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1.
The development of metal-halide perovskite nanocrystals (NCs) that yield bright and stable emission is of great importance. Previous reported perovskite NCs are mostly based on APbX3-type family fabricated via ligand- or surfactant-assisted chemical approaches. However, realizing bright and stable emission remains a challenge because of desorption of ligands/surfactants during long-term operation. Herein, Ruddlesden–Popper (RP)-type (A)2(MA)n-1PbnBr3n+1 NCs with size less than Bohr radius stabilized in mesoporous silica scaffold, which are prepared in situ via physical approach at low temperature are introduced. The RP NCs in mesoporous silica exhibit the formation of spatially and electronically separated quantum wells, efficient energy funneling between different n phases for bright emission (photoluminescence quantum yields of ≈99%), high irradiation stability (T70 = 110 days), and long-term stability (T90 = 110 days). These RP NCs have broad potential for bright light-emitting diodes, high-resolution PL imaging, and waterproof inks. Importantly, for the first time, stretchable perovskite X-ray scintillator is demonstrated with excellent X-ray imaging with resolution greater than 14 line pairs mm−1. These findings offer a paradigm to motivate future research toward stable and efficient perovskite optoelectronics.  相似文献   

2.
The development of an efficient fabrication route to achieve high-resolution perovskite pixel array is key for large-scale flexible image sensor devices. Herein, a high-resolution and stable 10 × 10 flexible PDs array based on formamidinium(FA+) and phenylmethylammonium (PMA+) quasi-2D (PMA)2FAPb2I7 (n = 2) perovskite is demonstrated by developing SiO2-assisted hydrophobic and hydrophilic treatment process on polyethylene terephthalate substrate. By introducing Au nanoparticles (Au NPs),  the perovskite film quality is improved and grain boundaries are reduced. The mechanism by which Au NPs upgrade the photoelectric quality of perovskite is mainly revealed by glow discharge-optical emission spectroscopy (GD-OES) and grazing-incidence wide-angle X-ray scattering (GIWAXS). To further improve the photoelectric performance of the devices, a post-treatment strategy with formamidinium chloride (FACl) is used . The optimized flexible PDs arrays show excellent optoelectronic properties with a high responsivity of 4.7 A W−1, a detectivity of 6.3 × 1012 Jones, and a broad spectral sensitivity. The device also exhibits excellent electrical stability even under severe bending and excellent flexural strength, as well as excellent environmental stability. Finally, the integrated flexible PDs arrays are used as sensor pixels in an imaging system to obtain high-resolution imaging patterns, demonstrating the imaging capability of the PDs arrays.  相似文献   

3.
2D Ruddlesden–Popper perovskites (2D PVKs) have attracted huge interest because of their excellent optoelectronic properties, yet the understanding of their electrical properties is inadequate due to the difficulties in obtaining 2D PVK field-effect transistors (FETs) with decent performance. Herein, the fabrication and characterization of 2D PVK ((BA)2(MA)n−1PbnI3n+1) single crystal FETs are reported, which exhibit reliable field effect electrical characteristics at low temperatures. Kelvin probe force microscopy (KPFM) results reveal that both ion migration and contact resistance seriously degrade device performance. While ion migration can be suppressed at low temperatures, contact resistance seems to fundamentally determine device performance. On one hand, Schottky contacts are observed to form at the metal/2D PVK interface because of Fermi level pinning, resulting in significant charge injection resistance, although this can be remarkably improved by replacing Au electrodes with Ca. On the other hand, the out-of-plane mobility is found to be three orders of magnitude lower than the in-plane mobility in 2D PVKs, causing large interlayer transport resistance. Thus, a low work-function metal and a thin crystal are important for achieving high device performance. This work provides important experimental insights into fabrication and electrical properties of 2D PVK FETs.  相似文献   

