Imperial College London
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ProfessorAronWalsh

Faculty of Engineering, Department of Materials

Chair in Materials Design
 
 
 
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Contact

 

+44 (0)20 7594 1178a.walsh Website

 
 
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Location

 

2.10Royal School of MinesSouth Kensington Campus

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Summary

 

Publications

Citation

BibTex format

@article{Li:2020:10.1039/D0TA07145E,
author = {Li, Z and Kavanagh, S and Napari, M and Palgrave, RG and Abdi-Jalebi, M and Andaji-Garmaroudi, Z and Davies, DW and Laitinen, M and Julin, J and Isaacs, MA and Friend, RH and Scanlon, DO and Walsh, A and Hoye, R},
doi = {10.1039/D0TA07145E},
journal = {Journal of Materials Chemistry A},
pages = {21780--21788},
title = {Bandgap lowering in mixed alloys ofCs2Ag(SbxBi1-x)Br6 double perovskite thin films},
url = {http://dx.doi.org/10.1039/D0TA07145E},
volume = {8},
year = {2020}
}
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RIS format (EndNote, RefMan)

TY  - JOUR
AB  - Halide double perovskites have gained significant attention, owing to their composition of low-toxicity elements, stability in air and long charge-carrier lifetimes. However, most double perovskites, including Cs2AgBiBr6, have wide bandgaps, which limits photoconversion efficiencies. The bandgap can be reduced through alloying with Sb3+, but Sb-rich alloys are difficult to synthesize due to the high formation energy of Cs2AgSbBr6, which itself has a wide bandgap. We develop a solution-based route to synthesize phase-pure Cs2Ag(SbxBi1−x)Br6 thin films, with the mixing parameter x continuously varying over the entire composition range. We reveal that the mixed alloys (x between 0.5 and 0.9) demonstrate smaller bandgaps than the pure Sb- and Bi-based compounds. The reduction in the bandgap of Cs2AgBiBr6 achieved through alloying (170 meV) is larger than if the mixed alloys had obeyed Vegard's law (70 meV). Through in-depth computations, we propose that bandgap lowering arises from the type II band alignment between Cs2AgBiBr6 and Cs2AgSbBr6. The energy mismatch between the Bi and Sb s and p atomic orbitals, coupled with their non-linear mixing, results in the alloys adopting a smaller bandgap than the pure compounds. Our work demonstrates an approach to achieve bandgap reduction and highlights that bandgap bowing may be found in other double perovskite alloys by pairing together materials forming a type II band alignment.
AU  - Li,Z
AU  - Kavanagh,S
AU  - Napari,M
AU  - Palgrave,RG
AU  - Abdi-Jalebi,M
AU  - Andaji-Garmaroudi,Z
AU  - Davies,DW
AU  - Laitinen,M
AU  - Julin,J
AU  - Isaacs,MA
AU  - Friend,RH
AU  - Scanlon,DO
AU  - Walsh,A
AU  - Hoye,R
DO  - 10.1039/D0TA07145E
EP  - 21788
PY  - 2020///
SN  - 2050-7488
SP  - 21780
TI  - Bandgap lowering in mixed alloys ofCs2Ag(SbxBi1-x)Br6 double perovskite thin films
T2  - Journal of Materials Chemistry A
UR  - http://dx.doi.org/10.1039/D0TA07145E
UR  - http://hdl.handle.net/10044/1/84697
VL  - 8
ER  -
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