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About perovskites

Metal halide perovskites are semiconductor materials which have attracted considerable attention because of their high compositional freedom and unique electrical and optical properties, in combination with low-cost fabrication. They are being produced all around the world because they are extremely promising for multiple optoelectronic applications such as solar cells, light emitting diodes (LEDs), photodetectors, or as photocatalysts, but the fundamental understanding is lagging behind. We don’t know why they work so well. Our goal at Hofkens’ lab is to fill in the blanks. Establishing the structural changes and the charge carrier dynamics of metal halide perovskites under influence of external stimuli (light, temperature, humidity) at high spatial and temporal resolutions will have far-reaching consequences for developing high-efficiency materials for optoelectronic applications.

LEDs

LEDs

The wide range of color tunability, high color purity and bright photoluminescence of lead halide perovskites has led to an impressive progress in the external quantum efficiency of perovskite-based LEDs. However, perovskites lose their emission efficiency owing to the materials’ poor stability due to the presence of unwanted surface defects. In Hofkens lab, we focus on the preparation and exploration of (low-dimensional) perovskite nanocrystals for application in LEDs by adjusting synthesis protocols which have been developed within our group. Surface engineering by post-synthetic treatment is applied in order to passivate nanocrystal surface defects and stabilize the material in environmental conditions. A combination of structural and micro-spectroscopic studies allows us to unravel the chemistry at the origin of efficient surface passivation.

Key publications:

Bhatia, H.; Steele, J.; Martin, C.; Keshavarz, M.; Solis-Fernandez, G.; Yuan, H.; Fleury, G.; Huang, H.; Dovgaliuk, I.; Chernyshov, D.; Hendrix, J.; Roeffaers, M.; Hofkens, J.; Debroye, E. Single-Step Synthesis of Dual Phase Bright Blue-Green Emitting Lead Halide Perovskite Nanocrystal Thin Films. Chemistry of Materials, 2019, 31, 6824-6832, DOI: 10.1021/acs.chemmater.9b01277.

Debroye, E.; Yuan, H.; Bladt, E.; Baekelant, W.; Van der Auweraer, M.; Hofkens, J.; Bals, S.; Roeffaers, M. Facile Morphology-Controlled Synthesis of Organolead Iodide Perovskite Nanocrystals Using Binary Capping Agents. ChemNanoMat, 2017, 3, 223, DOI: 10.1002/cnma.201700006.

Perovskite phase polymorphism and stabilization

It is known that perovskites undergo a number of structural phase transitions as a function of temperature that markedly alter their optical and electronic properties. The precise phase transition temperature and exact crystal structure in each phase, however, are controversially discussed in the literature. Our research approaches provide advanced insights into the evolution of the crystal structure that are essential to interpret future investigations of the electronic, optical, and photonic properties of lead-halide perovskite materials. Moreover, we introduce the concept of strain to render the high-temperature, metastable black-phase CsPbI3 thin films stable at room temperature. Synchrotron-based experiments and ab initio thermodynamic modeling indicated the introduction of crystal distortions within ‘strained’ black CsPbI3 thin films, of which the thermal stability is vastly improved.

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Key publications:

Steele, J.; Lai, M; Zhang, Y.; Lin, Z.; Hofkens, J.; Roeffaers, M.; Yang, P. Phase Transitions and Anion Exchange in All-Inorganic Halide Perovskites. Acc. Mater. Res. 2020, 1, 1, 3–15. DOI: 10.1021/accountsmr.0c00009

 

Steele, J.; Jin, H.; Dovgaliuk, I.; Berger, R.; Braeckevelt, T.; Yuan, H.; Martin, C.; Solano, E.; Lejaeghere, K.; Rogge, S.; Notebaert, C.; Vandezande, W.; Janssen, K.; Goderis, B.; Debroye, E.; Wang, Y.-K.; Dong, Y.; Ma, D.; Saidaminov, M.; Tan, H.; Lu, Z.; Dyadkin, V.; Chernyshov, D.; Van Speybroeck, V.; Sargent, E.; Hofkens, J.; Roeffaers, M. Thermal unequilibrium of strained black CsPbI3 thin films. Science 2019, 365 (6454), 679-684, DOI: 10.1126/science.aax3878.

Keshavarz, M.; Ottesen, M.; Wiedmann, S.; Wharmby, M.; Küchler, R.; Yuan,H.; Debroye, E.; Steele, J.; Martens, J.; Hussey, N.; Bremholm, M.; Roeffaers, M.; Hofkens, J. Tracking Structural Phase Transitions in Lead-Halide Perovskites by Means of Thermal Expansion. Advanced Materials 2019, 31 (24), 1900521, DOI: 10.1002/adma.201900521

Steele, J.; Yuan, H.; Tan, C.; Keshavarz, M.; Steuwe, C.; Roeffaers, M.; Hofkens, J. Direct Laser Writing of δ- to α-Phase Transformation in Formamidinium Lead Iodide. ACS Nano 2017, 11, 8, 8072–8083, DOI: 10.1021/acsnano.7b02777

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