An All‐Inorganic Perovskite‐Phase Rubidium Lead Bromide Nanolaser

Tang, Bing; Hu, Yingjie; Dong, Hongxing; Sun, Liaoxin; Zhao, Binbin; Jiang, Xiongwei; Zhang, Long

doi:10.1002/anie.201910617

Cited by 15 publications

(11 citation statements)

References 47 publications

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“…Lead–halide perovskite (LHP) semiconductors (MPbX 3 (M = organic cations or Cs; X = Cl, Br, and I)) are attracting attention due to their beneficial optoelectronic properties, including strong light absorption, high photoluminescence quantum yields (PLQYs), and versatile chemical processability, demonstrating great promise toward practical applications such as solar cells, LEDs, lasers and photocatalysts. − Meanwhile, due to the presence of lead and heavy halides, these systems have large spin–orbit coupling (SOC) which in the presence of structural distortions can lift the spin-degeneracy near the conduction and valence band edges, adding the potential of optospintronic applications for LHPs. − Opto-spintronic applications connect the spin degrees of freedom to light and charge and could lower power consumption and achieve faster switching times compared with conventional electronic systems. ,, The spin-relaxation time (the time it takes to randomize the optically oriented spin-polarization of photogenerated charge carriers, similar to longitudinal spin-flip time near zero magnetic field) plays an important role in determining the spintronic properties of the corresponding devices . Recent experiments have explored such spin-related control.…”

Section: Introductionmentioning

confidence: 99%

Tuning Spin-Polarized Lifetime in Two-Dimensional Metal–Halide Perovskite through Exciton Binding Energy

Chen

Wang

et al. 2021

J. Am. Chem. Soc.

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Metal−halide perovskite semiconductors have attracted attention for opto-spintronic applications where the manipulation of charge and spin degrees of freedom have the potential to lower power consumption and achieve faster switching times for electronic devices. Lower-dimensional perovskites are of particular interest since the lower degree of symmetry of the metal−halide connected octahedra and the large spin−orbit coupling can potentially lift the spin degeneracy. To achieve their full application potential, long spin-polarized lifetimes and an understanding of spin-relaxation in these systems are needed. Here, we report an intriguing spin-selective excitation of excitons in a series of 2D lead iodide perovskite (n = 1) single crystals by using timeand polarization-resolved transient reflection spectroscopy. Exciton spin relaxation times as long as ∼26 ps at low excitation densities and at room temperature were achieved for a system with small binding energy, 2D EOA 2 PbI 4 (EOA = ethanolamine). By tuning the excitation density and the exciton binding energy, we identify the dominant mechanism as the D'yakonov−Perel (DP) mechanism at low exciton densities and the Bir−Aronov−Pikus (BAP) mechanism at high excitation densities. Together, these results provide new design principles to achieve long spin lifetimes in metal−halide perovskite semiconductors.

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Section: Introductionmentioning

confidence: 99%

Tuning Spin-Polarized Lifetime in Two-Dimensional Metal–Halide Perovskite through Exciton Binding Energy

Chen

Wang

et al. 2021

J. Am. Chem. Soc.

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“…Solution-based routes to nanocrystals of all-inorganic metal halide perovskites and perovskite-related phases have been demonstrated to be important and useful. However, these methods are typically limited to a small number of systems that include the A-site cations Rb + and Cs + and the B-site cations Pb 2+ , Sn 2+ , and Ge 2+ . − Additional cations have been incorporated, including Ag + , Tl 3+ , Bi 3+ , and In 3+ , , albeit in the double-perovskite structure. Cadmium-based halide perovskites and perovskite-related phases, which offer unique properties in comparison to their lead halide counterparts, have been studied in the context of doping effects that modify electron paramagnetic resonance and photoluminescent signals, which are important for photon upconversion and higher excited-state luminescence. − CsCdCl 3 was also considered in the context of a computational screening effort to identify possible metal halide perovskite semiconductors, and CsCdBr 3 was studied for its nonlinear optical properties .…”

Section: Introductionmentioning

confidence: 99%

Phase-Selective Solution Synthesis of Perovskite-Related Cesium Cadmium Chloride Nanoparticles

et al. 2020

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All-inorganic metal halide perovskite-related phases are semiconducting materials that are of significant interest for a wide range of applications. Nanoparticles of these materials are particularly useful because they permit solution processing while offering unique and tunable properties. Of the many metal halide systems that have been studied extensively, cesium cadmium chlorides remain underexplored, and synthetic routes to access them as nanoscale materials have not been established. Here we demonstrate that a simple solution-phase reaction involving the injection of a cesium oleate solution into a cadmium chloride solution produces three distinct cesium cadmium chlorides: hexagonal CsCdCl3 and the Ruddlesden–Popper layered perovskites Cs2CdCl4 and Cs3Cd2Cl7. The phase-selective synthesis emerges from differences in reagent concentrations, temperature, and injection rates. A key variable is the rate at which the cesium oleate solution is injected into the cadmium chloride solution, which is believed to influence the local Cs:Cd concentration during precipitation, leading to control over the phase that forms. Band structure calculations indicate that hexagonal CsCdCl3 is a direct band gap semiconductor while Cs2CdCl4 and Cs3Cd2Cl7 have indirect band gaps. The experimentally determined band gap values for CsCdCl3, Cs2CdCl4, and Cs3Cd2Cl7 are 5.13, 4.91, and 4.70 eV, respectively, which places them in a rare category of ultrawide-band-gap semiconductors.

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“…Lead halides of perovskite lattices have emerged as a family of semiconductors promising for optoelectronic applications. − Nanocrystal structures can further improve the strength of light–matter interaction benefiting from the quantum confinement effect. − Highly efficient light absorption and emission make perovskite semiconductor nanocrystals ideal gain media for laser demonstration. ,− Nevertheless, the inherent degeneracies of band-edge states require a relatively high pump threshold of more than one exciton per nanocrystal to achieve the population inversion to support optical gain in these nanocrystals. − …”

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confidence: 99%

Electrical Switching of Optical Gain in Perovskite Semiconductor Nanocrystals

et al. 2021

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Perovskite semiconductor nanocrystals are promising for optical amplification and laser applications benefiting from efficient optical gain generation. Nevertheless, the pump threshold is limited by more than one exciton per nanocrystal required to generate population inversion in neutral nanocrystals due to the level degeneracy. Here, we show that by charging nanocrystals with current injection, the level degeneracy can be lifted to generate charged exciton gain with markedly low excitation density. On the basis of the scenario, we have demonstrated electrical switching of amplified spontaneous emission in films of CsPbBr3 nanocrystals sandwiched by two electrodes with over 50% threshold reduction owing to charged excitons. Our work provides an effective approach to electrically modulated optical gain in colloidal perovskite nanocrystals for potential applications in advanced laser and information technology.

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An All‐Inorganic Perovskite‐Phase Rubidium Lead Bromide Nanolaser

Cited by 15 publications

References 47 publications

Tuning Spin-Polarized Lifetime in Two-Dimensional Metal–Halide Perovskite through Exciton Binding Energy

Tuning Spin-Polarized Lifetime in Two-Dimensional Metal–Halide Perovskite through Exciton Binding Energy

Phase-Selective Solution Synthesis of Perovskite-Related Cesium Cadmium Chloride Nanoparticles

Electrical Switching of Optical Gain in Perovskite Semiconductor Nanocrystals

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