Study of disorder in pulsed laser deposited double perovskite oxides by first-principle structure prediction

Edoardo Fertitta; Sujit Das; Debalina Banerjee; Farbod Ebrahimi; Clément Barraud; Kai Du; He Tian; Chris J. Pickard; Cedric Weber; Ramamoorthy Ramesh; Peter Littlewood; David Dubbink

doi:10.1038/s41524-021-00561-1

Study of disorder in pulsed laser deposited double perovskite oxides by first-principle structure prediction

Edoardo Fertitta^*
, Sujit Das
, Debalina Banerjee
, Farbod Ebrahimi
, Clément Barraud
, Kai Du
, He Tian
, Chris J. Pickard
, Cedric Weber
, Ramamoorthy Ramesh
, Peter Littlewood
, David Dubbink

^*Corresponding author for this work

School of Physics and Astronomy

Research output: Contribution to journal › Article › peer-review

Abstract

Double perovskite oxides, with generalized formula A₂BB′O₆, attract wide interest due to their multiferroic and charge transfer properties. They offer a wide range of potential applications such as spintronics and electrically tunable devices. However, great practical limitations are encountered, since a spontaneous order of the B-site cations is notoriously hard to achieve. In this joint experimental-theoretical work, we focused on the characterization of double perovskites La₂TiFeO₆ and La₂VCuO₆ films grown by pulsed laser deposition and interpretation of the observed B-site disorder and partial charge transfer between the B-site ions. A random structure sampling method was used to show that several phases compete due to their corresponding configurational entropy. In order to capture a representative picture of the most relevant competing microstates in realistic experimental conditions, this search included the potential formation of non-stoichiometric phases as well, which could also be directly related to the observed partial charge transfer. We optimized the information encapsulated in the potential energy landscape, captured via structure sampling, by evaluating both enthalpic and entropic terms. These terms were employed as a metric for the competition of different phases. This approach, applied herein specifically to La₂TiFeO₆, highlights the presence of highly entropic phases above the ground state which can explain the disorder observed frequently in the broader class of double perovskite oxides.

Original language	English
Article number	92
Number of pages	8
Journal	npj Computational Materials
Volume	7
DOIs	https://doi.org/10.1038/s41524-021-00561-1
Publication status	Published - 15 Jun 2021

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@article{bbdc7a3151ad479888b34d3f3a5fd9b1,

title = "Study of disorder in pulsed laser deposited double perovskite oxides by first-principle structure prediction",

abstract = "Double perovskite oxides, with generalized formula A2BB′O6, attract wide interest due to their multiferroic and charge transfer properties. They offer a wide range of potential applications such as spintronics and electrically tunable devices. However, great practical limitations are encountered, since a spontaneous order of the B-site cations is notoriously hard to achieve. In this joint experimental-theoretical work, we focused on the characterization of double perovskites La2TiFeO6 and La2VCuO6 films grown by pulsed laser deposition and interpretation of the observed B-site disorder and partial charge transfer between the B-site ions. A random structure sampling method was used to show that several phases compete due to their corresponding configurational entropy. In order to capture a representative picture of the most relevant competing microstates in realistic experimental conditions, this search included the potential formation of non-stoichiometric phases as well, which could also be directly related to the observed partial charge transfer. We optimized the information encapsulated in the potential energy landscape, captured via structure sampling, by evaluating both enthalpic and entropic terms. These terms were employed as a metric for the competition of different phases. This approach, applied herein specifically to La2TiFeO6, highlights the presence of highly entropic phases above the ground state which can explain the disorder observed frequently in the broader class of double perovskite oxides.",

author = "Edoardo Fertitta and Sujit Das and Debalina Banerjee and Farbod Ebrahimi and Cl{\'e}ment Barraud and Kai Du and He Tian and Pickard, \{Chris J.\} and Cedric Weber and Ramamoorthy Ramesh and Peter Littlewood and David Dubbink",

note = "Funding: Part of this work was performed at the Stanford Nano Shared Facilities (SNSF), supported by the National Science Foundation under award ECCS-1542152. C.W. was supported by a grant [EP/R02992X/1] from the UK Engineering and Physical Sciences Research Council (EPSRC). This work was performed using resources provided by the ARCHER UK National Supercomputing Service and the Cambridge Service for Data-Driven Discovery (CSD3) operated by the University of Cambridge Research Computing Service (www.csd3.cam.ac.uk), provided by Dell EMC and Intel using Tier-2 funding from the Engineering and Physical Sciences Research Council (capital grant [EP/P020259/1]), and DiRAC funding from the Science and Technology Facilities Council (www.dirac.ac.uk).",

year = "2021",

month = jun,

day = "15",

doi = "10.1038/s41524-021-00561-1",

language = "English",

volume = "7",

journal = "npj Computational Materials",

issn = "2057-3960",

publisher = "Nature publishing group",

}

TY - JOUR

T1 - Study of disorder in pulsed laser deposited double perovskite oxides by first-principle structure prediction

