr...Organic cation and halide anion defects are omnipresent in the perovskite films,which will destroy perovskite electronic structure and downgrade the properties of devices.Defect passivation in halide perovskites is crucial to the application of solar cells.Herein,tiny amounts of trivalent rhodium ion incorporation can help the nucleation of perovskite grain and passivate the defects in the grain boundaries,which can improve efficiency and stability of perovskite solar cells.Through first-principle calculations,rhodium ion incorporation into the perovskite structure can induce ordered arrangement and tune bandgap.In experiment,rhodium ion incorporation with perovskite can contribute to preparing larger crystalline and uniform film,reducing trap-state density and enlarging charge carrier lifetime.After optimizing the content of 1% rhodium,the devices achieved an efficiency up to 20.71% without obvious hysteresis,from 19.09% of that pristine perovskite.In addition,the unencapsulated solar cells maintain 92% of its initial efficiency after 500 h in dry air.This work highlights the advantages of trivalent rhodium ion incorporation in the characteristics of perovskite solar cells,which will promote the future industrial application.展开更多
Defect passivation is one of the most important strategies to boost both the efficiency and stability of perovskite solar cells(PSCs).Here,nontoxic and sustainable forest-based biomaterial,betulin,is first introduced ...Defect passivation is one of the most important strategies to boost both the efficiency and stability of perovskite solar cells(PSCs).Here,nontoxic and sustainable forest-based biomaterial,betulin,is first introduced into perovskites.The experiments and calculations reveal that betulin can effectively passivate the uncoordinated lead ions in perovskites via sharing the lone pair electrons of hydroxyl group,promoting charge transport.As a result,the power conversion efficiencies of the p-i-n planar PSCs remarkably increase from 19.14%to 21.15%,with the improvement of other parameters.The hydrogen bonds of betulin lock methylamine and halogen ions along the grain boundaries and on the film surface and thus suppress ion migration,further stabilizing perovskite crystal structures.These positive effects enable the PSCs to maintain 90%of the initial efficiency after 30 days in ambient air with 60%±5%relative humidity,75%after 300 h aging at 85℃,and 55%after 250 h light soaking,respectively.This work opens a new pathway for using nontoxic and low-cost biomaterials from forest to make highly efficient and stable PSCs.展开更多
Surface passivation via post-treatment is an important strategy for improving power conversion efficiency and operational stability of perovskite solar cells.However,so far the interaction mechanisms between passivati...Surface passivation via post-treatment is an important strategy for improving power conversion efficiency and operational stability of perovskite solar cells.However,so far the interaction mechanisms between passivating additive and perovskite are not well understood.Here,we report the atomic-scale interaction of surface passivating additive 2,2-difluoroethylammonium bromine(2FEABr)on the MAPbI_(3).It is found that the bulky 2FEA+cations tend to distribute at film surface,while the Br−anions diffuse from surface into bulk.A combination of 19F,207Pb,and 2H solid-state NMR further reveal the Br−anions’partial substitution for the I−sites,the restricted motion of partial MA+cations,and the firmed perovskite lattices,which would improve charge transport and stability of the perovskite films.Optical spectroscopy and ultraviolet photoelectron spectroscopy demonstrate that the 2FEABr induced surface passivation and energetic modification suppress the nonradiative recombination loss.These findings enable the efficiency of the p-i-n structured PSC significantly increasing from 19.44 to 21.06%,accompanied by excellent stability.Our work further establishes more knowledge link between passivating additive and PSC performance.展开更多
Wide-bandgap(WBG)perovskite solar cells suffer from severe non-radiative recombination and exhibit relatively large opencircuit voltage(V_(OC))deficits,limiting their photovoltaic performance.Here,we address these iss...Wide-bandgap(WBG)perovskite solar cells suffer from severe non-radiative recombination and exhibit relatively large opencircuit voltage(V_(OC))deficits,limiting their photovoltaic performance.Here,we address these issues by in-situ forming a well-defined 2D perovskite(PMA)_(2)PbCl_(4)(phenmethylammonium is referred to as PMA)passivation layer on top of the WBG active layer.The 2D layer with highly pure dimensionality and halide components is realized by intentionally tailoring the side-chain substituent at the aryl ring of the post-treatment reagent.First-principle calculation and single-crystal X-ray diffraction results reveal that weak intermolecular interactions between bulky PMA cations and relatively low cation-halide hydrogen bonding strength are crucial in forming the well-defined 2D phase.The(PMA)_(2)PbCl_(4)forms improved type-I energy level alignment with the WBG perovskite,reducing the electron recombination at the perovskite/hole-transport-layer interface.Applying this strategy in fabricating semi-transparent WBG perovskite solar cells(indium tin oxide as the back electrode),the V_(OC)deficits can be reduced to 0.49 V,comparable with the reported state-of-the-art WBG perovskite solar cells using metal electrodes.Consequently,we obtain hysteresis-free 18.60%-efficient WBG perovskite solar cells with a high V_(OC)of 1.23 V.展开更多
