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K. M. Ranjith

Publications and source records attributed to K. M. Ranjith.

At least 19 recordsLinked to original sources

Microscopic NMR evidence for successive antiferroelectric and antiferromagnetic order in the van der Waals magnet CuCrP$_2$S$_6$

We present a comprehensive $^{31}$P and $^{65}$Cu nuclear magnetic resonance (NMR) study of the layered van der Waals magnet CuCrP$_2$S$_6$. The compound exhibits a sequence of structural and magnetic phase transitions: a high-temperature paraelectric state, followed by a quasi-antiferroelectric (QAFE) state near 185 K, a long-range antiferroelectric (AFE) phase below 150 K, and finally, antiferromagnetic (AFM) order below $T_\mathrm{N}$ = 30 K. The evolution of the NMR spectra, NMR shift, and spin-lattice ($T_1^{-1}$) and spin-spin ($T_2^{-1}$) relaxation rates provide direct microscopic fingerprints of these transitions. The splitting of both the NMR line and $T_1^{-1}$ below the AFE transition demonstrates the emergence of two inequivalent P sites. From $K - χ$ analysis, we extract nearly isotropic transferred hyperfine couplings and show that the NMR shift anisotropy originates primarily from the dipolar contribution, in contrast to Mn$_2$P$_2$S$_6$ and Ni$_2$P$_2$S$_6$. We determine the ferromagnetic intralayer exchange $J_{intra}\approx$ -4.9 K from the Curie Weiss temperature, consistent with ferromagnetic layers antiferromagnetically stacked along the $c$ axis, and evaluate the Moriya high temperature relaxation rate including cross correlation effects of the P P dimer. Critical divergence of $T_1^{-1}$ near $T_\mathrm{N}$ yields a critical exponent $γ\simeq$ 0.45(4), placing CuCrP$_2$S$_6$ in a three dimensional Heisenberg universality regime.

cond-mat.str-el

Critical Berezinskii-Kosterlitz-Thouless dynamics in the archetypal two-dimensional spin system Ba$_2$CuSi$_2$O$_6$Cl$_2$

We study the spin dynamics in the quasi-2D spin-$1/2$ dimer compound Ba$_2$CuSi$_2$O$_6$Cl$_2$, which exhibits a magnetic field-induced Bose-Einstein condensate (BEC) of triplons. Using nuclear magnetic resonance spin-lattice relaxation rate ($T_1^{-1}$) measurements combined with large-scale quantum Monte Carlo (QMC) simulations, we investigate critical fluctuations across the field-temperature phase diagram. Bridging the behavior observed in 1D and 3D systems, the $T_1^{-1}$ relaxation rate shows a pronounced peak extending well above the Néel temperature $T_N$, indicating strong two-dimensional Berezinskii-Kosterlitz-Thouless (BKT)-type fluctuations. A quantitative match between experimental and theoretical BEC phase boundaries validates an effective XXZ model. The study determines the intrinsic BKT transition temperature $T_{\mathrm{BKT}}$ from QMC, revealing a nearly field-independent $T_{\mathrm{BKT}}/T_N \approx 0.74$. Scaling analysis of the relaxation rate shows critical exponents consistent with 2D universality, and a narrow temperature window is identified where 2D physics dominates. These findings establish Ba$_2$CuSi$_2$O$_6$Cl$_2$ as a model system for exploring BKT dynamics in quantum magnets.

cond-mat.str-el

Disorder-driven coexistence of distinct dynamical states in frustrated Sr$_3$CuNb$_2$O$_9$: a microscopic $μ$SR and $^{93}$Nb NMR study

