One-Dimensional Quantum Magnetism in the S = 1/2 Mo(V) system, KMoOP2O7

Abstract

We present a comprehensive experimental and ab-initio study of the $S=1/2$ Mo${}^{5+}$ system, KMoOP${}_2$O${}_7$, and show that it realizes the $S=1/2$ Heisenberg chain antiferromagnet model. Powder neutron diffraction reveals that KMoOP${}_2$O${}_7$ forms a magnetic network comprised of pairs of Mo${}^{5+}$ chains within its monoclinic $P{2}_1/n$ structure. Antiferromagnetic interactions within the Mo${}^{5+}$ chains are identified through magnetometry measurements and confirmed by analysis of the magnetic specific heat. The latter reveals a broad feature centred on $T_{\text{N}}=0.54$ K, which we ascribe to the onset of long-range antiferromagnetic order. No magnetic Bragg scattering is observed in powder neutron diffraction data collected at 0.05 K, however, which is consistent with a strongly suppressed ordered moment with an upper limit ${\mu }_{\text{ord}}<0.15{\mu }_{\text{B}}$. The one-dimensional character of the magnetic correlations in KMoOP${}_2$O${}_7$ is verified through analysis of inelastic neutron scattering data, resulting in a model with $J_{\text{1}}\approx 34$ K and $J_{\text{2}}\approx -2$ K for the intrachain and interchain exchange interactions, respectively. The origin of these experimental findings are addressed through density-functional theory calculations.

arXiv comment10 pages, 7 figures

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