Role of microstructure in the electron–hole interaction of hybrid lead halide perovskites

Giulia Grancini, Ajay Ram Srimath Kandada, Jarvist M. Frost, Alex J. Barker, Michele De Bastiani, Marina Gandini, Sergio Marras, Guglielmo Lanzani, Aron Walsh, Annamaria Petrozza

Research output: Contribution to journalArticle

143 Citations (Scopus)
88 Downloads (Pure)

Abstract

Organic–inorganic metal halide perovskites have demonstrated high power conversion efficiencies in solar cells and promising performance in a wide range of optoelectronic devices. The existence and stability of bound electron–hole pairs in these materials and their role in the operation of devices with different architectures remains a controversial issue. Here we demonstrate, through a combination of optical spectroscopy and multiscale modelling as a function of the degree of polycrystallinity and temperature, that the electron–hole interaction is sensitive to the microstructure of the material. The long-range order is disrupted by polycrystalline disorder and the variations in electrostatic potential found for smaller crystals suppress exciton formation, while larger crystals of the same composition demonstrate an unambiguous excitonic state. We conclude that fabrication procedures and morphology strongly influence perovskite behaviour, with both free carrier and excitonic regimes possible, with strong implications for optoelectronic devices.
Original languageEnglish
Pages (from-to)695-701
JournalNature Photonics
Volume9
Early online date17 Aug 2015
DOIs
Publication statusPublished - Oct 2015

Fingerprint

perovskites
optoelectronic devices
Optoelectronic devices
halides
Lead
Metal halides
Crystals
microstructure
Microstructure
metal halides
Electrons
Excitons
Perovskite
Conversion efficiency
crystals
Electrostatics
Solar cells
solar cells
excitons
interactions

Cite this

Grancini, G., Srimath Kandada, A. R., Frost, J. M., Barker, A. J., De Bastiani, M., Gandini, M., ... Petrozza, A. (2015). Role of microstructure in the electron–hole interaction of hybrid lead halide perovskites. Nature Photonics, 9, 695-701. https://doi.org/10.1038/nphoton.2015.151

Role of microstructure in the electron–hole interaction of hybrid lead halide perovskites. / Grancini, Giulia; Srimath Kandada, Ajay Ram; Frost, Jarvist M.; Barker, Alex J.; De Bastiani, Michele; Gandini, Marina; Marras, Sergio; Lanzani, Guglielmo; Walsh, Aron; Petrozza, Annamaria.

In: Nature Photonics, Vol. 9, 10.2015, p. 695-701.

