The 14th China-Japan Symposium on
Ferroelectric Materials and Their Applications(CJFMA14)
Kanazawa, Japan
December 8-9, 2022

Abstract & Technical Book

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CJFMA14 Welcome Message
The 14th China-Japan Symposium on Ferroelectric Materials and Their Applications(CJFMA14) will be held in a hybrid format from December 8 to 9, 2022. The main venue
is in Kanazawa, Japan. On behalf of the Organizing Committee, it is my great pleasure towelcome you to this exciting event.
The CJFMA1 was held from August 19 to 22, 2009 in Dunhuang, China. Since thefirst Symposium, our CJFMA was successfully held annually in Japan and China. The
CJFMA2 was in Kurobe, Japan, the CJFMA3 in Xiangtan, China, the CJFMA4 in
Matsushima, Japan, the CJFMA5 in Suzhou, China, the CJFMA6 in Yamanashi, Japan,
the CJFMA7 in Beijing, China, the CJFMA8 in Tsukuba, Japan, the CJFMA9 in Chengdu,
China, the CJFMA10 in Inuyama, Japan, the CJFMA11 in Nanjing, China, the CJFMA13(hybrid format) in Shenyang, China. The 2021 International Workshop on New Domain
Technology of Ferroelectric Materials and Their Applications (NDTFMA2021) was held
online instead of the CJMAF12 by Toyama Prefectural University, Japan, because of thepandemic outbreak of Covid-19.
Ferroelectric materials, including piezoelectric materials, dielectric materials,
microwave materials, electro-optical materials, electro-caloric materials, and otherrelated materials, are an important class of functional materials that are widely used in
our modern society. New materials, fabrication methods, evaluation methods, devices,
applications, simulations, and theories are also the content of this Symposium.
Japan and China are the two most active countries in the world for ferroelectricmaterials research. The CJFMA is a platform for high-level academic exchange anddeepening friendship between the two countries in the field. More young researchers andstudents are expected to participate our Symposium.
We are very pleased to have 73 contributions (2 plenary talks, 40 invited talks, and31 posters) who submitted their current work to present at this hybrid conference. We
think, this conference will surely be a memorable, successful and grand meeting.

Tomoaki Karaki (Zhiming Chen), Dr.
The Chairperson of CJFMA14
1

Contents
CJFMA14 Welcome Message..........................................................................................1
Contents............................................................................................................................2CJFMA14 Organizing.....................................................................................................3
Oral presenters Guidelines Summary............................................................................4
Poster presenters Guidelines Summary.........................................................................5CJFMA14 Arrangement.................................................................................................6
List of Poster.....................................................................................................................8
Program……………………............................................................................................9
Abstract..........................................................................................................................19
Best Poster Presentation Award……………………...................................................92
Other information..........................................................................................................93

2

CJFMA14 Organizing
Conference Chair:Tomoaki Karaki (Zhiming Chen) (Toyama Prefecture University, Japan),Vice Chair:
Guorong Li (Shanghai Institute of Ceramics, CAS, China)
Advisory Committee:
Xi Yao (Xi'an Jiaotong University, China), T. Tsurumi (Tokyo Institute of Technology,
Japan), Cewen Nan (Tsinghua University, China), S. Wada (Yamanashi University,
Japan)
Academic Committee (arrange in alphabetical order of the surname):
Japan side: J. Akedo, A. Ando, R. Aoyagi, D. Fu, T. Fujii, T. Hoshina, K. Kakimoto, T.
Karaki, Y. Kuroiwa, N. Fujimura, W. Sakamoto, H. Takeda, E. Tokumitsu, S. Tsukada,
R. Wang, W. Wang, M. Yamaguchi, T. Yoshimura,
China side: Dinghua Bao, Xiangming Chen, Yanfeng Chen, Jinrong Cheng, Shuxiang
Dong, Haoshuang Gu, Dong Guo, Yunbin He, Li Jin, Guorong Li, Jiangyu Li, Jingfeng
Li, Hanxing Liu, Junming Liu, Shengguo Lu, Haosu Luo, Xiangjian Meng, Jun Ouyang,
Wei Ren, Chunlei Wang, Hong Wang, Jinbin Wang, Yaojin Wang, Zhanjie Wang,
Zhuo Xu, Tongqing Yang, Manwen Yao, Jiwei Zhai, Dou Zhang, Jialiang Zhang,
Yichun Zhou, Jianguo Zhu, Kongjun Zhu

Poster presentation award judging committee
Chair:
Eisuke Tokumitsu (JAIST)
Vice Chair:
Haosu Luo (Shanghai Institute of Ceramics, CAS, China)
Members:
Jianguo Zhu (Sichuan University)
Jun Ouyang (Qilu University of Technology)
Zhigao Hu (East China Normal University)
Tadashi Fujii (Toyama Prefectural University)
Wensheng Wang (Fujitsu Semi. Memory Solution Ltd.)
Local team:Tomoaki Karaki (Zhiming Chen) (Toyama Prefectural University), Chair
Eisuke Tokumitsu (JAIST), Program & Venue
Tadashi Fujii (Toyama Prefectural University), Secretariat
Wensheng Wang (Fujitsu Semi. Memory Solution Ltd.), Accountant

3

CJFMA14 Oral presenters Guidelines Summary
1. Please enter the meeting room 10 minutes before the session starts.
Zoom meeting ID: 805 936 4730, password: jcfma14
2. Check your speaker, microphone and camera.
3. Rename your screen name into【Presentation number】
4. Reply to the chair if your name is called during attendance confirmation.
5. Turn off your microphone and camera after the attendance confirmation.
6. When your presentation turn comes, the chair will call your presentation
number or name.
7. Turn on your microphone, camera and start sharing your screen(presentation files) to begin your presentation.
8. During the Q&A session, the chair will pick up the audience who hasquestions.
9. Please turn off your microphone, camera and stop sharing your screen after
the Q&A session.

Time limitation for each presenter
Plenary talks

40 minutes (35 min. for talk and 5 min. for Q&A)

Invited talks

20 minutes (15 min. for talk and 5 min. for Q&A)

First bell

Second bell

Third bell

2 mins before the talk ends

The end of the talkThe end of the presentation*Please make sure to finish your talk within the determined time period. Talk or
Q&A might be stopped by the chair if the presenter overran the allotted time.
*Please check out the Presenters Guidelines if you need more information:
https://www.pu-toyama.ac.jp/JCFMA14/Presenters Guidelines.pdf
4

CJFMA14 Poster presenters Guidelines Summary
1. Please enter the meeting room 15 minutes before the session starts.
Zoom Meeting ID: 521 666 2126, password: jcfma14
2. Check your speaker, microphone and camera.
3. Rename your screen name into【Poster number & last name】.
4. Enter the breakout room named by your poster number & name.
5. Make the screen-shear to show your ppt.
6. When someone(s) come(s) into your breakout room, you can begin yourpresentation in English.
7. If someone(s) aske(s) questions in English or Japanese or Chinese, you
can also answer in English or Japanese or Chinese.
8. The poster session period is 11:10-12:40 of Dec. 9, 2022 (Japan/Korea
Standard Time).
9. You can leave the breakout room after 12:40, if finished all answers toquestions.
*Please check out the Presenters Guidelines if you need more information:
https://www.pu-toyama.ac.jp/JCFMA14/Presenters Guidelines.pdf

5

CJFMA14 Arrangement
Dec. 8, 2022 (Japan/Korea Standard Time)
Opening Address

9:00-9:05

Tomoaki Karaki (Zhiming Chen)

9:05-9:45 (I-1)

Norihiko Oshime

9:45-10:25 (I-2)

Jiangyu Li

Introduce of CJFMA15

10:25-10:35

Jun Ouyang

Break

10:35-10:45

Plenary Talks

Invited Session A

Lunch

Invited Session B

Break

Invited Session C

Banquet10:45-11:05 (A-1)

Takeshi Yoshimura

11:05-11:25 (A-2)

Hang Luo

11:25-11:45 (A-3)

Yaojin Wang

11:45-12:05 (A-4)

Jun Ouyang

12:05-12:25 (A-5)

Yiping Guo

12:25-13:30
13:30-13:50 (B-1)

Hiroaki Takeda

13:50-14:10 (B-2)

Yuui Yokota

14:10-14:30 (B-3)

Limei Zheng

14:30-14:50 (B-4)

Muneyasu Suzuki

14:50-15:10 (B-5)

Yongke Yan

15:10-15:30 (B-6)

Yohachi Yamashita

15:30-15:50 (B-7)

Chengtao Luo

15:50-16:00
16:00-16:20 (C-1)

Nan Zhang

16:20-16:40 (C-2)

Zhiguo Yi

16:40-17:00 (C-3)

Jing Wang

17:00-17:20 (C-4)

Zhengqian Fu

17:20-17:40 (C-5)

Xiao Yu

17:40-18:00 (C-6)

Yanxue Tang

18:00-18:20 (C-7)

Jie Jiao

19:00-20:30
6

Dec. 9, 2022 (Japan/Korea Standard Time)

Invited Session D

9:00-9:20 (D-1)

Bo-Ping Zhang

9:20-9:40 (D-2)

Dawei Wang

9:40-10:00 (D-3)

Hajime Nagata

10:00-10:20 (D-4)

Zhang Jialiang

10:20-10:40 (D-5)

Wataru Sakamoto

10:40-11:00 (D-6)

Zhiyong Zhou

Break

11:00-11:10

Poster Session

11:10-12:40

Lunch

12:40-13:30

Invited Session E

Break

Invited Session F

Closing Remarks

P-01 – P-31

13:30-13:50 (E-1)

Yuji Noguch

13:50-14:10 (E-2)

Hua Hao

14:10-14:30 (E-3)

Zhigao Hu

14:30-14:50 (E-4)

Satoshi Wada

14:50-15:10 (E-5)

Masaki Yamaguchi

15:10-15:30 (E-6)

Wei Ren

15:30-15:50 (E-7)

Shinya Tsukada

15:50-16:00
16:00-16:20 (F-1)

Laiming Jiang

16:20-16:40 (F-2)

Jun Akedo

16:40-17:00 (F-3)

Eisuke Tokumitsu

17:00-17:20 (F-4)

Rao Badari Narayana

17:20-17:40 (F-5)

Jundong Song

17:40-18:00 (F-6)

Jing Yan

18:00-18:20 (F-7)

Xueyou Yuan

18:20-18:40 (F-8)

Lisha Liu

18:40-18:50

Tomoaki Karaki (Zhiming Chen)

7

List of Poster (11:10-12:40, Dec. 9, 2022)
No.

Name

Affiliation

P-01

Yao SuBaoji University of Arts and Sciences

P-02

Yu XieNanjing University of Aeronautics and Astronautics

P-03

Jinfeng Lin

Tongji University

P-04

Takayasu Shigemasu

Hiroshima University

P-05

Xiaonan Ma

Shanghai University

P-06

Mingyang Shao

Hiroshima University

P-07

Adil Emin

Lanzhou University

P-08

Xianfa Ai

Nanjing University of Aeronautics and Astronautics

P-09

Takumi Nozaki

Nagoya Institute of Technology

P-10

Zhe Wang

Xi’an Jiaotong University

P-11

Peimei Yuan

Baoji University of Arts and Sciences

P-12

Atsuto Fujisawa

Shizuoka University

P-13

Yu Xiang

Shonan Institute of Technology

P-14

Kohei Miyaji

Osaka Metropolitan University

P-15

Shuting Yang

Shandong University

P-16

Kazuto Yoshida

Shizuoka University

P-17

Soma Sakoda

Osaka Metropolitan University

P-18

Xiaojie Li

Shanghai University

P-19

Seiji Sogen

Shizuoka University

P-20
P-21

Weiwei Yang
Hongrui Jia

Shanghai Institute of Ceramics

P-22

Jun Hirade

Shibaura Institute of Technology

P-23

Kun Zhu

Tongji University

P-24

Jin Qian

Tongji University

P-25

Ying Shi

Shanghai Institute of Ceramics

P-26

Fei Jing

Baoji University of Arts and Sciences

P-27

Tomohiro Nishimoto

Shizuoka University

P-28

Ruixuan Xue

Baoji University of Arts and Sciences

P-29

Bo ZhaoBaoji University of Arts and Sciences

P-30

Nina Dai

Baoji University of Arts and Sciences

P-31

Shicheng Peng

Tokyo Institute of Technology

Xi’an Jiaotong University

8

PROGRAM(Hybrid format)
Dec. 8, 2022 (Japan/Korea Standard Time)
9:00
Opening address,
Tomoaki Karaki (Zhiming Chen)

Oral Session
9:05-10:35
Plenary Session
Chair: Hiroaki Takeda (Saitama University)
9:05
I-1
Bragg Coherent X-ray diffraction for visualization of the inhomogeneous structure of asingle ferroelectric particle
N. Oshime, K. Ohwada, K. Sugawara, A. Shimada, N. Fukushima, T. Ueno, A. Machida,
T. Watanuki, S. Ueno, I. Fujii, S. Wada, K. Momma, K. Ishii, H. Toyokawa, S. Kim, S.
Tsukada, and Y. Kuroiwa
National Institutes for Quantum Science and Technology, Japan
9:45
I-2
Polar orders across scales: the effect of strain and mechanics
Jiangyu Li
Southern University of Science and Technology, China
10:45-12:25
Invited Session A
Chair: Yuui Yokota (Tohoku University)
10:45 A-1
Energy Harvesting from Electric Power Lines Using Piezoelectric Resonator
Takeshi Yoshimura, Shuichi Murakami, and Norifumi Fujimura
Osaka Metropolitan University, Japan
11:05 A-2
Improved capacitive energy storage nanocomposites at high temperature utilizing
ultralow loading of bimetallic MOF
Hang Luo, Fan Wang, Xiaona Li, Dou Zhang
Central South University, China.
11:25 A-3
Ferroelectrics for emerging oral bioelectronics
Yaojin Wang, Xuehui Zhang and Xuliang Deng
Nanjing University of Science and Technology, China
11:45 A-4
High performance dielectric energy storage via nanograin engineering in ferroele
ctric/antiferr-oelectric film capacitors
Jun Ouyang, Hongbo Cheng, Xiao Zhai, Jing Yan, Yu Su
Qilu University of Technology, China.

912:05 A-5Reducing the coercive field of rhombohedral NBT-based crystals by domain engineering
Geng Huangfu, Haosu Luo,Yiping Guo
Shanghai Jiaotong University, China.
13:30-15:50
Invited Session B,
Chair: Wataru Sakamoto (Chubu University)
13:30 B-1
Growth and Characterization of Ba3TaGa3Si2O14 Single Crystals
H. Takeda, T. Hoshina, and T. Tsurumi
Saitama University, Japan.
13:50 B-2
Effects of Al substitution on crystal structure and piezoelectric properties of
Ca3NbGa3Si2O14 and Ca3TaGa3Si2O14 single crystals
Yuui Yokota, Yuji Ohashi,Takahiko Horiai, Akira Yoshikawa
Tohoku University, Japan.
14:10 B-3
Simultaneously achieving giant piezoelectricity and record coercive field enhancement
in relaxor-based ferroelectric crystals
Limei Zheng, Liya Yang, Gang Liu
Shandong University, China.
14:30 B-4
Enhanced polarization property of PZT produced by press forming
Muneyasu Suzuki, Harutaka Mekaru, Tetsuo Tsuchiya, Jun Akedo
AIST, Japan.

14:50 B-5
High Piezoelectric Performance of Textured Relaxor-PT/PZT Ceramics
Yan Yongke, Xu Zhuo, Priya ShashankXi’an Jiaotong University, China.
15:10 B-6
A Review of Lead Perovskite Piezoelectric Single Crystals and Their Medical
Transducers Application
Yohachi (john) Yamashita, Tomoaki Karaki, and Horoshi Maiwa
Toyama Prefectural University, Japan.
15:30 B-7
Domain Engineering Effect of Alternating Current Poling with Different Frequency on
PMN-PT Single Crystals
Chengtao Luo, Haotian Wan, Chang Liu, Wei-Yi Chang, Yohachi Yamashita, andXiaoning Jiang
Shanghai Jiaotong University, China.

10

16:00-18:20
Invited Session C,
Chair: Dou Zhang (Central South University)
16:00 C-1
Tuning of polar domain boundaries in non-polar perovskite
Nan Zhang, Zheyi An, Hiroko Yokota, Marek Paściak, Wei Ren, Zuo-Guang Ye
Xi’an Jiaotong University, China.
16:20 C-2
Microstructure Design and Exotic Electrostrain Response in Layer Structured
Perovskite Ferroelectric Ceramics
Xiang He, Zhiguo Yi
Shanghai Institute of Ceramics, China.
16:40 C-3
Synergic Modulation of the Multi-scale Structures on the Energy Storage Properties ofSilver Niobate-Based Ceramics
J. Wang, XH. Fan, Y. Rao, L. Zhao, KJ. Zhu
Nanjing University of Aeronautics and Astronautics, China.
17:00 C-4
Atomic-Scale Studies of PbZrO3-based Antiferroelectric Ceramics
Zhengqian Fu, Xuefeng Chen, Zhenqin Li, Tengfei Hu, Ziyi Yu, Linlin Zhang, Shujun
Zhang, Genshui Wang, Xianlin Dong, Fangfang Xu
Shanghai Institute of Ceramics, China.
17:20 C-5
Ferroelectric Materials and Devices for Intelligent Computing
Xiao Yu, Yue Peng, Jiuren Zhou, Genquan Han
Research Center for Intelligent Chips and Device, China.
17:40 C-6
Excellent pyroelectric properties of relaxor-based ferroelectric single crystals and thinfilms for infrared detection
Yanxue Tang, Haosu Luo
Shanghai Normal University, China.
18:00 C-7
Heterostructural magnetoelectric composites and application in magnetic field andcurrent sensing
Jie Jiao, Rui Chen, Hanzhou Wu, Yaojin Wang, Haosu Luo, Li Lu, Wenning Di
Shanghai Institute of Ceramics, China.

11

Dec. 9, 2022 (Japan/Korea Standard Time)

9:00-11:00
Invited Session D,
Chair: Jun Akedo, (AIST)
9:00
D-1
High Curie temperature BiFeO3-BaTiO3 lead-free piezoelectric ceramics: One-step
preparation
Yu-Cheng Tang, Ai-Zhen Song, Yang Yin, He-Zhang Li, Bo-Ping Zhang
University of Science and Technology Beijing, China.
9:20
D-2
Bismuth Ferrite Based Lead-Free Piezoelectric ceramics
Dawei Wang
Harbin Institute of Technology, China.
9:40
D-3
Mechanism of Material Hardening on (Bi0.5Na0.5)TiO3-based Lead-free Piezoelectric
Ceramics by Quenching Treatment
Takeru Tayama, Yuka Takagi, and Hajime Nagata
Tokyo University of Science, Japan.
10:00 D-4
Studies of Domain Structure in (K,Na)NbO3-based Ceramics with Acid-Etching
Zhang Jialiang
Shandong University, China.
10:20 D-5
Effect of Li2CO3 and MnCO3 Addition on Properties of (Ba,Ca)(Ti,Sn)O3 Piezoelectric
Ceramics Sintered Under Controlled Low Oxygen Partial Pressure
K. Uematsu, W. Sakamoto
Chubu University, Japan.
10:40 D-6
Investigations of multi-scale regulation and in-situ characterization of hightemperature piezoelectric ceramics
Zhiyong Zhou
Shanghai Institute of Ceramics, China.
11:10-12:40

Poster Session, P-01—P-31

13:30-15:50
Invited Session E,
Chair: Eisuke Tokumitsu (JAIST)
13:30 E-1
Enhanced energy storage ceramic capacitors utilizing ferrorestorable polarization
Yuji Noguchi, and Hiroki Matsuo
Kumamoto University, Japan.
12

13:50 E-2
High performance BaTiO3-based dielectric materials for capacitor applications
Cheng Chen, Hua Hao, Xin Lai, Appiah Millicent, Zhonghua Yao, Minghe Cao,
Hanxing Liu
Wuhan University of Technology, China.
14:10 E-3
Origin of High-Performance Energy Conversion in AgNbO3 Based Ceramics: Structure
Evidences
Zhigao Hu, Anyang Cui, Kai Dai, Kai Jiang, and Junhao Chu
East China Normal University, China.
14:30 E-4
Growth of Metal-free Perovskite-type Ferroelectric Crystals and Their Ferroelectric
Properties
S. Ueno, S. Ando, T. Moriyama, T. Unno, I. Fujii, S. Kawachi, J. Yamaura, S. Wada
University of Yamanashi, Japan.
14:50 E-5
Effect of Reaction Accelerator on Single Crystal Barium Titanate Fine Particle
Synthesis
Masaki YAMAGUCHI, Atsushi SAITOH, Misa YAMASAKI, Takashi YAMAMOTO
Shibaura Institute of Technology, Japan.
15:10 E-6
Ferroelectric and piezoelectric properties in simple binary compounds
Wei RenShanghai University, China.
15:30 E-7
Angle-resolved polarized Raman mapping on a compositionally gradedPb(Mg1/3Nb2/3)O3-PbTiO3
S. Tsukada, Y. Fujii, A. Kanagawa, Y. Akishige, and K. Ohwada
Shimane University, Japan.
16:00-18:40 Invited Session F, Chair: Masaki Yamaguchi (Shibaura Institute ofTechnology)
16:00 F-1
Flexible Lead-free Piezoelectric Arrays for High-Efficiency Wireless Ultrasonic
Energy Transfer and Communication
Laiming Jiang, Jiagang Wu, Jianguo Zhu
Sichuan University, China.

