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Title: Using Resonant Energy X-Ray Diffraction to Extract Chemical Order Parameters in Ternary Semiconductors

Abstract

II-IV-V2 materials, ternary analogs to III-V materials, are emerging for their potential applications in devices such as LEDs and solar cells. Controlling cation ordering in II-IV-V2 materials offers the potential to tune properties at nearly fixed compositions and lattice parameters. While tuning properties at a fixed lattice constant through ordering has the potential to be a powerful tool used in device fabrication, cation ordering also creates challenges with characterization and quantification of ordering. In this work, we investigate two different methods to quantify cation ordering in ZnGeP2 thin films: a stretching parameter calculated from lattice constants c/a, and an order parameter determined from the cation site occupancies (S). We use high resolution X-ray diffraction (HRXRD) to determine c/a and resonant energy X-ray diffraction (REXD) to extract S. REXD is critical to distinguish between elements with similar Z-number (e.g. Zn and Ge). We found that samples with a c/a corresponding to the ordered chalcopyrite structure had only partially ordered S values. The optical absorption onset for these films occurred at lower energy than expected for fully ordered ZnGeP2, indicating that S is a more accurate descriptor of cation order than the stretching parameter. Since disorder is complex and can occur onmore » many length scales, metrics for quantifying disorder should be chosen that most accurately reflect the physical properties of interest.« less

Authors:
 [1];  [2];  [1];  [3];  [1];  [4];  [4];  [4];  [1];  [1]
  1. National Renewable Energy Laboratory (NREL), Golden, CO (United States)
  2. SLAC National Accelerator Laboratory; Stanford University
  3. Colorado School of Mines
  4. SLAC National Accelerator Laboratory
Publication Date:
Research Org.:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1606128
Report Number(s):
NREL/JA-5K00-75485
DOE Contract Number:  
AC36-08GO28308
Resource Type:
Journal Article
Journal Name:
Journal of Materials Chemistry C
Additional Journal Information:
Journal Name: Journal of Materials Chemistry C
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; cation ordering; thin films; semiconductors

Citation Formats

Schnepf, Rekha, Levy-Wendt, Ben L., Tellekamp, Marshall B, Ortiz, Brenden R., Melamed, Celeste, Schelhas, Laura T., Stone, Kevin H., Toney, Michael F., Toberer, Eric, and Tamboli, Adele C. Using Resonant Energy X-Ray Diffraction to Extract Chemical Order Parameters in Ternary Semiconductors. United States: N. p., 2020. Web. doi:10.1039/C9TC06699C.
Schnepf, Rekha, Levy-Wendt, Ben L., Tellekamp, Marshall B, Ortiz, Brenden R., Melamed, Celeste, Schelhas, Laura T., Stone, Kevin H., Toney, Michael F., Toberer, Eric, & Tamboli, Adele C. Using Resonant Energy X-Ray Diffraction to Extract Chemical Order Parameters in Ternary Semiconductors. United States. doi:10.1039/C9TC06699C.
Schnepf, Rekha, Levy-Wendt, Ben L., Tellekamp, Marshall B, Ortiz, Brenden R., Melamed, Celeste, Schelhas, Laura T., Stone, Kevin H., Toney, Michael F., Toberer, Eric, and Tamboli, Adele C. Thu . "Using Resonant Energy X-Ray Diffraction to Extract Chemical Order Parameters in Ternary Semiconductors". United States. doi:10.1039/C9TC06699C.
@article{osti_1606128,
title = {Using Resonant Energy X-Ray Diffraction to Extract Chemical Order Parameters in Ternary Semiconductors},
author = {Schnepf, Rekha and Levy-Wendt, Ben L. and Tellekamp, Marshall B and Ortiz, Brenden R. and Melamed, Celeste and Schelhas, Laura T. and Stone, Kevin H. and Toney, Michael F. and Toberer, Eric and Tamboli, Adele C},
abstractNote = {II-IV-V2 materials, ternary analogs to III-V materials, are emerging for their potential applications in devices such as LEDs and solar cells. Controlling cation ordering in II-IV-V2 materials offers the potential to tune properties at nearly fixed compositions and lattice parameters. While tuning properties at a fixed lattice constant through ordering has the potential to be a powerful tool used in device fabrication, cation ordering also creates challenges with characterization and quantification of ordering. In this work, we investigate two different methods to quantify cation ordering in ZnGeP2 thin films: a stretching parameter calculated from lattice constants c/a, and an order parameter determined from the cation site occupancies (S). We use high resolution X-ray diffraction (HRXRD) to determine c/a and resonant energy X-ray diffraction (REXD) to extract S. REXD is critical to distinguish between elements with similar Z-number (e.g. Zn and Ge). We found that samples with a c/a corresponding to the ordered chalcopyrite structure had only partially ordered S values. The optical absorption onset for these films occurred at lower energy than expected for fully ordered ZnGeP2, indicating that S is a more accurate descriptor of cation order than the stretching parameter. Since disorder is complex and can occur on many length scales, metrics for quantifying disorder should be chosen that most accurately reflect the physical properties of interest.},
doi = {10.1039/C9TC06699C},
journal = {Journal of Materials Chemistry C},
number = ,
volume = ,
place = {United States},
year = {2020},
month = {3}
}

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