The pursuit of stability in halide perovskites : the monovalent cation and the key for surface and bulk self-healing

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2021
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Ceratti, Davide R.
Cohen, A. V.
Rakita, Yevgeny
Snarski, Lior
Jasti, Naga P.
Cremonesi, Llorenc
Kronik, Leeor
Hodes, Gary
Cahen, David
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Materials Horizons. Royal Society of Chemistry (RSC). 2021, 8(5), pp. 1570-1586. ISSN 2051-6347. eISSN 2051-6355. Available under: doi: 10.1039/d1mh00006c
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We find significant differences between degradation and healing at the surface or in the bulk for each of the different APbBr3 single crystals (A = CH3NH3+, methylammonium (MA); HC(NH2)2+, formamidinium (FA); and cesium, Cs+). Using 1- and 2-photon microscopy and photobleaching we conclude that kinetics dominate the surface and thermodynamics the bulk stability. Fluorescence-lifetime imaging microscopy, as well as results from several other methods, relate the (damaged) state of the halide perovskite (HaP) after photobleaching to its modified optical and electronic properties. The A cation type strongly influences both the kinetics and the thermodynamics of recovery and degradation: FA heals best the bulk material with faster self-healing; Cs+ protects the surface best, being the least volatile of the A cations and possibly through O-passivation; MA passivates defects via methylamine from photo-dissociation, which binds to Pb2+. DFT simulations provide insight into the passivating role of MA, and also indicate the importance of the Br3- defect as well as predicts its stability. The occurrence and rate of self-healing are suggested to explain the low effective defect density in the HaPs and through this, their excellent performance. These results rationalize the use of mixed A-cation materials for optimizing both solar cell stability and overall performance of HaP-based devices, and provide a basis for designing new HaP variants.

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ISO 690CERATTI, Davide R., A. V. COHEN, Ron TENNE, Yevgeny RAKITA, Lior SNARSKI, Naga P. JASTI, Llorenc CREMONESI, Leeor KRONIK, Gary HODES, David CAHEN, 2021. The pursuit of stability in halide perovskites : the monovalent cation and the key for surface and bulk self-healing. In: Materials Horizons. Royal Society of Chemistry (RSC). 2021, 8(5), pp. 1570-1586. ISSN 2051-6347. eISSN 2051-6355. Available under: doi: 10.1039/d1mh00006c
BibTex
@article{Ceratti2021-05-01pursu-57791,
  year={2021},
  doi={10.1039/d1mh00006c},
  title={The pursuit of stability in halide perovskites : the monovalent cation and the key for surface and bulk self-healing},
  number={5},
  volume={8},
  issn={2051-6347},
  journal={Materials Horizons},
  pages={1570--1586},
  author={Ceratti, Davide R. and Cohen, A. V. and Tenne, Ron and Rakita, Yevgeny and Snarski, Lior and Jasti, Naga P. and Cremonesi, Llorenc and Kronik, Leeor and Hodes, Gary and Cahen, David}
}
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