13

16:20 F-2
RTIC phenomenon on AD process and its application to dielectric / ferroelectric thickfilms
Jun AKEDO
National Institute of Advanced Industrial Science & Technology (AIST), Japan
16:40 F-3
Ferroelectric gate thin films transistors with Y-doped Hf-Zr-O gate insulator and In-SnO channel
E. Tokumitsu, Y. Kubota, Mohit, K. Sasaki
Japan Advanced Institute of Science and Technology, Japan.
17:00 F-4
Fabrication and characterization of La-doped HfO2 ferroelectric films on SrTiO3 single
crystal substrates
Badari Narayana Rao, HirokoYokota
Chiba University, Japan.
17:20 F-5
Energy-storage performance of antiferroelectric Pb(Zr,Hf)O3 films fabricated by solgel spin coating
J. Song, S. Kada, Y. Iwamoto, T. Iijima, and S. Okamura
Tokyo University of Science, Japan.
17:40 F-6
Low temperature deposition of BiFeO3 films on base metal foils for piezoelectric
applications
Jing Yan, Jun Ouyang, Isaku Kanno
Qilu Normal University, China.
18:00 F-7
Extraordinarily large domain switching contribution in epitaxial (K, Na)NbO3 films
Xueyou Yuan, Kazuki Okamoto, Mitsuki Kawano, Masahito Yoshino, Takanori
Nagasaki, Yasuhiko Imai, Osami Sakata, Tomoaki Yamada
Nagoya University, Japan.
18:20 F-8
Intrinsic properties of domain walls of BiFeO3
Lisha Liu, Jing-Feng Li, and Yaojin Wang
Nanjing University of Science and Technology, China.
18:40

Closing remarks,

Tomoaki Karaki (Zhiming Chen)

14

Poster Session
11:10-12:40,

Dec. 9, 2022 (Japan/Korea Standard Time)

P-01
Phase Transformation, Interfacial Coupling and Giant Charge-discharge Efficiencyof BaTiO3@PVP/PVDF Nanocomposite Films
Yao Su, Wenyi Li, Yan Wang, Peimei Yuan, Zhao Bo, Dengwei Hu
Baoji University of Arts and Sciences, China.
P-02
Crystal structure and microwave dielectric properties of Ba4(Sm1-xCex)9.33Ti18O54 solid
solutionsYu Xie, Kongjun Zhu, Kang Yan, Jing Wang, Jinsong Liu
Nanjing University of Aeronautics and Astronautics, China.
P-03
Ultrahigh energy harvesting properties in temperature insensitive eco-friendly highperformance KNN-based textured ceramics
Jinfeng Lin, Jiwei Zhai
Tongji University, China.
P-04
Characteristics of Chemical Bonding and Thermal Behavior of Atoms in Prototype
Structure of Double Perovskite-type Antiferroelectric Oxides
Takayasu Shigemasu, Sangwook Kim, Chikako Moriyoshi, Guorong Li, Chul-Hong
Park, and Yoshihiro Kuroiwa
Hiroshima University, Japan.
P-05
Tunable vertical ferroelectricity and domain walls by interlayer sliding in β-ZrI2
Xiaonan Ma, Chang Liu, Sergey A. Nikolaev, and Wei Ren
Shanghai University, China.
P-06
Crystal Structure of KNbO3/BaTiO3 Core-Shell Nanocomposite Particles Studied by
Synchrotron Radiation X-ray Diffraction
Shao Mingyang, Kaede Furuta, Sangwook Kim, Ichiro Fujii, Shintaro Ueno, Satoshi
Wada, and Yoshihiro Kuroiwa
Hiroshima University, Japan.
P-07
Brillouin Scattering Study of Ferroelastic Phase Transition of Lead Phosphate Single
CrystalAdil Emin, Anwar Hushur, and Seiji Kojima
Lanzhou University, China.
15

P-08
Structural evolution and electrical properties of BFO-BT based high temperature leadfree piezoelectric ceramics
X. Ai, J. Yang, K. Yan, K. Zhu
Nanjing University of Aeronautics and Astronautics, China.
P-09
Activation of lead-free (Na,K)NbO3 piezoceramics using pulsed electric field
Takumi Nozaki, Alexander Martin, Ryota Kobayashi, Tadachika Nakayama, Ken-ichi
Kakimoto
Nagoya Institute of Technology, Japan.
P-10
Realization of enhanced strain responses in lead-free (Bi0.5Na0.5)TiO3-based
ferroelectric thin films by active domain motions
Zhe Wanga, Jinyan Zhao, Gang Niu, Wei Ren, Nan Zhang, Kun Zheng, Yi Quan,
Henghui Cai, Xin Li, Genshui Wang
Xi’an Jiaotong University, China.
P-11
Preparation of high temperature resistant barium titanate/polyimide flexible
nanocomposite energy storage films
Peimei Yuan, Ruixuan Xue, ChenLi Wu, Rong Ma, Dengwei Hu
P-12
Change of crystal and microscopic structures of Ba0.95Sr0.05TiO3 ceramics prepared by
the combination of reaction sintering and spark plasma sintering
A Fujisawa, D Fu
Shizuoka University, Japan.
P-13
Microstructure of AC poled ternary PIN-PMN-PT single crystal after high temperatureannealing
Yu Xiang, Yinqin Sun, Y. Yamashita, T. Karaki, and H. Maiwa
Shonan Institute of Technology, Japan.
P-14
Effects of sputtering conditions on the growth of AlScN thin films and its conduction
mechanism
Kohei Miyaji, Norifumi, Fujimura, Takeshi Yoshimura
Osaka Metropolitan University, Japan.
P-15
High-Performance Neuromorphic Computing Based on Ferroelectric Synapses with
Excellent Conductance Linearity and Symmetry
Shuting Yang, Limei Zheng, Le Zhao
Shandong University, China.
16

P-16
Low-temperature deposition of transparent Pb(Zr1-xTix)O3 thin film on glass substratewith giant piezoelectric response
K. Yoshida, S. Sogen, H. Suzuki1, T. Arai, and D. Fu
Shizuoka University, Japan.
P-17
Mechanomyography Using Piezoelectric Materials
S. Sakoda, N. Fujimura and, T. Yoshimura
Osaka Metropolitan University, Japan
P-18
Unique Gas Sensing Performance of Sol-gel Derived BiFeO3 Nanoparticles
Xiaojie Li, Jinrong Cheng, Jiaqiang Xu
Shanghai University, China.
P-19
Ferroelectric and piezoelectric properties of c-axis oriented PbZr0.53Ti0.47O3 thin film
deposited on SUS substrate with large coefficient of thermal expansion
Seiji Sogen, Kazuto Yoshida, Takashi Arai, Hisao Suzuki, Desheng Fu
Shizuoka University, Japan.
P-20
Superior energy storage properties in NaNbO3-based ceramics via synergistically
optimizing domain and band structures
Weiwei Yang, Huarong Zeng, Guorong Li
Shanghai Institute of Ceramics, China.
P-21
Extremely large strain response under low driving electric fields in lead-based textured
piezoelectric ceramics
Hongrui Jia, Zhen Li, Linghang Wang
Xi’an Jiaotong University, China.
P-22
Experimental approach to residual hydrogen content in silicon substrates by proton
beam writing
Jun HIRADE and Masaki YAMAGUCHI
Shibaura Institute of Technology, Japan.
P-23
Polarization Rotation Control Domain Dynamic Response Modulates Piezoelectric
Properties of Lead-Free Thin Films
Kun Zhu, Guanglong Ge, Jinfeng Lin, Hairui Bai, Cheng Shi, Guohui Li, Fei Yan,
Liuxue Xu, Weiwei Yang, Huarong Zeng, Kunyu Zhao, Zhenyong Man, Feifei Wang,
Bo Shen, Jiwei Zhai, Xiujian Chou
Tongji University, China.
17

P-24
High Energy Storage Performance and Large Electrocaloric Response in Bi0.5Na0.5TiO3–
Ba(Zr0.2Ti0.8)O3 Thin Films
Jin Qian, Jiwei Zhai, Zhenxiang Cheng
Tongji University, China.
P-25
Enhanced stabilization of oxygen vacancies on the bipolar fatigue resistance of PNNPZT-based ceramics
Ying Shi, Guorong Li, Liaoying Zheng, Zhenyong Man, Xuezheng Ruan, Xue Shi
Shanghai Institute of Ceramics, China.
P-26
Preparation of Tetragonal BaTiO3 by Molten Salt Synthesis Process
Fei Jing, Nina Dai, Weixing Zhao, Dengwei Hu
Baoji University of Arts and Sciences, China.
P-27
Energy storage properties of antiferroelectric PbZrO3 thin films prepared by chemicalsolution deposition method
T. Nishimoto, S. Sougen, K. Yoshida, H. Suzuki, D. Fu
Shizuoka University, Japan.
P-28
3D Printing of Piezoelectric Biological Scaffolds for Bone Tissue Engineering
Ruixuan Xue, Peimei Yuan, Liying Yu, Rong Ma, Dengwei Hu
Baoji University of Arts and Sciences, China.
P-29
Flexible Piezoelectric Nanogenerators Based on Two-dimensional Barium Titanate
Nanosheets and Polymer Polylactic acid
Bo Zhao, Yao Su, Songlin Yu, Han Yu, Dengwei Hu
Baoji University of Arts and Sciences, China.
P-30
Energy storage of BT/PVP/PVDF nanocomposite films with multilayer structure
Nina Dai, Fei Jing, Peimei Yuan, Ruixuan Xue, Bo Zhao, Yao Su, Dengwei Hu
Baoji University of Arts and Sciences, China.
P-31
Fabrication of (Ba,Sr)TiO3 epitaxial thin films on mica substrate toward flexible
electronics
Shicheng Peng, Sou Yasuhara, Takaaki Tsurumi, Takuya Hoshina
Tokyo Institute of Technology, Japan.

18

I-1:
Bragg Coherent X-ray diffraction for visualization of the inhomogeneous structure of asingle ferroelectric particle
N. Oshime1, K. Ohwada1, K. Sugawara1, A. Shimada1, N. Fukushima2, T. Ueno1, A. Machida1, T.
Watanuki1, S. Ueno3, I. Fujii3, S. Wada3, K. Momma4, K. Ishii1, H. Toyokawa1,5, S. Kim2, S. Tsukada6,
and Y. Kuroiwa2
1

SRRC, National Institutes for Quantum Science and Technology (QST), Japan, 2Graduate School of
Advanced Science and Engineering, Hiroshima University, Japan, 3Graduate Faculty ofInterdisciplinary Research, University of Yamanashi, Japan, 4National Museum of Nature and Science,
Japan, 5Japan Synchrotron Radiation Research Institute (JASRI), SPring-8, Japan, 6Faculty of
Education, Shimane University, Japan*E-mail: oshime.norihiro@qst.go.jp
The shapes and sizes of crystal grains affect the anisotropy of the crystal structure and thearrangement of ferroelectric domains [1,2]. These ferroelectric size effects, however, have made little
progress in discussion due to the difficulty of simultaneously observing the crystal structure, external
shape, and domain structure of a particle with sizes ranging from several 10 to several 100 nm.
We are developing and improving Bragg coherent diffraction imaging (Bragg-CDI) [3] at
BL22XU at SPring-8[4], which is one of the promising methods to simultaneously visualize theheterogeneous structures (including domain structures) and external shapes of fine particles in a nondestructive manner. The Bragg-CDI system is now ready for application to ferroelectric size effectresearch since its applicable particle size has recently been expanded from the conventional 100-300 nm
to 40-500 nm [5]. For application to single ferroelectric BaTiO3 (BTO) particles with sizes of 200-500
nm, Bragg-CDI has visualized the reconstructed three-dimensional images with the external shape, size,
and internal strain distribution of single particles. The 500-nm BTO particle showed a linear and sharp
phase boundary shape, while smaller BTO particles showed different phase patterns.
To further understand these effects, we developed a method to track the ferroelectric phasetransition in a BTO single particle [6]. The phase transition was observed by cooling the 500-nm-sized
BTO to Curie temperature and recording the pattern changes in Bragg coherent X-ray diffraction. Cubic(200 peak)-to-tetragonal (200 and 002 peaks) transition was observed, with a bridge-like fringe pattern.
Bragg-CDI also imaged the inhomogeneous structure of the BTO single particle in the cubic phase fromthe diffraction patterns. The reconstructed images showed linear strains due to dislocations inside the
BTO particle.
[1] K. Ishikawa et al., Phys. Rev. B 37, 5852 (1988).
[2] S. Tsunekawa et al., Phys. Rev. Lett. 85, 3440 (2000).
[3] I. Robinson and H. Ross, Nat. Mater. 8, 291 (2009).
[4] K. Ohwada et al., Jpn. J. Appl. Phys. 58, SLLA05 (2019).
[5] N. Oshime et al., Jpn. J. Appl. Phys. 60, SFFA07 (2021).
[6] N. Oshime et al., Jpn. J. Appl. Phys. 61 SN1008 (2022).

19

I-2:

Polar orders across scales: the effect of strain and mechanics
Jiangyu Li
Southern University of Science and Technology

Ferroelectrics are materials with long-range polar orders, and they have important applications insensors, actuators, field effect transistors, and capacitors. Understanding polar orders acrossscales are thus of critical importance. In this talk, we will examine how ordinary domain patterns
are accommodating each other across grains, resulting in extraordinary piezoelectric coefficientat morphotropic phase boundary. We will discuss how topologically nontrivial polar orders
emerges and reconstruct in ferroelectrics, leading to exotic properties such as negative
capacitance. We will also discuss how dielectric materials fail under high electric field, which
has important implication for pulsed power capacitors. In all these examples, I will show how
coupling to strain, and thus mechanics, play an essential role in the configuration and evolutionof polar orders.

20

A-1:
Energy Harvesting from Electric Power Lines Using Piezoelectric Resonator
Takeshi Yoshimura1*, Shuichi Murakami2, and Norifumi Fujimura1
1
2

Osaka Metropolitan University, Japan

Osaka Research Institute of Industrial Science and Technology, Japan*E-mail: yoshimura@omu.ac.jp

Energy harvesting is expected to be a promising power source for IoT devices. We havedeveloped a dynamic model of piezoelectric vibration energy harvester (pVEH) andachieved a power density of 910 Wcm-2G-2 through device design based on this model andmaterial development of BiFeO3 thin film [1]. Moreover, using the knowledge obtained inthis process, we have developed a harvester that uses permanent magnets andpiezoelectric elements to extract electric power from the alternating magnetic field formed
around a power line, which is called a magnetic field oscillation energy harvester (MOEH)[2]. A permanent magnet placed near a conductor with a current flowing through it issubjected to a force in a direction perpendicular to both the current and the magnetic
moment. When an alternating current flows, the magnet oscillates, which can be used togenerate electric power using the mechanism of pVEH.
The force Fx acting on a permanent magnet placed in a magnetic field with a gradient is given by
𝐹𝑥 = 𝐵𝑟 ∫𝑑𝐻𝑦 (𝑥, 𝑦)
𝑑𝑉
𝑑𝑥

(1)

where Br is the residual flux density of thethe y component of the magnetic field. Based on
the calculation of the force acting on the permanent
magnet placed near the AC power line, the prototype of
MOEH was fabricated. The resonant frequency of theharvester was adjusted to about 50 Hz. Fig. 1 shows thefrequency dependence of the output power measured atvarious AC currents. The distance between the magnet

Output Power (W)magnet, V is the volume of the magnet, and Hy is

Acknowledgments This work was supported in part by

3.4A

1.1A

10-6
0.34A

10-7

0.11A

48

50

52

Fig. 1frequency dependence of the output
power measured at various AC currents.

JST CREST (JPMJCR20Q2)).
Reference
1) M. Aramaki et al, Sensors and Actuators A, 291, 167 (2019).
2) T. Yoshimura et al, Jpn. J. Appl. Phys., 58, SLLD10I (2019).

21

10-5

Frequency (Hz)at the resonant frequency increases in proportion to thecurrent of 3.4 A.

10-4

10-8

and the power line was 12.2 mm. The output powersquare of the current and reaches to 0.35mW at an AC

10-3

A-2:
Improved capacitive energy storage nanocomposites at high temperature
utilizing ultralow loading of bimetallic MOF
Hang Luo, Fan Wang, Xiaona Li, Dou Zhang
State Key Laboratory of Powder Metallurgy, Central South University, Changsha 410083,
Hunan Province, China
E-mail: hangluo@csu.edu.cn (Hang Luo)
Abstract: It is urgent to develop high-temperature dielectrics with high energy density and highenergy efficiency for next-generation capacitor demands. Metal organic frameworks (MOFs) havebeen widely used in the fields of electrochemistry, catalysis, gas storage, separation and sensing due
to their structural diversity and functionally adaptable properties. Doping of metal nodes in MOFs
is an effective strategy to change the band gap and band edge positions of the original MOFs, whichhelps to improve their ability to bind charges as traps. In this work, incorporation of ultralow loading(<1.5 wt%) of novel bimetallic metal-organic framework (ZIF 8-67) into PEI polymer matrix is
exhibited. ZIF 8-67 is a kind of bimetallic frame material with excellent thermal stability, good
insulation and microporous structure. With the addition of ZIF 8-67, the breakdown strength andenergy storage capacity of ZIF 8-67/PEI nanocomposites are significantly improved, especially athigh temperature (200 ℃). For example, the energy densities of the 0.5 wt% ZIF 8-67/PEI
nanocomposites is up to 2.96 J/cm3, with an efficiency (η) >90% at 150 ℃. At 200 ℃, the dischargeenergy density of 0.25 wt% ZIF 8-67/PEI nanocomposite can still reach 1.84 J/cm3 with a η >90%,
which is 9 times higher than that of pure PEI (0.21 J/cm3) under the same conditions, and it is thelargest improvement compared with the previous reports. Furthermore, at 200 ℃, the energy storage
density and efficiency of the nanocomposites show no sign of degradation after 20,000 cycles.

22

A-3:

Ferroelectrics for emerging oral bioelectronics
Yaojin Wang1, Xuehui Zhang2 and Xuliang Deng3

School of Materials Science and Engineering, Nanjing University of Science and Technology,
Nanjing 210094, Jiangsu, China
2
Department of Dental Materials & Dental Medical Devices Testing Center, Peking
University School and Hospital of Stomatology, Beijing 100081, China.
3
Department of Geriatric Dentistry, Peking University School and Hospital of Stomatology,
Beijing 100081, China.

1E-mail address: yjwang@njust.edu.cn
Tooth whitening has recently become one of the most popular aesthetic dentistry procedures.
Beyond classic hydrogen peroxide-based whitening agents, photo-catalysts and piezo-catalysts havebeen demonstrated for non-destructive on-demand tooth whitening. However, their usage has beenchallenged due to the relatively limited physical stimuli of light irradiation and ultrasonic mechanicalvibration. To address this challenge, we report here a non-destructive and convenient tooth whitening
strategy based on the pyro-catalysis effect, realized via ubiquitous oral motion-induced temperaturefluctuations. Degradation of organic dyes via pyro-catalysis is performed under cooling/heating
cycling to simulate natural temperature fluctuations associated with intake and speech. Teeth stainedby habitual beverages and flavorings can be notably whitened by the pyroelectric particles-embeddedhydrogel under a small surrounding temperature fluctuation. Furthermore, the pyro-catalysis based
tooth whitening procedure exhibits remarkably therapeutic biosafety and sustainability. In view of the
exemplary demonstration, the most prevalent oral temperature fluctuation will enable thepyro-catalysis based tooth whitening strategy to have tremendous potential for practical applications.

23

A-4:
High performance dielectric energy storage via nanograin engineeringin ferroelectric/antiferroelectric film capacitors
Jun Ouyang1,2, Hongbo Cheng,1 Xiao Zhai,2 Jing Yan2,3, Yu Su4
1

Qilu University of Technology, Jinan, 250353
2
3

4

Shandong University, Jinan, 250100

Qilu Normal University, Jinan, 250013

Beijing Institute of Technology, Beijing, 100081
Email: ouyangjun@qlu.edu.cn

In comparison with the ferroelectric and antiferroelectric bulk ceramics, their thin films can achieve
larger capacitive energy densities due to higher applicable electric fields. Recently, researchers haveinvestigated different methods to improve the capacitive energy densities of ferroelectric or
antiferroelectric ceramic film capacitors, such as “domain engineering”, “interface engineering” andchemical doping/substitution. In this work, we prepared high energy density film capacitors via a
combination of the low-temperature sputtering process and the buffer-layer technique, as well as a rapid
thermal annealing process. In comparison with the high-temperature processed films, our ferroelectric
BaTiO3 and CaBi2Nb2O9 films and antiferroelectric Ag(Nb, Ta)O3 films, displayed not only a greatly
reduced thermal budget, but also a significantly decreased grain size (down to 10-20 nm). The latter has
led to a slim and elongated P-E hysteresis loop and a high breakdown strength Eb, corresponding to amuch improved energy storage density and a high charge-discharge efficiency. These low temperatureprocessed films are also endowed with an excellent electric fatigue resistance and a high thermal stability.
Applying phase field modeling on a simple linear model of the BaTiO3 film consisting of periodicallyaligned and parallelly connected grains and grain boundaries, we explained its P-E characteristics andthe corresponding capacitive energy storage performance (Fig.1).

Fig1. Schematics of a high energy density columnar nanograined BaTiO3 film, and its P-E characteristics
simulated via phase field modeling (Zhao and Ouyang et al. Energy Storage Materials, 39, 81, 2021).

24

A-5:
Reducing the coercive field of rhombohedral NBT-based crystals by domain engineering
Geng Huangfu1, Haosu Luo2,Yiping Guo1*
1

State Key Laboratory of Metal Matrix Composites, School of Materials Science and Engineering,
Shanghai Jiao Tong University, Shanghai 200240, China

2

Artificial Crystal Research Center, Shanghai Institute of Ceramics, Chinese Academy of Sciences,
Shanghai 201800, China*E-mail: ypguo@sjtu.edu.cn(Na0.5Bi0.5)TiO3 (NBT)-based materials have been widely studied for their large electric-field-induced

strains. However, the high driving voltage and coercive field (Ec) have long hindered the applications
of NBT-based materials. Here, we propose a simple method to significantly reduce the Ec ofrhombohedral NBT-based single crystals through tailoring the domain configuration. By applying analternating-current (AC) electric field along the [001] direction, the Ec of Mn-doped(Na0.48K0.02Bi0.5)TiO3 single crystal can be reduced from 70 kV/cm to 20 kV/cm after about 25 cycles
without sacrificing the ferroelectric polarization. Meanwhile, the small-signal piezoelectric coefficient
d33 and the optical transparency of the crystals are also improved compared with those after directcurrent electric field poling.

The domain structure characterization shows that the AC cycles along the [001] direction can form alaminar domain configuration where the 71°domain walls are nearly eliminated, which is considered tobe the cause of the reduced Ec. In the laminar domain configuration, almost only 71°polarization
switching occurs when the external electric field is reversed, and 71°polarization switching has been
proved to require lower energy than the 109° or 180° polarization switching in rhombohedral
ferroelectric crystals. Therefore, the required energy for polarization reversal of the laminar domain
configuration is significantly lower than that of the randomly distributed domains, thus the Ec is reduced
greatly.
This method is also applicable to other rhombohedral single crystals (NBT, Mn-doped NBT, NBT4%BaTiO3, etc.) and may be applied to [001]-textured polycrystalline ceramics in the future to promote
the practical applications of NBT-based materials.

25

B-1:
Growth and Characterization of Ba3TaGa3Si2O14 Single Crystals
H. Takeda1,*, T. Hoshina2, and T. Tsurumi2
1
2

Saitama University, 255 Shimo-Okubo, Sakura-ku, Saitama 338-8570, JapanTokyo Institute of Technology, 2-12-1 Ookayama, Meguro, Tokyo 152-8552, Japan*E-mail: takeda@apc.saitama-u.ac.jp

High temperature piezoelectric materials are in high demand for gas sensors, combustion pressure
sensors and gas injectors directly placed in the cylinder of engines. La3Ga5SiO14 (langasite; LGS)-typesingle crystals are currently promising materials for this purpose. The LGS crystal has Ca3Ga2Ge4O14type structure (space group P321). There are four kinds of cation sites in the structure with the chemical
formula A3BC3D2O14. The notations A and B represent a decahedral (twisted Thomson cube) site
coordinated by eight oxygens, and an octahedral site coordinated by six oxygens, respectively. Moreover,
C and D represent tetrahedral sites coordinated by four oxygens, the size of the D site being smaller thanthat of the C site. In the LGS crystal, the A site is occupied by La3+ ion, the B and C sites are occupied
by Ga3+ ions, the D site is occupied by Ga3+ and Si4+ ions. Therefore, LGS is call as disordered-type.
Due to the existence of these many cation sites, a large number of Ca3Ga2Ge4O14-type compounds havebeen synthesized by isovalent and/or aliovalent substitution [1]. Based on this data, Sr3TaGa3Si2O14
single crystals was synthesized. In this crystal, each cation site is occupied by only single metal [2].
Nowadays, this kind of crystals is call as ordered-type. It has been reported [3] that an increase lattice
parameter a leads to an increase of the piezoelectric modulus |d11| of Ca3Ga2Ge4O14-type crystals. Basedon these knowledge, Ba3NbGa3Si2O14 and Ba3TaGa3Si2O14 (abbreviated as BTGS) single crystals weresynthesized and small information about their piezoelectric
properties was disclosed [4,5]. As far as we know, there is no
details of the structure analysis and piezoelectric propertiesof the BTGS single crystal.
We report structure and electric properties of the BTGS
crystals grown by the Czochralski technique using raw
materials with stoichiometric composition [6]. The crystal
structure of BTGS has been refined using single-crystal Xray diffraction data with a precision corresponding to an R
index less than 0.04. The crystal structure is isostructural tothat of langasite-type Ca3Ga2Ge4O14. It was confirmed thatthe distribution of each cation was ordered in each site. A Fig. 1 Resistivity as a function of temperature
piezoelectric d11 constant was 5.8 pC/N, which is the highest for Ba3TaGa3Si2O14 (BTGS) crystalsof those of order-type langasite crystals. The temperature compared with other langasite family
crystals. CTGS, CTAS, LTGA, LGS, anddependence of resistivity is similar to those of order-type LTG
aretheabbreviationsforlangasite crystals (Fig. 1) and higher than that of Ca3TaGa3Si2O14,
Ca3TaAl3Si2O14,
La3Ta0.5Ga5.5O14 (LTG) crystal, which is the most promising La3Ta0.5Ga5Al0.5O14, La3Ga5SiO14, and
La3Ta0.5Ga5.5O14, respectively.
candidates for combustion pressure sensor materials.
Acknowledgments: Part of this study was financially supported by JSPS KAKENHI (grant numbers 20H05879
and 22H02162) and the Kazuchika Okura Memorial Foundation.
References[1] B.V. Mill, E.L. Belokoneva, T. Fukuda, Russ. J. Inorg. Chem. 43 (1998) 1168.
[2] H. Takeda, J. Sato, T. Kato, K. Kawasaki, H. Morikoshi, K. Shimamura, T. Fukuda, Mater. Res. Bull. 35(2000) 245.
[3] H. Takeda, H. Nakao, S. Izukawa, H. Shimizu, T. Nishida, S. Okamura, T. Shiosaki, J. Alloys Compd. 408412 (2006) 474.
[4] H. Takeda, S. Izukawa, S. Okamura, T. Shiosaki, Key Eng. Mater. 269 (2004) 23.
[5] Y. Zheng, J. Xin, H. Kong, H. Chen, E. Shi, J. Cryst. Growth 310 (2008) 2284.
[6] H. Usui, H. Kusakabe, M. Tokuda, K. Sugiyama, T. Hoshina, T. Tsurumi, H. Takeda, J. Ceram. Soc. Jpn. 128(2020) 441.