4.
Time-domain study of coherent acoustic phonons in nanomaterials provides dynamic and unparalleled insight into their mechanical and structural features. Ruddlesden–Popper (RP) perovskite shows excellent acoustic behaviors due to the large impedance mismatch between its hard perovskite frameworks and soft organic chains. However, the optical probe-independent acoustic nano-mechanical resonance and its real application in this important class of semiconductors have not yet been achieved. Herein, the acoustic breathing mode of resonant coherent phonons (RCP) in nanoscale RP perovskite films is reported. In contrast to the previously reported Brillouin mode in thick materials, such resonant breathing mode is no longer interfered by the optical probe, but as a self-sustained acoustic oscillation source whose features are directly related to material geometry along the direction of phonon propagation. As a nano-mechanical resonance, RCP oscillation is applied as a novel and non-destructive approach for quantitatively evaluating the decomposition of moisture-exposed RP perovskite. These results reveal the decisive effect of structural geometry on acoustic performances in perovskite nanomaterials. The nanoscale counterparts show evident advantages in acoustic mode modulation and structure detection.  相似文献   

5.
Organic metal-halide perovskites (OHPs) have recently attracted much attention as next-generation semiconducting materials due to their outstanding opto-electrical properties. However, OHPs currently suffer from the lack of efficient doping methods, while the traditional method of atomistic doping having clear limitations in the achievable doping range. While doping with molecular dopants, has been suggested as a solution to this problem, the action of these dopants is typically restricted to perovskite surfaces, therefore significantly reducing their doping potential. In this study, successful bulk inclusion of “magic blue”, a molecular dopant, into 2D Ruddlesden–Popper perovskites is reported. This doping strategy of immersing the perovskite film in dopant solution increases the electrical current up to ≈60 times while maintaining clean film surface. A full mechanistic picture of such immersion doping is provided, in which the solvent molecule facilitates bulk diffusion of dopant molecule inside the organic spacer layer. Physical criteria for judicious choice of solvents in immersion doping are developed based on readily available solvent properties. The immersion doping method developed in this study that enables bulk molecular doping in OHPs will provide a strategic doping methodology for controlling electrical properties of OHPs for electronic and optoelectronic devices.  相似文献   

6.
Ruddlesden–Popper (RP) faults are well known in oxide perovskites, and are also observed in promising metal halide perovskites. However, the effect of RP faults on optical properties of perovskite has not been systematically investigated. In this study, it is found that RP faults are common planar faults in all-vacuum deposited CsPbBr3-based perovskite polycrystal thin films, and the density of RP planar faults can be greatly increased by non-stoichiometric composition (Cs-rich) as well as reduced dimensionality (quasi-2D) strategies. The photoluminescence (PL) measurement reveals monotonically increasing peak intensities with higher densities of RP planar faults from Cs-rich, quasi-2D to Cs-rich & quasi-2D samples. The corresponding atomic-scale differential phase contrast maps indicate strongly confined charges within the RP planar fault network, which explains well the relationship between PL enhancement and the density of RP planar faults, and offers an alternative pathway for tailoring the optoelectronic properties of perovskite.  相似文献   

7.
Lead-free 2D perovskites based on tin halide octahedron slabs with Dion–Jacobson (DJ) phases have drawn attention due to their improved stability; still, reports on light-emitting DJ lead-free perovskites are scarce. Herein, a room-temperature ligand assisted re-precipitation method is used to produce ODASnBr4 perovskite microcrystals (ODA denotes protonated 1,8-octanediamine). After incorporating molecular dopants chloroform and dichloromethane, not only the crystallinity of the DJ perovskite phase improves, but their emission becomes much stronger due to the formation of hydrogen bonds between [SnBr6]4− octahedra and acidic C H proton donors. ODASnBr4 microcrystals doped with these molecules show a high photoluminescence quantum yield (PLQY) approaching 90%, and their emission remains stable under a continuous UV irradiation, with less than 10% loss in intensity over 6 h. Moreover, by tuning the pristine ODASnBr4 with various degrees of exposure to the molecular dopants, the maximum of their self-trapped exciton emission can be fine-tuned over a spectral range of 570–608 nm while maintaining high PLQYs of 83–88%. This provides a convenient way to adjust the spectral position of DJ perovskite emission without changing halides or A-site spacers. Thus, stable and strongly emitting lead-free DJ perovskite materials have been developed.  相似文献   

