Two-dimensional(2D)/quasi-2D perovskite solar cells(PSCs)incorporating organic spacer cations exhibit appealing ambient stability in comparison with their 3D analogs.Most reported organic spacer cations are based on a...Two-dimensional(2D)/quasi-2D perovskite solar cells(PSCs)incorporating organic spacer cations exhibit appealing ambient stability in comparison with their 3D analogs.Most reported organic spacer cations are based on ammonium,whereas formamidinium(FA^(+))has been seldom applied despite that FA has been extensively used in high-efficiency 3D PSCs.Herein,a novel FA-based organic spacer cation,4-chloro-phenylformamidinium(CPFA^(+)),is applied in quasi-2D Ruddlesden-Popper(RP)PSCs for the first time,and methylammonium chloride(MACl)is employed to promote crystal growth and orientation of perovskite film,resulting in high power conversion efficiency(PCE)with improved stability.Upon incorporating CPFA+organic spacer cation and MACl additive,high-quality quasi-2D CPFA_(2)MA_(n-1)Pb_(n)(I_(0.857)Cl_(0.143))_(3n+1)(n=9)perovskite film forms,exhibiting improved crystal orientation,reduced trap state density,prolonged carrier lifetime and optimized energy level alignment.Consequently,the CPFA_(2)MA_(n-1)Pb_(n)(I_(0.857)Cl_(0.143))_(3n+1)(n=9)quasi-2D RP PSC devices deliver a highest PCE of 14.78%.Moreover,the un-encapsulated CPFA-based quasi-2D RP PSC devices maintain~80%of its original PCE after exceeding 2000 h storage under ambient condition,whereas the 3D MAPb I3counterparts retain only~45%of its original PCE.Thus,the ambient stability of quasi-2D RP PSC devices is improved obviously relative to its 3D MAPb I3counterpart.展开更多
The two-dimensional(2 D) Ruddlesden–Popper-type perovskites, possessing tunable bandgap, narrow light emission,strong quantum confinement effect, as well as a simple preparation method, are identified as a new genera...The two-dimensional(2 D) Ruddlesden–Popper-type perovskites, possessing tunable bandgap, narrow light emission,strong quantum confinement effect, as well as a simple preparation method, are identified as a new generation of candidate materials for efficient light-emitting diodes. However, the preparation of high-quality quasi-2 D perovskite films is still a challenge currently, such as the severe mixing of phases and a high density of defects within the films, impeding the further promotion of device performance. Here, we prepared the quasi-2 D PEA_(2) MA_(n-1) Pbn Br_(3 n+1) perovskite films by a modified spin-coating method, and the phases with large bandgap were effectively suppressed by the vacuum evaporation treatment. We systematically investigated the optical properties and stability of the optimized films, and the photoluminescence(PL) quantum yield of the treated films was enhanced from 23% to 45%. We also studied the emission mechanisms by temperature-dependent PL spectra. Moreover, the stability of films against moisture, ultraviolet light, and heat was also greatly improved.展开更多
In order to improve the efficiency and stability of inverted three-dimensional(3D) or quasi-2D perovskite solar cells(PSCs) for future commercialization, exploring high efficient dopant-free polymer holetransporting m...In order to improve the efficiency and stability of inverted three-dimensional(3D) or quasi-2D perovskite solar cells(PSCs) for future commercialization, exploring high efficient dopant-free polymer holetransporting materials(HTMs) is still desired and meaningful. One simple and efficient way to achieve high performance dopant-free HTMs is to synthesize novel non-conjugated side-chain polymers via rational molecular design. In this work, N-(4-methoxyphenyl)-9,9-dimethyl-9H-fluoren-2-amine(FMeNPh) groups are introduced into the poly(N-vinylcarbazole)(PVK) side chains to afford two nonconjugated polymers PVCz-DFMeNPh and PVCz-FMeNPh as dopant-free HTMs in inverted quasi-2D PSCs. Benefited from the flexible properties of polyethylene backbone and excellent optoelectronic natures of FMeNPh side-chain groups, PVCz-DFMeNPh with more FMeNPh units exhibited excellent thermal stability, well-matched energy levels and improved charge mobility as compared to PTAA and PVCzFMeNPh. Moreover, the morphologies investigation of quasi-2D perovskite on PVCz-DFMeNPh shows more compact and homogeneous perovskite films than those on PTAA and PVCz-FMeNPh. As a result,the dopant-free PVCz-DFMeNPh based inverted quasi-2D PSCs deliver power conversion efficiency(PCE) up to 18.44% as well as negligible hysteresis and favorable long-term stability, which represents as excellent performance reported to date for inverted quasi-2D PSCs. The results demonstrate the great potentials of constructing non-conjugated side-chain polymer HTMs based on phenylfluorenamine-func tionalized PVK for the development of high efficient and stable inverted 3D or quasi-2D PSCs.展开更多
Recent years has seen increasing interest in building artificial synaptic devices to emulate the computation performed by biological synapses.Biological synapses are functional links between neurons,through which info...Recent years has seen increasing interest in building artificial synaptic devices to emulate the computation performed by biological synapses.Biological synapses are functional links between neurons,through which information is transmitted in the neuron network.The information can be stored and processed simultaneously in the same synapse through tuning synaptic weight,which is defined as the strength of the correlation between展开更多
