Non-Linear Effects in CsPbBr3 Perovskite in a Strong Quantum Confinement Regime
Brener Rodrigo De Carvalho Vale a b, Andres Burgos-Caminal a, Marine Eva Fedora Bouduban a, Marco Antonio Schiavon b, Jacques-Edouard Moser a
a Institute of Chemical Sciences and Engineering, Ecole Polytechnique Fédérale de Lausanne (EPFL), CH-1015 Lausanne, Switzerland
Proceedings of International Conference on Hybrid and Organic Photovoltaics (HOPV19)
Roma, Italy, 2019 May 12th - 15th
Organizers: Prashant Kamat, Filippo De Angelis and Aldo Di Carlo
Poster, Brener Rodrigo De Carvalho Vale, 231
Publication date: 11th February 2019

Hybrid organic-inorganic and all-inorganic lead halide perovskites have emerged as promising materials for different technological applications, such as photovoltaic devices, LEDs, and lasers. These semiconductors have been studied in the bulk and in the form of nanoparticles with different quantum confinement geometries (1D to 3D). However, most studies reported in the literature regarding 3D quantum confined perovskite or quantum dots (QDs) were carried out in a weak confinement regime, with particle sizes equal or larger than the exciton Bohr radius. Here, we explore the non-linear properties of perovskites in a strong quantum confinement regime. We synthesized colloidal dispersions of CsPbBr3 perovskite QDs with nanoparticle radius of the order of 2-4 nm. The QDs were characterized by transmission electron microscopy, while their optical properties were studied by steady-state and time-resolved photoluminescence spectroscopy and ultrafast transient absorption spectroscopy. The photoluminescence maximum and first excitonic absorption peak are observed at wavelengths l = 450-460 nm, and 420-450 nm, respectively. Based on Poisson statistics for exciton population in QDs, we obtain an absorption cross-section of the material at 3.2 eV varying between 2.8×10–15 cm–2 and 5.0×10–15 cm–2, depending on the size of the QDs. The formation of biexcitons is evidenced by the non-linear optical response of QDs submitted to increasing photoexcitation energy fluences. The biexciton lifetime is found to be extremely short, only 5-8 ps. The biexciton binding energy is derived as being 99 meV. This value is significantly larger than the typical binding energy reported in the literature. The difference is clearly attributed to the strong quantum confinement regime.

We gratefully acknowledge NCCR-MUST, Swiss National Science Foundation, and Swiss Confederation for their financial support

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