Highly Luminescent and Stable CsPbI3 Perovskite Nanocrystals with Sodium Dodecyl Sulfate Ligand Passivation for Red-Light-Emitting Diodes.
04 Mar 2021-Journal of Physical Chemistry Letters (American Chemical Society (ACS))-Vol. 12, Iss: 9, pp 2437-2443
TL;DR: In this paper, a stable and highly luminescent black-phase CsPbI3 perovskite nanocrystals (NCs) passivated by novel ligands of sodium dodecyl sulfate (SDS) was reported.
Abstract: CsPbI3 perovskite nanocrystals (NCs) have recently emerged as promising materials for optoelectronic devices because of their superior properties. However, the poor stability of the CsPbI3 NCs induced by easy ligand desorption represents a key issue limiting their practical applications. Herein, we report stable and highly luminescent black-phase CsPbI3 NCs passivated by novel ligands of sodium dodecyl sulfate (SDS). Theoretical calculation results reveal a stronger adsorption energy of SDS molecules at the CsPbI3 surface than that of commonly used oleic acid. As a result, the defect formation caused by the ligand loss during the purification process is greatly suppressed. The optimized SDS-CsPbI3 NCs exhibit significantly reduced surface defects, much enhanced stability, and superior photoluminescence efficiency. The red perovskite light-emitting diodes based on the SDS-CsPbI3 NCs demonstrate an external quantum efficiency of 8.4%, which shows a 4-fold improvement compared to the devices based on the oleic acid-modified CsPbI3 NCs.
Citations
More filters
45 citations
TL;DR: In this paper, the enhanced stability of CsPbI3 nanocrystals is achieved by incorporating the Cu2+ ion into the lattice under mild conditions, which can maintain red luminescence for 35 days in air while the undoped ones transformed into the nonluminescent yellow phase in several days.
Abstract: Black phase CsPbI3 perovskites have emerged as one of the most promising materials for use in optoelectronic devices due to their remarkable properties. However, black phase CsPbI3 usually possesses poor stability and involves a phase change process, resulting in an undesired orthorhombic (δ) yellow phase. Here, the enhanced stability of CsPbI3 nanocrystals is achieved by incorporating the Cu2+ ion into the CsPbI3 lattice under mild conditions. In particular, the Cu2+-doped CsPbI3 film can maintain red luminescence for 35 days in air while the undoped ones transformed into the nonluminescent yellow phase in several days. Furthermore, first-principles calculations verified that the enhanced stability is ascribed to the increased formation energy due to the successful doping of Cu2+ in CsPbI3. Benefiting from such an effective doping strategy, the as-prepared Cu2+-doped CsPbI3 as an emitting layer shows much better performance compared with that of the undoped counterpart. The turn-on voltage of the Cu2+-doped quantum-dot light-emitting diode (QLED) (1.6 V) is significantly reduced compared with that of the pristine QLED (3.8 V). In addition, the luminance of the Cu2+-doped QLED can reach 1270 cd/m2, which is more than twice that of the pristine CsPbI3 QLED (542 cd/m2). The device performance is believed to be further improved by optimizing the purification process and device structure, shedding light on future applications.
24 citations
TL;DR: In this article , perovskite composite films for high performance PeLEDs by using zwitterion 3-aminopropanesulfonic acid (APS) as the additive are developed.
Abstract: Chemical passivation via functional additives plays a critical role in achieving high performance perovskite light‐emitting diodes (PeLEDs). Here, perovskite composite films for high performance PeLEDs by using zwitterion 3‐aminopropanesulfonic acid (APS) as the additive are developed. The sulfonic group of APS can simultaneously passivate deep and shallow level defects in perovskites via coordinate and hydrogen bonding, which leads to suppressed non‐radiative recombination and ion migration in the perovskite composite films. Based on this, PeLEDs with a peak external quantum efficiency of 19.2% and a half‐lifetime of 43 h at a constant current density of 100 mA cm−2 are obtained, representing one of the most stable and efficient PeLEDs under high current densities.
21 citations
TL;DR: In this article , the authors discuss the rationale of various strategies to enhance the stability of perovskite NCs and suggest possible future directions for the fabrication of optoelectronic devices with long-term stability while maintaining high efficiency.
Abstract: Over the past few years, metal halide perovskite nanocrystals have been at the forefront of colloidal semiconductor nanomaterial research because of their fascinating properties and potential applications. However, their intrinsic phase instability and chemical degradation under external exposures (high temperature, water, oxygen, and light) are currently limiting the real-world applications of perovskite optoelectronics. To overcome these stability issues, researchers have reported various strategies such as doping and encapsulation. The doping improves the optical and photoactive phase stability, whereas the encapsulation protects the perovskite NCs from external exposures. This perspective discusses the rationale of various strategies to enhance the stability of perovskite NCs and suggests possible future directions for the fabrication of optoelectronic devices with long-term stability while maintaining high efficiency.
21 citations
TL;DR: In this paper, a trioctylphosphine (TOP)-assisted pre-protection low-temperature solvothermal synthesis of highly stable CsPbBr3/TiO2 nanocomposites was proposed.
Abstract: Lead halide perovskite quantum dots (PQDs) are reported as a promising branch of perovskites, which have recently emerged as a field in luminescent materials research. However, before the practical applications of PQDs can be realized, the problem of poor stability has not yet been solved. Herein, we propose a trioctylphosphine (TOP)-assisted pre-protection low-temperature solvothermal synthesis of highly stable CsPbBr3/TiO2 nanocomposites. Due to the protection of branched ligands and the lower temperature of shell formation, these TOP-modified CsPbBr3 PQDs are successfully incorporated into a TiO2 monolith without a loss of fluorescence intensity. Because the excellent nature of both parent materials is preserved in CsPbBr3/TiO2 nanocomposites, it is found that the as-prepared CsPbBr3/TiO2 nanocomposites not only display excellent photocatalytic activity but also yield improved PL stability, enabling us to build highly stable white light-emitting diodes and to photodegrade rhodamine B.
