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Register a new userDetermination of effective microscopic models for the frustrated antiferromagnets Cs$_2$CuCl$_4$ and Cs$_2$CuBr$_4$ by density functional methods
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Kateryna Foyevtsova
Publication date
2010
fields
Physics
and research's language is
English
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We investigate the electronic and magnetic properties of the frustrated triangular-lattice antiferromagnets Cs$_2$CuCl$_4$ and Cs$_2$CuBr$_4$ in the framework of density functional theory. Analysis of the exchange couplings J and J using the available X-ray structural data corroborates the values obtained from experimental results for Cs$_2$CuBr$_4$ but not for Cs$_2$CuCl$_4$. In order to understand this discrepancy, we perform a detailed study of the effect of structural optimization on the exchange couplings of Cs$_2$CuCl$_4$ employing different exchange-correlation functionals. We find that the exchange couplings depend on rather subtle details of the structural optimization and that only when the insulating state (mediated through spin polarization) is present in the structural optimization, we do have good agreement between the calculated and the experimentally determined exchange couplings. Finally, we discuss the effect of interlayer couplings as well as longer-ranged couplings in both systems.
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We report $^{133}$Cs nuclear magnetic resonance (NMR) measurements on the 2D frustrated Heisenberg antiferromagnet Cs$_2$CuCl$_4$ down to 2 K and up to 15 T. We show that $^{133}$Cs NMR is a good probe of the magnetic degrees of freedom in this material. Cu spin degrees of freedom are sensed through a strong anisotropic hyperfine coupling. The spin excitation gap opens above the critical saturation field. The gap value was determined from the activation energy of the nuclear spin-lattice relaxation rate in a magnetic field applied parallel to the Cu chains (b axis). The values of the g-factor and the saturation field are consistent with the neutron-scattering and magnetization results. The measurements of the spin-spin relaxation time are exploited to show that no structural changes occur down to the lowest temperatures investigated.
The field induced magnetic phase transitions of Cs$_2$CuBr$_4$ were investigated by means of magnetization process and neutron scattering experiments. This system undergoes magnetic phase transition at Ne{e}l temperature $T_mathrm{N}=1.4$ K at zero field, and exhibits the magnetization plateau at approximately one third of the saturation magnetization for the field directions $Hparallel b$ and $Hparallel c$. In the present study, additional symptom of the two-third magnetization plateau was found in the field derivative of the magnetization process. The magnetic structure was found to be incommensurate with the ordering vector $boldsymbol{Q}=(0, 0.575, 0)$ at zero field. With increasing magnetic field parallel to the c-axis, the ordering vector increases continuously and is locked at $boldsymbol{Q}=(0, 0.662, 0)$ in the plateau field range $13.1 mathrm{T} < H < 14.4 mathrm{T}$. This indicates that the collinear textit{up-up-down} spin structure is stabilized by quantum fluctuation at the magnetization plateau.
The crystal structure of Cs$_2$CuBr$_4$ is the same as that of Cs$_2$CuCl$_4$, which has been characterized as a spin-1/2 quasi-two-dimensional frustrated system. The magnetic properties of Cs$_2$CuBr$_4$ were investigated by magnetization and specific heat measurements. The phase transition at zero magnetic field was detected at $T_{rm N}=1.4$ K. It was observed that the magnetization curve has a plateau at about one-third of the saturation magnetization for magnetic field $H$ parallel to the $b$- and $c$-axes, while no plateau was observed for $Hparallel a$. The field-induced phase transition to the plateau state appears to be of the first order. The mechanism leading to the magnetization plateau is discussed.
We report on electron spin resonance (ESR) studies of the spin relaxation in Cs$_2$CuCl$_4$. The main source of the ESR linewidth at temperatures $T leq 150$ K is attributed to the uniform Dzyaloshinskii-Moriya interaction. The vector components of the Dzyaloshinskii-Moriya interaction are determined from the angular dependence of the ESR spectra using a high-temperature approximation. Both the angular and temperature dependence of the ESR linewidth have been analyzed using a self-consistent quantum-mechanical approach. In addition analytical expressions based on a quasi-classical picture for spin fluctuations are derived, which show good agreement with the quantum-approach for temperatures $T geq 2J/k_{rm B} approx 15$ K. A small modulation of the ESR linewidth observed in the $ac$-plane is attributed to the anisotropic Zeeman interaction, which reflects the two magnetically nonequivalent Cu positions.
The spin excitations in the spin-liquid phase of the anisotropic triangular lattice quantum antiferromagnet Cs$_2$CuCl$_4$ have been shown to propagate dominantly along the crystallographic $b$ axis. To test this dimensional reduction scenario, we have performed ultrasound experiments in the spin-liquid phase of Cs$_2$CuCl$_4$ probing the elastic constant $c_{22}$ and the sound attenuation along the $b$ axis as a function of an external magnetic field along the $a$ axis. We show that our data can be quantitatively explained within the framework of a nearest-neighbor spin-$1/2$ Heisenberg chain, where fermions are introduced via the Jordan-Wigner transformation and the spin-phonon interaction arises from the usual exchange-striction mechanism.
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