Bulk and interface carrier nonradiative recombination losses impede the further improvement of power conversion efficiency(PCE)and stability of perovskite solar cells(PSCs).It is highly necessary to develop multifunct...Bulk and interface carrier nonradiative recombination losses impede the further improvement of power conversion efficiency(PCE)and stability of perovskite solar cells(PSCs).It is highly necessary to develop multifunctional strategy to minimize surface and interface nonradiative recombination losses.Herein,we report a bulk and interface defect passivation strategy via the synergistic effect of anions and cations,where multifunctional potassium sulphate(K_(2)SO_(4))is incorporated at SnO_(2)/perovskite interface.We find that K^(+)ions in K_(2)SO_(4)diffuse into perovskite layer and suppress the formation of bulk defects in perovskite films,and the SO_(4)^(2-)ions remain located at interface via the strong chemical interaction with SnO_(2)layer and perovskite layer,respectively.Through this synergistic modification strategy,effective defect passivation and improved energy band alignment are achieved simultaneously.These beneficial effects are translated into an efficiency increase from 19.45%to 21.18%with a low voltage deficit of0.53 V mainly as a result of boosted open-circuit voltage(V_(oc))after K_(2)SO_(4)modification.In addition,the K_(2)SO_(4)modification contributes to ameliorated stability.The present work provides a route to minimize bulk and interface nonradiative recombination losses for the simultaneous realization of PCE and stability enhancement by rational anion and cation synergistic engineering.展开更多
The grain surfaces(film surface and grain boundary)of polycrystalline perovskite films are vulnerable sites in solar cells since they pose a high defect density and initiate the degradation of perovskite absorber.Achi...The grain surfaces(film surface and grain boundary)of polycrystalline perovskite films are vulnerable sites in solar cells since they pose a high defect density and initiate the degradation of perovskite absorber.Achieving simultaneously defect passivation and grain protection from moisture is crucial for the viability of perovskite solar cells.Here,an in situ cross-linked grain encapsulation(CLGE)strategy that improves both device stability and defect passivation is reported.Cross-linkable semiconducting small molecules are mixed into the antisolvent to uniformly form a compact and conducting cross-linked layer over the grain surfaces.This cross-linked coating layer not only passivates trap states and facilitates hole extraction,but also enhances the device stability by preventing moisture diffusion.Using the CLGE strategy,a high power conversion efficiency(PCE)of 22.7%is obtained in 1.55-eV bandgap planar perovskite solar cells.The unencapsulated devices with CLGE exhibit significantly enhanced device stability again moisture and maintain>90%of their initial PCE after shelf storage under ambient condition for over10,000 h.展开更多
The application of ionic liquids in perovskite has attracted wide-spread attention for its astounding performance improvement of perovskite solar cells(PSCs).However,the detailed mechanisms behind the improvement rema...The application of ionic liquids in perovskite has attracted wide-spread attention for its astounding performance improvement of perovskite solar cells(PSCs).However,the detailed mechanisms behind the improvement remain mysterious.Herein,a series of imidazolium-based ionic liquids(IILs)with different cations and anions is systematically investigated to elucidate the passivation mechanism of IILs on inorganic perovskites.It is found that IILs display the following advantages:(1)They form ionic bonds with Cs^(+)and Pb^(2+)cations on the surface and at the grain boundaries of perovskite films,which could effectively heal/reduce the Cs^(+)/I−vacancies and Pb-related defects;(2)They serve as a bridge between the perovskite and the hole-transport-layer for effective charge extraction and transfer;and(3)They increase the hydrophobicity of the perovskite surface to further improve the stability of the CsPbI_(2)Br PSCs.The combination of the above effects results in suppressed non-radiative recombination loss in CsPbI_(2)Br PSCs and an impressive power conversion efficiency of 17.02%.Additionally,the CsPbI_(2)Br PSCs with IILs surface modification exhibited improved ambient and light illumination stability.Our results provide guidance for an indepth understanding of the passivation mechanism of IILs in inorganic perovskites.展开更多
Passivating undercoordinated ions is an effective way to reduce the defect densities at the surface and grain boundaries(GBs)of perovskite materials for enhanced photovoltaic performance and stability of perovskite so...Passivating undercoordinated ions is an effective way to reduce the defect densities at the surface and grain boundaries(GBs)of perovskite materials for enhanced photovoltaic performance and stability of perovskite solar cells(PSCs).Here,(BBF)complex is chosen as a multifunctional additive,which contains both C7H9N and BF3 groups working as Lewis base and Lewis acid,respectively,can bond with Pb^(2+)/I^(−) and FA+on the surface and in the GBs in the perovskite film,affording passivation of both cation and anion defects.The synergistic effect of the C7H9N and BF3 complex slows the crystallization during the perovskite film deposition to improve the crystalline quality,which reduces the trap density and the recombination in the perovskite film to suppress nonradiative recombination loss and minimizes moisture permeation to improve the stability of the perovskite material.Meanwhile,such an additive improves the energy-level alignment between the valence band of the perovskite and the highest occupied molecular orbital of the hole-transporting material,Spiro-OMeTAD.Consequently,our work achieves power conversion efficiency of 23.24%,accompanied by enhanced stability under ambient conditions and light illumination and opens a new avenue for improving the performance of PSCs through the use of a multifunctional complex.展开更多
