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Spin dynamics in S = 1/2 antiferromagnetic chain compounds delta-(EDT-TTF-CONMe_2)_2X (X=AsF_6, Br): a multi-frequency Electron Spin Resonance study

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 Added by Balint Nafradi
 Publication date 2010
  fields Physics
and research's language is English




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We present a multi-frequency Electron Spin Resonance (ESR) study in the range of 4 GHz to 420 GHz of the quasi-one-dimensional, non-dimerized, quarter-filled Mott insulators, delta-(EDT-TTF-CONMe_2)_2X (X=AsF_6, Br). In the high temperature orthorhombic phase above T~190 K, the magnitude and the temperature dependence of the high temperature spin susceptibility are described by a S = 1/2 Heisenberg antiferromagnetic chain with J_AsF6=298 K and J_Br=474 K coupling constants for X=AsF_6 and Br respectively. We estimate from the temperature dependence of the line width an exchange anisotropy, J/J of ~2 * 10^{-3}. The frequency dependence of the line width and the g-shift have an unusual quadratic dependence in all crystallographic orientations that we attribute to an antisymmetric exchange (Dzyaloshinskii--Moriya) interaction.

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We studied the magnetic properties, in particular dynamics, of the correlated spins associated with natural defects in the organic spin chain compounds ($o$-DMTTF)$_2X$ ($X$ = Br, Cl) by means of electron spin resonance (ESR) spectroscopy. Both materials exhibit spin-Peierls transitions at temperatures around 50 K [P. Foury-Leylekian et al. Phys. Rev. B 84, 195134 (2011)], which allow a separation of the properties of defects inside the chains from the magnetic response of the spin chains. Indeed, continuous wave ESR measurements performed over a wide temperature range evidence the evolution of the spin dynamics from being governed by the spins in the chains at elevated temperatures to a low-temperature regime which is dominated by defects within the spin-dimerized chains. Such defects polarize the antiferromagnetically coupled spins in their vicinity, thereby leading to a finite local alternating magnetization around the defect site which can be described in terms of a soliton, i.e. a spin 1/2 quasiparticle built of many correlated spins, pinned to the defect. In addition, contributions of triplon excitations of the spin-dimerized state to the ESR response below the transition temperature were observed which provides a spectroscopic estimate for the spin-gap of the studied systems. Moreover, details of spin dynamics deep in the spin-Peierls phase were investigated by pulse ESR experiments which revealed Rabi-oscillations as signatures of coherent spin dynamics. From a comparison of the characteristic damping times of the Rabi oscillations with measurements of the spin relaxation times by means of primary-echo decay and CPMG methods it becomes evident that inhomogeneities in local magnetic fields strongly contribute to the soliton decoherence.
The electron spin resonance spectrum of a quasi 1D S=1/2 antiferromagnet K2CuSO4Br2 was found to demonstrate an energy gap and a doublet of resonance lines in a wide temperature range between the Curie--Weiss and Ne`{e}l temperatures. This type of magnetic resonance absorption corresponds well to the two-spinon continuum of excitations in S=1/2 antiferromagnetic spin chain with a uniform Dzyaloshinskii--Moriya interaction between the magnetic ions. A resonance mode of paramagnetic defects demonstrating strongly anisotropic behavior due to interaction with spinon excitations in the main matrix is also observed.
We study the electron spin resonance (ESR) of low-dimensional spin systems at high temperature, and test the Kubo-Tomita theory of exchange narrowing. In finite-size systems (molecular magnets), we found a double-peak resonance which strongly differs from the usual Lorentzian. For infinite systems, we have predictions for the linewidth and lineshape as a function of the anisotropy strength. For this, we have used an interpolation between a non-perturbative calculation of the memory function at short times (exact diagonalization) and the hydrodynamic spin-diffusion at long times. We show that the Dzyaloshinskii-Moriya anisotropies generally induce a much larger linewidth than the exchange anisotropies in two dimensions, contrary to the one-dimensional case.
We measured X-band electron-spin resonance of single crystalline sodium vanadate doped with lithium, Na_{1-x}Li_xV_2O_5 for 0 < x < 1.3% . The phase transition into a dimerized phase that is observed at 34 K in the undoped compound, was found to be strongly suppressed upon doping with lithium. The spin susceptibility was analyzed to determine the transition temperature and the energy gap with respect to the lithium content. The transition temperature Tsp is suppressed following a square dependence of the lithium concentration while the energy gap is found to decrease linearly. At high temperatures (T>Tsp) the susceptibility remains nearly independent of doping.
163 - B. Nafradi , A. Antal , T. Feher 2016
The $1/4$-filled organic compound, $delta$-(EDT-TTF-CONMe$_{2}$)$_{2}$AsF$_6$ is a frustrated two-dimensional triangular magnetic system as shown by high-frequency (111.2 and 222.4 GHz) electron spin resonance (ESR) and structural data in the literature. The material gradually orders antiferromagnetically below 40~K but some magnetically disordered domains persist down to 4 K. We propose that in defect free regions frustration prevents true magnetic order down to at least 4 K in spite of the large first- and second-neighbor exchange interactions along chains and between chains, respectively. The antiferromagnetic (AFM) order gradually developing below 40 K nucleates around structural defects that locally cancel frustration. Two antiferromagnetic resonance modes mapped in the principal planes at 4~K are assigned to the very weakly interacting one-dimensional molecular chains in antiferromagnetic regions.
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