# Residual resistivity ratio and its relation to the magnetoresistance behavior in LaMn2Ge2-derived alloys

## Abstract

Results of low temperature magnetoresistance ($`\mathrm{\Delta }\rho /\rho `$) and isothermal magnetization (M) measurements on polycrystalline $`\mathrm{𝑓𝑒𝑟𝑟𝑜𝑚𝑎𝑔𝑛𝑒𝑡𝑖𝑐}`$ (T<sub>C</sub> close to 300 K) natural multilayers, LaMn<sub>2+x</sub>Ge<sub>2-y</sub>Si<sub>y</sub>, are reported. It is found that the samples with large residual resistivity ratio, $`\rho `$(300K)/$`\rho `$(4.2K), exhibit large positive magnetoresistance at high magnetic fields. The Kohler’s rule is not obeyed in these alloys. In addition, at 4.5 K, there is a tendency towards linear variation of $`\mathrm{\Delta }\rho /\rho `$ with magnetic field with increasing $`\rho `$(300K)/$`\rho `$(4.2K); however, the field dependence of $`\mathrm{\Delta }\rho /\rho `$ does not track that of M, thereby suggesting that the magnetoresistance originates from non-magnetic layers. It is interesting that these experimental findings on bulk polycrystals are qualitatively similar to what is seen in artificially grown multilayer systems recently.

The investigation of magnetic multilayers has been a field of active interest in view of the giant magnetoresistance behaviour (GMR) exhibited by these systems. The physics behind electron transport in these systems is not yet fully understood. Though the magnetic multilayers typically show  large negative magnetoresistance, $`\mathrm{\Delta }\rho /\rho `$, (defined as \[$`\rho `$(H)-$`\rho `$(0)\]/$`\rho `$(0) where H is the applied magnetic field), there have been recent reports of positive $`\mathrm{\Delta }\rho /\rho `$ of equally large magnitude in some systems, e.g. Dy/Sc superlattices with Dy being magnetic, and non magnetic Cr/Ag/Cr trilayers. In these systems, the application of an external magnetic field modifies the electron scattering/reflection across the interfaces; hence interfacial contribution to resistivity plays an important role in determining the $`\mathrm{\Delta }\rho /\rho `$ behavior as evidenced by higher $`\mathrm{\Delta }\rho /\rho `$ values if the mean free path ($`\mathrm{}`$) is large. There is a breakdown of Kohler’s rule and there is an inverse correlation between the residual resistivity ratio (RRR= $`\rho `$(300 K)/$`\rho `$(4.2 K)) and large positive magnetoresistance (LPMR) in Ref. 5.

We have earlier reported LPMR behavior, qualitatively similar to the Dy/Sc and Cr/Ag/Cr systems, on natural multilayer systems, viz., polycrystalline materials with a layered structure. These systems are: RMn<sub>2</sub>Ge<sub>2</sub> (R= Sm, La) crystallizing in the ThCr<sub>2</sub>Si<sub>2</sub>-type tetragonal structure, containing atoms in the layered sequence Th-Si-Cr-Si-Th-Si-Cr-Si-Th along the c-axis. The finding of note is that the sign of $`\mathrm{\Delta }\rho /\rho `$ is positive at low temperatures inspite of the fact that the compounds are ferromagnetic with the Curie temperature around 300 K. Here, we report the results of our studies on several annealed and as-cast alloys derived from the compound, LaMn<sub>2</sub>Ge<sub>2</sub>, to look for correlations between RRR and the magnitude as well as the field dependence of $`\mathrm{\Delta }\rho /\rho `$, seen in those multilayers. We induce a change in RRR by small variations in Mn-Ge ratio, small chemical substitutions at Mn/Ge sites and in the sample-preparative conditions.