Quasi-two-dimensional(2D)perovskite embodies characteristics of both three-dimensional(3D)and 2D perovskites,achieving the superior external environment stability structure of 2D perovskites alongside the high efficie...Quasi-two-dimensional(2D)perovskite embodies characteristics of both three-dimensional(3D)and 2D perovskites,achieving the superior external environment stability structure of 2D perovskites alongside the high efficiency of 3D perovskites.This effect is realized through critical structural modifications in device fabrication.Typically,perovskites have an octahedral structure,generally ABX3,where an organic ammonium cation(A’)participates in forming the perovskite structure,with A’_(n)(n=1 or 2)sandwiched between A_(n-1)B_(n)X_(3n+1)perovskite layers.Depending on whether A’is a monovalent or divalent cation,2D perovskites are classified into Ruddlesden-Popper perovskite or Dion-Jacobson perovskite,each generating different structures.Although each structure achieves similar effects,they incorporate distinct mechanisms in their formation.And according to these different structures,various properties appear,and additive and optimizing methods to increase the efficiency of 3D perovskites also exist in 2D perovskites.In this review,scientific understanding and engineering perspectives of the quasi-2D perovskite is investigated,and the optimal structure quasi-2D and the device optimization is also discussed to provide the insight in the field.展开更多
Despite the rapid advances of red and green perovskite light-emitting diodes(Pe LEDs),achieving high brightness with high external quantum efficiency(EQE)remains a challenge for the pure-blue Pe LEDs,which greatly hin...Despite the rapid advances of red and green perovskite light-emitting diodes(Pe LEDs),achieving high brightness with high external quantum efficiency(EQE)remains a challenge for the pure-blue Pe LEDs,which greatly hinders their practical applications,such as white-light illumination and in optical communication as a high-speed and low-loss light source.Herein,we report a high-performance pure-blue Pe LED based on mixed-halide quasi-2D perovskites incorporated with a zwitterionic molecule of 3-(benzyldimethylammonio)propanesulfonate(3-BAS).Experimental and density functional theory analysis reveals that 3-BAS can simultaneously eliminate non-radiative recombination loss,suppress halide migration,and regulate phase distribution for smoothing energy transfer in the mixed-halide quasi-2D perovskites,leading to the final perovskites with high photoluminescence quantum yield and robust spectrum stability.Thus,the highperformance pure-blue Pe LED with a recorded brightness with 1806 cd m-2and a relative higher EQE of 9.25%is achieved,which is successfully demonstrated in a visible light communication system for voice signal transmission.We pave the way for achieving highly efficient pure-blue Pe LEDs with great application potential in future optical communication networks.展开更多
Bubble dynamics properties play a crucial and significant role in the design and optimization of gas-solid fluidized beds.In this study,the bubble dynamics properties of four B-particles were investigated in a quasi-t...Bubble dynamics properties play a crucial and significant role in the design and optimization of gas-solid fluidized beds.In this study,the bubble dynamics properties of four B-particles were investigated in a quasi-two-dimensional(quasi-2D)fluidized bed,including bubble equivalent diameter,bubble size distribution,average bubble density,bubble aspect ratio,bubble hold-up,bed expansion ratio,bubble radial position,and bubble velocity.The studies were performed by computational particle fluid dynamics(CPFD)numerical simulation and post-processed with digital image analysis(DIA)technique,at superficial gas velocities ranging from 2u_(mf) to 7u_(mf).The simulated results shown that the CPFD simulation combining with DIA technique post-processing could be used as a reliable method for simulating bubble dynamics properties in quasi-2D gas-solid fluidized beds.However,it seemed not desirable for the simulation of bubble motion near the air distributor at higher superficial gas velocity from the simulated average bubble density distribution.The superficial gas velocity significantly affected the bubble equivalent diameter and evolution,while it had little influence on bubble size distribution and bubble aspect ratio distribution for the same particles.Both time-averaged bubble hold-up and bed expansion ratio increased with the increase of superficial gas velocity.Two core-annular flow structures could be found in the fluidized bed for all cases.The average bubble rising velocity increased with the increasing bubble equivalent diameter.For bubble lateral movement,the smaller bubbles might be more susceptible,and superficial gas velocity had a little influence on the absolute lateral velocity of bubbles.The simulated results presented a valuable and novel approach for studying bubble dynamics properties.The comprehensive understanding of bubble dynamics behaviors in quasi-2D gas-solid fluidized beds would provide support in the design,operation,and optimization of gas-solid fluidized bed reactors.展开更多
