Exciton dynamics and non-linearities in two-dimensional hybrid organic perovskites

Abdel-Baki, Katia; Boitier, Fabien; Diab, Hiba; Lanty, Gaëtan; Jemli, Khaoula; Lédée, Ferdinand; Garrot, Damien; Deleporte, Emmanuelle; Lauret, Jean‐sébastien

doi:10.1063/1.4941345

Cited by 40 publications

(53 citation statements)

References 52 publications

(81 reference statements)

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“…The (PEA) 2 PbI 4 flake was further characterized by a linear absorption measurement, as shown in Figure c. The absorption spectrum exhibits a sharp absorption peak at ≈518 nm (≈2.394 eV), which corresponds to the excitonic absorption of (PEA) 2 PbI 4 and agrees well with the previous study . Figure d shows the one‐ and two‐photon excited photoluminescence (PL) spectra measured under excitation by a continuous‐wave (CW) laser at 473 nm and a femtosecond laser at 800 nm, respectively.…”

Section: Resultssupporting

confidence: 83%

“…The hybrid dielectric structure exhibits a fast decay lifetime of 0.64 ns and a slow decay lifetime of 4.5 ns (τ ave = 3.74 ns). The fast decay is related to the radiative recombination, while the slow decay is caused by trap‐assisted recombination . For the bare perovskite flake, the fast and slow decay components have lifetimes of 0.63 and 3 ns (τ ave = 1.37 ns), respectively.…”

Section: Resultsmentioning

confidence: 99%

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Cooperative Enhancement of Two‐Photon‐Absorption‐Induced Photoluminescence from a 2D Perovskite‐Microsphere Hybrid Dielectric Structure

Liu

Song

et al. 2018

Adv Funct Materials

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Two-photon-absorption-induced photoluminescence (TPL) from nanostructures is generally inefficient since it is a typical third-order nonlinear optical process. Herein, a hybrid dielectric structure composed of dielectric microspheres (approximately micrometers in diameter) covering a 2D perovskite flake is reported, which provides a straightforward strategy for enhancing the TPL emission. The microspheres in the hybrid dielectric structure not only concentrate the pumping laser but also effectively increase the detection efficiency of the emitted TPL signal. The internal quantum efficiency of the 2D perovskite is also increased in the hybrid dielectric structure due to a reduced nonradiative rate. These effects cooperatively increase the TPL emission by two orders of magnitude in the hybrid dielectric structure. Moreover, the hybrid dielectric structure is proven to be useful for TPL-based superresolution imaging at a relatively low excitation power of 0.05 mW. This work demonstrates great promise for developing lowcost, high-performance nonlinear nanodevices based on hybrid dielectric structures.

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Section: Resultssupporting

confidence: 83%

Section: Resultsmentioning

confidence: 99%

Cooperative Enhancement of Two‐Photon‐Absorption‐Induced Photoluminescence from a 2D Perovskite‐Microsphere Hybrid Dielectric Structure

Liu

Song

et al. 2018

Adv Funct Materials

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“…[8][9][10][11] The thickness (n) of the perovskite sheets can be synthetically controlled by adjusting the ratio between the spacer cation and the small organic cation, thus allowing the onset of absorption to be tuned from violet to near infrared. [33,34] In this work, temperature-and power-dependent timeresolved photoluminescences (PLs) are performed to investigate band-edge excitonic features of 2D perovskite. [33,34] In this work, temperature-and power-dependent timeresolved photoluminescences (PLs) are performed to investigate band-edge excitonic features of 2D perovskite.…”

Section: Introductionmentioning

confidence: 99%

Band‐Edge Exciton Fine Structure and Exciton Recombination Dynamics in Single Crystals of Layered Hybrid Perovskites

