ࡱ> G ]bjbjَ y!=]... 8 DDDdX,$$|4D DD   DDDDDD  DD ਏ$ THE LOW-FREQUENCY DIELECTRIC RESPONSE AND NON-LINEAR DC ELECTRICAL TRANSPORT IN k(BEDT-TTF)2Cu[N(CN)2]Cl Marko Pinteri 1,2, Neven Biakup1, Silvia Tomi1, Dieter Schweitzer3, Werner Strunz4, Ilsabe Heinen4 1Institute of Physics, P. O. Box 304, 10000 Zagreb, Croatia, 2Faculty of Civil Engineering, University of Maribor, Slovenia, 33. Physikalisches Institut, Universitt Stuttgart, Germany, 4Anorganisch-chemisches Institut, Universitt Heidelberg, Germany ABSTRACT: We report AC transport and non-linear DC electrical transport in single crystals of the organic conductor 0000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000k-(BEDT-TTF)2Cu[N(CN)2]Cl. Non-linear conductivity emerges below 22K, which is the temperature of canted antiferromagnetic ordering. A broad dielectric relaxation mode of moderate strength (De ~ 3(103) appears at 32K, and weakens with temperature. The mean relaxation time, much larger than that expected for single-particle excitations, is thermally activated in a manner similar to the DC conductivity and saturates below 22K. The observed dielectric response data give evidence of a collective mode contribution to the dielectric properties, which might be attributed to charged domain walls in a ferromagnetic domain structure. Non-linear conductivity similar to those observed for commensurate spin and charge density waves are found. 1. INTRODUCTION One family of novel organic metals that received special interest in recent time is k(BEDT-TTF)2Cu[N(CN)2]X family, where BEDT-TTF is Bis(ethylenedithio) tetrathiafulvalene and X is a halogenide. That is, when substituting X for Br, the ground state is superconducting with the highest superconducting critical temperature among organic metals. On the other side, substituting X for Cl leads to semiconducting material with the canted antiferromagnetic ground state. Moreover, when subjected to the pressure of only 300 bars [1], the latter material undergoes a transition to superconducting state. In this case we face a competition between superconducting and antiferromagnetic states, which is also interesting for theoretical understanding of superconductivity. Here we present for the first time a complete account of the collective conduction properties of k(BEDT-TTF)2Cu[N(CN)2]Cl material. k-(BEDT-TTF)2Cu[N(CN)2]Cl material belongs to the k-(BEDT-TTF)2X (X is polymerised anion) class of BEDT-TTF systems in which orthogonally aligned BEDT-TTF dimers form 2D conducting layers sandwiched between the polymerised anion layers. Its unit cell contains two BEDT-TTF layers (i.e. 4 dimers) and 4 anions [2]. The donor molecules form face-to-face orthogonal dimers which are rotated by circa 45degrees with respect to the unit cell axes (a and c). The copper atoms complete their trigonal coordinate ion environment with a bond to a terminal chlorine atom. The 2D layers of the organic donor molecules lie in the crystallographic ac plane, which coincides with the large face of the crystal, and these layers are alternatively separated by anion layers along the b axis. Overlap between BEDT-TTF molecules leads to formation of two-dimensional band and strong anisotropy between in-plane and out-of plane conductivity. No anisotropy in in-plane electronic characteristics larger than a factor of 2 was found. Since we have one electron per one dimer (that is one electron per two BEDT-TTF molecules) and quarter-filled band, we expect ordering of periodicity N = 4. All conductivity properties were measured within the ac plane. 2. MAGNETIC PROPERTIES The results of NMR measurements of Miyagawa et al. [3] showed a large enhancement of the spin-lattice relaxation rate below 50K and a sharp peak at 27K. The former was interpreted to be due to the antiferromagnetic spin fluctuations, and the latter as a sign of an antiferromagnetic phase transition. The established order is commensurate with the underlying lattice and possesses a rather large moment of (0.4-1.0) mB per dimer. In addition, magnetisation measurements by the same authors showed that weak ferromagnetism appears below 23K due to the canting of spins. As in this temperature range a finite energy gap is already opened in the charge degrees of freedom, Miyagawa et al. suggested that the magnetic ordering of localised spins driven by electron-electron correlations was in origin of the observed phase transition. To get more information about the low-temperature state, we have performed measurements of the