Site-specific spectroscopic measurement of spin and charge in (LuFeO3)m/(LuFe2O4)1 multiferroic superlattices
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.
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Univ. of Tennessee, Knoxville, TN (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; National Science Foundation (NSF); Japan Society for the Promotion of Science (JSPS); USDOE
- OSTI Identifier:
- 1702282
- Alternate Identifier(s):
- OSTI ID: 1764547; OSTI ID: 1831752; OSTI ID: 1865805
- Grant/Contract Number:
- AC02-05CH11231; FG02-01ER45885; SC0002334; DMR-1644779; DMR-1229217; DMR-1719875; DMR-1539918; 19K05246
- Resource Type:
- Published Article
- Journal Name:
- Nature Communications
- Additional Journal Information:
- Journal Name: Nature Communications Journal Volume: 11 Journal Issue: 1; Journal ID: ISSN 2041-1723
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United Kingdom
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; multiferroic superlattices; interface effects; multiferroic superlattices, interface effects, magnetic circular dichroism, high temperature magnetism, charge ordering pattern
Citation Formats
Fan, Shiyu, Das, Hena, Rébola, Alejandro, Smith, Kevin A., Mundy, Julia, Brooks, Charles, Holtz, Megan E., Muller, David A., Fennie, Craig J., Ramesh, Ramamoorthy, Schlom, Darrell G., McGill, Stephen, and Musfeldt, Janice L. Site-specific spectroscopic measurement of spin and charge in (LuFeO3)m/(LuFe2O4)1 multiferroic superlattices. United Kingdom: N. p., 2020.
Web. doi:10.1038/s41467-020-19285-9.
Fan, Shiyu, Das, Hena, Rébola, Alejandro, Smith, Kevin A., Mundy, Julia, Brooks, Charles, Holtz, Megan E., Muller, David A., Fennie, Craig J., Ramesh, Ramamoorthy, Schlom, Darrell G., McGill, Stephen, & Musfeldt, Janice L. Site-specific spectroscopic measurement of spin and charge in (LuFeO3)m/(LuFe2O4)1 multiferroic superlattices. United Kingdom. https://doi.org/10.1038/s41467-020-19285-9
Fan, Shiyu, Das, Hena, Rébola, Alejandro, Smith, Kevin A., Mundy, Julia, Brooks, Charles, Holtz, Megan E., Muller, David A., Fennie, Craig J., Ramesh, Ramamoorthy, Schlom, Darrell G., McGill, Stephen, and Musfeldt, Janice L. Wed .
"Site-specific spectroscopic measurement of spin and charge in (LuFeO3)m/(LuFe2O4)1 multiferroic superlattices". United Kingdom. https://doi.org/10.1038/s41467-020-19285-9.
@article{osti_1702282,
title = {Site-specific spectroscopic measurement of spin and charge in (LuFeO3)m/(LuFe2O4)1 multiferroic superlattices},
author = {Fan, Shiyu and Das, Hena and Rébola, Alejandro and Smith, Kevin A. and Mundy, Julia and Brooks, Charles and Holtz, Megan E. and Muller, David A. and Fennie, Craig J. and Ramesh, Ramamoorthy and Schlom, Darrell G. and McGill, Stephen and Musfeldt, Janice L.},
abstractNote = {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.},
doi = {10.1038/s41467-020-19285-9},
journal = {Nature Communications},
number = 1,
volume = 11,
place = {United Kingdom},
year = {Wed Nov 04 00:00:00 EST 2020},
month = {Wed Nov 04 00:00:00 EST 2020}
}
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Works referenced in this record:
Complex magnetic phases in
journal, February 2010
- Phan, M. H.; Frey, N. A.; Angst, M.
- Solid State Communications, Vol. 150, Issue 7-8
Imaging and tuning polarity at SrTiO3 domain walls
journal, September 2017
- Frenkel, Yiftach; Haham, Noam; Shperber, Yishai
- Nature Materials, Vol. 16, Issue 12
Artificially engineered superlattices of pnictide superconductors
journal, March 2013
- Lee, S.; Tarantini, C.; Gao, P.
- Nature Materials, Vol. 12, Issue 5
Formation of Pancakelike Ising Domains and Giant Magnetic Coercivity in Ferrimagnetic
journal, September 2008
- Wu, Weida; Kiryukhin, V.; Noh, H. -J.
