3B2v7:51c                                                                        ED:