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Exotic magnetism and persistent short-range spin correlations in a frustrated honeycomb lattice antiferromagnet
Authors:
M. Barik,
Q. Faure,
F. Damay,
J. P. Embs,
S. Petit,
P. Khuntia
Abstract:
Two-dimensional high-spin bipartite honeycomb networks, where anisotropy, competing exchange interactions, and spin fluctuations interplay, provide an alternative platform to test theoretical models that distinguish between classical and quantum magnetism in the context of emergent many-body phenomena and exotic excitations. Here, we report the crystal structure, magnetization, specific heat, and…
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Two-dimensional high-spin bipartite honeycomb networks, where anisotropy, competing exchange interactions, and spin fluctuations interplay, provide an alternative platform to test theoretical models that distinguish between classical and quantum magnetism in the context of emergent many-body phenomena and exotic excitations. Here, we report the crystal structure, magnetization, specific heat, and inelastic neutron scattering measurements of the $S = 5/2$ distorted honeycomb magnet $\mathrm{CaZn_2Fe(PO_4)_3}$. Magnetization measurements reveal dominant antiferromagnetic interactions between the $\mathrm{Fe^{3+}}$ ($S = 5/2$) moments. The development and field evolution of a dip in the magnetic susceptibility under an external magnetic field indicate an unconventional field-induced transition, further supported by anomalies observed in magnetization isotherms. Zero-field specific heat measurements show an antiferromagnetic transition at $T_N \approx 1.67 \mathrm{K}$, which evolves under applied magnetic field, suggesting stabilization of a field-induced spin-canted state. Thermodynamic measurements reveal short-range spin correlations above the transition temperature. Inelastic neutron scattering results further corroborate antiferromagnetic ordering, consistent with specific heat data. Spin-wave calculations indicate competing exchange interactions that introduce magnetic frustration, along with weak Ising-like anisotropy. The interplay of competing interactions and anisotropy gives rise to exotic field-induced behavior and places the system in close proximity to a mean-field tricritical point in the $J_2/J_1$--$J_3/J_1$ phase diagram, opening a route to unconventional states in high-spin frustrated honeycomb magnets.
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Submitted 4 May, 2026;
originally announced May 2026.
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Magnetic ground state of a Jeff = 1/2 based frustrated triangular lattice antiferromagnet
Authors:
M. Barik,
J. Khatua,
Suyoung Kim,
Eundeok Mun,
Suheon Lee,
Bassam Hitti,
Gerald D. Morris,
Kwang-Yong Choi,
P. Khuntia
Abstract:
The subtle interplay between competing degrees of freedom, crystal electric fields, and spin correlations can lead to exotic quantum states in 4f ion-based frustrated triangular lattice antiferromagnets. We present the crystal structure, thermodynamic and muon spin relaxation (μSR) studies of the 4f ion-based frustrated magnet Ba4YbReWO12, wherein Yb3+ ions constitute a triangular lattice. The mag…
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The subtle interplay between competing degrees of freedom, crystal electric fields, and spin correlations can lead to exotic quantum states in 4f ion-based frustrated triangular lattice antiferromagnets. We present the crystal structure, thermodynamic and muon spin relaxation (μSR) studies of the 4f ion-based frustrated magnet Ba4YbReWO12, wherein Yb3+ ions constitute a triangular lattice. The magnetic susceptibility does not show any signature of spin freezing down to 1.9 K or long-range magnetic ordering down to 0.4 K. The low-temperature Curie-Weiss fit to the inverse magnetic susceptibility data reveals a weak antiferromagnetic exchange interaction, which is corroborated by the fit of magnetic specific heat data following the J1-J2 model with the nearest neighbor exchange interaction of J1 = -0.197 K between the Jeff = 1/2 states of the Yb3+ moments in the lowest Kramers doublet. The lowest Kramers ground state doublet is well separated from the first excited state with a gap of 278 K, as evidenced by our μSR experiments that support the realization of Jeff = 1/2 at low temperatures. The specific heat experiments do not detect a phase transition down to 56 mK. The magnetic specific heat shows a broad maximum 90 mK suggesting a disordered ground state with short range spin correlations. The associated magnetic entropy release at low temperatures is consistent with that expected for the Jeff = 1/2 state. The zero-field μSR measurements show neither the signature of spin freezing nor a phase transition, at least down to 43 mK. Our results suggest a dynamic, disordered ground state in this Jeff = 1/2 frustrated triangular lattice antiferromagnet. Ba4RReWO12 (R=rare earth) offers a viable platform to realize intriguing quantum states borne out of spin-orbit coupling and frustration
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Submitted 13 January, 2026; v1 submitted 9 April, 2025;
originally announced April 2025.
