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Weak ferromagnetism and glassy state in kappa-(BEDT-TTF)2Hg(SCN)2Br

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 Added by Mamoun Hemmida
 Publication date 2017
  fields Physics
and research's language is English




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Since the first observation of weak ferromagnetism in the charge-transfer salt kappa-(BEDT-TTF)2-Cu[N(CN)2]Cl [U. Welp et al., Phys. Rev. Lett. 69, 840 (1992)], no further evidence of ferromagnetism in this class of organic materials has been reported. Here we present static and dynamic spin susceptibility measurements on kappa-(BEDT-TTF)2Hg(SCN)2Br revealing weak ferromagnetism below about TWF = 20 K. We suggest that frustrated spins in the molecular dimers suppress long-range order, forming a spin-glass ground state in the insulating phase.



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We perform magnetic susceptibility and magnetic torque measurements on the organic $kappa$-(BEDT-TTF)$_2$Hg(SCN)$_2$Br, which is recently suggested to host an exotic quantum dipole-liquid in its low-temperature insulating phase. Below the metal-insulator transition temperature, the magnetic susceptibility follows a Curie-Weiss law with a positive Curie-Weiss temperature, and a particular $Mpropto sqrt{H}$ curve is observed. The emergent ferromagnetically interacting spins amount to about 1/6 of the full spin moment of localized charges. Taking account of the possible inhomogeneous quasi-charge-order that forms a dipole-liquid, we construct a model of antiferromagnetically interacting spin chains in two adjacent charge-ordered domains, which are coupled via fluctuating charges on a Mott-dimer at the boundary. We find that the charge fluctuations can draw a weak ferromagnetic moment out of the spin singlet domains.
The organic charge-transfer salt $kappa$-(BEDT-TTF)$_{2}$Hg(SCN)$_{2}$Br is a quasi two-dimensional metal with a half-filled conduction band at ambient conditions. When cooled below $T=80$ K it undergoes a pronounced transition to an insulating phase where the resistivity increases many orders of magnitude. In order to elucidate the nature of this metal-insulator transition we have performed comprehensive transport, dielectric and optical investigations. The findings are compared with other dimerized $kappa$-(BEDT-TTF) salts, in particular the Cl-analogue, where a charge-order transition takes place at $T_{rm CO}=30$ K.
In spite of extensive experimental studies of the angular dependent magnetoresistance (ADMR) of the low temperature phase (LTP) of alpha-(BEDT-TTF)_2KHg(SCN)_4 about a decade ago, the nature of LTP remains elusive. Here we present a new study of ADMR of LTP in alpha-(ET)_2 salts assuming that LTP is unconventional charge density wave (UCDW). In the presence of magnetic field the quasiparticle spectrum in UCDW is quantized, which gives rise to striking ADMR in UCDW. The present model appears to account for many existing ADMR data of alpha-(BEDT-TTF)_2KHg(SCN)_4 remarkably well.
The low temperature phase (LTP) of alpha-(BEDT-TTF)_2KHg(SCN)_4 salt is known for its surprising angular dependent magnetoresistance (ADMR), which has been studied intensively in the last decade. However, the nature of the LTP has not been understood until now. Here we analyse theoretically ADMR in unconventional (or nodal) charge density wave (UCDW). In magnetic field the quasiparticle spectrum in UCDW is quantized, which gives rise to spectacular ADMR. The present model accounts for many striking features of ADMR data in alpha-(BEDT-TTF)_2KHg(SCN)_4.
We present high-resolution measurements of the relative length change as a function of temperature of the organic charge-transfer salt $kappa$-(BEDT-TTF)$_2$Hg(SCN)$_2$Cl. We identify anomalous features at $T_g approx,63$ K which can be assigned to a kinetic glass-like ordering transition. By determining the activation energy $E_A$, this glass-like transition can be related to conformational degrees of freedom of the ethylene endgroups of the organic building block BEDT-TTF. As opposed to other $kappa$-(BEDT-TTF)$_2X$ salts, we identify a peculiar ethylene endgroup ordering in the present material in which only one of the two crystallographically inequivalent ethylene endgroups is subject to glass-like ordering. This experimental finding is fully consistent with our predictions from $ab,initio$ calculations from which we estimate the energy differences $Delta E$ and the activation energies $E_A$ between different conformations. The present results indicate that the specific interaction between the ethylene endgroups and the nearby anion layers leads to different energetics of the inequivalent ethylene endgroups, as evidenced by different ratios $E_A/Delta E$. We infer that the ratio $E_A/Delta E$ is a suitable parameter to identify the tendency of ethylene endgroups towards glass-like freezing.
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