arXiv subjects

R. Nath

Publications and source records attributed to R. Nath.

At least 37 records · Page 2Linked to original sources

arXiv2024

Ground-state properties of the double trillium lattice antiferromagnet KBaCr$_2$(PO$_4$)$_3$

Trillium lattices formed by corner-shared triangular units are the platform for magnetic frustration in three dimensions. Herein, we report structural and magnetic properties of the Cr-based double trillium lattice material KBaCr$_2$(PO$_4$)$_3$ studied by x-ray diffraction, magnetization, heat capacity, thermal conductivity, and $^{31}$P nuclear magnetic resonance (NMR) measurements complemented by density-functional band-structure calculations. Heat capacity and $^{31}$P NMR measurements reveal the magnetic transition at $T_{\rm N1} \simeq 13.5$ K in zero field followed by another transition at $T_{\rm N2} \simeq 7$ K in weak applied fields. The NMR sublattice magnetization confirms that the transition at $T_{\rm N1}$ is 3D in nature. The $^{31}$P spin-lattice relaxation rate in the ordered state follows the $T^3$ behavior indicative of the two-magnon Raman process. The spin lattice of KBaCr$_2$(PO$_4$)$_3$ comprises two crystallographically nonequivalent ferromagnetic sublattices that are coupled antiferromagnetically, thus eliminating frustration in this trillium network.

cond-mat.mtrl-sci↗

arXiv2024

Cluster-glass behaviour and large magnetocaloric effect in frustrated hyperkagome ferromagnet Li$_2$MgMn$_3$O$_8$

A detailed study of the structural and magnetic properties of the spin-$3/2$ hyperkagome lattice compound Li$_2$MgMn$_3$O$_8$ is reported. This material shows ferromagnetic response below $T_{\rm C} \simeq 20.6$ K, the temperature almost three times lower than the Curie-Weiss temperature $θ_{\rm CW} \simeq 56.6$ K. Density-functional band-structure calculations suggest that this reduction in $T_{\rm C}$ may be caused by long-range antiferromagnetic couplings that frustrate nearest-neighbor ferromagnetic couplings on the hyperkagome lattice. Large magnetocaloric effect is observed around the $T_{\rm C}$ with a maximum value of isothermal entropy change $ΔS_{\rm m}\simeq 20$ J/kg-K and a maximum relative cooling power of $RCP\simeq 840$ J/kg for the 7 T magnetic field change. Critical analysis of the magnetization data and scaling analysis of the magnetocaloric effect suggest the 3D Heisenberg/XY universality class of the transition. The DC and AC magnetization measurements further reveal glassy nature of the ferromagnetic transition. A detailed study of the non-equilibrium dynamics via magnetic relaxation and memory effect measurements demonstrates that the system evolves through a large number of intermediate metastable states and manifests significant memory effect in the cluster-glass state.

cond-mat.mtrl-sci↗

arXiv2024

Double magnetic transition, complex field-induced phases, and large magnetocaloric effect in the frustrated garnet compound Mn$_{3}$Cr$_{2}$Ge$_{3}$O$_{12}$

A detailed study of the magnetic and magnetocaloric properties of a garnet compound Mn$_{3}$Cr$_{2}$Ge$_{3}$O$_{12}$ is carried out using x-ray diffraction, magnetization, heat capacity, and neutron diffraction measurements as well as \textit{ab initio} band-structure calculations. This compound manifests two successive magnetic transitions at $T_{\rm N1} \simeq 4.5$ K and $T_{\rm N2} \simeq 2.7$ K. Neutron powder diffraction experiments reveal that these two transitions correspond to the collinear and non-collinear antiferromagnetic ordering of the nonfrustrated Cr$^{3+}$ and frustrated Mn$^{2+}$ sublattices, respectively. The interactions within each of the Cr and Mn sublattices are antiferromagnetic, while the inter-sublattice interactions are ferromagnetic. The $H-T$ phase diagram is quite complex and displays multiple phases under magnetic field, which can be attributed to the frustrated nature of the spin lattice. Mn$_{3}$Cr$_{2}$Ge$_{3}$O$_{12}$ shows a large magnetocaloric effect with a maximum value of isothermal entropy change $ΔS_{\rm m} \simeq -23$ J/kg-K and adiabatic temperature change $ΔT_{\rm ad} \simeq 9$ K for a field change of 7 T. Further, a large value of the relative cooling power ($RCP \simeq 360$ J/kg) demonstrates the promise of using this compound in magnetic refrigeration.