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A novel Gapless Quantum Spin Liquid in the S = 1 4d4-honeycomb material Cu$_3$LiRu$_2$O$_6$
Authors:
Sanjay Bachhar,
Nashra Pistawala,
S. Kundu,
Maneesha Barik,
M. Baenitz,
Jorg Sichelschmidt,
Koji Yokoyama,
P. Khuntia,
Surjeet Singh,
A. V. Mahajan
Abstract:
We report the discovery of a novel gapless quantum spin liquid in the S=1 honeycomb system Cu$_3$LiRu$_2$O$_6$ with Ru$^{4+}$ ($4d^4$) where moments remain dynamic down to 50 mK. Heat capacity measurements show no sign of magnetic ordering down to 60 mK in spite of a Curie-Weiss temperature = -222 K indicating a strong antiferromagnetic interaction. In zero field, magnetic heat capacity shows a li…
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We report the discovery of a novel gapless quantum spin liquid in the S=1 honeycomb system Cu$_3$LiRu$_2$O$_6$ with Ru$^{4+}$ ($4d^4$) where moments remain dynamic down to 50 mK. Heat capacity measurements show no sign of magnetic ordering down to 60 mK in spite of a Curie-Weiss temperature = -222 K indicating a strong antiferromagnetic interaction. In zero field, magnetic heat capacity shows a linear T-dependence with Sommerfeld coefficient = 107 mJ/mol K$^2$ is much larger than that found in typical Fermi liquids. Our local probe $^7$Li nuclear magnetic resonance (NMR) measurements find a significant temperature-independent $^7$Li NMR shift (and hence a non-zero spin susceptibility) at low-T and a linear T-variation of the $^7$Li NMR spin-lattice relaxation rate 1/T$_1$ at low-T reminiscent of fermionic excitations. Muon spin relaxation measurements detect neither long-range ordering nor spin freezing down to 50 mK and the temperature variation of the muon depolarization rate shows a gradual increase with decreasing temperature and a leveling off below about 1 K evincing a persistent spin dynamics common to several spin liquid candidates. Our results provide strong signatures of a quantum spin liquid in the titled honeycomb material.
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Submitted 28 January, 2025;
originally announced January 2025.
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Possible realization of a randomness-driven quantum disordered state in an S = 1/2 antiferromagnet Sr3CuTa2O9
Authors:
B. Sana,
M. Barik,
S. Lee,
U. Jena,
M. Baenitz,
J. Sichelschmidt,
S. Luther,
H. Kuehne,
K. Sethupathi,
M. S. Ramachandra Rao,
K. Y. Choi,
P. Khuntia
Abstract:
Collective behavior of spins, frustration-induced strong quantum fluctuations, and subtle interplay between competing degrees of freedom in quantum materials can lead to correlated quantum states with exotic excitations that are essential ingredients for establishing paradigmatic models and have immense potential for quantum technologies. Disorder is ubiquitous in real materials, and the detailed…
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Collective behavior of spins, frustration-induced strong quantum fluctuations, and subtle interplay between competing degrees of freedom in quantum materials can lead to correlated quantum states with exotic excitations that are essential ingredients for establishing paradigmatic models and have immense potential for quantum technologies. Disorder is ubiquitous in real materials, and the detailed insights into the role of disorder on the intriguing ground state borne out of quenched randomness provide a route toward the design and discovery of functional quantum materials. Herein, we report magnetization, specific heat, electron spin resonance, and muon spin resonance studies on a 3d-electron-based antiferromagnet Sr3CuTa2O9. The negative Curie- Weiss temperature value, obtained from the Curie-Weiss fit of high-temperature magnetic susceptibility data, indicates antiferromagnetic interaction between Cu2+ moments. Specific heat data show the absence of long-range magnetic ordering down to 64 mK despite a reasonably strong exchange interaction between Cu2+ (S =1/2) spins as reflected from a Curie-Weiss temperature of -27 K. The power-law behavior and the data collapse of specific heat and magnetization data evince the emergence of a random-singlet state in Sr3CuTa2O9. The power-law-like spin auto-correlation function and the data collapse of muon polarization asymmetry with longitudinal field dependence of t(μ0H)^γ further support credence to the presence of a randomness-induced quantum disordered state. Our results suggest that randomness induced by disorder is an alternate route to realize a quantum disordered state in this antiferromagnet.