The polycrystalline samples, LaMn<sub>2+x</sub>Ge<sub>2-y</sub>Si<sub>y</sub>, mentioned in table 1 (except the sample 1, which was prepared by arc melting), were prepared by melting together constituent elements in an induction furnace. Slight excess of Mn was added to compensate for weight loss while melting. In the present studies, we have adopted an induction melting method for the preparation of samples since this method is found to allow better control over Mn loss compared to the arc melting method. For each sample, a part of the as-cast ingot was homogenised in an evacuated sealed quartz tube at 800 C for 1 week. X-ray diffraction patterns (Cu K<sub>α</sub>) confirm single phase nature of the alloys. The basal plane parameter is close to 4.2Å and the c-parameter is close to 11Å in all the alloys. The electrical resistivity ($`\rho `$) measurements were performed by a conventional four-probe method employing silver paint for making electrical contacts of the leads with the samples, with the direction of the current being the same as that of H (longitudinal mode). The isothermal magnetization (M) was measured at 4.5 K using a commercial (Quantum design Inc.) superconducting quantum interference device.

In Table 1, we summarize the values of RRR and $`\mathrm{\Delta }\rho /\rho `$ to highlight the disorder effect on the $`\mathrm{\Delta }\rho /\rho `$ of the LaMn<sub>2</sub>Ge<sub>2</sub>-derived alloys. It is interesting to note that the LaMn<sub>2</sub>Ge<sub>2</sub> sample prepared by induction method (sample 6) is characterized by a smaller magnetoresistance compared to the previous sample prepared by arc melting (sample 1). Thus different preparative conditions introduce different degree of defects and disorder in the samples. It is clear that, as the RRR decreases, the LPMR effect as seen at 4.5 K is gradually washed out, viz., for RRR $`<`$ 10, the low temperature $`\mathrm{\Delta }\rho /\rho `$, though positive, is of small magnitude, showing that disorder, as inferred from the magnitude of RRR, kills the LPMR behavior in these systems. It appears that the ferromagnetism of Mn layer in LaMn<sub>2</sub>Ge<sub>2</sub> plays no direct role on the magnetoresistance, as otherwise one would have seen negative magnetoresistance as is usually the case with polycrystalline ferromagnetic materials; this is further corroborated by a comparison of $`\mathrm{\Delta }\rho /\rho `$ with the isothermal magnetization behavior at 4.5 K: M saturates for small values of H for all samples (typical behavior is shown for a few samples in Fig. 2c). Thus, as in the case of Dy/Sc multilayer, M and $`\mathrm{\Delta }\rho /\rho `$ do not track each other. At this juncture, it may be stated that the electrical conduction may be favored along the basal plane as indicated by single crystal investigations on SmMn<sub>2</sub>Ge<sub>2</sub>. However, the non-magnetic layers, but not the Mn layer, are the ones which contribute to magnetic response from the above arguments. The fact that we have observed LPMR even in nonmagnetic alloys belonging to the same structure if RRR is large, supports the idea that the magnetic Mn layer is not responsible for the observed behavior. However, the choice of a ferromagnetic layered compound enables us to draw definitive conclusions on the selective role of nonmagnetic layers on the magnetoresistance behavior; though we have seen large values in layered antiferromagnets in the past, such a conclusion was not possible from those data, as antiferromagnetism can also give rise to positive values. We further speculate that the non-magnetic layer acting as an interface is the one that contains Ge, since low temperature positive magnetoresistance could be observed even in the ferromagnetic, isomorphous Sm sample in which Sm layer is ferromagnetic at 4.2K.

In Fig. 1b and 1d we show the temperature dependence of $`\mathrm{\Delta }\rho /\rho `$, derived from the data shown in Fig 1a and 1c respectively. The values of $`\mathrm{}`$ have also been evaluated from the $`\rho `$ data from the knowledge of the unit-cell density (6.8 gm/cc) and the number of conduction electrons (estimated to be 19, assuming tri, tetra, and tetra positive La, Mn and Si/Ge respectively) within the Sommerfeld theory of conduction. The assumption of theoretical mass density and uncertainties in the absolute determination of $`\rho `$, for instance, due to microcracks in the sample, and in the number of conduction electrons introduce errors in the derived values of $`\mathrm{}`$. Therefore, not much significance may be attached to these values of $`\mathrm{}`$. For qualitative arguments, $`\mathrm{}`$ thus obtained for the two most magnetoresistive samples are shown in the figures 1b and 1d (continuous lines through the data points). The point to be noted is that the $`\mathrm{}`$ closely follows $`\mathrm{\Delta }\rho /\rho `$ as a function of temperature. It may be remarked that the value of $`\mathrm{}`$ at which significant positive $`\mathrm{\Delta }\rho /\rho `$ starts appearing is above 3Å. We derived the same cut-off limit from the low temperature $`\rho `$ data of all the samples (see table 1) as well. Therefore, though the absolute values of $`\mathrm{}`$ may not be reliable, on this basis, one can draw a conclusion that there is a close relationship between the magnitude of the magnetoresistance and $`\mathrm{}`$. However, for the reason mentioned above, we refrain from drawing more conclusions from the derived $`\mathrm{}`$ values.

