Out-of-equilibrium behavior in CuCl

doi:10.21203/rs.3.rs-3403588/v1

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Out-of-equilibrium behavior in CuCl

https://doi.org/10.21203/rs.3.rs-3403588/v1

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The results shown here provide some information about electric field-induced metallic state in CuCl. It is notable that in addition to the applied electric field inducing the transition from a high-resistance state to a low-resistance state, the electric field can drive the sample back to the high-resistance state. This means that the metallic state of CuCl is out of equilibrium. In addition, the contribution of the antiferromagnetic fluctuations of Clinoatacamite to the magnetotransport properties of oxidized CuCl is evident.

field-induced metallic state

Copper chloride (CuCl)

Clinoatacamite (Cu2Cl(OH)3

A drop in resistivity from 10⁷ Ω (insulating state) to 3 Ω (metallic phase) in polycrystalline samples of Copper Chloride when were subjected to a pressure of 40 kbar at room temperature [1], but measurements carried out years later showed that the metallic state does not behave like a metal [2]. A possible explanation for this behavior observed in CuCl, an abrupt drop in electrical resistivity, is that the pressure applied produced an unstable metallic copper/insulating CuCl₂ layer interface which can be represented by the following reaction: 2CuCl → Cu + CuCl₂ [2]. Another way of inducing the transition from a state of high electrical resistance to a state of low electrical resistance in CuCl, which has been little explored, is by applying an electric field. In 1966, Gentile [3] observed a dielectric break in CuCl crystals induced by an electric field and that this behavior was possibly due to the formation of copper filaments in the form of dentrites in the CuCl crystals created by the application of the electric field. Following this line, Divakar et al. [4] showed a transition from a state of high electrical resistance to a state of low electrical resistance in pressed copper chloride powder pellets by applying voltage and it was observed that the return time to the insulating state can last days, but this is only possible when the low resistance state is maintained for 48 hours. One property of the low resistance state calculated was the temperature coefficient of resistance (α) of the low electrical resistance state, the authors found a positive value of ~ 0.004º C-1, which is very close to that of metals. Kopelevich et al. [5], showed for the first time that the application of an electric field does in fact induce a metallic state (dR/dT > 0) and this was confirmed by the electrical resistance curves as a function of temperature in CuCl. In this work, I study the normal part of the CuCl superconductor. The two main conclusions observed are that the magnetotransport properties of CuCl are Out-of-equilibrium, as well as depending on the Clinoatacamite that arises from the oxidation of CuCl.

For electrical transport measurements, samples were prepared in the form of cylindrical pellets, from CuCl powder in a steel matrix of diameter, d = 5 mm. The pressure used in the press was 15 kbar for about 10 minutes for compaction of the CuCl powder forming a pellet. With the pellets prepared, we made electrical contacts using silver paint and gold wires for magneto-transport measurements. The magneto-transport measurements were carried out in the following equipment: The PPMS-9T (Physical Properties Measurement System), manufactured by the company Quantum Design, the PPMS-14T, also manufactured by the company Quantum Design and the cryostat Janis-He4, which is manufactured by the company Janis Inc.

Magnetic measurements obtained for CuCl

During the measurements, the samples were kept in an inert atmosphere of He gas inside commercial cryostats from Janis. The equipment allows the temperature and magnetic field to be varied in the following ranges: 2 K < T < 350 K and - 9 T < H < 9 T. The electrical transport measurements were made using silver paste (Ag) electrodes placed on the top and bottom faces of the sample, as shown in (figure 1). Measurements of resistance as a function of time R(t).

The figure 2(a) shows the intermittent dependence of the applied voltage (Vg) on time and its respective transition induced by the electric field in CuCl at T = 300 K (fig. 2b). In addition to the applied electric field inducing the transition from a high-resistance state to a low-resistance state, the electric field can lead the sample back to the high-resistance state. This result shows completely out-of-equilibrium behavior.

To clarify the origin of the metastable conductive state in CuCl, we studied the dependence of resistance on temperature R(T). Figure 3 shows R(T) measured in the ohmic regime for a CuCl sample with a certain degree of oxidation. A metallic behavior is observed (dR/dT > 0) over a wide temperature range with R (T) ~ T^4/3, but around T ~ 42 K there is a minimum. Then, a new metallic behavior is observed and another minimum not shown is noticed at T ~ 8 K such that for 8 K < T < 42 K we now have R (T) ~ T³. Resistance behavior like that shown in (Fig. 3) was obtained in other CuCl samples in the low-resistance state. For a second CuCl sample, see (Fig. 4), after applying the electric field, we also observed metallic behavior of the resistance with R (T) ~ T^1.2 for a wide temperature range, as well as a minimum T ~ 18 K and a sharp drop in resistivity around T ~ 9 K.

The resistance behavior shown in (figure 4.18) and (figure 4.19) with exponents η ~ 1.3, η ~ 1.2 and η ~ 3 is characteristic of non-Fermi liquid systems of magnetic systems, i.e. it is not explained by a simple scattering mechanism. On the other hand, the theory of spin fluctuations shows that the behaviors R ~ T^1.3 [6,7,10,12,13], R ~ T^1.2 [6,7,8,10,11,12,13] and R ~ T³ [9,12,13] are due to scattering by strong spin fluctuations that possibly occur on(in) the surface/intergrain boundary of magnetic media and that are consistent with my results. Finally, electrical resistance measurements were carried out as a function of the magnetic field R(H) in the metallic state, up to 9T, for various fixed temperatures, as shown in (figure 5). The result shows a negative magnetoresistance for T < 60 K and a positive magnetoresistance for T > 60 K, showing that this crossover may be related to the coexistence of ferromagnetic and antiferromagnetic phases [14,15] that are present in CuCl due to oxidation, agreeing with the set of results presented, as well as providing evidence of the effects of weak electron localization or electron-electron interaction [16,17,18,19,20,21]. Negative magnetoresistance is a typically two-dimensional phenomenon [22,23,24], reinforcing that the magneto-transport properties in CuCl in the metallic state are possibly occurring at the surfaces/intergrain boundaries.

From the measurements of electrical resistance as a function of time in CuCl, it is concluded a behavior out of equilibrium after CuCl changes to the state of low resistance with application of gate voltage. The only way to hold the low-resistance state where superconductivity can be observed is to maintain the low-resistance state at low temperature [25,26]. In addition, one can observe a non-liquid fermi behavior of the metallic state of the low resistance state. This behavior is due to scattering by strong spin fluctuations of Clinoatacamite [25,26,27,28]. Negative magnetoresistance and a positive magnetoresistance, showing that this crossover may be related to the coexistence of ferromagnetic and antiferromagnetic phases that are present in CuCl due to oxidation.

Data Availability

The data used to support the findings of this study are available upon reasonable request from the corresponding authors.

Conflicts of Interest

The author declares that there are no conflicts of interest.

Acknowledgements

This work was carried out with the support of the Coordination for the Improvement of Higher Education Personnel - Brazil (CAPES) - Financing Code 001 for 1 year. I thank the “Ministry of Science, Technology and Innovations” and “National Council of Scientific and Technological Development” – CNPq” for the financial support granted to me for 3 years.

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Out-of-equilibrium behavior in CuCl

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