26

B-2:
Effects of Al substitution on crystal structure and piezoelectric propertiesof Ca3NbGa3Si2O14 and Ca3TaGa3Si2O14 single crystals
Yuui Yokota1, Yuji Ohashi1, Takahiko Horiai1, Akira Yoshikawa1
1

Tohoku University, 2-1-1 Katahira Aoba-ku Sendai, Japan*E-mail: yui.yokota.a5@tohoku.ac.jp

Ca3NbGa3Si2O14 [CNGS] and Ca3TaGa3Si2O14 [CTGS] piezoelectric single crystals with thelangasite-type structure have been studied for applications of pressure sensor at high temperature andsmall oscillator with low power consumption because of their stable piezoelectric properties at hightemperature, stable temperature coefficient of frequency and low impedance. Ga site in the CNGS and
CTGS single crystals can be substituted by Al ion, and we reported the crystal growth and thepiezoelectric properties of Ca3Nb(Ga,Al)3Si2O14 [CNGAS] single crystals with 0-50% Al concentrations
and Ca3Ta(Ga,Al)3Si2O14 [CTGAS] single crystals with 0-100% Al concentrations[1-4]. In the previous
reports, the lattice parameters and piezoelectric properties systematically changed with the Alconcentration. In this study, we conducted more detailed crystal structure analysis using X-ray to reveal
the relationship between crystal structures and piezoelectric properties of CNGAS and CTGAS single
crystals to clarify effects of Al substitution.
Ca3Nb(Ga1-xAlx)3Si2O14 [x = 0, 0.25, 0.5] and Ca3Ta(Ga1-yAly)3Si2O14 [y = 0, 0.25, 0.5, 0.75, 1.0] single
crystals were grown by the Czochralski method[1,2] and crystal structures of single crystals were
investigated by the X-ray diffractometer with an imaging plate. Bulk wave velocities were measured bya plane-wave ultrasonic material characterization system[3,4]. Dielectric constants and coefficients ofthermal expansion were determined by an impedance analyzer and a dilatometer, respectively.
Crystal structures of CNGAS and CTGAS single crystals could be obtained with high precision[5],and Figure 1 is the SiO4 tetrahedron and of the Ca3Nb(Ga0.5Al0.5)3Si2O14 [x = 0.5] single crystal withbond lengths and angles. O(2)-Si-O(2) and Si-O(2)-(Ga,Al) bond angles systematically increased withthe shift of Si in z-axis by increasing Al concentration. Cation shift of the Si ion out of center from thebarycenter of the oxygen coordination environment in CNGAS and CTGAS single crystals
systematically decreased with increasing Al concentration, and cation shift of the (Ga,Al) ion slightly
decreased, suggesting the decrease of the dielectric constants are attributable to the decrease of cation
shifts of Si and (Ga,Al) ions by Al substitution.
[1] Y. Yokota, et al.: Jpn. J. Appl. Phys., 54(10) (2015)
10ND13[2] Y. Yokota, et al.: J. Cryst. Growth, 468 (2017) 321[3] Y. Ohashi, Y. Yokota, et al., IEEE Trans. Ultrason.
Ferroelectr. Freq. Control, 63(10) (2016) 1575
[4] Y. Ohashi, Y. Yokota, et al.: Jpn. J. Appl. Phys., 56(7)(2017) 07JB03[5] Y. Yokota, et al., J. Solid State Chem. 277 (2019) 195

27

Fig. 1 Bond lengths and angles on SiO4
tetrahedron of Ca3Nb(Ga0.5Al0.5)3Si2O14
single crystal.

B-3:

Simultaneously achieving giant piezoelectricity and record coercive fieldenhancement in relaxor-based ferroelectric crystals
Limei Zheng1*, Liya Yang2, Gang Liu3
1

Shandong University, Jinan 250100 China
Henan University, Kaifeng 475004, China
3
Center for High Pressure Science and Technology Advanced Research, Shanghai 201203,
China
2*E-mail: zhenglm@mail.sdu.edu.cn
Both a large coercive field (EC) and a giant piezoelectric activity are essential for the ferroelectricmaterials used in high-drive electromechanical applications, especially the case for greater power
efficiency, smaller size, and lighter weight. A breakthrough in ferroelectric material is the discovery of
relaxor-PbTiO3 crystals, which have the highest piezoelectricity known today, but usually with low EC
being on the order of only 2-3 kV/cm. Such a performance deterioration is originated from the fact thatthe high piezoelectricity is usually interlinked to an easy polarization rotation, then favoring a dipole
switch under small external stimuli. Therefore, searching for new types of ferroelectrics withsimultaneously large EC and ultrahigh piezoelectricity becomes an imminent challenge. Here, byadopting a microstructure design strategy involving small amount of scandium (Sc) doping, a novel
ternary Pb(Sc1/2Nb1/2)O3-Pb(Mg1/3Nb2/3)O3-PbTiO3 crystal is reported, where the dispersed local
heterogeneity featuring a considerable amount of tetragonal phase is confirmed. As a result, both
elevated energy barriers and flattened potential wells are thermodynamically achieved, demonstrating alarge EC of 8.2 kV/cm (a factor of 3 greater than that of Pb(Mg1/3Nb2/3)O3-PbTiO3) and ultrahighpiezoelectricity (d33=2630 pC/N; d15=490 pC/N). The observed EC enhancement is the largest for
ultrahigh-piezoelectric ferroelectric crystals, far exceeding the previously reported enhancements
induced by the doping effects and other techniques. This updating investigation provides a simple,
practical, and universal route for improving functionalities in ferroelectrics with an atomic-level
understanding, which is critical for future material-by-design.

28

B-4:
Enhanced polarization property of PZT produced by press forming
Muneyasu Suzuki*, Harutaka Mekaru, Tetsuo Tsuchiya, Jun Akedo
AIST, JAPAN*E-mail: suzuki.muneyasu@aist.go.jp
Ferroelectrics are one of the most attractive materials to produce various electronic ceramics and to
generate electricity, because of their high permittivity, excellent piezoelectricity and pyroelectricity
derived from their unique crystal structures. In particular, lead zirconate titanate (PZT) is applied tovarious applications such as energy harvesting units, optical mirrors for laser displays, SAW/BAW filters,
or gyrosensors, which are essential for suppling functionality or power to electrical devices. Since
flexible substrates are sometimes indispensable in order to mount these oxide ferroelectrics on flexible
or stretchable devices which have attracted attention recently, heat treatment in ceramic synthesis isoften a problem. Therefore, advanced ceramics synthesis technique that eliminate for high-temperatureprocess during manufacturing are strongly required in those research and development. In other words,
low temperature synthesis of highly dense PZT ceramics that usually require sintering at temperatures
above 1000°C via a solid-state reaction have been actively researched. For example, the PZT can beobtained at temperatures below 300°C by using cold sintering.1) Aerosol deposition allows the
production of fully dense nanocrystalline ceramic films with a thickness of more than 1 μm at room
temperature.2) Technologies for transferring single-crystal thin films deposited by epitaxial growth or
high-temperature crystallized films onto plastic substrates have also been advanced.3) Thin films havebeen successfully formed by using regularly arrayed nanomaterials such as nanocubes.4)
We developed a new press forming-based, room temperaturedense aggregate oxide films at a pressure below 1 GPa, which is lower
than that at which oxide particles fracture, by taking advantage of thedifferences in the cohesive force between microsized and nanosized4)

particles. The MF method allowed us to produce high dense ceramic
films with both high gas permeability and high impregnability. We
succeeded in producing a PZT MF film with relative density of 94 %on an aluminum foil at room temperature that when impregnated withsilicone oil exhibited saturated polarization hysteresis [see fig.1].

80

Polarization ( C/cm2)

process, the mega-press forming (MF) method, that produces highly

40

0

-40

＠1Hz, R.T.

-80
-800

-400

0
Electric field (kV/cm)

400

800

Fig.1 Polarization property for
PZT film produced by press
forming at room temperatureon Al foil. This PZT film was
not done any heat treatment.

References
1) J. Guo, H, Guo, A. Baker, M. Lanagan, E. Kupp, G. Messing, et al., Angew. Chemie Int. Ed. 55,
11457 (2016).
2) J. Akedo, J. Am. Ceram. Soc. 89, 1834 (2006).
3) T. Liu, M. Wallace, S. Trolier-McKinstry, T. Jackson, J Appl Phys. 122, 164103 (2017).
4) Y. Takada, K. Mimura Z. Liu and K. Kato, Journal of Crystal Growth 548, 125811 (2020).
5) M. Suzuki, Y. Kusaka, T. Tsuchiya, H. Ushijima and J. Akedo, J. Am. Ceram. Soc. 103, 3479 (2020).

29

B-5:
High Piezoelectric Performance of Textured Relaxor-PT/PZT Ceramics
Yan Yongke1,2,*, Xu Zhuo1, Priya Shashank2
1Electronic Materials Research Laboratory, Key Laboratory of the Ministry of Education &International Center for Dielectric Research, School of Electronic Science and Engineering, Xi’an
Jiaotong University, Xi’an 710049, P.R. China
2

Department of Materials Science and Engineering, The Pennsylvania State University, University
Park, PA, 16802, USA*E-mail: yanyongke@xjtu.edu.cn
High performance piezoelectric materials have attracted great attention from both the high-tech

application and fundamental research due to wide applications as actuators, sensors, and transducers.
Particularly, textured piezoelectric ceramics are highly demanded, considering of excellent performance
similar to that of single crystal and low cost similar to that of random ceramics. In this talk, we firstpresent our prior achievements in textured relaxor-PT/PZT ceramics, and then introduce our recent
progress on achieving ultra-high piezoelectricity in rare-earth doped textured PMN-PT ceramics andnear-ideal electromechanical coupling in highly textured PMN-PZT ceramics. Several representative
characteristics of textured piezoelectric ceramics will be highlighted:
High energy density: We demonstrated textured PMN-PZT ceramics which provide highest
known energy density in piezoelectric materials through simultaneously enhancement of piezoelectriccharge and voltage coefficients (d and g). We obtained a giant magnitude of d·g coefficient with valueof 59000 × 10-15 m2 N-1 (comparable to that of the single crystal counterpart and 360% higher than thatof the best commercial compositions).
High piezoelectric voltage coefficient: Single-phase oxide piezoelectric materials with giant
piezoelectric voltage coefficient (g, induced voltage under applied stress) and high Curie temperature(Tc) are crucial towards providing desired performance for sensing, especially, under harshenvironmental conditions. We provided a rational design of high g textured piezoelectric ceramics forsensing via incorporating (a) anisotropy/composition/phase structure, (b) microstructure and (c) domain
engineering. We reported a <001> textured PbTiO3-based ceramics that has a high Tc (~364 °C) and an
extremely large g33 (115 ×10-3 Vm/N) in comparison to other known single-phase oxide materials.
Near-ideal electromechanical coupling: Electromechanical coupling factor, k, of piezoelectricmaterials determines the conversion efficiency of mechanical to electrical energy or electrical tomechanical energy. We reported a near-ideal k value of 0.93 in textured PMN-PZT which reaches thesame magnitude as that for a single crystal, far beyond the average value of traditional ceramics. This
demonstration of near-ideal k value in textured ceramics will have tremendous impact on design of ultrawide bandwidth, high efficiency, high power density, and high stability piezoelectric devices.

30

B-6:

A Review of Lead Perovskite Piezoelectric Single Crystals and Their Medical Transducers
Application
Yohachi (john) Yamashita1,2,3, 1Tomoaki Karaki, and 2Horoshi Maiwa
1

Toyama Prefect. Univ, Japan, 2Shonan IT, Japan, and 3NCSU, USA,

*E-mail:sxjwg220@ybb.ne.jp

Piezoelectric materials have been developed since early 1900s and many research had been conductedon the composition and process to obtain higher piezoelectric constants (d33). Within composition
research, lead perovskite relaxor piezoelectric single crystals (SCs) of binary Pb(Mg1/3Nb2/3)O3-

lead titanate PbTiO3 (PMN-PT) and ternary Pb(In1/2Nb1/2)O3-PMN-PT SCs have been actively studied
since 1990s because of their outstanding d33>1,500 pC/N compared to those of conventional Pb(Zr,Ti)O3
ceramics.

A major driving force of these SC research has been promoted by mass-production ofultrasound transducers and arrays probes for medical diagnostic systems since early 2000s. However,
the higher d33 material and process research for these ultrasound devices are almost saturated. In thisreview article, we present a brief overview of the history, current situation, and future perspective ofpiezoelectric SCs. Authors believe that main research in the next century is high d33 SCs with a highcomposition uniformity and low-energy SC growth methods, such as solid-state-SC growth, lowmaterial loss SC transducer manufacturing technique, and improved poling process. This is a big
technical challenge for all scientists; however, the relatively large market of medical ultrasound has been
expanded year by year, and we hope that the community is motivated to solve such technical problems
in the near future.

31

B-7:
Domain Engineering Effect of Alternating Current Poling with Different Frequency on
PMN-PT Single Crystals
Chengtao Luo1,*, Haotian2 Wan2, Chang Liu2, Wei-Yi Chang2, Yohachi Yamashita2,3, and Xiaoning
Jiang2,*
1

School of Sensing Science and Engineering, School of Electronic Information and ElectricalEngineering, Shanghai Jiao Tong University, Shanghai 200240, China

2State Key Laboratory of Metal Matrix Composites, School of Materials Science and Engineering,
Shanghai Jiao Tong University, Shanghai 200240, China

3

Artificial Crystal Research Center, Shanghai Institute of Ceramics, Chinese Academy of Sciences,
Shanghai 201800, China*E-mail: cluo1989@sjtu.edu.cn, xjiang5@ncsu.edu

The alternating current (electric field) poling (ACP) was applied on [001]-oriented
0.7Pb(Mg1/3Nb2/3)O3 - 0.3PbTiO3 (PMN-0.3PT) single crystal samples with dimensions of 5mm-thick k33 mode and the influence of ACP frequency (fACP) was studied. Compared tothose from traditional direct (electric field) poling (DCP) samples, d33 and εT33/ε0) of ACP
samples could gain up to 67% increase to 3200 pC/N and 10500, respectively. In this work, low
fACP is preferred for better enhancement. The ACP dynamics and the corresponding domain
engineering effect during the saturation process were studied by both P-E loops and phase-field
simulation.

Figure 1. The saturation process as a function of cycle number (cycle 2 to saturated cycle 30) for (a)coercive field and (b) positive remnant polarization (c) The current density changes between
unsaturated (cycle 2) and saturated cycles are compared.
(a)

[100]
[010]

(b)

(c)

(d)

(e)

[001]

E-Field
71 domain wall
109 domain wall

Figure 2. Phase-field simulation of the domain structures evolution during ACP form ‘4R’ to ‘2R’
configuration.
32

C-1:

Tuning of polar domain boundaries in non-polar perovskite
Nan Zhang1, Zheyi An1, Hiroko Yokota 2,3, Marek Paściak4, Wei Ren1, Zuo-Guang Ye5
Electronic Materials Research Laboratory, Key Laboratory of the Ministry of Education &International Center for Dielectric Research, School of Electronic Science and Engineering, Xi’an
Jiaotong University, Xi'an 710049, China
2
Department of Physics, Chiba University, 1-33 Yayoi-cho, Inage-ku, Chiba City, 263-8522, Japan
3
JST PRESTO, 7 Goban-cho, Chiyoda-Ku, Tokyo, 102-0076, Japan4
FZU - Institute of Physics of the Czech Academy of Sciences, Na Slovance 2, 182 21 Prague 8,
Czech Republic
5
Department of Chemistry and 4D LABS, Simon Fraser University, 8888 University Drive, Burnaby,
British Columbia V5A 1S6, Canada
1

Domain-boundary engineering possesses great potential in nanotechnology industries. Domainboundaries in ferroic materials, as 2D topological defects, are found to have various physicalproperties not found in the surrounding domains, such as high conductivity, photovoltaic effect, andchirality. These properties can be enhanced and bring promising functionalities when centrosymmetricnon-polar materials encounter polar domain boundaries.
In this work, a tunable polar domain boundary is discovered in an antiferroelectric single crystal.
Under a small stress or electric field, the density, volume, and polarity of the boundaries are
successfully controlled. We first confirmed the macroscopic polarity of the domain boundaries in
antiferroelectric PbZr1-xTixO3 (PZT) single crystals, using Second Harmonic Generation (SHG).
Structural studies unveiled that the origin of the polarity comes from the atomistic structure of the
antiphase boundaries, which possess a slightly different ionic displacement pattern from the bulk.
Because of the structural compatibility, they occur more abundantly than in other ferroelastic materials
and are proved to be easier to control. The domain boundaries can be preferentially created and erased
by applying a small stress. The polarity of domain boundaries can be enhanced or switched with asmall electric field. This work sheds light on this area not only by confirming its potential applicationin nanotechnology but also by promoting a fundamental understanding on this issue.

33

C-2:
Microstructure Design and Exotic Electrostrain Response in Layer Structured
Perovskite Ferroelectric Ceramics
Xiang He1, Zhiguo Yi1*
1

Shanghai Institute of Ceramics, Chinese Academy of Sciences, China*E-mail: zhiguo@mail.sic.ac.cn

It is well known that the electrostrain of ferroelectric materials mainly comes from the contributionsof intrinsic strain (electrostriction and piezoelectric response) and extrinsic strain (domain inversion andphase transition). In the past few decades, in order to improve the electrostrain output of ferroelectricmaterials, researchers have generally used crystal structure regulation and Morphotropic phase boundary
design to improve the electromechanical response characteristics of samples, and achieved great successin lead containing material systems. Its typical feature is the significantly enhanced butterfly strain curve
value. Compared with lead containing materials, Bi2WO6 has the advantages of high Curie temperatureand environmental friendliness, and is a promising high-temperature piezoelectric actuator material.
However, due to the two-dimensional lamellar grain growth habit, large polarization anisotropy and low
piezoelectric activity of Bi2WO6, its electromechanical response characteristics have not been reported.
In this paper, bismuth layered Bi2WO6 ferroelectric ceramics with different microstructures wereprepared by combining discharge plasma sintering and traditional solid phase sintering. A strange loop
shaped strain curve was observed in textured Bi2WO6 ceramics for the first time. The maximum apparent
strain was up to 0.75%, and it also had good cycle stability, superior to most lead-free ferroelectrics. It
is worth noting that this loop type strain curve is different from the asymmetric strain electric field curve
observed in traditional hard doped ceramic materials, and its asymmetric direction does not reverse withthe sample turnover. Through repeated verification of the test system and test conditions, combined with
piezoelectric response force microscope observation and X-ray photoelectron spectroscopy analysis, theauthor revealed that the singular strain curve originated from the reversible bending deformation causedby the asymmetric inversion of 90 °ferroelastic domains on the upper and lower surfaces of ceramicmaterials. Unlike the electromechanical response characterized by butterfly loops, which reflects theuniform expansion or contraction of the sample along the thickness direction under the action of electricfield, and also different from the asymmetric strain curve caused by defects or internal bias fields, thisstudy reveals a new strain mode that may exist in ferroelectric materials, that is, the bending deformation
caused by the non-uniform deformation of the sample under the action of electric field. This discovery
not only provides a new idea for the design of piezoelectric actuators, but also provides a new idea forthe origin of asymmetric strain curves.

34

C-3:
Synergic Modulation of the Multi-scale Structures on the Energy Storage Properties ofSilver Niobate-Based Ceramics
J Wang1*, XH Fan1,2, Y Rao1,2, L Zhao3*, KJ Zhu11
1

State Key Laboratory of Mechanics and Control of Mechanical Structures, College of Aerospace
Engineering, Nanjing University of Aeronautics and Astronautics, Nanjing 210016, China

2

School of Materials Science and Engineering, Nanjing University of Aeronautics and Astronautics,
Nanjing 210016, China
3

Hebei Key Lab of Optic-Electronic Information and Materials, College Physics Science &Technology, Hebei University, Baoding 071002, China*E-mail: wang-jing@nuaa.edu.cn;leizhao@hbu.edu.cn

Silver niobate AgNbO3 ceramics have been regarded as a promising lead-free material for energy
storage applications. Benefiting from the hydrothermal synthesised AgNbO3 powders, AgNbO3
ceramics with fine-grain of ~3.4 m were obtained. The fine-grain leads to increased electric breakdown
strength Eb up to 250 kV/cm, which is the highest among the pure AgNbO3 ceramics to our best
knowledge. Extending beyond prior art for the compositional modification, synergic modulation of themulti-scale structures on the energy storage properties of AgNbO3-based ceramics was reported, inwhich the introduction of MnO2 at the atomic-scale improves the electric field of the FE-AFE phasetransitions (EA) while the SiO2 coating on the AgNbO3 particles at the micro-scale greatly increases theelectric filed inducing the AFE-FE transitions (EF) and Eb. As a result, 0.10 wt% MnO2-doped
AgNbO3@SiO2 ceramics reveal a recoverable energy density up to 3.34 J/cm3 and efficiency of 60.0%,
indicating 2.3 and 1.6 times larger than its counterpart of pristine AgNbO3. Furthermore, equivalentamount Bi2O3 and Sc2O3 were subsequently introduced to improve the energy storage property of 0.10
wt% MnO2-doped AgNbO3@SiO2 ceramics by simultaneously enhancing the maximum polarization,
breakdown strength and relaxation feature. Of particular interest is that the AgNbO 3-based ceramics
with 4 mol% Bi2O3 and Sc2O3 demonstrate the recoverable energy storage density of 5.9 J/cm3 with theenergy storage efficiency of 71%. In addition, the benign energy storage performance can be maintainedat elevated temperatures, frequencies and up to 105 cycling, foreshowing great potential in advanced
high-power applications. Our work provides a rational approach to synergically modulate the energy
storage properties via the design of multi-scale structures.

35

C-4:

Atomic-Scale Studies of PbZrO3-based Antiferroelectric Ceramics
Zhengqian Fu 1 , Xuefeng Chen 2 , Zhenqin Li 1,3, Tengfei Hu 1,4, Ziyi Yu 1,4, Linlin Zhang 1, Shujun
Zhang 5, Genshui Wang 1,2, Xianlin Dong 1,2,4, Fangfang Xu 1,4

Affiliations:
1State Key Laboratory of High Performance Ceramics and Superfine Microstructures, Shanghai

Institute of Ceramics, Chinese Academy of Sciences, Shanghai 200050, China.
2

The Key Lab of Inorganic Functional Materials and Devices, Shanghai Institute of Ceramics,

Chinese Academy of Sciences, Shanghai 200050, China.
3

University of Chinese Academy of Sciences, Beijing 100049, China.

4

School of Physical Science and Technology, ShanghaiTech University, Shanghai 201210, China.

5Institute for Superconducting and Electronic Materials, Australian Institute of Innovative Materials,

University of Wollongong, Wollongong, New South Wales 2500, Australia.

Abstract:
Benefitting from the reversible phase transition between antiferroelectric and ferroelectric states,
antiferroelectric materials have recently received widespread attentions for energy storage applications.
Antiferroelectric configuration with specific antiparallel dipoles has been used to establish
antiferroelectric theories and understand its characteristic behaviors. In this presentation, we present
that the so-called antiferroelectric (Pb,La)(Zr,Sn,Ti)O3 system is actually ferrielectric in nature. We
demonstrate that the width and net polarization of ferroelectric ordering segments can be tailored bycomposition, which is linearly related to the key electrical characteristics, including switching field,
remanent polarization and dielectric constant. Furthermore, we show how the modulated structure
respond toexternal stimulus.

These findings

provide opportunities

for comprehending

structure-property correlation and fundamental understanding on antiferroelectric materials.

