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Carbon-based hole transport layer-free perovskite solar cells (PSCs) based on methylammonium lead triiodide (MAPbI3 ) have become one of the research focus due to low cost, easy preparation, and good optoelectronic properties. However, instability of perovskite under vacancy defects and stress-strain makes it difficult to achieve high-efficiency and stable power output. Here, a soft-structured long-chain 2D pentanamine iodide (abbreviated as "PI") is used to improve perovskite quality and interfacial mechanical compatibility. PI containing CH3 (CH2 )4 NH3 + and I- ions not only passivate defects at grain boundaries, but also effectively alleviate residual stress during high temperature annealing via decreasing Young's modulus of perovskite film. Most importantly, PI effectively increases matching degree of Young's modulus between MAPbI3 (47.1 GPa) and carbon (6.7 GPa), and strengthens adhesive fracture energy (Gc ) between perovskite and carbon, which is helpful for outward release of nascent interfacial stress generated under service conditions. Consequently, photoelectric conversion efficiency (PCE) of optimal device is enhanced from 10.85% to 13.76% and operational stability is also significantly improved. 83.1% output is maintained after aging for 720 h at room temperature and 25-60% relative humidity (RH). This strategy of regulation from chemistry and physics provides a strategy for efficient and stable carbon-based PSCs.
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This study demonstrates an acetate ligand (AcO-)-assisted strategy for the controllable and tunable synthesis of colloidal methylammonium lead iodide (MAPbI3) perovskite nanocrystals (PNCs) for efficient photovoltaic and photodetector devices. The size of colloidal MAPbI3 PNCs can be tuned from 9 to 20 nm by changing the AcO-/MA ratio in the reaction precursor. In situ observations and detailed characterization results show that the incorporation of the AcO- ligand alters the formation of PbI6 octahedral cages, which controls PNC growth. A well-optimized AcO-/MA ratio affords MAPbI3 PNCs with a low defect density, a long carrier lifetime, and unique solid-state isotropic properties, which can be used to fabricate solution-processed dual-mode photovoltaic and photodetector devices with a conversion efficiency of 13.34% and a detectivity of 2 × 1011 Jones, respectively. This study provides an avenue to further the precisely controllable synthesis of hybrid PNCs for multifunctional optoelectronic applications.
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Here, we have synthesized methylammonium based two metal halide perovskites (MHP) such as MAPbBr3, and MAPbI3 using methylammonium bromide, methylammonium iodide, lead bromide, respective at room temperature under certain experimental conditions. All synthesized MHPs have been confirmed through X-ray diffraction technique (XRD), scanning electron microscope (SEM), Fourier transform infra-red (FTIR) and photoluminescence (PL) analysis. Afterward, comparative evaluation on optical sensing capability has been made for both MHPs using PL in different solvents. Importantly, we find out that MAPbBr3 exhibit an excellent optical feature over MAPbI3 in hexane only. Afterward, MAPbBr3 has also been explored to know the sensing capability for nitrobenzene sensing. Our model study confirms that MAPbBr3 is an excellent sensing material with R square (0.87), selectivity (16.9%) and Stern Volmer constant (Ksv=10- 2 × 0.464) for nitrobenzene in hexane.
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Inspired by its great success in the photovoltaic field, methylammonium lead iodide perovskite (MAPbI3 ) has recently been actively explored as photocatalysts in H2 evolution reactions. However, the practical application of MAPbI3 photocatalysts remains hampered by the intrinsically fast trapping and recombination of photogenerated charges. Herein, we propose a novel strategy of regulating the distribution of defective areas to promote charge-transfer dynamics of MAPbI3 photocatalysts. By deliberately designing and synthesizing the MAPbI3 photocatalysts featuring a unique continuation of defective areas, we demonstrate that such a feature enables retardation of charge trapping and recombination via lengthening the charge-transfer distance. As an outcome, such MAPbI3 photocatalysts turn out to achieve an impressive photocatalytic H2 evolution rate as high as 0.64â mmol â g-1 â h-1 , one order of magnitude higher than that of the conventional MAPbI3 photocatalysts. This work establishes a new paradigm for controlling charge-transfer dynamics in photocatalysis.
