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Journal ArticleDOI: 10.1021/ACS.JPCLETT.1C00008

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
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.

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Topics: Perovskite (structure) (52%)
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10 results found


Journal ArticleDOI: 10.1021/ACS.JPCLETT.1C00515
Zhuo Chen1, Binze Zhou1, Jun-Hui Yuan1, Ni Tang1  +6 moreInstitutions (1)
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.

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3 Citations



Journal ArticleDOI: 10.1021/ACS.JPCLETT.1C00693
Yongqiang Ji1, Minqiang Wang1, Zhi Yang1, Hengwei Qiu1  +7 moreInstitutions (4)
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.

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1 Citations


Open accessPosted Content
Abstract: Halide perovskites are a promising class of materials for optoelectronic applications, due to their excellent optoelectronic performance. However, they suffer several dynamical degradation problems, the characterization of which is challenging in experiments. Atomic scale simulations can provide valuable insights, however, the high computational cost of traditional quantum mechanical methods such as DFT makes it difficult to model dynamical processes in large perovskite systems. In this work, we present a re-parameterized GFN1-xTB method for the accurate description of structural and dynamical properties of CsPbBr\textsubscript{3}, CsPbI\textsubscript{3}, and CsPb(I\textsubscript{1-x}Br\textsubscript{x})\textsubscript{3}. Our molecular dynamics simulations show that the phase stability is strongly correlated to the displacement of ions in the perovskites. In the low temperature orthorhombic phase, the directional movement of the Cs cations decreases contact with the surrounding halides, initiating a transition to the non-perovskite phase. However, this loss of contact can be compensated by increased halide displacement, once enough thermal energy is available, resulting in a transition to the tetragonal or cubic phases. Furthermore, we find the mixing of halides increase halide displacement over a significant range of temperatures, resulting in lower phase transition temperatures and therefore improved phase stability.

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Topics: Phase transition (54%), Phase (matter) (52%), Perovskite (structure) (52%) ... show more

Journal ArticleDOI: 10.1016/J.NANOEN.2021.106583
Yuliang Ye1, Wang Jiaxiang1, Yinglin Qiu1, Jiahui Liu1  +16 moreInstitutions (2)
01 Dec 2021-Nano Energy
Abstract: Recently, perovskite quantum dots (PQDs) were employed as promising emitters in light-emitting diode devices (LEDs) mainly owing to their marvelous photoelectronics properties. However, these perovskite QLEDs suffered from the inefficient performance, especially their serious efficiency roll-off probably due to the exciton recombination dynamic in the interface of PQDs films and charge imbalance resulting from low electrical transportation. Herein, sodium dodecyl sulfate (SDS) was effectively introduced to synthesize PQDs with many excellent properties and eventually suppressed the efficiency roll-off of QLEDs. SDS-based PQDs films exhibited obviously enhanced radiative recombination, reduced trap density, and increased carrier mobility, especially the transportation of electrons. Therefore, the charge carrier was balanced at high current density together with the remarkably suppressed efficiency roll-off. QLEDs fabricated by SDS-capped PQDs exhibited significantly improved maximum brightness of 193,810 cd/m2, and achieve the external quantum efficiency of 10.13%. More importantly, the EQE roll-off of QLED optimized in the thickness of emitting layer was only 1.5% at the current density of 200 mA/cm2, representing a prominent achievement of our strategy.

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Topics: Quantum efficiency (53%), Quantum dot (50%)

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40 results found


Open accessJournal ArticleDOI: 10.1021/NL5048779
02 Feb 2015-Nano Letters
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...

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Topics: Quantum dot (53%), Photoluminescence (51%), Halide (51%) ... show more

4,445 Citations


Open accessJournal ArticleDOI: 10.1126/SCIENCE.AAG2700
07 Oct 2016-Science
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.

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Topics: Quantum dot (54%), Perovskite (structure) (53%), Photovoltaics (50%)

1,615 Citations


Journal ArticleDOI: 10.1002/ADMA.201603885
Jianhai Li1, Leimeng Xu1, Tao Wang1, Jizhong Song1  +7 moreInstitutions (1)
01 Feb 2017-Advanced Materials
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.

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Topics: Quantum efficiency (52%), Passivation (50%)

794 Citations


Open accessJournal ArticleDOI: 10.1038/NATURE10569
10 Nov 2011-Nature
Abstract: Photoluminescence blinking—random switching between states of high (ON) and low (OFF) emissivities—is a universal property of molecular emitters found in dyes1, polymers2, biological molecules3 and artificial nanostructures such as nanocrystal quantum dots, carbon nanotubes and nanowires4, 5, 6. For the past 15 years, colloidal nanocrystals have been used as a model system to study this phenomenon5, 6. The occurrence of OFF periods in nanocrystal emission has been commonly attributed to the presence of an additional charge7, which leads to photoluminescence quenching by non-radiative recombination (the Auger mechanism)8. However, this ‘charging’ model was recently challenged in several reports9, 10. Here we report time-resolved photoluminescence studies of individual nanocrystal quantum dots performed while electrochemically controlling the degree of their charging, with the goal of clarifying the role of charging in blinking. We find that two distinct types of blinking are possible: conventional (A-type) blinking due to charging and discharging of the nanocrystal core, in which lower photoluminescence intensities correlate with shorter photoluminescence lifetimes; and a second sort (B-type), in which large changes in the emission intensity are not accompanied by significant changes in emission dynamics. We attribute B-type blinking to charge fluctuations in the electron-accepting surface sites. When unoccupied, these sites intercept ‘hot’ electrons before they relax into emitting core states. Both blinking mechanisms can be electrochemically controlled and completely suppressed by application of an appropriate potential.

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Topics: Fluorescence intermittency (61%), Quantum dot (55%), Nanocrystal (55%) ... show more

549 Citations


Journal ArticleDOI: 10.1021/ACSNANO.7B05442
Feng Liu1, Yaohong Zhang1, Chao Ding1, Syuusuke Kobayashi1  +9 moreInstitutions (5)
19 Sep 2017-ACS Nano
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...

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Topics: Quantum dot (56%), Perovskite (structure) (55%), Photoluminescence (52%) ... show more

485 Citations