TY - JOUR
T1 - Systematic Band Gap Tuning of BaSnO3 via Chemical Substitutions
T2 - The Role of Clustering in Mixed-Valence Perovskites
AU - Lee, Seunghun
AU - Wang, Haihang
AU - Gopal, Priya
AU - Shin, Jongmoon
AU - Jaim, H. M.Iftekhar
AU - Zhang, Xiaohang
AU - Jeong, Se Young
AU - Usanmaz, Demet
AU - Curtarolo, Stefano
AU - Fornari, Marco
AU - Buongiorno Nardelli, Marco
AU - Takeuchi, Ichiro
N1 - Funding Information:
We are grateful to the High Performance Computing Center at Michigan State University, the Texas Advanced Computing Center at the University of Texas at Austin, and the Duke Center for Materials Genomics. The members of the AFLOW Consortium (http://www.aflow.org) acknowledge support by DOD-ONR (N00014-13-1-0635, N00014-11-1-0136, and N00014-15-1-2863). The work was also supported by AFOSR (Grant FA9550-14-10332).
Publisher Copyright:
© 2017 American Chemical Society.
PY - 2017/11/14
Y1 - 2017/11/14
N2 - By combining high-throughput experiments and first-principles calculations based on the DFT-ACBN0 approach, we have investigated the energy band gap of Sr-, Pb-, and Bi-substituted BaSnO3 over wide concentration ranges. We show that the band gap energy can be tuned from 3 to 4 eV by chemical substitution. Our work indicates the importance of considering the mixed-valence nature and clustering effects upon substitution of BaSnO3 with Pb and Bi. Starting from the band gap of ?3.4 eV for pure BaSnO3, we find that Pb substitution changes the gap in a nonmonotonic fashion, reducing it by as much as 0.3 eV. Bi substitution provides a monotonic reduction but introduces electronic states into the energy gap due to Bi clustering. Our findings provide new insight into the ubiquitous phenomena of chemical substitutions in perovskite semiconductors with mixed-valence cations that underpin their physical properties.
AB - By combining high-throughput experiments and first-principles calculations based on the DFT-ACBN0 approach, we have investigated the energy band gap of Sr-, Pb-, and Bi-substituted BaSnO3 over wide concentration ranges. We show that the band gap energy can be tuned from 3 to 4 eV by chemical substitution. Our work indicates the importance of considering the mixed-valence nature and clustering effects upon substitution of BaSnO3 with Pb and Bi. Starting from the band gap of ?3.4 eV for pure BaSnO3, we find that Pb substitution changes the gap in a nonmonotonic fashion, reducing it by as much as 0.3 eV. Bi substitution provides a monotonic reduction but introduces electronic states into the energy gap due to Bi clustering. Our findings provide new insight into the ubiquitous phenomena of chemical substitutions in perovskite semiconductors with mixed-valence cations that underpin their physical properties.
UR - http://www.scopus.com/inward/record.url?scp=85034073748&partnerID=8YFLogxK
U2 - 10.1021/acs.chemmater.7b03381
DO - 10.1021/acs.chemmater.7b03381
M3 - Article
AN - SCOPUS:85034073748
VL - 29
SP - 9378
EP - 9385
JO - Chemistry of Materials
JF - Chemistry of Materials
SN - 0897-4756
IS - 21
ER -