TY - JOUR
T1 - Massive band gap variation in layered oxides through cation ordering
AU - Balachandran, Prasanna V.
AU - Rondinelli, James M.
N1 - Funding Information:
P.V.B. and J.M.R. acknowledge support from DARPA (grant no. N66001-12-1-4224). P.V.B. acknowledges discussions with Dr A. Saxena, J. Young and N. Charles. We thank Professor S. Halasyamani, Professor B. Nelson-Cheeseman, Dr A. Bhattacharya and Dr J. Íñiguez for insightful conversations, and gratefully thank Professor L.D. Marks for performing the Wien2k calculations. P.V.B. and J.M.R. acknowledge the help of Dr J. Deslippe and Dr D. Strubbe with the BerkeleyGW code. The computational work made use of the GARNET and SPIRIT clusters at the ERDC and AFRL HPC resources, respectively, under the HPCMP initiative, and facilities available at the Center for Nanoscale Materials (CARBON Cluster) at Argonne National Laboratory, supported by the U.S. DOE, Office of Basic Energy Sciences (BES), DE-AC02-06CH11357. The views, opinions and/or findings reported here are solely those of the authors and do not represent any official views of DARPA.
Publisher Copyright:
© 2015 Macmillan Publishers Limited. All rights reserved.
PY - 2015/1/30
Y1 - 2015/1/30
N2 - The electronic band gap is a fundamental material parameter requiring control for light harvesting, conversion and transport technologies, including photovoltaics, lasers and sensors. Although traditional methods to tune band gaps rely on chemical alloying, quantum size effects, lattice mismatch or superlattice formation, the spectral variation is often limited to <1eV, unless marked changes to composition or structure occur. Here we report large band gap changes of up to 200% or ∼2eV without modifying chemical composition or use of epitaxial strain in the LaSrAlO4 Ruddlesden-Popper oxide. First-principles calculations show that ordering electrically charged [LaO]1+ and neutral [SrO]0 monoxide planes imposes internal electric fields in the layered oxides. These fields drive local atomic displacements and bond distortions that control the energy levels at the valence and conduction band edges, providing a path towards electronic structure engineering in complex oxides.
AB - The electronic band gap is a fundamental material parameter requiring control for light harvesting, conversion and transport technologies, including photovoltaics, lasers and sensors. Although traditional methods to tune band gaps rely on chemical alloying, quantum size effects, lattice mismatch or superlattice formation, the spectral variation is often limited to <1eV, unless marked changes to composition or structure occur. Here we report large band gap changes of up to 200% or ∼2eV without modifying chemical composition or use of epitaxial strain in the LaSrAlO4 Ruddlesden-Popper oxide. First-principles calculations show that ordering electrically charged [LaO]1+ and neutral [SrO]0 monoxide planes imposes internal electric fields in the layered oxides. These fields drive local atomic displacements and bond distortions that control the energy levels at the valence and conduction band edges, providing a path towards electronic structure engineering in complex oxides.
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U2 - 10.1038/ncomms7191
DO - 10.1038/ncomms7191
M3 - Article
C2 - 25635516
AN - SCOPUS:84929990368
SN - 2041-1723
VL - 6
JO - Nature Communications
JF - Nature Communications
M1 - 6191
ER -