8.
Halide perovskites are potential next-generation optoelectronic devices. However, the film quality of this charming material fabricated by the conventional spin-coating method is far from satisfactory, significantly affecting the optoelectronic devices' performance. Here, one facile slow-evaporating solvent (SE) method is demonstrated to synthesize high-quality organic–inorganic halide perovskite films. Compared with the conventional spin coating method, the films fabricated by this SE method show much higher crystallinity, oriented lattice, smoother surface morphology, and lower trap density. Besides, the photodetector manufactured by the SE method-based film also performs much better than the ones by the spin-coating method. Importantly, this universal method can be applied to different organic–inorganic halide perovskites, such as Dion–Jacobson (DJ) type and Ruddlesden–Popper type 2D halide perovskites and conventional 3D halide perovskites. This work gives an effective solution to improve the quality of the DJ-type halide perovskites, which endows the halide perovskites with a more practical chance to be commercialized cosmically.  相似文献   

9.
Dion–Jacobson (DJ)-type 2D halide perovskites present superior environmental stability and a narrower bandgap, yet a contradiction between charge transport and stability remains to be resolved. Herein, it is shown that both symmetry and substitution of the organic spacer in DJ perovskites synergistically direct the narrow interlayer spacing, staggered spacer alignment, and regular phase arrangement, thereby promoting out-of-plane carrier transport and ambient stability. Compared to its symmetric para-xylylenediamine (PDMA) counterpart, the asymmetric 2-(4-aminophenyl)ethylamine (PMEA) spacer largely aids in compressing the inorganic octahedra layer to form a non-confinement structure with decreased exciton binding energy, while stacked benzene rings enable a staggered alignment of spacers. Such non-confined structures are less remarkable in meta-substituted diamine-based DJ perovskites than those para-ones, which retard carrier transport from 2D to quasi-2D phases. The preferential PMEA spacer however requires a long relaxation time to form a dense and ordered staggered alignment, which is realized by a slight addition of strong-coordinating DMSO into the DMF solvent, thus decelerating crystallization and further optimizing lamellar orientation. As a result, a best efficiency of ≈ 12% is achieved in (PMEA)MA3Pb4I13 based p-i-n type planar solar cells. Importantly, such unencapsulated devices can maintain 81% initial efficiencies after storage in ambient conditions ( ≈ 60% relative humidity, ≈ 20 °C) for 700 h.  相似文献   

10.
Quasi-2D CsPbI3 perovskites have emerged as excellent candidates for advanced photovoltaic technologies due to their fundamentally enhanced stability than conventional 3D counterparts. However, the applications of quasi-2D perovskites are plagued with their poor out-of-plane carrier mobility induced by the intercalated insulating organic layers. In this work, a new strategy is explored to significantly enhance the out-of-plane charge transport in quasi-2D Dion–Jacobson (DJ) CsPbI3 perovskites via leveraging the intercalation of aromatic diamine cations (p-phenylenediamine, PPDA) with unique π-conjugated bond based on the first-principles calculations. The strong interactions between PPDA2+ cations and inorganic Pb-I framework (i.e., I–I interaction, p-π coupling, and H-bonds) provide three carrier pathways to facilitate the out-of-plane charge transport. Furthermore, the restricted in-plane and out-of-plane structural distortion induced by the π-conjugated bond could improve the electronic coupling and charge mobility along the out-of-plane direction with reduced bandgaps. As a proof of concept, the calculated average photovoltaic conversion efficiency of such engineered DJ CsPbI3 perovskite solar cells is ≈17%, which is very close to the certificated champion efficiency of 3D α-CsPbI3, underscoring their potential for solar cell applications.  相似文献   