The point-contact high-purity germanium detector(HPGe)has the advantages of low background,low energy threshold,and high energy resolution and can be applied in the detection of rare-event physics.However,the performa...The point-contact high-purity germanium detector(HPGe)has the advantages of low background,low energy threshold,and high energy resolution and can be applied in the detection of rare-event physics.However,the performance of HPGe must be further improved to achieve superior energy resolution,low noise,and long-term reliability.In this study,we combine computational simulations and experimental comparisons to deeply understand the passivation mechanism of Ge.The surface passivation effect is calculated and inferred from the band structure and density of interface states,and further con-firmed by the minority carrier lifetime.The first-principles method based on the density functional theory was adopted to systematically study the lattice structure,band structure,and density of state(DOS)of four different systems:Ge–H,Ge–Ge-NH 2,Ge-OH,and Ge-SiO_(x).The electronic char-acteristics of the Ge(100)unit cell with different passi-vation groups and Si/O atomic ratios were compared.This shows that H,N,and O atoms can effectively reduce the surface DOS of the Ge atoms.The passivation effect of the SiO_(x) group varied with increasing O atoms and Si/O atomic ratios.Experimentally,SiO and SiO_(2) passivation films were fabricated by electron beam evaporation on a Ge substrate,and the valence state of Si and resistivity was measured to characterize the film.The minority carrier lifetime of Ge-SiO_(2) is 21.3 ls,which is approximately quadruple that of Ge-SiO.The passivation effect and mechanism are discussed in terms of hopping conduction and surface defect density.This study builds a relationship between the passivation effect and different termination groups,and provides technical support for the potential passivation layer,which can be applied in Ge detectors with ultralow energy thresholds and especially in HPGe for rare-event physics detection experiments in future.展开更多
The light weight,good bending resistance and low production cost make flexible perovskite solar cells(PSCs)good candidates in wearable electronics,portable charger,remote power,and flying objects.High power conversion...The light weight,good bending resistance and low production cost make flexible perovskite solar cells(PSCs)good candidates in wearable electronics,portable charger,remote power,and flying objects.High power conversion efficiency(PCE)plays a crucial role on obtaining the high mass specific power of flexible devices.However,the performance for flexible PSCs is still having a large room to be improved.Here,we added the 2-amino-5-cyanopyridine(ACP)molecule with a polar electron density distribution in the perovskite precursor solution to improve the performance of flexible PSCs.The cyano groups with electron-withdrawing ability are expected to passivate positively charged point defects,while amines with electron donating ability are expected to passivate negatively charged point defects in perovskite films.Thanks to the effective passivation of defects at the grain boundary and surface of perovskite films,the PCE of flexible PSCs is obviously increased from 16.9%to 18.0%.These results provide a universal approach to improve performance of flexible PSCs by healing the defects in perovskite films through electrostatic interactions.展开更多
基金supported by the National Natural Science Foundation of China(51802081,62074052,and 62104061)the Natural Science Foundation of Henan Province(232300420145).
文摘The presence of SnZn-related defects in Cu_(2)ZnSn(S,Se)_(4)(CZTSSe)absorber results in large irreversible energy loss and extra irreversible electron-hole non-radiative recombination,thus hindering the efficiency enhancement of CZTSSe devices.Although the incorporation of Ag in CZTSSe can effectively suppress the SnZn-related defects and significantly improve the resulting cell performance,an excellent efficiency has not been achieved to date primarily owing to the poor electrical-conductivity and the low carrier density of the CZTSSe film induced by Ag substitution.Herein,this study exquisitely devises an Ag/H co-doping strategy in CZTSSe absorber via Ag substitution programs followed by hydrogen-plasma treatment procedure to suppress SnZn defects for achieving efficient CZTSSe devices.In-depth investigation results demonstrate that the incorporation of H in Ag-based CZTSSe absorber is expected to improve the poor electrical-conductivity and the low carrier density caused by Ag substitution.Importantly,the C=O and O-H functional groups induced by hydrogen incorporation,serving as an electron donor,can interact with under-coordinated cations in CZTSSe material,effectively passivating the SnZn-related defects.Consequently,the incorporation of an appropriate amount of Ag/H in CZTSSe mitigates carrier non-radiative recombination,prolongs minority carrier lifetime,and thus yields a champion efficiency of 14.74%,showing its promising application in kesterite-based CZTSSe devices.
基金supported by the Science and Technology Development Fund,Macao SAR(File no.FDCT-0082/2021/A2,0010/2022/AMJ,006/2022/ALC)UM's research fund(File no.MYRG2022-00241-IAPME,MYRGCRG2022-00009-FHS)+2 种基金the research fund from Wuyi University(EF38/IAPME-XGC/2022/WYU)the Natural Science Foundation of China(61935017,62175268)Science,Technology and Innovation Commission of Shenzhen Municipality(Project Nos.JCYJ20220530113015035,JCYJ20210324120204011,and KQTD2015071710313656).
文摘Metal halide perovskites,particularly the quasi-two-dimensional perovskite subclass,have exhibited considerable potential for next-generation electroluminescent materials for lighting and display.Nevertheless,the presence of defects within these perovskites has a substantial influence on the emission efficiency and durability of the devices.In this study,we revealed a synergistic passivation mechanism on perovskite films by using a dual-functional compound of potassium bromide.The dual functional potassium bromide on the one hand can passivate the defects of halide vacancies with bromine anions and,on the other hand,can screen the charged defects at the grain boundaries with potassium cations.This approach effectively reduces the probability of carriers quenching resulting from charged defects capture and consequently enhances the radiative recombination efficiency of perovskite thin films,leading to a significant enhancement of photoluminescence quantum yield to near-unity values(95%).Meanwhile,the potassium bromide treatment promoted the growth of homogeneous and smooth film,facilitating the charge carrier injection in the devices.Consequently,the perovskite light-emitting diodes based on this strategy achieve a maximum external quantum efficiency of~21%and maximum luminance of~60,000 cd m^(-2).This work provides a deeper insight into the passivation mechanism of ionic compound additives in perovskite with the solution method.
