# Thickness dependent magnetotransport in ultra-thin manganite films

## Abstract

To understand the near-interface magnetism in manganites, uniform, ultra-thin films of La<sub>0.67</sub>Sr<sub>0.33</sub>MnO<sub>3</sub> were grown epitaxially on single crystal (001) LaAlO<sub>3</sub> and (110) NdGaO<sub>3</sub> substrates. The temperature and magnetic field dependent film resistance is used to probe the film’s structural and magnetic properties. A surface and/or interface related dead-layer is inferred from the thickness dependent resistance and magnetoresistance. The total thickness of the dead layer is estimated to be $`30\AA `$ for films on NdGaO<sub>3</sub> and $`50\AA `$ for films on LaAlO<sub>3</sub>.

One issue in manganite trilayer junction is the premature disappearance of magnetoresistance (MR) upon temperature increase. The MR in La<sub>0.67</sub>Sr<sub>0.33</sub>MnO<sub>3</sub> based trilayer junctions disappears above $`150K`$, well below the electrode’s Curie temperature of $`360K`$ . Recently, spin-resolved photoemission measured the spin-polarization of surface electronic density-of-state of epitaxial thin films of La<sub>0.67</sub>Sr<sub>0.33</sub>MnO<sub>3</sub> . It revealed, as a function of increasing temperature, a more rapid decrease of the surface spin polarization than the film’s overall magnetization. Both transport and photoemission experiments suggest the possible existence of a surface dead-layer with depressed magnetic order at elevated temperatures. Questions remain as to the depth of this dead-layer, and its physical origin. In this paper, we experimentally establish some estimates about the dead-layer thickness. The approach is to study the thickness dependent electrical transport, including resistance and magnetoresistance, in ultra-thin epitaxial films of La<sub>0.67</sub>Sr<sub>0.33</sub>MnO<sub>3</sub> (LSMO). To estimate the effect of lattice strain, films on two types of substrates are compared — those grown on (001) LaAlO<sub>3</sub>(LAO) and on (110) NdGaO<sub>3</sub> (NGO). The film thickness range covered by this study is between $`15\AA `$ and $`240\AA `$.

Films were grown epitaxially using laser ablation from a stoichiometric La<sub>0.67</sub>Sr<sub>0.33</sub>MnO<sub>3</sub> target. A Nd-YAG laser was used for ablation, operating in frequency-tripled mode at $`355nm`$, with a pulse energy of $`140mJ/pulse`$ at $`10Hz`$ repetition. The deposition rate was about $`0.6\AA /\mathrm{sec}`$. A series of films were made in the thickness range between $`15\AA `$ and $`240\AA `$. Two substrates, one LAO and one NGO, each $`1cm\times 2mm\times 0.5mm`$ in size, were loaded side-by-side for simultaneous deposition at each thickness. The substrate holder’s temperature during growth was $`750C`$, and the growth ambient consisted of $`300m\tau `$ of oxygen at a flow rate of $`50sccm`$.

The films were subsequently coated with four in-line contact pads, $`1mm`$ diameter and $`2.2mm`$ apart from each other, for transport measurement. These contact pads, usually silver or gold, about $`1000\AA `$ thick, were sputter deposited through a stencil mask. The four-point resistance thus measured was assumed to be the resistance-square $`R_{\mathrm{}}`$. The film thickness was deduced from deposition time normalized to calibration runs.

A summary of the temperature dependent film resistivity, $`\rho (T)`$, is shown in Fig.1(a). An increase of resistivity is seen as the film thickness is decreased, for films both on NGO and on LAO. Films on LAO show faster increase in resistivity upon thickness reduction. At $`15\AA `$, the $`\rho (T)`$ for film on NGO just begins to show a negative temperature slope at $`14K`$, with its $`\rho (T)`$ peak temperature moved down to around $`240K`$ from the bulk value of $`360K`$. The $`\rho (T)`$ for the $`15\AA `$ film on LAO, on the other hand, already shows a pronounced resistivity rise for $`T<150K`$. The increase of resistivity with decreasing film thickness indicates the presence of a dead-layer with reduced conductivity. This can be seen more clearly in the thickness dependence of the film’s total conductance $`G`$ (defined as $`G=1/R_{\mathrm{}}`$, where $`R_{\mathrm{}}`$ is the film’s 4-probe-measured resistance).

