Nanophotonic Enhanced Multiphoton-Excited Photoluminescence of Perovskite Quantum Dots
Christiane Becker a, Sven Burger b, Carlo Barth a, Phillip Manley a, Klaus Jäger a, David Eisenhauer a, Grit Köppel a, Pavel Chabera c, Junsheng Chen c, Kaibo Zheng c, Tönu Pullerits c
a Helmholtz-Zentrum Berlin für Materialien und Energie GmbH, 12489 Berlin, Germany
b Zuse Institute Berlin, Takustr. 7, 14195 Berlin, Germany
c Department of Chemical Physics and NanoLund, Lund University, 22100 Lund, Sweden
nanoGe Perovskite Conferences
Proceedings of nanoGe International Conference on Perovskite Solar Cells, Photonics and Optoelectronics (NIPHO19)
International Conference on Perovskite Photonics and Optoelectronics
Jerusalem, Israel, 2019 February 24th - 27th
Organizers: Lioz Etgar and Paul Meredith
Oral, Christiane Becker, presentation 011
Publication date: 21st November 2018

All-inorganic perovskite lead halide semiconductors in the form of colloidal nanocrystals have recently caused a stir as an excellent class of materials for optoelectronic applications [1]. Their advantages range from extremely high photoluminescence efficiencies up to 90%, narrow and tunable emission spectra, facile solution deposition on arbitrary substrates, to the presence of surface-capping ligands for further electronic and optical adjustments. An additional feature of this material family stimulated developments in the field of multi-photon optics: Nanocrystals based on all-inorganic cesium lead bromide (CsPbBr3) perovskite colloidal quantum dots exhibit a giant two-photon absorption cross section in the order of 2·105 GM [2], inspiring applications on low-threshold multi-photon pumped stimulated emission and lasing. Nevertheless, high irradiance levels are generally required for such multi-photon processes. One strategy to enhance the multi-photon absorption is taking advantage of high local light intensities using photonic nanostructures.

In this study, we investigate the two-photon excited photoluminescence of CsPbBr3 perovskite quantum dots with 9.4 nm size interacting with the leaky modes of a silicon photonic crystal slab with a hexagonal nanohole geometry. [3]. By systematic excitation of optical resonances using a pulsed near-infrared laser beam (fwhm = 40 nm), we observe an enhancement of two-photon-excited photoluminescence by more than one order of magnitude when comparing to using a bulk silicon film. Experimental and numerical analyses allow relating these findings to near-field enhancement effects on the nanostructured silicon surface. We show that the electric field distributions close to the photonic crystal surface can be numerically classified and optimized by means of machine learning techniques [4]. The results reveal a promising approach for significantly decreasing the required irradiance levels for multi-photon processes being of advantage in applications like biomedical imaging, lighting and solar energy.

We thank Carola Klimm from Helmholtz-Zentrum Berlin for SEM imaging. We acknowledge the German Federal Ministry of Education and Research for funding the research activities of the Nano-SIPPE group within the program NanoMatFutur (No. 03X5520). The simulation results were obtained at the Berlin Joint Lab on Optical Simulations for Energy Research (BerOSE) of Helmholtz-Zentrum Berlin für Materialien und Energie, Zuse Institute Berlin and Freie Universität Berlin. Work in Lund was financed by the Swedish Research Council (VR), the Knut and Alice Wallenberg Foundation, the Swedish Energy Agency, NanoLund and the Crafoord Foundation. We acknowledge Einstein Foundation Berlin for funding within ECMath-OT9 and Deutsche Forschungsgemeinschaft (DFG) for funding within SFB787-B4.

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