In Fig. 2a and 2b, we present the results of $`\mathrm{\Delta }\rho /\rho `$ as a function of H at 4.5 K for some of the samples which exhibit significant magnetoresistance. It is to be remarked that the plot of $`\mathrm{\Delta }\rho /\rho `$ versus H/$`\rho `$ is not a single line (shown for one sample in Fig. 3) and thus the Kohler’s rule is found to break down - this is similar to the observations in Cr/Ag/Cr trilayers. For the most magnetoresistive alloy (sample 1), the field dependence is linear in the entire field range of measurement, instead of a classical quadratic dependence. For samples 2 and 3, we observe a deviation from this linearity at low fields (shown in the inset of Fig. 2a for sample 2) beyond which there is a linear behaviour. The low field quadratic dependence could be observable for samples 3 and 4 with still smaller RRR values. Thus there is a tendency towards classical quadratic dependence with a decrease of RRR. (In one of the samples, LaMn<sub>1.9</sub>Ge<sub>2.1</sub> (I) in Fig. 2b, we see a convex curvature around a higher field of 20 kOe, the reason for which is unclear). Thus, the low field linear dependence of magnetoresistance appears to be a signature of relatively better crystallographic order in these alloys. In the same way, in the Cr/Ag/Cr multilayers, an increase in RRR brings about a transition from quadratic to linear behavior in the $`\mathrm{\Delta }\rho /\rho `$ vs H plots, in addition to increasing the magnitude of observed $`\mathrm{\Delta }\rho /\rho `$. At this juncture, we would like to recall a recent report on nonmagnetic bulk silver chalcogenides of the type Ag<sub>2+δ</sub>(Se,Te): For stoichiometric ($`\delta `$= 0) samples, there is no significant magnetoresistance; however, possible introduction of electronic defects for $`\delta `$ $`>`$ 0 gives rise to LPMR behavior. In these systems also, the magnetoresistance is found to exhibit an almost linear dependence on the applied field. Our samples being magnetic, the following point may have to be considered in addition to various other explanations which can be offerred to the above non-magnetic systems; that is, in large RRR alloys, the internal magnetic fields due to ferromagnetism of Mn is large enough that one is well above the quadratic region already in zero external field; however, the deviation from the linearity in smaller RRR samples may possibly be due to randomness of this local field caused by disorder.

In conclusion, we have brought out the effect of residual resistivity ratio on the magnitude of the magnetoresistance and its dependence on H at low fields in LaMn<sub>2</sub>Ge<sub>2</sub>-derived alloys, resembling those of some multilayers. The expected negative sign of $`\mathrm{\Delta }\rho /\rho `$ is not seen in any of these ferromagnetic alloys and this observation, alongwith the isothermal magnetization behavior which is different from that of $`\mathrm{\Delta }\rho /\rho `$, is taken as the evidence for selective magnetic field response from the non-magnetic layers. The present results appear to render an experimental support to a proposal that these layered compounds may serve as model systems for artificial multilayers. It is however not clear whether there are unusual domain wall effects in such ferromagnetic alloys, an aspect which is yet to be settled even in simple ferromagnetic systems. In this sense, it is worthwhile to study the $`\mathrm{\Delta }\rho /\rho `$ behaviour on clean single crystal samples of RMn<sub>2</sub>Ge<sub>2</sub>(Si<sub>2</sub>); this will also enable to comfortably probe the magnetoresistance in a geometry with the current perpendicular to the plane, an important investigation difficult to make on multilayers. In addition, the studies on artificially grown layers of the constituent elements in the sequence present in the crystal structure may be rewarding. We hope that this work will motivate further investigations of such natural multilayer systems.