Despite recent progress in identifying the exotic random singlet (RS) state in disordered frustrated magnets as a distinct correlated phase, three-dimensional (3D) realizations remain scarce. Sr$_3$CuNb$_2$O$_9$ was proposed to be one of such 3D frustrated systems with magnetic site disorder hosting an RS ground state. Here, we report a detailed microscopic investigation of Sr$_3$CuNb$_2$O$_9$ employing muon spin relaxation ($μ$SR) and $^{93}$Nb nuclear magnetic resonance (NMR) techniques. The $μ$SR zero-field relaxation rate reveals a power-law divergence of the relaxation rate as a function of temperature. Also, a power-law divergence is present in the relaxation rate as a function of applied longitudinal field, consistent with the formation of an RS phase. The $^{93}$Nb NMR spectra unambiguously resolve two components with distinct local magnetic environments, whose nature is further elucidated through spin-lattice relaxation measurements analyzed via an inverse Laplace transform (ILT) of the nuclear magnetization recovery. The relaxation-rate distribution obtained from ILT reveals two well-separated channels: a fast component, $(1/T_1)_{\mathrm{fast}}$, and a slow component, $(1/T_1)_{\mathrm{slow}}$. Both components follow distinct power-law temperature dependences ($T^α$), with $α= 0.6$ and $1.1$ for the fast and slow channels, respectively. The combined spectral and relaxation data demonstrate that the fast channel qualitatively represents an RS-like state, whereas the slow channel exhibits quantum spin liquid (QSL) like behavior, thereby establishing the microscopic coexistence of RS and QSL-like phases in Sr$_3$CuNb$_2$O$_9$.

cond-mat.str-el

Magnetic anisotropy and dipolar interactions in the frustrated triangular-lattice magnet NaGdS_2

In this comprehensive study, we present results of bulk measurements (magnetization, specific heat, ac susceptibility, thermal expansion, and magnetostriction) combined with local methods such as nuclear magnetic resonance (^23Na NMR) and electron spin resonance (ESR) and simulations (McPhase) on polycrystalline and single-crystalline NaGdS_2 samples. The rare-earth delafossite NaGdS_2 is a triangular-lattice magnet with S = 7/2 spin-only Gd^3+ moments with suppressed single-ion anisotropy. In our study, we estimate that NaGdS_2 has a weak antiferromagnetic exchange (J_H/k_B is about 52mK) and signs of long-range magnetic order are absent down to lowest temperature. However, indications of short range magnetic order are found below 180 mK in the ac susceptibility and thermal expansion. Our results indicate an interplay of Heisenberg-type and dipolar exchange. Due to the large moment of the Gd^3+ ions, one expects a strong impact of the dipolar coupling in NaGdS_2, in contrast to the related NaYbS_2. ESR and ^23Na NMR measurements, indeed, indicate the formation of short-range ferromagnetic correlations. NaGdS_2 appears to be a rare system, in which magnetic order is suppressed by a competition between Heisenberg and dipolar interactions.

cond-mat.str-el

Ground state properties of a spin-$\frac{5}{2}$ frustrated triangular lattice antiferromagnet NH$_{4}$Fe(PO$_{3}$F)$_2$

Structural and magnetic properties of a two-dimensional spin-$\frac{5}{2}$ frustrated triangular lattice antiferromagnet NH$_{4}$Fe(PO$_{3}$F)$_2$ are explored via x-ray diffraction, magnetic susceptibility, high-field magnetization, heat capacity, and $^{31}$P nuclear magnetic resonance experiments on a polycrystalline sample. The compound portrays distorted triangular units of the Fe$^{3+}$ ions with anisotropic bond lengths. The magnetic susceptibility shows a broad maxima around $T^{\rm{max}}_χ\simeq 12$ K, mimicking the short-range antiferromagnetic order of a low-dimensional spin system. The magnetic susceptibility and NMR shift could be modeled assuming the spin-$5/2$ isotropic triangular lattice model and the average value of the exchange coupling is estimated to be $J/k_{\rm B} \simeq 1.7$ K. This value of the exchange coupling is reproduced well from the saturation field of the pulse field data. It shows the onset of a magnetic ordering at $T_{\rm N} \simeq 5.7$ K, setting the frustration ratio of $f = \frac{|θ_{\rm CW}|}{T_{\rm N}} \simeq 5.7$. Such a value of $f$ reflects moderate magnetic frustration in the compound. The d$M$/d$H$ vs $H$ plots of the low temperature magnetic isotherms exhibit a sharp peak at $H_{\rm SF} \simeq 1.45$ T, suggesting a field-induced spin-flop transition and magnetic anisotropy. The rectangular shape of the $^{31}$P NMR spectra below $T_{\rm N}$ unfolds that the ordering is commensurate antiferromagnet type. Three distinct phase regimes are clearly discerned in the $H - T$ phase diagram, redolent of a frustrated magnet with in-plane (XY-type) anisotropy.

