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Title: Deep level defects and cation sublattice disorder in ZnGeN2

Abstract

The III-nitrides have revolutionized lighting technology and power electronics. Expanding the nitride semiconductor family to include the heterovalent ternary nitrides opens up new and exciting opportunities for device design that may help overcome some of the limitations of the binary nitrides as well as new applications. However, the more complex cation sublattice also gives rise to new complexities with both native and extrinsic defects, such as disorder on the cation sublattice. Here, depth-resolved cathodoluminescence spectroscopy and surface photovoltage spectroscopy measurements of defect energy levels in ZnGeN2 combined with transmission microscopy and crystal lattice diffraction reveal optical signatures of mid-gap states that can be associated with cation sublattice disorder. The energies of these characteristic optical signatures in ZnGeN2 thin films grown by metal-organic chemical vapor deposition are in good agreement with energy levels predicted by density functional theory for specific thermodynamically stable native point defects. To test the dependence of these defect signatures on crystal atomic composition, we correlated spatially-resolved optical and atomic composition measurements using spatially resolved x-ray photoelectron spectroscopy with systematically varied growth conditions on the same ZnGeN2 films. The resultant elemental maps versus defect spectral energies and intensities suggest that cation antisite complexes (ZnGe-GeZn) versus isolated native pointmore » defects form preferentially and introduce mid-gap states that dominate electron-hole pair recombination. Complexing of ZnGe and GeZn antisites manifests as disorder in the cation sub-lattice and leads to the formation of wurtzitic ZnGeN2 as indicated by transmission electron microscopy diffraction patterns and x-ray diffraction (XRD) reciprocal space maps. Furthermore, these findings emphasize the importance of growth conditions to control cation place exchange.« less

Authors:
ORCiD logo [1]; ORCiD logo [1];  [1];  [1];  [2]; ORCiD logo [3]; ORCiD logo [3];  [1];  [1]; ORCiD logo [3]; ORCiD logo [1]; ORCiD logo [1]
  1. Ohio State University, Columbus, OH (United States)
  2. Columbus School for Girls, Columbus, OH (United States)
  3. Case Western Reserve University, Cleveland, OH (United States)
Publication Date:
Research Org.:
The Ohio State Univ., Columbus, OH (United States); Case Western Reserve Univ., Cleveland, OH (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE); National Science Foundation (NSF)
Contributing Org.:
Case Western Reserve University
OSTI Identifier:
1677498
Grant/Contract Number:  
EE0008718; DMREF:SusChEM:-1533957; DMR-18-00130; DMR-14-20451
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Applied Physics
Additional Journal Information:
Journal Volume: 127; Journal Issue: 13; Journal ID: ISSN 0021-8979
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
42 ENGINEERING; Depth-resolved cathodoluminescence spectroscopy; Transmission electron microscopy; Chemical vapor deposition; X-ray photoelectron spectroscopy; Power electronics; Thin films; Density functional theory; Crystal lattices; Crystallographic defects; X-ray diffraction

Citation Formats

Haseman, Micah S., Karim, Md Rezaul, Ramdin, Daram, Noesges, Brenton A., Feinberg, Ella, Jayatunga, Benthara Hewage Dinushi, Lambrecht, Walter R. L., Zhu, Menglin, Hwang, Jinwoo, Kash, Kathleen, Zhao, Hongping, and Brillson, Leonard J.. Deep level defects and cation sublattice disorder in ZnGeN2. United States: N. p., 2020. Web. https://doi.org/10.1063/1.5141335.
Haseman, Micah S., Karim, Md Rezaul, Ramdin, Daram, Noesges, Brenton A., Feinberg, Ella, Jayatunga, Benthara Hewage Dinushi, Lambrecht, Walter R. L., Zhu, Menglin, Hwang, Jinwoo, Kash, Kathleen, Zhao, Hongping, & Brillson, Leonard J.. Deep level defects and cation sublattice disorder in ZnGeN2. United States. https://doi.org/10.1063/1.5141335
Haseman, Micah S., Karim, Md Rezaul, Ramdin, Daram, Noesges, Brenton A., Feinberg, Ella, Jayatunga, Benthara Hewage Dinushi, Lambrecht, Walter R. L., Zhu, Menglin, Hwang, Jinwoo, Kash, Kathleen, Zhao, Hongping, and Brillson, Leonard J.. Fri . "Deep level defects and cation sublattice disorder in ZnGeN2". United States. https://doi.org/10.1063/1.5141335. https://www.osti.gov/servlets/purl/1677498.
@article{osti_1677498,
title = {Deep level defects and cation sublattice disorder in ZnGeN2},
author = {Haseman, Micah S. and Karim, Md Rezaul and Ramdin, Daram and Noesges, Brenton A. and Feinberg, Ella and Jayatunga, Benthara Hewage Dinushi and Lambrecht, Walter R. L. and Zhu, Menglin and Hwang, Jinwoo and Kash, Kathleen and Zhao, Hongping and Brillson, Leonard J.},
abstractNote = {The III-nitrides have revolutionized lighting technology and power electronics. Expanding the nitride semiconductor family to include the heterovalent ternary nitrides opens up new and exciting opportunities for device design that may help overcome some of the limitations of the binary nitrides as well as new applications. However, the more complex cation sublattice also gives rise to new complexities with both native and extrinsic defects, such as disorder on the cation sublattice. Here, depth-resolved cathodoluminescence spectroscopy and surface photovoltage spectroscopy measurements of defect energy levels in ZnGeN2 combined with transmission microscopy and crystal lattice diffraction reveal optical signatures of mid-gap states that can be associated with cation sublattice disorder. The energies of these characteristic optical signatures in ZnGeN2 thin films grown by metal-organic chemical vapor deposition are in good agreement with energy levels predicted by density functional theory for specific thermodynamically stable native point defects. To test the dependence of these defect signatures on crystal atomic composition, we correlated spatially-resolved optical and atomic composition measurements using spatially resolved x-ray photoelectron spectroscopy with systematically varied growth conditions on the same ZnGeN2 films. The resultant elemental maps versus defect spectral energies and intensities suggest that cation antisite complexes (ZnGe-GeZn) versus isolated native point defects form preferentially and introduce mid-gap states that dominate electron-hole pair recombination. Complexing of ZnGe and GeZn antisites manifests as disorder in the cation sub-lattice and leads to the formation of wurtzitic ZnGeN2 as indicated by transmission electron microscopy diffraction patterns and x-ray diffraction (XRD) reciprocal space maps. Furthermore, these findings emphasize the importance of growth conditions to control cation place exchange.},
doi = {10.1063/1.5141335},
journal = {Journal of Applied Physics},
number = 13,
volume = 127,
place = {United States},
year = {2020},
month = {4}
}

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