One-step deposition approaches have been widely applied and developed in the fabrication of quasi-2D perovskites.However,the regulation of quantum wells(QWs)and crystalline orientation is difficult and complicated whe...One-step deposition approaches have been widely applied and developed in the fabrication of quasi-2D perovskites.However,the regulation of quantum wells(QWs)and crystalline orientation is difficult and complicated when using this methodology.Sequential deposition is another widespread synthetic approach for preparing perovskite films and perovskite dimension engineering.In this article,δ-CsPbI_(3)intermediate phase assisted sequential(IPAS)deposition is successfully carried out to fabricate MA-free quasi-2D ACI perovskites.The amount of theδ-CsPbI_(3)intermediate phase in the PbI2 layer and the concentration of GAI molecule in the IPA solution both play important roles in the production of MA-free quasi-2D ACI perovskite films.The n value of the MA-free quasi-2D ACI perovskites can be adjusted,which affects the photovoltaic performance and device stability.Compared with one-step deposition,the MA-free quasi-2D ACI perovskites prepared via IPAS deposition have opposite reverse-graded QW distribution and improved vertical orientation,leading to a remarkable PEC of up to 18.86%and allowing the preparation of unpackaged devices with prominent working stability(80%,400 h).The underlying mechanism and crystallization pathway of IPAS deposition confirm that sequential deposition has unique superiority in regulating the QW distribution and crystalline orientation of quasi-2D perovskites.展开更多
Quasi-2D perovskites have attracted tremendous interest for application as lightemission layers in light-emitting diodes(LEDs).However,the heterogeneous n phase and non-uniform distribution still severely limit the fu...Quasi-2D perovskites have attracted tremendous interest for application as lightemission layers in light-emitting diodes(LEDs).However,the heterogeneous n phase and non-uniform distribution still severely limit the further development of quasi-2D perovskite LEDs(Pero-LEDs).Meanwhile,the increased defect density caused by the reduced dimension and grain size induces non-radiative recombination and further deteriorates the device performance.Here,we found that a series of molecules containing phosphoryl chloride functional groups have noticeable enhancement effects on the device performance of quasi-2D Pero-LEDs.Then,we studied the modification mechanism by focusing on the bis(2-oxo-3-oxazolidinyl)phosphinic chloride(BOPCl).It is concluded that the BOPCl can not only regulate the phase distribution by decreasing the crystallization rate but also remain in the grain boundaries and passivate the defects.As a result,the corresponding quasi-2D Pero-LEDs obtained a maximum external quantum efficiency(EQE_(max))of 20.82%and an average EQE(EQE_(ave))of around 20%on the optimal 50 devices,proving excellent reproducibility.Our work provides a new selection of molecular types for regulating the crystallization and passivating the defects of quasi-2D perovskite films.展开更多
Based on the 2D horizontal plane numerical model, a quasi-3D numerical model is established for coastal regions of shallow water. The characteristics of this model are that the velocity profiles;can be obtained at the...Based on the 2D horizontal plane numerical model, a quasi-3D numerical model is established for coastal regions of shallow water. The characteristics of this model are that the velocity profiles;can be obtained at the same time when the equations of the value of difference between the horizontal current velocity and its depth-averaged velocity in the vertical direction are solved and the results obtained are consistent with the results of the 2D, model. The circulating flow in the rectangular area induced by wind is simulated and applied to the tidal flow field of the radial sandbanks in the South Yellow Sea. The computational results from this quasi-3D model are in good agreement with analytical results and observed data. The solution of the finite difference equations has been found to be stable, and the model is simple, effective and practical.展开更多
Recent advances in heterojunction and interfacial engineering of perovskite solar cells(PSCs)have enabled great progress in developing highly efficient and stable devices.Nevertheless,the effect of halide choice on th...Recent advances in heterojunction and interfacial engineering of perovskite solar cells(PSCs)have enabled great progress in developing highly efficient and stable devices.Nevertheless,the effect of halide choice on the formation mechanism,crystallography,and photoelectric properties of the lowdimensional phase still requires further detailed study.In this work,we present key insights into the significance of halide choice when designing passivation strategies comprising large organic spacer salts,clarifying the effect of anions on the formation of quasi-2D/3D heterojunctions.To demonstrate the importance of halide influences,we employ novel neo-pentylammonium halide salts with different halide anions(neoPAX,X=I,Br,or Cl).We find that regardless of halide selection,iodide-based(neoPA)_(2)(FA)_((n-1))PbnI_((3n+1))phases are formed above the perovskite substrate,while the added halide anions diffuse and passivate the perovskite bulk.In addition,we also find the halide choice has an influence on the degree of dimensionality(n).Comparing the three halides,we find that chloride-based salts exhibit superior crystallographic,enhanced carrier transport,and extraction compared to the iodide and bromide analogs.As a result,we report high power conversion efficiency in quasi-2D/3D PSCs,which are optimal when using chloride salts,reaching up to 23.35%,and improving long-term stability.展开更多
