RESUMEN
The highly oriented 2D perovskite templates of n = 1 have typically been created to attain controllable and oriented crystallization of 3D α-phase formamidinium lead triiodide (α-FAPbI3) perovskites. However, the role of methylammonium iodide (MAI), a widely used α-FAPbI3 phase stabilizer, in regulating the growth dynamics of 2D/3D perovskites is generally ignored. Herein, Ruddlesden-Popper type n = 1 2D octylammonium lead iodide (OA2PbI4) perovskites are added into FAPbI3 precursor solution. The template of n = 2 (OA2MAPb2I7), which is spontaneously constructed by the mixture of n = 1 2D and methylammonium chloride (MACl), acts as a skeleton to template the epitaxial growth of α-FAPbI3. However, the volatilization of MACl inevitably causes damage to the 2D structure during thermal annealing. This study reveals that small amounts of less volatile MAI additive enables the creation of stable 2D template, leading to more controlled vertical orientation crystallization. Consequently, the high-quality mixed-dimensional perovskite film delivers a high efficiency of 24.19% together with improved intrinsic stability. This work provides an in-depth understanding of 2D-assisted controlled epitaxial growth of α-FAPbI3.
RESUMEN
The stabilization of the formamidinium lead iodide (FAPbI3) structure is pivotal for the development of efficient photovoltaic devices. Employing two-dimensional (2D) layers to passivate the three-dimensional (3D) perovskite is essential for maintaining the α-phase of FAPbI3 and enhancing the power conversion efficiency (PCE) of perovskite solar cells (PSCs). However, the role of bulky ligands in the phase management of 2D perovskites, crucial for the stabilization of FAPbI3, has not yet been elucidated. In this study, we synthesized nanoscale 2D perovskite capping crusts with
RESUMEN
Metal halide perovskite solar cells have achieved tremendous progress and have attracted enormous research and development efforts since the first report of demonstration in 2009. Due to fabrication versatility, many heat treatment methods can be utilized to achieve perovskite film crystallization. Herein, 10.6 µm carbon dioxide laser process is successfully developed for the first time for perovskite film crystallization. In addition, this is the first time formamidinium lead triiodide solar cells by laser annealing under ambient are demonstrated. The champion cell produces a power conversion efficiency of 21.8%, the highest for laser-annealed perovskite cells. And this is achieved without any additive, passivation, or post-treatment.
RESUMEN
Photoactive black-phase formamidinium lead triiodide (α-FAPbI3) perovskite has dominated the prevailing high-performance perovskite solar cells (PSCs), normally for those spin-coated, conventional n-i-p structured devices. Unfortunately, α-FAPbI3 has not been made full use of its advantages in inverted p-i-n structured PSCs fabricated via blade-coating techniques owing to uncontrollable crystallization kinetics and complicated phase evolution of FAPbI3 perovskites during film formation. Herein, a customized crystal surface energy regulation strategy has been innovatively developed by incorporating 0.5â mol % of N-aminoethylpiperazine hydroiodide (NAPI) additive into α-FAPbI3 crystal-derived perovskite ink, which enabled the formation of highly-oriented α-FAPbI3 films. We deciphered the phase transformation mechanisms and crystallization kinetics of blade-coated α-FAPbI3 perovskite films via combining a series of in-situ characterizations and theoretical calculations. Interestingly, the strong chemical interactions between the NAPI and inorganic Pb-I framework help to reduce the surface energy of (100) crystal plane by 42 %, retard the crystallization rate and lower the formation energy of α-FAPbI3. Benefited from multifaceted advantages of promoted charge extraction and suppressed non-radiative recombination, the resultant blade-coated inverted PSCs based on (100)-oriented α-FAPbI3 perovskite films realized promising efficiencies up to 24.16 % (~26.5 % higher than that of the randomly-oriented counterparts), accompanied by improved operational stability. This result represented one of the best performances reported to date for FAPbI3-based inverted PSCs fabricated via scalable deposition methods.