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The properties of CH3NH3PbI3(MAPbI3) crystalline thin films and the device performance of highly efficient MAPbI3photovoltaic cells are investigated by varying the temperature of the antisolvent from 20 °C to 50 °C during the washing enhanced nucleation (WEN) process. The surface, structural, optoelectronic and defect properties of the perovskite thin films are characterized through atomic-force microscopy, X-ray diffractometry and photoluminescence spectrometry. The experimental results show that changing the temperature of the antisolvent during the WEN process can manipulate the MAPbI3crystalline thin films from the (110)-(002) complex phase to a (002) preferred phase. It is noted that the highest power conversion efficient of the inverted MAPbI3photovoltaic cells is 19.30%, mainly due to the increased carrier collection efficiency and reduced carrier recombination when the temperature of the antisolvent is 30 °C.
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Organic-inorganic hybrid MAPbI3 microwires show unique optoelectronic properties for high performances of photodetectors (PDs). However, the defects-assisted nonradiative recombination is harmful for carrier transport, which limits the performances improvement of MAPbI3 microwires PDs. Traditional organic passivation agents effectively combine the surface defects of microwires and also reduce the mobility of overall film based on the perovskite microwires. Therefore, the improvement of internal carrier transport of microwires and the mobility of integrated film simultaneously is a particular challenge for fabrication of performances enhanced perovskite microwires PDs. Here, the Ti3 C2 Tx NCs are fabricated by nonfocus laser irradiation in liquid environment, and hybrids the high conductive NCs in the MAPbI3 microwires. The presence of Ti3 C2 Tx NCs renders defects passivation, enhancement of crystalline orientation, charge transport, and carrier extraction for MAPbI3 microwires, and boots the mobility of microwires based film, leading to about tenfolds enhancement of performances of PDs than that of the control. The maximum responsivity and the detectivity of the Ti3 C2 Tx NCs embedded MAPbI3 microwires PDs reach to 1.70 A W-1 and 7.0 × 1011 Jones in visible window, respectively. The findings suggest that the laser generated high conductive Ti3 C2 Tx NCs is an effective additive for perovskite microwires to fabricate performances enhanced optoelectronics.
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Pyro-phototronic and piezo-phototronic effect have shown their important roles for high performance heterojunction-based photodetectors (PDs). Here, a coupling effect of pyro-phototronic and piezo-phototronic effect is utilized to fabricate a self-powered and broadband PD based on the MAPbI3 single-crystal film/n-Si heterojunction. First, by using the pyro-phototronic effect derived from MAPbI3 , the maximum photoresponsivity of the self-powered PD is 1.5 mA W-1 for 780 nm illumination, which is enhanced by more than 20 times in consideration of the relative peak-to-peak output current. Light-induced temperature change in MAPbI3 film will create pyro-charges distributed at heterojunction interface, resulting in a downward bending of the energy band, facilitating the transport of photon-generated electrons and holes, and generating spike-like output currents. Second, piezo-phototronic effect is further introduced by applying vertical pressures onto the PD. With a vertical pressure of 155 kPa, the responsivity can be improved by more than 120% compared to the condition with no pressure. The overall enhancement is due to the piezo-phototronic and pyro-phototronic coupling effects which utilize the polarization charges to modulate the band structure of heterojunction. These results provide a promising approach to develop high-performance self-powered and broadband perovskite-based PDs by coupling pyro-phototronic and piezo-phototronic effect.
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Organic-inorganic hybrid perovskites (OIHPs) have recently emerged as groundbreaking semiconductor materials owing to their remarkable properties. Transmission electron microscopy (TEM), as a very powerful characterisation tool, has been widely used in perovskite materials for structural analysis and phase identification. However, the perovskites are highly sensitive to electron beams and easily decompose into PbX2 (X = I, Br, Cl) and metallic Pb. The electron dose of general high-resolution TEM is much higher than the critical dose of MAPbI3 , which results in universal misidentifications that PbI2 and Pb are incorrectly labelled as perovskite. The widely existed mistakes have negatively affected the development of perovskite research fields. Here misidentifications of the best-known MAPbI3 perovskite are summarised and corrected, then the causes of mistakes are classified and ascertained. Above all, a solid method for phase identification and practical strategies to reduce the radiation damage for perovskite materials have also been proposed. This review aims to provide the causes of mistakes and avoid misinterpretations in perovskite research fields in the future.
