Local orbital degeneracy lifting as a precursor to an orbital-selective Peierls transition
Abstract
Fundamental electronic principles underlying all transition metal compounds are the symmetry and filling of the d-electron orbitals and the influence of this filling on structural configurations and responses. Here we use a sensitive local structural technique, x-ray atomic pair distribution function analysis, to reveal the presence of fluctuating local-structural distortions at high temperature in one such compound, CuIr2S4. We show that this hitherto overlooked fluctuating symmetry-lowering is electronic in origin and will modify the energy-level spectrum and electronic and magnetic properties. The explanation is a local, fluctuating, orbital-degeneracy-lifted state. The natural extension of our result would be that this phenomenon is likely to be widespread amongst diverse classes of partially filled nominally degenerate d-electron systems, with potentially broad implications for our understanding of their properties.
- Authors:
-
[1];
[1];
[3]
- Brookhaven National Lab. (BNL), Upton, NY (United States)
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Brookhaven National Lab. (BNL), Upton, NY (United States); Columbia Univ., New York, NY (United States)
- Publication Date:
- Research Org.:
- Argonne National Laboratory (ANL), Argonne, IL (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division
- OSTI Identifier:
- 1560035
- Alternate Identifier(s):
- OSTI ID: 1543404; OSTI ID: 1670676
- Report Number(s):
- BNL-211872-2019-JAAM; BNL-219937-2020-JAAM
Journal ID: ISSN 2041-1723; 150997
- Grant/Contract Number:
- AC02-06CH11357; SC0012704
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Communications
- Additional Journal Information:
- Journal Volume: 10; Journal Issue: 1; Journal ID: ISSN 2041-1723
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; 36 MATERIALS SCIENCE; Electronic properties and materials; Structure of solids and liquids
Citation Formats
Bozin, Emil S., Yin, W. G., Koch, R. J., Abeykoon, M., Hor, Y. S., Zheng, H., Lei, H. C., Petrovic, C., Mitchell, J. F., and Billinge, S. J. L. Local orbital degeneracy lifting as a precursor to an orbital-selective Peierls transition. United States: N. p., 2019.
Web. doi:10.1038/s41467-019-11372-w.
Bozin, Emil S., Yin, W. G., Koch, R. J., Abeykoon, M., Hor, Y. S., Zheng, H., Lei, H. C., Petrovic, C., Mitchell, J. F., & Billinge, S. J. L. Local orbital degeneracy lifting as a precursor to an orbital-selective Peierls transition. United States. https://doi.org/10.1038/s41467-019-11372-w
Bozin, Emil S., Yin, W. G., Koch, R. J., Abeykoon, M., Hor, Y. S., Zheng, H., Lei, H. C., Petrovic, C., Mitchell, J. F., and Billinge, S. J. L. Tue .
"Local orbital degeneracy lifting as a precursor to an orbital-selective Peierls transition". United States. https://doi.org/10.1038/s41467-019-11372-w. https://www.osti.gov/servlets/purl/1560035.
@article{osti_1560035,
title = {Local orbital degeneracy lifting as a precursor to an orbital-selective Peierls transition},
author = {Bozin, Emil S. and Yin, W. G. and Koch, R. J. and Abeykoon, M. and Hor, Y. S. and Zheng, H. and Lei, H. C. and Petrovic, C. and Mitchell, J. F. and Billinge, S. J. L.},
abstractNote = {Fundamental electronic principles underlying all transition metal compounds are the symmetry and filling of the d-electron orbitals and the influence of this filling on structural configurations and responses. Here we use a sensitive local structural technique, x-ray atomic pair distribution function analysis, to reveal the presence of fluctuating local-structural distortions at high temperature in one such compound, CuIr2S4. We show that this hitherto overlooked fluctuating symmetry-lowering is electronic in origin and will modify the energy-level spectrum and electronic and magnetic properties. The explanation is a local, fluctuating, orbital-degeneracy-lifted state. The natural extension of our result would be that this phenomenon is likely to be widespread amongst diverse classes of partially filled nominally degenerate d-electron systems, with potentially broad implications for our understanding of their properties.},
doi = {10.1038/s41467-019-11372-w},
journal = {Nature Communications},
number = 1,
volume = 10,
place = {United States},
year = {Tue Aug 13 00:00:00 EDT 2019},
month = {Tue Aug 13 00:00:00 EDT 2019}
}
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Figures / Tables:
Fig. 1: Observation of high-temperature fluctuating ODL state in CuIr2S4. a Temperature waterfall stack of xPDFs measured on warming from 10 K (bottom) to 500 K (top) in 2 K increments. TMI is the MIT transition temperature (226 K). The dimer peak at ~3 Å (marked by arrow) is onlymore »
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