cond-mat.mtrl-sci

Anisotropic magnetism and spin fluctuations in the triangular-lattice spin-liquid candidate NaYbSe$_2$: a single-crystal $^{23}$Na and $^{77}$Se NMR study

The ytterbium-based delafossite NaYbSe$_2$ is discussed as a prototype for a spin-orbit entangled, effective spin-1/2 triangular spin lattice with emerging antiferromagnetic correlations and a quantum-spin-liquid (QSL) ground state. We report on a comprehensive study of the static and dynamic anisotropic magnetism in single-crystalline samples of NaYbSe$_2$, using NMR spectroscopy as a local-probe technique. We performed $^{23}$Na and $^{77}$Se NMR measurements in magnetic fields up to 16 T, applied along the in-plane and out-of-plane crystallographic directions and at temperatures from 300 down to 0.3 K. We could determine the anisotropic hyperfine contributions from the angular dependence of the $^{23}$Na and $^{77}$Se NMR spectra. In the paramagnetic regime, we probed the temperature dependence of the $^{23}$Na and $^{77}$Se spectral shift and the hyperfine coupling constants for fields applied along the principal crystal axes. The spin-lattice relaxation-rate data indicate critical spin fluctuations and the absence of long-range magnetic order at low magnetic fields and temperatures down to 0.3 K, evidenced by a monotonic increase of $1/T_1$ and associated spectral broadening. This is a clear proof of the evolution of a critical QSL ground state with residual fluctuations down to lowest temperatures. At elevated fields, we observe the emergence of long-range order, as the temperature-dependent $1/T_1$ rate passes through a pronounced maximum at $T_N$ at given field, followed by a decrease at lower temperatures. Further, we find an inhomogeneous broadening of the $^{23}$Na spectra below $T_N$, probing the histogram of the local-field distribution in the presence of the field-induced order.

cond-mat.str-el

Static and Dynamic Electronic Properties of Weyl Semimetal NbP -- A Single Crystal $^{93}$Nb-NMR Study

Nuclear magnetic resonance (NMR) techniques have been used to study the static and dynamic microscopic properties of the Weyl semimetal NbP. From a complete analysis of the angular dependence of the $^{93}$Nb-NMR spectra in a single crystal, the parameters for the electric quadrupole interactions and the magnetic hyperfine interactions were determined to be $ν_{\rm Q} = 0.61$\,MHz, $η= 0.20$, $(K_{XX}, K_{YY}, K_{ZZ}) = (- 0.06, 0.11, - 0.11)$\% at 4.5\,K. The temperature and field dependence of the $^{93}$Nb Knight shift revealed a characteristic feature of the shape of the density of states with nearly massless fermions. We clearly observed a quantum oscillation of the Knight shift associated with the band structure, whose frequency was in good agreement with the previous bulk measurements. The temperature dependence of the spin-lattice relaxation rate, $1 / T_{1} T$, showed an almost constant behavior for $30 < T < 180$\,K, while a weak temperature dependence was observed below $\sim 30$\,K. This contrasts with the behavior observed in TaP and TaAs, where the $1 / T_{1} T$ measured by the $^{181}$Ta nuclear quadrupole resonance (NQR) shows $1 / T_{1} T \propto T^{2}$ and $T^{4}$ above approximately 30\,K. In TaP, the temperature dependent orbital hyperfine interaction plays a signficant role in nuclear relaxation, whereas this contribution is not observed in TaAs. Two-component spin echo oscillations were observed. The shorter-period oscillation is attributed to the origin of quadrupole coupling, while the longer-period oscillation indicates the presence of indirect nuclear spin-spin coupling, as discussed in other Weyl semimetal like TaP.

