TY - JOUR
T1 - The Role of Cation Coordination in the Electrical and Optical Properties of Amorphous Transparent Conducting Oxides
AU - Husein, Sebastian
AU - Medvedeva, Julia E.
AU - Perkins, John D.
AU - Bertoni, Mariana I.
N1 - Funding Information:
This material is based on work partially supported by the National Science Foundation and the Department of Energy under NSF CA no. EEC-1041895. J.E.M. acknowledges the support of NSF-DMREF grant DMR-1729779 as well as NSF-supported XSEDE for computer allocation. Any opinions, findings, and conclusions or recommendations expressed in this material are those of the author(s) and do not necessarily reflect those of the National Science Foundation or the Department of Energy. The authors acknowledge the use of facilities within the Eyring Materials Center at Arizona State University supported in part by NNCI-ECCS-1542160 and the Michigan Ion Beam Laboratory.
Publisher Copyright:
Copyright © 2020 American Chemical Society.
PY - 2020/8/11
Y1 - 2020/8/11
N2 - Amorphous oxide semiconductor materials have demonstrated numerous advantages without compromise of electrical properties as compared to their crystalline counterparts, yet understanding of the fundamental principles allowing this has remained elusive. To study the origins of enhanced optoelectronic properties, we apply high-throughput, combinatorial sputtering, structural and spectral mapping, and computationally intensive ab initio molecular dynamics simulations with density functional theory to a ternary, post-transition metal oxide system, namely, zinc tin oxide. The deposited thin films exhibit a high figure of merit, achieving carrier densities in the range of 1019 to 1020 cm-3 and carrier mobilities up to 35 cm2/Vs. These results highlight the role of local distortions and cation coordination in determining the microscopic origins of carrier generation and transport. In particular, we identify the strong likelihood of Sn undercoordination in both Zn-poor and Zn-rich phases leading to the high carrier concentrations observed. This not only diverges from the still widespread historical indictment of oxygen vacancies controlling carrier population in crystalline oxides but also provides a comprehensive framework to describe the unique structure-property relationships using specific structural and electronic descriptors in disordered phase materials.
AB - Amorphous oxide semiconductor materials have demonstrated numerous advantages without compromise of electrical properties as compared to their crystalline counterparts, yet understanding of the fundamental principles allowing this has remained elusive. To study the origins of enhanced optoelectronic properties, we apply high-throughput, combinatorial sputtering, structural and spectral mapping, and computationally intensive ab initio molecular dynamics simulations with density functional theory to a ternary, post-transition metal oxide system, namely, zinc tin oxide. The deposited thin films exhibit a high figure of merit, achieving carrier densities in the range of 1019 to 1020 cm-3 and carrier mobilities up to 35 cm2/Vs. These results highlight the role of local distortions and cation coordination in determining the microscopic origins of carrier generation and transport. In particular, we identify the strong likelihood of Sn undercoordination in both Zn-poor and Zn-rich phases leading to the high carrier concentrations observed. This not only diverges from the still widespread historical indictment of oxygen vacancies controlling carrier population in crystalline oxides but also provides a comprehensive framework to describe the unique structure-property relationships using specific structural and electronic descriptors in disordered phase materials.
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U2 - 10.1021/acs.chemmater.0c01672
DO - 10.1021/acs.chemmater.0c01672
M3 - Article
AN - SCOPUS:85092075657
SN - 0897-4756
VL - 32
SP - 6444
EP - 6455
JO - Chemistry of Materials
JF - Chemistry of Materials
IS - 15
ER -