Effect of sub-bandgap defects on radiative and non-radiative open-circuit voltage losses in perovskite solar cells

Guus J.W. Aalbers; Tom P.A. van der Pol; Kunal Datta; Willemijn H.M. Remmerswaal; Martijn M. Wienk; René A.J. Janssen

doi:10.1038/s41467-024-45512-8

Effect of sub-bandgap defects on radiative and non-radiative open-circuit voltage losses in perovskite solar cells

Guus J.W. Aalbers, Tom P.A. van der Pol, Kunal Datta, Willemijn H.M. Remmerswaal, Martijn M. Wienk, René A.J. Janssen (Corresponding author)

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Abstract

The efficiency of perovskite solar cells is affected by open-circuit voltage losses due to radiative and non-radiative charge recombination. When estimated using sensitive photocurrent measurements that cover the above- and sub-bandgap regions, the radiative open-circuit voltage is often unphysically low. Here we report sensitive photocurrent and electroluminescence spectroscopy to probe radiative recombination at sub-bandgap defects in wide-bandgap mixed-halide lead perovskite solar cells. The radiative ideality factor associated with the optical transitions increases from 1, above and near the bandgap edge, to ~2 at mid-bandgap. Such photon energy-dependent ideality factor corresponds to a many-diode model. The radiative open-circuit voltage limit derived from this many-diode model enables differentiating between radiative and non-radiative voltage losses. The latter are deconvoluted into contributions from the bulk and interfaces via determining the quasi-Fermi level splitting. The experiments show that while sub-bandgap defects do not contribute to radiative voltage loss, they do affect non-radiative voltage losses.

Original language	English
Article number	1276
Number of pages	10
Journal	Nature Communications
Volume	15
Issue number	1
DOIs	https://doi.org/10.1038/s41467-024-45512-8
Publication status	Published - 10 Feb 2024

Bibliographical note

Publisher Copyright:
© 2024. The Author(s).

Funding

The authors are grateful for fruitful discussions with Thomas Kirchartz (Forschungszentrum Jülich, Germany) regarding the radiative ideality factor. We acknowledge funding from the Netherlands Ministry of Education, Culture, and Science (Gravity program 024.001.035) (T.P.A.v.d.P., R.A.J.J.) and the Netherlands Organization for Scientific Research (NWO) for funding through the Joint Solar Programme III (project 680.91.011) (K.D., R.A.J.J.) and the Spinoza prize (G.J.W.A., W.H.M.R., M.M.W., R.A.J.J.).

Funders	Funder number
Ministerie van Onderwijs, Cultuur en Wetenschap	024.001.035
Nederlandse Organisatie voor Wetenschappelijk Onderzoek	680.91.011

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title = "Effect of sub-bandgap defects on radiative and non-radiative open-circuit voltage losses in perovskite solar cells",

abstract = "The efficiency of perovskite solar cells is affected by open-circuit voltage losses due to radiative and non-radiative charge recombination. When estimated using sensitive photocurrent measurements that cover the above- and sub-bandgap regions, the radiative open-circuit voltage is often unphysically low. Here we report sensitive photocurrent and electroluminescence spectroscopy to probe radiative recombination at sub-bandgap defects in wide-bandgap mixed-halide lead perovskite solar cells. The radiative ideality factor associated with the optical transitions increases from 1, above and near the bandgap edge, to \textasciitilde{}2 at mid-bandgap. Such photon energy-dependent ideality factor corresponds to a many-diode model. The radiative open-circuit voltage limit derived from this many-diode model enables differentiating between radiative and non-radiative voltage losses. The latter are deconvoluted into contributions from the bulk and interfaces via determining the quasi-Fermi level splitting. The experiments show that while sub-bandgap defects do not contribute to radiative voltage loss, they do affect non-radiative voltage losses.",

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AU - Aalbers, Guus J.W.

AU - van der Pol, Tom P.A.

AU - Datta, Kunal

AU - Remmerswaal, Willemijn H.M.

AU - Wienk, Martijn M.

AU - Janssen, René A.J.

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N2 - The efficiency of perovskite solar cells is affected by open-circuit voltage losses due to radiative and non-radiative charge recombination. When estimated using sensitive photocurrent measurements that cover the above- and sub-bandgap regions, the radiative open-circuit voltage is often unphysically low. Here we report sensitive photocurrent and electroluminescence spectroscopy to probe radiative recombination at sub-bandgap defects in wide-bandgap mixed-halide lead perovskite solar cells. The radiative ideality factor associated with the optical transitions increases from 1, above and near the bandgap edge, to ~2 at mid-bandgap. Such photon energy-dependent ideality factor corresponds to a many-diode model. The radiative open-circuit voltage limit derived from this many-diode model enables differentiating between radiative and non-radiative voltage losses. The latter are deconvoluted into contributions from the bulk and interfaces via determining the quasi-Fermi level splitting. The experiments show that while sub-bandgap defects do not contribute to radiative voltage loss, they do affect non-radiative voltage losses.

AB - The efficiency of perovskite solar cells is affected by open-circuit voltage losses due to radiative and non-radiative charge recombination. When estimated using sensitive photocurrent measurements that cover the above- and sub-bandgap regions, the radiative open-circuit voltage is often unphysically low. Here we report sensitive photocurrent and electroluminescence spectroscopy to probe radiative recombination at sub-bandgap defects in wide-bandgap mixed-halide lead perovskite solar cells. The radiative ideality factor associated with the optical transitions increases from 1, above and near the bandgap edge, to ~2 at mid-bandgap. Such photon energy-dependent ideality factor corresponds to a many-diode model. The radiative open-circuit voltage limit derived from this many-diode model enables differentiating between radiative and non-radiative voltage losses. The latter are deconvoluted into contributions from the bulk and interfaces via determining the quasi-Fermi level splitting. The experiments show that while sub-bandgap defects do not contribute to radiative voltage loss, they do affect non-radiative voltage losses.

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Effect of sub-bandgap defects on radiative and non-radiative open-circuit voltage losses in perovskite solar cells

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