AU - Fertitta, Edoardo

AU - Das, Sujit

AU - Banerjee, Debalina

AU - Ebrahimi, Farbod

AU - Barraud, Clément

AU - Du, Kai

AU - Tian, He

AU - Pickard, Chris J.

AU - Weber, Cedric

AU - Ramesh, Ramamoorthy

AU - Littlewood, Peter

AU - Dubbink, David

N1 - Funding: Part of this work was performed at the Stanford Nano Shared Facilities (SNSF), supported by the National Science Foundation under award ECCS-1542152. C.W. was supported by a grant [EP/R02992X/1] from the UK Engineering and Physical Sciences Research Council (EPSRC). This work was performed using resources provided by the ARCHER UK National Supercomputing Service and the Cambridge Service for Data-Driven Discovery (CSD3) operated by the University of Cambridge Research Computing Service (www.csd3.cam.ac.uk), provided by Dell EMC and Intel using Tier-2 funding from the Engineering and Physical Sciences Research Council (capital grant [EP/P020259/1]), and DiRAC funding from the Science and Technology Facilities Council (www.dirac.ac.uk).

PY - 2021/6/15

Y1 - 2021/6/15

N2 - Double perovskite oxides, with generalized formula A2BB′O6, attract wide interest due to their multiferroic and charge transfer properties. They offer a wide range of potential applications such as spintronics and electrically tunable devices. However, great practical limitations are encountered, since a spontaneous order of the B-site cations is notoriously hard to achieve. In this joint experimental-theoretical work, we focused on the characterization of double perovskites La2TiFeO6 and La2VCuO6 films grown by pulsed laser deposition and interpretation of the observed B-site disorder and partial charge transfer between the B-site ions. A random structure sampling method was used to show that several phases compete due to their corresponding configurational entropy. In order to capture a representative picture of the most relevant competing microstates in realistic experimental conditions, this search included the potential formation of non-stoichiometric phases as well, which could also be directly related to the observed partial charge transfer. We optimized the information encapsulated in the potential energy landscape, captured via structure sampling, by evaluating both enthalpic and entropic terms. These terms were employed as a metric for the competition of different phases. This approach, applied herein specifically to La2TiFeO6, highlights the presence of highly entropic phases above the ground state which can explain the disorder observed frequently in the broader class of double perovskite oxides.

AB - Double perovskite oxides, with generalized formula A2BB′O6, attract wide interest due to their multiferroic and charge transfer properties. They offer a wide range of potential applications such as spintronics and electrically tunable devices. However, great practical limitations are encountered, since a spontaneous order of the B-site cations is notoriously hard to achieve. In this joint experimental-theoretical work, we focused on the characterization of double perovskites La2TiFeO6 and La2VCuO6 films grown by pulsed laser deposition and interpretation of the observed B-site disorder and partial charge transfer between the B-site ions. A random structure sampling method was used to show that several phases compete due to their corresponding configurational entropy. In order to capture a representative picture of the most relevant competing microstates in realistic experimental conditions, this search included the potential formation of non-stoichiometric phases as well, which could also be directly related to the observed partial charge transfer. We optimized the information encapsulated in the potential energy landscape, captured via structure sampling, by evaluating both enthalpic and entropic terms. These terms were employed as a metric for the competition of different phases. This approach, applied herein specifically to La2TiFeO6, highlights the presence of highly entropic phases above the ground state which can explain the disorder observed frequently in the broader class of double perovskite oxides.

U2 - 10.1038/s41524-021-00561-1

DO - 10.1038/s41524-021-00561-1

M3 - Article

AN - SCOPUS:85108118404

SN - 2057-3960

VL - 7

JO - npj Computational Materials

JF - npj Computational Materials

M1 - 92

ER -

Study of disorder in pulsed laser deposited double perovskite oxides by first-principle structure prediction

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