19 citations
References
More filters
TL;DR: The compelling combination of enhanced optical properties and chemical robustness makes CsPbX3 nanocrystals appealing for optoelectronic applications, particularly for blue and green spectral regions (410–530 nm), where typical metal chalcogenide-based quantum dots suffer from photodegradation.
Abstract: Metal halides perovskites, such as hybrid organic–inorganic CH3NH3PbI3, are newcomer optoelectronic materials that have attracted enormous attention as solution-deposited absorbing layers in solar cells with power conversion efficiencies reaching 20%. Herein we demonstrate a new avenue for halide perovskites by designing highly luminescent perovskite-based colloidal quantum dot materials. We have synthesized monodisperse colloidal nanocubes (4–15 nm edge lengths) of fully inorganic cesium lead halide perovskites (CsPbX3, X = Cl, Br, and I or mixed halide systems Cl/Br and Br/I) using inexpensive commercial precursors. Through compositional modulations and quantum size-effects, the bandgap energies and emission spectra are readily tunable over the entire visible spectral region of 410–700 nm. The photoluminescence of CsPbX3 nanocrystals is characterized by narrow emission line-widths of 12–42 nm, wide color gamut covering up to 140% of the NTSC color standard, high quantum yields of up to 90%, and radiativ...
6,170 citations
TL;DR: N nanoscale phase stabilization of CsPbI3 quantum dots (QDs) to low temperatures that can be used as the active component of efficient optoelectronic devices and describe the formation of α-CsP bI3 QD films that are phase-stable for months in ambient air.
Abstract: We show nanoscale phase stabilization of CsPbI 3 quantum dots (QDs) to low temperatures that can be used as the active component of efficient optoelectronic devices. CsPbI 3 is an all-inorganic analog to the hybrid organic cation halide perovskites, but the cubic phase of bulk CsPbI 3 (α-CsPbI 3 )—the variant with desirable band gap—is only stable at high temperatures. We describe the formation of α-CsPbI 3 QD films that are phase-stable for months in ambient air. The films exhibit long-range electronic transport and were used to fabricate colloidal perovskite QD photovoltaic cells with an open-circuit voltage of 1.23 volts and efficiency of 10.77%. These devices also function as light-emitting diodes with low turn-on voltage and tunable emission.
2,103 citations
TL;DR: Solution-processed CsPbBr3 quantum-dot light-emitting diodes with a 50-fold external quantum efficiency improvement are achieved through balancing surface passivation and carrier injection via ligand density control, which induces the coexistence of high levels of ink stability, photoluminescence quantum yields, thin-film uniformity, and carrier-injection efficiency.
Abstract: Solution-processed CsPbBr3 quantum-dot light-emitting diodes with a 50-fold external quantum efficiency improvement (up to 6.27%) are achieved through balancing surface passivation and carrier injection via ligand density control (treating with hexane/ethyl acetate mixed solvent), which induces the coexistence of high levels of ink stability, photoluminescence quantum yields, thin-film uniformity, and carrier-injection efficiency.
977 citations
TL;DR: It is shown that a high room-temperature photoluminescence quantum yield of up to 100% can be obtained in CsPbI3 perovskite QDs, signifying the achievement of almost complete elimination of the trapping defects.
Abstract: Perovskite quantum dots (QDs) as a new type of colloidal nanocrystals have gained significant attention for both fundamental research and commercial applications owing to their appealing optoelectronic properties and excellent chemical processability. For their wide range of potential applications, synthesizing colloidal QDs with high crystal quality is of crucial importance. However, like most common QD systems such as CdSe and PbS, those reported perovskite QDs still suffer from a certain density of trapping defects, giving rise to detrimental nonradiative recombination centers and thus quenching luminescence. In this paper, we show that a high room-temperature photoluminescence quantum yield of up to 100% can be obtained in CsPbI3 perovskite QDs, signifying the achievement of almost complete elimination of the trapping defects. This is realized with our improved synthetic protocol that involves introducing organolead compound trioctylphosphine–PbI2 (TOP–PbI2) as the reactive precursor, which also leads...
684 citations
TL;DR: This work demonstrates an effective strategy through Mn2+ substitution to fundamentally stabilize perovskite lattices of CsPbX3 QDs even at high temperatures up to 200 °C under ambient air conditions and derives significantly improved thermal stability and optical performance from the enhanced formation energy due to the successful doping of Mn2-doped QDs.
Abstract: All-inorganic cesium lead halide perovskite (CsPbX3, X = Cl, Br, and I) quantum dots (QDs), possessing high photoluminescence quantum yields and tunable color output, have recently been endowed great promise for high-performance solar cells and light-emitting diodes (LEDs). Although moisture stability has been greatly improved through separating QDs with a SiO2 shell, the practical applications of CsPbX3 QDs are severely restricted by their poor thermal stability, which is associated with the intrinsically low formation energies of perovskite lattices. In this regard, enhancing the formation energies of perovskite lattices of CsPbX3 QDs holds great promise in getting to the root of their poor thermal stability, which hitherto remains untouched. Herein, we demonstrate an effective strategy through Mn2+ substitution to fundamentally stabilize perovskite lattices of CsPbX3 QDs even at high temperatures up to 200 °C under ambient air conditions. We employ first-principle calculations to confirm that the signi...
631 citations