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Title: Phase stability, ordering tendencies, and magnetism in single-phase fcc Au-Fe nanoalloys

Abstract

Bulk Au-Fe alloys separate into Au-based fcc and Fe-based bcc phases, but L1 0 and L1 2 orderings were reported in single-phase Au-Fe nanoparticles. Motivated by these observations, we study the structural and ordering energetics in this alloy by combining density functional theory (DFT) calculations with effective Hamiltonian techniques: a cluster expansion with structural filters, and the configuration-dependent lattice deformation model. The phase separation tendency in Au-Fe persists even if the fcc-bcc decomposition is suppressed. The relative stability of disordered bcc and fcc phases observed in nanoparticles is reproduced, but the fully ordered L1 0 AuFe, L1 2 Au 3Fe, and L1 2 AuFe 3 structures are unstable in DFT. But, a tendency to form concentration waves at the corresponding [001] ordering vector is revealed in nearly-random alloys in a certain range of concentrations. Furthermore, this incipient ordering requires enrichment by Fe relative to the equiatomic composition, which may occur in the core of a nanoparticle due to the segregation of Au to the surface. Effects of magnetism on the chemical ordering are also discussed.

Authors:
 [1];  [2];  [1]; ORCiD logo [1]
  1. Univ. of Nebraska, Lincoln, NE (United States). Dept. of Physics and Astronomy, Nebraska Center for Materials and Nanoscience
  2. Univ. of Nebraska, Lincoln, NE (United States). Dept. of Physics and Astronomy, Nebraska Center for Materials and Nanoscience; Intermolecular Inc., San Jose, CA (United States)
Publication Date:
Research Org.:
Univ. of Nebraska, Lincoln, NE (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1399581
Alternate Identifier(s):
OSTI ID: 1399641
Grant/Contract Number:  
SC0001269
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review B
Additional Journal Information:
Journal Volume: 96; Journal Issue: 13; Journal ID: ISSN 2469-9950
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Fe-Au alloys; phase transitions; ordering; nanoparticles; strain-induced interaction; first-principles calculations; magnetism; Kanzaki forces; force constants

Citation Formats

Zhuravlev, I. A., Barabash, S. V., An, J. M., and Belashchenko, K. D. Phase stability, ordering tendencies, and magnetism in single-phase fcc Au-Fe nanoalloys. United States: N. p., 2017. Web. doi:10.1103/PhysRevB.96.134109.
Zhuravlev, I. A., Barabash, S. V., An, J. M., & Belashchenko, K. D. Phase stability, ordering tendencies, and magnetism in single-phase fcc Au-Fe nanoalloys. United States. doi:10.1103/PhysRevB.96.134109.
Zhuravlev, I. A., Barabash, S. V., An, J. M., and Belashchenko, K. D. Sun . "Phase stability, ordering tendencies, and magnetism in single-phase fcc Au-Fe nanoalloys". United States. doi:10.1103/PhysRevB.96.134109. https://www.osti.gov/servlets/purl/1399581.
@article{osti_1399581,
title = {Phase stability, ordering tendencies, and magnetism in single-phase fcc Au-Fe nanoalloys},
author = {Zhuravlev, I. A. and Barabash, S. V. and An, J. M. and Belashchenko, K. D.},
abstractNote = {Bulk Au-Fe alloys separate into Au-based fcc and Fe-based bcc phases, but L10 and L12 orderings were reported in single-phase Au-Fe nanoparticles. Motivated by these observations, we study the structural and ordering energetics in this alloy by combining density functional theory (DFT) calculations with effective Hamiltonian techniques: a cluster expansion with structural filters, and the configuration-dependent lattice deformation model. The phase separation tendency in Au-Fe persists even if the fcc-bcc decomposition is suppressed. The relative stability of disordered bcc and fcc phases observed in nanoparticles is reproduced, but the fully ordered L10 AuFe, L12 Au3Fe, and L12 AuFe3 structures are unstable in DFT. But, a tendency to form concentration waves at the corresponding [001] ordering vector is revealed in nearly-random alloys in a certain range of concentrations. Furthermore, this incipient ordering requires enrichment by Fe relative to the equiatomic composition, which may occur in the core of a nanoparticle due to the segregation of Au to the surface. Effects of magnetism on the chemical ordering are also discussed.},
doi = {10.1103/PhysRevB.96.134109},
journal = {Physical Review B},
number = 13,
volume = 96,
place = {United States},
year = {2017},
month = {10}
}