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Narrowly avoided spin-nematic phase in BaCdVO(PO$_4$)$_2$: NMR evidence

We present a $^{31}$P nuclear magnetic resonance (NMR) investigation of BaCdVO(PO$_4$)$_2$ focusing on the nearly saturated regime between $μ_0H_{c1}$ = 4.05 T and $μ_0H_{c2}$ = 6.5 T, which used to be considered a promising candidate for a spin-nematic phase. NMR spectra establish the absence of any dipolar order there, whereas the weak field dependence of the magnetization above $H_{c1}$ is accounted for by Dzyaloshinskii-Moriya interaction terms. The low-energy spin dynamics (fluctuations), measured by the nuclear spin-lattice relaxation rate $T_1^{-1}$, confirms the continuity of this phase and the absence of any low-temperature phase transition. Unexpectedly, the spin dynamics above $H_{c1}$ is largely dominated by two-magnon processes, which is expected above the saturation field of a spin-nematic phase, but not inside. This shows that BaCdVO(PO$_4$)$_2$ is indeed close to a spin-nematic instability; however, this phase is not stabilized. We thus confirm recent theoretical predictions that the spin-nematic phase can be stabilized, at most, in an extremely narrow field range close to saturation or is rather narrowly avoided [Jiang et al., Phys. Rev. Lett. 130, 116701 (2023)].

cond-mat.str-el

Repulsive Tomonaga-Luttinger Liquid in Quasi-one-dimensional Alternating Spin-$1/2$ Antiferromagnet NaVOPO$_4$

We probe the magnetic field-induced Tomonaga-Luttinger liquid (TLL) state in the bond-alternating spin-$1/2$ antiferromagnetic (AFM) chain compound NaVOPO$_4$ using thermodynamic as well as local $μ$SR and $^{31}$P NMR probes down to milli-K temperatures in magnetic fields up to 14~T. The $μ$SR and NMR relaxation rates in the gapless TLL regime decay slowly following characteristic power-law behaviour, enabling us to directly determine the interaction parameter $K$ as a function of the magnetic field. These estimates are cross-checked using magnetization and specific heat data. The field-dependent $K$ lies in the range of $0.4 < K < 1$ and indicates repulsive nature of interactions between the spinless fermions, in line with the theoretical predictions. This renders NaVOPO$_4$ the first experimental realization of TLL with repulsive fermionic interactions in hitherto studied $S=1/2$ bond-alternating AFM-AFM chain compounds.

cond-mat.str-el

Adiabatic demagnetization refrigeration to mK temperatures with the distorted square lattice magnet NaYbGeO$_{4}$

We report the synthesis, characterization, low-temperature magnetic, and thermodynamic measurements of the novel milli-Kelvin adiabatic demagnetization refrigeration (mK-ADR) candidate material NaYbGeO$_4$ which exhibits a distorted square lattice arrangement of YbO$_{6}$ magnetic units. Magnetization and specific heat indicate weakly interacting effective spin-1/2 moments below 10~K, with a Curie-Weiss temperature of only 15~mK, that can be polarized by magnetic fields of order 1~T. For the ADR performance test, we start the demagnetization from 5~T at a temperature of $\sim 2$~K and reach a minimum temperature of 150~mK at zero field. The warming curve indicates a sharp magnetic transition in the heat capacity at 210~mK, implying only weak magnetic frustration. The entropy density of $S_{\rm GS}\simeq 101$ mJ K$ ^{-1}$cm$^{-3}$ and hold time below 2~K of 220~min are competitive while the minimal temperature is higher compared to frustrated Ytterbium-oxide ADR materials studied under similar conditions.