cond-mat.str-el↗

arXiv2023

Disordered ground state in the spin-orbit coupled $J_{\rm eff}= 1/2$ cobalt-based metal-organic framework magnet with orthogonal spin dimers

We present the magnetic properties of a strongly spin-orbit coupled quantum dimer magnet based on Co$^{2+}$. The metal-organic framework compound Co$_2$(BDC)$_2$(DPTTZ)$_2$$\cdot$DMF features Co$^{2+}$ dimers arranged nearly orthogonal to each other, similar to the Shastry-Sutherland lattice. Our assessment based on the magnetization and heat capacity experiments reveals that the magnetic properties at low temperatures can be described by an effective $J_{\rm eff} = 1/2$ Kramers doublet and the ground state is a singlet with a tiny spin gap. Although the magnetic susceptibility could be analyzed in terms of the interacting dimer model with an isotropic intradimer coupling $J_0/k_{\rm B} \simeq 7.6$ K, this model fails to reproduce the shape of magnetization isotherm and heat capacity data. A model of isolated spin dimers with the anisotropic exchange couplings $J_{xy} \simeq 3.5$ K and $J_{z} \simeq 11$ K provides an adequate description to the magnetic susceptibility, magnetization isotherm, and heat capacity data at low temperatures. Interestingly, no field-induced quantum phase phase is detected down to 100~mK around the critical field of gap closing, suggesting the absence of Bose-Einstein condensation of triplons and establishing isolated dimers with a negligible interdimer coupling.

cond-mat.str-el↗

arXiv2023

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↗

arXiv2023

Structural and double magnetic transitions in the frustrated spin-$\frac{1}{2}$ capped-kagome antiferromagnet (RbCl)Cu$_{5}$P$_{2}$O$_{10}$

The structural and magnetic properties of the geometrically frustrated spin-$1/2$ capped-kagome antiferromagnet (RbCl)Cu$_{5}$P$_{2}$O$_{10}$ are investigated via temperature dependent x-ray diffraction, magnetization, heat capacity, and $^{31}$P NMR experiments on a polycrystalline sample. It undergoes a structural transition at around $T_{\rm t} \simeq 310$ K from a high temperature trigonal ($P\bar{3}m1$) to a low temperature monoclinic ($C2/c$) unit cell, where the low temperature structure features the capped-kagome geometry of Cu$^{2+}$ ions. Interestingly, it shows the onset of two successive magnetic transitions at $T_{\rm N1} \simeq 20$ K and $T_{\rm N2} \simeq 7$ K. The shape of the $^{31}$P NMR spectra unfold the possible nature of the transitions below $T_{\rm N1}$ and $T_{\rm N2}$ to be of incommensurate and commensurate antiferromagnetic type, respectively. A large value of the Curie-Weiss temperature as compared to $T_{\rm N1}$ sets the frustration parameter $f \simeq 8$, ensuring strong magnetic frustration in the compound. From the $^{31}$P NMR spin-lattice relaxation rate, the leading antiferromagnetic exchange coupling is estimated to be $J/k_{\rm B} \simeq 117$ K. These unusual double magnetic transitions make this compound beguiling for further investigations.

cond-mat.mtrl-sci↗

arXiv2023

Double magnetic transitions and exotic field induced phase in the triangular lattice antiferromagnets Sr$_3$Co(Nb,Ta)$_2$O$_9$