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Works referenced in this record:

Microscopic first-principles model of strain-induced interaction in concentrated size-mismatched alloys
journal, December 2014


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

Magnetic and transport properties of Fe‐Au and Co‐Au films
journal, March 1981

  • McGuire, T. R.; Aboaf, J. A.; Klokholm, E.
  • Journal of Applied Physics, Vol. 52, Issue 3
  • DOI: 10.1063/1.328879

Calculation of the lattice constant of solids with semilocal functionals
journal, February 2009


Defect-mediated nucleation of α-iron in Au-Fe alloys
journal, September 1991


Competition between ordering, twinning, and segregation in binary magnetic 3d-5d nanoparticles: A supercomputing perspective
journal, October 2011

  • Gruner, Markus E.; Entel, Peter
  • International Journal of Quantum Chemistry, Vol. 112, Issue 1
  • DOI: 10.1002/qua.23254

Projector augmented-wave method
journal, December 1994


Ferromagnetic phases of bcc and fcc Fe, Co, and Ni
journal, August 1986


Effects of alloying and strain on the magnetic properties of Fe 16 N 2
journal, July 2013


Accurate spin-dependent electron liquid correlation energies for local spin density calculations: a critical analysis
journal, August 1980

  • Vosko, S. H.; Wilk, L.; Nusair, M.
  • Canadian Journal of Physics, Vol. 58, Issue 8
  • DOI: 10.1139/p80-159

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


Point defects in face-centred cubic lattice—I distortion around defects
journal, March 1957


Generalized cluster description of multicomponent systems
journal, November 1984

  • Sanchez, J. M.; Ducastelle, F.; Gratias, D.
  • Physica A: Statistical Mechanics and its Applications, Vol. 128, Issue 1-2
  • DOI: 10.1016/0378-4371(84)90096-7

Formation of non-equilibrium Fe-Au solid solutions in nanoclusters
journal, June 2013

  • Mukherjee, P.; Zhou, Lin; Kramer, M. J.
  • Applied Physics Letters, Vol. 102, Issue 24
  • DOI: 10.1063/1.4811412

Automating first-principles phase diagram calculations
journal, August 2002


Electronic Correlations at the α γ Structural Phase Transition in Paramagnetic Iron
journal, March 2011


Microscopic first-principles model of strain-induced interaction in concentrated size-mismatched alloys
journal, December 2014


Self-driven lattice-model Monte Carlo simulations of alloy thermodynamic properties and phase diagrams
journal, July 2002

  • Walle, A. van de; Asta, M.
  • Modelling and Simulation in Materials Science and Engineering, Vol. 10, Issue 5
  • DOI: 10.1088/0965-0393/10/5/304

Theory of Diffuse Scattering of X-rays by Local Lattice Distortions
journal, May 1952

  • Matsubara, Takeo
  • Journal of the Physical Society of Japan, Vol. 7, Issue 3
  • DOI: 10.1143/JPSJ.7.270

Ab initio calculation of the phase stability in Au-Pd and Ag-Pt alloys
journal, May 2006


Conditions for the Existence of Ordered Structure in Binary Alloy Systems
journal, December 1977


First-Principles Calculations of Free Energies of Unstable Phases: The Case of fcc W
journal, February 2009


Point defect modeling in materials: Coupling ab initio and elasticity approaches
journal, October 2013

  • Varvenne, Céline; Bruneval, Fabien; Marinica, Mihai-Cosmin
  • Physical Review B, Vol. 88, Issue 13
  • DOI: 10.1103/PhysRevB.88.134102

Cluster expansion made easy with Bayesian compressive sensing
journal, October 2013


Ab Initio Construction of Magnetic Phase Diagrams in Alloys: The Case of Fe 1 x Mn x Pt
journal, July 2015


First-principles determination of low-temperature order and ground states of Fe-Ni, Fe-Pd, and Fe-Pt
journal, December 2009


