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Title: Reducing Coercive-Field Scaling in Ferroelectric Thin Films via Orientation Control

Journal Article · · ACS Nano
ORCiD logo [1];  [1];  [2];  [1];  [3];  [1]; ORCiD logo [1];  [4];  [5];  [6];  [1];  [7];  [8]; ORCiD logo [6]
  1. Univ. of California, Berkeley, CA (United States)
  2. Univ. Andres Bello, Santiago (Chile); Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  3. Univ. of Science and Technology of China, Hefei (China)
  4. Harbin Institute of Technology, Harbin (China)
  5. Hubei Univ., Wuhan (China)
  6. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  7. Argonne National Lab. (ANL), Argonne, IL (United States)
  8. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Kavli Energy NanoScience Institute at Berkeley, CA (United States)

The desire for low-power/voltage operation of devices is driving renewed interest in understanding scaling effects in ferroelectric thin films. As the dimensions of ferroelectrics are reduced, the properties can vary dramatically, including the robust scaling relationship between coercive field (Ec) and thickness (d), also referred to as the Janovec-Kay-Dunn (JKD) law, wherein Ec ∝ d-2/3. Here, we report that whereas (001)-oriented heterostructures follow JKD scaling across the thicknesses range of 20-330 nm, (111)-oriented heterostructures of the canonical tetragonal ferroelectric PbZr0.2Ti0.8O3 exhibit a deviation from JKD scaling wherein a smaller scaling exponent for the evolution of Ec is observed in films of thickness ≤ 165 nm. X-ray diffraction reveals that whereas (001)-oriented heterostructures remain tetragonal for all thicknesses, (111)-oriented heterostructures exhibit a transition from tetragonal-to-monoclinic symmetry in films of thickness ≤ 165 nm as a result of the compressive strain. First-principles calculations suggest that this symmetry change contributes to the deviation from the expected scaling, as the monoclinic phase has a lower energy barrier for switching. This structural evolution also gives rise to changes in the c/a lattice parameter ratio, wherein this ratio increases and decreases in (001)- and (111)-oriented heterostructures, respectively, as the films are made thinner. In (111)-oriented heterostructures, this reduced tetragonality drives a reduction of the remanent polarization and, therefore, a reduction of the domain-wall energy and overall energy barrier to switching, which further exacerbates the deviation from the expected scaling. Altogether, this work demonstrates a route toward reducing coercive fields in ferroelectric thin films and provides a possible mechanism to understand the deviation from JKD scaling.

Research Organization:
Argonne National Lab. (ANL), Argonne, IL (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC02-06CH11357; AC02-05CH11231
OSTI ID:
1466327
Alternate ID(s):
OSTI ID: 1462002
Journal Information:
ACS Nano, Vol. 12, Issue 5; ISSN 1936-0851
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 32 works
Citation information provided by
Web of Science

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Cited By (2)

Obvious ferroelectricity in undoped HfO 2 films by chemical solution deposition journal January 2020
Progress, Outlook, and Challenges in Lead‐Free Energy‐Storage Ferroelectrics journal December 2019

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