11.
While quasi-2D perovskite is often used in inverted perovskite solar cells (PSCs) to improve the interfacial carrier transfer, the development of pure 2D perovskite with superior stability is rarely seen and the corresponding carrier-extraction kinetics remains unclear. Here, a variety of hexatomic ring cations including piperidine, pyridine, and cyclohexane are introduced to modify the perovskite/electron transport layer interface. The Dion–Jacobson phase 2D cladding (n = 1) based on 3-(aminomethyl) piperidinium is proved to form a coordinated energy landscape and homogeneous surface potential distribution, and effectively prolong the electron diffusion length (≈1.58 µm) and accelerate the hot-carrier extraction rate (2.5 times that of Control at 400 K). Furthermore, the quasi-2D treatment (n ≈ 3,4) demonstrated a slight escalation in short-circuit current, but failed to inhibit the interdiffusion of Ag, Pb, and I under illumination. Finally, one of the state-of-art power conversion efficiency (PCE) for MA-free inverted PSCs is achieved at 23.62% with increased open-circuit voltage (≈1.15 V) and fill factor (≈82.8%). Most importantly, 89% and 93.6% of initial PCE are retained after 720 h under 85 °C heating and 1000 h under maximum power point tracking, illustrating satisfactory thermal and operational stability with pure 2D perovskite capping layer.  相似文献   

12.
2D Dion–Jacobson (DJ) tin halide perovskite shows impressive stability by introducing diamine organic spacer. However, due to the dielectric confinement and uncontrollable crystallization process, 2D DJ perovskite usually exhibits large exciton binding energy and poor film quality, resulting in unfavorable charge dissociation, carrier transport and device performance. Here, the ortho-, meta-, and para-isomers of phenylenediamine (PDA) are designed for 2D DJ tin halide perovskites. Theoretical simulation and experimental characterizations demonstrate that compared with p-PDA and m-PDA, o-PDA shows larger dipole moment, which further reduces the exciton binding energy for the 2D perovskites. Besides, there is a strong hydrogen bond interaction between o-PDA cation and inorganic octahedron, which not only improves the structural stability, but also induces larger aggregates in the precursor to form dense and uniform high-quality films, and strengthens the antioxidant barrier. More interestingly, femtosecond transient absorption further proves that o-PDA organic spacers can reduce unfavorable small n-phases, resulting in sufficient and effective charge transfer between different n-value. As a result, the 2D DJ (o-PDA)FA3Sn4I13 solar cells achieve a record power conversion efficiency of 7.18%. The study furnishes an effective method to optimize the carrier transport and device performance by tailoring the chemical structure of organic spacers.  相似文献   

13.
As the power-conversion efficiency (PCE) of organic–inorganic lead halide perovskite solar cells (PSCs) is approaching the theoretical maximum, the most crucial issue concerns long-term ambient stability. Here, the application of PCN-224 quantum dots (QDs) is reported, a typical Zr-based porphyrinic metal–organic framework (MOF), to enhance the ambient stability of PSCs. PCN-224 QDs with abundant Lewis-base groups (e.g., CO, C−N, CN) contribute to high-quality perovskite films with enlarged grain size and reduced defect density by interaction with under-coordinated Pb2+. Meanwhile, PCN-224 QDs enable the well-matched energy level at the perovskite/hole transport layer (HTL) interface, thereby facilitating hole extraction and transport. More importantly, PCN-224 QDs-treated HTL can capture Li+ from bis(trifluoromethanesulfonyl)imide additive, leading to the reduced aggregation and less direct contact with moisture for hygroscopic Li-TFSI. Moreover, PCN-224 QDs mitigated Li+ ion migration into the perovskite layer, thus avoiding the formation of deleterious defects. The resultant devices yield a champion PCE of 22.51%, along with substantially improved durability, including humidity, thermal and light soaking stabilities. The findings provide a new approach toward efficient and stable PSCs by applying MOF QDs.  相似文献   