Canonical description of electron states in random alloys
journal, February 1987


Linear stability analysis of phase separation in nanoscale systems
journal, February 2009


Artificial fabrication of an L 1 0 ‐type ordered FeAu alloy by alternate monatomic deposition
journal, August 1995

  • Takanashi, K.; Mitani, S.; Sano, M.
  • Applied Physics Letters, Vol. 67, Issue 7
  • DOI: 10.1063/1.114715

Evolutionary approach for determining first-principles hamiltonians
journal, April 2005

  • Hart, Gus L. W.; Blum, Volker; Walorski, Michael J.
  • Nature Materials, Vol. 4, Issue 5
  • DOI: 10.1038/nmat1374

Ab initio theory of phase stability and structural selectivity in Fe-Pd alloys
journal, April 2012


Gradient-corrected density functionals: Full-potential calculations for iron
journal, May 1991


Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
journal, July 1996


Origin of the 〈11/20〉 atomic short-range order in Au-rich Au-Fe alloys
journal, August 1995


Nucleation-Suppressed Phase Stabilization in Fe–Au Nanoparticles
journal, October 2013

  • Mukherjee, P.; Jiang, Xiujuan; Wu, Y. Q.
  • The Journal of Physical Chemistry C, Vol. 117, Issue 45
  • DOI: 10.1021/jp409015y

Ab initio molecular dynamics for open-shell transition metals
journal, November 1993


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


Nonlocal First-Principles Calculations in Cu-Au and Other Intermetallic Alloys
journal, February 2014


Temperature dependence of magnetic anisotropy: An ab initio approach
journal, October 2006


Cohesion in alloys — fundamentals of a semi-empirical model
journal, April 1980


Efficient cluster expansion for substitutional systems
journal, November 1992


Determination of the short-range order structure of Au-25 At. Pct Fe using wide-angle diffuse synchrotron X-Ray scattering
journal, August 1994

  • Anderson, J. P.; Chen, Haydn
  • Metallurgical and Materials Transactions A, Vol. 25, Issue 8
  • DOI: 10.1007/BF02668522

Surface segregation energies in transition-metal alloys
journal, June 1999


First-principles theory of short-range order, electronic excitations, and spin polarization in Ni-V and Pd-V alloys
journal, September 1995


Special quasirandom structures
journal, July 1990


Theoretical study of noble-metal (100) surface reconstructions using first-principles techniques
journal, September 1989


L1 0 structure formation in slow-cooled Fe-Au nanoclusters
journal, May 2012

  • Mukherjee, P.; Zhang, Y.; Kramer, M. J.
  • Applied Physics Letters, Vol. 100, Issue 21
  • DOI: 10.1063/1.4720180

Origin of the spin reorientation transitions in (Fe1–xCox)2B alloys
journal, February 2015

  • Belashchenko, Kirill D.; Ke, Liqin; Däne, Markus
  • Applied Physics Letters, Vol. 106, Issue 6
  • DOI: 10.1063/1.4908056

Prediction of unusual stable ordered structures of Au-Pd alloys via a first-principles cluster expansion
journal, July 2006


Absence of metastable states in strained monatomic cubic crystals
journal, July 2004


Cu-Au, Ag-Au, Cu-Ag, and Ni-Au intermetallics: First-principles study of temperature-composition phase diagrams and structures
journal, March 1998


L10 Type Ordered Phase Formation in Fe-Au Nanoparticles
journal, January 2002

  • Sato, Kazuhisa; Bian, Bo; Hirotsu, Yoshihiko
  • Japanese Journal of Applied Physics, Vol. 41, Issue Part 2, No. 1A/B
  • DOI: 10.1143/JJAP.41.L1

Structure, energetics, and mechanical stability of Fe-Cu bcc alloys from first-principles calculations
journal, October 2005


Size-Induced Chemical and Magnetic Ordering in Individual Fe–Au Nanoparticles
journal, July 2014

  • Mukherjee, Pinaki; Manchanda, Priyanka; Kumar, Pankaj
  • ACS Nano, Vol. 8, Issue 8
  • DOI: 10.1021/nn5022007

Cluster expansion and the configurational theory of alloys
journal, June 2010


Noncollinear full-potential studies of γ Fe
journal, July 2002