Emergency retention basins (ERB) are diked enclosures alongside rivers into which water from the main river channel is diverted during extreme floods. If the basins are operated during extreme flooding, two negative e...Emergency retention basins (ERB) are diked enclosures alongside rivers into which water from the main river channel is diverted during extreme floods. If the basins are operated during extreme flooding, two negative environmental impacts may occur: 1) contamination of the soils due to their transport by suspended sediments to the basin and 2) depletion of dissolved oxygen in the basin water. A computer-based methodology is presented which was used to assess the environmental risk exhibited by the operation of an ERB system proposed for the Elbe River in Germany. The August 2002 extreme flood event was used as a test case. For such a flood, the results showed that there is a 77% risk that dissolved oxygen levels fall below 2 mg/L in the water and a 48% chance of exceeding the inspection value of 500 mg zinc/kg in the soil.展开更多
Quasi-two dimensional(2D)perovskites have emerged as a promising class of materials due to their remarkable photoluminescence efficiency,which stems from their exceptionally high exciton binding energies.The spatial c...Quasi-two dimensional(2D)perovskites have emerged as a promising class of materials due to their remarkable photoluminescence efficiency,which stems from their exceptionally high exciton binding energies.The spatial confinement of excitons within smaller grain sizes could enhance the formation of biexcitons leading to higher radiative recombination efficiency.However,the synthesis of high-quality quasi-2D perovskite thin films with controllable grain sizes remains a challenging task.In this study,we present a facile method for achieving quasi-2D perovskite thin films with controllable grain sizes ranging from 500 to 900 nm.This is accomplished by intermediate phase engineering during the film fabrication process.Our results demonstrate that quasi-2D perovskite films with smaller grain sizes exhibit more efficient bound exciton generation and a reduced stimulated emission threshold down to 15.89µJ cm^(−2).Furthermore,femtosecond transient absorption measurements reveal that the decay time of bound excitons is shorter in quasi-2D perovskites with smaller grain sizes compared to that of those with larger grains at the same pump density,which is 230.5 ps.This observation suggests a more efficient exciton recombination process in the smaller grain size regime.Our findings would offer a promising approach for the development of efficient bound exciton lasers.展开更多
We study the two-dimensional above-barrier penetration and the sub-barrier tunneling of non-relativistic particles and photons, described in the quasi-monochromatic approximation by simple plane waves. Our scheme repr...We study the two-dimensional above-barrier penetration and the sub-barrier tunneling of non-relativistic particles and photons, described in the quasi-monochromatic approximation by simple plane waves. Our scheme represents the motion from the left free-motion zero-potential region to the right zero-potential region through the intermediate region with a one-dimensional rectangular potential barrier along the axis, normal to the both parallel interfaces between all three regions, and with the zero potential along the axis, parallel to the those interfaces. We have firstly obtained the analytical expressions for the infinite series of multiple internal and external reflections and also of multiple transmitted waves of particles and photons, with equal shifts between them along the interfaces for the above-barrier penetration and with various shifts between them in the case of the sub-barrier tunneling. Finally the Hartman and Fletcher effect for any transmitted wave is established.展开更多
基金supported by the National Key Research and Development Program of China(2017YFA0402800)the National Natural Science Foundation of China(51925206,U1932214)。
文摘Two-dimensional(2D)/quasi-2D perovskite solar cells(PSCs)incorporating organic spacer cations exhibit appealing ambient stability in comparison with their 3D analogs.Most reported organic spacer cations are based on ammonium,whereas formamidinium(FA^(+))has been seldom applied despite that FA has been extensively used in high-efficiency 3D PSCs.Herein,a novel FA-based organic spacer cation,4-chloro-phenylformamidinium(CPFA^(+)),is applied in quasi-2D Ruddlesden-Popper(RP)PSCs for the first time,and methylammonium chloride(MACl)is employed to promote crystal growth and orientation of perovskite film,resulting in high power conversion efficiency(PCE)with improved stability.Upon incorporating CPFA+organic spacer cation and MACl additive,high-quality quasi-2D CPFA_(2)MA_(n-1)Pb_(n)(I_(0.857)Cl_(0.143))_(3n+1)(n=9)perovskite film forms,exhibiting improved crystal orientation,reduced trap state density,prolonged carrier lifetime and optimized energy level alignment.Consequently,the CPFA_(2)MA_(n-1)Pb_(n)(I_(0.857)Cl_(0.143))_(3n+1)(n=9)quasi-2D RP PSC devices deliver a highest PCE of 14.78%.Moreover,the un-encapsulated CPFA-based quasi-2D RP PSC devices maintain~80%of its original PCE after exceeding 2000 h storage under ambient condition,whereas the 3D MAPb I3counterparts retain only~45%of its original PCE.Thus,the ambient stability of quasi-2D RP PSC devices is improved obviously relative to its 3D MAPb I3counterpart.
