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Title: Giant Ferroelectric Polarization in Ultrathin Ferroelectrics via Boundary-Condition Engineering

Abstract

Tailoring and enhancing the functional properties of materials at reduced dimension is critical for continuous advancement of modern electronic devices. Here, the discovery of local surface induced giant spontaneous polarization in ultrathin BiFeO 3 ferroelectric films is reported. Using aberration‐corrected scanning transmission electron microscopy, it is found that the spontaneous polarization in a 2 nm‐thick ultrathin BiFeO 3 film is abnormally increased up to ≈90–100 µC cm −2 in the out‐of‐plane direction and a peculiar rumpled nanodomain structure with very large variation in c / a ratios, which is analogous to morphotropic phase boundaries (MPBs), is formed. By a combination of density functional theory and phase‐field calculations, it is shown that it is the unique single atomic Bi 2 O 3 x layer at the surface that leads to the enhanced polarization and appearance of the MPB‐like nanodomain structure. This finding clearly demonstrates a novel route to the enhanced functional properties in the material system with reduced dimension via engineering the surface boundary conditions.

Authors:
 [1];  [2];  [3];  [2];  [4];  [5];  [5];  [4];  [5];  [4];  [3];  [6];  [1]
  1. Univ. of California, Irvine, CA (United States). Dept. of Chemical Engineering and Materials Science; Nanjing Univ. (China). National Lab. of Solid State Microstructures. College of Engineering and Applied Sciences
  2. Univ. of California, Irvine, CA (United States). Dept. of Chemical Engineering and Materials Science
  3. Cornell Univ., Ithaca, NY (United States). Dept. of Materials Science and Engineering
  4. Pennsylvania State Univ., University Park, PA (United States). Dept. of Materials Science and Engineering
  5. Univ. of Michigan, Ann Arbor, MI (United States). Dept. of Materials Science and Engineering
  6. Nanjing Univ. (China). National Lab. of Solid State Microstructures. College of Engineering and Applied Sciences
Publication Date:
Research Org.:
Pennsylvania State Univ., University Park, PA (United States); Cornell Univ., Ithaca, NY (United States); Univ. of California, Irvine, CA (United States); Nanjing Univ. (China)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); National Basic Research Program of China; National Natural Science Foundation of China (NSFC)
OSTI Identifier:
1533044
Alternate Identifier(s):
OSTI ID: 1374090
Grant/Contract Number:  
FG02-07ER46417; SC0002334; SC0014430; AC02-05CH11231; DMR-1210588; DMR-1420620; ECCS-0335765; 2015CB654901; 51302132; 11474147
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Materials
Additional Journal Information:
Journal Volume: 29; Journal Issue: 30; Journal ID: ISSN 0935-9648
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; polarization; scanning transmission electron microscopy; surface effect; ultrathin ferroelectric films

Citation Formats

Xie, Lin, Li, Linze, Heikes, Colin A., Zhang, Yi, Hong, Zijian, Gao, Peng, Nelson, Christopher T., Xue, Fei, Kioupakis, Emmanouil, Chen, Longqing, Schlom, Darrel G., Wang, Peng, and Pan, Xiaoqing. Giant Ferroelectric Polarization in Ultrathin Ferroelectrics via Boundary-Condition Engineering. United States: N. p., 2017. Web. doi:10.1002/adma.201701475.
Xie, Lin, Li, Linze, Heikes, Colin A., Zhang, Yi, Hong, Zijian, Gao, Peng, Nelson, Christopher T., Xue, Fei, Kioupakis, Emmanouil, Chen, Longqing, Schlom, Darrel G., Wang, Peng, & Pan, Xiaoqing. Giant Ferroelectric Polarization in Ultrathin Ferroelectrics via Boundary-Condition Engineering. United States. https://doi.org/10.1002/adma.201701475
Xie, Lin, Li, Linze, Heikes, Colin A., Zhang, Yi, Hong, Zijian, Gao, Peng, Nelson, Christopher T., Xue, Fei, Kioupakis, Emmanouil, Chen, Longqing, Schlom, Darrel G., Wang, Peng, and Pan, Xiaoqing. Tue . "Giant Ferroelectric Polarization in Ultrathin Ferroelectrics via Boundary-Condition Engineering". United States. https://doi.org/10.1002/adma.201701475. https://www.osti.gov/servlets/purl/1533044.
@article{osti_1533044,
title = {Giant Ferroelectric Polarization in Ultrathin Ferroelectrics via Boundary-Condition Engineering},
author = {Xie, Lin and Li, Linze and Heikes, Colin A. and Zhang, Yi and Hong, Zijian and Gao, Peng and Nelson, Christopher T. and Xue, Fei and Kioupakis, Emmanouil and Chen, Longqing and Schlom, Darrel G. and Wang, Peng and Pan, Xiaoqing},
abstractNote = {Tailoring and enhancing the functional properties of materials at reduced dimension is critical for continuous advancement of modern electronic devices. Here, the discovery of local surface induced giant spontaneous polarization in ultrathin BiFeO 3 ferroelectric films is reported. Using aberration‐corrected scanning transmission electron microscopy, it is found that the spontaneous polarization in a 2 nm‐thick ultrathin BiFeO 3 film is abnormally increased up to ≈90–100 µC cm −2 in the out‐of‐plane direction and a peculiar rumpled nanodomain structure with very large variation in c / a ratios, which is analogous to morphotropic phase boundaries (MPBs), is formed. By a combination of density functional theory and phase‐field calculations, it is shown that it is the unique single atomic Bi 2 O 3 − x layer at the surface that leads to the enhanced polarization and appearance of the MPB‐like nanodomain structure. This finding clearly demonstrates a novel route to the enhanced functional properties in the material system with reduced dimension via engineering the surface boundary conditions.},
doi = {10.1002/adma.201701475},
journal = {Advanced Materials},
number = 30,
volume = 29,
place = {United States},
year = {Tue Jun 06 00:00:00 EDT 2017},
month = {Tue Jun 06 00:00:00 EDT 2017}
}

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