Fig.1(b) shows the thickness dependence of $`G`$ at $`T=14K`$, the lowest temperature the film resistance was measured down to. A linear thickness dependence of $`G`$ is expected. If the films were uniform, the line should intercept the horizontal axis at zero thickness. Data in Fig.1(b) shows a linear thickness dependence for films thicker than $`60\AA `$, but with a finite intercept. This intercept represents the total thickness of the dead-layer(s), if these dead-layers are much less conducting than the center part of the film. The total dead-layer thickness according to this estimate is around $`30\AA `$ for films grown on NGO, and around $`50\AA `$ for films on LAO. This thickness estimate combines the contribution of the surface dead-layer and the film-substrate interface dead-layer. It is not yet clear whether the thicknesses of these two types of dead-layers are the same for a given film.

Next we rule out two other possibilities that could contribute to a thickness-dependent film resistivity, namely the film’s strain variation, and the incomplete film coverage over the substrate during initial growth.

Fig.2 shows results of X-ray diffraction measurements on lattice parameters of the films. Both out-of-plane and in-plane lattice parameters were measured, using normal and grazing incident X-ray diffraction. The film’s unit cell dimensions deviate from their bulk values for the entire thickness range, presumably due to the combined effect of epitaxial strain and oxygen defects. The deviation is greater for films on LAO than for films on NGO. A thickness-dependent change of lattice parameter is seen. This change, $`<0.76\%`$ for out-of-plane, $`<1.2\%`$ for in-plane lattice in the case of film on LAO, is small compared to the difference in corresponding lattice parameters between films grown on LAO and NGO.

The main contribution to resistivity’s thickness dependence is not from film strain variation. This can be seen by comparing the strain-field difference and resistivity difference for films grown on different substrates. For the $`240\AA `$ film on LAO and NGO, their out-of-plane lattice constants differ from bulk value by $`2.12\%`$ and $`0.83\%`$, respectively. This is a difference in strain-field of over a factor of $`2.5`$ in the out-of-plane direction. Yet their averaged resistivity at $`14K`$ differ only by a factor of $`1.3`$, with dead-layer effects included. Thus, a relatively small strain variation of $`0.2\%0.5\%`$ over the thickness range is not expected to cause much variation to the resistivity. The observed thickness-dependent resistivity varies over an order of magnitude, and can not be explained away by strain variation.

The continuous coverage of such thin films over the substrate surface was confirmed using atomic force microscopy (AFM). Fig.3 shows a morphology image of two $`30\AA `$ films, one on LAO, another on NGO. From these images the film’s surface roughness is estimated to be about $`5\AA `$ peak-to-peak in both cases, indicating continuous film coverage without large voids.

With strain effect and initial coverage issues resolved, we thus conclude that the thickness-dependent resistivity is most likely caused by the presence of a surface and/or interface dead-layer.

The MR of the films also show thickness and substrate dependence. Fig.4 shows MR vs. temperature for films on NGO and LAO at different thicknesses. Two types of behaviors are distinguishable. In the first type the MR rises monotonically as a function of temperature. This is what normally expected, since the Curie temperature of bulk LSMO is around $`360K`$ which is above the maximum measurement temperature of $`300K`$. This normal behavior is associated with thicker films. The second type of MR vs. temperature shows a peak between $`100200K`$. This only appears in very thin films ($`15\AA `$ film on NGO, $`30`$ and $`60\AA `$ film on LAO). It is the signature MR behavior of the dead-layer. The peak temperature in MR could be used as an empirical estimate to the Curie temperature, $`T_c`$ of the dead-layer, which thus comes to be around $`100200K`$.

In conclusion, we have obtained an experimental estimate of the total thickness of the dead-layers associated with the surface and film-substrate interface in epitaxial films of LSMO on NGO and LAO substrates. The total dead-layer thickness in these two cases are estimated to be about $`30\AA `$ and $`50\AA `$, respectively. The dead-layer has a magnetoresistance peak temperature of around $`100`$ to $`200K`$, and is likely to have a magnetic Curie temperature in the same range.

JZS wishs to thank Pat Mooney for some early X-ray analysis. CBE would like to acknowledge support from NSF Grant No. DMR9802444 and from NSF’s Young Investigator Award.