Abstract
This paper explores thin films of the entropy-stabilized oxide (ESO) composition MgxNixCoxCuxZnxScxO (x~ 0.167) grown by laser ablation in incremental gas pressures and O2/Ar ratios to modulate particle kinetic energy and plume reactivity. Low pressures supporting high kinetic energy adatoms favor the kinetic stabilization of a single rocksalt phase, while high pressures (low kinetic energy adatoms) result in phase separation. The pressure threshold for phase separation is a function of O2/Ar ratio. These findings suggest large kinetic energies facilitate the assembly and quench of metastable ESO phases that may require immoderate physical or chemical conditions to synthesize using near-equilibrium techniques.
Similar content being viewed by others
References
C.M. Rost, E. Sachet, T. Borman, A. Moballegh, E.C. Dickey, D. Hou, J.L. Jones, S. Curtarolo, and J.-P. Maria: Entropy-stabilized oxides. Nat. Commun. 6, 8485 (2015).
D. Bérardan, S. Franger, D. Dragoe, A.K. Meena, and N. Dragoe: Colossal dielectric constant in high entropy oxides. Phys. Status Solidi—Rapid Res. Lett. 10, 328 (2016).
D. Berardan, S. Franger, A.K. Meena, and N. Dragoe: Room temperature lithium superionic conductivity in high entropy oxides. J. Mater. Chem. A 4, 9536 (2016).
D. Berardan, A.K. Meena, S. Franger, C. Herrero, and N. Dragoe: Controlled Jahn-Teller distortion in (MgCoNiCuZn)O-based high entropy oxides. J. Alloys Compd. 704, 693 (2017).
C.M. Rost: Entropy-Stabilized Oxides: Explorations of a Novel Class of Multicomponent Materials. Doctoral Dissertation, North Carolina State University, Raleigh, NC, USA, 2016.
Z. Rak, C.M. Rost, M. Lim, P. Sarker, C. Toher, S. Curtarolo, J.P. Maria, and D.W. Brenner: Charge compensation and electrostatic transferability in three entropy-stabilized oxides: Results from density functional theory calculations. J. Appl. Phys. 120, 095105 (2016).
A. Sarkar, R. Djenadic, N.J. Usharani, K.P. Sanghvi, V.S.K. Chakravadhanula, A.S. Gandhi, H. Hahn, and S.S. Bhattacharya: Nanocrystalline multicomponent entropy stabilised transition metal oxides. J. Eur. Ceram. Soc. 37, 747 (2017).
P.B. Meisenheimer, T.J. Kratofil, and J.T. Heron: Giant enhancement of exchange coupling in entropy-stabilized oxide heterostructures. Sci. Rep. 7, 3 (2017).
D.B. Miracle and O.N. Senkov: A critical review of high entropy alloys and related concepts. Acta Mater. 122, 448 (2017).
J.P. Zheng, Z.Q. Huang, D.T. Shaw, and H.S. Kwok: Generation of high-energy atomic beams in laser-superconducting target interactions. Appl. Phys. Lett. 54, 280 (1989).
D.B. Geohegan: Physics and diagnostics of laser ablation plume propagation for high-Tc superconductor film growth. Thin Solid Films 220, 138 (1992).
D.B. Geohegan and A.A. Puretzky: Laser ablation plume thermalization dynamics in background gases: combined imaging, optical absorption and emission spectroscopy, and ion probe measurements. Appl. Surf. Sci. 96-98, 131 (1996).
S. Amoruso, C. Aruta, R. Bruzzese, D. Maccariello, L. Maritato, F. Miletto Granozio, P. Orgiani, U. Scotti di Uccio, and X. Wang: Optimization of La0.7Ba0.3MnO3−δ complex oxide laser ablation conditions by plume imaging and optical emission spectroscopy. J. Appl. Phys. 108, 043302 (2010).
C. Aruta, S. Amoruso, R. Bruzzese, X. Wang, D. Maccariello, F. Miletto Granozio, and U. Scotti Di Uccio: Pulsed laser deposition of SrTiO3/LaGaO3 and SrTiO3/LaAlO3: plasma plume effects. Appl. Phys. Lett. 97, 252105 (2010).
A. Sambri, D.V. Cristensen, F. Trier, Y.Z. Chen, S. Amoruso, N. Pryds, R. Bruzzese, and X. Wang: Plasma plume effects on the conductivity of amorphous-LaAlO3/SrTiO3 interfaces grown by pulsed laser deposition in O2 and Ar. Appl. Phys. Lett. 100, 231605 (2012).