RESUMEN
Formamidinium lead triiodide quantum dot (FAPbI3 QD) exhibits substantial potential in solar cells due to its suitable band gap, extended carrier lifetime, and superior phase stability. However, despite great attempts toward reconfiguring the surface chemical environment of FAPbI3 QDs, achieving the optimal efficiency of charge carrier extraction and transfer in cells remains a challenge. To circumvent this problem, we selectively introduced Au/FAPbI3 Schottky heterojunctions by reducing Au+ to Au0 and subsequently anchoring them on the surface of FAPbI3 QDs, which acts as a light-harvesting layer and establishes high-speed electron transfer channels (Au dot â Au dot). As a result, the champion photoelectric conversion efficiency of solar cells reached 13.68%, a significant improvement over 11.19% of that of FAPbI3-based solar cells. The enhancement is attributed to efficient and directed electron transfer as well as a more aligned energy level arrangement. This work constructed Au/FAPbI3 QD Schottky heterojunctions, providing a viable strategy to enhance QD electron coupling for high-performance optoelectronic applications.
RESUMEN
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.
RESUMEN
It is a crucial role for enhancing the power conversion efficiency (PCE) of perovskite solar cells (PSCs) to prepare high-quality perovskite films, which can be achieved by delaying the crystallization of perovskite film. Hence, we designed difluoroacetic anhydride (DFA) as an additive to regulating crystallization process thus reducing defect formation during perovskite film formation. It was found DFA reacts with DMSO by forming two molecules, difluoroacetate thioether ester (DTE) and difluoroacetic acid (DA). The strong bonding DTEâ PbI2 and DAâ PbI2 retard perovskite crystallization process for high-quality film formation, which was monitored through in situ UV/Vis and PL tests. By using DFA additives, we prepared perovskite films with high-quality and low defects. Finally, a champion PCE of 25.28 % was achieved with excellent environmental stability, which retained 95.75 % of the initial PCE after 1152â h at 25 °C under 25 % RH.
RESUMEN
α-Phase formamidinium lead iodide (FAPbI3) perovskite solar cells (PSCs) have garnered significant attention, owing to their remarkable efficiency. Methylammonium chloride (MACl), a common additive, is used to control the crystallization of FAPbI3, thereby facilitating the formation of the photoactive α-phase. However, MACl's high volatility raises concerns regarding its stability and potential impact on the stability of the device. In this study, we partially substituted MACl with n-propylammonium chloride (PACl), which has a long alkyl chain, to promote the oriented crystallization of FAPbI3, ultimately forming an δ-phase-free perovskite. The FAPbI3 film containing PACl demonstrates an enhanced photoluminescence intensity and lifetime. Additionally, PACl's presence at grain boundaries acts as a protective layer for the PSCs. Consequently, we achieved a power conversion efficiency (PCE) of 22.4% and exceptional stability. It maintains over 95% of initial PCE for 100 days in an N2 glovebox, over 85% after 100 h of maximum power point tracking, and over 80% after 60 °C thermal aging.
RESUMEN
Formamidinium-lead triiodide (FAPbI3) perovskite holds promise as a prime candidate in the realm of perovskite photovoltaics. However, the photo-active α-FAPbI3 phase, existing as a metastable state, is observable solely at elevated temperatures and is susceptible to degradation into the δ-phase in ambient air. Therefore, the attainment of phase-stable α-FAPbI3 in ambient conditions has become a crucial objective in perovskite research. Here, we proposed an efficient conversion process of PbI2 into the α-FAPbI3 perovskites in ambient air. This conversion was facilitated by the introduction of chelating molecules, which interacted with PbI2 to form an intermediate phase. Due to the reduced formation barrier resulting from the altered reaction pathway, this stable intermediate phase transitioned directly into α-FAPbI3 upon the deposition of the organic cation solution, effectively bypassing the formation of δ-FAPbI3. Consequently, the ambient-fabricated FAPbI3 perovskite solar cells (PSCs) exhibited an outstanding power conversion efficiency of 25.08 %, along with a high open-circuit voltage of 1.19â V. Furthermore, the unencapsulated devices demonstrated remarkable environmental stability. Notably, this innovative approach promises broad applicability across various chelating molecules, opening new avenues for further progress in the ambient air fabrication of FAPbI3 PSCs.