基金financially supported by the National Natural Science Foundation of China (51971080)the Shenzhen Bureau of Science,Technology and Innovation Commission (GXWD20201230155427003-20200730151200003 and JSGG20200914113601003)。
文摘The function of solid electrolytes and the composition of solid electrolyte interphase(SEI)are highly significant for inhibiting the growth of Li dendrites.Herein,we report an in-situ interfacial passivation combined with self-adaptability strategy to reinforce Li_(0.33)La_(0.557)TiO_(3)(LLTO)-based solid-state batteries.Specifically,a functional SEI enriched with LiF/Li_(3)PO_(4) is formed by in-situ electrochemical conversion,which is greatly beneficial to improving interface compatibility and enhancing ion transport.While the polarized dielectric BaTiO_(3)-polyamic acid(BTO-PAA,BP)film greatly improves the Li-ion transport kinetics and homogenizes the Li deposition.As expected,the resulting electrolyte offers considerable ionic conductivity at room temperature(4.3 x 10~(-4)S cm^(-1))and appreciable electrochemical decomposition voltage(5.23 V)after electrochemical passivation.For Li-LiFePO_(4) batteries,it shows a high specific capacity of 153 mA h g^(-1)at 0.2C after 100 cycles and a long-term durability of 115 mA h g^(-1)at 1.0 C after 800 cycles.Additionally,a stable Li plating/stripping can be achieved for more than 900 h at 0.5 mA cm^(-2).The stabilization mechanisms are elucidated by ex-situ XRD,ex-situ XPS,and ex-situ FTIR techniques,and the corresponding results reveal that the interfacial passivation combined with polarization effect is an effective strategy for improving the electrochemical performance.The present study provides a deeper insight into the dynamic adjustment of electrode-electrolyte interfacial for solid-state lithium batteries.
基金National Natural Science Foundation of China (62104136, 22179051, 62204098, 52104258)Project of Shandong Province Higher Educational Young Innovative Team (2022KJ218)+3 种基金China Postdoctoral Science Foundation (2023M732104)Qingdao Postdoctoral Funding Program (QDBSH20220201002)Postdoctoral Innovation Project of Shandong Province (SDCX-ZG-202303032)Shandong Provincial Natural Science Foundation (ZR2021ME016)。
文摘Rational interface engineering is essential for minimizing interfacial nonradiative recombination losses and enhancing device performance.Herein,we report the use of bidentate diphenoxybenzene(DPOB)isomers as surface modifiers for perovskite films.The DPOB molecules,which contain two oxygen(O)atoms,chemically bond with undercoordinated Pb^(2+) on the surface of perovskite films,resulting in compression of the perovskite lattice.This chemical interaction,along with physical regulations,leads to the formation of high-quality perovskite films with compressive strain and fewer defects.This compressive strain-induced band bending promotes hole extraction and transport,while inhibiting charge recombination at the interfaces.Furthermore,the addition of DPOB will reduce the zero-dimensional(OD) Cs_4PbBr_6 phase and produce the two-dimensional(2D) CsPb_(2)Br_5 phase,which is also conducive to the improvement of device performance.Ultimately,the resulting perovskite films,which are strain-released and defect-passivated,exhibit exceptional device efficiency,reaching 10.87% for carbon-based CsPbBr_(3) device,14.86% for carbon-based CsPbI_(2)Br device,22,02% for FA_(0.97)Cs_(0.03)PbI_(3) device,respectively.Moreover,the unencapsulated CsPbBr_(3) PSC exhibits excellent stability under persistent exposure to humidity(80%) and heat(80℃) for over 50 days.
基金funded by the Yunnan Yunling Scholars Project,the National Natural Science Foundation of China(No.51562038)the Young-Middle-Aged Academic and Technical Leaders Reserve Talent Project in Yunnan Province(No.202005AC160015)the Yunnan Basic Applied Research Project(No.202101AT070013).
文摘Printable mesoscopic perovskite solar cells(PM-PSCs)possess notable merits in terms of cost-effectiveness,easy manufacturing,and large scale applications.Nevertheless,the absence of a hole transport layer contributes to the exacerbation of carrier recombination,and the defects between the perovskite and electron transport layer(ETL)interfaces significantly decrease the efficiency of the devices.In this study,a bifunctional surface passivation approach is proposed by applying a thioacetamide(TAA)surfactant on the mesoporous TiO_(2)interface.The results demonstrate that TAA molecules could interact with TiO_(2),thereby diminishing the oxygen vacancy defects.Additionally,the amino group and sulfur atoms in TAA molecules act as Lewis base to effectively passivate the uncoordinated Pb^(2+)in perovskite and improve the morphology of perovskite,and decrease the trap-state density of perovskite.The TAA passivation mechanism improves the alignment of energy levels between TiO_(2)and perovskite,facilitating electron transport and reducing carrier recombination.Consequently,the TAA-passivated device achieved a champion power conversion efficiency(PCE)of 17.86%with a high fill factor(FF)of 79.16%and an open-circuit voltage(V_(OC))of 0.971 V.This investigation presents a feasible strategy for interfacial passivation of the ETL to further improve the efficiency of PM-PSCs.
