quasi-2D Perovskite Research Articles

TuningHole Transport Properties and Perovskite Crystallization via Pyridine-Based Molecules for Quasi-2D Perovskite Solar Cells.

Quasi-2D perovskites show great potential as photovoltaic devices with superior stability, but the power conversion efficiency (PCE) is limited by poor carrier transport. Here, it is simultaneously affected the hole transport layer (HTL) and the perovskite layer by incorporating pyridine-based materials into poly(3,4-ethylenedioxythiophene): polystyrene sulfonate (PEDOT:PSS) to address the key problem above in 2D perovskites. With this approach, the enhanced optoelectronic performance of the novel PEDOT:PSS is due to electron transfer between the additives and PEDOT or PSS, as well as a dissociation between PEDOT and PSS based on experimental and theoretical studies, which facilitates the charge extraction and transfer. Concurrently, in-situ X-ray scattering studies reveal that the introduction of pyridine-based molecules alters the transformation process of the perovskite intermediate phase, which leads to a preferred orientation and ordered distribution caused by the Pb─N chemical bridge, achieving efficient charge transport. As a result, the pyridine-treated devices achieve an increased short-circuit current density (Jsc) and PCE of over 17%.

Aqueous-phase dual-functional chiral perovskites for hydrogen sulfide (H2S) detection and antibacterial applications in Escherichia coli

Perovskite nanocrystals (PNCs) have attracted extensive attention for their potential applications in biology. However, only a handful of PNCs have been scrutinized in the biological domain due to issues such as instability, poor dispersion, and size inhomogeneity in polar solvents. The development of dual-functional perovskite nanomaterials with hydrogen sulfide (H2S) sensing and antibacterial capabilities is particularly intriguing. In this study, we prepared chiral quasi-two-dimensional (quasi-2D) perovskite nanomaterials, Bio(S-PEA)2CsPb2Br7 and Bio(R-PEA)2CsPb2Br7, that were uniformly dispersed in aqueous media. The effective encapsulation of methoxypolyethylene glycol amine (mPEG-NH2) improved water stability and uniformity of particle size. Circular dichroism (CD) signals were created by the successful insertion of chiral cations. These perovskites as probes showed a rapid and sensitive fluorescence quenching response to H2S, and the effect of imaging detection was observed at the Escherichia coli (E. coli) level. As antibacterial agents, their pronounced positive charge properties facilitated membrane lysis and subsequent E. coli death, indicating a significant antibacterial effect. This work has preliminary explored the application of chiral perovskites in biology and provides insight into the development of bifunctional perovskite nanomaterials for biological applications.

Phase Engineering Reinforced Energy Transfer for High-Performance Blue Perovskite Light-Emitting Diodes.

Layered metal-halide perovskites, a category of self-assembled quantum wells, are of paramount importance in emerging photonic sources, such as lasers and light-emitting diodes (LEDs). Despite high trap density in two-dimensional (2D)perovskites, efficient non-radiative energy funneling from wide- to narrow-bandgap components, sustained by the Förster resonance energy transfer (FRET) mechanism, contributes to efficient luminescence by light or electrical injection. Herein, it is demonstrated that bandgap extension of layered perovskites to the blue-emitting regime will cause sluggish and inefficient FRET, stemming from the tiny spectral overlap between different phases. Motivated by the importance of blue LEDs and inefficient energy transfer in materials with phase polydispersity, wide-bandgap quasi-2D perovskites with narrow phase distribution, improved crystallinity, and the pure crystal orientation perpendicular to the charge transport layer are developed. Based on this emitter, high-performance blue perovskite LEDs with improved electroluminescence (EL) external quantum efficiency (EQE) of 7.9% at 478nm, a narrow full width at half-maximum (FWHM) of 22nm and a more stable EL spectra are achieved. These results provide an important insight into spectrally stable and efficient blue emitters and EL devices based on perovskites.

Development of Quasi-Two-Dimensional Perovskites and Their Application in Light-Emitting Diodes.

Quasi-two-dimensional (quasi-2D) perovskites have attracted much attention due to their outstanding properties, such as inherent quantum-well structure, strong dielectric and quantum confinement, large exciton binding energy, and high photoluminescence quantum yield. By virtue of these superior merits, quasi-2D perovskites have shown great potential for next-generation light-emitting diodes (LEDs). Herein, this review presents an overview of the basic properties of quasi-2D perovskites and their photoluminescence modulations by large organic cation engineering, monovalent cation engineering, halogen engineering, defect passivation engineering, and dimensionality engineering. Furthermore, the strategies of charge-transport layer optimization, interfacial engineering, light-outcoupling efficiency improvement, and operating stability improvement are summarized for fabricating high-performance quasi-2D perovskite LEDs (PeLEDs). Finally, the challenges and outlook for the future development of quasi-2D PeLEDs are unambiguously proposed.