基金supported by the National Natural Science Foundation of China (Grant Nos. 11774318, 12074347, 12004346, and 61935009)the Open Fund of State Key Laboratory of Integrated Optoelectronics (Grant No. IOSKL2020KF04)。
文摘The two-dimensional(2 D) Ruddlesden–Popper-type perovskites, possessing tunable bandgap, narrow light emission,strong quantum confinement effect, as well as a simple preparation method, are identified as a new generation of candidate materials for efficient light-emitting diodes. However, the preparation of high-quality quasi-2 D perovskite films is still a challenge currently, such as the severe mixing of phases and a high density of defects within the films, impeding the further promotion of device performance. Here, we prepared the quasi-2 D PEA_(2) MA_(n-1) Pbn Br_(3 n+1) perovskite films by a modified spin-coating method, and the phases with large bandgap were effectively suppressed by the vacuum evaporation treatment. We systematically investigated the optical properties and stability of the optimized films, and the photoluminescence(PL) quantum yield of the treated films was enhanced from 23% to 45%. We also studied the emission mechanisms by temperature-dependent PL spectra. Moreover, the stability of films against moisture, ultraviolet light, and heat was also greatly improved.
基金financially supported by the National Key Research and Development Program of China (2018YFB0406704)the National Natural Science Foundation of China (61974066, 61725502, 61634001)+3 种基金the Major Research Plan of the National Natural Science Foundation of China (91733302)the fund for Talented of Nanjing Tech University (201983)the Major Program of Natural Science Research of Jiangsu Higher Education Institutions of China (18KJA510002)the Synergetic Innovation Center for Organic Electronics and Information Displays。
文摘In order to improve the efficiency and stability of inverted three-dimensional(3D) or quasi-2D perovskite solar cells(PSCs) for future commercialization, exploring high efficient dopant-free polymer holetransporting materials(HTMs) is still desired and meaningful. One simple and efficient way to achieve high performance dopant-free HTMs is to synthesize novel non-conjugated side-chain polymers via rational molecular design. In this work, N-(4-methoxyphenyl)-9,9-dimethyl-9H-fluoren-2-amine(FMeNPh) groups are introduced into the poly(N-vinylcarbazole)(PVK) side chains to afford two nonconjugated polymers PVCz-DFMeNPh and PVCz-FMeNPh as dopant-free HTMs in inverted quasi-2D PSCs. Benefited from the flexible properties of polyethylene backbone and excellent optoelectronic natures of FMeNPh side-chain groups, PVCz-DFMeNPh with more FMeNPh units exhibited excellent thermal stability, well-matched energy levels and improved charge mobility as compared to PTAA and PVCzFMeNPh. Moreover, the morphologies investigation of quasi-2D perovskite on PVCz-DFMeNPh shows more compact and homogeneous perovskite films than those on PTAA and PVCz-FMeNPh. As a result,the dopant-free PVCz-DFMeNPh based inverted quasi-2D PSCs deliver power conversion efficiency(PCE) up to 18.44% as well as negligible hysteresis and favorable long-term stability, which represents as excellent performance reported to date for inverted quasi-2D PSCs. The results demonstrate the great potentials of constructing non-conjugated side-chain polymer HTMs based on phenylfluorenamine-func tionalized PVK for the development of high efficient and stable inverted 3D or quasi-2D PSCs.
基金supported by the National Natural Science Foundation of Chinathe Ministry of Science and Technology of Chinathe Chinese Academy of Sciences
文摘Recent years has seen increasing interest in building artificial synaptic devices to emulate the computation performed by biological synapses.Biological synapses are functional links between neurons,through which information is transmitted in the neuron network.The information can be stored and processed simultaneously in the same synapse through tuning synaptic weight,which is defined as the strength of the correlation between
基金the Research Grant of Kwangwoon University in 2024 and the National Research Foundation of Korea(RS-2023-00236572 and RS-2023-00212110)funded by the Korea government(MSIT)the project for Collabo R&D between Industry,University,and Research Institute(RS-2024-00414524)funded by Korea Ministry of SMEs and Startups.