magnetic anisotropy using torque method [4]. Temperature dependant susceptibility anisotropy and especially appearance of spin-flop effect below 22K have given clear evidence of a canted antiferromagnetic state established below 22K, with the easy axis in the direction of b axis. Besides that, the angular dependent susceptibility anisotropy in bc plane has revealed that the vector of ferromagnetic magnetization is directed along c axis. The size of ferromagnetic effect corresponds to situation in which 1/1000 of total number of spins would arrange in ferromagnetic manner. That correspond to the canting of all spins for 6(10-2 degrees from b axis. We have suggested that the features observed could be accounted for taking into consideration the Dzyaloshinsky-Moriya interaction. In a two-sublattice model of antiferromagnetism, such an interaction will cant the sublattices toward one another and hence create a weak magnetic moment of the order of |D((M1(M2)|. Mi is the static sublattice magnetization, and D is a constant vector. This argument was supported by symmetry considerations. Finally, the hysteresis of the order 1kOe in the spin-flop transition and magnetic field reversal of the ferromagnetic magnetisation are features not encountered in the standard antiferromagnets and spin density waves. The latter feature indicates the existence of a domain structure, which is a well-known property of magnetically ordered state. That is, when the magnetic field is absent the energy of the ferromagnetic crystal is lowered when the crystal is divided into domains with equivalent spin configurations. 3. ELECTRICAL PROPERTIES We report results obtained on three different crystals. All crystals have showed the same properties. Their room temperature (RT) conductivity has been about 5 Scm-1. The ohmic and non-ohmic resistivity have been measured in the four probe configuration using a standard DC technique. The complex admittance (G(w), B(w)) has been measured by a Hewlett Packard HP4284A impedance analyser (20Hz-1MHz) in the two probe configuration in the temperature range between 7K and 40K. Dielectric functions have been extracted from the conductivity using relations e'(w)=B(w)/w, and e"(w)=(G(w)-G0)/w, where G0 is DC conductivity obtained from measured G(w) at low frequencies where G(w) was independent of w.  Figure 1: Resistivity and gap width (Inset) versus inverse temperature. The fits represent Arrhenius behaviour.  Figure 2: Non-ohmic conductivity versus electric field at few typical temperatures. Resistance as the function of inverse temperature is shown in Figure 1. Resistivity follows semiconducting (Arrhenius) behaviour and the gap width d(ln R)/d(1/T) changes with the temperature (see Inset). On first cooling, the gap width below 50K is about 275K and then it abruptly changes to 153K below 22K. On first warming and also on subsequent temperature cycles, the change is no longer sharp and gap width changes continuously. This might not be surprising, since we have already reported changes in some magnetic properties of the sample with thermal cycling in the high temperature range [4].  Figure 3: Threshold electrical field versus temperature.  Figure 4: Non-ohmic conductivity at two threshold electrical field, normalised to its ohmic value, versus temperature.  Figure 5: Real part of the conductivity normalised to the DC value versus frequency for temperature range between 30K and 15K. Full lines are fits to HN form.  Figure 8: (a) Relaxation strength, (b)shape parameter, (c) mean relaxation time (full points) and DC resistance (full line) versus inverse temperature.  Figure 6: Cole-Cole plots of the dielec-tric response at two selected tempera-tures. Full lines are fits to the HN form.  Figure 7: Frequency dependence (log scale) of the real and imaginary parts of the dielectric function for three representative temperatures. Full lines are fits to the HN form. Figure 2 shows the field-dependent conductivity normalised to its ohmic value at a few selected temperatures. Above a certain threshold electrical field, ET, conductivity starts to increase, since the additional, collective conducting channel opens. The magnitude of non-linear conductivity is negligible above 12K, as shown in Figure 4. Below that temperature it increases concomitantly with the rise of the threshold electrical field (see Figure 3). This behaviour is somewhat surprising. That is, the increase of threshold field suggests that the sliding mechanism starts to freeze below 12K. In