Resonantly enhanced multiple exciton generation through below-band-gap multi-photon absorption in perovskite nanocrystals

Manzi, Aurora; Tong, Yu; Feucht, Julius; Yao, En‐Ping; Polavarapu, Lakshminarayana; Urban, Alexander S.; Feldmann, Jochen

doi:10.1038/s41467-018-03965-8

Cited by 77 publications

(72 citation statements)

References 28 publications

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“…For example, it is still not clear how different types of ligands, defects, dopants, and crystalline phases influence the optical properties, stability, and activity of the heterostructures. We also have little knowledge of whether the other unique properties of MHPs, such as multiple carrier generation, piezoelectric, and ferroelectric properties of MHPs, could be employed to promote the photoredox catalytic reaction. It is still unknown to us whether the key parameters of an unsuccessful/unpleasant photoredox catalytic conversion are attributed to the diminishing photophysical properties of MHPs or the incompatibility of MHPs with external photocatalytic reaction conditions.…”

Section: Discussionsupporting

confidence: 89%

Recent Progress in Engineering Metal Halide Perovskites for Efficient Visible‐Light‐Driven Photocatalysis

et al. 2020

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Artificial photosynthesis has attracted increasing attention due to recent environmental and energy concerns. Metal halide perovskites (MHPs) demonstrating excellent optoelectronic properties have currently emerged as novel and efficient photocatalytic materials. Herein, the structural features of MHPs that are responsible for the photoinduced charge separation and charge migration properties are briefly introduced, and then important and necessary photophysical and photochemical aspects of MHPs related to photoredox catalysis are summarized. Subsequently, the applications of MHPs for solar energy harvesting and photocatalytic conversion, including H2 evolution, CO2 reduction, degradation of organic pollutants, and photoredox organic synthesis, are extensively demonstrated, with a focus on strategies for improving the performance (e.g., selectivity, activity, stability, recyclability, and environmental compatibility) of these MHP‐based photocatalytic systems. To conclude, existing challenges and prospects on the future development of MHP‐based materials towards photoredox catalysis applications are detailed.

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Section: Discussionsupporting

confidence: 89%

Recent Progress in Engineering Metal Halide Perovskites for Efficient Visible‐Light‐Driven Photocatalysis

et al. 2020

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“…In the case of IP-NCs, CM would be of great fundamental impact on this upcoming material and directly beneficial to its application in novel optoelectronic nanodevices, most notably photodetectors, while the band gaps of the currently available IP-NCs are still too large for practical impact in solar cells. Nevertheless, the research continues vigorously and rapid progress is being made—see, e.g., ref 42 for a very recent report on the possibility of multiple exciton generation in CsPbBr 3 upon nonlinear absorption at sub-band energies. That is why CM in IP-NCs is of interest and has been investigated further.…”

Section: Introductionmentioning

confidence: 99%

Efficient carrier multiplication in CsPbI3 perovskite nanocrystals

et al. 2018

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The all-inorganic perovskite nanocrystals are currently in the research spotlight owing to their physical stability and superior optical properties—these features make them interesting for optoelectronic and photovoltaic applications. Here, we report on the observation of highly efficient carrier multiplication in colloidal CsPbI3 nanocrystals prepared by a hot-injection method. The carrier multiplication process counteracts thermalization of hot carriers and as such provides the potential to increase the conversion efficiency of solar cells. We demonstrate that carrier multiplication commences at the threshold excitation energy near the energy conservation limit of twice the band gap, and has step-like characteristics with an extremely high quantum yield of up to 98%. Using ultrahigh temporal resolution, we show that carrier multiplication induces a longer build-up of the free carrier concentration, thus providing important insights into the physical mechanism responsible for this phenomenon. The evidence is obtained using three independent experimental approaches, and is conclusive.

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“…On one hand, there have been many experimental reports [5][6][7][8][9][10][11][12][13][14][15] on the enhancement of MPA coefficients or cross-sections if one utilizes nanostructured perovskites, such as in 2D forms, or quantum dots (QDs). For example, the three-photon absorption (3PA) action cross sections have been reported as high as 10 −73 cm 6 s 2 photon −2 for perovskite QDs with diameters of 8-10 nm.…”

Section: Introductionmentioning

confidence: 99%

Layered Hybrid Perovskites for Highly Efficient Three‐Photon Absorbers: Theory and Experimental Observation

Zhou

Zhang

et al. 2018

Advanced Science

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Multiphoton absorption may find many technological applications, such as enhancing the conversion efficiency of solar cells by the utilization of sub‐band‐energy photons, below‐bandgap photodetection through the simultaneous absorption of several infrared photons for photocurrent generation, or light frequency upconversion for high‐resolution, 3D imaging. To enhance multiphoton absorption in semiconducting materials, one of the strategies is to explore low‐dimensional excitons. Here, a quantum perturbation theory on a giant enhancement in three‐photon absorption (3PA) arising from 2D excitons in multilayered crystals of organic–inorganic hybrid perovskites is presented. The maximal 3PA coefficient is predicted to be in the range of 2–7 cm 3 GW −2 at 1100 nm, the largest values reported so far for any 2D and bulk semiconductors at room temperature. Excellent agreement between theory and the experimental findings unambiguously demonstrates a pivotal role in the enhancement of 3PA played by 2D excitons. The theory predicts that the resonant 3PA coefficient should be enhanced further by at least two orders of magnitude with very low temperature. The findings are essential for understanding giant 3PA arising from 2D excitons in layered hybrid perovskites and may open new pathways for highly efficient conversion from infrared light energy to either electrical energy or higher‐frequency light emission/lasing.

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Resonantly enhanced multiple exciton generation through below-band-gap multi-photon absorption in perovskite nanocrystals

Cited by 77 publications

References 28 publications

Recent Progress in Engineering Metal Halide Perovskites for Efficient Visible‐Light‐Driven Photocatalysis

Recent Progress in Engineering Metal Halide Perovskites for Efficient Visible‐Light‐Driven Photocatalysis

Efficient carrier multiplication in CsPbI3 perovskite nanocrystals

Layered Hybrid Perovskites for Highly Efficient Three‐Photon Absorbers: Theory and Experimental Observation

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