36

C-5:

Ferroelectric Materials and Devices for Intelligent Computing
Xiao Yu1,2, Yue Peng2, Jiuren Zhou2, Genquan Han2,*
Research Center for Intelligent Chips and Device, Zhejiang Lab, Hangzhou 311121, China

1

2

School of Microelectronics, Xidian University, Xi’an 710071, China*E-mail: gqhan@xidian.edu.cn

Recently, transistor scaling is approaching its physical limit, hindering the further development of
the computing capability, as shown in Fig. 1(a). The first is “power wall”, which block theenhancement of main frequency of the processer due to rising power density and heating effect; thesecond is “memory wall”, which is induced by huge performance or area gap between logic device andmemory cell. The last is called Von Neumann bottleneck (BN) that huge data move between memory
and processor would induce obvious delay and power issues.
In the post-Moore era, emerging logic and storage devices have been the fundamental hardware for
expanding the capability of intelligent computing. Among them the emerging ferroelectricmaterials-based devices could reduce the obstacles of “power wall” “memory wall” and Von Neumannbottleneck, as illustrated in Fig. 1(b). In this presentation, the recent progress of ferroelectric devices
for intelligent computing is discussed. The material properties and electrical characteristics offerroelectric devices are elucidated, followed by a discussion of novel ferroelectric materials anddevices that can be used for intelligent computing. Ferroelectric capacitors, transistors, and tunneling
junction devices used for low-power logic, high-performance memory, and neuromorphic applications
are comprehensively reviewed and compared. In addition, to provide useful guidance for developing
high-performance ferroelectric-based intelligent computing systems, the key challenges for realizing
ultrascaled ferroelectric devices for high-efficiency computing are discussed.

Fig. 1 Schematics of (a) challenges faced by modern computers using von Neumann architecture and (b)solutions for “heat wall”, “memory wall”, and von Neumann bottleneck based on ferroelectric devices.

37

C-6:
Excellent pyroelectric properties of relaxor-based ferroelectric
single crystals and thin films for infrared detection
Yanxue Tang1*, Haosu Luo 2
1

Shanghai Normal University, China

2

Shanghai Institute of Ceramics, Chinese Academy of Sciences, China*E-mail: yanxuetang@shnu.edu.cn

Infrared detectors and imagers based on a pyroelectric detection mechanism can be operated atambient temperatures without cooling systems, as well as having broader spectral responsivity comparedto the photon-based ones. The development of highly-sensitive, high-stability, and low-power uncooled
infrared detectors and imagers has a strong need for pyroelectric materials with high pyroelectriccoefficients and low dielectric loss. All pyroelectric crystals are also piezoelectric, the thermal expansion
induced by heating leads to a strain which operates through the piezoelectric effect to give an additional
secondary pyroelectric effect, therefore, large primary but low secondary pyroelectric coefficients aredesirable for pyroelectric sensors.
We have investigated the composition, orientation, and temperature dependence of structures andpyroelectric properties for pure and Mn-doped binary Pb(Mg1/3Nb2/3)O3–PbTiO3 and ternary
Pb(In1/2Nb1/2)O3-Pb(Mg1/3Nb2/3)O3–PbTiO3 relaxor-based ferroelectric single crystals and thin films.
The secondary pyroelectric coefficients were calculated using thermodynamics method. Excellent
pyroelectric properties with good thermal stability have been achieved for infrared detecting andimaging applications. The essential relationship between pyroelectric properties and microstructures
have been determined. The high figures of merit, together with good thermal stability, make thematerials promising candidates for high-performance infrared detectors and thermal imagers.
Key words: Ferroelectric, Pyroelectric properties, Infrared detection

38

C-7:
Heterostructural magnetoelectric composites and application in magnetic field andcurrent sensing
Jie Jiao1*, Rui Chen1, Hanzhou Wu2, Yaojin Wang2, Haosu Luo1, Li Lu1, Wenning Di1
1
Shanghai Institute of Ceramics, Chinese Academy of Sciences, China
2
Nanjing University of Science and Technology, China*E-mail: jiejiao@mail.sic.ac.cn
Abstract: High-performance weak magnetic sensors have important uses in medical diagnostics,
resource exploration, military anti-submarine and automotive electronics. In this study, we optimize
the overall performance of magnetoelectric weak magnetic sensors from the perspective of noiseequivalent magnetic field by both reducing the noise level and improving the magnetoelectric response,and explore its application prospects in the field of current sensing. Magnetoelectric composites are
the core of magnetoelectric sensors, whose noise at low frequencies mainly originates from DC
resistance noise and dielectric loss noise, of which dielectric loss noise dominates. It was found thatannealing under high-temperature oxygen-rich conditions significantly reduces the dielectric loss ofthe crystal, resulting in a reduction in the overall noise level of the sensor. On the other hand, thepiezoelectric performance is enhanced by using AC polarization to enhance the non-intrinsic
piezoelectric effect, resulting in a 54.6% increase in the responsivity of the magnetoelectric sensor at
low frequencies. Based on the optimization results of the above two aspects, the noise equivalentmagnetic field of the magnetoelectric sensor prepared by exploiting the bulk effect reaches 0.7±0.2
pT/Hz1/2@1Hz, and the detection capability far exceeds that of the embargoed version of the fluxgate(6 pT/Hz1/2@1Hz). Compared to conventional current sensors (current transformers, Hall effectcurrent sensors, etc.), magnetoelectric devices are considered as a new solution for current sensing due
to their low power consumption and high sensitivity. Here, we report a current visualization sensor,
working on the magnetoelectric/electrochromic principle, that converts the current energy in theenvironment into an electrical signal and subsequently into an easily observable color change, which
has important applications in current monitoring, alarming, etc.

39

D-1:

High Curie temperature BiFeO3-BaTiO3 lead-free piezoelectric ceramics: One-step
preparation
Yu-Cheng Tang1, Ai-Zhen Song1, Yang Yin1, He-Zhang Li2, Bo-Ping Zhang1*
University of Science and Technology Beijing, China

1National Institute for Materials Science (NIMS) 1-2-1 Sengen, Japan2*E-mail: bpzhang@ustb.edu.cn
A notorious problem in BiFeO3-based piezoelectric ceramics is how to limit the formation of the
impurities Bi25FeO39 and/or Bi2Fe4O9 to give them excellent piezoelectric performance. Based on the
Gibbs free energies of BiFeO3, Bi25FeO40 and Bi2Fe4O9, a new one-step calcining and sintering process
was proposed to prepare BiFeO3-xBaTiO3 (BF-xBT) ceramics at a low sintering temperature, which
can prevent impurity formation and realize the low-temperature sintering of single BF-xBT ceramics.
The resultant ceramics are compact, porous-less, display macro-scale stripe dmains along with a small
amount of island-like domains, and exhibite saturated P-E loops, typical I-V characteristics, butterfly
S-E curves and excellent piezoelectric properties (d33 = 198–203 pC/N; TC = 494–513 °C). A carefulanalysis of the XRD patterns of BF-xBT (0 ≤ x ≤ 1) powder at different calcination temperatures
reveals that the diffusion reaction path of ions is critical to prevent the formation of the impurities. It isalso found that the Bi content and sintering temperature (Tsint) have a little effect on the phase structure,insulation, ferroelectric, piezoelectric and dielectric properties for 0.7Bi(1+x)FeO3-0.7BaTiO3 ceramics
prepared by one-step preparation. Stable piezoelectric properties of d33 = 180–205 pC/N, Pr = 17.9–23.8
μC/cm2, Pm = 25.9–33.6 μC/cm2, TC = 485~518 °C was achieved at -0.03 ≤ x ≤ 0.05 and 930 °C ≤ Tsint ≤970 °C. Our results clarify the reaction mechanism and provide a synthesis strategy for designing highperformance piezoelectric materials with good stability and easy industrialization.

40

D-2:

Bismuth Ferrite Based Lead-Free Piezoelectric ceramics
Dawei Wang*
Functional Materials and Acousto-Optic Instruments Institute, School of Instrumentation Science andEngineering, Harbin Institute of Technology, Harbin 150080, China*E-mail: wangdawei102@gmail.com
Bismuth ferrite (BF)-based solid solutions are considered candidates as lead-free functional
ceramics due to their promising ferroelectric properties. Among various BF-based solid solutions,(1-x)BiFeO3-xBaTiO3 (BF-BT) has attracted attention for compositions within or close to a mixed
phase region (MPR) in which rhombohedral and cubic polymorphs coexist. These compositions havehigh ferroelectric Curie temperature (TC > 400 oC) but are also reported to have large remanent (Pr)and saturation (Ps) polarization coupled with large piezoelectric coefficients (d33), particularly forsamples quenched from the sintering temperature. More importantly, large electric field-induced
strains and strain coefficients have been extensively reported in doped BF-BT within the MPR for 0.25
< BT < 0.35. The element doping or substitution of a third component (often a nominal perovskite
composition) in the BF-BT solid solution, results in a ferroelectric to relaxor-ferroelectric phasetransition and further enhances strain. In this presentation, recent progress on the high electrostrains
for BF-BT-based lead-free piezoelectric ceramics will be reviewed and the origin of the large
electrostrain using in situ poling synchrotron X-ray diffraction will be discussed.

41

D-3:
Mechanism of Material Hardening on (Bi0.5Na0.5)TiO3-based
Lead-free Piezoelectric Ceramics by Quenching Treatment
Takeru Tayama1, Yuka Takagi1, and Hajime Nagata1*
1

Tokyo University of Science, Japan*E-mail: h-nagata@rs.tus.ac.jp

Bismuth sodium titanate (Bi0.5Na0.5)TiO3 (BNT)-based solid solutions have relatively highpiezoelectric properties and mechanical quality factor in lead-free piezoelectric materials; therefore,
they have attracted attention as the candidate lead-free materials for ultrasonic devices. However, BNT
has the problem of having a low depolarization temperature Td of approximately 180oC, resulting in
narrow working temperature. In particular, the morphotropic phase boundaries (MPBs) of BNT-basedsolid solutions have a low Td of approximately 100oC, even though an MPB has excellent piezoelectric
properties. That is, the piezoelectric constant and Td show a trade-off relationship, so that the elevationof Td without the deterioration of piezoelectric activities is strongly demanded for practical piezoelectric
applications using BNT-based ceramics.
Recently, our group has reported that a quenching procedure during the sintering process was aneffective way of increasing the Td of pure BNT ceramics without deteriorating their ferroelectric andpiezoelectric properties.1) The Td of a BNT sample quenched from 1100 oC was 223 oC, which was
almost 50 oC higher than that prepared by the ordinary cooling process. On the other hand, it is generally
known that quenching process affects the mechanical bending strength of the ceramics weaken by athermal shock. Since the Td increased by the quenching treatment from above 800˚C in our previous
study, we controlled quenching rate QR in the range from 1100˚C to 800˚C. Then, both Td andmechanical strength reached higher values by controlling the QR.
In the presentation therefore, we will focus on a mechanism of the quenching effects and it
influence for electrical and mechanical properties on BNT-based ceramics. Then, it is concluded that
controlling QR is an effective method to improve both Td, piezoelectric properties and mechanicalstrength simultaneously. Furthermore, we have applied the quenching procedure to the BNT-based solid
solution systems with MPB and tetragonal phase. Even though in the MPB and tetragonal phases, BNTbased solid solution system (BNT-BaTiO3 system) indicated higher Td after the quenching treatment.2)
Piezoelectric performances were slightly decreased, whereas the Td was increased significantly.
Additionally, an elastic compliance s33E was decreased and a mechanical quality factor Qm was increased
after the quenching treatment. In other word, a hardening effect was observed after the quenchingtreatment on this composition. We will also discuss about the reasons of hardening effects by quenchingtreatment from the measurements of oxygen vacancies (by SIMS) and microstructure (by SEM and
TEM). Then, a product of piezoelectric constant d and Qm (dQ product: one of the figure of merit for
high-power piezoelectric properties) was increased after the quenching treatment. We think this is goodsign for the high-power piezoelectric applications.
1) H. Muramatsu, H. Nagata, and T. Takenaka, Jpn. J. Appl. Phys., 55 (2016) 10TB07.
2) T. Miura, H. Nagata, and T. Takenaka, Jpn. J. Appl. Phys., 56 (2017) 10PD05.

42

D-4:

Studies of Domain Structure in (K,Na)NbO3-based Ceramics with Acid-Etching
Zhang Jialiang
School of Physics, State Key Laboratory of Crystal Materials, Shandong University, Jinan 250100, P.
R. China*E-mail: zhangjialiang@sdu.edu.cn
Piezoelectric performance of a ferroelectric ceramic can be greatly affected by its domain structure,
which in turn is usually determined by chemical composition, microstructure, phase state andtemperature. How to characterize the domain structure is important for the understanding ofpiezoelectric performance. The structural observation of thin specimens with a transmission electron
microscope (TEM) and the morphological observation of chemically etched surface with an optical
microscope or a scanning electron microscope (SEM) are the two commonly used methods.
The TEM observation can give the details of both lattice structure and nanodomain structure owing
to high magnification. However, it requires very thin specimens that is sensitive to the preparation
procedure, in which domain structure may change irreversibly due to the mechanical stresses ofgrinding, dimpling and focused ion-beam milling. Further, grains in a thin ceramic specimen are
obviously in the different clamping state from those in a bulk ceramic, which may also lead to a
substantial change in the domain structure. The case becomes even more critical when observing thedomain structure for those ferroelectric ceramics that have one phase transition occurring around room
temperature. Additionally, the obtained information comes only from a very limited area and thus may
not be representative, but be regional with large randomicity since the actual domain structure may
differ significantly from grains to grains. Therefore, it is safe to take great caution when reading thoseresults obtained by the TEM observation. On the other hand, acid-etching is considered as aconvenient and quite reliable technique. Its working principle is based on the difference in etching rate
between two adjacent domains of different polarization orientations at the specimen surface. Since theetched domain patterns can be easily observed with an optical microscope or a scanning electron
microscope (SEM), acid-etching facilitates the study of domain structure for a large number of grains
and makes it possible to acquire the overall characteristic and regularity, thereby enabling us to draw
the credible conclusions on the basis of statistical information.
Due to the reasons described above, the acid-etching method has been frequently adopted in ourstudies of the various KNN-based ceramics. This talk will mainly report the results obtained in our
two recent studies. One is to explore the compositional effects on piezoelectric properties, phasetransitions and domain structure in a series of (1-x)(K0.48Na0.52)Nb0.955Sb0.045O3–x(Bi0.50Na0.50)HfO3
ceramics with 0.01 ≦ x ≦ 0.04. The other is to systematically investigate the evolution of domain
structure in the 0.96(K0.48Na0.52)(Nb0.96Sb0.04)O3−0.04(Bi0.50Na0.50)ZrO3 ceramics of a large d33 of 512
pC/N with poling and temperature.
[1] J. L. Zhang and X. M. Wang, Materialia, 17 (2021) 101120.
[2] J. L. Zhang and C. M. Zhou, J. Materiomics, 8 (2022) 9.

43

D-5:

Effect of Li2CO3 and MnCO3 Addition on Properties of (Ba,Ca)(Ti,Sn)O3 Piezoelectric
Ceramics Sintered Under Controlled Low Oxygen Partial Pressure
K. Uematsu, W. Sakamoto*Department of Applied Chemistry, College of Engineering, Chubu University, Japan*E-mail: sakamoto@isc.chubu.ac.jp
Pb(Zr,Ti)O3 (PZT)-based materials have been widely used as piezoelectric ceramics for a longtime. However, these materials contain toxic PbO as a major component. Because of growing concerns
about the global environmental issues, development of materials which do not contain toxic elements
is strongly demanded. Among several lead-free piezoelectric ceramics, BaTiO3–based materials havebeen receiving much attention as a potential candidate. Chemical composition modification of BaTiO3
has been extensively investigated to realize the desired electrical properties. Furthermore, for thedevelopment of the multilayer devices with high performance and low cost, reduction-resistantpiezoelectric ceramics, which can use base metal electrodes, are also important.
In this study, reduction-resistant lead-free (Ba,Ca)(Ti,Sn)O3 piezoceramics with highpiezoelectric constants were firstly investigated by optimizing the Li2CO3 addition. For the sintering ofthe (Ba,Ca)(Ti,Sn)O3 ceramics in a reducing atmosphere, the oxygen partial pressure was controlled
by using Ar-H2–CO2 mixed gas. Enhanced grain growth and a high polarization state after polingtreatment were achieved by adding Li2CO3 to (Ba,Ca)(Ti,Sn)O3. Among various amount of Li2CO3
added (Ba0.95Ca0.05)(Ti0.95Sn0.05)O3, (Ba0.95Ca0.05)(Ti0.95Sn0.05)O3 ceramics with 3 mol% Li2CO3 addition
were found to exhibit excellent piezoelectric properties while maintaining the high sintered density.
Sintered bodies of the 3 mol% Li2CO3-added (Ba0.95Ca0.05)(Ti0.95Sn0.05)O3 ceramics prepared in aCO2(1.5%)–H2(0.3%)/Ar reducing atmosphere (PO2 = 10−8 atm at 1350°C) showed a piezoelectric
constant (d33) exceeding 500 pC/N. The piezoelectric properties of the Li2CO3-added(Ba0.95Ca0.05)(Ti0.95Sn0.05)O3 ceramics were comparable or superior to those of the same ceramicsintered in air. Also, grain growth was promoted even in Li2CO3-added (Ba0.95Ca0.05)(Ti0.95Sn0.05)O3
samplessintered

at

a

lower

temperaturethan

1350°C.

The

3

mol%

Li2CO3-added(Ba0.95Ca0.05)(Ti0.95Sn0.05)O3 ceramics fabricated at 1250°C in a reducing atmosphere exhibited the d33
approximately 580 pC/N.
MnCO3 and Li2CO3 (3 mol%)-added (Ba0.95Ca0.05)(Ti0.95Sn0.05)O3 ceramics were also studied not
only to improve reduction resistance but also to control the stability of ferroelectric domain structure.
In this case, Mn can act as an acceptor ion. The optimization of the amount of MnCO3 addition was
examined to increase the Qm value. As a result, the samples sintered at 1250°C in a reducing
atmosphere with 0.4 mol% of MnCO3 addition showed the d33 value of 500 pC/N or higher.
Furthermore, a relatively high mechanical quality factor Qm value (approximately 600) was alsoachieved. These results suggest that Li, Mn co-doped (Ba,Ca)(Ti,Sn)O3 ceramics sintered in a
reducing atmosphere could be applied to high-power piezoelectric devices.

44

D-6:
Investigations of multi-scale regulation and in-situ characterization of high temperature
piezoelectric ceramics
Zhiyong Zhou
Shanghai Institute of Ceramics, Chinese Academy of Sciences, 201899, Shanghai, China*E-mail: zyzhou@mail.sic.ac.cn
High temperature piezoelectric ceramics with layered structures (including bismuth layer andperovskite layer), characterized by high Curie temperature (TC: 650~1500 °C), are the key functional
components of high temperature piezoelectric sensors, transducers and other devices at 500 °C andabove, and are widely used in the fields of aerospace and nuclear energy for vibration monitoring andstructural health management under high temperature, high radiation, complex vibration and other harshenvironments.
Focusing on the bottleneck of low piezoelectric coefficient d33 of layered piezoelectric ceramics,
the piezoelectric properties were improved by means of A/B co-doping and ion-pairing effect doping,
and the structure-property relationship between structure and piezoelectric properties was systematicallystudied. d33 of bismuth layered Bi4Ti3O12 piezoelectric ceramic was increased from 7 pC/N to 40.2 pC/N.
In view of the lack of in situ high-temperature testing technology and equipment to study the service
stability of high-temperature piezoelectric ceramics, based on the quasi-static and dynamic resonancemethods, a multi parameter in-situ characterization technology and testing system from room
temperature to 700 °C were developed, and the temperature stability of high-temperature piezoelectric
ceramics was studied in depth, which promoted the practical application of piezoelectric materials andrelated devices in high-temperature fields.

45

E-1:
Enhanced energy storage ceramic capacitors utilizing ferrorestorable polarization
Yuji Noguchi1* and Hiroki Matsuo 2
1

Division of Information and Energy, Faculty of Advanced Science and Technology, Kumamoto University,
2-39-1, Kurokami, Chuo-ku, Kumamoto 860-8555, Japan
2
International Research Organization for Advanced Science & Technology (IROAST), Kumamoto University,
2-39-1, Kurokami, Chuo-ku, Kumamoto 860-8555, Japan*Corresponding author, e-mail: ynoguchi@cs.kumamoto-u.ac.jp

A self-powered system with a long lifetime offers an opportunity to develop a next-generation,
standalone Internet of Things. Ceramic capacitors are promising candidates for energy storage
components because of their stability and fast charge/discharge capability. Even for state-of-the-art
capacitors, the energy density needs to be increased markedly. Improving breakdown electric fields
provides a potential solution, but operations at such high fields relying on unchanged dielectric
permittivity sacrifice the lifetime to some degree. Here, we report a ferrorestorable polarizationengineering capable of enhancing effective permittivity over twice. Our experiments and ab initio
calculations demonstrate that a defect dipole composed of 3d transition metal acceptors such as
Cu3+ and oxygen vacancy in a prototypical ferroelectric BaTiO3 ceramic is coupled withspontaneous polarization1). The resultant ferrorestorable polarization delivers an extraordinarily
large effective relative permittivity beyond 7,000 with a high energy efficiency up to 89 %2). Our
work paves the way to realizing efficient ceramic capacitors for self-powered applications.

Fig. 1 | Ferrorestorable polarization2). a, Typical P-E loop of ferroelectrics (pristine). b, Shifted
P-E loop with an internal electric field (Ei) caused by the ground-state configuration of def ∥ Ps
(controlled). The controlled sample has a large Urec as a result of ΔP, which is termed
ferrorestorable polarization. The interaction between def and Ps stabilizes the downwards
polarization (Pdown) at zero field, i.e., P0 = Pdown, because the P-E loop shifts to a positive field by
the magnitude of Ei. Ei is defined as the average of Ec+ and Ec−, that is, 𝐸𝑖 = (𝐸c+ + 𝐸c− )/2, where
Ec+ and Ec− are the electric fields at the extreme polarization switching currents in the positive andnegative field sweeps, respectively.
1)
2)

Y. Noguchi, Y. Taniguchi, R. Inoue and M. Miyayama, Nat. Commun. 11, 966 (2020).
DOI: https://doi.org/10.21203/rs.3.rs-1429045/v1

46

E-2:
High performance BaTiO3-based dielectric materials for capacitor applications
Cheng Chen1, Hua Hao1,2*, Xin Lai1, Appiah Millicent1, Zhonghua Yao1,Minghe Cao1, Hanxing Liu1
1

State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, School ofMaterials Science and Engineering, Wuhan University of Technology, Wuhan 430070, China
2

Foshan Xianhu Laboratory of the Advanced Energy Science and Technology Guangdong Laboratory,

Xianhu hydrogen Valley, Foshan 528200, P.R.China*

E-mail: haohua@whut.edu.cn

BaTiO3 (BT) is an important dielectric material, which have extensively been applied in electronicand electrical industries such as multilayer ceramic capacitors (MLCC), random access memory, sensors,
and actuators. The harsh and extreme working environments have put forward strict requirements fortemperature stability of dielectric materials, especially at higher temperatures. Intense efforts have been
devoted to maintaining high dielectric constant over a wide range of temperature. It has been reported
that forming solid solutions and constructing core-shell structures by doping with various additives are
the most effective approaches to enhance dielectric temperature stability of BT based ceramics. As weall know, core-shell structure is a metastable state in thermodynamics, and will evolve to a more stablehomogenous state depending on changes in producing conditions, such as sintering temperature,dwelling time, coating conditions, starting particle size, internal stress and thermal procedure.
In this work, the influence of different oxides, starting particle size and sintering conditions on the
microstructures and dielectric properties of BaTiO3-based ceramics were investigated to reveal the coreshell structure by high resolution transmission electron microscopy techniques with EDS analysis. The
ion diffusion behavior plays a critical role in the formation and evolution of core-shell structure, andtherefore influences the dielectric properties. When using more than 100 nm BaTiO3 as starting powders
and sintering for relatively shorter dwelling times (0.5 h-2.0 h), the chemical heterogeneity core-shellstructure could be formed and retained owing to the limited diffusion behavior. However, when using
80 nm BaTiO3 nanopowders and further extending dwelling times to 6 hours, the diffusion length was
shortened and more driving energy was provided to prompt ion diffusion behavior, which made elements
distribute uniformly and compositional inhomogeneity become homogenized. The double dielectricpeaks in εr-T curves would become a single diffused peak with the collapse of core-shell structure.

