journal article·2016-07-12Open access

Lone-Pair Stabilization in Transparent Amorphous Tin Oxides: A Potential Route to p-Type Conduction Pathways

Matthew J. Wahila, Keith T. Butler, Zachary W. Lebens-Higgins, Christopher H. Hendon, Abhishek S. Nandur, Robert E. Treharne, Nicholas F. Quackenbush, Shawn Sallis, Katie Mason, Hanjong Paik, Darrell G. Schlom, Joseph C. Woicik, Jinghua Guo, Dario A. Arena, Bruce E. White, Graeme W. Watson, Aron Walsh, Louis F. J. Piper

Chemistry of Materials· Volume 28· Issue 13

Abstract

The electronic and atomic structures of amorphous transparent tin oxides have been investigated by a combination of X-ray spectroscopy and atomistic calculations. Crystalline SnO is a promising p-type transparent oxide semiconductor due to a complex lone-pair hybridization that affords both optical transparency despite a small electronic band gap and spherical s-orbital character at the valence band edge. We find that both of these desirable properties (transparency and s-orbital valence band character) are retained upon amorphization despite the disruption of the layered lone-pair states by structural disorder. We explain the anomalously large band gap widening necessary to maintain transparency in terms of lone-pair stabilization via atomic clustering. Our understanding of this mechanism suggests that continuous hole conduction pathways along extended lone pair clusters should be possible under certain stoichiometries. Moreover, these findings should be applicable to other lone-pair active semiconductors.
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Research context

OpenAlex topics: ZnO doping and properties · Transition Metal Oxide Nanomaterials · Thin-Film Transistor Technologies

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Department of Physics, Applied Physics and Astronomy, Binghamton University, Binghamton, New York 13902, United States

Department of Chemistry, University of Bath, Claverton Down, Bath BA2 7AY, United Kingdom

Materials Science and Engineering, Binghamton University, Binghamton, New York 13902, United States

Stephenson Institute for Renewable Energy, University of Liverpool, Liverpool, L69 7ZF, United Kingdom

Department of Materials Science and Engineering, Cornell University, Ithaca, New York 14853-1501, United States

Kavli Institute at Cornell for Nanoscale Science, Ithaca, New York 14853, United States

Materials Science and Engineering Laboratory, National Institute of Standards and Technology, Gaithersburg, Maryland 20899, United States

Advanced Light Source, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States

National Synchrotron Light Source-II, Basic Energy Sciences Directorate, Brookhaven National Laboratory, Upton, New York 11973, United States

School of Chemistry and CRANN, Trinity College Dublin, Dublin 2, Ireland

Funding

Engineering and Physical Sciences Research Council · Defense Advanced Research Projects Agency · Science Foundation Ireland · Microelectronics Advanced Research Corporation · Division of Materials Research

References (49)

Show source-provided references
1. 10.1088/0953-8984/18/43/R0110.1088/0953-8984/18/43/R01 ↗
2. 10.1103/PhysRevB.80.08520210.1103/PhysRevB.80.085202 ↗
3. 10.1038/nature0309010.1038/nature03090 ↗
4. 10.1103/PhysRevB.83.07520510.1103/PhysRevB.83.075205 ↗
5. 10.1016/S0921-4526(01)00417-310.1016/S0921-4526(01)00417-3 ↗
6. 10.1039/c2jm34352e10.1039/c2jm34352e ↗
7. 10.1038/4008710.1038/40087 ↗
8. 10.1021/jz101172510.1021/jz1011725 ↗
9. 10.1016/0022-3697(84)90101-X10.1016/0022-3697(84)90101-X ↗
10. 10.1002/adma.20030494710.1002/adma.200304947 ↗
11. 10.1002/aelm.20140002310.1002/aelm.201400023 ↗
12. 10.1109/LED.2012.218763310.1109/LED.2012.2187633 ↗
13. 10.1063/1.486164810.1063/1.4861648 ↗
14. 10.1021/jp205148y10.1021/jp205148y ↗
15. 10.1039/c3tc31863j10.1039/c3tc31863j ↗
16. 10.1103/PhysRevB.70.23511410.1103/PhysRevB.70.235114 ↗
17. 10.1021/jp051822r10.1021/jp051822r ↗
18. 10.1039/c1cs15098g10.1039/c1cs15098g ↗
19. 10.1063/1.133110210.1063/1.1331102 ↗
20. 10.1002/aelm.20150045310.1002/aelm.201500453 ↗
21. 10.1021/cm401343a10.1021/cm401343a ↗
22. 10.1002/pssa.20088179210.1002/pssa.200881792 ↗
23. 10.1063/1.327715310.1063/1.3277153 ↗
24. 10.1063/1.488325710.1063/1.4883257 ↗
25. 10.1002/pssa.20143180610.1002/pssa.201431806 ↗
26. 10.1002/pssa.20143187110.1002/pssa.201431871 ↗
27. 10.1002/adma.20110322810.1002/adma.201103228 ↗
28. 10.1002/pssr.20151001610.1002/pssr.201510016 ↗
29. Mott, N. F.Oxford science publications;Conduction in Non-Crystalline MaterialsOxford science publications; 1987.
30. 10.1002/aenm.20150119010.1002/aenm.201501190 ↗
31. 10.1016/j.susc.2006.01.15010.1016/j.susc.2006.01.150 ↗
32. Scofield J. H. · 197310.2172/4545040 ↗
33. 10.1016/j.tsf.2013.05.14610.1016/j.tsf.2013.05.146 ↗
34. 10.1063/1.481598410.1063/1.4815984 ↗
35. 10.1039/C5CP02255J10.1039/C5CP02255J ↗
36. 10.1021/cm502689x10.1021/cm502689x ↗
37. 10.1038/nmat379010.1038/nmat3790 ↗
38. Elschner A. · 201010.1201/b10318 ↗
39. 10.1103/PhysRevB.86.15531910.1103/PhysRevB.86.155319 ↗
40. 10.1103/PhysRevB.91.20530710.1103/PhysRevB.91.205307 ↗
41. 10.1116/1.57986810.1116/1.579868 ↗
42. 10.1103/PhysRevB.54.1116910.1103/PhysRevB.54.11169 ↗
43. 10.1103/PhysRevB.50.1795310.1103/PhysRevB.50.17953 ↗
44. 10.1103/PhysRevB.59.175810.1103/PhysRevB.59.1758 ↗
45. 10.1103/PhysRevLett.100.13640610.1103/PhysRevLett.100.136406 ↗
46. 10.1063/1.367006810.1063/1.3670068 ↗
47. 10.1103/PhysRevB.45.1389110.1103/PhysRevB.45.13891 ↗
48. 10.1063/1.240466310.1063/1.2404663 ↗
49. 10.1016/j.commatsci.2010.04.02310.1016/j.commatsci.2010.04.023 ↗