RESUMEN
The two-step sequential deposition strategy has garnered widespread usage in the fabrication of high-performance perovskite solar cells based on FAPbI3. However, the rapid reaction between FAI and PbI2 during preparation often leads to incomplete reactions, reducing the device efficiency and stability. Herein, we introduced a multifunctional additive, 2-thiophenyl trifluoroacetone (TTA), into the FAI precursor. The incorporation of TTA has proven to be highly effective in slowing the reaction rate between FAI and PbI2, resulting in increased perovskite formation and improved efficiency and stability of the devices. TTA's CF3 groups interact with FAI via hydrogen bonding, effectively suppressing FA+ defects. The S and CâO groups share lone pair electrons with uncoordinated Pb2+, leading to a reduction in perovskite film defects and suppressing nonradiative recombination. Additionally, the CF3 groups impart hydrophobicity, protecting the perovskite film from moisture-induced erosion. As a result, the TTA-modified perovskite film achieves a Champion efficiency of 23.42% compared to the control's 21.52, with 20.58% efficiency for a 25 cm2 solar module. Remarkably, the unencapsulated Champion device retains 86% of its initial PCE after 1080 h under dark conditions (60 ± 5 °C, 35 ± 5% RH), indicating enhanced long-term stability. These findings offer a promising and cost-effective tactic for high-quality perovskite film fabrication.
RESUMEN
Halide perovskite-based resistive switching memory (memristor) has potential in an artificial synapse. However, an abrupt switch behavior observed for a formamidinium lead triiodide (FAPbI3)-based memristor is undesirable for an artificial synapse. Here, we report on the δ-FAPbI3/atomic-layer-deposited (ALD)-SnO2 bilayer memristor for gradual analogue resistive switching. In comparison to a single-layer δ-FAPbI3 memristor, the heterojunction δ-FAPbI3/ALD-SnO2 bilayer effectively reduces the current level in the high-resistance state. The analog resistive switching characteristics of δ-FAPbI3/ALD-SnO2 demonstrate exceptional linearity and potentiation/depression performance, resembling an artificial synapse for neuromorphic computing. The nonlinearity of long-term potentiation and long-term depression is notably decreased from 12.26 to 0.60 and from -8.79 to -3.47, respectively. Moreover, the δ-FAPbI3/ALD-SnO2 bilayer achieves a recognition rate of ≤94.04% based on the modified National Institute of Standards and Technology database (MNIST), establishing its potential in an efficient artificial synapse.
RESUMEN
FAPbI3 stands out as an ideal candidate for the photoabsorbing layer of perovskite solar cells (PSCs), showcasing outstanding photovoltaic properties. Nonetheless, stabilizing photoactive α-FAPbI3 remains a challenge due to the lower formation energy of the competitive photoinactive δ-phase. In this study, we employ tetraethylphosphonium lead tribromide (TEPPbBr3) single crystals as templates for the epitaxial growth of PbI2. The strategic use of TEPPbBr3 optimizes the evolution of intermediates and the crystallization kinetics of perovskites, leading to high-quality and phase-stable α-FAPbI3 films. The TEPPbBr3-modified perovskite exhibits optimized carrier dynamics, yielding a champion efficiency of 25.13% with a small voltage loss of 0.34 V. Furthermore, the target device maintains 90% of its initial PCE under maximum power point (MPP) tracking over 1000 h. This work establishes a promising pathway through single crystal seed based epitaxial growth for achieving satisfactory crystallization regulation and phase stabilization of α-FAPbI3 perovskites toward high-efficiency and stable PSCs.
RESUMEN
Energy loss in perovskite grain boundaries (GBs) is a primary limitation toward high-efficiency perovskite solar cells (PSCs). Two critical strategies to address this issue are high-quality crystallization and passivation of GBs. However, the established methods are generally carried out discretely due to the complicated mechanisms of grain growth and defect formation. In this study, a combined method is proposed by introducing 3,4,5-Trifluoroaniline iodide (TFAI) into the perovskite precursor. The TFAI triggers the union of nano-sized colloids into microclusters and facilitates the complete phase transition of α-FAPbI3 at room temperature. The controlled chemical reactivity and strong steric hindrance effect enable the fixed location of TFAI and suppress defects at GBs. This combination of well-crystallized perovskite grains and effectively passivated GBs leads to an improvement in the open circuit voltage (Voc) of PSCs from 1.08 V to 1.17 V, which is one of the highest recorded Voc without interface modification. The TFAI-incorporated device achieved a champion PCE of 24.81%. The device maintained a steady power output near its maximum power output point, showing almost no decay over 280 h testing without pre-processing.