文摘Quasi-two-dimensional(2D)perovskite embodies characteristics of both three-dimensional(3D)and 2D perovskites,achieving the superior external environment stability structure of 2D perovskites alongside the high efficiency of 3D perovskites.This effect is realized through critical structural modifications in device fabrication.Typically,perovskites have an octahedral structure,generally ABX3,where an organic ammonium cation(A’)participates in forming the perovskite structure,with A’_(n)(n=1 or 2)sandwiched between A_(n-1)B_(n)X_(3n+1)perovskite layers.Depending on whether A’is a monovalent or divalent cation,2D perovskites are classified into Ruddlesden-Popper perovskite or Dion-Jacobson perovskite,each generating different structures.Although each structure achieves similar effects,they incorporate distinct mechanisms in their formation.And according to these different structures,various properties appear,and additive and optimizing methods to increase the efficiency of 3D perovskites also exist in 2D perovskites.In this review,scientific understanding and engineering perspectives of the quasi-2D perovskite is investigated,and the optimal structure quasi-2D and the device optimization is also discussed to provide the insight in the field.
基金the support of the National Natural Science Foundation of China(NSFC)(61774077,12304473,62175094)the Key Projects of Joint Fund of Basic and Applied Basic Research Fund of Guangdong Province(2019B1515120073,2019B090921002)+3 种基金the Guangdong Science and Technology Research Foundation(2020A1414010036)the High-End Foreign Experts Project(G20200019046)the Young Talent Support Project of Henan Province(2024HYTP001)the Opening Project of Key Laboratory of Optoelectronic Chemical Materials and Devices,Ministry of Education,Jianghan University(JDGD-202302)
文摘Despite the rapid advances of red and green perovskite light-emitting diodes(Pe LEDs),achieving high brightness with high external quantum efficiency(EQE)remains a challenge for the pure-blue Pe LEDs,which greatly hinders their practical applications,such as white-light illumination and in optical communication as a high-speed and low-loss light source.Herein,we report a high-performance pure-blue Pe LED based on mixed-halide quasi-2D perovskites incorporated with a zwitterionic molecule of 3-(benzyldimethylammonio)propanesulfonate(3-BAS).Experimental and density functional theory analysis reveals that 3-BAS can simultaneously eliminate non-radiative recombination loss,suppress halide migration,and regulate phase distribution for smoothing energy transfer in the mixed-halide quasi-2D perovskites,leading to the final perovskites with high photoluminescence quantum yield and robust spectrum stability.Thus,the highperformance pure-blue Pe LED with a recorded brightness with 1806 cd m-2and a relative higher EQE of 9.25%is achieved,which is successfully demonstrated in a visible light communication system for voice signal transmission.We pave the way for achieving highly efficient pure-blue Pe LEDs with great application potential in future optical communication networks.
基金the financial support provided by National Key R&D Project of China(grant No.2020YFB0606303)the technical supports received from Sam Clark in CPFD Software,LLC of USA,and from Hi-Key Technology Incorporated of China.
文摘Bubble dynamics properties play a crucial and significant role in the design and optimization of gas-solid fluidized beds.In this study,the bubble dynamics properties of four B-particles were investigated in a quasi-two-dimensional(quasi-2D)fluidized bed,including bubble equivalent diameter,bubble size distribution,average bubble density,bubble aspect ratio,bubble hold-up,bed expansion ratio,bubble radial position,and bubble velocity.The studies were performed by computational particle fluid dynamics(CPFD)numerical simulation and post-processed with digital image analysis(DIA)technique,at superficial gas velocities ranging from 2u_(mf) to 7u_(mf).The simulated results shown that the CPFD simulation combining with DIA technique post-processing could be used as a reliable method for simulating bubble dynamics properties in quasi-2D gas-solid fluidized beds.However,it seemed not desirable for the simulation of bubble motion near the air distributor at higher superficial gas velocity from the simulated average bubble density distribution.The superficial gas velocity significantly affected the bubble equivalent diameter and evolution,while it had little influence on bubble size distribution and bubble aspect ratio distribution for the same particles.Both time-averaged bubble hold-up and bed expansion ratio increased with the increase of superficial gas velocity.Two core-annular flow structures could be found in the fluidized bed for all cases.The average bubble rising velocity increased with the increasing bubble equivalent diameter.For bubble lateral movement,the smaller bubbles might be more susceptible,and superficial gas velocity had a little influence on the absolute lateral velocity of bubbles.The simulated results presented a valuable and novel approach for studying bubble dynamics properties.The comprehensive understanding of bubble dynamics behaviors in quasi-2D gas-solid fluidized beds would provide support in the design,operation,and optimization of gas-solid fluidized bed reactors.
