Site-specific spectroscopic measurement of spin and charge in (LuFeO3)m/(LuFe2O4)1 multiferroic superlattices

Shiyu Fan, Hena Das, Alejandro Rébola, Kevin A. Smith, Julia Mundy, Charles Brooks, Megan E. Holtz, David A. Muller, Craig J. Fennie, Ramamoorthy Ramesh, Darrell G. Schlom, Stephen McGill and Janice L. Musfeldt ()
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Shiyu Fan: University of Tennessee
Hena Das: Cornell University
Alejandro Rébola: Instituto de Física Rosario-CONICET, Boulevard 27 de Febrero 210 bis
Kevin A. Smith: University of Tennessee
Julia Mundy: Cornell University
Charles Brooks: Cornell University
Megan E. Holtz: Cornell University
David A. Muller: Cornell University
Craig J. Fennie: Cornell University
Ramamoorthy Ramesh: University of California
Darrell G. Schlom: Cornell University
Stephen McGill: National High Magnetic Field Laboratory
Janice L. Musfeldt: University of Tennessee

Nature Communications, 2020, vol. 11, issue 1, 1-9

Abstract: Abstract Interface materials offer a means to achieve electrical control of ferrimagnetism at room temperature as was recently demonstrated in (LuFeO3)m/(LuFe2O4)1 superlattices. A challenge to understanding the inner workings of these complex magnetoelectric multiferroics is the multitude of distinct Fe centres and their associated environments. This is because macroscopic techniques characterize average responses rather than the role of individual iron centres. Here, we combine optical absorption, magnetic circular dichroism and first-principles calculations to uncover the origin of high-temperature magnetism in these superlattices and the charge-ordering pattern in the m = 3 member. In a significant conceptual advance, interface spectra establish how Lu-layer distortion selectively enhances the Fe2+ → Fe3+ charge-transfer contribution in the spin-up channel, strengthens the exchange interactions and increases the Curie temperature. Comparison of predicted and measured spectra also identifies a non-polar charge ordering arrangement in the LuFe2O4 layer. This site-specific spectroscopic approach opens the door to understanding engineered materials with multiple metal centres and strong entanglement.

Date: 2020
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DOI: 10.1038/s41467-020-19285-9

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