47

E-3:

Origin of High-Performance Energy Conversion in AgNbO3 Based Ceramics:
Structure Evidences
Zhigao Hu, * Anyang Cui, Kai Dai, Kai Jiang, and Junhao Chu
Department of Physics, School of Physics and Electronic Science,
East China Normal University, Shanghai 200241, China*Corresponding Author: zghu@ee.ecnu.edu.cn
Lead-free AgNbO3 has attracted great attentions in ferroelectric physics due to its excellent
energy storage and conversion properties. However, to develop lead-free energy conversion devices
and the performance of AgNbO3 based materials, the intrinsic mechanism of the high energy storage
performance is still unclear, due to their complex lattice structure and doping engineering. In thisreport, a refined phase diagram was firstly constructed by studying the condensed-matter
spectroscopies under the changes of chemical dopant, temperature and pressure fields. It is revealed
that structural transformation is closely related to the antipolarity of the cation and the distortion of theoxygen octahedron, where the successive lattice transitions of AgNbO3 are associated withdisplacive-type characterized by soft mode. Simultaneously, the synergistic study of phonon dynamics
and electronic transition behaviors have been illustrated under the doping contents, the external
temperature and stress fields. Furthermore, we confirmed that the main factors determining theexcellent energy conversion performance of AgNbO3 ceramics are including the large remanentpolarization for enhancing the energy storage density, the wide bandgap and small crystalline grain forimproving the intrinsic breakdown strength, as well as the coexistence of polar and non-polar phasefor reducing FE-AFE energy barrier. Our work provides a full strategy to explore the physicalmechanism of the polar-nonpolar structural transition and the intrinsic correlation between the lattice
structure and the functionalities, which would promote the development of lead-free energy storage
ceramic.
References:[1] K. Dai, A.Y. Cui*, Y. Ye, K. Jiang, J.Z. Zhang, Y.W. Li, G.S. Wang, X.L. Dong, Z.G. Hu*, and J.H.
Chu, Phys. Rev. B 104 (17): 174104 (2021).

[2] A.Y. Cui, Y. Ye, K. Dai, Y.W. Li, L.Q. Zhu, K. Jiang, L.Y. Shang, G.S. Xu, Z.G. Hu*, S.J. Zhang
and J.H. Chu, ACS Appl. Mater. Interfaces 14(8): 10535-10545 (2022).
[3] D. Yang, J. Gao, L. Shu, Y.-X. Liu, J.R. Yu, Y.Y. Zhang, X.P. Wang, B.-P. Zhang and J.-F. Li, J.
Mater. Chen. A 8: 23724-23735 (2020).

48

E-4:

Growth of Metal-free Perovskite-type Ferroelectric Crystals
and Their Ferroelectric Properties
S. Ueno1, S. Ando1, T. Moriyama1, T. Unno1, I. Fujii1, S. Kawachi2, J. Yamaura3, S. Wada1*
1

University of Yamanashi, Japan2

3

University of Hyogo, JapanTokyo Institute of Technology, Japan*E-mail: swada@yamanashi.ac.jp

Recently, it was reported that metal-free perovskite-type crystals such as (MDABCO)(NH4)I3
crystals were true ferroelectric crystals with larger spontaneous polarization (Ps) of almost 20 µC/cm2,
very slimier to Ps of BaTiO3 (Ps ~ 26 µC/cm2)1). Until today, various metal-free ferroelectric crystals
were reported by many researchers, but most of crystals showed very low spontaneous polarization
below 5 µC/cm2.

So, we believe that it is very important to confirm Ps value (almost 20 µC/cm2) of(MDABCO)(NH4)I3 crystals. In this study, two oriented (MDABCO)(NH4)I3 crystals along to <111>
and <100> directions were grown by conventional crystal growth method at room temperature. Then,
crystal structure of these crystals was measured.

At the same time, various ferroelectric related

properties were measured. These detailed results will be reported at the conference.
References
1) Heng-Yun Ye et. al., Science, 361, 151-155 (2018).

49

E-5:
Effect of Reaction Accelerator on Single Crystal Barium Titanate Fine Particle Synthesis
Masaki YAMAGUCHI1*, Atsushi SAITOH1, Misa YAMASAKI1, Takashi YAMAMOTO2
1

Shibaura Institute of Technology, Japan
2

Osaka Metropolitan University, Japan*E-mail: yamag@sic.shibaura-it.ac.jp
1. Introduction
Barium titanate (BT), one of the important electro-ceramic materials, is used to multi-layer ceramic
capacitors (MLCCs), electro-optical (EO) devices, sensor devices and so on. In particulars, BT fineparticles are expected to be applied to miniaturization of ceramic capacitors and as ordered
accumulations. Considering that the space is filled with only one type of solid, its shape is limited to
cubic, rhombic dodecahedrons, and so on. The case of liquid phase crystal growth, the particle shape
can be controlled by adsorbing the additive on specific surface of the crystal. Therefore, in this study,
we describe the results of examining the effect of synthetic conditions on the shape of BT fine particles.
2. Experimental Procedure
BT fine particles were fabricated by hydrothermal synthesis method, in this study. The precursor
solution is mixture of barium hydroxide, titanium lactic acid complex, sodium hydroxide, activator andsurfactant. The Ba/Ti ratios was controlled exactly1.0. During the heating of solution, it was mechanicalstirring. After the synthesis, the samples were washed and classification. Particle synthesis and particle
shape evaluation were performed as in previous reports.1
3. Results and Discussions
In this study, tert-butylamine (tBA) and tert-amylamine (tAA) was used as a reaction accelerator. We
can see from the figures, microparticles grow independently of the type of reaction accelerator. In
addition, although not shown here, it was confirmed from the results of XRD observation that the fineparticles synthesized by tBA were perovskite-type BT, and high-resolution image analysis indicates thatthe microparticles are single crystals surrounded by {100} planes and belong to the tetragonal systemwith a lattice constant of approximately 0.4 nm. The oxygen octahedral structure, which is the basic
skeleton of the perovskite structure, is formed by dissociating lactic acid from the titanium complex.
Considering the molecular structure and Pauling's electronegativity, tBA, which is smaller and has
higher electrical symmetry, is expected to have a greater reaction-promoting effect. In fact, the synthetic
particle size of tBA is larger than that of tAA. Therefore, we think that tBA is suitable as a reaction
accelerator. However, there is a problem that the particle shape is not uniform.
Acknowledgements
This work was supported in part by International ResearchCenter for Green Electronics (IRCGE), Shibaura Institute ofTechnology (SIT). The authors would like to thank Prof. H. Seki
and Mr. M. Kaneko for their cooperation in sample evaluation.
References
1. M. Yamaguchi et al., CJfma-13, I-49 (2021), M. Yamasaki et al.,
IEICE Trans. on Electron., 104 (2022). [in Japanese]

Fig. Shape changes of synthesis BT fine particles by areaction accelerator.

50

E-6:
Ferroelectric and piezoelectric properties in simple binary compounds
Wei Ren1
1

Physics Department, International Centre of Quantum and Molecular Structures, Shanghai University,
99 Shangda Road, Shanghai 200444, China*E-mail: renwei@shu.edu.cn
First-principles calculations are performed to investigate ferroelectricity in some binary compounds,

including bilayer two-dimensional (2D) hexagonal boron nitride (h-BN) and rocksalt oxide family (AO
with A=Cd, Ba, Sr, Ca, Mg, etc.) via the application of biaxial strain. The origins of such unconventional
ferroelectricity are discussed from the lattice perspective and electronic structure properties. Thesefindings have the potential to motivate the study of simple materials possessing ferroelectricity andpiezoelectricity that may lead to novel devices.
Anomalous ferroelectricity and double-negative effects in bilayer hexagonal boron nitride.
Wen Jiang, et al., and Wei Ren, Physical Review B, 106, 054104 (2022)
Strain-induced ferroelectricity and piezoelectricity in centrosymmetric binary oxides.
X. Yang, et al., and W. Ren, Physical Review B, 106, 064106 (2022)
Volume-matched ferroelectric and piezoelectric ZnO/MgO superlattice.
X. Yang, et al., and W. Ren, Journal of Alloys and Compounds, 876, 160167 (2021)
Huge Piezoelectric Response of LaN-based Superlattices.
Minglang Hu, et al., and W. Ren, ACS Appl. Mater. Interfaces 12, 49805 (2020)

51

E-7:

Angle-resolved polarized Raman mapping on a compositionally gradedPb(Mg1/3Nb2/3)O3-PbTiO3
S. Tsukada1, 2*, Y. Fujii3, A. Kanagawa2, Y. Akishige1, and K. Ohwada4
1

Faculty of Education, Shimane University, Japan

2

Graduate School of Natural Science and Technology, Shimane University, Japan3

Department of Physical Sciences, College of Science and Engineering, Ritsumeikan University, Japan
4

National Institutes for Quantum and Radiological Science and Technology (in SPring-8), Japan*E-mail: tsukada@edu.shimane-u.ac.jp

Explaining the “properties and functions of materials” in terms of “atomic arrangement and various
inhomogeneous structures” is a fundamental challenge for developing ferroelectric oxides. Dielectricity,
one of the most fundamental properties of matter, can be explained by long-wavelength polar lattice
vibrations and dipole relaxations, accompanied by the bias of electricity. Therefore spectroscopic
methods such as Raman spectroscopy are used to investigate the origin of the property. Using a recently
advanced angle-resolved polarized Raman mapping, we investigate the correlation between the phaseboundary and the giant dielectric responses in relaxor Pb(Mg1/3Nb2/3)O3 and ferroelectric PbTiO3 solid
solution (PMN-xPT) system using a compositionally graded crystal [1].
Angle-resolved polarization Raman mapping, X- mapping, which was developed by incorporating
information of polarization of light  into Raman mapping, was performed [2]. A schematic diagram ofthe experiment is shown in FIG. 1(a), and the X-contour map on the peak at 750 cm-1 is shown in FIG.
1(b). Gradual changes in polarization direction are visualized by Raman mapping the crystal. And byanalyzing quasi-elastic scattering from dipole relaxation, the origin of the enormous dielectric response
found in PMN-xPT can be understood as follows: The mesoscopic ferroelectric domains, which arecomposed of polar nano regions, become smaller and slowly fluctuate near the phase boundary, resulting
in an enormous dielectric response, which is the characteristic of relaxor-ferroelectric solid solution
system and the difference from other ferroelectrics.

FIG. 1 (a) Schematics of sample setting in Raman microscope with the relationship between
structure and polarization direction. MB, MC, and T denote monoclinic (type B), monoclinic (typeC), and tetragonal crystal structures, respectively. (b) An X- Raman mapping image colored by
the area around 750 cm-1 of the spectra measured under the conditions Y~ 7 mm.
[1] D. Shimizu, et al., Phys. Rev. B 92, 174121 (2015).

[2] S. Tsukada, et al., Phys. Rev. B 97, 024116 (2018).

52

F-1:
Flexible Lead-free Piezoelectric Arrays for High-Efficiency Wireless Ultrasonic Energy
Transfer and Communication
Laiming Jiang*, Jiagang Wu, Jianguo Zhu
Country College of Materials Science and Engineering, Sichuan University, Chengdu 610064, China*E-mail: laimingjiang@scu.edu.cn
Implantable medical electronics (IMEs) are now becoming increasingly prevalent for diagnostic
and therapeutic purposes. Despite extensive efforts, a primary challenge for IMEs is reliable wirelesspower and communication to provide well-controlled, therapeutically relevant effects. Ultrasonic energy
transfer and communication (UETC) employing traveling ultrasound waves to transmit energy has
emerged as a promising wireless strategy for IMEs. Nevertheless, conventional UETC systems are rigid,
bulky, and based on toxic lead-based piezoelectric materials, raising efficiency and safety concerns.
Here, we present a novel transcutaneous UETC system based on a two-dimensional flexible lead-freepiezoelectric array (f-LFPA) that hybridizes high-performance (piezoelectric coefficient d33 ≈503 pCN-1) (K,Na)NbO3-based eco-friendly piezo-units with soft structural components. The newly developed
lead-free piezo-unit exhibits submicron ferroelectric domains and superior energy harvesting figures ofmerit (d33g33 ≈20000 × 10-15 m2 N-1), resulting in the prepared f-LFPA demonstrating a high output
voltage of 22.4 V, a power density of

0.145 W cm-2, and a signal-to-noise ratio of more than 30 dB

within the FDA safety limits, while maintaining the flexibility for wide-angle receiving. Further ex vivo
experiment demonstrates the adequate power supply capabilities of the f-LFPA and its possible
application in future implantable eco-friendly bioelectronics for diagnostics, therapy, and real-timemonitoring.

Fig. 1 Schematics and design of the flexible lead-free ultrasonic device.

53

F-2:

RTIC phenomenon on AD process and its
application to dielectric / ferroelectric thick films
Jun AKEDO
National Institute of Advanced Industrial Science & Technology (AIST),
Email : akedo-j@aist.go.jp
Aerosol Deposition (AD) method[1]-[4] is a unique approach for metal and ceramic coating, where
solid state submicron metal and ceramics particles are accelerated by gas flow up to 100 - 500 m/s andthen impacted onto a substrate. AIST found interesting consolidation phenomenon of ceramic particles
in this method over 20 years ago. During collision of fine particles and interaction with substrate, theseceramic particles, not only for oxide materials but also for non-oxide materials, formed thick, denseand hard ceramic layers at room temperature. No additional heating for solidification of ceramic
powder was required. We named this phenomenon “Room Temperature Impact Consolidation(R.T.I.C)” [2],[4]. Consolidated ceramic powder with R.T.I.C. via AD method can be called as a highdensity binder less ceramic green. It can form rapidly a thick dense, and uniform ceramic layer at room
temperature without additional heating for solidifying starting powders, even in low vacuums, using
relatively cheap and simple production facilities. Metal-based optical scanning devices, tube-typeultrasonic motors, piezoelectric energy harvesters and energy storage using dielectric / ferroelectric
AD thick films have been developed for sensor & actuator and energy device applications.[3]Figure 1：The configuration of AD machine and the deposition example of AD method (PZT thickfilm on glass and Si wafer)(Reference)[1] J. Akedo and M. Lebedev, Jpn. J. Appl. Phys., vol.38-9B, pp.5297-5401 (1999)[2] J. Akedo, J. Am. Ceram. Soc., 89, 1834-1839 (2006).
[3] J. Akedo, J-H. Park1, and Y. Kawakami, Jpn. J. Appl. Phys., vol.57, 07LA02 (2018).
[4] J. Akedo, J. Ceram. Soc. Jpn., 128 (3), 101-116 (2020).

54

F-3:

Ferroelectric gate thin films transistors with Y-doped Hf-Zr-O gate insulator
and In-Sn-O channel
E Tokumitsu1*, Y Kubota1, Mohit1, K Sasaki1
1

Japan Advanced Institute of Science and Technology, Japan*E-mail: e-toku@jaist.ac.jp

HfO2-based ferroelectric materials, whose ferroelectricity was reported in 2011[1], have attracted
much attention as candidates for future electronics applications, such as nonvolatile memories and steepslope MOSFETs. One of the most promising applications is a ferroelectric-gate field effect transistor,
called FeFET or FGT. In this device, a ferroelectric material is used as a gate insulator, which results inhysteresis characteristics in the transfer curve. In addition, because of the spontaneous polarization, theferroelectric gate insulator can induce large charge density so that conductive oxide such as indium-tinoxide (ITO) can be used as a channel of the FGT [2]. One of the advantages of ITO channel FGT is its
low “on”-resistance and low resistivity of local metallization, especially when it is used in NAND strings.
ITO channel FGT is also applicable for 3D NAND structures.
In this talk, we report ferroelectric properties of Y-doped Hf-Zr-O (Y-HZO) thin films preparedby chemical solution deposition (CSD). Figure 1 shows polarization – electric filed (P-E) hysteresis
loops of Y-HZO films prepared by CSD with an Y concentration of 3.2 % [3]. The film was annealed
at 800 oC for 3 min at a reduced pressure of 50 Pa. Clear ferroelectric properties were observed with aremanent polarization, Pr, of approximately 12 μC/cm2. The Pr values estimated from P-E measurements
are plotted in Fig.2 as a function of Y concentration and it was found that the maximum Pr was obtained
when the Y concentration is around 3 %. Next, we apply the CSD ferroelectric Y-HZO film to FGT. To
fabricated FGTs, ITO layer with a Sn concentration of 5% is fabricated by CSD on the Y-HZO gateinsulator. Figure 3 shows transfer curve obtained for ITO/Y-HZO structure FGT. A clear hysteresis witha memory window of as large as 10 V was observed. The details will be presented at the conference.

Fig.1 P-E loops of Y-HZO films
Prepared by CSD

Fig.2 Remanent polarization as afunction of Y concentration

Fig.3 Transfer curve of ITO/YHZO FGT.

References[1] T. S. Böscke, J. Müller, D. Bräuhaus, U. Shröder, and U. Böttger, Appl. Phys. Lett., 99, 102903 (2011).
[2] T. Miyasako, M. Senoo and E. Tokumitsu, Appl. Phys. Lett., 86, 162902 (2005).
[3] K. Sasaki, Mohit, S. Hashiguchi, and E. Tokumitsu, Jpn. J. Appl. Phys., 61, SN1027 (2022).

55

F-4:
Fabrication and characterization of La-doped HfO2 ferroelectric films on SrTiO3 single
crystal substrates.
Rao Badari Narayana1* HirokoYokota2
1

Center for frontier sciences, Chiba University, Japan2

Department of Physics, Chiba University, Japan*E-mail: rao.badari@chiba-u.jp

Several doped-hafnium oxide films have recently been discovered to have ferroelectric properties.
These films are peculiar because unlike conventional ferroelectric materials, their ferroelectricity does
not diminish with decreasing film-thickness. In the present work, La-doped hafnia films were depositedby pulsed laser deposition on La2/3Sr1/3MnO3 buffered SrTiO3 (100) substrates. The crystal structure andferroelectric properties were studied with varying deposition and annealing conditions. Films deposited
at high-temperature showed good crystallinity but also exhibited more leakage current. On the other
hand, films deposited at room-temperature which were later annealed in a nitrogen atmosphere showed
low leakage current, but had poorer crystallinity. Various aspects of optimization of the fabrication
process, and the parameters critical for enhanced ferroelectric properties are discussed.

56

F-5:
Energy-storage performance of antiferroelectric Pb(Zr,Hf)O3 films fabricated by sol-gel
spin coating
J. Song1, S. Kada1, Y. Iwamoto1, T. Iijima1,2, and S. Okamura1∗
1

Tokyo University of Science, Japan

2

National Institute of Advanced Industrial Science and Technology, Japan*E-mail: s_okamura@rs.tus.ac.jp

Antiferroelectric (AFE) materials, such as PbZrO3 (PZ) and AgNbO3, are competitive candidates
for the energy-storage application, owing to their large saturated polarization and small remanentpolarization[1]. PbHfO3 (PH), with a similar crystal structure of PZO, has also attracted great attention
in recent years and comparable recoverable energy (Wre) with PZO has been reported[2-3]. However,investigation on the microstructure and energy-storage performance of Pb(Zr1−xHfx)O3 (PZH) is quite
limited. In this study, PZ, PH and PZH films with the Zr/Hf ratio of 90/10, 80/20 and 50/50 were
fabricated on Si substrates using the sol-gel spin coating method. The P–E hysteresis loops showed that
all the samples exhibited similar remanent polarization and low leakage current. The maximum
polarization increased with Zr content, indicating the enhancement of Wre in Zr-rich films. The energy
efficiency was more affected by the existence of Hf than the amount of Hf. As a result, the PZH (90/10)
film with the highest Wre of 11.3 J/cm and a larger energy efficiency of 55%, measured at 800 kV/cm,
was obtained in this study. This suggests that the Hf-doped PZ film is promising for the energy-storage
application.

Fig. 1 (a) The P–E hysteresis loop of PZH (90/10), measured at 10kHz. (b) Recoverable energy
density (Wre) and (c) energy efficiency of the fabricated films, changed with the applied electric field.
References[1] X. Hao, J. Adv. Dielectr. 3, 1330001 (2013).
[2] J. Wei, T. Yang, and H. Wang, J. Eur. Ceram. Soc. 39, 624 (2019).
[3] X. Huang, T. Zhang, W. Wang, P. Ge, and X. Tang, Mater. Des. 204, 109666 (2021).

57

F-6:
Low temperature deposition of BiFeO3 films on base metal foils for piezoelectric
applications

Jing Yan1, Jun Ouyang2*, Isaku Kanno3*，
1

College of Physics and Electronic Engineering, Qilu Normal University, Jinan, Shandong 250013,

China.
2

Institute of Advanced Energy Materials and Chemistry, Jinan Engineering Laboratory for Multi-scale

Functional Materials, School of Chemistry and Chemical Engineering, Qilu University of Technology(Shandong Academy of Sciences), Jinan 250353, China.
3

Mechanical Engineering, Kobe University, Kobe 657-8501, Japan.

*: Corresponding authors: ouyangjun@qlu.edu.cn, kanno@mech.kobe-u.ac.jp

Piezoelectric BiFeO3 (BFO) films were successfully prepared on 304 stainless steel (SS) and Ti
foils via RF-magnetron sputtering at 450 °C. By adopting a LaNiO3/Pt/Ti tri-layer bottom electrode, apredominant (100)-orientation and a dense fine-grained morphology were achieved in these BFO films,
resulting in good ferroelectric and dielectric properties targeted for piezoelectric applications. These
properties include a large remnant polarization (Pr~68C/cm2 for BFO-SS, Pr ~72 μC/cm2 for BFO-Ti),a sizable self-bias (Ebi~ 158 kV/cm for BFO-SS, Ebi~ 145 kV/cm for BFO-Ti), and very decent dielectric
properties (r  270, tan 0.026 in 1 kHz-1MHz). Large transverse piezoelectric coefficients of |e31,f| ~2.2± 0.2 C/m2 and |e31,f| ~ 1.7 ± 0.1 C/m2 were achieved in patterned BFO-Ti and BFO-SS cantilevers,
respectively. A decent direct transverse piezoelectric coefficient (~1.07 ± 0.03 C/m2) was also achieved
in BFO-SS based prototype piezoelectric energy harvesters. These results suggest that BiFeO3 films havea great potential for applications in lead-free, metal-based piezoelectric micro-electro-mechanicalsystems (Piezo-MEMS).

58

F-7:
Extraordinarily large domain switching contribution in epitaxial (K, Na)NbO3
films
Xueyou Yuan1, Kazuki Okamoto1, Mitsuki Kawano1, Masahito Yoshino1, Takanori Nagasaki1,
Yasuhiko Imai2, Osami Sakata2,3, Tomoaki Yamada1
1

Nagoya Univ, Japan
2

JASRI, Japan

3

NIMS, Japan*E-mail: t-yamada@energy.nagoya-u.ac.jp(K, Na)NbO3 (KNN) as a promising alternative to the-state-of-art PZT has drawn enormous
attention due to high curie temperature and excellent piezoelectric response.[1] The piezoelectric
response is derived from intrinsic the lattice deformation and extrinsic domain wall motion and domain
volume variation. Despite significant efforts on the piezoelectric response in KNN films, the ratio of
intrinsic and extrinsic contributions remains elusive. Yet, in-situ time-resolved synchrotron X-ray
diffraction can offer assistance to clarify the origin of large piezo-response.[2, 3] Here, we successfully
grew the KNN films in monoclinic phase, of which sole (001) domain in KNN (001)pc films, but (1̅11)
and (111) domains in KNN (111)pc films. Notably, KNN (111)pc films manifest the fast and reversible
domain switching, whose contribution to the piezoelectric response surpasses 100% under the moderatebias..
The piezo-response is intimately relevant to the orientation of the domains. Fig. 1 exhibits the fieldinduced strain for KNN (111)pc films. The intrinsic and extrinsic piezoelectric responses are highly
relying on the applied field; the moderate bias enhances the extrinsic response via domain switching,whereas the intrinsic response emerges only over it. The extrinsic contribution to d33,f exceeds 100%due to the slightly negative intrinsic response under it. Fig. 2 shows the time evolution for the (111)pc
KNN film under electric field of 36 kV/cm. The domain switching in the (111)pc film is fully reversible.
The domain switching is saturated during the interval of the voltage pulse of 50 s. Both time of inducing
the domain switching and relax back to the original state after releasing the bias was around 30 s.

Fig. 1 Field-induced strain for KNN (111)pc films. Fig. 2 Time evolution of domain switching for
KNN (111)pc film under 36 kV/cm.
Reference: [1] Y. Saito et al., Nature 432, 84−87 (2004). [2] Y. Liu et al., Scr. Mater. 207, 114283(2022). [3] J. L. Jones et al., J. Appl. Phys. 97, 034113 (2005).