Fang

Yang

Adjokatse

et al. 2019

Adv Funct Materials

118

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2D perovskite materials have recently reattracted intense research interest for applications in photovoltaics and optoelectronics. As a consequence of the dielectric and quantum confinement effect, they show strongly bound and stable excitons at room temperature. Here, the band-edge exciton fine structure and in particular its exciton and biexciton dynamics in high quality crystals of (PEA) 2 PbI 4 are investigated. A comparison of bulk and surface exciton lifetimes yields a room temperature surface recombination velocity of 2 × 10 3 cm s −1 and an intrinsic lifetime of 185 ns. Biexciton emission is evidenced at room temperature, with a binding energy of ≈45 meV and a lifetime of 80 ps. At low temperature, exciton state splitting is observed, which is caused by the electron-hole exchange interaction. Transient photoluminescence resolves the low-lying dark exciton state, with a bright/dark splitting energy estimated to be 10 meV. This work contributes to the understanding of the complex scenario of the elementary photoexcitations in 2D perovskites. materials such as transition metal dichalcogenides, phosphorene, and graphene. They can be easily grown by both solution methods and vapor transport methods at low temperature, [14][15][16][17] with a tunable bulk direct bandgap. [18] These advantages make them appealing for future optoelectronic and photonic applications.Unlike their 3D counterparts, the dielectric and quantum confinement of carriers in the 2D perovskite layers gives rise to unusually strong excitonic effects. [19,20] It has been experimentally observed that excitons are tightly confined in the inorganic layers with binding energy as high as a few hundred millielectronvolts (significantly higher than that of 3D perovskites). [21] This greatly enhanced exciton binding energy makes them particularly interesting for light-emitting applications. [8,22] Moreover, 2D perovskites can exhibit a variety of multiexciton species, including biexcitons and trions. [20,23,24] The presence of these quasiparticles is exciting due to their unique role, leading to a better understanding of many body effects and their great promise for photonic applications. In addition, recent experiments reveal an important role of electron-phonon couplings on the exciton dynamics in 2D lead-iodide perovskite, suggesting a complex scenario for carrier relaxation and exciton formation. [25,26] It is therefore crucial to understand elementary photoexcitations in these layered materials. However, exciton fine structures and their properties are usually masked by local energy fluctuations resulting from disorder in thin films or broad emission due to the formation of self-trapped excitons. [27] Whereas their steady-state optical properties have

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“…When increasing the ratio of OA + in layered perovskite, each inorganic layer will contain less corner‐shared inorganic octahedral layers as shown in Fig. a, leading to the thinner inorganic layer and stronger quantum confinement effect . Therefore, layered perovskite can have strong exciton recombination under high OA + concentration .…”

Section: Introductionmentioning

confidence: 99%

“…a, leading to the thinner inorganic layer and stronger quantum confinement effect . Therefore, layered perovskite can have strong exciton recombination under high OA + concentration . Furthermore, the stability of layered perovskite is better than 3D perovskite MAPbX 3 due to the large van der Waals force of OA + .…”

Section: Introductionmentioning

confidence: 99%

Highly luminescent and stable layered perovskite as the emitter for light emitting diodes

Wei

Sun

Liu

et al. 2016

Physica Status Solidi (a)

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Air instability and poor exciton recombination of 3D perovskites MAPbX 3 (MA ¼ CH 3 NH 3 , X ¼ halogens) seriously hinder their applications in light emitting diodes. Herein, we report a promising alternative to solve these two critical drawbacks. Layered perovskite OA 2 (MA) nÀ1 Pb n Br 3nþ1 (OA ¼ C 8 H 17 NH 3 ) has higher binding energy and is passivated by long organic chain, which can be synthesized using a facile method. By increasing the OA þ ratio in layered perovskite, strong quantum confinement effect and obvious features of exciton were observed in photoluminescence and UV-Vis absorption spectra. Notably, the photoluminescence quantum yield (PLQY) of (OA) 2 (MA) 2 Pb 3 Br 10 (n ¼ 3 layered perovskite) can be up to 67.3% due to the enhanced exciton recombination, significantly higher than its 3D counterpart. Moreover, layered perovskite exhibits promoted stability in air than that of the 3D perovskite. The layered perovskite (OA) 2 (MA) 2 Pb 3 Br 10 -based perovskite light emitting diodes (PeLEDs) with a maximum current efficiency, a maximum power efficiency and the external quantum efficiency (EQE) of 1.43 cd A À1 , 0.89 lm W À1 , and 0.53% was demonstrated, which can be compared with that of the best-reported perovskite quantum dots LEDs so far. The demonstration of layered perovskite renders its bright future in optoelectronic applications, such as displays and photodetections.

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Exciton dynamics and non-linearities in two-dimensional hybrid organic perovskites

Cited by 40 publications

References 52 publications

Cooperative Enhancement of Two‐Photon‐Absorption‐Induced Photoluminescence from a 2D Perovskite‐Microsphere Hybrid Dielectric Structure

Cooperative Enhancement of Two‐Photon‐Absorption‐Induced Photoluminescence from a 2D Perovskite‐Microsphere Hybrid Dielectric Structure

Band‐Edge Exciton Fine Structure and Exciton Recombination Dynamics in Single Crystals of Layered Hybrid Perovskites

Highly luminescent and stable layered perovskite as the emitter for light emitting diodes

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