Issue 3, 2015

First-principles study of negative thermal expansion mechanism in A-site-ordered perovskite SrCu3Fe4O12

Abstract

Negative thermal expansion (NTE) materials offer a tremendous opportunity for fundamental as well as applied research, yet the origin remains difficult to understand. Here we perform a systematic first-principles calculation to investigate electrical and magnetic properties of an A-site-ordered perovskite SrCu3Fe4O12 and clarify its NTE mechanism. We find that SrCu3Fe4O12 is an antiferromagnetic metal, and its magnetic ordering can be demonstrated as C-type within Fe ions of mixed valence at the B-site and paramagnetic Cu3+ at the A-site. Electronic structure analysis reveals that there occurs temperature-induced Cu–Fe intersite charge transfer, which is mediated by the corner-sharing O atoms. Meanwhile, the magnetic interaction is found to undergo a transition from antiferromagnetism to ferrimagnetism. Further phonon calculations demonstrate that the SrCu3Fe4O12 is thermodynamically stable both at low and high temperature, and that there appear degenerated phonon branches, indicating that it is easy to transfer energy between these modes. We also find that the large NTE of SrCu3Fe4O12 originates from intermetallic charge transfer induced by temperature, which relaxes the Sr–O and Fe–O bonding units in the oxide.

Graphical abstract: First-principles study of negative thermal expansion mechanism in A-site-ordered perovskite SrCu3Fe4O12

Article information

Article type
Paper
Submitted
14 Aug 2014
Accepted
26 Nov 2014
First published
27 Nov 2014

RSC Adv., 2015,5, 1801-1807

First-principles study of negative thermal expansion mechanism in A-site-ordered perovskite SrCu3Fe4O12

H. Li, S. Liu, L. Chen, J. Zhao, B. Chen, Z. Wang, J. Meng and X. Liu, RSC Adv., 2015, 5, 1801 DOI: 10.1039/C4RA08652J

To request permission to reproduce material from this article, please go to the Copyright Clearance Center request page.

If you are an author contributing to an RSC publication, you do not need to request permission provided correct acknowledgement is given.

If you are the author of this article, you do not need to request permission to reproduce figures and diagrams provided correct acknowledgement is given. If you want to reproduce the whole article in a third-party publication (excluding your thesis/dissertation for which permission is not required) please go to the Copyright Clearance Center request page.

Read more about how to correctly acknowledge RSC content.

Social activity

Spotlight

Advertisements