Two triangular lattice antiferromagnets Sr$_3$Co(Nb,Ta)$_2$O$_9$ with an effective $j_{\rm eff}=1/2$ of Co$^{2+}$ are synthesized and their magnetic properties are investigated via magnetization and heat capacity measurements. The leading in-plane antiferromagnetic exchange coupling is estimated to be $J/k_{\rm B} \simeq 4.7$ K and 5.8 K, respectively. Both the compounds feature two-step magnetic transitions at low temperatures [($T_{\rm N1} \simeq 1.47$ K and $T_{\rm N2} \simeq 1.22$ K) and ($T_{\rm N1} \simeq 0.88$ K and $T_{\rm N2} \simeq 0.67$ K), respectively], driven by weak easy-axis anisotropy. Under magnetic field Sr$_3$CoNb$_2$O$_9$ evinces a plateau at $1/3$ magnetization. Interestingly, the high field magnetization of Sr$_3$CoTa$_2$O$_9$ reveals an exotic regime (between $H_{\rm S1}$ and $H_{\rm S2}$), below the fully polarized state in which the heat capacity at low temperatures is governed by a power law ($C_{\rm p} \propto T^α$) with a reduced exponent $α\simeq 2$. These results demonstrate an unusual field induced state with gapless excitations in the strongly frustrated magnet Sr$_3$CoTa$_2$O$_9$. The complete $T-H$ phase diagram is discussed for both the compounds.

cond-mat.str-el↗

arXiv2023

Crystal structure and magnetic properties of spin-$1/2$ frustrated two-leg ladder compounds (C$_4$H$_{14}$N$_2$)Cu$_2X_6$ ($X$= Cl and Br)

We have successfully synthesized single crystals, solved the crystal structure, and studied the magnetic properties of a new family of copper halides (C$_4$H$_{14}$N$_2$)Cu$_2X_6$ ($X$= Cl, Br). These compounds crystallize in an orthorhombic crystal structure with space group $Pnma$. The crystal structure features Cu$^{2+}$ dimers arranged parallel to each other that makes a zig-zag two-leg ladder-like structure. Further, there exists a diagonal interaction between two adjacent dimers which generates inter-dimer frustration. Both the compounds manifest a singlet ground state with a large gap in the excitation spectrum. Magnetic susceptibility is analyzed in terms of both interacting spin-$1/2$ dimer and two-leg ladder models followed by exact diagonalization calculations. Our theoretical calculations in conjunction with the experimental magnetic susceptibility establish that the spin-lattice can be described well by a frustrated two-leg ladder model with strong rung coupling ($J_0/k_{\rm B} \simeq 116$ K and 300 K), weak leg coupling ($J^{\prime\prime}/k_{\rm B} \simeq 18.6$ K and 105 K), and equally weak diagonal coupling ($J^{\prime }/k_{\rm B} \simeq 23.2$ K and 90 K) for Cl and Br compounds, respectively. These exchange couplings set the critical fields very high, making them experimentally inaccessible. The correlation function decays exponentially as expected for a gapped spin system. The structural aspects of both the compounds are correlated with their magnetic properties. The calculation of entanglement witness divulges strong entanglement in both the compounds which persists upto high temperatures, even beyond 370~K for the Br compound.

cond-mat.mtrl-sci↗

arXiv2023

Quantum disordered ground state in the spin-orbit coupled Jeff = 1/2 distorted honeycomb magnet BiYbGeO5

We delineate quantum magnetism in the strongly spin-orbit coupled, distorted honeycomb-lattice antiferromagnet BiYbGeO$_{5}$. Our magnetization and heat capacity measurements reveal that its low-temperature behavior is well described by an effective $J_{\rm eff}=1/2$ Kramers doublet of Yb$^{3+}$. The ground state is nonmagnetic with a tiny spin gap. Temperature-dependent magnetic susceptibility, magnetization isotherm, and heat capacity could be modeled well assuming isolated spin dimers with anisotropic exchange interactions $J_{\rm Z} \simeq 2.6$~K and $J_{\rm XY} \simeq 1.3$~K. Heat capacity measurements backed by muon spin relaxation suggest the absence of magnetic long-range order down to at least 80\,mK both in zero field and in applied fields. This sets BiYbGeO$_5$ apart from Yb$_2$Si$_2$O$_7$ with its unusual regime of magnon Bose-Einstein condensation and suggests negligible interdimer couplings, despite only a weak structural deformation of the honeycomb lattice.

cond-mat.str-el↗

arXiv2023

Large magnetocaloric effect in the kagome ferromagnet Li$_9$Cr$_3$(P$_2$O$_7$)$_3$(PO$_4$)$_2$