cond-mat.str-el

Efficient adiabatic demagnetization refrigeration to below 50 mK with UHV compatible Ytterbium diphosphates $A$YbP$_2$O$_7$ ($A=$Na, K)

Attaining milli-Kelvin temperatures is often a prerequisite for the study of novel quantum phenomena and the operation of quantum devices. Adiabatic demagnetization refrigeration (ADR) is an effective, easy and sustainable alternative to evaporation or dilution cooling with the rare and super-expensive $^3$He. Paramagnetic salts, traditionally used for mK-ADR, suffer from chemical instability related to water of crystallization. We report synthesis, characterization as well as low-temperature magnetization and specific heat measurements of two new UHV compatible candidate materials NaYbP$_2$O$_7$ and KYbP$_2$O$_7$. Utilizing the PPMS at 2 K, the ADR of sintered pellets with Ag powder admixture starting at 5 T yields base temperatures (warm-up times) of 45 mK (55 min) and 37 mK (35 min) for NaYbP$_2$O$_7$ and KYbP$_2$O$_7$, respectively, slightly advantageous to KBaYb(BO$_3$)$_2$ (45 mK and 40 min) studied under similar conditions.

cond-mat.mtrl-sci

Structural 130-K Phase Transition and Emergence of a Two-Ion Kondo State in HT-Ce$_2$Rh$_2$Ga Explored by $^{69,71}$Ga Nuclear Quadrupole Resonance

We have studied the microscopic magnetic properties, the nature of the 130-K phase transition, and the ground state in the recently synthesized compound Ce$_2$Rh$_2$Ga by use of $^{69,71}$Ga nuclear quadrupole resonance (NQR). The NQR spectra clearly show an unusual phase transition at $T_t$ $\sim$ 130 K yielding a splitting of the high-temperature single NQR line into two clearly resolved NQR lines, providing evidence for two crystallographically inequivalent Ga sites. The NQR frequencies are in good agreement with fully-relativistic calculations of the band structure. Our NQR results indicate the absence of magnetic or charge order down to 0.3 K. The temperature dependence of the spin-lattice relaxation rate, 1/$T_1$, shows three distinct regimes, with onset temperatures at $T_t$ and 2 K. The temperature-independent 1/$T_1$, observed between $T_t$ and 2 K, crosses over to a Korringa process, 1/$T_1$ $\propto$ $T$, below $\sim$ 2 K, which evidences a rare two-ion Kondo scenario: the system goes into a dense Kondo coherent state at 2.0 and 0.8 K for the two different Ga sites.

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NMR evidence against a spin-nematic nature of the presaturation phase in the frustrated magnet SrZnVO(PO4)2

Using $^{31}$P nuclear magnetic resonance (NMR) we investigate the recently discovered presaturation phase in the highly frustrated two-dimensional spin system SrZnVO(PO$_4$)$_2$ [F. Landolt et al., Phys. Rev. B 104, 224435 (2021)]. Our data provide two pieces of evidence against the presumed spin-nematic character of this phase: i) NMR spectra reveal that it hosts a dipolar spin order and ii) the 1/$T_1$ relaxation rate data recorded above the saturation field can be fitted by the sum of a single-magnon term, exponential in the gap, and a critical second-order term, exponential in the triple gap, leaving no space for a nematic spin dynamics, characterized by a double-gap exponential. We explain the unexpectedly broad validity of the simple fit and the related critical spin dynamics.

