Lattice Compression Increases the Activation Barrier for Phase Segregation in Mixed-Halide Perovskites

Loreta A. Muscarella; Eline M. Hutter; Francesca Wittmann; Young Won Woo; Young-Kwang Jung; Lucie McGovern; Jan Versluis; Aron Walsh; Huib J. Bakker; Bruno Ehrler

doi:10.1021/acsenergylett.0c01474

Lattice Compression Increases the Activation Barrier for Phase Segregation in Mixed-Halide Perovskites

Loreta A. Muscarella, Eline M. Hutter, Francesca Wittmann, Young Won Woo, Young-Kwang Jung, Lucie McGovern, Jan Versluis, Aron Walsh, Huib J. Bakker, Bruno Ehrler

Research output: Contribution to Journal › Article › Academic › peer-review

Abstract

The bandgap tunability of mixed-halide perovskites makes them promising candidates for light-emitting diodes and tandem solar cells. However, illuminating mixed-halide perovskites results in the formation of segregated phases enriched in a single halide. This segregation occurs through ion migration, which is also observed in single-halide compositions, and whose control is thus essential to enhance the lifetime and stability. Using pressure-dependent transient absorption spectroscopy, we find that the formation rates of both iodide-and bromide-rich phases in MAPb(BrxI1-x)3 reduce by 2 orders of magnitude on increasing the pressure to 0.3 GPa. We explain this reduction from a compression-induced increase of the activation energy for halide migration, which is supported by first-principle calculations. A similar mechanism occurs when the unit cell volume is reduced by incorporating a smaller cation. These findings reveal that stability with respect to halide segregation can be achieved either physically through compressive stress or chemically through compositional engineering.

Original language	English
Pages (from-to)	3152-3158
Journal	ACS Energy Letters
Volume	5
Issue number	10
DOIs	https://doi.org/10.1021/acsenergylett.0c01474
Publication status	Published - 9 Oct 2020
Externally published	Yes

Funding

The work of L.A.M., E.M.H., F.W., L.McG., J.V., H.J.B., and B.E. is part of the Dutch Research Council (NWO) and was performed at the research institute AMOLF. The work of L.A.M. and L.McG. was supported by NWO Vidi grant 016.Vidi.179.005. The work of Y.W.W., Y.K.J., and A.W. was supported by the Creative Materials Discovery Program through the National Research Foundation of Korea (NRF) funded by Ministry of Science and ICT (2018M3D1A1058536). Y.W.W., Y.K.J., and A.W. are grateful to the UK Materials and Molecular Modelling Hub for computational resources, which is partially funded by EPSRC (EP/P020194/1).

Funders	Funder number
Engineering and Physical Sciences Research Council	EP/P020194/1
Nederlandse Organisatie voor Wetenschappelijk Onderzoek	016
Ministry of Science, ICT and Future Planning	2018M3D1A1058536
National Research Foundation of Korea

Access to Document

10.1021/acsenergylett.0c01474

Persistent URL (handle)

Persistent link

Cite this

@article{62d7da46b3c4441b9ab468afd8f060a8,

title = "Lattice Compression Increases the Activation Barrier for Phase Segregation in Mixed-Halide Perovskites",

abstract = "The bandgap tunability of mixed-halide perovskites makes them promising candidates for light-emitting diodes and tandem solar cells. However, illuminating mixed-halide perovskites results in the formation of segregated phases enriched in a single halide. This segregation occurs through ion migration, which is also observed in single-halide compositions, and whose control is thus essential to enhance the lifetime and stability. Using pressure-dependent transient absorption spectroscopy, we find that the formation rates of both iodide-and bromide-rich phases in MAPb(BrxI1-x)3 reduce by 2 orders of magnitude on increasing the pressure to 0.3 GPa. We explain this reduction from a compression-induced increase of the activation energy for halide migration, which is supported by first-principle calculations. A similar mechanism occurs when the unit cell volume is reduced by incorporating a smaller cation. These findings reveal that stability with respect to halide segregation can be achieved either physically through compressive stress or chemically through compositional engineering.",

author = "Muscarella, {Loreta A.} and Hutter, {Eline M.} and Francesca Wittmann and Woo, {Young Won} and Young-Kwang Jung and Lucie McGovern and Jan Versluis and Aron Walsh and Bakker, {Huib J.} and Bruno Ehrler",

year = "2020",

month = oct,

day = "9",

doi = "10.1021/acsenergylett.0c01474",

language = "English",

volume = "5",

pages = "3152--3158",

journal = "ACS Energy Letters",

issn = "2380-8195",

publisher = "American Chemical Society",

number = "10",

}

TY - JOUR

T1 - Lattice Compression Increases the Activation Barrier for Phase Segregation in Mixed-Halide Perovskites

AU - Muscarella, Loreta A.

AU - Hutter, Eline M.

AU - Wittmann, Francesca

AU - Woo, Young Won

AU - Jung, Young-Kwang

AU - McGovern, Lucie

AU - Versluis, Jan

AU - Walsh, Aron

AU - Bakker, Huib J.

AU - Ehrler, Bruno

PY - 2020/10/9

Y1 - 2020/10/9

N2 - The bandgap tunability of mixed-halide perovskites makes them promising candidates for light-emitting diodes and tandem solar cells. However, illuminating mixed-halide perovskites results in the formation of segregated phases enriched in a single halide. This segregation occurs through ion migration, which is also observed in single-halide compositions, and whose control is thus essential to enhance the lifetime and stability. Using pressure-dependent transient absorption spectroscopy, we find that the formation rates of both iodide-and bromide-rich phases in MAPb(BrxI1-x)3 reduce by 2 orders of magnitude on increasing the pressure to 0.3 GPa. We explain this reduction from a compression-induced increase of the activation energy for halide migration, which is supported by first-principle calculations. A similar mechanism occurs when the unit cell volume is reduced by incorporating a smaller cation. These findings reveal that stability with respect to halide segregation can be achieved either physically through compressive stress or chemically through compositional engineering.

AB - The bandgap tunability of mixed-halide perovskites makes them promising candidates for light-emitting diodes and tandem solar cells. However, illuminating mixed-halide perovskites results in the formation of segregated phases enriched in a single halide. This segregation occurs through ion migration, which is also observed in single-halide compositions, and whose control is thus essential to enhance the lifetime and stability. Using pressure-dependent transient absorption spectroscopy, we find that the formation rates of both iodide-and bromide-rich phases in MAPb(BrxI1-x)3 reduce by 2 orders of magnitude on increasing the pressure to 0.3 GPa. We explain this reduction from a compression-induced increase of the activation energy for halide migration, which is supported by first-principle calculations. A similar mechanism occurs when the unit cell volume is reduced by incorporating a smaller cation. These findings reveal that stability with respect to halide segregation can be achieved either physically through compressive stress or chemically through compositional engineering.

UR - http://www.scopus.com/inward/record.url?scp=85092462932&partnerID=8YFLogxK

U2 - 10.1021/acsenergylett.0c01474

DO - 10.1021/acsenergylett.0c01474

M3 - Article

SN - 2380-8195

VL - 5

SP - 3152

EP - 3158

JO - ACS Energy Letters

JF - ACS Energy Letters

IS - 10

ER -

Lattice Compression Increases the Activation Barrier for Phase Segregation in Mixed-Halide Perovskites

Abstract

Funding

Access to Document

Persistent URL (handle)

Other files and links

Fingerprint

Cite this