A. Ojeda-G-P, C.W. Schneider, T. Lippert, and A. Wokaun: Pressure and temperature dependence of the laser-induced plasma plume dynamics Pressure and temperature dependence of the laser-induced plasma plume dynamics. J. Appl. Phys. 120, 225301 (2016).
K. Orsel, R. Groenen, B. Bastiaens, G. Koster, G. Rijnders, and K.J. Boller: Influence of the oxidation state of SrTiO3 plasmas for stoichiometric growth of pulsed laser deposition films identified by laser induced fluorescence. APL Mater. 3, 106103 (2015).
R. Groenen, J. Smit, K. Orsel, A. Vailionis, B. Bastiaens, M. Huijben, K. Boller, G. Rijnders, and G. Koster: Research Update: Stoichiometry controlled oxide thin film growth by pulsed laser deposition. APL Mater. 3, 070701 (2015).
T.F. Tseng, M.H. Yeh, K.S. Liu, and I.N. Lin: Effects of ambient gas pressure on (1-x)SrTiO3-xBaTiO3 films prepared by pulsed laser deposition. J. Appl. Phys. 80, 4984 (1996).
J.-P. Maria, S. Trolier-McKinstry, D.G. Schlom, M.E. Hawley, and G.W. Brown: The influence of energetic bombardment on the structure and properties of epitaxial SrRuO3 thin films grown by pulsed laser deposition. J. Appl. Phys. 83, 4373 (1998).
C. Wang, B.L. Cheng, S.Y. Wang, H.B. Lu, Y.L. Zhou, Z.H. Chen, and G.Z. Yang: Effects of oxygen pressure on lattice parameter, orientation, surface morphology and deposition rate of (Ba0.02Sr0.98)TiO3 thin films grown on MgO substrate by pulsed laser deposition. Thin Solid Films 485, 82 (2005).
S. Saremi, R. Xu, L.R. Dedon, J.A. Mundy, S. Hsu, Z. Chen, A.R. Damodaran, S.P. Chapman, J.T. Evans, and L.W. Martin: Enhanced electrical resistivity and properties via ion bombardment of ferroelectric thin films. Adv. Mater. 28, 10750 (2016).
D.E. Work and H.A. Eick: On the preparation of condensed ScO. J. Less-Common Met. 26, 413 (1972).
O.Y. Gorbenko, S.V. Samoilenkov, I.E. Graboy, and A.R. Kaul: Epitaxial stabilization in thin films of oxides. Chem. Mater. 14, 4026 (2002).
C.M. Rost, Z. Rak, and J.-P. Maria: Local structure of the MgxNixCoxCuxZnxO(x=0.2) entropy-stabilized oxide: an EXAFS study. J. Am. Ceram. Soc. 100, 1 (2017).
A. Navrotsky and O.J. Kleppa: The thermodynamics of cation distributions in simple spinels. J. Inorg. Nucl. Chem. 29, 2701 (1967).
R.W.G. Wyckoff: Crystal Structures, Vol. 2, 2nd ed. (Interscience, New York, 1964), pp. 2–6.
N. Kato and A.R. Lang: A study of pendellossung fringes in X-ray diffraction. Acta Cryst. 12, 787 (1959).
E.H. Smith, P.D.C. King, A. Soukiassian, D.G. Ast, and D.G. Schlom: Hybrid reflections from multiple x-ray scattering in epitaxial oxide films. Appl. Phys. Lett. 111, 131903 (2017).
C.-S. Zha, H. Mao, and R.J. Hemley: Elasticity of MgO and a primary pressure scale to 55 GPa. Proc. Natl. Acad. Sci. U. S. A. 97, 13494 (2000).
Acknowledgments
The authors acknowledge support from NSF Ceramics, award 1610844.
Author information
Authors and Affiliations
Corresponding author
Supplementary Material
Supplementary material
Supplementary material
The supplementary material for this article can be found at https://doi.org/10.1557/mrc.2018.184.
Rights and permissions
About this article
Cite this article
Kotsonis, G.N., Rost, C.M., Harris, D.T. et al. Epitaxial entropy-stabilized oxides: growth of chemically diverse phases via kinetic bombardment. MRS Communications 8, 1371–1377 (2018). https://doi.org/10.1557/mrc.2018.184
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1557/mrc.2018.184