cond-mat.str-el

Quantum magnetism of ferromagnetic spin dimers in $α$-KVOPO$_4$

Magnetism of the spin-$\frac12$ $α$-KVOPO$_4$ is studied by thermodynamic measurements, $^{31}$P nuclear magnetic resonance (NMR), neutron diffraction, and density-functional band-structure calculations. Ferromagnetic Curie-Weiss temperature of $θ_{\rm CW}\simeq 15.9$ K and the saturation field of $μ_0H_s\simeq 11.3$ T suggest the predominant ferromagnetic coupling augmented by a weaker antiferromagnetic exchange that leads to a short-range order below 5 K and the long-range antiferromagnetic order below $T_{\rm N}\simeq 2.7$ K in zero field. Magnetic structure with the propagation vector $\mathbf k=(0,\frac12,0)$ and the ordered magnetic moment of 0.58 $μ_B$ at 1.5 K exposes a non-trivial spin lattice where strong ferromagnetic dimers are coupled antiferromagnetically. The reduction in the ordered magnetic moment with respect to the classical value (1 $μ_{\rm B}$) indicates sizable quantum fluctuations in this setting, despite the predominance of ferromagnetic exchange. We interpret this tendency toward ferromagnetism as arising from the effective orbital order in the folded chains of the VO$_6$ octahedra.

cond-mat.mtrl-sci

The planar triangular $S=3/2$ magnet AgCrSe$_2$: magnetic frustration, short range correlations, and field tuned anisotropic cycloidal magnetic order

Our studies evidence an anisotropic magnetic order below $T_N = 32$~K. Susceptibility data in small fields of about 1~T reveal an antiferromagnetic (AFM) order for $H \perp c$, whereas for $H \parallel c$ the data are reminiscent of a field-induced ferromagnetic (FM) structure. At low temperatures and for $H \perp c$, the field-dependent magnetization and AC susceptibility data evidence a metamagnetic transition at $H^+ = 5$~T, which is absent for $H \parallel c$. We assign this to a transition from a planar cycloidal spin structure at low fields to a planar fan-like arrangement above $H^+$. A fully FM polarized state is obtained above the saturation field of $H_{\perp S} = 23.7$~T at 2~K with a magnetization of $M_s = 2.8$~$μ_{\rm B}{\rm /Cr}$. For $H \parallel c$, $M(H)$ monotonously increases and saturates at the same $M_s$ value at $H_{\parallel S} = 25.1$~T at 4.2~K. Above $T_N $, the magnetic susceptibility and specific heat indicate signatures of two dimensional (2D) frustration related to the presence of planar ferromagnetic and antiferromagnetic exchange interactions. We found a pronounced nearly isotropic maximum in both properties at about $T^* = 45$~K, which is a clear fingerprint of short-range correlations and emergent spin fluctuations. Calculations based on a planar 2D Heisenberg model support our experimental findings and suggest a predominant FM exchange among nearest and AFM exchange among third-nearest neighbors. Only a minor contribution might be assigned to the antisymmetric Dzyaloshinskii-Moriya interaction possible related to the non-centrosymmetric polar space group $R3m$. Due to these competing interactions, the magnetism in AgCrSe$_{2}$, in contrast to the oxygen based delafossites, can be tuned by relatively small, experimentally accessible, magnetic fields, allowing us to establish the complete anisotropic magnetic $H-T$ phase diagram in detail.

cond-mat.str-el

Yb delafossites: unique exchange frustration of 4f spin 1/2 moments on a perfect triangular lattice