RESUMEN
Perovskite light-emitting diodes (PeLEDs) are the next promising display technologies because of their high color purity and wide color gamut, while two classical emitter forms, i.e., polycrystalline domains and quantum dots, are encountering bottlenecks. Weak carrier confinement of large polycrystalline domains leads to inadequate radiative recombination, and surface ligands on quantum dots are the main annihilation sites for injected carriers. Here, pinpointing these issues, we screened out an amphoteric agent, namely, 2-(2-aminobenzoyl)benzoic acid (2-BA), to precisely control the in situ growth of FAPbI3 (FA: formamidine) nanodomains with enhanced space confinement, preferred crystal orientation, and passivated trap states on the transport-layer substrate. The amphoteric 2-BA performs bidentate chelating functions on the formation of ultrasmall perovskite colloids (<1 nm) in the precursor, resulting in a smoother FAPbI3 emitting layer. Based on monodispersed and homogeneous nanodomain films, a near-infrared PeLED device with a champion efficiency of >22% plus enhanced T80 operational stability was achieved. The proposed perovskite nanodomain film tends to be a mainstream emitter toward the performance breakthrough of PeLED devices covering visible wavelengths beyond infrared.
RESUMEN
Fabricating perovskite solar cells (PSCs) in an ambient environment provides low-cost preparation routes for solar cells that are suitable for large-scale production. Compared with methylammonium (MA)- based perovskite materials, formamidinium lead iodide (FAPbI3) possesses a more favorable bandgap for light harvesting and better thermostability. However, the phase transition from the α-phase to the δ-phase easily occurs, making it challenging for ambient-air processing. Herein, we develop a buried interface engineering strategy via two molecules including 1,4-bis(diphenylphosphino)butane (DPPB) as well as [4-(3,6-dimethyl-9H-carbazol-9-yl)butyl] phosphonic acid (Me-4PACz) to optimize air-processed inverted FAPbI3 PSCs. This strategy regulates the crystallization process of the air-fabricated FAPbI3 perovskite film, leading to a purer α-phase with significantly enhanced crystallinity and enlarged grain sizes. Apart from improving the bulk perovskite film, the defects at the NiOx/perovskite interface are passivated, and the energy levels are better matched in the modified device, which facilitates efficient carrier extraction. Resultantly, the target device processed in the open air achieves a dramatically improved power conversion efficiency from 11.37% to 18.45%, in association with an enhanced device stability.
RESUMEN
Formamidinium lead triiodide (FAPbI3) perovskite quantum dot has outstanding durability, reasonable carrier lifetime, and long carrier diffusion length for a new generation of highly efficient solar cells. However, ligand engineering is a dilemma because of the highly ionized and dynamic characteristics of quantum dots. To circumvent this issue, herein, we employed a mild solution-phase ligand-exchange approach through adding short-chain amino acids that contain amino and carboxyl groups to modify quantum dots and passivate their surface defects during the purification process. As a result, the photoelectric conversion efficiency of FAPbI3 perovskite quantum dot solar cells (PQDSCs) increased from 11.23 to 12.97% with an open-circuit voltage of 1.09 V, a short-circuit current density of 16.37 mA cm-2, and a filling factor of 72.13%. Furthermore, the stability of the device modified by amino acids retains over 80% of the initial efficiency upon being exposed to 20-30% relative humidity for 240 h of aging treatment. This work may offer an innovative concept and approach for surface ligand treatment to improve the photovoltaic performance of PQDSCs toward large-scale manufacture.
