Effect of interconnectivity on the photophysics of perovskite QD networks
Juan F. Galisteo-López a, David O. Tiede a, Mauricio E. Calvo a, Katherine A. Koch b, Carlos Romero-Pérez a, K. Burak Ucer b, Ajay Ram Srimath Kandada b, Hernán Míguez a
a Multifunctional Optical Materials Group, Institute of Materials Science of Seville (CSIC-US), C/Américo Vespucio 49, 41092 Sevilla, Spain.
b Department of Physics and Center for Functional Materials, Wake Forest University, Winston-Salem, NC 27109, United States
Materials for Sustainable Development Conference (MATSUS)
Proceedings of MATSUS Spring 2025 Conference (MATSUSSpring25)
Photophysics of metal halide perovskites: from fundamentals to emerging applications - #PeroLight
Sevilla, Spain, 2025 March 3rd - 7th
Organizers: Ivan Scheblykin and Yana Vaynzof
Oral, Juan F. Galisteo-López, presentation 175
DOI: https://doi.org/10.29363/nanoge.matsusspring.2025.175
Publication date: 16th December 2024

In order to implement quantum dots (QDs) into most optoelectronic applications, from photovoltaic to light emitting devices, one needs to organize them into an interconnected array in the shape of a QD film. In this configuration a certain degree of electronic coupling among QDs is achieved, allowing for charge injection/extraction, at the expense of a reduction of the quantum confinement that characterizes these structures.

In this presentation we will discuss recent results where carrier cooling and recombination have been studied in QD solids as a function of connectivity. In order to exert control on electronic coupling among QDs we vary their average separation through their concentration when grown within the pores of nanoporous metal-oxide matrices. [1] We perform a thorough photophysical characterization comprising linear spectroscopy, PL quantum yield and ultrafast spectroscopic measurements while tuning the average QD separation and observe a transition in carrier recombination from isolated nanostructures to interconnected ones. The effects on global emission properties in terms of isolated and bulk-like behavior are pointed out in detail. [2]

Similar studies in the initial instants after carrier photo-excitation allow us to unveil the role of electronic coupling in the intra-band cooling of excited carriers. A retardation of the cooling dynamics is observed as we reduce QD connectivity and associated with carrier reheating taking place as a consequence of Auger-like processes. [3]

Thus a broad picture is provided on the fate of photoexcited carriers in QD films as a function of connectivity that can help to build an intuition when planning the use of these structures in devices operating in different carrier density regimes.     

H.M. is thankful for the financial support of the Spanish Ministryof Science and Innovation under grant PID2020-116593RB-I00, fundedby MCIN/AEI/10.13039/501100011033, the Junta de Andalucía undergrant P18-RT-2291 (FEDER/UE) and TED2021-129679B-C22, funded byMCIN/AEI/10.13039/ 501100011033 and by Unión Europea NextGener-ationEU/PRTR. H.M., J.F.G.L., and D.O.T. acknowledges financial sup-port from the European Union’s Horizon 2020 research and innovationprogram under the Marie Skłodowska-Curie grant agreement No 956270(Persephone). A.R.S.K. acknowledges the start-up funds provided by WakeForest University and funding from the Center for Functional Materials andthe Office of Research and Sponsored Programs at WFU.

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