Emergent interface vibrational structure of oxide superlattices

Eric R. Hoglund (), Bao De-Liang, Andrew O’Hara, Sara Makarem, Zachary T. Piontkowski, Joseph R. Matson, Ajay K. Yadav, Ryan C. Haislmaier, Roman Engel-Herbert, Jon F. Ihlefeld, Jayakanth Ravichandran, Ramamoorthy Ramesh, Joshua D. Caldwell, Thomas E. Beechem, John A. Tomko, Jordan A. Hachtel (), Sokrates T. Pantelides (), Patrick E. Hopkins () and James M. Howe ()
Additional contact information
Eric R. Hoglund: University of Virginia
Bao De-Liang: Vanderbilt University
Andrew O’Hara: Vanderbilt University
Sara Makarem: University of Virginia
Zachary T. Piontkowski: Sandia National Laboratories
Joseph R. Matson: Vanderbilt University
Ajay K. Yadav: University of California Berkley
Ryan C. Haislmaier: Pennsylvania State University
Roman Engel-Herbert: Paul-Drude-Institut für Festkörperelektronik
Jon F. Ihlefeld: University of Virginia
Jayakanth Ravichandran: University of Southern California
Ramamoorthy Ramesh: University of California Berkley
Joshua D. Caldwell: Vanderbilt University
Thomas E. Beechem: Sandia National Laboratories
John A. Tomko: University of Virginia
Jordan A. Hachtel: Center for Nanophase Materials Sciences, Oak Ridge National Laboratory
Sokrates T. Pantelides: Vanderbilt University
Patrick E. Hopkins: University of Virginia
James M. Howe: University of Virginia

Nature, 2022, vol. 601, issue 7894, 556-561

Abstract: Abstract As the length scales of materials decrease, the heterogeneities associated with interfaces become almost as important as the surrounding materials. This has led to extensive studies of emergent electronic and magnetic interface properties in superlattices1–9. However, the interfacial vibrations that affect the phonon-mediated properties, such as thermal conductivity10,11, are measured using macroscopic techniques that lack spatial resolution. Although it is accepted that intrinsic phonons change near boundaries12,13, the physical mechanisms and length scales through which interfacial effects influence materials remain unclear. Here we demonstrate the localized vibrational response of interfaces in strontium titanate–calcium titanate superlattices by combining advanced scanning transmission electron microscopy imaging and spectroscopy, density functional theory calculations and ultrafast optical spectroscopy. Structurally diffuse interfaces that bridge the bounding materials are observed and this local structure creates phonon modes that determine the global response of the superlattice once the spacing of the interfaces approaches the phonon spatial extent. Our results provide direct visualization of the progression of the local atomic structure and interface vibrations as they come to determine the vibrational response of an entire superlattice. Direct observation of such local atomic and vibrational phenomena demonstrates that their spatial extent needs to be quantified to understand macroscopic behaviour. Tailoring interfaces, and knowing their local vibrational response, provides a means of pursuing designer solids with emergent infrared and thermal responses.

Date: 2022
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DOI: 10.1038/s41586-021-04238-z

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