基金supported by the National Natural Science Foundation of China(Grant/Award Numbers:52262033,51862017,51962015,52162028,and 21603086)the Science and Technology Department of Hubei Province(Grant/Award Number:2019AAA020)The authors also acknowledge the financial support by the Natural Science Foundation of Hunan Province(No.2022JJ40551).
文摘One-step deposition approaches have been widely applied and developed in the fabrication of quasi-2D perovskites.However,the regulation of quantum wells(QWs)and crystalline orientation is difficult and complicated when using this methodology.Sequential deposition is another widespread synthetic approach for preparing perovskite films and perovskite dimension engineering.In this article,δ-CsPbI_(3)intermediate phase assisted sequential(IPAS)deposition is successfully carried out to fabricate MA-free quasi-2D ACI perovskites.The amount of theδ-CsPbI_(3)intermediate phase in the PbI2 layer and the concentration of GAI molecule in the IPA solution both play important roles in the production of MA-free quasi-2D ACI perovskite films.The n value of the MA-free quasi-2D ACI perovskites can be adjusted,which affects the photovoltaic performance and device stability.Compared with one-step deposition,the MA-free quasi-2D ACI perovskites prepared via IPAS deposition have opposite reverse-graded QW distribution and improved vertical orientation,leading to a remarkable PEC of up to 18.86%and allowing the preparation of unpackaged devices with prominent working stability(80%,400 h).The underlying mechanism and crystallization pathway of IPAS deposition confirm that sequential deposition has unique superiority in regulating the QW distribution and crystalline orientation of quasi-2D perovskites.
基金supported by the National Natural Science Foundation of China(U21A2078)Natural Science Foundation of Fujian Province(2020J06021,2019J01057,and 2020J01064)Scientific Research Funds of Huaqiao University.
文摘Quasi-2D perovskites have attracted tremendous interest for application as lightemission layers in light-emitting diodes(LEDs).However,the heterogeneous n phase and non-uniform distribution still severely limit the further development of quasi-2D perovskite LEDs(Pero-LEDs).Meanwhile,the increased defect density caused by the reduced dimension and grain size induces non-radiative recombination and further deteriorates the device performance.Here,we found that a series of molecules containing phosphoryl chloride functional groups have noticeable enhancement effects on the device performance of quasi-2D Pero-LEDs.Then,we studied the modification mechanism by focusing on the bis(2-oxo-3-oxazolidinyl)phosphinic chloride(BOPCl).It is concluded that the BOPCl can not only regulate the phase distribution by decreasing the crystallization rate but also remain in the grain boundaries and passivate the defects.As a result,the corresponding quasi-2D Pero-LEDs obtained a maximum external quantum efficiency(EQE_(max))of 20.82%and an average EQE(EQE_(ave))of around 20%on the optimal 50 devices,proving excellent reproducibility.Our work provides a new selection of molecular types for regulating the crystallization and passivating the defects of quasi-2D perovskite films.
基金National Natural Science Foundation of China(Grant No.49236120)
文摘Based on the 2D horizontal plane numerical model, a quasi-3D numerical model is established for coastal regions of shallow water. The characteristics of this model are that the velocity profiles;can be obtained at the same time when the equations of the value of difference between the horizontal current velocity and its depth-averaged velocity in the vertical direction are solved and the results obtained are consistent with the results of the 2D, model. The circulating flow in the rectangular area induced by wind is simulated and applied to the tidal flow field of the radial sandbanks in the South Yellow Sea. The computational results from this quasi-3D model are in good agreement with analytical results and observed data. The solution of the finite difference equations has been found to be stable, and the model is simple, effective and practical.