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Submitted 25 September, 2024; v1 submitted 25 April, 2023;
originally announced April 2023.
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Magnetic properties of a spin-orbit entangled Jeff=1/2 three-dimensional frustrated rare-earth hyperkagome
Authors:
B. Sana,
M. Barik,
M. Pregelj,
U. Jena,
M. Baenitz,
J. Sichelschmidt,
K. Sethupathi,
P. Khuntia
Abstract:
The interplay between competing degrees of freedom can stabilize non-trivial magnetic states in correlated electron materials. Frustration-induced strong quantum fluctuations can evade long-range magnetic ordering leading to exotic quantum states such as spin liquids in two-dimensional spin-lattices such as triangular and kagome structures. However, the experimental realization of dynamic and corr…
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The interplay between competing degrees of freedom can stabilize non-trivial magnetic states in correlated electron materials. Frustration-induced strong quantum fluctuations can evade long-range magnetic ordering leading to exotic quantum states such as spin liquids in two-dimensional spin-lattices such as triangular and kagome structures. However, the experimental realization of dynamic and correlated quantum states is rare in three-dimensional (3D) frustrated magnets wherein quantum fluctuations are less prominent. Herein, we report the crystal structure, magnetic susceptibility, electron spin resonance (ESR) and specific heat studies accompanied by crystal electric field (CEF) calculations on a 3D frustrated magnet Yb3Sc2Ga3O12. In this material, Yb3+ ions form a three-dimensional network of corner-sharing triangles known as hyperkagome lattice without any detectable anti-site disorder. Our results reveal a low energy state with Jeff = 1/2 degrees of freedom in the Kramers doublet state. The zero field-cooled and field cooled magnetic susceptibility taken in 0.001 T rules out the presence of spin-freezing down to 1.8K. The Curie-Weiss (CW) fit to low-T susceptibility data yields a small and negative CW temperature indicating the presence of a weak antiferromagnetic interaction between Jeff = 1/2 (Yb3+) moments. The Yb-ESR displays a broad line of non-Lorentzian shape that suggests considerable magnetic anisotropy in Yb3Sc2Ga3O12. The CEF calculations suggest that the ground state is well separated from the excited states, which are in good agreement with experimental results. The absence of long-range magnetic ordering indicates a dynamic liquid-like ground state at least down to 130 mK. Furthermore, zero field specific heat shows a broad maximum around 200 mK suggesting the presence of short-range spin correlations in this 3D frustrated antiferromagnet.
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Submitted 26 August, 2023; v1 submitted 14 April, 2023;
originally announced April 2023.
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Pressure induced semiconductor to metal phase transition in CsSnBr3 perovskite
Authors:
Md. Sajib Hossain,
Md. Majibul Haque Babu,
Tusar Saha,
Md. Sazzad Hossain,
Jiban Podder,
Md. Shohel Rana,
Md. Abdul Barik,
Protima Rani
Abstract:
Phase transitions in metal halide perovskites triggered by external provocations produce significantly different material properties, providing a prodigious opportunity for a comprehensive applications. In the present study, the first principles calculation has been performed with the help of density functional theory (DFT) using CASTEP code to investigate the physical properties of lead-free CsSn…
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Phase transitions in metal halide perovskites triggered by external provocations produce significantly different material properties, providing a prodigious opportunity for a comprehensive applications. In the present study, the first principles calculation has been performed with the help of density functional theory (DFT) using CASTEP code to investigate the physical properties of lead-free CsSnBr3 metal halide under various hydrostatic pressures. The pressure effect is determined in the range of 0-16 GPa. Subsequently, a significant change is observed in lattice constant and volume with increasing pressure. The electronic band structure show semiconductor to metal phase transition under elevated pressure. The investigation of optical functions displays that the absorption edge of CsSnBr3 perovskite is shifted remarkably toward the low energy region (red shift) with improved pressure up to 16 GPa. In addition, the absorptivity and dielectric constant also upsurges with the applied hydrostatic pressure. Finally, the mechanical properties reveal that CsSnBr3 perovskite is mechanically stable and highly ductile; the ductility is increased with raising pressure. This type of semiconductor to metal phase transition may inspire a wide range of potential applications.
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Submitted 10 February, 2021; v1 submitted 5 February, 2021;
originally announced February 2021.