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Atomic-force microscopic images, x-ray diffraction patterns, Urbach energies and photoluminescence quenching experiments show that the interfacial contact quality between the hydrophobic [6,6]-phenyl-C61-buttric acid methyl ester (PCBM) thin film and hydrophilic CH3NH3PbI3(MAPbI3) thin film can be effectively improved by using a binary antisolvent mixture (toluene:dichloromethane or chlorobenzene:dichloromethane) in the anti-solvent mixture-mediated nucleation process, which increases the averaged power conversion efficiency of the resultant PEDOT:PSS (P3CT-Na) thin film based MAPbI3solar cells from 13.18% (18.52%) to 13.80% (19.55%). Beside, the use of 10% dichloromethane (DCM) in the binary antisolvent mixture results in a nano-textured MAPbI3thin film with multicrystalline micrometer-sized grains and thereby increasing the short-circuit current density and fill factor (FF) of the resultant solar cells. It is noted that a remarkable FF of 80.33% is achieved, which can be used to explain the stable photovoltaic performance without additional encapsulations.
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Perovskite crystal quality plays an important role in perovskite solar cells, given that multiple grain boundaries and trap states in the perovskite films hamper further enhancement of solar cell efficiency. Using the solution method to prepare perovskite films with large grains and high coverage requires further improvements. Herein, we introduce Lewis base urea as an additive into the precursor of perovskite to control the crystallization dynamics, allowing for large-grain crystal growth. As a result, MAPbI3films with urea as an additive are well crystallized with large crystal grains of sizes >3µm. The large-grain perovskite is found to simultaneously improve the power-conversion efficiency (PCE) and device stability. With an optimal urea additive of 20 mol%, the PCE is significantly increased from 15.47% for the reference MAPbI3solar cell to 18.53% for the device with MAPbI3with urea as an additive. Finally, the optimized device demonstrates excellent stability and maintains 80% of the initial PCE after 60 days.
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The averaged power conversion efficiency of polyelectrolytes (P3CT-Na) based MAPbI3solar cells can be increased from 14.94% to 17.46% with a wetting method before the spin-coating process of MAPbI3precursor solutions. The effects of the wetting process on the surface, structural, optical and excitonic properties of MAPbI3thin films are investigated by using the atomic-force microscopic images, x-ray diffraction patterns, transmittance spectra, photoluminescence spectra and Raman scattering spectra. The experimental results show that the wetting process of MAPbI3precursor solution on top of the P3CT-Na/ITO/glass substrate can be used to manipulate the molecular packing structure of the P3CT-Na thin film, which determines the formation of MAPbI3thin films.
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This work demonstrates a novel photovoltaic application in which graphdiyne (GD) can be employed as a host material in a perovskite active layer for the first time. In the device fabrication, the best molar ratio for active materials is verified as PbI2/MAI/GD being 1:1:0.25, yielding a peak power-conversion efficiency of 21.01%. We find that graphdiyne, as the host material, exerts significant influence on the crystallization, film morphology, and a series of optoelectronic properties of the perovskite active layer. A uniform MAPbI3 film with highly crystalline qualities, large domain sizes, and few grain boundaries was realized with the introduction of graphdiyne. Moreover, the current-voltage hysteresis was negligible, and device stability was significantly improved as well. The results indicate that graphdiyne as the host active material presents great potential for the enhancement of the performance of perovskite solar cells.
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Raman and photoluminescence (PL) spectroscopy are used to investigate dynamic structure-function relationships in methylammonium lead iodide (MAPbI3) perovskite. The intensity of the 150 cm-1 methylammonium (MA) librational Raman mode is found to be correlated with PL intensities in microstructures of MAPbI3. Because of the strong hydrogen bond between hydrogens in MA and iodine in the PbI6 perovskite octahedra, the Raman activity of MA is very sensitive to structural distortions of the inorganic framework. The structural distortions directly influence PL intensities, which in turn have been correlated with microstructure quality. Our measurements, supported with first-principles calculations, indicate how excited-state MA librational displacements mechanistically control PL efficiency and lifetime in MAPbI3-material parameters that are likely important for efficient photovoltaic devices.
