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Title: High-temperature magnetostructural transition in van der Waals-layered α - MoCl 3

Here, the crystallographic and magnetic properties of the cleavable 4d 3 transition metal compound α–MoCl 3 are reported, with a focus on the behavior above room temperature. Crystals were grown by chemical vapor transport and characterized using temperature dependent x-ray diffraction, Raman spectroscopy, and magnetization measurements. A structural phase transition occurs near 585 K, at which the Mo-Mo dimers present at room temperature are broken. A nearly regular honeycomb net of Mo is observed above the transition, and an optical phonon associated with the dimerization instability is identified in the Raman data and in first-principles calculations. The crystals are diamagnetic at room temperature in the dimerized state, and the magnetic susceptibility increases sharply at the structural transition. Moderately strong paramagnetism in the high-temperature structure indicates the presence of local moments on Mo. This is consistent with results of spin-polarized density functional theory calculations using the low- and high-temperature structures. Above the magnetostructural phase transition the magnetic susceptibility continues to increase gradually up to the maximum measurement temperature of 780 K, with a temperature dependence that suggests two-dimensional antiferromagnetic correlations.
Authors:
ORCiD logo [1] ; ORCiD logo [1] ;  [1] ; ORCiD logo [1] ; ORCiD logo [1] ; ORCiD logo [1] ; ORCiD logo [1] ; ORCiD logo [1] ;  [1] ; ORCiD logo [1] ; ORCiD logo [1] ; ORCiD logo [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Grant/Contract Number:
AC05-00OR22725; AC02-05CH11231
Type:
Accepted Manuscript
Journal Name:
Physical Review Materials
Additional Journal Information:
Journal Volume: 1; Journal Issue: 6; Journal ID: ISSN 2475-9953
Publisher:
American Physical Society (APS)
Research Org:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE
OSTI Identifier:
1407774
Alternate Identifier(s):
OSTI ID: 1407843

McGuire, Michael A., Yan, Jiaqiang, Lampen-Kelley, Paula, May, Andrew F., Cooper, Valentino R., Lindsay, Lucas R., Puretzky, Alexander A., Liang, Liangbo, KC, Santosh, Cakmak, Ercan, Calder, Stuart, and Sales, Brian C.. High-temperature magnetostructural transition in van der Waals-layered α-MoCl3. United States: N. p., Web. doi:10.1103/PhysRevMaterials.1.064001.
McGuire, Michael A., Yan, Jiaqiang, Lampen-Kelley, Paula, May, Andrew F., Cooper, Valentino R., Lindsay, Lucas R., Puretzky, Alexander A., Liang, Liangbo, KC, Santosh, Cakmak, Ercan, Calder, Stuart, & Sales, Brian C.. High-temperature magnetostructural transition in van der Waals-layered α-MoCl3. United States. doi:10.1103/PhysRevMaterials.1.064001.
McGuire, Michael A., Yan, Jiaqiang, Lampen-Kelley, Paula, May, Andrew F., Cooper, Valentino R., Lindsay, Lucas R., Puretzky, Alexander A., Liang, Liangbo, KC, Santosh, Cakmak, Ercan, Calder, Stuart, and Sales, Brian C.. 2017. "High-temperature magnetostructural transition in van der Waals-layered α-MoCl3". United States. doi:10.1103/PhysRevMaterials.1.064001.
@article{osti_1407774,
title = {High-temperature magnetostructural transition in van der Waals-layered α-MoCl3},
author = {McGuire, Michael A. and Yan, Jiaqiang and Lampen-Kelley, Paula and May, Andrew F. and Cooper, Valentino R. and Lindsay, Lucas R. and Puretzky, Alexander A. and Liang, Liangbo and KC, Santosh and Cakmak, Ercan and Calder, Stuart and Sales, Brian C.},
abstractNote = {Here, the crystallographic and magnetic properties of the cleavable 4d3 transition metal compound α–MoCl3 are reported, with a focus on the behavior above room temperature. Crystals were grown by chemical vapor transport and characterized using temperature dependent x-ray diffraction, Raman spectroscopy, and magnetization measurements. A structural phase transition occurs near 585 K, at which the Mo-Mo dimers present at room temperature are broken. A nearly regular honeycomb net of Mo is observed above the transition, and an optical phonon associated with the dimerization instability is identified in the Raman data and in first-principles calculations. The crystals are diamagnetic at room temperature in the dimerized state, and the magnetic susceptibility increases sharply at the structural transition. Moderately strong paramagnetism in the high-temperature structure indicates the presence of local moments on Mo. This is consistent with results of spin-polarized density functional theory calculations using the low- and high-temperature structures. Above the magnetostructural phase transition the magnetic susceptibility continues to increase gradually up to the maximum measurement temperature of 780 K, with a temperature dependence that suggests two-dimensional antiferromagnetic correlations.},
doi = {10.1103/PhysRevMaterials.1.064001},
journal = {Physical Review Materials},
number = 6,
volume = 1,
place = {United States},
year = {2017},
month = {11}
}