14.
Lead selenide (PbSe)-based nanomaterials have been extensively investigated as building blocks for next-generation optoelectronic devices owing to their unique properties. In this work, PbSe nanocrystals (NCs) have been successfully fabricated by a facile liquid phase exfoliation approach and directly applied as active materials for photo-electrochemical (PEC)-type photodetectors (PDs). Taking advantage of broadband absorption and fast carrier dynamics, the PbSe NCs-based PDs exhibit excellent photo-current density (11.88 μA cm−2), photo-responsivity (12.37 mA W−1), response/recovery time (0.12/0.13 s), and long-term cycling stability. The working mechanism of PbSe NCs-based PDs is explored by density functional theory calculations based on their structural and electronic properties under various conditions. It is anticipated that this contribution paves the way to readily fabricate low-dimensional PbSe NCs and extend their practical applications in PEC-type PDs.  相似文献   

15.
Organic—inorganic hybrid perovskites have attracted considerable attention for developing novel optoelectronic devices owing to their excellent photoresponses. However, conventional nanolithography of hybrid perovskites remains a challenge because they undergo severe damage in standard lithographic solvents, which prohibits device miniaturization and integration. In this study, a novel transparent stencil nanolithography (t-SL) technique is developed based on focused ion beam (FIB)-assisted polyethylene terephthalate (PET) direct patterning. The proposed t-SL enables ultrahigh lithography resolution down to 100 nm and accurate stencil mask alignment. Moreover, the stencil mask can be reused more than ten times, which is cost-effective for device fabrication. By applying this lithographic technique to hybrid perovskites, a high-performance 2D hybrid perovskite heterostructure photodetector is fabricated. The responsivity and detectivity of the proposed heterostructure photodetector can reach up to 28.3 A W−1 and 1.5 × 1013 Jones, respectively. This t-SL nanolithography technique based on FIB-assisted PET direct patterning can effectively support the miniaturization and integration of hybrid-perovskite-based electronic devices.  相似文献   

16.
Aqueous supercapacitors (ASCs) and batteries (ABs) have drawn great attention as promising energy storage devices. However, the key issues of limited energy density of ASCs and inferior power density/poor cycling life of ABs discourage their further application. Herein, a new concept of advanced aqueous supercabatteries (ASCBs) realized by nanosilver-promoted trimetallic Ni–Co–Mn perovskite fluorides (K1.0Ni0.4Co0.2Mn0.4F3.2 (KNCMF-10#)/Ag(37%), denoted as 10#/Ag(37%)) electrode materials is proposed, integrating with the respective superior specific power/cycling behavior and energy density of ASCs and ABs. A pseudocapacitance-dominated multielectrons phase conversion mechanism of the 10#/Ag(37%) electrode materials can be deduced by ex situ characterizations and electrochemical techniques. The constructed ASCBs by matching 10#/Ag(37%) cathode with activated carbon (AC)/Bi(17%) anode achieve great energy density without sacrifice of power density and cycling life in wide temperatures, benefiting from the synergistic energy storage superiority of ASCs and ABs containing capacitive, pseudocapacitive, and Faradaic response in electrochemical processes. Overall, this work highlights the new idea of nano-Ag-promoted trimetallic Ni–Co–Mn perovskite fluorides with a pseudocapacitive multielectrons phase conversion mechanism as a new pop star for advanced ASCBs, showing a great significance in the context of designing advanced electrode materials and in-depth understanding of their complicated charge storage mechanisms for aqueous electrochemical energy storage systems.  相似文献   

