hybrid perovskite; photovoltaics; metavalent bonding; mvb; halide perovskite; ab initio
Abstract :
[en] Abstract Outstanding photovoltaic (PV) materials combine a set of advantageous properties including large optical absorption and high charge carrier mobility, facilitated by small effective masses. Halide perovskites (ABX3, where X = I, Br, or Cl) are among the most promising PV materials. Their optoelectronic properties are governed by the BX bond, which is responsible for the pronounced optical absorption and the small effective masses of the charge carriers. These properties are frequently attributed to the ns2 configuration of the B atom, i.e., Pb 6s2 or Sn 5s2 (“lone-pair”) states. The analysis of the PV properties in conjunction with a quantum-chemical bond analysis reveals a different scenario. The BX bond differs significantly from ionic, metallic, or conventional 2c2e covalent bonds. Instead it is better regarded as metavalent, since it shares about one p-electron between adjacent atoms. The resulting σ-bond, formally a 2c1e bond, is half-filled, causing pronounced optical absorption. Electron transfer between B and X atoms and lattice distortions open a moderate bandgap resulting in charge carriers with small effective masses. Hence, metavalent bonding explains favorable PV properties of halide perovskites, as summarized in a map for different bond types, which provides a blueprint to design PV materials.
Disciplines :
Physics
Author, co-author :
Wuttig, Matthias
Schön, Carl-Friedrich
Schumacher, Mathias
Robertson, John
Golub, Pavlo
Bousquet, Eric ; Université de Liège - ULiège > Département de physique > Physique théorique des matériaux
Gatti, Carlo
Raty, Jean-Yves ; Université de Liège - ULiège > Département de physique > Physique des solides, interfaces et nanostructures
Language :
English
Title :
Halide Perovskites: Advanced Photovoltaic Materials Empowered by a Unique Bonding Mechanism
Publication date :
2022
Journal title :
Advanced Functional Materials
ISSN :
1616-301X
eISSN :
1616-3028
Publisher :
John Wiley & Sons, United Kingdom
Volume :
32
Issue :
2
Pages :
2110166
Peer reviewed :
Peer Reviewed verified by ORBi
Tags :
Tier-1 supercomputer CÉCI : Consortium des Équipements de Calcul Intensif
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