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Double-Bilayer polar nanoregions and Mn antisites in (Ca, Sr)3Mn2O7

Author

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  • Leixin Miao

    (The Pennsylvania State University)

  • Kishwar-E Hasin

    (University of California)

  • Parivash Moradifar

    (The Pennsylvania State University
    Stanford University)

  • Debangshu Mukherjee

    (Oak Ridge National Laboratory)

  • Ke Wang

    (The Pennsylvania State University)

  • Sang-Wook Cheong

    (Rutgers University)

  • Elizabeth A. Nowadnick

    (University of California)

  • Nasim Alem

    (The Pennsylvania State University
    The Pennsylvania State University)

Abstract

The layered perovskite Ca3Mn2O7 (CMO) is a hybrid improper ferroelectric candidate proposed for room temperature multiferroicity, which also displays negative thermal expansion behavior due to a competition between coexisting polar and nonpolar phases. However, little is known about the atomic-scale structure of the polar/nonpolar phase coexistence or the underlying physics of its formation and transition. In this work, we report the direct observation of double bilayer polar nanoregions (db-PNRs) in Ca2.9Sr0.1Mn2O7 using aberration-corrected scanning transmission electron microscopy (S/TEM). In-situ TEM heating experiments show that the db-PNRs can exist up to 650 °C. Electron energy loss spectroscopy (EELS) studies coupled with first-principles calculations demonstrate that the stabilization mechanism of the db-PNRs is directly related to an Mn oxidation state change (from 4+ to 2+), which is linked to the presence of Mn antisite defects. These findings open the door to manipulating phase coexistence and achieving exotic properties in hybrid improper ferroelectric.

Suggested Citation

  • Leixin Miao & Kishwar-E Hasin & Parivash Moradifar & Debangshu Mukherjee & Ke Wang & Sang-Wook Cheong & Elizabeth A. Nowadnick & Nasim Alem, 2022. "Double-Bilayer polar nanoregions and Mn antisites in (Ca, Sr)3Mn2O7," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
  • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-32090-w
    DOI: 10.1038/s41467-022-32090-w
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    References listed on IDEAS

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    2. Matteo Rini & Ra'anan Tobey & Nicky Dean & Jiro Itatani & Yasuhide Tomioka & Yoshinori Tokura & Robert W. Schoenlein & Andrea Cavalleri, 2007. "Control of the electronic phase of a manganite by mode-selective vibrational excitation," Nature, Nature, vol. 449(7158), pages 72-74, September.
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