RESUMEN
Tin dioxide (SnO2 ) with high conductivity and low photocatalytic activity has been reported as one of the best candidates for highly efficient electron transport layer (ETL) in perovskite solar cell (PSC). The state-of-the-art SnO2 layer is achieved by chemical bath deposition with tunable properties, while the commercial SnO2 nanocrystals (NCs) with low tunability still face the necessity of further improvement. Here, a kind of highly crystallized Cl-doped SnO2 NCs is reported that can form very stable aqueous dispersion with shelf life up to one year without any stabilizer, which can facilitate the fabrication of PSCs with satisfactory performance. Compared to the commercial SnO2 NCs regardless of the extrinsic Cl-doping conditions, the intrinsic Cl-doped SnO2 NCs effectively suppress the energy barrier and reduces the trap state density at the buried interface between perovskite and ETL. Consequently, stable PSCs based on such Cl-doped SnO2 NCs achieve a champion efficiency up to ≈25% for small cell (0.085 cm2 ) and ≈20% for mini-module (12.125 cm2 ), indicating its potential as a promising candidate for ETL in high-performance perovskite photovoltaics.
RESUMEN
Perovskite solar cells (PSCs) are promising candidates for next-generation photovoltaics owing to their unparalleled power conversion efficiencies (PCEs). Currently, approaches to further improve device efficiencies tend to focus on the passivation of interfacial defects. Although various strategies have been developed to mitigate these defects, many involve complex and time-consuming post-treatment processes, thereby hindering their widespread adoption in commercial applications. In this work, a concise but efficient in situ dual-interface passivation strategy is developed wherein 1-butyl-3-methylimidazolium methanesulfonate (MS) is employed as a precursor additive. During perovskite crystallization, MS can either be enriched downward through precipitation with SnO2 , or can be aggregated upward through lattice extrusion. These self-assembled MS species play a significant role in passivating the defect interfaces, thereby reducing nonradiative recombination losses, and promoting more efficient charge extraction. As a result, a PCE >25% (certified PCE of 24.84%) is achieved with substantially improved long-term storage and photothermal stabilities. This strategy provides valuable insights into interfacial passivation and holds promise for the industrialization of PSCs.
RESUMEN
The critical requirement for ambient-printed formamidinium lead iodide (FAPbI3 ) lies in the control of nucleation-growth kinetics and defect formation behavior, which are extensively influenced by interactions between the solvent and perovskite. Here, a strategy is developed that combines a cosolvent and an additive to efficiently tailor the coordination between the solvent and perovskite. Through in situ characterizations, the direct crystallization from the sol-gel phase to α-FAPbI3 is illustrated. When the solvent exhibits strong interactions with the perovskite, the sol-gel phases cannot effectively transform into α-FAPbI3 , resulting in a lower nucleation rate and confined crystal growth directions. Consequently, it becomes challenging to fabricate high-quality void-free perovskite films. Conversely, weaker solvent-perovskite coordination promotes direct crystallization from sol-gel phases to α-FAPbI3 . This process exhibits more balanced nucleation-growth kinetics and restrains the formation of defects and microstrains in situ. This strategy leads to improved structural and optoelectronic properties within the FAPbI3 films, characterized by more compact grain stacking, smoother surface morphology, released lattice strain, and fewer defects. The ambient-printed FAPbI3 perovskite solar cells fabricated using this strategy exhibit a remarkable power conversion efficiency of 24%, with significantly reduced efficiency deviation and negligible decreases in the stabilized output.
RESUMEN
Pure-phase α-FAPbI3 quantum dots (QDs) are the focus of an increasing interest in photovoltaics due to their superior ambient stability, large absorption coefficient, and long charge-carrier lifetime. However, the trap states induced by the ligand-exchange process limit the photovoltaic performances. Here, a simple post treatment using methylamine thiocyanate is developed to reconstruct the FAPbI3 -QD film surface, in which a MAPbI3 capping layer with a thickness of 6.2 nm is formed on the film top. This planar perovskite heterojunction leads to a reduced density of trap-states, a decreased band gap, and a facilitated charge carrier transport. As a result, a record high power conversion efficiency (PCE) of 16.23% with negligible hysteresis is achieved for the FAPbI3 QD solar cell, and it retains over 90% of the initial PCE after being stored in ambient environment for 1000 h.