Single-crystal growth, magnetic properties, and magnetocaloric effect of the $S = 3/2$ kagome ferromagnet Li$_9$Cr$_3$(P$_2$O$_7$)$_3$(PO$_4$)$_2$ (trigonal, space group: $P\bar{3}c1$) are reported. Magnetization data suggest dominant ferromagnetic intra-plane coupling with a weak anisotropy and the onset of ferromagnetic ordering at $T_{\rm C} \simeq 2.6$ K. Microscopic analysis reveals a very small ratio of interlayer to intralayer ferromagnetic couplings ($J_{\perp}/J \simeq 0.02$). Electron spin resonance data suggest the presence of short-range correlations above $T_{\rm C}$ and confirms quasi-two-dimensional character of the spin system. A large magnetocaloric effect characterized by isothermal entropy change of $-ΔS_{\rm m}\simeq 31$ J kg$^{-1}$ K$^{-1}$ and adiabatic temperature change of $-ΔT_{\rm ad}\simeq 9$ K upon a field sweep of 7 T is observed around $T_{\rm C}$. This leads to a large relative cooling power of $RCP \simeq 284$ J kg$^{-1}$. The large magnetocaloric effect, together with negligible hysteresis render Li$_9$Cr$_3$(P$_2$O$_7$)$_3$(PO$_4$)$_2$ a promising material for magnetic refrigeration at low temperatures. The magnetocrystalline anisotropy constant $K \simeq -7.42 \times 10^4$ erg cm$^{-3}$ implies that the compound is an easy-plane type ferromagnet with the hard axis normal to the $ab$-plane, consistent with the magnetization data.

cond-mat.mtrl-sci↗

arXiv2022

Static magnetic and ESR spectroscopic properties of the dimer-chain antiferromagnet BiCoPO$_5$

We report a comprehensive study of the static susceptibility, high-field magnetization and high-frequency/high-magnetic field electron spin resonance (HF-ESR) spectroscopy of polycrystalline samples of the bismuth cobalt oxy-phosphate BiCoPO$_5$. This compound features a peculiar spin system that can be considered as antiferromagnetic (AFM) chains built of pairs of ferromagnetically coupled Co spins and interconnected in all three spatial directions. It was previously shown that BiCoPO$_5$ orders antiferromagnetically at $T_{\rm N} \approx 10$ K and this order can be continuously suppressed by magnetic field towards the critical value $μ_0H_{\rm c} \approx 15$ T. In our experiments we find strongly enhanced magnetic moments and spectroscopic $g$ factors as compared to the expected spin-only values, suggesting a strong contribution of orbital magnetism for the Co$^{2+}$ ions. This is quantitatively confirmed by ab initio quantum chemical calculations. Within the AFM ordered phase, we observe a distinct field-induced magnetic phase transition. Its critical field rises to $\sim 6$ T at $T \ll T_{\rm N}$. The HF-ESR spectra recorded at $T\ll T_{\rm N}$ are very rich comprising up to six resonance modes possibly of the multimagnonic nature that soften towards the critical region around 6 T. Interestingly, we find that the Co moments are not yet fully polarized at $H_{\rm c}$ which supports a theoretical proposal identifying $H_{\rm c}$ as the quantum critical point for the transition of the spin system in BiCoPO$_5$ to the quantum disordered state at stronger fields.

cond-mat.str-el↗

arXiv2022

Absence of magnetic order and emergence of unconventional fluctuations in $J_{\rm eff} =1/2$ triangular lattice antiferromagnet YbBO$_3$

We present the ground state properties of a new quantum antiferromagnet YbBO$_3$ in which the isotropic Yb$^{3+}$ triangular layers are separated by a non-magnetic layer of partially occupied B and O(2) sites. The magnetization and heat capacity data establish a spin-orbit entangled effective spin $J_{\rm eff} = 1/2$ state of Yb$^{3+}$ ions at low temperatures, interacting antiferromagnetically with an intra-layer coupling $J/k_{\rm B} \simeq 0.53$ K. The absence of oscillations and a $1/3$ tail in the zero-field muon asymmetries rule out the onset of magnetic long-range-order as well as spin-freezing down to 20~mK. An anomalous broad maximum in the temperature dependent heat capacity with a unusually reduced value and a broad anomaly in zero-field muon depolarization rate centered at $T^*\simeq 0.7 \frac{J}{k_{\rm B}}$ provide compelling evidence for a wide fluctuating regime ($0.182 \leq T/J \leq 1.63$) with slow relaxation. We infer that the fluctuating regime is a universal feature of a highly frustrated triangular lattice antiferromagnets while the absence of magnetic long-range-order is due to perfect two-dimensionality of the spin-lattice protected by non-magnetic site disorder.