Investigation of the Role of K2SO4 Electrolyte in Hole Transport Layer for Efficient Quasi-2D Perovskite Light-Emitting Diodes.

Quasi-two-dimensional (2D) perovskite light-emitting diodes are promising light sources for color display and lighting. However, poor carrier injection and transport between the bottom hole transport layer (HTL) and perovskite limit the device performance. Here we demonstrate a simple and effective way to modify the HTL for enhancing the performance of perovskite light-emitting diodes (PeLEDs). An electrolyte K2SO4 is used to mix with poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS) as the hole transport layer. The K+ doping helped the quasi-2D perovskite phases grow vertically along the interface of the PEDOT:PSS, fine-modulate the phase distribution, and simultaneously reduce the defect density of quasi-2D perovskites. It also significantly reduced the exciton quenching and injection barrier at PEDOT:PSS and quasi-2D perovskite interface. The optimized green PeLEDs with the K2SO4 doped PEDOT:PSS HTL showed a maximum luminance of 17185 cd/m2 which is almost 4.7 times brighter than the control one, with a maximum external quantum efficiency of 18.64%.

High-Performance Blue Perovskite Light-Emitting Diodes Enabled by Synergistic Effect of Additives.

While quasi-two-dimensional (quasi-2D) perovskites have good properties of cascade energy transfer, high exciton binding energy, and high quantum efficiency, which will benefit high-efficiency blue PeLEDs, inefficient domain distribution management and unbalanced carrier transport impede device performance improvement. Herein, (2-(9H-carbazol-9-yl)ethyl)phosphonic acid (2PACz) and methyl 2-aminopyridine-4-carboxylate (MAC) were simultaneously introduced to a blue quasi-2D perovskite film. Relying on the synergistic effect of 2PACz and MAC, it not only modulates the phase distribution inhibiting the n = 2 phase but also greatly improves the electrical property of the quasi-2D perovskite film. As a result, the as-modified blue quasi-2D PeLED demonstrated an external quantum efficiency (EQE) of 17.08% and a luminance of 10142 cd m-2. This study exemplifies the synergistic effect among dual additives and offers a new effective additive strategy modulating phase distribution and building balanced carrier transport, which paves the way for the fabrication of highly efficient blue PeLEDs.

Regulating the continuous and concentrated distribution of Quasi-2D perovskite phases to achieve Sky-Blue Light-Emitting diodes with efficiency approaching 17%

Blue perovskite light-emitting diodes (PeLEDs) are increasingly crucial for manufacturing high-definition full-color displays due to their outstanding electroluminescent properties. Quasi-two-dimensional (quasi-2D) perovskite stands out as the most promising material for blue light-emitting layer, given its robust quantum/dielectric confinement. In this study, we present the preparation of PeLEDs with a tunable blue emission wavelength using pure bromide perovskite components by adjusting the content of halogenated organic ammonium bromide [2-bromoethylamine hydrobromide (BEABr)]. The bifunctional ligand BEABr not only achieves an excellent phase distribution of quasi-2D perovskite but also reduces the weak van der Waals gap between individual perovskite layers, facilitating effective energy transfer in perovskite films. Additionally, the bifunctional groups passivate perovskite defects and inhibit phase separation, leading to efficient and stable sky-blue luminescence. The BEABr-doped sky-blue PeLED demonstrated superior device performance, achieving a maximum external quantum efficiency of 16.98 % at 493 nm. This work serves as inspiration for further exploration of efficient and stable commercial blue PeLED devices.

Regulating Perovskite Crystallization through Interfacial Engineering Using a Zwitterionic Additive Potassium Sulfamate for Efficient Pure-Blue Light-Emitting Diodes.