59

F-8:

Intrinsic properties of domain walls of BiFeO3
Lisha Liu1, Jing-Feng Li2, and Yaojin Wang3

School of Materials Science and Engineering, Nanjing University of Science and Technology,
Nanjing 210094, Jiangsu, China
2
School of Materials Science and Engineering, Tsinghua University, Beijing 100081, China.

1E-mail address: lishaliu@njust.edu.cn
Embedded in the bulk of an insulating material, ferroelectric domain walls have the capability of
being (re)created, displaced, erased, and altered in their spatial configurations and electronic
characteristics. In recent years, domain walls themselves have attracted extensive attention, due to richintriguing physics and novel ideas of designing nanoelectronics based on these interfaces. Intrinsic
properties of domain walls, e.g., domain wall conductivity, domain wall type, and domain wall width,
are thus particularly important in understanding characteristics of ferroelectrics involving domain
walls. In recent years, we obtained domain wall conductivity (> 10 µA) more than one order ofmagnitude higher than previously reported maximum value (~ 0.6 µA). However, reliable routine todesign a giant conductivity for random domain walls is lacking. Such discussion is in great demands.
Moreover, these free-carrier compensated non-180° CDW may show a thickness as thin as ~2 unit
cells, with a Néel-like character, unlike prior beliefs.
Domain walls are interesting themselves, containing rich physics and are related to many new
phenomena, as well are critical tangling with their macroscopic performances. Interacting with theinsulating bulk within the piezoelectric materials, conductive domain walls would induce peculiar bulk
property response of these materials, for example decoupling of lattice strain and domain wall motion
induced strain in both the frequency and field amplitude domains. These are surprising and unexpectedwith fundamental implications for a broad range of materials as well as for device design. The intrinsic
properties of domain walls worth more thorough investigations.

60

P-01:
Phase Transformation, Interfacial Coupling and Giant Charge-discharge Efficiency of
BaTiO3@PVP/PVDF Nanocomposite Films
Yao Su, Wenyi Li, Yan Wang, Peimei Yuan, Zhao Bo, Dengwei Hu*
Baoji University of Arts and Sciences, 1 Hi-Tech Avenue, Baoji, Shaanxi, 721013 P.R. China(* Corresponding author, E-mail address: dwhu@bjwlxy.edu.cn)
Abstract: The introduction of BaTiO3 (BT) nanoparticle modified on the surface of
Polyvinylpyrrolidone (PVP) into semi-crystalline polyvinylidene fluoride (PVDF) matrix caneffectively enhance the interfacial coupling, charge-discharge efficiency and energy storage
performance of inorganic-organic nanocomposite films. In this study, compared with the BT/PVDF
composite films, the interfacial coupling ability of BT@PVP/PVDF has been greatly improved, which
is attributed to the bridge effect of PVP. Besides, when the BT@PVP is filled with 5 vol%, the energy
density, the breakdown field strength, and the efficiency are respectively increased by 257.8% (18.39
J/cm3 vs 5.14 J/cm3), and 51.5% (458.3 MV/m vs 302.5 MV/m) and 47.56% (79.8% vs 54.08) comparedwith BT/PVDF composite films. Outstandingly, the remarkable charge-discharge efficiency is the higher
value than reported so for. Furthermore, the enhancements of these performance are importantly related
not only to the interfacial coupling of inorganic-organic nanocomposite films, but also to the increaseof the α+γ phases (the α+γ phases content of 5 vol.% BT@PVP/PVDF increased by 7.82% comparedwith BT/PVDF composite films). This work demonstrates a possible mechanism for the improvementsof the PVDF-based surface-modified inorganic ceramic nanocomposites’ energy storage performance.
Keywords: interface couple, inorganic-organic, BT@PVP/PVDF composite film

Fig. 1 (a) The Fourier transform infrared spectra of pure PVDF films, 5 vol.% BT/PVDF and 5 vol.%BT@PVP/PVDF nanocomposite films. (b) Phase content analysis of BT@PVP/PVDF composite films for
α+γ phases and β phase. (c) α+γ phases increasing of and (d) β phase decreasing of BT@PVP/PVDF
nanocomposite films comparing with pure PVDF films and BT/PVDF nanocomposite films. (e) Energy
density and (f) Discharge-charge efficiency of BT/PVDF and BT@PVP/PVDF composite films.
Referencesa) Tang H, Zhou Z, Sodano H A, et al. 2014, 6, 5450. b) Huang X, Sun B, Zhu Y, et al. 2019, 100, 187. c) Li H,

Liu F, Fan B, et al. 2018, 2. d) Li L, Cheng J, Cheng Y, et al. 2021, 33, e2102392.

61

P-02:
Crystal structure and microwave dielectric properties of
Ba4(Sm1-xCex)9.33Ti18O54 solid solutions
Yu Xie1,2, Kongjun Zhu1,*, Kang Yan1, Jing Wang1, Jinsong Liu2
1
State Key Laboratory of Mechanics and Control of Mechanical Structures, Nanjing University of
Aeronautics and Astronautics, Nanjing 210016, China.
2
College of Materials Science and Technology, Nanjing University of Aeronautics and Astronautics,
Nanjing 210016, China.
E-mail address: kjzhu@nuaa.edu.cn
The rapid development of the fifth generation (5G) wireless communication technology has madegreater performance demands for microwave components such as dielectric resonator and dielectricfilter. Microwave dielectric ceramics, as the core materials of microwave devices, have been a research
hotspot. In order to meet the requirements of microwave devices, superior performance of microwave
dielectric ceramics must require, have medium/high relative dielectric constants (εr) to realize theintegration and miniaturization of microwave devices, have high quality factor (Q×f ) to enhance thefrequency selection characteristics of the device, have near-zero temperature coefficient of resonancefrequency (τf ) to obtain high temperature stability. The Ba4Sm9.33Ti18O54 ceramic system belongs to thetungsten bronze structure, which is composed of titanium-oxygen octahedra interconnected by meansof shared vertices, forming three kinds of voids in space: the quadrilateral position A1 occupied by Sm3+,
the pentagonal position A2 occupied by Ba2+ with a slightly larger ionic radius, and the triangular void
not occupied by ions. The uniformly ordered arrangement of Sm3+ and Ba2+ in the voids A1 and A2
arrangement reduces the internal stresses making the Q×f value maximum. In order to further improve
the Q×f value, many doping modification studies were carried out.
In this work, Ba4(Sm1-xCex)9.33Ti18O54 (x = 0.000, 0.125, 0.250, 0.375, 0.500) microwave dielectric
ceramics were prepared by the conventional solid-phase method. The effects of Ce3+ substitution for Asite Sm3+ on the microscopic morphology, crystal structure and microwave dielectric properties of theceramics were investigated. A single tungsten-bronze phase was obtained for all the studied components.
With the increase of Ce3+ substitution, the cell volume gradually increases, the internal stress inside thecrystal decreases, the stability of the crystal structure increases, the value of quality factor Q×f
increases, the relative permittivity εr increases, and the temperature coefficient τf of resonant frequency
shifts toward positive values. At x = 0.250, Ba4(Sm1-xCex)9.33Ti18O54 ceramics exhibit excellent
microwave dielectric properties when sintered at 1325 °C for 4 h: εr = 81.04 (4.914957 GHz), Q×f =9013 GHz, and τf = -0.61 ppm/°C.

Reference
1. Hill, D.H. et al., Applied Physics Letters 118 (12) (2021).
2. Wang, G. et al., Ceramics International 45 (17) 22148-22155 (2019).
3. Xiong, Z. et al., Journal of Alloys and Compounds 723 580-588 (2017).
4. Yang, H.C. et al., Journal of Advanced Ceramics 10 (5) 885-932 (2021).

62

P-03:

Ultrahigh energy harvesting properties in temperature insensitive eco-friendly highperformance KNN-based textured ceramics
Jinfeng Lin1, Jiwei Zhai1*
1
Key Laboratory of Advanced Civil Engineering Materials of Ministry of Education, Functional
Materials Research Laboratory, School of Materials Science and Engineering, Tongji University,
Shanghai, 201804, China*E-mail: apzhai@tongji.edu.cn
High-performance potassium sodium niobate (KNN) based texture ceramics and its potential
application on energy harvesting device are the first time to be presented in this work. A series oflead-free 0.99K0.5Na0.5Nb(1-x)TaxO3-0.01Bi(Ni2/3Nb1/3)O3 [KNNTa-BNN] piezoceramics are designed
and prepared to search for good comprehensive properties. The comprehensive performance of
KNN-based piezoelectric ceramics have reached a new level in T-Ta-9 (d33 ~435 pC/N, kp ~71%, Tc~360℃) via the synergy of textured structure (f(00l) > 94%) and multiphase coexistence (O-T) nearroom temperature. Based on the advanced in-situ TEM and PFM analysis, it is found that the regularlarge-scale domains and corresponding poling patterns of the T-Ta-9 can be well maintained atrelatively high temperatures (180-330℃), resulting in excellent temperature stability. Hence, the d33
value of T-Ta-9 can be maintained above 300 pC/N over a wide range from room temperature to
300°C, which rarely happens in the previously reported KNN-based materials. More importantly, thepiezoelectric circular diaphragm (PCD) vibration energy harvester based on the T-Ta-9 texture
ceramic possesses high output voltage (~13 V) and output power (~3 mW), and can still maintainabove 60% after heated at 200℃ for 30 min. This work represents a significant advancement inlead-free piezoelectric energy-harvesting field (especially for high temperature applications) and canprovide guidelines for future efforts in this direction.

63

P-04:
Characteristics of Chemical Bonding and Thermal Behavior of Atoms inPrototype Structure of Double Perovskite-type Antiferroelectric Oxides
Takayasu Shigemasu,1* Sangwook Kim,1 Chikako Moriyoshi,1 Guorong Li,2 Chul-Hong Park,3 andYoshihiro Kuroiwa1
1Graduate School of Advanced Science and Engineering, Hiroshima University, Hiroshima 739-8511,
Japan
2
Chinese Academy of Sciences, Shanghai Institute of Ceramics, PRChina 200050, China
3
Department of Physics Education, Pusan National University, Busan 46241, Korea*Corresponding author, e-mail: t-shigemasu@hiroshima-u.ac.jp
The solid solution Pb(Yb1/2Nb1/2)O3 (PYN) is a double perovskite-type oxide with an ordered arrangementof Yb and Nb atoms at the B-site. PYN undergoes the antiferroelectric phase transition at 575K, and exhibits
an orthorhombic structure with the space group of Pbnm at room temperature. The phase transition should
not be discussed only by the tolerance factor t (t = 0.957 < 1), but the intrinsic origin should be discussed
from the lattice instability in the prototype structure.
In this study, we have revealed the structural characteristics on the lattice instability in the paraelectricphase of PYN, which causes the antiferroelectric phase transition, by visualizing the electron charge density
distribution from the synchrotron radiation X-ray powder diffraction (SXRD) data. The Pb atom was offcentered at 12 equivalent sites at random in the <110> directions in the paraelectric phase, while the Pb atom
was ordered at one of the off-centered sites in the antiferroelectric phase as shown in Fig 1. The electron
charge density analysis of the paraelectric phase revealed the hybridization of atomic orbitals between the
Nb and surrounding O atoms, while the Yb atom was fairly ionic. The thermal motion of the O atom wassignificantly anisotropic. The electron charge density distributions around the O atoms were extended toward
the directions perpendicular to the Yb-O bond. We consider that the lattice instability to the antiferroelectricphase is due to the ionic Yb ion, which causes the tilting of the oxygen octahedra at the phase transition. The
ordered direction of the off-centered Pb atom should be associated with the direction of the local polarizationin the antiferroelectric phase.
The detail of crystal structures and the origin of the antiferroelectric phase transition will be discussed inpresentation.
(a)Fig. 1 Crystal structures of PYN obtained by the Rietveld analysis;(a) paraelectric phase at 673 K, and (b) antiferroelectric phase at room temperature.

64P-05:
Tunable vertical ferroelectricity and domain walls by interlayer sliding in -ZrI2
Xiaonan Ma1, Chang Liu2, Sergey A. Nikolaev2*, Wei Ren1*
1
1Physics Department, State Key Laboratory of Advanced Special Steel, and International Centerof Quantum and Molecular Structures, Shanghai University, China
2
Tokyo Tech World Research Hub Initiative (WRHI), Institute of Innovative Research, Tokyo
Institute of Technology, Japan*E-mail: nikolaev.s.aa@m.titech.ac.jp and renwei@shu.edu.cn
Layered transition-metal dichalcogenides have gained enormous attention because of theirferroelectric properties caused by in-plane ionic displacements. In this study, we predict robust vertical
ferroelectricity upon interlayer sliding in beta-ZrI2, a sister material of polar semimetals MoTe2 and
WTe2. Based on extensive first-principles calculations, we elaborate the microscopic origin of electric
polarization in ZrI2 and investigate the variety of ferroelectric domain boundaries, that alongside withthe semiconducting behavior and a small switching barrier can hold promise for novel ferroelectric
applications.

65

P-06:
Crystal Structure of KNbO3/BaTiO3 Core-Shell Nanocomposite Particles Studied
by Synchrotron Radiation X-ray Diffraction
Shao Mingyang ,1, * Kaede Furuta,1 Sangwook Kim,1 Ichiro Fujii,2 Shintaro Ueno,2Satoshi Wada,2 and Yoshihiro Kuroiwa1
1 Graduate School of Advanced Science and Engineering, Hiroshima University, Hiroshima, Japan
2 Graduate Faculty of Interdisciplinary Research, University of Yamanashi, Kofu, Japan*E-mail: shaomingyang@hiroshima-u.ac.jp
Considering environmental issues, the development of high-performance lead-free ferroelectrics toreplace lead-based ferroelectrics is an urgent issue. Lead-free ferroelectric with an artificial superlattice
have a remarkable effect on improving the dielectric properties of lead-free. For example,
heteroepitaxial thin films exhibit excellent dielectric properties. A lattice-strain-layer appears at theinterface due to the lattice mismatch, which enhances the polarization. Our group has attempted toform a lattice-strain-layer in a nanocomposite ceramic particle with a core-shell structure. We haverevealed that the lattice-strain-layer governs the dielectric property of the nanocomposite particle.
In this study, we demonstrated the temperature variation of the crystal structure of lattice-strain-layer
in the KNbO3(KN)/BaTiO3(BT) nanocomposite particles. The nanoparticles were prepared by thesolvothermal method. The core of the particle is BT with a diameter of 300 nm, and the shell is KN
heteroepitaxially covering the BT core. The synchrotron radiation X-ray powder diffraction revealed
the crystal structure of the nanoparticle. The Rietveld method was used for the structural refinement.
However, the powder pattern of the KN/BT nanoparticles at 800 K could not be refined with a
combination of single structural components with a cubic structure of KN and BT, respectively. Two
cubic components models with different lattice parameters for KN and BT respectively gave the best
fitting result in the Rietveld refinement. The schematic diagram of the one KN/BT nanoparticle is shownin Fig. 1, where the four components in all are arranged. It can be confirmed that the lattice-strainlayer exists at the interface in the combination of cubic KN and cubic BT. The crystal symmetry of KN
at 600 K is tetragonal, while BT is cubic. In the case the crystal system is different, the lattice-strain-layer
at 600 K is revealed to exist in a wider area near the interface.

Fig. 1 Schematic of heteroepitaxial KN/BT nanocomposite particle with core-shell structure.

66

P-07:

Brillouin Scattering Study of Ferroelastic Phase Transition of Lead
Phosphate Single Crystal
Adil Emin1,2,*, Anwar Hushur2, and Seiji Kojima3
1

School of Physical Science and Technology, Lanzhou University, Lanzhou 730000, China
2

School of Physics Science and Technology, Xinjiang University, Urumqi 830046, China

Division of Materials Science, University of Tsukuba, Tsukuba, Ibaraki 305-8573, Japan3*E-mail: corresponding author adl19@lzu.edu.cn
Graphical abstract

Abstract
Brillouin scattering spectroscopy plays a vital role in the study of various kinds of phase transitions
and critical phenomena in condensed matters. For structural phase transitions in crystalline solids,
Brillouin scattering experiments provide detailed information on elastic and gigahertz dynamical
properties. We have used the Brillouin scattering technique to investigate the pure ferroelastic phasetransition of a lead phosphate Pb3(PO4)2 crystal at high temperatures. The ferroelastic domain
configuration confirms previous identifications of the symmetry elements lost at the transition. The
temperature dependence of acoustic mode frequency indicates that these lead phosphate Pb3(PO4)2
undergoes a first-order ferroelastic phase transition at TC = 182 oC from the paraelastic hightemperature (HT) trigonal (rhombohedral) phase (the space group R 3 m-�53� ) to the ferroelastic lowtemperature (LT) monoclinic phase (the space group C2/c-�62ℎ ) caused by L-point instability in thetrigonal phase, which doubles the volume of the unit cell. Neither soft acoustic mode and central peak
was observed in the vicinity of TC. The results show that the staggered ferroelactic phase transition isorder-disorder type.
Keywords: Pb3(PO4)2, ferroelastic phase transition, Brillouin scattering, elastic anomaly, hightemperature.

67

P-08:
Structural evolution and electrical properties of BFO-BT based high temperature leadfree piezoelectric ceramics
X. Ai1,2, J. Yang1,2, K. Yan1,*, K. Zhu1
1

State Key Laboratory of Mechanics and Control of Mechanical Structures, College of Aerospace
Engineering, Nanjing University of Aeronautics and Astronautics, Nanjing 210016, China.

2

College of Materials Science and Technology, Nanjing University of Aeronautics and Astronautics,
Nanjing 210016, China.
*E-mail: yankang@nuaa.edu.cn

Bismuth ferrite-barium titanate (BiFeO3-BaTiO3, BFO-BT)-based piezoelectric ceramic is one of
the most important lead-free ferroelectric material systems, because it has high Curie temperature, goodtemperature stability and low cost of raw materials. On the other hand, the relative small piezoelectricity
limits the practical application of the BFO-BT based ceramics. The morphotropic phase boundary(MPB), a ferroelectric phase transition boundary, is considered as the origin of high piezoelectricity of
the Pb(Zr,Ti)O3 (PZT) piezoelectric materials. Based on the MPB effects in the classical PZT systems,
tailoring a MPB by chemical modification becomes a promising strategy to design high-performance
BFO-BT based lead-free piezoelectric ceramics.
In this work, the (1-x)BiFe0.97Ga0.03O3-xBaTiO3 (abbreviated as BFO-xBT) ceramics weresynthesized by conventional solid state reaction method. The effects of BT content on its phase structure,
microstructure and electrical properties were investigated. A MPB between rhombohedral (R) andtetragonal (T) phases was found at x = 0.30. Moreover, with increase of BT content, the ceramics
gradually transform from ferroelectric to relaxor ferroelectric phases. Due to the multiphase coexistence
structure at the MPB, the BFO-30BT ceramic exhibited the superior properties with large remnant
polarization Pr=40.8μC/cm2, high dielectric constant εr= 80,000 at TC, medium piezoelectric coefficient
d33 = 114 pC/N and kp = 0.284, and high Curie temperature TC = 470 oC. In addition, the temperaturedependent piezoelectric and ferroelectric analysis confirmed that the BFO-BT ceramics possessincreasing piezoelectric coefficient d33 to 200 pC/N at 300°C, and a large electric-field-induced unipolarstrain of 0.5% at 190°C. These superior high-temperature piezoelectric properties indicates the goodtemperature stability of the BFO-BT based piezoelectric ceramics. These results indicates that the BFOBT ceramic is a potential lead-free piezoelectric materials for high temperature applications.

Reference
1．

S. J. Zhang, et al., J Mater Res. 36 985-995 (2021)

2．

M. H. Lee, et al., Adv Mater. 27 6976-6982 (2015)

3．

B. W. Xun, et al., Acs Appl Mater Inter. 13 4192-4202(2021)

68

P-09:
Activation of lead-free (Na,K)NbO3 piezoceramics using pulsed electric field
Takumi Nozaki1, Alexander Martin1, Ryota Kobayashi1, Tadachika Nakayama2, Ken-ichi Kakimoto1*
1

Nagoya Institute of Technology, Japan

2

Nagaoka University of Technology, Japan*E-mail: kakimoto.kenichi@nitech.ac.jp

To take advantage of the piezoelectric effect, which describes the ability of a material to transduce
electrical into mechanical energy, and vice versa, piezoceramics need prior electrical poling. The polingprocess is generally carried out at a constant voltage under a direct current (DC)-poling field. Recently,
studies have shown that pulsed electric fields can have certain advantages, such as the enhancement of
the piezoelectric properties of lead-base materials, over DC-poling fields.[1, 2] However, these pulsed
electric fields can take the form of different waves, such as triangular, sinusoidal, or rectangular, withvarying results. In addition, the electric fields can be unipolar, as well as sesquipolar, or bipolar, meaningalternating current (AC-)poling fields. As such, three different types of pulsed electric field using several
waveforms were applied to (Na,K)NbO3 (NKN)-based ceramics. Here, NKN ceramics are a promising
candidate for lead-free piezoceramics, as they demonstrate a high Curie temperature and goodpiezoelectric properties.[3] In this study, the different effect each pulsed field had on the activation of thepiezoelectric properties was compared, and the underlying mechanisms discussed.
0.20 mol% MnO-added (Na0.55K0.45)NbO3 (NKN) ceramics were prepared by a solid-state reaction
method. The compacted disks of NKN powder were sintered at 1060°C for 2h. Poling experiments were
performed at ambient temperature in a silicon oil bath. Four different waveforms of 3DC and 1AC, as
illustrated in Fig. 1(a)–1(c-2), were applied to the NKN ceramics. The electrical properties were
measured using a ferroelectric tester and d33-meter. In order to understand the changes to the electricalproperties, characterization of the domain structure was conducted using a scanning electron microscope.
Conventional DC-poling with a poling time of 100 sec resulted in NKN ceramics with apiezoelectric charge coefficient d33 of 141.3 pC/N. Equivalent values were achieved by pulsed DCpoling in only 10 sec. On the other hand, a lower value (d33 = 135 pC/N) was recorded after pulsed ACpoling. As such, the activation of the piezoelectric properties depended on the waveforms of pulsed
electric field. A correlation between piezoelectric properties and domain structure was discussed, as wellas the viability of pulsed electric fields.

Fig. 1. Schematics of waveforms for (a) conventional DC-poling, (b) triangular pulsed AC-poling,(c-1) triangular pulsed DC-poling, (c-2) rectangular pulsed DC-poling.
References[1] T. Kobayashi, Y. Suzuki, N. Makimoto, H. Funakubo, and R. Maeda, AIP Adv. 4, 117116 (2014).
[2] Y. Yamashita, N. Yamamoto, Y. Hosono, and K. Itsumi, U.S. Patent 0372219 A1 (2015).

69

P-10:

Realization of enhanced strain responses in lead-free (Bi0.5Na0.5)TiO3-based ferroelectricthin films by active domain motions
Zhe Wanga, Jinyan Zhao*a, Gang Niu*a, Wei Ren*a, Nan Zhanga, Kun Zhenga, Yi Quana, Henghui Caib,
Xin Lib, Genshui WangbaElectronic Materials Research Laboratory, Key Laboratory of the Ministry of Education & International
Center for Dielectric Research, School of Electronic Science and Engineering, Xi’an Jiaotong University,
Xi’an 710049, Chinab
Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai, 200050, China

Abstract
Lead-free (Bi0.5Na0.5)TiO3-based ferroelectric ceramics and thin films with excellent
piezoelectric properties and strain responses possess broad application prospects for precision
actuators and transducer applications. In this work, (Bi0.5Na0.5)TiO3-BaTiO3-NaNbO3(BNT-BT-NN) thin films were prepared by sol-gel methods and deposited on Pt/TiO2/SiO2/Si(001) substrates. An ultrahigh strain response of 1.7% was obtained in the BNT-BT-NN thinfilms as the NN substitution of 6%. Low dielectric loss tanδ of ~ 0.03 and low leakage currentof ~ 9 × 10-9 ~ 2 × 10-7 A/cm2 thank to the high quality and well-organized microstructures by
optimizing the solution preparation and cautious control of the film deposition process. The
BNT-BT-NN samples exhibited a phase coexistence of ferroelectric (FE) phase and relaxor(RE) state in a pseudo-cubic structure. It is believed that the enhanced strain responses areclosely related to the reversible phase transition between the RE state and FE phase. Largetransient currents related to domain switching measured by PUND method indicated that
active domain wall motions contribute to higher dielectric and piezoelectric responses.
Further, the intensity of the current peak related to the domain switching in the BNT-BT-NN
thin films as the NN substitution of 6% is higher than that of other compositions. The
enhanced strain response renders the NN-modified BNT-based thin films appealing for
precise actuator and transducer applications.

