Unconventional magnetism in the 
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-based 
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 honeycomb system 
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Kumar, Rakesh; Dey, Tusharkanti; Ramesha, K.; Chakraborty, Atasi; Dasgupta, Indra; Orain, Jean-Christophe; Baines, C.; Tóth, S.; Shahee, Aga; Kundu, Sumit; Prinz-Zwick, M.; Gippius, A. A.; Büttgen, N.; Gegenwart, P.; Mahajan, A. V.

doi:10.1103/physrevb.99.054417

Cited by 19 publications

(15 citation statements)

References 54 publications

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“…But the expected long-range ordered state was not seen in spite of the apparently unfrustrated geometry of the honeycomb lattice. Rather, the local moments were found to be on the borderline of being dynamic and static at low temperatures, based on muon spin relaxation (μSR) data [23]. Such behavior is likely driven by higher order biquadratic or ring exchange terms in the Hamiltonian over and above the usual Heisenberg couplings.…”

Section: Introductionmentioning

confidence: 99%

Unusual spin dynamics in the low-temperature magnetically ordered state of Ag3LiIr2O6

et al. 2021

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Recently, there have been contrary claims of Kitaev spin-liquid behavior and ordered behavior in the honeycomb compound Ag 3 LiIr 2 O 6 based on various experimental signatures. Our investigations on this system reveal a low-temperature ordered state with persistent dynamics down to the lowest temperatures. Magnetic order is confirmed by clear oscillations in the muon spin relaxation (μSR) time spectrum below 9 K until 52 mK. Coincidentally in 7 Li nuclear magnetic resonance, a wipeout of the signal is observed below ∼10 K, which again strongly indicates magnetic order in the low-temperature regime. This is supported by our density functional theory calculations which show an appreciable Heisenberg exchange term in the spin Hamiltonian that favors magnetic ordering. The 7 Li shift and spin-lattice relaxation rate also show anomalies at ∼50 K. They are likely related to the onset of dynamic magnetic correlations, but their origin is not completely clear. Detailed analysis of our μSR data is consistent with a coexistence of incommensurate Néel and striped environments. A significant and undiminished dynamical relaxation rate (∼5 MHz) as seen in μSR deep into the ordered phase indicates enhanced quantum fluctuations in the ordered state.

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Section: Introductionmentioning

confidence: 99%

Unusual spin dynamics in the low-temperature magnetically ordered state of Ag3LiIr2O6

et al. 2021

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“…Surprisingly, the asymmetry in spectra was also seen in the isostructural material Ag 3 LiRu 2 O 6 [Ref. [9]]. Interestingly, the hydrogenated analogue of Ag 3 LiIr 2 O 6 , i.e.…”

Section: E Nmr Resultsmentioning

confidence: 99%

Structural, thermodynamic, and local probe investigations of the honeycomb material Ag3LiMn2O6

et al. 2019

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Here we present the structural and magnetic properties of a new honeycomb material Ag3LiMn2O6. The system Ag[Li 1/3 Mn 2/3 ]O2 belongs to a quaternary 3R-delafossite family and crystallizes in a monoclinic symmetry with space group C 2/m and the magnetic Mn 4+ (S = 3/2) ions form a honeycomb network in the ab-plane. An anomaly around 50 K and the presence of antiferromagnetic (AFM) coupling (Curie-Weiss temperature θCW ∼ −51 K) were inferred from our magnetic susceptibility data. The magnetic specific heat clearly manifests the onset of magnetic ordering in the vicinity of 48 K and the recovered magnetic entropy, above the ordering temperature, falls short of the expected value, implying the presence of short-range magnetic correlations. An asymmetric Bragg peak (characteristic of two dimensional order), seen in neutron diffraction, gains intensity even above the ordering temperature, thus showing the existence of short-range spin correlations. Our electron spin resonance ESR experiments corroborate the bulk magnetic data. Additionally, the (ESR) line broadening on approaching the ordering temperature T N could be described in terms of a Berezinski-Kosterlitz-Thouless (BKT) scenario with T KT = 40(1) K. 7 Li NMR line-shift probed as a function of temperature tracks the static susceptibility (Kiso) of magnetically coupled Mn 4+ ions. The 7 Li spin-lattice relaxation rate (1/T 1) exhibits a sharp decrease below about 50 K. A critical divergence is absent at the ordering temperature perhaps because of the filtering out of the antiferromagnetic fluctuations at the Li site, i.e., at the centers of the hexagons in the honeycomb network. Combining our bulk and local probe measurements, we establish the presence of an ordered ground state for the honeycomb system Ag3LiMn2O6. Our ab initio electronic structure calculations suggest that in the ab-plane, the nearest neighbor (NN) exchange interaction is strong and AFM, while the next NN and the third NN exchange interactions are FM and AFM respectively. The interplanar exchange interaction is found to be relatively small. In the absence of any frustration the system is expected to exhibit long-range, AFM order, in agreement with experiment. arXiv:1903.08366v2 [cond-mat.str-el]

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“…But the expected long-range ordered state was not seen in spite of the apparently unfrustrated geometry of the honeycomb lattice. Rather, the local moments were found to be on the borderline of being dynamic and static at low temperatures, based on muon spin relaxation (µSR) data [23]. Such behavior is likely driven by higher order bi-quadratic or ring exchange terms in the Hamiltonian over and above the usual Heisenberg couplings.…”

Section: Introductionmentioning

confidence: 99%

Unusual spin dynamics in the low-temperature magnetically ordered state of Ag$_{3}$LiIr$_{2}$O$_{6}$

Chakraborty,

Kumar,

Bachhar

et al. 2021

Preprint

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Recently, there have been contrary claims of Kitaev spin-liquid behaviour and ordered behavior in the honeycomb compound Ag3LiIr2O6 based on various experimental signatures. Our investigations on this system reveal a low-temperature ordered state with persistent dynamics down to the lowest temperatures. Magnetic order is confirmed by clear oscillations in the muon spin relaxation (µSR) time spectrum below 9 K till 52 mK. Coincidentally in 7 Li nuclear magnetic resonance, a wipe-out of the signal is observed below ∼ 10 K which again strongly indicates magnetic order in the low temperature regime. This is supported by our density functional theory calculations which show an appreciable Heisenberg exchange term in the spin Hamiltonian that favors magnetic ordering. The 7 Li shift and spin-lattice relaxation rate also show anomalies at ∼ 50 K. They are likely related to the onset of dynamic magnetic correlations, but their origin is not completely clear. Detailed analysis of our µSR data is consistent with a co-existence of incommensurate Néel and striped environments. A significant and undiminished dynamical relaxation rate (∼ 5 MHz) as seen in µSR deep into the ordered phase indicates enhanced quantum fluctuations in the ordered state.

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

Cited by 19 publications

References 54 publications

Unusual spin dynamics in the low-temperature magnetically ordered state of Ag3LiIr2O6

Unusual spin dynamics in the low-temperature magnetically ordered state of Ag3LiIr2O6

Structural, thermodynamic, and local probe investigations of the honeycomb material Ag3LiMn2O6

Unusual spin dynamics in the low-temperature magnetically ordered state of Ag$_{3}$LiIr$_{2}$O$_{6}$

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