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Longer carrier diffusion length and improved power conversion efficiency have been reported for thin-film solar cell of organolead mixed-halide perovskite MAPbI3- x Cl x in comparison with MAPbI3 . Instead of substituting I in the MAPbI3 lattice, Cl-incorporation has been shown to mainly improve the film morphology of perovskite absorber. Well-defined crystal structure, adjustable composition (x), and regular morphology, remains a formidable task. Herein, a facile solution-assembly method is reported for synthesizing single-crystalline nanofibers (NFs) of tetragonal-lattice MAPbI3- x Cl x with the Cl-content adjustable between 0 ≤ x ≤ 0.75, leading to a gradual blueshift of the absorption and photoluminescence maxima from x = 0 to 0.75. The photoresponsivity (R) of MAPbI3 NFs keeps almost unchanging at a value independent of the white-light illumination intensity (P). In contrast, R of MAPbI3- x Cl x NFs decreases rapidly with increasing both the x and P values, indicating Cl-substitution increases the recombination traps of photogenerated free electrons and holes. This study provides a model system to examine the role of extrinsic Cl ions in both perovskite crystallography and optoelectronic properties.
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Additive engineering, with its excellent ability to passivate bulk or surface perovskite defects, has become a common strategy to improve the performance and stability of perovskite solar cells (PVSCs). Among the various additives reported so far, ammonium salts are considered an important branch. It is worth noting that although both ammonium-based additives (R-NH3 +) and amine-based additives (R-NH2) are derivatives of ammonia (NH3), the functions of the two can be easily confused due to their structural similarities. Moreover, there is no comprehensive comparative analysis of them in the literature. Here, the differences between phenethylammonium iodide (PEA+) and phenethylamine (PEA) additives are revealed experimentally and theoretically. The results clearly show that PEA outperforms PEA+ in terms of device performance and stability based on the following three factors: i) PEA's defect passivation capability is superior to that of PEA+; ii) PEA has better hydrophobicity to hinder water ingress; and iii) PEA completely improves the stability of PVSCs by enhancing thermal stability and inhibiting iodide migration in perovskite more effectively than PEA+. As a result, the power conversion efficiency (PCE) of the inverted methylammonium triiodide (MAPbI3) device using PEA increases by ≈15% to over 21%. More importantly, this device exhibits greater ability to prevent water invasion, thermal-induce degradation, and inhibit iodide ion migration, resulting in better long-term stability.
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The study elucidates the potential benefits of incorporating a BiI3 interfacial layer into perovskite solar cells (PSCs). Using MAPbI3 and MAGeI3 as active layers, complemented by the robust TiO2 and Spiro-OMeTAD as the charge-transport-layers, we employed the SCAPS-1D simulation tool for our investigations. Remarkably, the introduction of the BiI3 layer at the perovskite-HTL interface significantly enhanced hole extraction and effectively passivated defects. This approach minimized charge recombination and ion migration towards opposite electrodes, thus elevating device performance relative to conventional configurations. The efficiency witnessed a rise from 19.28 to 20.30% for MAPbI3 and from 11.90 to 15.57% for MAGeI3. Additionally, MAGeI3 based PSCs saw an improved fill-factor from 50.36 to 62.85%, and a better Jsc from 13.22 to 14.2 mA/cm2, signifying reduced recombination and improved charge extraction. The FF for MAPbI3 based PSCs saw a minor decline, while the Voc slightly ascended from 1.24 to 1.25 V and Jsc from 20.01 to 21.6 mA/cm2. A thorough evaluation of layer thickness, doping, and temperature further highlighted the critical role of the BiI3 layer for both perovskite variants. Our examination of bandgap alignments in devices with the BiI3 interfacial layer also offers valuable understanding into the mechanisms fueling the observed improvements.
