skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Templated Growth of Metastable Polymorphs on Amorphous Substrates with Seed Layers

Abstract

Metastable inorganic materials with unique properties are vital in many practical applications, but their synthesis is often challenging. In physics, epitaxial stabilization, also known as pseudomorphic growth, is used to synthesize metastable polymorphs, but usually only as very thin films and on expensive single-crystal substrates. In chemistry, the templated growth of inorganic solid-state materials on self-assembled monolayers of organic molecules is reported. Bridging these two fields, here, we show that the synthesis of metastable polymorphs is possible up to large film thickness on amorphous substrates covered with thin inorganic seed layers that serve as templates. The stabilization of a 500-nm-thick metastable wurtzite (WZ) MnTe film by a 5-nm-thick ZnTe seed layer sputtered on amorphous glass substrates is experimentally demonstrated. Theoretical calculations explain this experimental observation by the small WZ polymorph energy relative to that of the ground-state nickeline (NC) structure of MnTe and a large lattice constant difference of the two. The resulting metastable WZ-MnTe polymorph exhibits a wide band gap of 2.7 eV and a low hole density of 10 12cm -3, which is relevant to optoelectronic applications. These properties are in sharp contrast to those of the narrow-band-gap highly doped NC-MnTe with 1.3 eV band gap and 10more » 19cm -3 hole density. The difference in hole density is due to the calculated difference in the formation energy of manganese vacancy acceptor defects. Overall, these results suggest that templated growth on amorphous substrates with seed layers can be used to synthesize metastable polymorphs of other materials, without the need for expensive single-crystal substrates.« less

Authors:
 [1];  [2];  [3];  [4];  [3];  [2]; ORCiD logo [3];  [5];  [6];  [7]; ORCiD logo [3]
  1. National Renewable Energy Lab. (NREL), Golden, CO (United States); Fudan Univ., Shanghai (China); ZhengZhou Univ. (China)
  2. Univ. of Colorado, Boulder, CO (United States)
  3. National Renewable Energy Lab. (NREL), Golden, CO (United States)
  4. National Renewable Energy Lab. (NREL), Golden, CO (United States); Oregon State Univ., Corvallis, OR (United States)
  5. Oregon State Univ., Corvallis, OR (United States)
  6. Fudan Univ., Shanghai (China)
  7. National Renewable Energy Lab. (NREL), Golden, CO (United States); Univ. of Colorado, Boulder, CO (United States)
Publication Date:
Research Org.:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1598128
Report Number(s):
NREL/JA-5K00-75602
Journal ID: ISSN 2331-7019; PRAHB2
Grant/Contract Number:  
AC36-08GO28308
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Physical Review Applied
Additional Journal Information:
Journal Volume: 13; Journal Issue: 1; Journal ID: ISSN 2331-7019
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; thin film sputtering; Hall effect measurement; metastable polymorph; wide-bandgap p-type semiconductors; first principles defect calculations; epitaxial growth; pseudomorphic stabilization