70

P-11:

Preparation of high temperature resistant barium titanate/polyimide flexible
nanocomposite energy storage films
Peimei Yuan, Ruixuan Xue, ChenLi Wu, Rong Ma, Dengwei Hu*
Faculty of Chemistry and Chemical Engineering, Engineering Research Center of Advanced
Ferroelectric Functional Materials, Baoji University of Arts and Sciences, Baoji, Shaanxi, China,
721013(* Corresponding author, E-mail address: dwhu@bjwlxy.edu.cn)
Abstract: Dielectric energy storage capacitors can release stored energy in a very short time
(microsecond level) to produce large power pulses. At present, its practical applications placed in highpower, high current and high temperature working conditions. Therefore, it is urgent to develop
dielectric materials with high energy storage density and high temperature resistance which suitablefor high temperature dielectric energy storage capacitors.Here, the two-dimensional barium titanate
powder was prepared by combining with solid and hydrothermal method, and the barium
titanate/polyimide (BT/PI) composite films were prepared by the diffusion method. When 5% filled at
the condition of 150 ℃, the energy density of the composite film can reach 0.7 J/cm3, the charging anddischarging efficiency can reach 77.1%, and the dielectric constant was stable at about 5.0 within therange of 150 ℃.
Keywords: High-temperature energy storage, Polyimide, Barium titanate

Fig1.(a) The Fourier transform infrared spectra, (b) TG curves, (c) D-E loops at 150 ℃, (d) dielectric
permittivity on temperature at 106 Hz, (e) Energy density and Efficiency and (f) Dr, Dmax and Dmax-Dr
of 0, 1, 3, 5, 7 and 9 wt% BT/PI nanocomposite films.
References[1] Wang P, Yao LM, Pan ZB, et al. Adv Mater. 2021, 33(42):2103338.
[2] Li H, Zhou Y, Liu Y, et al. Chem Soc Rev. 2021, 50(11):6369.
[3] Dong JF, Hu RC, Xu XW, et al. Adv Funct Mater. 2021, 31(32):2102644.

71

P-12:
Change of crystal and microscopic structures of Ba0.95Sr0.05TiO3 ceramics
prepared by the combination of reaction sintering and spark plasma sintering
A Fujisawa, D Fu
Shizuoka University, Japan*E-mail: fu.tokusho@shizuoka.ac.jp
Controlling the microstructure of ceramics is of great importance to improve their properties. Here,
we report the change of crystal and microstructure of Ba0.95Sr0.05TiO3 (BSTO-5) ceramics prepared by
the one-step reaction sintering using the system of Spark Plasma Sintering (SPS), in which solid phasereaction and sintering can proceed simultaneously within a very short time under the application ofhigh pressure. It is found that the solid-state reaction between BaTiO3 and SrTiO3 can be finished as
the sample is heated to 1200 oC at a heating rate of 100 oC /min under a 1 atm N2 atmosphere . In
association with the complete of the reaction, the microstructure is changed sharply, leading to therapid densification of the BSTO-5 ceramics. By using this approach, we can prepare BSTO-5 ceramicwith a relative density higher than 99 % and with an extremely dense and homogeneous
microstructure. In addition, the dielectric and ferroelectric properties of the obtained sample have been
investigated and will be reported in detail.

72

P-13:
Microstructure of AC poled ternary PIN-PMN-PT single crystal after high temperatureannealing.
Yu Xiang¹, Yinqin Sun², Y. Yamashita1,2,3, T. Karaki², and H. Maiwa¹*
1
Shonan Institute of Technology, Japan
2
Toyama Prefect. Univ., Japan
3
North Carolina State Univ., USA,
*E-mail: maiwa@mate.shonan-it.ac.jp
Ternary system of Pb(In1/2Nb1/2)O3-Pb(Mg1/3Nb2/3)O3-PbTiO3 (PIN-PMN-PT) piezoelectric single
crystals (SCs) have been utilized as high-frequency>5 MHz medical array transducers because of theirhigher coercive field Ec>4 kV/cm and higher phase transition temperature Tpc>100°C compared tothose of binary system PMN-PT SCs. Recently, Yamamoto and Yamashita have reported that enhanced
di- and piezoelectric properties are obtained by applying AC polarization (ACP) to SCs in the [001]orientation of the rhombohedral phase compared to conventional DC polarization (DCP), which has
attracted worldwide attention. [ref. 1-3]. Many reports have been published on the microstructures of
DCP and ACP piezoelectric SCs observed using piezoelectric force microscopy (PFM) and scanningelectron microscopy (SEM). The ACP piezoelectric SCs have been reported to show stripe 109° domainsof 0.5 to several μm parallel to the electrodes, unlike DCP products. However, there has been no reportcomparing the microstructure of DCP and ACP SCs once depolarized (DEP) by annealing at 300°C,
which was fairly higher than Curie temperature (Tc) of these materials (Tc=130-220°C).
We performed DCP and ACP on the 0.24PIN-0.46PMN-0.30PT SC plates with a Tc of 180°C producedby continuous feeding Bridgman method, which provides excellent uniformity of composition andproperties, followed by DEP at 300°C for 10 min of annealing. The piezoelectric constants (d33) of thesamples after high-temperature annealing was less than 10 pC/N, and no piezoelectric response wasobserved in the impedance spectra measurements. The microstructures of (a) ACP and (b) ACP-DEP
samples observed by SEM were shown in Figure 1. The ACP sample showed stripe like layered structureof 109° domains as reported previously. However, the ACP-DEP sample showed no piezoelectric
response but a microstructure with residual striped 109° domains.
This result indicates that stripe 109° domains formed once by ACP still maintained after annealing
temperature of 300°C, which is 120°C higher than the Tc even the SC does not show any piezoelectric
responses. These results suggest that repeated ACP-DEP on the same piezoelectric SC sample may bepreserve the past history of the microstructure. Therefore, we have to take care that the microstructuresof SC have a past poling history, which may lead to a different judgment of microstructure.

(a)

(b)

Fig.1 SEM microstructure of (a) ACP and (b) ACP-DEP of PIN-PMN-PT SCs. Note, the ACP-DEP SC
showed 109° stripe like domains after 300℃ annealing.
References(1) N. Yamamoto and Y. Yamashita, USP 2014/0062261 A1, 2015/0372219 A1.
(2) Y. Sun et al, JJAP, vol.61, SB0802 (2022)(3) H-P. Kim et al, IEEE TUFFC, Vol. 69, No. 11, Nov 2022 3037 (2022)73

P-14:
Effects of sputtering conditions on the growth of AlScN thin films
and its conduction mechanism
Kohei Miyaji1, Norifumi, Fujimura1, Takeshi Yoshimura1*
1

Osaka Metropolitan University, Japan*E-mail: yoshimura@omu.ac.jp[Introduction] Recently, Al1-xScxN (AlScN) thin films have attracted much attention due to the increasein piezoelectric constant [1] and the appearance of ferroelectricity [2]. However, (AlScN) thin films
have an issue of reliability because the coercive electric field (Ec) is close to the breakdown electric field(Ebd) [3][4]. To utilize the ferroelectricity of AlScN thinfilms in electronic devices, the leakage current should
be low enough even near Ebd. In this study, theconductive mechanism of AlScN thin films fabricatedunder different conditions was investigated to discuss
the factors affecting the leakage current.
[Experiments and results] AlScN films were
deposited by RF magnetron sputtering on 2-inch(111)Si wafer using a Al0.7Sc0.3 alloy target. The RF
power was set to 50 W, and the Ar/N2 ratio was varied
between 0.09 and 4.0. The substrate temperature andchamber pressure was kept at 300 °C and 0.8 Pa,
respectively, during the deposition. Fig. 1 shows the Xray diffraction patterns of AlScN thin films deposited

Fig. 1. X-ray diffraction patterns of
AlScN films deposited at various
Ar/N2 ratios.

at various Ar/N2 ratios. (0002) oriented AlScN films
were grown at the Ar/N2 ratio from 0.25 to 1.5. The caxis lattice constants, calculated from the data in the
figure were changed 0.74 %. Fig. 2 shows I-V
characteristics of the AlScN film deposited at Ar/N2 =0.25. By increasing the step delay time, which is thedelay time for each voltage step, from 0.1 s to 1 s, theleakage current increases. This result indicates that thevacancies in the thin film are filled in a short time.

Fig. 2. I-V characteristics of the AlScN
film deposited at Ar/N2 = 0.25.

[References][1] M. Akiyama et al., Adv. Mater., 21, 593 (2009).
[2] S. Fichtner et al., J. Appl. Phys. 125, 114103 (2019).
[3] J. Muller et al., ECS J Solid State Sci Technol, 4 N30 (2015).
[4] D. Wang et al., Phys. Status Solidi RRL,15, 2000575 (2021).

P-15:
High-Performance Neuromorphic Computing Based on Ferroelectric Synapses with
Excellent Conductance Linearity and Symmetry
Shuting Yang1, Limei Zheng1*, Le Zhao2
1
School of Physics, Shandong University, Jinan, P. R. China
2
School of Information and Automation Engineering Qilu University of Technology (Shandong
Academy of Science), Jinan, P. R. China*E-mail: zhenglm@sdu.edu.cn
Artificial synapses can boost neuromorphic computing to overcome the inherent limitations of von
Neumann architecture. As a promising memristor candidate, ferroelectric tunnel junctions (FTJ) enable
us to successfully emulate spike-timing dependent synapses. However, the nonlinear and asymmetricsynaptic weight update under repeated presynaptic stimulation hampers neuromorphic computing byfavoring the runaway of synaptic weights during learning.
Here we demonstrate an FTJ (Au/Cr/BaTiO3/Nb:SrTiO3) whose conductivity varies linearly andsymmetrically by judiciously combining ferroelectric domain switching and oxygen vacancy migration.
The artificial neural network based on this FTJ-synapse achieves classification accuracy of 96.7%
during supervised learning, which is the closest to the maximum theoretical value of 98% achieved todate. This artificial synapse also demonstrates stable unsupervised learning in a noisy environment for
its well-balanced spike timing-dependent plasticity response. Our novel concept of controlling ionicmigration in ferroelectric materials paves the way towards highly reliable and reproducible supervisedand unsupervised learning strategies.

FIG. (a) The balanced STDP is independent of initial states in our devices. (b) The classification
accuracy versus nonlinearity of some typical two-terminal artificial synapses. The linear weight update
makes the supervised learning classification accuracy in our device the best of all two-terminal devices.
(c) The variation of unsupervised learning recognition rate with the noise level. Our device demonstrates
that the balanced STDP contributes greatly to the robustness of unsupervised learning.

75

P-16:
Low-temperature deposition of transparent Pb(Zr1-xTix)O3 thin film on glass substratewith giant piezoelectric response
K. Yoshida1, S. Sogen1, H. Suzuki1, T. Arai2, and D. Fu1*
1

Shizuoka University, Japan, 2National Institute of Technology Numazu College, Japan*E-mail: fu.tokusho@shizuoka.ac.jp

Pb(Zr1-xTix)O3 (PZT) shows a morphotropic phase boundary (MPB) at the composition of
x=0.47~0.48, in which high piezoelectricity has been found [1], and its ceramics has been widely usedfor various devices. Also, PZT thin films deposited on Si substrate have been intensively investigated
for the applications in the semiconductor integration devices. For the development of next generation ofpiezoelectric devices, it is highly desired to deposit PZT film with excellent piezoelectric properties on
the transparent glass substrate. However, the issue remained to be solved is how to prepare the PZT filmon glass substrate at a deposition temperature lower than its strain point. For the commonly used TFT
glass substrate, it is necessary to prepare the PZT film at a low temperature of 550°C. However, theapproach for such a low-temperature deposition has not been established.
Here, we report a novel approach to deposit the PZT film on the glass substrate at a low temperatureof 550°C, in which the molecularly designed precursors were used. In our approach, a LaNiO3 (LNO)
conducting seed-layer was also introduced to control the orientation growth. Fig. 1 clearly shows that
our PZT film deposited at 550°C on glass substrate is transparent and preferably oriented along the[100]/[001] direction. As shown in Fig. 2, our PZT film with MPB composition of x= 0.47 exhibits alarge displacement of 5 nm at an applied voltage of 20 V, which corresponds to an effective piezoelectric
response of 250 pm/V that is higher than the reported value of 220 pm/V for the pure PZT ceramics[1].

More importantly, we found that the tetragonal PZT film with x= 0.55 shows higher piezoelectric
response than the PZT film with MPB composition. An extremely large displacement of 10 nm wasobserved for this film at the same applied voltage of 20 V, which corresponds to a giant piezoelectric
response of 500 pm/V. This value is twice of that of PZT film with MPB composition.

0
20

30

PZT(200)&(002)

Displacement (nm)400

LNO(200)

800

PZT(110)
LNO(110)1200

LNO(100)

Intensity [a.u.]

1600

PZT(100)&(001)[1] D. A. Berlincourt, C. Cmolik and H. Jaffe, Proceedings of the IRE 48, 220-229(1960).

40502 [deg]

60

70

10
9
8
7
6
5
4
3
2
1
0

x = 0.55

x = 0.47

0

5

10
15
Voltage (V)20

25

Fig. 1 XRD pattern of the PZT thin film with

Fig. 2. Displacement curves under the application of

x= 0.47. Insert shows the photographic

the unipolar voltage. The film thickness is estimatedimage of the deposited film.

to be 800 nm.

76

P-17:
Mechanomyography Using Piezoelectric Materials
S. Sakoda1, N. Fujimura1 and, T. Yoshimura1*
1

Osaka Metropolitan University, Japan*Email: yoshimura@omu.ac.jp

Introduction: There are increasing concerns about the utilization of electronic devices in the medical
and health fields. Detecting muscle fatigue during exercise is useful for rehabilitation and injury
prevention by optimizing exercise intensity. Mechanomyography (MMG) is one of the methods to detectmuscle fatigue and a technique that measures minute vibrations during muscle movement using acondenser microphone, accelerometer, and so on [1]. Compared to the widely used surface
electromyography (sEMG), MMG is less susceptible to changes in skin condition caused by perspirationand is expected to be used under intense exercise and in daily life. However, due to the large noisecaused by motion artifacts, it has not yet been realized for these applications. In this work, we fabricateda sensor using organic piezoelectric material and investigated a way to measure muscle movement.
Measurement and result: Fig. 1 shows the structure of a fabricatedsensor. P(VDF-TrFE-CFE) sheet with a thickness of 25 μm,
manufactured by PolyK, was used for the sensor. Pt electrodes with athickness of about 40 nm were deposited on both sides of the P(VDFTrFE-CFE) sheet by sputtering. The frequency dependence of thedielectric constant and loss shown in Fig. 2 indicates that the capacitor

Fig. 1 The (b)structure of thevibration sensor.

structure is formed as expected. Then, comparative experiments of sEMG and MMG were conducted.
Commercially available electrodes (Ag/AgCl) were placed parallel to the muscle fibers as shown in Fig.
3 and the MMG sensor was also placed between them. The interface between the MMG sensor and theskin was wetted with water to facilitate the transmission of the muscle sound. Fig. 4 shows themeasurement results. The peaks of the sEMG and MMG signals appear synchronously, which indicatesthat MMG can be measured with the fabricated sensor. It appears that the large SNR of MMG is causedby poor contact with the skin.

Fig. 2 Dielectric constant andtan as a function of frequency.

Fig. 3 Placement of sEMG
and MMG sensors on thearm.

Fig. 4 sEMG and MMG signals.

References: [1] H. Han et al., Med. Biol. Eng. Comput. 53, 577–588 (2015).

77

P-18:
Unique Gas Sensing Performance of Sol-gel Derived BiFeO3 Nanoparticles
Xiaojie Li 1, 2, Jinrong Cheng 1*, Jiaqiang Xu 2
1

School of Material Science and Engineering, Shanghai University, Shanghai 200444, China
2

NEST Lab, College of Science, Shanghai University, Shanghai 200444, China*E-mail: jrcheng@shu.edu.cn

Perovskite BiFeO3 (BFO) oxides, a kind of ferroelectric semiconductors with rich physical andchemical properties, have been regarded as promising sensing materials for the toxic and harmful gas
detection. In this talk, BFO nanoparticles and tourmaline@BFO composites were prepared by a facile
sol-gel method. Micro-Electro-Mechanical System (MEMS) gas sensors were fabricated by using BFO
based materials. The corona poling treatment has great effects on the gas sensing behavior by regulating
the polarization field and carrier movements of BFO nanoparticles. The BFO-P4 (poled under 4 kV)
sensor exhibits a high response value of 4.8 for H2S with concentration of 1200 ppb at 220°C, achieving
a detection limit of 10 ppb and a short response/recovery time of only 3s/7s respectively. In addition,
tourmaline@BFO composites with the growth of nano-sized BFO on the tourmaline laminar exhibit thetemperature-dependent dual selectivity for C3H6O and H2S at 150 and 210 oC respectively. Our results
indicate that BFO based sensors with unique gas sensing performances have great potentials in detectionof polar H2S and C3H6O gases.
Key words: BiFeO3 nanoparticles; tourmaline@BiFeO3 composites, corona poling; MEMS gas
sensor; H2S and C3H6O

78

P-19:
Ferroelectric and piezoelectric properties of c-axis oriented PbZr0.53Ti0.47O3 thin film
deposited on SUS substrate with large coefficient of thermal expansion
Seiji Sogen1, Kazuto Yoshida1, Takashi Arai2, Hisao Suzuki1, Desheng Fu1*
1

Shizuoka University, Japan

2

Numazu college, National Institute of Technology, Japan*E-mail: fu.tokusho@shizuoka.ac.jp

Pb(Zr1-xTix)O3 (PZT) ceramics and thin films with composition near the morphotropic phase boundary(MPB, x=0.47-0.48)

have been widely applied due to their excellent ferroelectric and piezoelectric

properties. However, there is a lack of understanding of it its intrinsic physical properties owing to thedifficulty in the growth of single crystal since it was discovered several decades ago. Here, we report
the ferroelectric and piezoelectric of polar-axis-oriented PZT thin film with the MPB composition(x=0.47) . The PZT film was deposited on SUS substrate that has a 1.5-time coefficient of thermal
expansion of PZT. Such larger coefficient of thermal expansion allows to apply an in-plane compressive
stress to the PZT film as cooling down from the firing temperature to room temperature, leading to thec-axis orientated growth of PZT film with the help of the seed layer of a-axis oriented LaNiO3 (LNO)electrode. Our PZT precursor was prepared by a partial hydrolysis method and had a high degree ofhomogeneity of B-sites. As evident from the x-ray diffraction pattern shown in Fig. 1, the c(polar)-axis
oriented PZT film has been successfully prepared on the SUS substrate. More importantly, the remanentpolarization of our PZT film shows nearly the same value of the saturation polarization, indicatingthat all ferroelectric domains were aligned along the same direction under the application of a highelectric field. This is further confirmed by the displacement-field loop, in which a pure linear
piezoelectric response was observed when the domains were nearly aligned along the field direction for
E>Ec. The piezoelectric constant d33 of PZT along the polar axis was then calculated from this linear
relationship between the displacement and the applied voltage and was estimated to be 40~49 pm/V
from several samples. Our experimental result is in good agreement with the value of 50~55 pC/N
predicted from first principles calculations for PZT single crystal. [1] Our finding indicates that the large
piezoelectric response observed in PZT polycrystalline is essentially dominated by the domain effects.
(001)

1500

P

(400)

*

30

40

50
2 (deg)

60

95

1000
500
0

-50
-600

100

D

0

-300

0

300

Displacement (pm)

2

(004)

(002)
*

20

Polarization (C/cm )

50

(110)

Intensity (a.u.)

* LNO

-500
600

Electric Field (kV/cm)

Fig.1 XRD patterns of PZT film with x=0.47. Fig.2 P -E and displacement loops of PZT film with x=0.47.

References[1] L. Bellaiche, A. García, and D. Vanderbilt, Finite-Temperature Properties of Pb(Zr1-xTix)O3 Alloys
from First Principles, Phys. Rev. Lett. 84, 5427 (2000).

79

P-20:
Superior energy storage properties in NaNbO3-based ceramics via synergistically
optimizing domain and band structures
Weiwei Yang1,2, Huarong Zeng1,2*, Guorong Li1,2
1
Key Laboratory of Inorganic Functional Materials and Devices, Shanghai Institute of
Ceramics, Chinese Academy of Sciences, Shanghai 201899, China
2Center of Materials Science and Optoelectronics Engineering, University of Chinese
Academy of Sciences, Beijing 100049, China*E-mail: huarongzeng@mail.sic.ac.cn
Environmental-friendly ceramic capacitors with outstanding energy storage properties (ESP)
are greatly desired for the advanced pulsed power systems. However, it is still a greatchallenge to develop lead-free dielectric materials with simultaneous excellent recoverable
energy storage density (Wrec) and energy storage efficiency (η). In the present work, asynergistic optimization strategy with regard to ferroelectric domain and band structure isapplied to NaNbO3 (NN)-based ceramics, where the introduction of Bi3+ induces theelongated ferroelectric P-E loops due to nanodomains formation, and the further modificationof Ta doping content remarkably reduces the grain size and widens the band gap (Eg), leading
to a high breakdown strength. As a result, the involved Na0.7Bi0.1Nb0.9Ta0.1O3 ceramics exhibit
excellent comprehensive ESP (Wrec = 7.33 J/cm3, η = 83.68%, Eb = 530 kV/cm) and goodstability. Moreover, ultrafast discharge time of 60 ns and high power density of 320.21
MW/cm3 are also achieved. The Na0.7Bi0.1Nb0.9Ta0.1O3 ceramics with uncomplicated chemicalcomposition and prominent properties demonstrate promising applications to pulsed powersystem and the synergistic optimization strategy in this study offers an important clue for
future lead-free ceramic capacitors.

80

P-21:
Extremely large strain response under low driving electric fields in lead-based
textured piezoelectric ceramics
Hongrui Jia1, Zhen Li1, Linghang Wang1*
1
Electronic Materials Research Laboratory, Key Laboratory of the Ministry of Education andInternational Center for Dielectric Research, School of Electronic Science and Engineering, Xi’an
Jiaotong University, Xi’an, 710049, P. R. China*
E-mail: corresponding. lhwang@xjtu.edu.cn
Precision positioning technology is one of the key technology to achieve precision manufacturing,
precision measurement and precision drive, and it has been receiving great attentions and widely usedin optical engineering, aerospace, semiconductor industry and many other high-tech fields. As the key
part of precision positioning system, micro-displacement actuator play an important role in sensitivity
and resolution of precision positioning system. In order to achieve large driving force and high-precisiondisplacement of micro-displacement actuator, it is particularly necessary for piezoelectric ceramics topossess a high strain value and low strain hysteresis under small driving electric fields. Up to date, itremains grand challenge for piezoelectric ceramics to simultaneously possess large strain response andlow strain hysteresis under low driving electric fields. At present, texture technique, which can makeceramic grains oriented along specific crystallographic orientation, is considered one of the mostpromising means to significantly improve the strain response of piezoelectric ceramics. In this work, we
adopted a combination strategy of composition design and texture technique to develop a novel textured
ceramics to address this challenge. In this paper, 1%Sm-PMN-30PT textured ceramics with highly[001]c orientation was successfully manufactured and an ultrahigh strain response of 0.27 % and a low
strain hysteresis of 15 % at 2 kV/mm were obtained concurrently.

Fig. 1. Structural and strain characterizations of 1%Sm-PMN-30PT ceramics. (a) Surface SEM image ofrandom ceramics. (b) Fracture surface SEM images of textured ceramics. (c) XRD patterns of random andtextured ceramics. (d) Unipolar strain curves of random and textured ceramics.