While the Heisenberg model for magnetic Mott insulators on planar lattice structures is comparatively well understood in the case of transition metal ions, the intrinsic spin-orbit entanglement of 4f magnetic ions on such lattices shows fascinating new physics largely due to corresponding strong anisotropies both in their single-ion and their exchange properties. We show here that the Yb delafossites, containing perfect magnetic Yb$^{3+}$ triangular lattice planes with pseudospin $s=1/2$ at low temperatures, are an ideal platform to study these new phenomena. Competing frustrated interactions may lead to an absence of magnetic order associated to a gapless spin liquid ground state with a huge linear specific heat exceeding that of many heavy fermions, whereas the application of a magnetic field induces anisotropic magnetic order with successive transitions into different long ranged ordered structures. In this comparative study, we discuss our experimental findings in terms of a unified crystal-field and exchange model. We combine electron paramagnetic resonance (EPR) experiments and results from neutron scattering with measurements of the magnetic susceptibility, isothermal magnetization up to full polarization, and specific heat to determine the relevant model parameters. The impact of the crystal field is discussed as well as the symmetry-compatible form of the exchange tensor, and we give explicit expressions for the anisotropic g factor, the temperature dependence of the susceptibility, the exchange-narrowed EPR linewidth and the saturation field.

cond-mat.str-el

Gapless quantum spin liquid in the triangular system Sr$_{3}$CuSb$_{2}$O$_{9}$

We report gapless quantum spin liquid behavior in the layered triangular Sr$_{3}$CuSb$_{2}$O$_{9}$ (SCSO) system. X-ray diffraction shows superlattice reflections associated with atomic site ordering into triangular Cu planes well-separated by Sb planes. Muon spin relaxation ($μ$SR) measurements show that the $S = \frac{1}{2}$ moments at the magnetically active Cu sites remain dynamic down to 65 mK in spite of a large antiferromagnetic exchange scale evidenced by a large Curie-Weiss temperature $θ_{\mathrm{cw}} \simeq $ -143 K as extracted from the bulk susceptibility. Specific heat measurements also show no sign of long-range order down to 0.35 K. The magnetic specific heat ($\mathit{C}$$_{\mathrm{m}}$) below 5 K reveals a $\mathit{C}$$_{\mathrm{m}}$ $=$ $γT$ + $αT$$^{2}$ behavior. The significant $T$$^{2}$ contribution to the magnetic specific heat invites a phenomenology in terms of the so-called Dirac spinon excitations with a linear dispersion. From the low-$T$ specific heat data, we estimate the dominant exchange scale to be $\sim $ 36 K using a Dirac spin liquid ansatz which is not far from the values inferred from microscopic density functional theory calculations ($\sim $ 45 K) as well as high-temperature susceptibility analysis ($\sim$ 70 K). The linear specific heat coefficient is about 18 mJ/mol-K$^2$ which is somewhat larger than for typical Fermi liquids.

cond-mat.str-el

Two types of alternating spin-$\frac12$ chains and their field-induced transitions in $\varepsilon$-LiVOPO$_4$

Thermodynamic properties, $^{31}$P nuclear magnetic resonance (NMR) measurements, and density-functional band-structure calculations for $\varepsilon$-LiVOPO$_4$ are reported. This quantum magnet features a singlet ground state and comprises two types of alternating spin-$\frac12$ chains that manifest themselves by the double maxima in the susceptibility and magnetic specific heat, and by the two-step magnetization process with an intermediate $\frac12$-plateau. From thermodynamic data and band-structure calculations, we estimate the leading couplings of $J_1\simeq 20$ K and $J_2\simeq 60$ K and the alternation ratios of $α_1=J_1'/J_1\simeq 0.6$ and $α_2=J_2'/J_2\simeq 0.3$ within the two chains, respectively. The zero-field spin gap $Δ_0/k_{\rm B}\simeq 7.3$ K probed by thermodynamic and NMR measurements is caused by the $J_1$-$J_1'$ spin chains and can be closed in the applied field of $μ_{0}H_{\rm c1}\simeq 5.6$ T, giving rise to a field-induced long-range order. The NMR data reveal predominant three-dimensional spin-spin correlations at low temperatures. Field-induced magnetic ordering transition observed above $H_{c1}$ is attributed to the Bose-Einstein condensation of triplons in the sublattice formed by the $J_1$-$J_1'$ chains with weaker exchange couplings.

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