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Organic-inorganic hybrid perovskite solar cells (PSCs) have recently been demonstrated to be promising renewable harvesters because of their prominent photovoltaic power conversion efficiency (PCE), although their stability and efficiency still have not reached commercial criteria. Trouble-oriented analyses showcase that defect reduction among the grain boundaries and interfaces in the prepared perovskite polycrystalline films is a practical strategy, which has prompted researchers to develop functional molecules for interface passivation. Herein, the pyridine-based bifunctional molecule dimethylpyridine-3,5-dicarboxylate (DPDC) was employed as the interface between the electron-transport layer and perovskite layer, which achieved a champion PCE of 21.37% for an inverted MAPbI3-based PSC, which was greater than 18.64% for the control device. The mechanistic studies indicated that the significantly improved performance was mainly attributed to the remarkably enhanced fill factor with a value greater than 83%, which was primarily due to the nonradiative recombination suppression offered by the passivation effect of DPDC. Moreover, the promoted carrier mobility together with the enlarged crystal size contributed to a higher short-circuit current density. In addition, an increase in the open-circuit voltage was also observed in the DPDC-treated PSC, which benefited from the improved work function for reducing the energy loss during carrier transport. Furthermore, the DPDC-treated PSC showed substantially enhanced stability, with an over 80% retention rate of its initial PCE value over 300 h even at a 60% relative humidity level, which was attributed to the hydrophobic nature of the DPDC molecule and effective defect passivation. This work is expected not only to serve as an effective strategy for using a pyridine-based bifunctional molecule to passivate perovskite interfaces to enhance photovoltaic performance but also to shed light on the interface passivation mechanism.
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Recently, perovskite photodetectors (PDs) are risen to prominence due to substantial research interest. Beyond merely tweaking the composition of materials, a cutting-edge advancement lies in leveraging the innate piezoelectric polarization properties of perovskites themselves. Here, the investigation shows utilizing Ti3C2Tx, a typical MXene, as an intermediate layer for significantly boosting the piezoelectric property of MAPbI3 thin films. This improvement is primarily attributed to the enhanced polarization of the methylammonium (MA+) groups within MAPbI3, induced by the OH groups present in Ti3C2Tx. A flexible PD based on the MAPbI3/MXene heterostructure is then fabricated. The new device is sensitive to a wide range of wavelengths, displays greatly enhanced performance owing to the piezo-phototronic coupling. Moreover, the device is endowed with a greatly reduced response time, down to millisecond level, through the pyro-phototronic effect. The characterization shows applying a -1.2% compressive strain on the PD leads to a remarkable 102% increase in the common photocurrent, and a 76% increase in the pyro-phototronic current. The present work reveals how the emerging piezo-phototronic and pyro-phototronic effects can be employed to design high-performance flexible perovskite PDs.
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This study compared the photoluminescence (PL) stabilities of formamidinium (FA) and methylammonium (MA) in lead iodide perovskite quantum dots (QDs). To exclude other factors, such as size and purity, that may affect stability, MAPbI3 and FAPbI3 QDs with nearly identical sizes (~10.0â nm) were synthesized by controlling the ligand concentration and synthesis temperature. Transmission electron microscopy images and X-ray diffraction patterns confirmed homogeneous single-phase perovskite structures. Additionally, the bandgaps and sizes of the synthesized QDs closely matched those of the infinite quantum well model, which guaranteed that the photostability was solely caused by the different organic molecules in the two QDs. We analyzed the PL peak centers and full-width at half maximum of the QDs for 32â days. The enhanced stability of FAPbI3 was found to be caused by the nearly zero redshift (1.615â eV) of its PL peak, in contrast to the redshift (1.685â1.670â eV) of MAPbI3.
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The phase-transfer ligand exchange of PbS quantum dots (QDs) has substantially simplified device fabrication giving hope for future industrial exploitation. However, this technique when applied to QDs of large size (>4 nm) gives rise to inks with poor colloidal stability, thus hindering the development of QDs photodetectors in short-wavelength infrared range. Here, it is demonstrated that methylammonium lead iodide ligands can provide sufficient passivation of PbS QDs of size up to 6.7 nm, enabling inks with a minimum of ten-week shelf-life time, as proven by optical absorption and solution-small angle X-ray scattering. Furthermore, the maximum linear electron mobility of 4.7 × 10-2 cm2 V-1 s-1 is measured in field-effect transistors fabricated with fresh inks, while transistors fabricated with the same solution after ten-week storage retain 74% of the average starting electron mobility, demonstrating the outstanding quality both of the fresh and aged inks. Finally, photodetectors fabricated via blade-coating exhibit 76% external quantum efficiency at 1300 nm and 1.8 × 1012 Jones specific detectivity, values comparable with devices fabricated using ink with lower stability and wasteful methods such as spin-coating.