基金supported by the National Natural Science Foundation of China(Grant Nos.62321166653,22090044,and 12350410372).Calculations were performed in part at the high-performance computing center of Jilin University.
文摘Inverted perovskite solar cells have gained prominence in industrial advancement due to their easy fabrication,low hysteresis effects,and high stability.Despite these advantages,their efficiency is currently limited by excessive defects and poor carrier transport at the perovskite-electrode interface,particularly at the buried interface between the perovskite and transparent conductive oxide(TCO).Recent efforts in the perovskite community have focused on designing novel self-assembled molecules(SAMs)to improve the quality of the buried interface.However,a notable gap remains in understanding the regulation of atomic-scale interfacial properties of SAMs between the perovskite and TCO interfaces.This understanding is crucial,particularly in terms of identifying chemically active anchoring groups.In this study,we used the star SAM([2-(9H-carbazol-9-yl)ethyl]phosphonic acid)as the base structure to investigate the defect passivation effects of eight common anchoring groups at the perovskite-TCO interface.Our findings indicate that the phosphonic and boric acid groups exhibit notable advantages.These groups fulfill three key criteria:they provide the greatest potential for defect passivation,exhibit stable adsorption with defects,and exert significant regulatory effects on interface dipoles.Ionized anchoring groups exhibit enhanced passivation capabilities for defect energy levels due to their superior Lewis base properties,which effectively neutralize local charges near defects.Among various defect types,iodine vacancies are the easiest to passivate,whereas iodine-substituted lead defects are the most challenging to passivate.Our study provides comprehensive theoretical insights and inspiration for the design of anchoring groups in SAMs,contributing to the ongoing development of more efficient inverted perovskite solar cells.
基金Natural Science Foundation of China (51972278)Outstanding Youth Science and Technology Talents Program of Sichuan (19JCQN0085)Open Project of State Key Laboratory of Environment-friendly Energy Materials (Southwest University of Science and Technology, 21fksy19)。
文摘Phenyl-C_(61)-butyric acid methyl ester(PCBM) serves as a common electron transport layer(ETL) in inverted p-i-n structure perovskite solar cells(IPSCs),yet energy barriers and insufficient passivation at the PCBM-perovskite interface hinder device effectiveness and durability.In this study,we present a series of novel Fullerene Phenylacid Ester Derivatives(FPEDs:FPP,FTPP,FDPP) incorporated into PCBM.Our investigations illustrate that FPEDs effectively act to passivate the perovskite surface by forming robust interactions with uncoordinated Pb^(2+) ions via the phosphine oxide groups present in their molecular structures,thereby enhancing the stability of the devices.Moreover,these additives elevate the energy level of the lowest unoccupied molecular orbital(LUMO) of ETL,diminish the electron injection barrier,and enhance the efficiency of interlayer electron transport.Incorporating FPEDs enhances ETL coverage on the perovskite layer,reducing leakage current significantly.Notably,Devices with PCBM/FTPP achieved a peak PCE of 23.62% and showed superior stability,maintaining 96,8% of the initial PCE after 500 h,while control devices retained merely 80.7% over the same period.
基金supported by the National Research Foundation of Korea(NRF)funded by the Korean Government(NRF2021R1A2C1008598)the program of Phased Development of Carbon Neutral Technologies through the National Research Foundation of Korea(NRF)funded by the Ministry of Science,ICT(NRF-2022M3J1A1064220)。
文摘Ag substitution in Cu_(2)ZnSn(S,Se)_(4)(CZTSSe)is a promising way to mitigate Cu/Zn related defects,electrostatic fluctuations and Shockley-Read-Hall(SRH)recombination centers.However,high performance ACZTSSe solar cells are generally demonstrated with more Ag amounts and strenuous fabrication processes,which are not ideal when using cheap constituent materials CZTSSe.To reduce the Ag amount(2%-3%),local Ag substitutions into CZTSSe at front(F),back(B)and dual front/back(FB)were proposed.Experimental results revealed that F-passivation effectively reduced the Cu/Zn related defects and further limits the interface/bulk recombination whereas B-passivation improved the grain growth at the back interface and further allows enhanced transport of charge carriers.By employing the dual Agpassivation approach,the final ACZTSSe device parameters were significantly improved and remarkable power conversion efficiency(PCE)of 12.43%was achieved with eco-friendly aqueous solution process.