Quasi-two-dimensional (quasi-2D) perovskites are emerging as efficient emitters in blue perovskite light-emitting diodes (PeLEDs), while the imbalanced crystallization of the halide-mixed system limits further improvements in device performance. The rapid crystallization caused by Cl doping produces massive defects at the interface, leading to aggravated non-radiative recombination. Meanwhile, unmanageable perovskite crystallization is prone to facilitate the formation of nonuniform low-dimensional phases, which results in energy loss during the exciton transfer process. Here, we propose a multifunctional interface engineering for nucleation and phase regulation by incorporating the zwitterionic additive potassium sulfamate into the hole transport layer. By using potassium ions (K+ ) as heterogeneous nucleation seeds, finely controlled growth of interfacial K+ -guided grains is achieved. The sulfamate ions can simultaneously regulate the phase distribution and passivate defects through coordination interactions with undercoordinated lead atoms. Consequently, such synergistic effect constructs quasi-2D blue perovskite films with smooth energy landscape and reduced trap states, leading to pure-blue PeLEDs with a maximum external quantum efficiency (EQE) of 17.32 %, spectrally stable emission at 478 nm and the prolonged operational lifetime. This work provides a unique guide to comprehensively regulate the halide-mixed blue perovskite crystallization by manipulating the characteristics of grain-growth substrate.

Dual ligands synergy enables thermal and moisture stability-enhanced blue quasi-2D perovskite for efficient light-emitting diodes

Quasi-2D metal halide perovskite is rising for efficient blue light-emitting diodes due to strong quantum confinement and tunable emission, while a challenge remains in its poor stability of n-phase distribution under external stresses. Herein, the stable blue quasi-2D perovskite under heat and moisture conditions is achieved by dual ligand engineering. The Lewis base moieties − SO3− from taurine (3S) bind tightly with perovskite edges, inhibiting Ostwald ripening of the perovskite phase caused by the heat, and 3, 3-diphenylpropylamine (DPPA) provides a strong hydrophobicity to the perovskite film, suppressing phase disproportionation induced by the moisture. Accordingly, the blue perovskite film, modified synergistically by the 3S and DPPA dual ligands, maintains its initial photoluminescence quantum yield (PLQY) after over 200 h with 70 °C heating, and only exhibiting a redshift in PL peak wavelength less than 10 nm. Exposing under environment condition of 20 % relative humidity for 300 h, the blue perovskite film still retains its initial PL peak wavelength with PLQY exceeding 50 % of the initial value. This achievement establishes a notable strategy for enhancing both the thermal and moisture stability of blue quasi-2D perovskite. Furthermore, the light-emitting diodes based on the perovskite films display the enhanced operating stability. This work offers an efficient strategy for stabilizing blue quasi-2D perovskite and the corresponding devices for the display application.

Ionic liquid tailoring defect/interface-induced recombination loss toward efficient Dion-Jacobson quasi-2D perovskite solar cells

Dion-Jacobson (DJ) quasi-two-dimensional (quasi-2D) perovskites have emerged as a potential photovoltaic material due to their versatile n-layer variation and superior stable structure. However, compared to their three-dimensional counterparts, the power conversion efficiency (PCE) of quasi-2D perovskite solar cells (PSCs) reported to date still lags behind the detailed balance (DB) limit for single-junction PSCs, which derives from the presence of non-radiative recombination loss. Herein, we demonstrated that the defect/interface-induced recombination loss in DJ quasi-2D PSCs could be significantly suppressed by introducing a green ionic liquid methylammonium acetate (MAAc) into (BDA)(MA)4Pb5I16 (n = 5) (BDA, 1,4-butanediamine) perovskite precursor. Both the film quality of 2D perovskites and the interfacial property of perovskite/charge transporting layer (CTL) were improved after introducing MAAc in precursor solution. Correspondingly, a champion PCE of 18.76 % with a remarkable open-circuit voltage (Voc) of 1.24 V was achieved. Through the quantitative loss analysis, which involved the calculation of photovoltaic parameters relative to DB limit and quasi-Fermi level splitting values, the improvement of PCE and Voc by introducing MAAc was mainly attributed to the reduction of defects in perovskite films and at perovskite/CTL interfaces, and the optimization of interfacial energy-level alignment. The present work provides a green solvent strategy for improving the performance of quasi-2D PSCs, and offers an insight into the fundamental physics of non-radiative recombination loss tailored by ionic liquid.

Engineering of Molecular Bridge on Buried Interface via Ferrocene Carboxylic Acid for High Performance Perovskite Light‐Emitting Devices

AbstractQuasi‐two‐dimensional (Quasi2D) perovskite materials gained widespread attention due to whose unique and highly desirable luminescence properties. However, the behavior of perovskite lightemitting diodes (PeLEDs) is prejudiced by inefficient cascading energy transfer of perovskite film and unbalanced charges injection. Here, ferrocene carboxylic acid (FcAd) is employed between hole transport layer (HTL) and perovskite layer as a molecular bridge to solve the current problems of PeLEDs. Ferrocene units can bond with [PbBr6]4−, forming one‐dimensional (1D) intermediate phases of FcPbBr3 at the interface, which can manipulate the growth kinetics of perovskite and reconstruct the phase distribution. Therefore, due to the suppression of low dimensional phase content, not only is the cascaded energy transfer of PEA2(CsPbBr3)2PbBr4 films effectively achieved, but also the quasi‐2D perovskite's work function is reduced. Additionally, Pb2+ coordinated with the carboxyl group of FcAd, inducing an electric dipole effect that leads to an further upward shift of the perovskite energy level. Eventually, the synergy achieves a significant tailoring between the perovskite and HTL energy exhibits the most excellent external quantum efficiency (EQE) exceeds 27% and optimal brightness exceeds 240000 cd m−2. Therefore, the preparation method will provide an effective strategy to widen the color gamut of next‐generation displays.