- Physical Review Letters, Vol. 101, Issue 13
Spatially resolved steady-state negative capacitance
journal, January 2019
- Yadav, Ajay K.; Nguyen, Kayla X.; Hong, Zijian
- Nature, Vol. 565, Issue 7740
Unusual temperature dependence of the magnetic anisotropy constant in barium ferrite BaFe 12 O 19
journal, November 2011
- Wang, Jun; Zhao, Fan; Wu, Wei
- Journal of Applied Physics, Vol. 110, Issue 9
Improper ferroelectricity in perovskite oxide artificial superlattices
journal, April 2008
- Bousquet, Eric; Dawber, Matthew; Stucki, Nicolas
- Nature, Vol. 452, Issue 7188
Observation of polar vortices in oxide superlattices
journal, January 2016
- Yadav, A. K.; Nelson, C. T.; Hsu, S. L.
- Nature, Vol. 530, Issue 7589
Charge Order in : Antiferroelectric Ground State and Coupling to Magnetism
journal, November 2008
- Angst, M.; Hermann, R. P.; Christianson, A. D.
- Physical Review Letters, Vol. 101, Issue 22
Persistent optically induced magnetism in oxygen-deficient strontium titanate
journal, March 2014
- Rice, W. D.; Ambwani, P.; Bombeck, M.
- Nature Materials, Vol. 13, Issue 5
Charge Order, Dynamics, and Magnetostructural Transition in Multiferroic
journal, November 2008
- Xu, X. S.; Angst, M.; Brinzari, T. V.
- Physical Review Letters, Vol. 101, Issue 22
Observation of room-temperature polar skyrmions
journal, April 2019
- Das, S.; Tang, Y. L.; Hong, Z.
- Nature, Vol. 568, Issue 7752
Bulk magnetoelectricity in the hexagonal manganites and ferrites
journal, January 2014
- Das, Hena; Wysocki, Aleksander L.; Geng, Yanan
- Nature Communications, Vol. 5, Issue 1
Predicting Polarization and Nonlinear Dielectric Response of Arbitrary Perovskite Superlattice Sequences
journal, August 2008
- Wu, Xifan; Stengel, Massimiliano; Rabe, Karin M.
- Physical Review Letters, Vol. 101, Issue 8
Interface-induced phenomena in magnetism
journal, June 2017
- Hellman, Frances; Hoffmann, Axel; Tserkovnyak, Yaroslav
- Reviews of Modern Physics, Vol. 89, Issue 2
Electric Polarization, Magnetoelectric Effect, and Orbital State of a Layered Iron Oxide with Frustrated Geometry
journal, November 2007
- Nagano, A.; Naka, M.; Nasu, J.
- Physical Review Letters, Vol. 99, Issue 21
Magnetic Structure and Ordering of Multiferroic Hexagonal
journal, May 2015
- Disseler, Steven M.; Borchers, Julie A.; Brooks, Charles M.
- Physical Review Letters, Vol. 114, Issue 21
First-principles calculations of optical and magneto-optical properties of and MnAs
journal, November 2009
- Amft, M.; Burkert, T.; Sanyal, B.
- Physica B: Condensed Matter, Vol. 404, Issue 20
The stability and surface termination of hexagonal LuFeO 3
journal, March 2015
- Cao, Shi; Paudel, Tula R.; Sinha, Kishan
- Journal of Physics: Condensed Matter, Vol. 27, Issue 17
Interface Control of Emergent Ferroic Order in Ruddlesden-Popper
journal, December 2011
- Birol, Turan; Benedek, Nicole A.; Fennie, Craig J.
- Physical Review Letters, Vol. 107, Issue 25
Direct band gaps in multiferroic h -LuFeO 3
journal, February 2015
- Holinsworth, B. S.; Mazumdar, D.; Brooks, C. M.
- Applied Physics Letters, Vol. 106, Issue 8
Enhanced ordering temperatures in antiferromagnetic manganite superlattices
journal, October 2009
- May, S. J.; Ryan, P. J.; Robertson, J. L.
- Nature Materials, Vol. 8, Issue 11
Ferroelectric polarization reversal via successive ferroelastic transitions
journal, October 2014
- Xu, Ruijuan; Liu, Shi; Grinberg, Ilya
- Nature Materials, Vol. 14, Issue 1
Coupled Magnetic-Ferroelectric Metal-Insulator Transition in Epitaxially Strained from First Principles
journal, August 2011
- Lee, Jun Hee; Rabe, Karin
- Physical Review Letters, Vol. 107, Issue 6, Article No. 067601
Intrinsic magnetic properties of hexagonal LuFeO 3 and the effects of nonstoichiometry
journal, January 2014
- Moyer, Jarrett A.; Misra, Rajiv; Mundy, Julia A.