基金financially supported by the National Natural Science Foundation of China,China(51672094,51861145404,51822203,and 11627801)the National Key Research and Development Program of China,China(2016YFA0201001)+4 种基金the China Postdoctoral Science Foundation(2016M602286)the Fundamental Research Funds for the Central Universities,China(2016JCTD111,2018RCPY003,2020kfy XJJS008)the Shenzhen Science and Technology Innovation Committee,China(JCYJ20170307165905513,JCYJ20180507182257563)the Natural Science Foundation of Guangdong Province,China(2017A030313342)the Outstanding Young Talent Research Fund of Zhengzhou University,China。
文摘Defect-induced charge carrier recombination at the interfaces between perovskite and adjacent charge transport layers restricts further improvements in the device performance of perovskite solar cells(PSCs).Defect passivation at these interfaces can reduce trap states and inhibit the induced nonradiative recombination.Herein,we report a double-sided interfacial passivation via simply evaporating potassium chloride(DIP-KCl)at both the hole transport layer(HTL)/perovskite and perovskite/electron transport layer(ETL)interfaces in inverted planar PSCs.We demonstrate that the bottom KCl layer at the HTL/perovskite interface not only reduces the interfacial defects and improves the interfacial contact,but also leads to increased perovskite crystallinity,while the top KCl layer at the perovskite/ETL interface efficiently passivates the perovskite top surface defects and facilitates electron extraction at this interface.Thus,suppressed nonradiative recombination and faster charge extraction at both interfaces close to the perovskite layer can be achieved by using our DIP-KCl strategy.As a result,inverted PSCs based on DIP-KCl present an increased efficiency from 17.1% to 19.2% and enhanced stability,retaining over 90% of their initial efficiency after aging at maximum power point tracking for 1000 h.This work provides a simple and efficient way for defect passivation to further increase the efficiency and stability of PSCs.
基金supported by the Ministry of Education of China(IRT1148)the National Natural Science Foundation of China(U1732126,11804166,51602161,51372119)+3 种基金China Postdoctoral Science Foundation(2018M630587)the Priority Academic Program Development of Jiangsu Higher Education Institutions(YX03001)Guangdong Science and Technology Program(2017B030314002)Graduate Research Innovation Fund of Jiangsu Province(KYCX18_0863,KYCX18_0847,KYCX18_0869)。
文摘Organic cation and halide anion defects are omnipresent in the perovskite films,which will destroy perovskite electronic structure and downgrade the properties of devices.Defect passivation in halide perovskites is crucial to the application of solar cells.Herein,tiny amounts of trivalent rhodium ion incorporation can help the nucleation of perovskite grain and passivate the defects in the grain boundaries,which can improve efficiency and stability of perovskite solar cells.Through first-principle calculations,rhodium ion incorporation into the perovskite structure can induce ordered arrangement and tune bandgap.In experiment,rhodium ion incorporation with perovskite can contribute to preparing larger crystalline and uniform film,reducing trap-state density and enlarging charge carrier lifetime.After optimizing the content of 1% rhodium,the devices achieved an efficiency up to 20.71% without obvious hysteresis,from 19.09% of that pristine perovskite.In addition,the unencapsulated solar cells maintain 92% of its initial efficiency after 500 h in dry air.This work highlights the advantages of trivalent rhodium ion incorporation in the characteristics of perovskite solar cells,which will promote the future industrial application.
基金supported by the National Natural Science Foundation of China(21875067,51811530011,11604099)the Fundamental Research Funds for the Central Universities,Shanghai Rising-Star(19QA1403100)+2 种基金ECNU Multifunctional Platform for Innovation(006)the National Key Research and Development Program of China(2017YFA0206600)the National Natural Science Foundation of China(51773045,21772030,51922032,21961160720)for financial support。
文摘Defect passivation is one of the most important strategies to boost both the efficiency and stability of perovskite solar cells(PSCs).Here,nontoxic and sustainable forest-based biomaterial,betulin,is first introduced into perovskites.The experiments and calculations reveal that betulin can effectively passivate the uncoordinated lead ions in perovskites via sharing the lone pair electrons of hydroxyl group,promoting charge transport.As a result,the power conversion efficiencies of the p-i-n planar PSCs remarkably increase from 19.14%to 21.15%,with the improvement of other parameters.The hydrogen bonds of betulin lock methylamine and halogen ions along the grain boundaries and on the film surface and thus suppress ion migration,further stabilizing perovskite crystal structures.These positive effects enable the PSCs to maintain 90%of the initial efficiency after 30 days in ambient air with 60%±5%relative humidity,75%after 300 h aging at 85℃,and 55%after 250 h light soaking,respectively.This work opens a new pathway for using nontoxic and low-cost biomaterials from forest to make highly efficient and stable PSCs.
基金supported by the National Science Foundation of China grant(21875067)the Fundamental Research Funds for the Central Universities,Shanghai Rising-Star(19QA1403100)+4 种基金East China Normal University(ECNU)Multifunctional Platform for InnovationThe Ministry of Science and Technology of the People’s Republic of China(No.2018YFF01012504)the National Key Research and Development Program of China(2017YFA0206600)the National Natural Science Foundation of China(51773045,21772030,51922032,21961160720)for financial support。
文摘Surface passivation via post-treatment is an important strategy for improving power conversion efficiency and operational stability of perovskite solar cells.However,so far the interaction mechanisms between passivating additive and perovskite are not well understood.Here,we report the atomic-scale interaction of surface passivating additive 2,2-difluoroethylammonium bromine(2FEABr)on the MAPbI_(3).It is found that the bulky 2FEA+cations tend to distribute at film surface,while the Br−anions diffuse from surface into bulk.A combination of 19F,207Pb,and 2H solid-state NMR further reveal the Br−anions’partial substitution for the I−sites,the restricted motion of partial MA+cations,and the firmed perovskite lattices,which would improve charge transport and stability of the perovskite films.Optical spectroscopy and ultraviolet photoelectron spectroscopy demonstrate that the 2FEABr induced surface passivation and energetic modification suppress the nonradiative recombination loss.These findings enable the efficiency of the p-i-n structured PSC significantly increasing from 19.44 to 21.06%,accompanied by excellent stability.Our work further establishes more knowledge link between passivating additive and PSC performance.