Effective Small Organic Molecule as a Defect Passivator for Highly Efficient Quasi-2D Perovskite Light-Emitting Diodes.

The use of a small organic molecular passivator is proven to be a successful strategy for producing higher-performing quasi-2D perovskite light-emitting diodes (PeLEDs). The small organic molecule can passivate defects on the grain surround and surface of perovskite crystal structures, preventing nonradiative recombination and charge trapping. In this study, a new small organic additive called 2, 8-dibromodibenzofuran (diBDF) is reported and examines its effectiveness as a passivating agent in high-performance green quasi-2D PeLEDs. The oxygen atom in diBDF, acting as a Lewis base, forms coordination bonds with uncoordinated Pb2+, so enhancing the performance of the device. In addition, the inclusion of diBDF in the quasi-2D perovskite results in a decrease in the abundance of low-n phases, hence facilitating efficient carrier mobility. Consequently, PeLED devices with high efficiency are successfully produced, exhibiting an external quantum efficiency of 19.9% at the emission wavelength of 517 nm and a peak current efficiency of 65.0 cd A-1.

Boosting the performance of Quasi-2D perovskite Light-Emitting diodes by tailoring molecular configurations of Carboxyl-Based additives

Quasi two-dimensional (quasi-2D) perovskites have shown huge potential for perovskite light-emitting diodes (PeLEDs). Nevertheless, the serious non-radiative recombination induced by numerous defects in polycrystalline quasi-2D perovskite films hinders their further development. Herein, three carboxyl-based additives with different molecular configurations, i.e. butyric acid (BAC), glutaric acid (GAC) and tricarballylic acid (TAC), are adopted as passivation agents for quasi-2D PeLEDs. Benefiting from the strong coordination interaction between –COOH and perovskites, the inclusion of carboxyl-based additives can effectively optimize film morphologies, regulate the distribution of small-n phases, passivate defects and enhance film stability. With the increase of the carboxyl group number and molecular spatial dimension of carboxyl-based additives, more compact and smoother quasi-2D perovskite films, together with narrower phase distribution, lower defect density and better stability, can be obtained. Consequently, the unpacked quasi-2D PeLED treated with TAC, which is tested in the ambient air with the relative humidity of about 50 %, delivers an external quantum efficiency (EQE) of 14.21 % and prolonged operational lifetime (T50) of 2160 s, while the pristine device only gives an EQE of 7.63 % and T50 of 460 s. Our work provides guidance for boosting the performance of quasi-2D PeLEDs by rationally tailoring molecular configurations of carboxyl-based additives.

Phase distribution regulation of formamidinium-based quasi-2D perovskites through solution engineering.

Quasi-2D perovskites have attracted attention as potential solar energy absorber materials due to their balanced efficiency and stability and their unique quantum-well structures. In order to facilitate directional excitons and charge carrier transport and preferential energy transfer landscape in photovoltaic thin films, the phase distribution formed by different types of microstructural domains should be regulated. In this work, the Dion-Jacobson-type spacer 1,4-phenylenedimethanammonium (PDMA) was used, and different strategies were pursued to control the phase distribution in formamidinium-based (FA) quasi-2D perovskites based on the composition of (PDMA)FA4Pb5I16. In general, doping with FACl modulated the crystallization kinetics, forming 2D low-n crystals on the top surface or a reversed-gradient phase distribution, depending on whether excess or substitutional doping was employed. Alternatively, mixing with a Ruddlesden-Popper spacer helped bridging to adjacent octahedra in pure PDMA-based perovskites and improved crystallization, while regulating the quantum-well structures to give a normal-gradient phase distribution, where 2D domains resided on the bottom side. By combining FACl doping and spacer mixing, the film showed both a reversed-gradient phase distribution and larger vertically aligned grains. This work contributes to the knowledge of how to manipulate and regulate the phase distribution in FA-based quasi-2D perovskites and further paves the way for fabricating corresponding devices with high efficiency and stability.