that case one would expect concomitant decrease of non-linear conductivity as reported in commensurate charge density wave system [5]. However, such unexpected behaviour was also observed in the system with commensurate spin density wave [6]. The real part of the conductivity normalised to the DC value (G(00000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000w)-G0)/G0 as a function of frequency at a few selected temperatures between 15K and 30K is shown in Figure5 [4]. At T > 32K a frequency independent conductivity is found. Note that an enhanced AC conductivity grows in importance and starts at lower frequencies as the temperature lowers. The initial analysis of the dielectric function was performed by the inspection of Cole-Cole plots, which are presented in Figure6. The intersection of the arcs with e' axis at high and low e' values, corresponding to low and high frequencies, indicates the values of the static dielectric constant e0 and the high frequency dielectric constant eHF, respectively. The value of the relaxation strength De(= e0 - eHF is moder-ate, of the order of 1000. Figure 7 shows frequency domain plots of the real and ima-ginary part of the dielectric function at three selected temperatures. It should be noted that e''(n) curves move toward lower peak frequencies (n0 = w0/2p = 1/2pt0) and smaller peak amplitudes with decreasing temperature without significant change in the shape. Detailed analysis of the collective mode was made in terms of the complex dielectric function e(w) given by a generalisation of the Debye expressionknown as the phenomenological Havriliak-Negami (HN) function [7]  EMBED Equation.2  (1) where b=1 for symmetrical cases. t0 and 1-a are the mean relaxation time and the shape parameter, which describes the symmetric broadening of the relaxation time distribution function, respectively. The full lines in Figures 5, 6 and 7 correspond to the calculated fits. The fit parameters as a function of inverse temperature are shown in Figure 8. The parameter De corresponds to the static dielectric susceptibility and decreases with temperature less than one order of magnitude between 32K and 14K. The width of the relaxation time distribution expressed by the (1 - a) parameter is close to 1 at 32K. However, already below 28K the mode broadens and the value of (1 - a) ~ 0.7 does not change significantly with temperature. The mean relaxation time t0 closely follows the thermally activated behaviour in a manner similar to the DC conductivity in the temperature range 32K  25K, and saturates below 22K. 4. DISCUSSION The dielectric relaxation appears below 32K. The width is larger than for the Debye process and does not change with temperature below 28K. The relaxation strength is of the order of 1000 and decreases on lowering the temperature. The characteristic relaxation time is too long to be attributed to free carriers. 000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000000t0 is thermally activated with the activation energy close the free-carriers one in the narrow temperature range 32K  25K and saturates below TN = 22K. Therefore, we are led to identify the origin of this relaxation as an intrinsic property of the weak ferromagnetic state established below 22K. We propose a charged domain wall in the ferromagnetic domain structure as the relaxation entity. The broad distribution of relaxation times (1  a) ~ 0.7 might be reasonably assumed to be due to a distribution of activation energies. Then, the dielectric response is due to the activation between different metastable states over energy barriers. These metastable states correspond to local changes of the spin configuration. The length scale over which such processes occur defines the thickness of the wall and is set by the competition between relevant energies of the problem. The fact that the energy scale for the barrier heights is close to the free-carrier activation energy only above TN = 22K indicates that the free-carrier screening influences the relaxation only in the fluctuating pretransitional regime. At 22K the relaxation time levels off. The change in the log t0 versus 1/T plot at TN = 22K might indicate that the resistive dissipation is not the dominant dissipation mechanism in the weak ferromagnetic state. That is, one could expect that the free-carrier screening becomes unimportant once the electron density becomes smaller than the one electron per the domain wall length LWF. 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