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Issue 3, 2019
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Broadband ultrafast nonlinear optical studies revealing exciting multi-photon absorption coefficients in phase pure zero-dimensional Cs4PbBr6 perovskite films

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Abstract

Lead halide perovskite nanocrystals (NCs) apart from their overwhelming optoelectronic applications have recently demonstrated promising nonlinear optical (NLO) properties such as strong two-photon absorption cross-sections (∼105 GM), two-photon fluorescence, and saturable absorption even at very high peak intensity. Zero-dimensional perovskite-related materials (0-D PRMs) are a new class of materials offering a high exciton binding energy (Eg ≥ 180 meV) with a strong photoluminescence (PL) quantum yield in few cases. Herein, we report the broadband third-order NLO properties of phase pure Cs4PbBr6 0-D PRM achieved using the Z-scan and degenerate four-wave mixing techniques in the femtosecond regime. Considering the growing content of the fluorescent and non-fluorescent forms of this material, we have performed our studies on both of them. These perovskite NCs exhibited strong multi-photon absorption properties in the near-infrared region with two-photon absorption (2PA) (cross-section, σ2 = 10−43–10−44 cm4 s equivalent to ∼106 GM) in the 500–800 nm region, three-photon absorption (3PA) (cross-section, σ3 ∼10−73 cm6 s2) in the 900–1200 nm region and four-photon absorption (4PA) (cross-section, σ4 ∼10−100 cm8 s3) in the 1300–1500 nm spectral region. These multi-photon absorption processes are explained using a simple band diagram. The measured NLO coefficients and cross-sections are fairly large when compared to some of the earlier reports on perovskite-based NCs. Cs4PbBr6 0-D PRM also demonstrated a large third-order NLO susceptibility χ(3) (∼10−7 esu), which can be attributed to the strong quantum confinement arising from spatially isolated, exciton containing individual [PbBr6]4− octahedron. These results clearly suggest the potential of 0D-PRMs in applications such as photonics and ultrafast all-optical switching devices.

Graphical abstract: Broadband ultrafast nonlinear optical studies revealing exciting multi-photon absorption coefficients in phase pure zero-dimensional Cs4PbBr6 perovskite films

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Publication details

The article was received on 28 Aug 2018, accepted on 29 Nov 2018 and first published on 30 Nov 2018


Article type: Paper
DOI: 10.1039/C8NR06969G
Nanoscale, 2019,11, 945-954

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    Broadband ultrafast nonlinear optical studies revealing exciting multi-photon absorption coefficients in phase pure zero-dimensional Cs4PbBr6 perovskite films

    K. N. Krishnakanth, S. Seth, A. Samanta and S. Venugopal Rao, Nanoscale, 2019, 11, 945
    DOI: 10.1039/C8NR06969G

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