Hole transport layer engineering in high performance quasi-2D perovskite blue light emitting diodes.

Quasi-2D perovskites have emerged as highly promising materials for application in perovskite light-emitting diodes (PeLEDs), garnering significant attention due to their outstanding semiconductor properties. These materials boast an inherent multi-quantum well structure that imparts a robust confinement effect, particularly advantageous for blue emission. However, the development of blue emitters utilizing quasi-2D perovskites encounters challenges, notably colour instability, multipeak emission, and suboptimal fluorescence yield. The hole transfer layer (HTL) on which the perovskite layer is deposited in PeLEDs further affects the performance and efficiency. In this review, we delve into the evolution of blue PeLEDs and elucidate the optical properties of quasi-2D perovskites with the primary focus on HTL materials. We explore different HTL materials like PEDOT:PSS, metal oxides, and conjugated polyelectrolytes as well as ionic liquids, and their role in enhancing the colour stability, minimizing interfacial defects and increasing the fluorescence yield. This review endeavours to provide a holistic perspective of the different HTLs and serve as a valuable reference for researchers navigating the realm of HTL engineering towards the realization of high-performance blue quasi-2D PeLEDs.

Antisolvent effects in green solvent engineering of FA-based quasi-2D Ruddlesden–Popper perovskite films for efficient solar cells

We investigate the proper green solvents for fabricating the high performance formamidinium (FA)-based quasi-2D perovskites solar cells. We find the petroleum ether is a more suitable antisolvent for quasi-2D perovskite crystallization than the traditional used antisolvent dibutyl ether.

A modulated heterojunction interface via ferroelectric P(VDF-TrFE) towards high performance quasi-2D perovskite self-powered photodetectors

By incorporating P(VDF-TrFE) into quasi-2D perovskites, favorable energy band alignment is achieved at the junction. This leads to reduced dark current and facilitated charge transport, thereby achieving high performance self-powered photodetector.

Dual-ligand quasi-2D perovskites with chiral-induced spin selectivity for room temperature spin-LEDs.

Spin-LEDs have been a central topic in semiconductor spintronics research and represent a promising avenue for advanced optoelectronic devices and applications. The future advancements of spin-LEDs will undoubtedly hinge on the generation and manipulation of spin-polarized population at room temperature. In this research, we elucidate the development of room-temperature spin-LEDs using quasi-2D perovskites, based on the chiral-induced spin selectivity (CISS) effect. During the carrier transfer from the chiral n2 phase to the randomly oriented high-n phase caused by the bandgap gradient distribution, CISS works to generate non-equilibrium spin population, leading to room-temperature spin-polarized fluorescence. A spin-polarization of ∼93% is observed for the films. Finally, we realize spin-LEDs at room temperature, exhibiting a |gCP-EL| value of 0.05 and an EQE of 3.8%. This work highlights the potential of integrating dual ligands to optimize the phase distribution and crystalline orientation in quasi-2D films to achieve efficient CISS for spin-LED applications.

Modification of mixed-halide quasi-2D perovskites by aminophylline towards efficient and spectrally stable blue light-emitting diodes with low efficiency roll-off

Blue perovskite light-emitting diodes (PeLEDs) based on the quasi two-dimensional (quasi-2D) perovskites with chloride (Cl) and bromine (Br) ions have made significant progress in improving external quantum efficiencies (EQEs) during...

Organic ammonium salt assisted crystallization and defect passivation of a quasi-two-dimensional pure blue perovskite at the buried interface.

Quasi-two-dimensional (quasi-2D) perovskites exhibit excellent performance in light-emitting diodes (LEDs). However, the quality of perovskite films prepared via the solution method is significantly impacted by the enormous number of defects that unavoidably form at the grain boundaries and interfaces during the precursor to the crystal formation process. Here, we propose a strategy to assist perovskite crystallization and defect passivation at the buried interface through interfacial modification. The organic ammonium salt, ethylamine chloride (EACl), is added to the hole transport material and modifies the buried interface of the perovskite film. EACl introduces the nucleation sites for perovskite precursors, and promotes the crystallization process of the perovskite grains, contributing to the formation of high-quality perovskite films. At the same time, the presence of Lewis base (-NH2) groups in EACl and their lone electron pairs effectively inactivate unlocated Pb2+ ions at the buried interface, thereby reducing non-radiative recombination. In addition, chloride ions help to mitigate defects and to improve the morphology of perovskite films. Devices with this modification show a higher performance than control devices on all metrics. This work proposes a facile but efficient way for improving quasi-2D pure blue perovskite crystallization and growth.