基金X.L.and T.W.are contributed equally to this work.W.Z.acknowledges the Engineering and Physical Sciences Research Council(EPSRC)New Investigator Award(2018EP/R043272/1)+8 种基金Marie Skłodowska-Curie Actions Individual Fellowships(839136)H.L.acknowledges the Newton Advanced Fellowship(192097)X.L.acknowledges the financial support from Zhengzhou University ScholarshipT.W thanks the University of Surrey Doctoral College for financial supportS.J.S.gratefully acknowledges the support of EPSRC(UK)under grant number EP/N021037/1L.D.thanks the China Scholarship Council and the Cambridge Trusts for fundingR.C.K.and J.A.S.thank the company Xenocs for their ongoing support through the X-ray scattering user program at the University of Sheffield and the EPSRC for funding the purchase of this instrumentZ.W.,Y.S.,and G.S.thank the financial support from Zhengzhou Materials Genome InstituteS.D.S.and K.J.acknowledge the Royal Society for funding。
文摘Recent advances in heterojunction and interfacial engineering of perovskite solar cells(PSCs)have enabled great progress in developing highly efficient and stable devices.Nevertheless,the effect of halide choice on the formation mechanism,crystallography,and photoelectric properties of the lowdimensional phase still requires further detailed study.In this work,we present key insights into the significance of halide choice when designing passivation strategies comprising large organic spacer salts,clarifying the effect of anions on the formation of quasi-2D/3D heterojunctions.To demonstrate the importance of halide influences,we employ novel neo-pentylammonium halide salts with different halide anions(neoPAX,X=I,Br,or Cl).We find that regardless of halide selection,iodide-based(neoPA)_(2)(FA)_((n-1))PbnI_((3n+1))phases are formed above the perovskite substrate,while the added halide anions diffuse and passivate the perovskite bulk.In addition,we also find the halide choice has an influence on the degree of dimensionality(n).Comparing the three halides,we find that chloride-based salts exhibit superior crystallographic,enhanced carrier transport,and extraction compared to the iodide and bromide analogs.As a result,we report high power conversion efficiency in quasi-2D/3D PSCs,which are optimal when using chloride salts,reaching up to 23.35%,and improving long-term stability.
文摘Emergency retention basins (ERB) are diked enclosures alongside rivers into which water from the main river channel is diverted during extreme floods. If the basins are operated during extreme flooding, two negative environmental impacts may occur: 1) contamination of the soils due to their transport by suspended sediments to the basin and 2) depletion of dissolved oxygen in the basin water. A computer-based methodology is presented which was used to assess the environmental risk exhibited by the operation of an ERB system proposed for the Elbe River in Germany. The August 2002 extreme flood event was used as a test case. For such a flood, the results showed that there is a 77% risk that dissolved oxygen levels fall below 2 mg/L in the water and a 48% chance of exceeding the inspection value of 500 mg zinc/kg in the soil.
基金supported by the National Natural Science Foundation of China(U21A20496 and 12104334)the Fund Program for the Scientific Activities of Selected Returned Overseas Professionals in Shanxi Province(20230011)+5 种基金the Research Program Supported by ShanxiZheda Institute of Advanced Materials and Chemical Engineering(2022SXTD020)the Central Government Guides Local Funds for Scientific and Technological Development(YDZJSX20231A010)the Natural Science Foundation of Shanxi Province(202203021222102)the State Key Laboratory Program of Quantum Optics and Quantum Optics Devices(KF202306)the support from a research grant(VIL50350)from VILLUM FONDEN,Denmark,the Swedish Research Council(2021-05319)the Swedish foundation of international cooperation in research and higher education(CH2019-8248)。
文摘Quasi-two dimensional(2D)perovskites have emerged as a promising class of materials due to their remarkable photoluminescence efficiency,which stems from their exceptionally high exciton binding energies.The spatial confinement of excitons within smaller grain sizes could enhance the formation of biexcitons leading to higher radiative recombination efficiency.However,the synthesis of high-quality quasi-2D perovskite thin films with controllable grain sizes remains a challenging task.In this study,we present a facile method for achieving quasi-2D perovskite thin films with controllable grain sizes ranging from 500 to 900 nm.This is accomplished by intermediate phase engineering during the film fabrication process.Our results demonstrate that quasi-2D perovskite films with smaller grain sizes exhibit more efficient bound exciton generation and a reduced stimulated emission threshold down to 15.89µJ cm^(−2).Furthermore,femtosecond transient absorption measurements reveal that the decay time of bound excitons is shorter in quasi-2D perovskites with smaller grain sizes compared to that of those with larger grains at the same pump density,which is 230.5 ps.This observation suggests a more efficient exciton recombination process in the smaller grain size regime.Our findings would offer a promising approach for the development of efficient bound exciton lasers.
文摘We study the two-dimensional above-barrier penetration and the sub-barrier tunneling of non-relativistic particles and photons, described in the quasi-monochromatic approximation by simple plane waves. Our scheme represents the motion from the left free-motion zero-potential region to the right zero-potential region through the intermediate region with a one-dimensional rectangular potential barrier along the axis, normal to the both parallel interfaces between all three regions, and with the zero potential along the axis, parallel to the those interfaces. We have firstly obtained the analytical expressions for the infinite series of multiple internal and external reflections and also of multiple transmitted waves of particles and photons, with equal shifts between them along the interfaces for the above-barrier penetration and with various shifts between them in the case of the sub-barrier tunneling. Finally the Hartman and Fletcher effect for any transmitted wave is established.
