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Title: Infrared nano-spectroscopy of ferroelastic domain walls in hybrid improper ferroelectric Ca 3Ti 2O 7

Abstract

Ferroic materials are well known to exhibit heterogeneity in the form of domain walls. Understanding the properties of these boundaries is crucial for controlling functionality with external stimuli and for realizing their potential for ultra-low power memory and logic devices as well as novel computing architectures. In this work, we employ synchrotron-based near-field infrared nano-spectroscopy to reveal the vibrational properties of ferroelastic (90° ferroelectric) domain walls in the hybrid improper ferroelectric Ca 3Ti 2O 7. By locally mapping the Ti-O stretching and Ti-O-Ti bending modes, we reveal how structural order parameters rotate across a wall. Thus, we link observed near-field amplitude changes to underlying structural modulations and test ferroelectric switching models against real space measurements of local structure. This initiative opens the door to broadband infrared nano-imaging of heterogeneity in ferroics.

Authors:
ORCiD logo [1];  [2];  [1]; ORCiD logo [3];  [4]; ORCiD logo [4]; ORCiD logo [1];  [1];  [1]; ORCiD logo [5]; ORCiD logo [6];  [7];  [8]; ORCiD logo [9];  [10];  [5]; ORCiD logo [1]
  1. Univ. of Tennessee, Knoxville, TN (United States)
  2. New Jersey Institute of Technology, Newark, NJ (United States); Cornell Univ., Ithaca, NY (United States); Univ. of California, Merced, CA (United States)
  3. Univ. of Colorado, Boulder, CO (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
  4. Rutgers Univ., Piscataway, NJ (United States)
  5. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
  6. Pohang Accelerator Lab. (PAL) (Korea, Republic of); Pohang Univ. of Science and Technology (POSTECH) (Korea, Republic of)
  7. Univ. of Colorado, Boulder, CO (United States)
  8. Rutgers Univ., Piscataway, NJ (United States); Pohang Accelerator Lab. (PAL) (Korea, Republic of); Pohang Univ. of Science and Technology (POSTECH) (Korea, Republic of)
  9. Cornell Univ., Ithaca, NY (United States)
  10. Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division
OSTI Identifier:
1579491
Report Number(s):
BNL-212398-2019-JAAM
Journal ID: ISSN 2041-1723
Grant/Contract Number:  
SC0012704; FG02-01ER45885; AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 10; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Smith, K. A., Nowadnick, E. A., Fan, S., Khatib, O., Lim, S. J., Gao, B., Harms, N. C., Neal, S. N., Kirkland, J. K., Martin, M. C., Won, C. J., Raschke, M. B., Cheong, S. -W., Fennie, C. J., Carr, G. L., Bechtel, H. A., and Musfeldt, J. L. Infrared nano-spectroscopy of ferroelastic domain walls in hybrid improper ferroelectric Ca3Ti2O7. United States: N. p., 2019. Web. doi:10.1038/s41467-019-13066-9.
Smith, K. A., Nowadnick, E. A., Fan, S., Khatib, O., Lim, S. J., Gao, B., Harms, N. C., Neal, S. N., Kirkland, J. K., Martin, M. C., Won, C. J., Raschke, M. B., Cheong, S. -W., Fennie, C. J., Carr, G. L., Bechtel, H. A., & Musfeldt, J. L. Infrared nano-spectroscopy of ferroelastic domain walls in hybrid improper ferroelectric Ca3Ti2O7. United States. doi:10.1038/s41467-019-13066-9.
Smith, K. A., Nowadnick, E. A., Fan, S., Khatib, O., Lim, S. J., Gao, B., Harms, N. C., Neal, S. N., Kirkland, J. K., Martin, M. C., Won, C. J., Raschke, M. B., Cheong, S. -W., Fennie, C. J., Carr, G. L., Bechtel, H. A., and Musfeldt, J. L. Wed . "Infrared nano-spectroscopy of ferroelastic domain walls in hybrid improper ferroelectric Ca3Ti2O7". United States. doi:10.1038/s41467-019-13066-9. https://www.osti.gov/servlets/purl/1579491.
@article{osti_1579491,
title = {Infrared nano-spectroscopy of ferroelastic domain walls in hybrid improper ferroelectric Ca3Ti2O7},
author = {Smith, K. A. and Nowadnick, E. A. and Fan, S. and Khatib, O. and Lim, S. J. and Gao, B. and Harms, N. C. and Neal, S. N. and Kirkland, J. K. and Martin, M. C. and Won, C. J. and Raschke, M. B. and Cheong, S. -W. and Fennie, C. J. and Carr, G. L. and Bechtel, H. A. and Musfeldt, J. L.},
abstractNote = {Ferroic materials are well known to exhibit heterogeneity in the form of domain walls. Understanding the properties of these boundaries is crucial for controlling functionality with external stimuli and for realizing their potential for ultra-low power memory and logic devices as well as novel computing architectures. In this work, we employ synchrotron-based near-field infrared nano-spectroscopy to reveal the vibrational properties of ferroelastic (90° ferroelectric) domain walls in the hybrid improper ferroelectric Ca3Ti2O7. By locally mapping the Ti-O stretching and Ti-O-Ti bending modes, we reveal how structural order parameters rotate across a wall. Thus, we link observed near-field amplitude changes to underlying structural modulations and test ferroelectric switching models against real space measurements of local structure. This initiative opens the door to broadband infrared nano-imaging of heterogeneity in ferroics.},
doi = {10.1038/s41467-019-13066-9},
journal = {Nature Communications},
number = 1,
volume = 10,
place = {United States},
year = {2019},
month = {11}
}

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