基金supported by the National Natural Science Foundation of China(22179042,U21A2078,and 51902110)the Natural Science Foundation of Fujian Province(2020J06021 and 2020J01064).
文摘Wide-bandgap(WBG)perovskite solar cells suffer from severe non-radiative recombination and exhibit relatively large opencircuit voltage(V_(OC))deficits,limiting their photovoltaic performance.Here,we address these issues by in-situ forming a well-defined 2D perovskite(PMA)_(2)PbCl_(4)(phenmethylammonium is referred to as PMA)passivation layer on top of the WBG active layer.The 2D layer with highly pure dimensionality and halide components is realized by intentionally tailoring the side-chain substituent at the aryl ring of the post-treatment reagent.First-principle calculation and single-crystal X-ray diffraction results reveal that weak intermolecular interactions between bulky PMA cations and relatively low cation-halide hydrogen bonding strength are crucial in forming the well-defined 2D phase.The(PMA)_(2)PbCl_(4)forms improved type-I energy level alignment with the WBG perovskite,reducing the electron recombination at the perovskite/hole-transport-layer interface.Applying this strategy in fabricating semi-transparent WBG perovskite solar cells(indium tin oxide as the back electrode),the V_(OC)deficits can be reduced to 0.49 V,comparable with the reported state-of-the-art WBG perovskite solar cells using metal electrodes.Consequently,we obtain hysteresis-free 18.60%-efficient WBG perovskite solar cells with a high V_(OC)of 1.23 V.
基金financially supported by the Defense Industrial Technology Development Program(JCKY2017110C0654)the National Natural Science Foundation of China(11974063,61904023)the Chongqing Special Postdoctoral Science Foundation(cstc2019jcyj-bsh0026)。
文摘Bulk and interface carrier nonradiative recombination losses impede the further improvement of power conversion efficiency(PCE)and stability of perovskite solar cells(PSCs).It is highly necessary to develop multifunctional strategy to minimize surface and interface nonradiative recombination losses.Herein,we report a bulk and interface defect passivation strategy via the synergistic effect of anions and cations,where multifunctional potassium sulphate(K_(2)SO_(4))is incorporated at SnO_(2)/perovskite interface.We find that K^(+)ions in K_(2)SO_(4)diffuse into perovskite layer and suppress the formation of bulk defects in perovskite films,and the SO_(4)^(2-)ions remain located at interface via the strong chemical interaction with SnO_(2)layer and perovskite layer,respectively.Through this synergistic modification strategy,effective defect passivation and improved energy band alignment are achieved simultaneously.These beneficial effects are translated into an efficiency increase from 19.45%to 21.18%with a low voltage deficit of0.53 V mainly as a result of boosted open-circuit voltage(V_(oc))after K_(2)SO_(4)modification.In addition,the K_(2)SO_(4)modification contributes to ameliorated stability.The present work provides a route to minimize bulk and interface nonradiative recombination losses for the simultaneous realization of PCE and stability enhancement by rational anion and cation synergistic engineering.
基金financially supported by the National Key R&D Program of China(2018YFB1500102,2018YFB2200101)the National Natural Science Foundation of China(61974063,61921005)+3 种基金Natural Science Foundation of Jiangsu Province(BK20190315)the Fundamental Research Funds for the Central Universities(14380168)the Thousand Talent Program for Young Outstanding Scientists in ChinaProgram for Innovative Talents and Entrepreneur in Jiangsu。
文摘The grain surfaces(film surface and grain boundary)of polycrystalline perovskite films are vulnerable sites in solar cells since they pose a high defect density and initiate the degradation of perovskite absorber.Achieving simultaneously defect passivation and grain protection from moisture is crucial for the viability of perovskite solar cells.Here,an in situ cross-linked grain encapsulation(CLGE)strategy that improves both device stability and defect passivation is reported.Cross-linkable semiconducting small molecules are mixed into the antisolvent to uniformly form a compact and conducting cross-linked layer over the grain surfaces.This cross-linked coating layer not only passivates trap states and facilitates hole extraction,but also enhances the device stability by preventing moisture diffusion.Using the CLGE strategy,a high power conversion efficiency(PCE)of 22.7%is obtained in 1.55-eV bandgap planar perovskite solar cells.The unencapsulated devices with CLGE exhibit significantly enhanced device stability again moisture and maintain>90%of their initial PCE after shelf storage under ambient condition for over10,000 h.
基金support from the National Natural Science Foundation of China(62074095)the National Key Research and Development Program of China(2016YFA0202403)+3 种基金the Fundamental Research Funds for the Central Universities(GK202002001)the 111 Project(Grant No.B21005)the DNL Cooperation Fund CAS(DNL180311)the support of H2 cluster in Xi’an Jiaotong University.
