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Charge Carrier Diffusion Dynamics in Multisized Quaternary Alkylammonium-Capped CsPbBr3 Perovskite Nanocrystal Solids

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    0555266 - ÚFP 2022 RIV US eng J - Journal Article
    Alvarez, S. - Lin, W. - Abdellah, M. - Meng, J. - Žídek, Karel - Pullerits, T. - Zheng, K.
    Charge Carrier Diffusion Dynamics in Multisized Quaternary Alkylammonium-Capped CsPbBr3 Perovskite Nanocrystal Solids.
    ACS Applied Materials and Interfaces. Roč. 13, č. 37 (2021), s. 44742-44750. ISSN 1944-8244. E-ISSN 1944-8252
    R&D Projects: GA MŠk(CZ) EF16_026/0008390
    Institutional support: RVO:61389021
    Keywords : light-emitting-diodes * metal-halide perovskites * quantum dots * energy-transfer * lengths * mobilities * efficiency * trihalide * films * ultrafast spectroscopy * diffusion lengths * CsPbBr3 * ddab * quantum dot photovoltaics * carrier transport * charge transfer
    OECD category: Materials engineering
    Impact factor: 10.383, year: 2021
    Method of publishing: Open access
    https://pubs.acs.org/doi/pdf/10.1021/acsami.1c11676

    CsPbBr3 quantum dots (QDs) are promising candidates for optoelectronic devices. The substitution of oleic acid ( OA) and oleylamine ( OLA) capping agents with a quaternary alkylammonium such as di-dodecyl dimethyl ammonium bromide (DDAB) has shown an increase in external quantum efficiency (EQE) from 0.19% (OA/OLA) to 13.4% (DDAB) in LED devices. The device performance significantly depends on both the diffusion length and the mobility of photoexcited charge carriers in QD solids. Therefore, we investigated the charge carrier transport dynamics in DDAB-capped CsPbBr3 QD solids by constructing a bi-sized QD mixture film. Charge carrier diffusion can be monitored by quantitatively varying the ratio between two sizes of QDs, which varies the mean free path of the carriers in each QD cluster. Excited-state dynamics of the QD solids obtained from ultrafast transient absorption spectroscopy reveals that the photogenerated electrons and holes are difficult to diffuse among small-sized QDs (4 nm) due to the strong quantum confinement. On the other hand, both photoinduced electrons and holes in large-sized QDs (10 nm) would diffuse toward the interface with the small-sized QDs, followed by a recombination process. Combining the carrier diffusion study with a Monte Carlo simulation on the QD assembly in the mixture films, we can calculate the diffusion lengths of charge carriers to be similar to 239 +/- 16 nm in 10 nm CsPbBr3 QDs and the mobility values of electrons and holes to be 2.1 (+/- 0.1) and 0.69 (+/- 0.03) cm(2)/V s, respectively. Both parameters indicate an efficient charge carrier transport in DDAB-capped QD films, which rationalized the perfect performance of their LED device application.
    Permanent Link: http://hdl.handle.net/11104/0329789

     
     
Number of the records: 1