skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Mechanistic Insights into the Superexchange-Interaction-Driven Negative Thermal Expansion in CuO

Abstract

The negative thermal expansion (NTE) in CuO is explained via electron-transfer-driven superexchange interaction. The elusive connection between the spin–lattice coupling and NTE of CuO is investigated by neutron scattering and principal strain axes analysis. The density functional theory calculations show as the temperature decreases, the continuously increasing electron transfer accounts for enhancing the superexchange interaction along [$$ 10\bar{1} $$], the principal NTE direction. It is further rationalized that only when the interaction along [$$ 10\bar{1} $$] is preferably enhanced to a certain level compared to the other competing antiferromagnetic exchange pathways can the corresponding NTE occur. Outcomes from this work have implications for controlling the thermal expansion through superexchange interaction, via, for example, optical manipulation, electron or hole doping, etc.

Authors:
ORCiD logo [1]; ORCiD logo [2];  [2];  [2]
  1. Neutron Scattering Division, Oak Ridge National Laboratory (ORNL), Oak Ridge, Tennessee 37831, United States; Materials Measurement Science Division, National Institute of Standards and Technology (NIST), 100 Bureau Drive, Gaithersburg, Maryland 20899, United States
  2. Neutron Scattering Division, Oak Ridge National Laboratory (ORNL), Oak Ridge, Tennessee 37831, United States
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory-National Energy Research Scientific Computing Center (NERSC)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1528939
DOE Contract Number:  
AC05-00OR22725; AC02-05CH11231
Resource Type:
Journal Article
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 141; Journal Issue: 15; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English

Citation Formats

Zhang, Yuanpeng, McDonnell, Marshall, Calder, Stuart A., and Tucker, Matthew G. Mechanistic Insights into the Superexchange-Interaction-Driven Negative Thermal Expansion in CuO. United States: N. p., 2019. Web. doi:10.1021/jacs.9b00569.
Zhang, Yuanpeng, McDonnell, Marshall, Calder, Stuart A., & Tucker, Matthew G. Mechanistic Insights into the Superexchange-Interaction-Driven Negative Thermal Expansion in CuO. United States. doi:10.1021/jacs.9b00569.
Zhang, Yuanpeng, McDonnell, Marshall, Calder, Stuart A., and Tucker, Matthew G. Sun . "Mechanistic Insights into the Superexchange-Interaction-Driven Negative Thermal Expansion in CuO". United States. doi:10.1021/jacs.9b00569.
@article{osti_1528939,
title = {Mechanistic Insights into the Superexchange-Interaction-Driven Negative Thermal Expansion in CuO},
author = {Zhang, Yuanpeng and McDonnell, Marshall and Calder, Stuart A. and Tucker, Matthew G.},
abstractNote = {The negative thermal expansion (NTE) in CuO is explained via electron-transfer-driven superexchange interaction. The elusive connection between the spin–lattice coupling and NTE of CuO is investigated by neutron scattering and principal strain axes analysis. The density functional theory calculations show as the temperature decreases, the continuously increasing electron transfer accounts for enhancing the superexchange interaction along [$ 10\bar{1} $], the principal NTE direction. It is further rationalized that only when the interaction along [$ 10\bar{1} $] is preferably enhanced to a certain level compared to the other competing antiferromagnetic exchange pathways can the corresponding NTE occur. Outcomes from this work have implications for controlling the thermal expansion through superexchange interaction, via, for example, optical manipulation, electron or hole doping, etc.},
doi = {10.1021/jacs.9b00569},
journal = {Journal of the American Chemical Society},
issn = {0002-7863},
number = 15,
volume = 141,
place = {United States},
year = {2019},
month = {3}
}