Synthesis method comparison of compositionally complex rare earth-based Ruddlesden–Popper n = 1 T′-type cuprates

Brianna L. Musicó; Quinton Wright; Cordell Delzer; T. Zac Ward; Claudia J. Rawn; David G. Mandrus; Veerle Keppens

doi:10.1111/jace.17750

Synthesis method comparison of compositionally complex rare earth-based Ruddlesden–Popper n = 1 T′-type cuprates

Brianna L. Musicó, Quinton Wright, Cordell Delzer, T. Zac Ward, Claudia J. Rawn, David G. Mandrus, Veerle Keppens

Quantum Heterostructures

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

11 Scopus citations

Abstract

The multicomponent approach has been successfully expanded to the Ruddlesden–Popper structure with the synthesis of two different high-entropy cuprate compositions: (La_0.2Nd_0.2Gd_0.2Tb_0.2Dy_0.2)₂CuO₄ and (La_0.2Pr_0.2Nd_0.2Sm_0.2Eu_0.2)₂CuO₄. The effect of synthesis method is explored using both solid-state reaction and polymeric steric entrapment (PSE) methods. It is found that PSE leads to more randomly distributed cation species, providing an advantageous method of synthesis for the growing field of high entropy oxides. In situ high-temperature x-ray diffraction tracks the amorphous to crystalline phase transformation in (La_0.2Nd_0.2Gd_0.2Tb_0.2Dy_0.2)₂CuO₄ powder, synthesized using the PSE method. Using the High-Temperature XRD data, a method for gaining information on the kinetic behavior is also applied. Magnetometry of both compositions indicates ferrimagnetic behavior at low temperatures.

Original language	English
Pages (from-to)	3750-3759
Number of pages	10
Journal	Journal of the American Ceramic Society
Volume	104
Issue number	7
DOIs	https://doi.org/10.1111/jace.17750
State	Published - Jul 2021

Funding

B.L.M. acknowledges the support of the Center for Materials Processing, a Tennessee Higher Education Commission (THEC) supported Accomplished Center of Excellence. T.Z.W. was supported by the US Department of Energy (DOE), Office of Basic Energy Sciences (BES), and Materials Sciences and Engineering Division. D.G.M acknowledges support from the Gordon and Betty Moore Foundation’s EPiQS Initiative, Grant GBMF9069. Powder XRD and microscopy was performed at the Joint Institute for Advanced Materials (JIAM) Diffraction Facility, and Microscopy Facility, respectively, located at the University of Tennessee, Knoxville. C.D. acknowledges support by the Department of Energy National Nuclear Security Administration through the Nuclear Science and Security Consortium under Award Number DE‐NA0003180. This paper was prepared as an account of work sponsored by an agency of the United States Government. Neither the United States Government nor any agency thereof, nor any of their employees, makes any warranty, express or limited, or assumes any legal liability or responsibility for the accuracy, completeness, or usefulness of any information, apparatus, product, or process disclosed, or represents that its use would not infringe privately owned rights. Reference herein to any specific commercial product, process, or service by trade name, trademark, manufacturer, or otherwise does not necessarily constitute or imply its endorsement, recommendation, or favoring by the United States Government or any agency thereof. The views and opinions of authors expressed herein do not necessarily state or reflect those of the United States Government or any agency thereof. B.L.M. acknowledges the support of the Center for Materials Processing, a Tennessee Higher Education Commission (THEC) supported Accomplished Center of Excellence. T.Z.W. was supported by the US Department of Energy (DOE), Office of Basic Energy Sciences (BES), and Materials Sciences and Engineering Division. D.G.M acknowledges support from the Gordon and Betty Moore Foundation’s EPiQS Initiative, Grant GBMF9069. Powder XRD and microscopy was performed at the Joint Institute for Advanced Materials (JIAM) Diffraction Facility, and Microscopy Facility, respectively, located at the University of Tennessee, Knoxville. C.D. acknowledges support by the Department of Energy National Nuclear Security Administration through the Nuclear Science and Security Consortium under Award Number DE-NA0003180. This paper was prepared as an account of work sponsored by an agency of the United States Government. Neither the United States Government nor any agency thereof, nor any of their employees, makes any warranty, express or limited, or assumes any legal liability or responsibility for the accuracy, completeness, or usefulness of any information, apparatus, product, or process disclosed, or represents that its use would not infringe privately owned rights. Reference herein to any specific commercial product, process, or service by trade name, trademark, manufacturer, or otherwise does not necessarily constitute or imply its endorsement, recommendation, or favoring by the United States Government or any agency thereof. The views and opinions of authors expressed herein do not necessarily state or reflect those of the United States Government or any agency thereof.

Keywords

kinetics
oxides
phase transformations
synthesis

Access to Document

10.1111/jace.17750

Cite this

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title = "Synthesis method comparison of compositionally complex rare earth-based Ruddlesden–Popper n = 1 T′-type cuprates",

abstract = "The multicomponent approach has been successfully expanded to the Ruddlesden–Popper structure with the synthesis of two different high-entropy cuprate compositions: (La0.2Nd0.2Gd0.2Tb0.2Dy0.2)2CuO4 and (La0.2Pr0.2Nd0.2Sm0.2Eu0.2)2CuO4. The effect of synthesis method is explored using both solid-state reaction and polymeric steric entrapment (PSE) methods. It is found that PSE leads to more randomly distributed cation species, providing an advantageous method of synthesis for the growing field of high entropy oxides. In situ high-temperature x-ray diffraction tracks the amorphous to crystalline phase transformation in (La0.2Nd0.2Gd0.2Tb0.2Dy0.2)2CuO4 powder, synthesized using the PSE method. Using the High-Temperature XRD data, a method for gaining information on the kinetic behavior is also applied. Magnetometry of both compositions indicates ferrimagnetic behavior at low temperatures.",

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author = "Music{\'o}, {Brianna L.} and Quinton Wright and Cordell Delzer and Ward, {T. Zac} and Rawn, {Claudia J.} and Mandrus, {David G.} and Veerle Keppens",

note = "Publisher Copyright: {\textcopyright} 2021 The American Ceramic Society",

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AU - Musicó, Brianna L.

AU - Wright, Quinton

AU - Delzer, Cordell

AU - Ward, T. Zac

AU - Rawn, Claudia J.

AU - Mandrus, David G.

AU - Keppens, Veerle

PY - 2021/7

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N2 - The multicomponent approach has been successfully expanded to the Ruddlesden–Popper structure with the synthesis of two different high-entropy cuprate compositions: (La0.2Nd0.2Gd0.2Tb0.2Dy0.2)2CuO4 and (La0.2Pr0.2Nd0.2Sm0.2Eu0.2)2CuO4. The effect of synthesis method is explored using both solid-state reaction and polymeric steric entrapment (PSE) methods. It is found that PSE leads to more randomly distributed cation species, providing an advantageous method of synthesis for the growing field of high entropy oxides. In situ high-temperature x-ray diffraction tracks the amorphous to crystalline phase transformation in (La0.2Nd0.2Gd0.2Tb0.2Dy0.2)2CuO4 powder, synthesized using the PSE method. Using the High-Temperature XRD data, a method for gaining information on the kinetic behavior is also applied. Magnetometry of both compositions indicates ferrimagnetic behavior at low temperatures.

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