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Title: Phase coexistence and electric-field control of toroidal order in oxide superlattices

Abstract

Systems that exhibit phase competition, order parameter coexistence, and emergent order parameter topologies constitute a major part of modern condensed-matter physics. Here, by applying a range of characterization techniques, and simulations, we observe that in PbTiO3/SrTiO3 superlattices all of these effects can be found. By exploring superlattice period-, temperature- and field-dependent evolution of these structures, we observe several new features. First, it is possible to engineer phase coexistence mediated by a first-order phase transition between an emergent, low-temperature vortex phase with electric toroidal order and a high-temperature ferroelectric a1/a2 phase. At room temperature, the coexisting vortex and ferroelectric phases form a mesoscale, fibre-textured hierarchical superstructure. The vortex phase possesses an axial polarization, set by the net polarization of the surrounding ferroelectric domains, such that it possesses a multi-order-parameter state and belongs to a class of gyrotropic electrotoroidal compounds. Finally, application of electric fields to this mixed-phase system permits interconversion between the vortex and the ferroelectric phases concomitant with order-of-magnitude changes in piezoelectric and nonlinear optical responses. Our findings suggest new cross-coupled functionalities.

Authors:
ORCiD logo [1];  [1];  [2];  [3]; ORCiD logo [1];  [1];  [1];  [4];  [5]; ORCiD logo [5]; ORCiD logo [6];  [3];  [3];  [3];  [7];  [8];  [9]; ORCiD logo [8];  [6];  [5] more »;  [2];  [3];  [1]; ORCiD logo [1] « less
+ Show Author Affiliations
  1. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  2. Pennsylvania State Univ., University Park, PA (United States)
  3. Argonne National Lab. (ANL), Argonne, IL (United States)
  4. Univ. of California, Berkeley, CA (United States)
  5. Univ. of Colorado, Boulder, CO (United States)
  6. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  7. Univ. del Pais Vasco, San Sebastian (Spain); Donostia International Physics Center, San Sebastian (Spain)
  8. Univ. de Cantabria, Santander (Spain)
  9. Luxembourg Institute of Science and Technology (LIST), Esch/Alzette (Luxembourg)
Publication Date:
Research Org.:
Argonne National Laboratory (ANL), Argonne, IL (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; U.S. Army Research Office (ARO); National Science Foundation (NSF); Swiss National Science Foundation (SNSF); Spanish Ministerio de Economia y Competitividad (MINECO); Luxembourg National Research Fund; Gordon and Betty Moore Foundation
OSTI Identifier:
1400404
Alternate Identifier(s):
OSTI ID: 1637274
Grant/Contract Number:  
AC02-06CH11357; SC0012375; AC02-05CH11231; SC0008807; FG02-07ER46417; W911NF-14-1-0104; DMR-1420620; DMR-1210588; DGE-1106400; FIS2015-64886-C5-2-P; FNR/C15/MS/10458889-NEWALLS; GBMF5307
Resource Type:
Accepted Manuscript
Journal Name:
Nature Materials
Additional Journal Information:
Journal Volume: 16; Journal Issue: 10; Journal ID: ISSN 1476-1122
Publisher:
Springer Nature - Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY

Citation Formats

Damodaran, A. R., Clarkson, J. D., Hong, Z., Liu, H., Yadav, A. K., Nelson, C. T., Hsu, S. -L., McCarter, M.  R., Park, K. -D., Kravtsov, V., Farhan, A., Dong, Y., Cai, Z., Zhou, H., Aguado-Puente, P., Garcia-Fernandez, P., Iniguez, J., Junquera, J., Scholl, A., Raschke, M. B., Chen, L. -Q., Fong, D. D., Ramesh, R., and Martin, L. W. Phase coexistence and electric-field control of toroidal order in oxide superlattices. United States: N. p., 2017. Web. doi:10.1038/NMAT4951.
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Damodaran, A. R., Clarkson, J. D., Hong, Z., Liu, H., Yadav, A. K., Nelson, C. T., Hsu, S. -L., McCarter, M.  R., Park, K. -D., Kravtsov, V., Farhan, A., Dong, Y., Cai, Z., Zhou, H., Aguado-Puente, P., Garcia-Fernandez, P., Iniguez, J., Junquera, J., Scholl, A., Raschke, M. B., Chen, L. -Q., Fong, D. D., Ramesh, R., & Martin, L. W. Phase coexistence and electric-field control of toroidal order in oxide superlattices. United States. https://doi.org/10.1038/NMAT4951
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Damodaran, A. R., Clarkson, J. D., Hong, Z., Liu, H., Yadav, A. K., Nelson, C. T., Hsu, S. -L., McCarter, M.  R., Park, K. -D., Kravtsov, V., Farhan, A., Dong, Y., Cai, Z., Zhou, H., Aguado-Puente, P., Garcia-Fernandez, P., Iniguez, J., Junquera, J., Scholl, A., Raschke, M. B., Chen, L. -Q., Fong, D. D., Ramesh, R., and Martin, L. W. Mon . "Phase coexistence and electric-field control of toroidal order in oxide superlattices". United States. https://doi.org/10.1038/NMAT4951. https://www.osti.gov/servlets/purl/1400404.
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@article{osti_1400404,
title = {Phase coexistence and electric-field control of toroidal order in oxide superlattices},
author = {Damodaran, A. R. and Clarkson, J. D. and Hong, Z. and Liu, H. and Yadav, A. K. and Nelson, C. T. and Hsu, S. -L. and McCarter, M.  R. and Park, K. -D. and Kravtsov, V. and Farhan, A. and Dong, Y. and Cai, Z. and Zhou, H. and Aguado-Puente, P. and Garcia-Fernandez, P. and Iniguez, J. and Junquera, J. and Scholl, A. and Raschke, M. B. and Chen, L. -Q. and Fong, D. D. and Ramesh, R. and Martin, L. W.},
abstractNote = {Systems that exhibit phase competition, order parameter coexistence, and emergent order parameter topologies constitute a major part of modern condensed-matter physics. Here, by applying a range of characterization techniques, and simulations, we observe that in PbTiO3/SrTiO3 superlattices all of these effects can be found. By exploring superlattice period-, temperature- and field-dependent evolution of these structures, we observe several new features. First, it is possible to engineer phase coexistence mediated by a first-order phase transition between an emergent, low-temperature vortex phase with electric toroidal order and a high-temperature ferroelectric a1/a2 phase. At room temperature, the coexisting vortex and ferroelectric phases form a mesoscale, fibre-textured hierarchical superstructure. The vortex phase possesses an axial polarization, set by the net polarization of the surrounding ferroelectric domains, such that it possesses a multi-order-parameter state and belongs to a class of gyrotropic electrotoroidal compounds. Finally, application of electric fields to this mixed-phase system permits interconversion between the vortex and the ferroelectric phases concomitant with order-of-magnitude changes in piezoelectric and nonlinear optical responses. Our findings suggest new cross-coupled functionalities.},
doi = {10.1038/NMAT4951},
journal = {Nature Materials},
number = 10,
volume = 16,
place = {United States},
year = {Mon Aug 07 00:00:00 EDT 2017},
month = {Mon Aug 07 00:00:00 EDT 2017}
}
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https://doi.org/10.1038/NMAT4951
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Cited by: 134 works
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Figures / Tables:

Figure 1 Figure 1: Structural evolution of ferroelectric and vortex phases with superlattice periodicity. a, High resolution θ-2θ scans of 100 nm thick (PbTiO3)n/(SrTiO3)n superlattices grown on DyScO3 (001)pc substrates for n = 4, 6, 10, 14 and 16 (top to bottom, respectively) revealing evolution from a single a1/a2 alloy peak andmore » corresponding superlattice peaks at short periodicities to mixed phase films revealing an extra set of alloy and superlattice peaks corresponding to the vortex (V) phase. Three-dimensional, synchrotron-based symmetric reciprocal space maps about the 002pc-diffraction condition of the DyScO3 substrate containing the in-plane [010]pc and out-of-plane [001]pc confirming b, single a1/a2 alloy peak and corresponding superlattice peaks at n = 4, and c, mixed-phase coexistence for n = 16 showing additional set of alloy and superlattice peaks corresponding to the vortex phase along with the appearance of characteristic satellite peaks corresponding to an in-plane periodicity of ~11 nm along the in-plane [010]pc direction. d, 2D intensity color-map summarizing temperature-dependent synchrotron X-ray diffraction θ-2θ scans about the 002pc-diffraction condition of the DyScO3 substrate, and e, a plot of the ratio of diffracted beam intensity from a vortex superlattice peak (IV(1)) to the a1/a2 superlattice peak (IF(1)) revealing hysteresis indicative of a first-order phase transition from the vortex-phase to the a1/a2 phase at ~200°C.« less
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