Physical Review B
covering condensed matter and materials physics
- Highlights
- Recent
- Accepted
- Collections
- Authors
- Referees
- Search
- Press
- About
- Editorial Team
Electrically variable interfaces in polymer nanocomposite dielectrics
Wen-Zhi Luo, Zhong-Hui Shen, Yang Shen, Long-Qing Chen, and Ce-Wen Nan
Phys. Rev. B 109, 184205 – Published 9 May 2024
- Article
- References
- No Citing Articles
- Supplemental Material
PDFHTMLExport Citation
- Abstract
- Authors
- Article Text
Abstract
Polymer nanocomposites generally exhibit unexpected dielectric/electrical performance far beyond the sum of every component, which is mainly due to the interface effect induced by the differences in structures and properties between the nanofillers and the polymer matrix. However, understanding the capricious interface effect in different polymer nanocomposites remains a major challenge. Here, we perform density functional theory calculations to investigate the atomic/molecular configurations and local charge behaviors of heterogeneous interfaces between the fillers of perovskites, oxides, two-dimensional materials, and polar/nonpolar polymers. Our findings demonstrate that atomic reconfiguration takes place during the formation of the inorganic/organic interface in order to minimize the overall energy of the system. Significant charge accumulation occurs at heterogeneous interfaces due to electron redistribution, especially for the examples of and negatively charged . When applying an electric field, local polarization, especially around the interface, will be distorted and enhanced as a result of interfacial interaction. Even for the nonpolar polymer with linear dielectric oxides such as , induced dipole moments also appear near the interface, leading to the improvement of overall polarizability. The outcomes of our study verify that the variable electrical behaviors at the interfaces are highly dependent on the feature of every component constituting the inorganic/organic interface, which offers valuable insights for optimizing the experimental design of heterogeneous interfaces in polymer nanocomposites.
- Received 22 January 2024
- Revised 2 April 2024
- Accepted 15 April 2024
DOI:https://doi.org/10.1103/PhysRevB.109.184205
©2024 American Physical Society
Physics Subject Headings (PhySH)
- Research Areas
Electric polarization
- Physical Systems
Solid-solid interfaces
- Techniques
Density functional calculations
Condensed Matter, Materials & Applied Physics
Authors & Affiliations
Wen-Zhi Luo1, Zhong-Hui Shen1,2,*, Yang Shen3, Long-Qing Chen4, and Ce-Wen Nan3
- 1State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Center of Smart Materials and Devices, Wuhan University of Technology, Wuhan 430070, China
- 2School of Materials and Microelectronics, Wuhan University of Technology, Wuhan 430070, China
- 3School of Materials Science and Engineering, State Key Lab of New Ceramics and Fine Processing, Tsinghua University, Beijing 100084, China
- 4Department of Materials Science and Engineering, The Pennsylvania State University, University Park, Pennsylvania 16802, United States
- *Corresponding author: zhshen@whut.edu.cn
Article Text (Subscription Required)
Click to Expand
Supplemental Material (Subscription Required)
Click to Expand
References (Subscription Required)
Click to Expand
Issue
Vol. 109, Iss. 18 — 1 May 2024
Access Options
- Buy Article »
- Log in with individual APS Journal Account »
- Log in with a username/password provided by your institution »
- Get access through a U.S. public or high school library »
Images
Figure 1
The schematic diagram of PNs with (a) a multitude of heterogeneous interfaces, where significant charge redistribution occurs. (b) Some changes in material properties at the interface, such as electrostatic potential distribution and dielectric constant modulation. The interface thickness is usually on nanometric scale. (c) The representative inorganic fillers with three primary categories: namely perovskites, oxides, and two-dimensional layered structures. (d) The polymer structures of the nonpolar iPP and polar PVDF used as the matrices in this work.
Figure 2
The atomic structure model of /PVDF and /iPP in the view of [001] plane in the unrelaxed state. The -terminated with (a) H- and (c) F-, and BaO-terminated with (b) H- and (d) F-. The (e) -terminated and (f) BaO-terminated of /iPP interfaces. (g) The interfaces' relative energies versus interface width. The markers are calculated values, and the curves are fitted UBER models. (h) The separations of all stable interface models in this work.
Figure 3
The electron transfer isosurfaces and charge displacement curve (CDC) along of (a) perovskite fillers, (b) oxides fillers, (c) 2D layered fillers with PVDF matrix. The schematic diagrams above the curve represent BFO/PVDF, /PVDF, and CNO/PVDF, respectively. The yellow and blue isosurfaces represent charge accumulation and depletion. The gray area denotes the interface region.
Figure 4
The electron transfer isosurfaces and charge displacement curve (CDC) along of (a) perovskite fillers, (b) oxides fillers, (c) 2D layered fillers with iPP matrix. The schematic diagrams above the curve represent BTO/iPP, /iPP, and CNO/iPP, respectively. The yellow and blue isosurfaces represent charge accumulation and depletion. The gray area denotes the interface region.
Figure 5
Microscopic polarization along the axis in PVDF matrix with (a) perovskite fillers, (b) oxide fillers, and (c) 2D layered fillers, averaged along the x-y plane. (d) The polarization charge distribution of BFO/PVDF, /PVDF, CNO/PVDF, where the yellow and bule isosurfaces represent the induced positive and negative charge. Microscopic polarization occurs from areas of positive charge towards regions of negative charge.
Figure 6
Microscopic polarization along the axis in iPP matrix with (a) perovskite fillers, (b) oxide fillers, and (c) 2D layered fillers, averaged along the x-y plane. (d) The polarization charge distribution of BNT/iPP, /iPP, CNO/iPP, where the yellow and blue isosurfaces represent the induced positive and negative charge. Microscopic polarization occurs from areas of positive charge towards regions of negative charge.
