Unconventional magnetism in the 4d4 -based S = 1 honeycomb system Ag3 LiRu2 O6

We have investigated the thermodynamic and local magnetic properties of the Mott insulating system Ag3 LiRu2 O6 containing Ru4+ (4d4) for novel magnetism. The material crystallizes in a monoclinic C2/m structure with RuO6 octahedra forming an edge-shared two-dimensional honeycomb lattice with limite...

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Bibliographic Details
Published in:Physical review. B 2019-02, Vol.99 (5), p.054417
Main Authors: Kumar, R, Dey, Tusharkanti, Ette, P M, Ramesha, K, Chakraborty, Atasi, Dasgupta, I, Orain, J C, Baines, C, Tóth, Sándor, Shahee, A, Kundu, S, Prinz-Zwick, M, Gippius, A Gippius, Büttgen, N, Gegenwart, P, Mahajan, A V
Format: Article
Language:English
Subjects:
Antiferromagnetism
Curie temperature
Electron spin
Electronic structure
Freezing
Heat exchange
Honeycomb construction
Long range order
Magnetic permeability
Magnetic properties
Magnetism
Muon spin rotation
NMR
Nuclear magnetic resonance
Spin dynamics
Spin-lattice relaxation
Temperature dependence
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Summary:We have investigated the thermodynamic and local magnetic properties of the Mott insulating system Ag3 LiRu2 O6 containing Ru4+ (4d4) for novel magnetism. The material crystallizes in a monoclinic C2/m structure with RuO6 octahedra forming an edge-shared two-dimensional honeycomb lattice with limited stacking order along the c direction. The large negative Curie-Weiss temperature (θCW = − 57 K) suggests antiferromagnetic interactions among Ru4+ ions, though magnetic susceptibility and heat capacity show no indication of magnetic long-range order down to 1.8 and 0.4 K, respectively. 7Li nuclear magnetic resonance (NMR) shift follows the bulk susceptibility between 120 and 300 K and levels off below 120 K. Together with a power-law behavior in the temperature-dependent spin-lattice relaxation rate between 0.2 and 2 K, it suggest dynamic spin correlations with gapless excitations. Electronic structure calculations suggest an S = 1 description of the Ru moments and the possible importance of further neighbor interactions as well as biquadratic and ring-exchange terms in determining the magnetic properties. Analysis of our muon spin rotation data indicates spin freezing below 5 K, but the spins remain on the borderline between static and dynamic magnetism even at 20 mK.
ISSN:2469-9950
2469-9969
DOI:10.1103/PhysRevB.99.054417