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Title: Novel phase diagram behavior and materials design in heterostructural semiconductor alloys

Structure and composition control the behavior of materials. Isostructural alloying is historically an extremely successful approach for tuning materials properties, but it is often limited by binodal and spinodal decomposition, which correspond to the thermodynamic solubility limit and the stability against composition fluctuations, respectively. We show that heterostructural alloys can exhibit a markedly increased range of metastable alloy compositions between the binodal and spinodal lines, thereby opening up a vast phase space for novel homogeneous single-phase alloys. We distinguish two types of heterostructural alloys, that is, those between commensurate and incommensurate phases. Because of the structural transition around the critical composition, the properties change in a highly nonlinear or even discontinuous fashion, providing a mechanism for materials design that does not exist in conventional isostructural alloys. The novel phase diagram behavior follows from standard alloy models using mixing enthalpies from first-principles calculations. Furthermore, thin-film deposition demonstrates the viability of the synthesis of these metastable single-phase domains and validates the computationally predicted phase separation mechanism above the upper temperature bound of the nonequilibrium single-phase region.
Authors:
ORCiD logo [1] ; ORCiD logo [2] ; ORCiD logo [3] ;  [4] ;  [5] ;  [6] ; ORCiD logo [7] ;  [7] ;  [8] ; ORCiD logo [3] ;  [3] ; ORCiD logo [3] ;  [5] ;  [6] ;  [3] ; ORCiD logo [3]
  1. National Renewable Energy Lab. (NREL), Golden, CO (United States); Univ. of Colorado, Boulder, CO (United States)
  2. National Renewable Energy Lab. (NREL), Golden, CO (United States); Swiss Federal Labs. for Materials Science and Technology, Dubendorf (Switzerland)
  3. National Renewable Energy Lab. (NREL), Golden, CO (United States)
  4. National Renewable Energy Lab. (NREL), Golden, CO (United States); Temple Univ., Philadelphia, PA (United States)
  5. Colorado School of Mines, Golden, CO (United States)
  6. Oregon State Univ., Corvallis, OR (United States)
  7. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  8. Harvard Univ., Cambridge, MA (United States)
Publication Date:
Report Number(s):
NREL/JA-5K00-68325
Journal ID: ISSN 2375-2548
Grant/Contract Number:
AC36-08GO28308; AC02-76SF00515; ID0EUSDI18002
Type:
Accepted Manuscript
Journal Name:
Science Advances
Additional Journal Information:
Journal Volume: 3; Journal Issue: 6; Journal ID: ISSN 2375-2548
Publisher:
AAAS
Research Org:
National Renewable Energy Lab. (NREL), Golden, CO (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
14 SOLAR ENERGY; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; non-equilibrium materials; phase diagrams; semiconductor alloys; materials design; metastable materials; alloy theory; computational materials science
OSTI Identifier:
1364056
Alternate Identifier(s):
OSTI ID: 1390707

Holder, Aaron M., Siol, Sebastian, Ndione, Paul F., Peng, Haowei, Deml, Ann M., Matthews, Bethany E., Schelhas, Laura T., Toney, Michael F., Gordon, Roy G., Tumas, William, Perkins, John D., Ginley, David S., Gorman, Brian P., Tate, Janet, Zakutayev, Andriy, and Lany, Stephan. Novel phase diagram behavior and materials design in heterostructural semiconductor alloys. United States: N. p., Web. doi:10.1126/sciadv.1700270.
Holder, Aaron M., Siol, Sebastian, Ndione, Paul F., Peng, Haowei, Deml, Ann M., Matthews, Bethany E., Schelhas, Laura T., Toney, Michael F., Gordon, Roy G., Tumas, William, Perkins, John D., Ginley, David S., Gorman, Brian P., Tate, Janet, Zakutayev, Andriy, & Lany, Stephan. Novel phase diagram behavior and materials design in heterostructural semiconductor alloys. United States. doi:10.1126/sciadv.1700270.
Holder, Aaron M., Siol, Sebastian, Ndione, Paul F., Peng, Haowei, Deml, Ann M., Matthews, Bethany E., Schelhas, Laura T., Toney, Michael F., Gordon, Roy G., Tumas, William, Perkins, John D., Ginley, David S., Gorman, Brian P., Tate, Janet, Zakutayev, Andriy, and Lany, Stephan. 2017. "Novel phase diagram behavior and materials design in heterostructural semiconductor alloys". United States. doi:10.1126/sciadv.1700270. https://www.osti.gov/servlets/purl/1364056.
@article{osti_1364056,
title = {Novel phase diagram behavior and materials design in heterostructural semiconductor alloys},
author = {Holder, Aaron M. and Siol, Sebastian and Ndione, Paul F. and Peng, Haowei and Deml, Ann M. and Matthews, Bethany E. and Schelhas, Laura T. and Toney, Michael F. and Gordon, Roy G. and Tumas, William and Perkins, John D. and Ginley, David S. and Gorman, Brian P. and Tate, Janet and Zakutayev, Andriy and Lany, Stephan},
abstractNote = {Structure and composition control the behavior of materials. Isostructural alloying is historically an extremely successful approach for tuning materials properties, but it is often limited by binodal and spinodal decomposition, which correspond to the thermodynamic solubility limit and the stability against composition fluctuations, respectively. We show that heterostructural alloys can exhibit a markedly increased range of metastable alloy compositions between the binodal and spinodal lines, thereby opening up a vast phase space for novel homogeneous single-phase alloys. We distinguish two types of heterostructural alloys, that is, those between commensurate and incommensurate phases. Because of the structural transition around the critical composition, the properties change in a highly nonlinear or even discontinuous fashion, providing a mechanism for materials design that does not exist in conventional isostructural alloys. The novel phase diagram behavior follows from standard alloy models using mixing enthalpies from first-principles calculations. Furthermore, thin-film deposition demonstrates the viability of the synthesis of these metastable single-phase domains and validates the computationally predicted phase separation mechanism above the upper temperature bound of the nonequilibrium single-phase region.},
doi = {10.1126/sciadv.1700270},
journal = {Science Advances},
number = 6,
volume = 3,
place = {United States},
year = {2017},
month = {6}
}

Works referenced in this record:

Generalized Gradient Approximation Made Simple
journal, October 1996
  • Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
  • Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
  • DOI: 10.1103/PhysRevLett.77.3865

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

Polymer-Polymer Phase Behavior
journal, February 1991

Atomic Layer Deposition of Tin Monosulfide Thin Films
journal, September 2011
  • Sinsermsuksakul, Prasert; Heo, Jaeyeong; Noh, Wontae
  • Advanced Energy Materials, Vol. 1, Issue 6, p. 1116-1125
  • DOI: 10.1002/aenm.201100330