Abstract
All-inorganic CsPbBr3 perovskite colloidal quantum dots have recently emerged as promising material for a variety of optoelectronic applications, among others for multi-photon-pumped 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. Here, we investigate two-photon-excited photoluminescence of CsPbBr3 perovskite quantum dots on a silicon photonic crystal slab. By systematic excitation of optical resonances using a pulsed near-infrared laser beam, we observe an enhancement of two-photon-pumped 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. The results reveal a promising approach for significant decreasing the required irradiance levels for multi-photon processes being of advantage in applications like low-threshold lasing, biomedical imaging, lighting and solar energy.
Highlights
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.[1−5] Their advantages range from extremely high photoluminescence efficiencies up to 90%, narrow and tunable emission spectra, and facile solution deposition on arbitrary substrates, to the presence of surface-capping ligands for further electronic and optical adjustments
By systematic excitation of optical resonances using a pulsed near-infrared laser beam, we observe an enhancement of two-photon-pumped photoluminescence by more than 1 order of magnitude when comparing to using a bulk silicon film
An additional feature of this material family stimulated developments in the field of multiphoton optics: Nanocrystals based on allinorganic cesium lead bromide (CsPbBr3) perovskite colloidal quantum dots exhibit a large two-photon absorption cross section on the order of 2 × 105 GM,[6−9] inspiring applications on low-threshold multiphoton pumped stimulated emission[6] and lasing.[7,10]
Summary
Photonic crystal slab with a hexagonal nanohole geometry and a lattice constant of 600 nm. In this case, we observe an enhancement of two-photon-pumped photoluminescence by a factor of 15 by using a nanopatterned instead of a planar substrate. Both experimentally and numerically, a single peak is observed occurring at an incident angle of 24° (experiment) and 26° (simulation), respectively. Christiane Becker: 0000-0003-4658-4358 Sven Burger: 0000-0002-3140-5380 Pavel Chabera: 0000-0002-0531-5138 Junsheng Chen: 0000-0002-2934-8030 Kaibo Zheng: 0000-0002-7236-1070 Tõnu Pullerits: 0000-0003-1428-5564
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