Citation Formats

Han, Yanbing, Trottier, Ryan, Siol, Sebastian, Matthews, Bethany, Young, Matthew R., Musgrave, Charles B., Lany, Stephan, Tate, Janet, Zhang, Qun, Holder, Aaron M, and Zakutayev, Andriy. Templated Growth of Metastable Polymorphs on Amorphous Substrates with Seed Layers. United States: N. p., 2020. Web. doi:10.1103/PhysRevApplied.13.014012.
Han, Yanbing, Trottier, Ryan, Siol, Sebastian, Matthews, Bethany, Young, Matthew R., Musgrave, Charles B., Lany, Stephan, Tate, Janet, Zhang, Qun, Holder, Aaron M, & Zakutayev, Andriy. Templated Growth of Metastable Polymorphs on Amorphous Substrates with Seed Layers. United States. https://doi.org/10.1103/PhysRevApplied.13.014012
Han, Yanbing, Trottier, Ryan, Siol, Sebastian, Matthews, Bethany, Young, Matthew R., Musgrave, Charles B., Lany, Stephan, Tate, Janet, Zhang, Qun, Holder, Aaron M, and Zakutayev, Andriy. Wed . "Templated Growth of Metastable Polymorphs on Amorphous Substrates with Seed Layers". United States. https://doi.org/10.1103/PhysRevApplied.13.014012. https://www.osti.gov/servlets/purl/1598128.
@article{osti_1598128,
title = {Templated Growth of Metastable Polymorphs on Amorphous Substrates with Seed Layers},
author = {Han, Yanbing and Trottier, Ryan and Siol, Sebastian and Matthews, Bethany and Young, Matthew R. and Musgrave, Charles B. and Lany, Stephan and Tate, Janet and Zhang, Qun and Holder, Aaron M and Zakutayev, Andriy},
abstractNote = {Metastable inorganic materials with unique properties are vital in many practical applications, but their synthesis is often challenging. In physics, epitaxial stabilization, also known as pseudomorphic growth, is used to synthesize metastable polymorphs, but usually only as very thin films and on expensive single-crystal substrates. In chemistry, the templated growth of inorganic solid-state materials on self-assembled monolayers of organic molecules is reported. Bridging these two fields, here, we show that the synthesis of metastable polymorphs is possible up to large film thickness on amorphous substrates covered with thin inorganic seed layers that serve as templates. The stabilization of a 500-nm-thick metastable wurtzite (WZ) MnTe film by a 5-nm-thick ZnTe seed layer sputtered on amorphous glass substrates is experimentally demonstrated. Theoretical calculations explain this experimental observation by the small WZ polymorph energy relative to that of the ground-state nickeline (NC) structure of MnTe and a large lattice constant difference of the two. The resulting metastable WZ-MnTe polymorph exhibits a wide band gap of 2.7 eV and a low hole density of 1012cm-3, which is relevant to optoelectronic applications. These properties are in sharp contrast to those of the narrow-band-gap highly doped NC-MnTe with 1.3 eV band gap and 1019cm-3 hole density. The difference in hole density is due to the calculated difference in the formation energy of manganese vacancy acceptor defects. Overall, these results suggest that templated growth on amorphous substrates with seed layers can be used to synthesize metastable polymorphs of other materials, without the need for expensive single-crystal substrates.},
doi = {10.1103/PhysRevApplied.13.014012},
url = {https://www.osti.gov/biblio/1598128}, journal = {Physical Review Applied},
issn = {2331-7019},
number = 1,
volume = 13,
place = {United States},
year = {2020},
month = {1}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Save / Share:

Works referenced in this record:

Wide-bandgap semiconductor ultraviolet photodetectors
journal, March 2003


Generalized Gradient Approximation Made Simple
journal, October 1996


A Thin Film Approach to Engineering Functionality into Oxides
journal, August 2008


Stabilization of wide band-gap p-type wurtzite MnTe thin films on amorphous substrates
journal, January 2018


Projector augmented-wave method
journal, December 1994


Templated growth of calcite, vaterite and aragonite crystals onself-assembled monolayers of substituted alkylthiols on gold
journal, January 1998


An open experimental database for exploring inorganic materials
journal, April 2018


p-type transparent conducting oxides
journal, June 2006


Defect Tolerant Semiconductors for Solar Energy Conversion
journal, March 2014


Role of substrate in the pseudomorphic stabilization of rocksalt-type AlN phase in AlN/TiN superlattices
journal, June 2002


Combinatorial Reactive Sputtering of In 2 S 3 as an Alternative Contact Layer for Thin Film Solar Cells
journal, May 2016


Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996


From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999


Combinatorial substrate epitaxy: a new approach to growth of complex metastable compounds
journal, January 2013


Negative-pressure polymorphs made by heterostructural alloying
journal, April 2018


Electron-energy-loss spectra and the structural stability of nickel oxide: An LSDA+U study
journal, January 1998


(Invited) Advances in Oxide Thin-Film Transistors in Recent Decade and Their Future
journal, May 2015


Identification and design principles of low hole effective mass p-type transparent conducting oxides
journal, August 2013


Zinc-Stabilized Manganese Telluride with Wurtzite Crystal Structure
journal, July 2018


Pseudomorphic stabilization of rocksalt GaN in TiN/GaN multilayers and superlattices
journal, July 2009


COMBIgor: Data-Analysis Package for Combinatorial Materials Science
journal, May 2019


Epitaxial Stabilization of Oxides in Thin Films
journal, October 2002


Template-directed nucleation and growth of inorganic materials
journal, January 1994


Growth and stability of zinc blende MgS on GaAs, GaP, and InP substrates
journal, January 2013


Metastable rocksalt ZnO is p -type dopable
journal, August 2018


Defects in Amorphous Semiconductors: The Case of Amorphous Indium Gallium Zinc Oxide
journal, May 2018


Strongly Constrained and Appropriately Normed Semilocal Density Functional
journal, July 2015


Strain Tuning of Ferroelectric Thin Films
journal, August 2007