- APL Materials, Vol. 2, Issue 1
Colloquium : Emergent properties in plane view: Strong correlations at oxide interfaces
journal, October 2014
- Chakhalian, Jak; Freeland, John W.; Millis, Andrew J.
- Reviews of Modern Physics, Vol. 86, Issue 4
Coupling between octahedral rotations and local polar displacements in / superlattices
journal, May 2014
- Schick, Joseph T.; Jiang, Lai; Saldana-Greco, Diomedes
- Physical Review B, Vol. 89, Issue 19
The adsorption-controlled growth of LuFe 2 O 4 by molecular-beam epitaxy
journal, September 2012
- Brooks, Charles M.; Misra, Rajiv; Mundy, Julia A.
- Applied Physics Letters, Vol. 101, Issue 13
Landau theory of topological defects in multiferroic hexagonal manganites
journal, October 2013
- Artyukhin, Sergey; Delaney, Kris T.; Spaldin, Nicola A.
- Nature Materials, Vol. 13, Issue 1
A high-mobility electron gas at the LaAlO3/SrTiO3 heterointerface
journal, January 2004
- Ohtomo, A.; Hwang, H. Y.
- Nature, Vol. 427, Issue 6973
Atomically engineered ferroic layers yield a room-temperature magnetoelectric multiferroic
journal, September 2016
- Mundy, Julia A.; Brooks, Charles M.; Holtz, Megan E.
- Nature, Vol. 537, Issue 7621
Crossover from incoherent to coherent phonon scattering in epitaxial oxide superlattices
journal, December 2013
- Ravichandran, Jayakanth; Yadav, Ajay K.; Cheaito, Ramez
- Nature Materials, Vol. 13, Issue 2
FEA-Aided Design for a Working Model of a Split Florida-Helix
journal, June 2008
- Toth, J.; Bird, M. D.
- IEEE Transactions on Applied Superconductivity, Vol. 18, Issue 2
Lattice dynamical probe of charge order and antipolar bilayer stacking in
journal, July 2010
- Xu, X. S.; de Groot, J.; Sun, Q. -C.
- Physical Review B, Vol. 82, Issue 1
Ubiquitous strong electron–phonon coupling at the interface of FeSe/SrTiO3
journal, February 2017
- Zhang, Chaofan; Liu, Zhongkai; Chen, Zhuoyu
- Nature Communications, Vol. 8, Issue 1
Charge Order and the Origin of Giant Magnetocapacitance in
journal, June 2007
- Xiang, H. J.; Whangbo, M. -H.
- Physical Review Letters, Vol. 98, Issue 24
Charge Order in : An Unlikely Route to Ferroelectricity
journal, May 2012
- de Groot, J.; Mueller, T.; Rosenberg, R. A.
- Physical Review Letters, Vol. 108, Issue 18
Temperature dependence of coercive field of ZnFe 2 O 4 nanoparticles
journal, March 2012
- Mendonça, E. C.; Jesus, C. B. R.; Folly, W. S. D.
- Journal of Applied Physics, Vol. 111, Issue 5
Modification of Properties of Yttria Stabilized Zirconia Epitaxial Thin Films by Excimer Laser Annealing
journal, December 2014
- Bayati, R.; Molaei, R.; Richmond, A.
- ACS Applied Materials & Interfaces, Vol. 6, Issue 24
Compositional tuning of the strain-induced structural phase transition and of ferromagnetism in Bi 1− x Ba x FeO 3− δ
journal, May 2011
- Bennett, Charlee J. C.; Kim, Hyun Sik; Varela, Maria
- Journal of Materials Research, Vol. 26, Issue 10
Near room-temperature multiferroic materials with tunable ferromagnetic and electrical properties
journal, May 2014
- Zhao, Hong Jian; Ren, Wei; Yang, Yurong
- Nature Communications, Vol. 5, Issue 1
Controlling the Curie temperature in (Ga,Mn)As through location of the Fermi level within the impurity band
journal, February 2012
- Dobrowolska, M.; Tivakornsasithorn, K.; Liu, X.
- Nature Materials, Vol. 11, Issue 5