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Optimized in situ crystal growth and disordered quasi-one-dimensional magnetism in Li2Mn2(MoO4)3

C. Franco1, A. Wustrow2, B. Xia1, A. M. Baccarella1, F. Burgos1, J. Nicasio1, E. Dooryhee3, J. R. Neilson2, and J. W. Simonson1,*

  • 1Department of Physics, Farmingdale State College, Farmingdale, New York 11735, USA
  • 2Department of Chemistry, Colorado State University, Fort Collins, Colorado 80523, USA
  • 3National Synchrotron Light Source II, Brookhaven National Laboratory, Upton, New York 11973, USA

  • *jack.simonson@farmingdale.edu

Phys. Rev. Materials 4, 045404 – Published 13 April, 2020

DOI: https://doi.org/10.1103/PhysRevMaterials.4.045404

Abstract

The quasi-one-dimensional structure of Li2Mn2(MoO4)3 consists of three mutually distinct chains of Li1xMnx-centered polyhedra in which Mn ostensibly adopts a J=5/2Mn2+ configuration. In situ x-ray scattering experiments carried out as crystallites emerge from a molten oxide solution facilitate the synthesis of large single crystals. Ex situ x-ray diffraction finds no evidence of long-range Li/Mn occupancy ordering, suggesting that the structure is effectively composed of finite chains of Mn moments of statistically varying lengths. UV/visible diffuse reflectance spectroscopy measurements establish a wide 3.43(12)-eV direct charge gap consistent with the local polyhedral coordination of the nominally Mn2+ species. The temperature T dependence of the DC magnetic susceptibility χ reveals a fluctuating moment of only 2.74μB±0.01μB/Mn, dramatically reduced from the 5.9μB/Mn expected for Mn2+. Meanwhile, the Weiss temperature ΘW=89±1 K reveals antiferromagnetic fluctuations that are stymied from reaching an ordered state apparently by the chemical disorder intrinsic to the polyhedral chains. Measurements of magnetization vs field H at T10 K are far from saturation even at H=5 T and are strongly non-Brillouin-like, instead scaling as H/T0.24(3) and suggesting the presence of quantum fluctuations associated with an eventual quasi-one-dimensional, disordered magnetic phase.

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