17.
Formamidinium lead triiodide (FAPbI3) with an ideal bandgap and good thermal stability has received wide attention and achieved a record efficiency of 26% in n–i–p (regular) perovskite solar cells (PSCs). However, imperfect FAPbI3 formation on the typical hole transport layer (HTL), high interfacial trap-state density, and unfavorable energy alignment between the HTL and FAPbI3 result in the inferior photovoltaic performance of p–i–n (inverted) PSCs with FAPbI3 absorber. Herein, the α-phase FAPbI3 is stabilized by constructing a buffer interface region between the NiOx HTL and FAPbI3, which not only diminishes NiOx/FAPbI3 interfacial reactions and defects but also facilitates carrier transport. Upon the construction of a buffer interface region, FAPbI3 inverted PSC exhibits a high-power conversion efficiency of 23.56% (certified 22.58%) and excellent stability, retaining 90.7% of its initial efficiency after heating at 80 °C for 1000 h and 84.6% of the initial efficiency after operating at the maximum power point under continuous illumination for 1100 h. Besides, as a light-emitting diode device, the FAPbI3 inverted PSC can be directly lit with an external quantum efficiency of 1.36%. This study provides a unique and efficient strategy to advance the application of α-phase FAPbI3 in inverted PSCs.  相似文献   

18.
The development of mutually reinforcing solar-driven interfacial evaporation (SDIE) and integrated functional materials/systems to achieve efficient production of freshwater and energy/matters simultaneously under extremely high solar utilization is in high demand. Herein, an integrated SDIE reaction system (reduced graphene oxide (rGO)-palladium (Pd) catalytic evaporator, rGO-Pd) is first reported, where SDIE and the integrated catalytic reaction are mutually reinforced. The apparent utilization of solar to thermal energy by the integrated SDIE reaction system is a combination of evaporative utilization and catalytic utilization. The reaction heat released by the rGO-Pd catalytic evaporator enhances its anti-salt water production performance to a record of 12.7 L m−2 h−1, surpassing the reported performance of other integrated SDIE reaction systems. In the rGO-Pd catalytic evaporator, the synergetic effect of photothermal and rapid mass transfer significantly increases the catalytic activity (turnover frequency) of Pd catalysts up to a record 125.07 min−1, which is about 3.75 times of the condition without light. This integrated SDIE reaction system can effectively and simultaneously produce freshwater, salt, and catalyzed chemicals after evaporating water to dryness. This study paves the way for SDIE's high-performance applications in future integrated water, energy, and environmental systems.  相似文献   

19.
In this paper, we utilize clustering to achieve energy efficiency for the on–off wireless sensor network, whose member nodes alternate between active and inactive states. In the proposed Distributed and Energy Efficient Self Organization (DEESO) scheme, the head election is adjusted adaptively to the remaining battery levels of local active nodes, which is a completely distributed approach compared to LEACH that relying on other routing schemes to access global information. Furthermore, we apply the Adaptive Channel Assignment (ACA) to address the on-off topology changes. Simulation results show that DEESO delivers 184% amount of data to the base station as LEACH for the same amount of energy consumption and the effective network lifetime is extended by around 50%.  相似文献   

20.
Inorganic hole-transport layers (HTLs) are widely investigated in perovskite solar cells (PSCs) due to their superior stability compared to the organic HTLs. However, in p–i–n architecture when these inorganic HTLs are deposited before the perovskite, it forms a suboptimal interface quality for the crystallization of perovskite, which reduces device stability, causes recombination, and limits the power conversion efficiency of the device. The incorporation of an appropriate functional group such as sulfur-terminated surface on the HTL can enhance the interface quality due to its interaction with perovskite during the crystallization process. In this work, a bifunctional Al-doped CuS film is wet-deposited as HTL in p–i–n architecture PSC, which besides acting as an HTL also improves the crystallization of perovskite at the interface. Urbach energy and light intensity versus open-circuit voltage characterization suggest the formation of a better-quality interface in the sulfide HTL–perovskite heterojunction. The degradation behavior of the sulfide-HTL-based perovskite devices is studied, where it can be observed that after 2 weeks of storage in a controlled environment, the devices retain close to 95% of their initial efficiency.  相似文献   

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