文摘The application of ionic liquids in perovskite has attracted wide-spread attention for its astounding performance improvement of perovskite solar cells(PSCs).However,the detailed mechanisms behind the improvement remain mysterious.Herein,a series of imidazolium-based ionic liquids(IILs)with different cations and anions is systematically investigated to elucidate the passivation mechanism of IILs on inorganic perovskites.It is found that IILs display the following advantages:(1)They form ionic bonds with Cs^(+)and Pb^(2+)cations on the surface and at the grain boundaries of perovskite films,which could effectively heal/reduce the Cs^(+)/I−vacancies and Pb-related defects;(2)They serve as a bridge between the perovskite and the hole-transport-layer for effective charge extraction and transfer;and(3)They increase the hydrophobicity of the perovskite surface to further improve the stability of the CsPbI_(2)Br PSCs.The combination of the above effects results in suppressed non-radiative recombination loss in CsPbI_(2)Br PSCs and an impressive power conversion efficiency of 17.02%.Additionally,the CsPbI_(2)Br PSCs with IILs surface modification exhibited improved ambient and light illumination stability.Our results provide guidance for an indepth understanding of the passivation mechanism of IILs in inorganic perovskites.
基金The authors acknowledge support from the National Natural Science Foundation of China(62074095/61704101/91733301)the National Key Research and Development Program of China(2016YFA0202403)+3 种基金the Fundamental Research Funds for the Central Universities GK(201903048)the 111 Project(Grant No.B21005)the Fundament Research Funds for the Central University(2019TS004)DNL Cooperation Fund CAS(DNL180311).
文摘Passivating undercoordinated ions is an effective way to reduce the defect densities at the surface and grain boundaries(GBs)of perovskite materials for enhanced photovoltaic performance and stability of perovskite solar cells(PSCs).Here,(BBF)complex is chosen as a multifunctional additive,which contains both C7H9N and BF3 groups working as Lewis base and Lewis acid,respectively,can bond with Pb^(2+)/I^(−) and FA+on the surface and in the GBs in the perovskite film,affording passivation of both cation and anion defects.The synergistic effect of the C7H9N and BF3 complex slows the crystallization during the perovskite film deposition to improve the crystalline quality,which reduces the trap density and the recombination in the perovskite film to suppress nonradiative recombination loss and minimizes moisture permeation to improve the stability of the perovskite material.Meanwhile,such an additive improves the energy-level alignment between the valence band of the perovskite and the highest occupied molecular orbital of the hole-transporting material,Spiro-OMeTAD.Consequently,our work achieves power conversion efficiency of 23.24%,accompanied by enhanced stability under ambient conditions and light illumination and opens a new avenue for improving the performance of PSCs through the use of a multifunctional complex.
基金supported by the National Natural Science Foundation of China Youth Fund(No.12005017)。
文摘The point-contact high-purity germanium detector(HPGe)has the advantages of low background,low energy threshold,and high energy resolution and can be applied in the detection of rare-event physics.However,the performance of HPGe must be further improved to achieve superior energy resolution,low noise,and long-term reliability.In this study,we combine computational simulations and experimental comparisons to deeply understand the passivation mechanism of Ge.The surface passivation effect is calculated and inferred from the band structure and density of interface states,and further con-firmed by the minority carrier lifetime.The first-principles method based on the density functional theory was adopted to systematically study the lattice structure,band structure,and density of state(DOS)of four different systems:Ge–H,Ge–Ge-NH 2,Ge-OH,and Ge-SiO_(x).The electronic char-acteristics of the Ge(100)unit cell with different passi-vation groups and Si/O atomic ratios were compared.This shows that H,N,and O atoms can effectively reduce the surface DOS of the Ge atoms.The passivation effect of the SiO_(x) group varied with increasing O atoms and Si/O atomic ratios.Experimentally,SiO and SiO_(2) passivation films were fabricated by electron beam evaporation on a Ge substrate,and the valence state of Si and resistivity was measured to characterize the film.The minority carrier lifetime of Ge-SiO_(2) is 21.3 ls,which is approximately quadruple that of Ge-SiO.The passivation effect and mechanism are discussed in terms of hopping conduction and surface defect density.This study builds a relationship between the passivation effect and different termination groups,and provides technical support for the potential passivation layer,which can be applied in Ge detectors with ultralow energy thresholds and especially in HPGe for rare-event physics detection experiments in future.
基金financial support from the National Natural Science Foundation of China(No.NSFC21773218)。
文摘The light weight,good bending resistance and low production cost make flexible perovskite solar cells(PSCs)good candidates in wearable electronics,portable charger,remote power,and flying objects.High power conversion efficiency(PCE)plays a crucial role on obtaining the high mass specific power of flexible devices.However,the performance for flexible PSCs is still having a large room to be improved.Here,we added the 2-amino-5-cyanopyridine(ACP)molecule with a polar electron density distribution in the perovskite precursor solution to improve the performance of flexible PSCs.The cyano groups with electron-withdrawing ability are expected to passivate positively charged point defects,while amines with electron donating ability are expected to passivate negatively charged point defects in perovskite films.Thanks to the effective passivation of defects at the grain boundary and surface of perovskite films,the PCE of flexible PSCs is obviously increased from 16.9%to 18.0%.These results provide a universal approach to improve performance of flexible PSCs by healing the defects in perovskite films through electrostatic interactions.