cond-mat.str-el↗

arXiv2022

Deformed spin-$\frac12$ square lattice in antiferromagnetic NaZnVOPO$_4$(HPO$_4$)

We report the structural and magnetic properties of a new spin-$\frac12$ antiferromagnet NaZnVOPO$_4$(HPO$_4$) studied via x-ray diffraction, magnetic susceptibility, high-field magnetization, specific heat, and $^{31}$P nuclear magnetic resonance (NMR) measurements, as well as density-functional band-structure calculations. While thermodynamic properties of this compound are well described by the $J_1-J_2$ square-lattice model, \textit{ab initio} calculations suggest a significant deformation of the spin lattice. From fits to the magnetic susceptibility we determine the averaged nearest-neighbor and second-neighbor exchange couplings of $\bar J_1\simeq -1.3$ K and $\bar J_2\simeq 5.6$ K, respectively. Experimental saturation field of 15.3\,T is consistent with these estimates if 20\% spatial anisotropy in $J_1$ is taken into account. Specific heat data signal the onset of a magnetic long-range order at $T_{\rm N} \simeq 2.1$ K, which is further supported by a sharp peak in the NMR spin-lattice relaxation rate. The NMR spectra mark the superposition of two P lines due to two noneqivalent P sites where the broad line with the strong hyperfine coupling and short $T_1$ is identified as the P(1) site located within the magnetic planes, while the narrow line with the weak hyperfine coupling and long $T_1$ is designated as the P(2) site located between the planes.

cond-mat.mtrl-sci↗

arXiv2022

Collinear antiferromagnetic order in spin-$\frac52$ triangle lattice antiferromagnet Na$_3$Fe(PO$_4$)$_2$

We set forth the structural and magnetic properties of the frustrated spin-$5/2$ triangle lattice antiferromagnet Na$_3$Fe(PO$_4$)$_2$ examined via x-ray diffraction, magnetization, heat capacity, and neutron diffraction measurements on the polycrystalline sample. No structural distortion was detected from the temperature-dependant x-ray diffraction down to 12.5 K, except a systematic lattice contraction. The magnetic susceptibility at high temperatures agrees well with the high-temperature series expansion for a spin-$5/2$ isotropic triangular lattice antiferromagnet with an average exchange coupling of $J/k_{\rm B} \simeq 1.8$ K rather than a one-dimensional spin-$5/2$ chain model. This value of the exchange coupling is consistently reproduced by the saturation field of the pulse field magnetization data. It undergoes a magnetic long-range-order at $T_{\rm N} \simeq 10.4$ K. Neutron diffraction experiments elucidate a collinear antiferromagnetic ordering below $T_{\rm N}$ with the propagation vector $k = (1,0,0)$. An intermediate value of frustration ratio ($f \simeq 3.6$) reflects moderate frustration in the compound which is corroborated by a reduced ordered magnetic moment of $\sim 1.52$ $μ_{\rm B}$ at 1.6 K, compared to its classical value ($5 μ_{\rm B}$). Magnetic isotherms exhibit a change of slope envisaging a field induced spin-flop transition at $H_{\rm SF}\simeq3.2$ T. The magnetic field vs temperature phase diagram clearly unfold three distinct phase regimes, reminiscent of a frustrated magnet with in-plane (XY-type) anisotropy.

cond-mat.mtrl-sci↗

arXiv2021

Imaging the interface of a qubit and its quantum-many-body environment

Decoherence affects all quantum systems, natural or artificial, and is the primary obstacle impeding quantum technologies. We show theoretically that for a Rydberg qubit in a Bose condensed environment, experiments can image the system-environment interface that is central for decoherence. High precision absorption images of the condensed environment will be able to capture transient signals that show the real time build up of a mesoscopic entangled state in the environment. This is possible before decoherence sources other than the condensate itself can kick in, since qubit decoherence time-scales can be tuned from the order of nanoseconds to microseconds by choice of the excited Rydberg principal quantum number ν. Imaging the interface will allow detailed explorations of open quantum system concepts and may offer guidance for coherence protection in challenging scenarios with non-Markovian environments.