81P-22:
Experimental approach to residual hydrogen content in silicon substrates
by proton beam writing
Jun HIRADE and Masaki YAMAGUCHI*
Shibaura Institute of Technology, Japan*E-mail: yamag@sic.shibaura-it.ac.jp
Water lithography, electron beam induced reaction, inkjet printing, screen printing, three-dimensional
printing, etc. have been actively investigated as microfabrication techniques for piezoelectric materials.
Among them, we think that the focused proton beam writing (PBW) is very effective formicrofabrication of piezoelectric materials containing heavy elements. However, in our previous report,
it has been confirmed that irradiated protons go through piezoelectric films to reach the substrate byMonte Carlo simulation results.1-3 In semiconductor technology, hydrogen implantation is used to
manufacture Silicon-On-Insulator (SOI) wafers, formation of porous silicon, and increase the resistanceof silicon substrates.4-6 This suggests that the protons remaining in the substrate affect the characteristicsof the fabricated device. Therefore, in this study, the residual amount of irradiated protons to the silicon
substrate was estimated by the infrared (IR) absorption method.
A focused proton beam lithography system (KOBELCO, MB-S1000) with an acceleration voltage of
1 MV was used to prepare the measurement silicon samples. In this study, silicon with a resistivity of 5
ohm-cm was used as the proton-irradiated substrate. The IR absorption spectra were measured using
FTIR (JASCO, FT/IR-4100) in a dry nitrogen atmosphere.
Figure shows the IR spectra at various proton doses. As can be seen from the figure, absorption due
to the Si-H bonds could not be observed in the irradiation range up to 300 µC/cm2. Monte Carlosimulation results indicate that most of the irradiated protons are distributed only within 2 µm in thedepth direction. In this region, the maximum hydrogen concentration is calculated to be 0.02 at%.
However, it is possible that the detection limit has not been reached. Therefore, we will continue toevaluate the amount of residual hydrogen in the substrate by further increasing the proton dose.
Acknowledgements
The authors would like to thank Prof. H. Nishikawa and Mr.
K. Kawamura for their cooperation in sample fabrication.
References
1. H. Kimura et al., Nanoscale ferroelectric-multiferroic
materials for energy harvesting applications, Chap. 5,
Elsevier, 2019.
2. M. Yamaguchi et al., J. Korean Phys. Soc., 71, 88, 2017.
3. J. Hirade et al., IEICE technical report, SDM2017-83,
2017. [in Japanese]
4. B. Aspar et al., Microelectron. Eng., 36, 233, 1997.
5. P. Polesello et al., Nucl. Instrum. Methods Phys. Res. B,
158, 173, 1999.
6.

T. Inoue et al., IEICE Trans. J101-C, 344, 2018. [inJapanese]

Fig. IR spectra of silicon substrates with various proton
doses. The spectrum has not been normalized.

82

P-23:

Polarization Rotation Control Domain Dynamic Response Modulates Piezoelectric
Properties of Lead-Free Thin Films
Kun Zhu1, Guanglong Ge1, Jinfeng Lin1, Hairui Bai1, Cheng Shi1, Guohui Li1, Fei Yan1, Liuxue Xu1,
Weiwei Yang2, Huarong Zeng2, Kunyu Zhao2, Zhenyong Man2, Feifei Wang3, Bo Shen,1* Jiwei Zhai,1*Xiujian Chou4*
1
Key Laboratory of Advanced Civil Engineering Materials of Ministry of Education Functional
Materials Research Laboratory, School of Materials Science and Engineering, Tongji University,
Shanghai, 201804, China
2
CAS Key Laboratory of Inorganic Functional Materials and Devices, Shanghai Institute of Ceramics,
Chinese Academy of Sciences, Shanghai 201899, China
3
Key Laboratory of Optoelectronic Material and Device, Department of Physics, Shanghai Normal
University, Shanghai 200234, China
4
Key Laboratory of Instrumentation and Dynamic Measurement of Ministry of Education, North
University of China, Taiyuan, 030051, China* E-mail: shenbo@tongji.edu.cn; apzhai@tongji.edu.cn; chouxiujian@nuc.edu.cn
Domain orientation engineering regulates the polarization direction of thin film and facilitates theenhancement of piezoelectric properties. A change in polarization direction implies a structural change
in the piezoelectric thin film. In this work, some unexpected results have been obtained by preparing
three orientations of Bi0.5Na0.5TiO3-based lead-free piezoelectric thin films to amplify this structuralchange. In distinction to the conventional perception, the piezoelectric properties decrease withincreasing polarization direction. This anomaly is influenced by the concentration of structural defects,
and rotation of the polarization direction may induce a change in the electronic structure of thematerial and hence in the concentration of structural defects. Ultimately, the suppression of the domain
dynamics response by increasing structural defects leads to the worst piezoelectric properties for thinfilms with the traditionally perceived optimal (100) orientation. The revelation of this anomaly has
implications for the design of the next generation of high-performance piezoelectric thin films.

83

P-24:High Energy Storage Performance and Large Electrocaloric Response in
Bi0.5Na0.5TiO3–Ba(Zr0.2Ti0.8)O3 Thin Films
Jin Qiana, Jiwei Zhaia, Zhenxiang Chengb

Shanghai Key Laboratory for R&D and Application of Metallic Functional Materials, Functional MaterialsaResearch Laboratory, School of Materials Science and Engineering, Tongji University, Shanghai, 201804,
China.
b

Institute for Superconducting and Electronic Materials, Australian Institute for Innovative Materials,

University of Wollongong, Innovation Campus, North Wollongong, NSW 2500, Australia.

*E-mail: apzhai@tongji.edu.cn

With regard to the global energy crisis and environmental pollution, ferroelectric thin films withunique polarization behavior have garnered considerable attention for energy storage and electrocaloric
refrigeration. Herein, a series of (1−x)Bi0.5Na0.5TiO3–xBa(Zr0.2Ti0.8)O3 (x = 0.3–0.9; (1−x)BNT–xBZT)
films was fabricated on Pt(111)/Ti/SiO2/Si substrates. Incorporating BZT can tune the polarization behavior
and phase transition temperature of BNT. In this work, high energy storage performances of Wrec ≈ 78 J
cm−3 with η ≈ 72% and Wrec ≈ 82 J cm−3 with η ≈ 81% were observed in the 0.5BNT–0.5BZT and
0.3BNT–0.7BZT films, respectively. Both the capacitors have wide frequency and operating temperature
ranges (0.5–20 kHz, 20 °C–200 °C), robust fatigue endurance (107 cycles), and ultrafast discharge speed(<0.4 μs). Meanwhile, the 0.5BNT–0.5BZT film exhibited a high EC effect near room temperature (ΔT ≈−22.9 K, ΔS ≈ 33.4 J K−1 kg−1). These remarkable performances signify that the (1−x)BNT–xBZT system isa promising multifunctional electronic material for energy storage and solid-state cooling applications.

84

P-25:
Enhanced stabilization of oxygen vacancies on the bipolar fatigue resistance of PNNPZT-based ceramics
Ying Shi1,2, Guorong Li1, *, Liaoying Zheng1, Zhenyong Man1, Xuezheng Ruan1, Xue Shi1
1
Key Laboratory of Inorganic Functional Materials and Devices, Shanghai Institute of Ceramics,
Chinese Academy of Sciences, 1295 Dingxi Road, Shanghai 200050, PR China
2Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of
Sciences, Beijing 100049, China*E-mail: grli@mail.sic.ac.cn
The MPB structure PZN-PNN-PZT ceramics were prepared by Mn ions doping and the bipolar fatigue
behavior of samples was investigated at both 0.6 Ec and 2 Ec fatigue fields. Enhanced bipolar fatigue
resistance is found by 0.1wt% Mn doping and the remnant polarization Pr only reduces to 0.3% (0.6EC) and 5.8% (2 EC) of the initial value after 106 fatigue cycling. In this work, it is implied that in contrast
to the undoped sample, little oxygen vacancy with a weak pinning effect is advantageous to fatigue
resistance. These oxygen vacancies hinder crack propagation and stabilize the domain structure during
repeated electric cycling. The successive increase of oxygen vacancy leads to the severe pinning effectand degradation of polarization. The influence of oxygen vacancy on fatigue behavior depends on theamplitude of the fatigue field. The characteristics of ceramics in different fatigue fields can be attributed
to the pinning effect, mechanical damage, or coexistence of both for different Mn content. This finding
is significant to ceramics with MPB structure and has a guideline for the hard material applied in electricfield cycling.

Figure 1. The normalized Pr and EC of Mn-doped PZN-PNN-PZT ceramics as a function of (a-b) 0.6
EC, (c-d)2 EC bipolar fatigue cycles.

Figure 2 and Figure 3. The SEM images for cross sections of Mn-doped PZN-PNN-PZT ceramics
fatigued at 0.6 EC and 2EC. (a) x=0;(b) x=0.1;(c) x=0.2;(d) x=0.3;(e) x=0.4;(f) x=0.6.

85P-26:
Preparation of Tetragonal BaTiO3 by Molten Salt Synthesis Process
Fei Jing, Nina Dai, Weixing Zhao, Dengwei Hu*
Faculty of Chemistry and Chemical Engineering, Engineering Research Center of Advanced
Ferroelectric Functional Materials, Baoji University of Arts and Sciences, Baoji, Shaanxi, China,
721013(* Corresponding author, E-mail address: dwhu@bjwlxy.edu.cn)
Abstract: In this work, BaTiO3 powders were synthesized by molten-salt synthesis process using TiO2,
Ba(OH)2, and the eutectic salts (NaCl, KCl) as the raw materials. A systematic study is investigatedthat it indicates the effects of calcination temperature, time as well as the eutectic salts such as NaCl,KCl and NaCl-KCl are related to Ba(OH)2-TiO2 on the microstructures of BaTiO3 powders. The
results showed that all powders crystallized with tetragonal perovskite structure, it further conﬁrmed
through X-ray diffraction pattern and Raman spectra. Tetragonal BaTiO3 were prepared by molten-salt
synthesis process of reacting TiO2, Ba(OH)2 and KCl at 770 ºC for 2 h. The prepared BaTiO3 powers
exist characteristic tetragonal splitting of 002/200 in XRD peaks. Meanwhile, it also supports thetetragonal symmetry (c/a = 1.0139). The present results provide a generalized methodology forlarge-scale synthesizes of other perovskite transitional metal oxide powders with less energy
consumption.
Key Words: Tetragonal BaTiO3, Eutectic salts, Molten-salt synthesis process
(A)

(B)

(C)

Fig.1 (A) XRD patterns, (B) Raman spectra and (C) SEM images of the BaTiO3 powders prepared bymolten-salt synthesis method of reacting TiO2 and Ba(OH)2 at 770 ºC for 2 h with (a) 20 %, (b) 30 %,(c) 40 %, (d) 50 % KCl contents.
References[1] Hu D, Miao L, Zhang Z, et al. Crystal Growth & Design, 2018, 18(12): 7264-7274.
[2] Xue P, Hu Y, Xia W, et al. Journal of Alloys and Compounds, 2017, 695: 2870-2877.
[3] Mandal T K. Materials Letters, 2007, 61(3): 850-854.
[4] Charoonsuk T, Sriphan S, Nawanil C, et al. Journal of Materials Chemistry C, 2019, 7(27):8277-8286.
[5] Xue P, Wu H, Xia W, et al. Journal of the American Ceramic Society, 2019, 102(5): 2325-2336.

86

P-27:
Energy storage properties of antiferroelectric PbZrO3 thin films prepared by chemicalsolution deposition method
T. Nishimoto, S. Sougen, K. Yoshida, H. Suzuki, D. Fu,
Shizuoka University, Japan
E-mail: fu.tokusho@shizuoka.ac.jp
PbZrO3 (PZ) is a typical antiferroelectric material and is expected to be a high-density energy storage material.
Its energy storage properties have been extensively studied both for the bulk ceramic and thin film. Generally,
thin films exhibit a higher energy storage density (Wrec) than its ceramics, and the high energy storage densityof 19.4 J/cm3 has been reported for the PZ thin film [1]. However, further improvement of its properties isrequired for the applications. Here, we report the enhancement of the energy storage density of PZ thin film
prepared by chemical solution deposition (CSD) method from the molecularly designed precursors. In the
study, we have developed a novel process to prepare the precursors using partial hydrolysis, which allows us
to improve the crystalline quality of the PZ film. The PZ film was deposited on a Si substrate with a buffer
layer of LaNiO3 (LNO). The LNO buffer layer, which acts as the bottom electrode for the electricalmeasurements, was successfully controlled into the [100]-axis orientation, leading to the local epitaxial growthof PZ film. It is found that the films prepared Molecular-design of the precursor solution by partial hydrolysis
also resulted in the thicker film thickness per layer than those prepared without partial hydrolysis, because of
the higher degree of polymerization and higher homogeneity of the precursor solution. The PZ film with partialhydrolysis shows a larger value of energy storage density of 23.1 J/cm3 that is higher than the reported one[1].
Moreover, this value is 1.4 times higher than that of the PZ film without using the partial hydrolysis. It seems
that the molecularly designed precursors and the LNO buffer layers are of great importance to improve theenergy storage properties of PZ film.
【Reference】[1] M.D. Nguyen et al., Thin Solid Films 697, pp.5-7(2020).

87

P-28:
3D Printing of Piezoelectric Biological Scaffolds for Bone Tissue Engineering
Ruixuan Xue, Peimei Yuan, Liying Yu, Rong Ma, Dengwei Hu*
Faculty of Chemistry and Chemical Engineering, Engineering Research Center of Advanced
Ferroelectric Functional Materials, Baoji University of Arts and Sciences, Baoji, Shaanxi, China,
721013(* Corresponding author, E-mail address: dwhu@bjwlxy.edu.cn)
Abstract: Numerous studies have shown that the process of bone repair and regeneration requires avariety of physiological cues, including biological, electrical and mechanical cues. Piezoelectricmaterials can regulate the physiological micro-environment by changing the mechanical and electricalstimulation environment, which shows excellent potential in bone repair. However, the traditional
processing method cannot satisfy the diversified structure of piezoelectric biological scaffolds. 3D
printing technology has been introduced into bone tissue engineering due to its high efficiency, highresolution, low cost, efficient use of materials and the ability to manufacture complex structures, itbringing a new dawn for bone tissue repair. Here, the ceramic paste for printing was prepared bymixing the nano-BaTiO3 (BT) particles, commercial nano-Ca10(PO4)6OH (HA) and photosensitive
resin. Then the porous interconnecting ceramic bracket and ceramic cylinder are printed by digital
light processing technology. The compact structure of the ceramics was obtained after calcination, andthe dielectric constant εr reaches 2733 when 90 wt%BaTiO3 doped ceramics. DLP printing technology
can prepare high precision ceramic supports.
Key Words: 3D printing technology, BaTiO3, Ca10(PO4)6OH, Piezoelectric scaffolds.
(a)

(c)

(b)

5

1 cm

Fig.1 (a) Temperature dependence of dielectric constant and dielectric loss, (b) SEM image of
90wt%BT/HA sample after calcination, (c) Different types of piezoelectric scaffolds for 3D printing.
References
[1]
[2]
[3]
[4]
[5]

Mancuso E, Shah L, Jindal S, et al. Materials Science and Engineering: C, 2021, 126, 112192.
Chen J, Li S, Jiao Y, et al. ACS Applied Materials & Interfaces, 2021, 12, 51885−51903.
More N, Kapusetti G. Medical hypotheses, 2017, 108, 10-16.
Shuai C, Liu G, Yang Y, et al. Colloids and Surfaces B: Biointerfaces, 2020, 185, 110587.
Chen C, Wang X, Wang Y, et al. Advanced Functional Materials, 2020, 30(52), 2005141.

88

P-29:
Flexible Piezoelectric Nanogenerators Based on Two-dimensional Barium Titanate
Nanosheets and Polymer Polylactic acid
Bo Zhao, Yao Su, Songlin Yu, Han Yu, Dengwei Hu*
Faculty of Chemistry and Chemical Engineering, Engineering Research Center of Advanced
Ferroelectric Functional Materials, Baoji University of Arts and Sciences, Baoji, Shaanxi, China,
721013(*Corresponding author, E-mail address: dwhu@bjwlxy.edu.cn)
Abstract: With the increasing demand for green energy, piezoelectric nanogenerators (PNG) obtain
extensive attention in energy harvesting. In this work, high-performance PNG were successfully
fabricated from the composite of BaTiO3 (BT) (Fig.1b) and polylactic acid (PLA) via spin-coatingprocess. Among, high aspect ratio BT nanoparticle with 2D plate-like morphology synthesized by thesolvothermal method which significantly enhanced the piezoelectric properties of the BT/PLA
nanocomposite (Fig.1e). The piezoelectric properties of PNG enhanced with the increasing of doping
BT. The PNG with 6 wt% BT achieved a maximum output voltage of 11.97 V (Fig.1f) andshort-circuit current of 560 nA (Fig.1e). This study shows potential applications of flexible 2D
BT/PLA nanocomposite in human motion monitoring, smart skin, and soft robotics. Likewise, it
provides an ingenious idea for the disposal of wasted PNG devices and the recycle of piezoelectric
fillers.
Keywords: Piezoelectric nanogenerators, BaTiO3, Polylactic acid.

Fig.1 SEM images of (a) HTO and (b) BT crystals; (c) Schematic diagram of PNG structure and (d)Digital photo of flexible BT/PLA nanocomposite. (e) output voltages and (f) currents of BT/PLA PNG
with BT contents of 0, 2, 4, 6, 8 and 10 wt%, respectively. (g) Open circuit voltages and (h)short-circuit currents of 6 wt % BT/PLA nanocomposite films under different pressures.
References[1] ACS Appl. Mater. Interfaces 2018,10, 38359-38367.
[2] ACS Appl. Mater. Interfaces 2022, 12, 51885−51903.
[3] Energy Technol 2018, 6, 922-927.

89

P-30:
Energy storage of BT/PVP/PVDF nanocomposite films with multilayer structure

Nina Dai, Fei Jing, Peimei Yuan, Ruixuan Xue, Bo Zhao, Yao Su, Dengwei Hu*
Faculty of Chemistry and Chemical Engineering, Engineering Research Center of Advanced
Ferroelectric Functional Materials, Baoji University of Arts and Sciences, Baoji, Shaanxi, China,
721013(*Corresponding author, E-mail address: dwhu@bjwlxy.edu.cn)
Abstract: Dielectric capacitors are widely used in modern electronic technology. They have theadvantages of ultra-fast charge and discharge rates and ultra-high power density. In order to meet theincreasing demand for miniaturization of electronic products, dielectric capacitors with high energy
storage performance have been extensively studied. Barium titanate/polyvinylidene fluoride(BT/PVDF) based nanocomposite membrane is a kind of energy storage composite with excellent
physical and chemical properties, electrical properties and energy density. How to improve thestructural defects of inorganic nanomaterials and the interface polarization between materials are aserious problem at present. Further improving the energy storage performance of composite materials
is closely related to the capacitor structure, that is, reasonable structural design is needed. The current
research is expected to achieve the multi-scale engineering ceramic structures. Therefore,
BT/PVP/PVDF multilayer ceramic capacitors will be an important research direction in the future.
Key Words: BaTiO3, Energy storage, Dielectric capacitor.
(a)

(b)

Fig.1 (a) Representative emerging applications of dielectric capacitors, (b) Schematic illustrations (toppanel) and direct observations (bottom panel) of multiscale structures, including interface, grain,domain, and spontaneous polarization, for typical ferroelectric ceramic-based MLCCs.

References
[1]
[2]
[3]
[4]
[5]

Yao F Z, Yuan Q, Wang Q, et al. Nanoscale, 2020, 12(33): 17165-17184.
Dong X, Li X, Chen H, et al. Ceramics International, 2021, 47(5): 6077-6083.
Wang Y, Yao M, Ma R, et al. Journal of Materials Chemistry A, 2020, 8(3): 884-917.
Siddiqui S, Bhunia R, Singh N, et al. Materials Advances, 2020, 1(4): 680-688.
Bhunia R, Gupta S, Garg A, et al. Journal of Polymer Science, 2022, 60(6): 961-967.

90

P-31:

Fabrication of (Ba,Sr)TiO3 epitaxial thin films on mica substrate
toward flexible electronics
Shicheng Peng1, Sou Yasuhara1, Takaaki Tsurumi1, Takuya Hoshina1*
1
Tokyo Institute of Technology, 2-12-1 Ookayama, Meguro-ku, Tokyo,152-8550, Japan*E-mail: hoshina.t.aa@m.titech.ac.jp
Flexible devices are capable of attaching to curved surfaces and are expected to be applied
especially in the medical and healthcare fields. While the piezoelectric effect is often used in strain
sensors or vibration power generator, the flexoelectric effect is also effective for flexible devices withnanostructures. The flexoelectric effect is an electrical polarization phenomenon caused by a strain
gradient and is observed in all dielectrics. This phenomenon is especially prominent in perovskite
oxides, and it is known that (Ba,Sr)TiO3 (BST) exhibits a high flexoelectric coefficient near the
ferroelectric phase transition temperature. In this study, BST thin films were fabricated on a mica
substrate, which is known as a flexible substrate in order to demonstrate flexoelectric flexible devices.
Pulsed laser deposition (PLD) method was used to fabricate the thin films. To promote the crystal
growth of the perovskite phase, a seeding layer of CoFe2O4 (CFO) was first deposited on (001) mica
substrate. SrRuO3 (SRO) layer was deposited as the bottom electrode, and then Ba0.5Sr0.5TiO3 thin film
was deposited on the SRO layer.
Figure 1 shows the photograph of BST/SRO/CFO/mica flexible structure with a lateral size of 12 ×
12 mm2. The mica substrate was peeled off to a thickness of about 20 μm. Out-of-plane XRD results
showed that only mica (00l) and perovskite (111) diffraction peaks were detected, indicating the BST
thin film exhibits high crystallinity without any secondary phases. Furthermore, the φ-scans of BST(002), and mica (202) were performed to determine the in-plane orientation relationship. Based on the
XRD results, the epitaxial relationship of the heterostructure can be determined as (111) BST / (001)mica. Figure 2 indicates the dielectric property of BST thin film. The relative permittivities of the thinfilms were around 200 and the dielectric losses were less than 0.1. Flexible structure consisting of ahigh-quality dielectric film could be fabricated.

Fig.1 Photographflexible structure.

of

BST/SRO/CFO/mica

Fig.2 Dielectric property of Ba0.5Sr0.5TiO3 thinfilm on mica substrate.

91About the Best Poster Presentation Award
The best poster presentation award certificates and some memorial goods for student
poster presentations will be given from the Dielectric Society Japan (DSJ) by the Poster
Presentation Award Judging Committee.
The results will be shown in the CJFMA14 website.

92

93

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94

Call for Paper

40thMeeting on Ferroelectric Materials
and Their Applications (FMA40)
May 24-27, 2023, Kyoto, Japan
Scope & Topics
The purpose of the meeting is to bring together scientists and engineers engaged in thefields relating to polarization. Papers are presented in Japanese, or in English.
We are looking for contributors on, but not limited to, the following topics:・ New phenomena and measurement methods relating to polarization
・ Preparation, property and evaluation of materials(single crystal, ceramics, amorphous, thin film, polymer, liquid crystal, composite, etc.)
・ Applications relating to polarization(solid state capacitors, chemical capacitors, high-frequency dielectrics, PTC thermistors,piezoelectric applications [sensors, actuators, ultrasonic devices, filters and resonators] ,pyroelectric applications, electro-optic devices, memory devices, recording devices,displays, polarization in lithium ion batteries and solid state batteries etc.)

JJAP Special Issue
Authors of accepted papers in FMA are encouraged to submit their original papers to
the Special Issues of Japanese Journal of Applied Physics (JJAP), an international
journal published by the Japan Society of Applied Physics and IOP Publishing. The meritis that you can submit an extended version of your FMA paper as a full-length paper inEnglish and the paper will be reviewed for a short time. Note that a special rate of
publication charge (40,000JPY/paper) is available for the special issue.

Key Dates

Venue

Short Abstract Submission:
January 31, 2023
Extended Abstract Submission:
April 10, 2023
Manuscript Submission：
May 27, 2023
(JJAP Special Issue)

60th Anniversary Hall,
Kyoto Institute of Technology, Japan

Fees (Japanese Yen)

Early *2

Late

DESJ Member *1

15,00018,000DESJ Student Member *1

5,000

6,000

Non-member

24,00026,000*1 You can join DESJ (The Dielectric Society of Japan)*2 To be announced

Organization & Information
General Chair
Yoshihiro Kuroiwa (Hiroshima Univ.)
Program Committee Chair
Ken-ichi Kakimoto (Nagoya Inst. Tech.)
Executive Committee Chair
Takuya Hoshina (Tokyo Tech.)

See FMA39 (June 2022) >http://www.dielectric-jpn.org/index_en
http://fma-meeting.jp/en/index.html
94