Lengthening of Exciton Lifetime in Linear Perovskite-Upconversion Hybrid Assemblies
Alejandro Cortés-Villena a, Nestor Estebanez a, Juan Ferrera-González a, María González-Béjar a, Raquel E. Galian a, Soranyel González-Carrero b, Julia Pérez-Prieto a
a Institute of Molecular Science, University of Valencia C/ Catedrático José Beltrán Martínez 2, Paterna, 46980, Valencia, Spain
b Department of Chemistry, Imperial College London Molecular Sciences Research Hub, White City Campus 80 Wood Lane, London W12 0BZ, UK
Materials for Sustainable Development Conference (MATSUS)
Proceedings of MATSUS23 & Sustainable Technology Forum València (STECH23) (MATSUS23)
#NCFun23 - Fundamental Processes in Nanocrystals and 2D Materials
VALÈNCIA, Spain, 2023 March 6th - 10th
Organizers: Valerio Pinchetti and Shalini Singh
Poster, Alejandro Cortés-Villena, 313
Publication date: 22nd December 2022

One of the fundamental issues limiting the power conversion efficiency (PCE) of single-junction perovskite solar cells (PSCs) is their inability to absorb near-infrared (NIR) photons, being this the least exploited region of the solar spectrum. A promising alternative to overcome this limit is the use of upconversion nanomaterials since they can absorb low-energy photons. [1]

Moreover, the use of templates as directing agents for nanomaterials is increasingly becoming more prominent in the design of new materials with tailor-made properties. Specifically, lead sulfate molecular clusters play a key role in the linear assembly of nanoparticles of different compositions, sizes and shapes, leading to long, 1D nanoparticle arrays based on the strong interaction between the clusters and nanoparticles. [2]

In this work, the preparation of the first linear ternary hybrid assembly composed by: i) all-inorganic cesium lead halide perovskites (CsPbX3; X=Cl-, Br-, I- and their mixture), ii) lanthanide-doped upconversion (NaYF4:Yb3+, Ln3+; Ln3+=Tm3+, Er3+) nanoparticles, and iii) lead sulfate molecular clusters are reported both as colloid and solid film. [3] Efficient sensitized emission of perovskite nanocrystals is achieved triggered by nearby lanthanide-doped upconversion nanoparticles under NIR excitation (975 nm) thanks to the closeness between both nanoparticles in the template. We have observed that the photophysical properties regarding quenching in the lifetime of the upconversion emission band along with the lengthening of the perovskite exciton lifetime (from nano- to microseconds) in the hybrid assembly depend on irradiance and sample preparation conditions. Therefore, two techniques with different temporal resolutions (time-resolved photoluminescence spectroscopy and NIR laser scanning microscopy) were used to determine the efficiency of the lanthanide resonance energy transfer (LRET) mechanism involved in the sensitization of the perovskite emission. The chemical stability of the perovskite in the hybrid assembly against water is also analyzed. We believe this ternary hybrid assembly holds the promise for the fabrication of future light-harvesting devices extended to the NIR optical window.

We thank MCIN PID2020-115710GB-I00 and the FPI grant (A.C.V.) PRE2018-084294 funded by MCIN/AEI/10.13039/501100011033 and ESF Investing in your future, partially co-financed with FEDER and Generalitat Valenciana funds (PROMETEO/2019/080 and IDIFEDER/2018/064).

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