quant-ph↗

arXiv2021

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↗

arXiv2021

Negative thermal expansion and itinerant ferromagnetism in Mn$_{1.4}$Fe$_{3.6}$Si$_{3}$

We report the thermal expansion, critical behavior, magnetocaloric effect (MCE), and magnetoresistance ($MR$) on the polycrystalline Mn$_{1.4}$Fe$_{3.6}$Si$_{3}$ compound around the ferromagnetic transition. A large negative volume thermal expansion ($α_{\rm V}\sim -20 \times 10^{-6}$ K$^{-1}$) is observed across the transition temperature with a strong anisotropic variation of lattice parameters in the $ab$-plane. The anisotropic magnetoelasticity arises from the competition between magnetic ordering and structural deformation which could be responsible for the large MCE ($ΔS_{\rm m} \simeq -6$ J/Kg-K) across the magnetic transition in this compound. The large and negative $MR$ ($\sim -3\%$ in 80 kOe) is also observed at the transition temperature which can be attributed to the suppression of spin disorder. Further, the Rhodes-Wolfarth ratio (RWR $> 1$) and identical field dependence of $MR$ and MCE isotherms indicate the itinerant character of the $3d$ electrons. The critical exponents determined from the analysis of magnetization and MCE are consistent with the quasi-two-dimensional (2D) Ising model with long range exchange interactions which decays as $J(r)\sim r^{-3.41}$. This unconventional quasi-2D Ising character with long-range interactions can be ascribed to strong $ab$-plane anisotropy and the delocalized $3d$ electrons in the studied compound.

cond-mat.str-el↗

arXiv2021

Quasi-one-dimensional uniform spin-$\frac{1}{2}$ Heisenberg antiferromagnet KNaCuP$_2$O$_7$ probed by $^{31}$P and $^{23}$Na NMR

We present the structural and magnetic properties of KNaCuP$_2$O$_7$ investigated via x-ray diffraction, magnetization, specific heat, and $^{31}$P NMR and $^{23}$Na NMR measurements and complementary electronic structure calculations. The temperature dependent magnetic susceptibility and $^{31}$P NMR shift could be modeled very well by the uniform spin-$1/2$ Heisenberg antiferromagnetic chain model with nearest-neighbour interaction $J/k_{\rm B}\simeq 58.7$ K. The corresponding mapping using first principles electronic structure calculations leads to $J^{\rm DFT}/k_{\rm B} \simeq 59$ K with negligibly small inter-chain couplings ($J^{\prime}/k_{\rm B}$, $J^{\prime \prime}/k_{\rm B} < 0.1$ K), further confirming that the system is indeed an one-dimensional uniform spin-$1/2$ Heisenberg antiferromagnet. The temperature-dependent unit cell volume could be described well using the Debye approximation with a Debye temperature of $Θ_{\rm D} \simeq 294$ K, consistent with the heat capacity data. The diverging trend of the NMR spin-lattice relaxation rates ($^{31}1/T_1$ and $^{23}1/T_1$) imply the onset of a magnetic long-range-ordering at very low temperatures supporting the anticipated $T_{\rm N} \simeq 0.38$ K from the inter-chain couplings. Moreover, the NMR spin-lattice relaxation rates show the dominant contributions from uniform ($q=0$) and staggered ($q = \pm π/a$) spin fluctuations in the high and low temperature regimes, respectively mimicking one-dimensionality of the spin-lattice. We have also demonstrated that $^{31}1/T_1$ in high temperatures varies linearly with $1/\sqrt{H}$ reflecting the effect of spin diffusion on the dynamic susceptibility. Further, the inter-chain frustration also substantially impede the magnetic ordering rendering the spin-lattice a perfect one-dimensional uniform spin-$1/2$ Heisenberg antiferromagnet over a wide temperature range.

cond-mat.mtrl-sci↗