Research output: Contribution to journalArticle

Grancini, G, Srimath Kandada, AR, Frost, JM, Barker, AJ, De Bastiani, M, Gandini, M, Marras, S, Lanzani, G, Walsh, A & Petrozza, A 2015, 'Role of microstructure in the electron–hole interaction of hybrid lead halide perovskites', Nature Photonics, vol. 9, pp. 695-701. https://doi.org/10.1038/nphoton.2015.151
Grancini G, Srimath Kandada AR, Frost JM, Barker AJ, De Bastiani M, Gandini M et al. Role of microstructure in the electron–hole interaction of hybrid lead halide perovskites. Nature Photonics. 2015 Oct;9:695-701. https://doi.org/10.1038/nphoton.2015.151
Grancini, Giulia ; Srimath Kandada, Ajay Ram ; Frost, Jarvist M. ; Barker, Alex J. ; De Bastiani, Michele ; Gandini, Marina ; Marras, Sergio ; Lanzani, Guglielmo ; Walsh, Aron ; Petrozza, Annamaria. / Role of microstructure in the electron–hole interaction of hybrid lead halide perovskites. In: Nature Photonics. 2015 ; Vol. 9. pp. 695-701.
@article{2d5a8800a5674ddd82cefe88c7823da8,
title = "Role of microstructure in the electron–hole interaction of hybrid lead halide perovskites",
abstract = "Organic–inorganic metal halide perovskites have demonstrated high power conversion efficiencies in solar cells and promising performance in a wide range of optoelectronic devices. The existence and stability of bound electron–hole pairs in these materials and their role in the operation of devices with different architectures remains a controversial issue. Here we demonstrate, through a combination of optical spectroscopy and multiscale modelling as a function of the degree of polycrystallinity and temperature, that the electron–hole interaction is sensitive to the microstructure of the material. The long-range order is disrupted by polycrystalline disorder and the variations in electrostatic potential found for smaller crystals suppress exciton formation, while larger crystals of the same composition demonstrate an unambiguous excitonic state. We conclude that fabrication procedures and morphology strongly influence perovskite behaviour, with both free carrier and excitonic regimes possible, with strong implications for optoelectronic devices.",
author = "Giulia Grancini and {Srimath Kandada}, {Ajay Ram} and Frost, {Jarvist M.} and Barker, {Alex J.} and {De Bastiani}, Michele and Marina Gandini and Sergio Marras and Guglielmo Lanzani and Aron Walsh and Annamaria Petrozza",
year = "2015",
month = "10",
doi = "10.1038/nphoton.2015.151",
language = "English",
volume = "9",
pages = "695--701",
journal = "Nature Photonics",
issn = "1749-4885",
publisher = "Nature Research",

}

TY - JOUR

T1 - Role of microstructure in the electron–hole interaction of hybrid lead halide perovskites

AU - Grancini, Giulia

AU - Srimath Kandada, Ajay Ram

AU - Frost, Jarvist M.

AU - Barker, Alex J.

AU - De Bastiani, Michele

AU - Gandini, Marina

AU - Marras, Sergio

AU - Lanzani, Guglielmo

AU - Walsh, Aron

AU - Petrozza, Annamaria

PY - 2015/10

Y1 - 2015/10

N2 - Organic–inorganic metal halide perovskites have demonstrated high power conversion efficiencies in solar cells and promising performance in a wide range of optoelectronic devices. The existence and stability of bound electron–hole pairs in these materials and their role in the operation of devices with different architectures remains a controversial issue. Here we demonstrate, through a combination of optical spectroscopy and multiscale modelling as a function of the degree of polycrystallinity and temperature, that the electron–hole interaction is sensitive to the microstructure of the material. The long-range order is disrupted by polycrystalline disorder and the variations in electrostatic potential found for smaller crystals suppress exciton formation, while larger crystals of the same composition demonstrate an unambiguous excitonic state. We conclude that fabrication procedures and morphology strongly influence perovskite behaviour, with both free carrier and excitonic regimes possible, with strong implications for optoelectronic devices.

AB - Organic–inorganic metal halide perovskites have demonstrated high power conversion efficiencies in solar cells and promising performance in a wide range of optoelectronic devices. The existence and stability of bound electron–hole pairs in these materials and their role in the operation of devices with different architectures remains a controversial issue. Here we demonstrate, through a combination of optical spectroscopy and multiscale modelling as a function of the degree of polycrystallinity and temperature, that the electron–hole interaction is sensitive to the microstructure of the material. The long-range order is disrupted by polycrystalline disorder and the variations in electrostatic potential found for smaller crystals suppress exciton formation, while larger crystals of the same composition demonstrate an unambiguous excitonic state. We conclude that fabrication procedures and morphology strongly influence perovskite behaviour, with both free carrier and excitonic regimes possible, with strong implications for optoelectronic devices.

UR - http://dx.doi.org/10.1038/nphoton.2015.151

UR - http://www.nature.com/doifinder/10.1038/nphoton.2015.151

U2 - 10.1038/nphoton.2015.151

DO - 10.1038/nphoton.2015.151

M3 - Article

VL - 9

SP - 695

EP - 701

JO - Nature Photonics

JF - Nature Photonics

SN - 1749-4885

ER -