Electric field-dependent thermal conductivity of relaxor ferroelectric PMN-33PT through changes in the phonon spectrum†

IF 10.7 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Materials Horizons Pub Date : 2025-03-14 DOI:10.1039/D4MH01845A
Delaram Rashadfar, Brandi L. Wooten and Joseph P. Heremans
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Abstract

In ferroelectric materials, an electric field has been shown to change the phonon dispersion sufficiently to alter the lattice thermal conductivity, opening the possibility that a heat gradient could drive a polarization flux, and technologically, also opening a pathway towards voltage-driven, all solid-state heat switching. In this report, we confirm the validity of the theory originally developed for Pb(Zr,Ti)O3 (PZT) on the ferroelectric relaxor 0.67Pb[Mg1/3Nb2/3]O3–0.33PbTiO3 (PMN–33PT). In theory, the change in sound velocity and thermal conductivity with an electric field relates to the piezoelectric coefficients and the Grüneisen parameter. It predicts that in PMN–33PT the effect should be an order of magnitude larger and of opposite sign as in PZT; this is confirmed here experimentally. The effects are measured on samples never poled before and on samples that underwent multiple field sweep cycles and passed through two phase transitions with change in temperature. The thermal conductivity changes are linked to variations in the piezoelectric coefficients and can be as large as 8–11% at T ≥ 300 K. To date, this has been the only means of heat conduction modulation that utilizes changes in the phonon spectrum. While this technology is in its infancy, it offers another path to future active thermal conduction control.

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弛豫铁电PMN-33PT通过声子谱变化的电场依赖热导率。
在铁电材料中,电场已被证明足以改变声子色散,从而改变晶格的导热性,从而开启了热梯度驱动极化通量的可能性,并且在技术上,也开辟了电压驱动的全固态热开关的途径。在本报告中,我们证实了最初建立的Pb(Zr,Ti)O3 (PZT)对铁电弛豫剂0.67Pb[Mg1/3Nb2/3]O3-0.33 pbtio3 (PMN-33PT)的理论的有效性。理论上,声速和导热系数随电场的变化与压电系数和颗粒尼森参数有关。它预测PMN-33PT的效应应该比PZT大一个数量级,而且符号相反;这在实验中得到了证实。对从未极化过的样品和经过多次场扫描循环并随温度变化经历两次相变的样品进行了测量。热导率的变化与压电系数的变化有关,在温度≥300 K时,热导率的变化可高达8-11%。到目前为止,这是利用声子光谱变化进行热传导调制的唯一方法。虽然这项技术还处于起步阶段,但它为未来的主动热传导控制提供了另一条途径。
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来源期刊
Materials Horizons
Materials Horizons CHEMISTRY, MULTIDISCIPLINARY-MATERIALS SCIENCE, MULTIDISCIPLINARY
CiteScore
18.90
自引率
2.30%
发文量
306
审稿时长
1.3 months
期刊介绍: Materials Horizons is a leading journal in materials science that focuses on publishing exceptionally high-quality and innovative research. The journal prioritizes original research that introduces new concepts or ways of thinking, rather than solely reporting technological advancements. However, groundbreaking articles featuring record-breaking material performance may also be published. To be considered for publication, the work must be of significant interest to our community-spanning readership. Starting from 2021, all articles published in Materials Horizons will be indexed in MEDLINE©. The journal publishes various types of articles, including Communications, Reviews, Opinion pieces, Focus articles, and Comments. It serves as a core journal for researchers from academia, government, and industry across all areas of materials research. Materials Horizons is a Transformative Journal and compliant with Plan S. It has an impact factor of 13.3 and is indexed in MEDLINE.
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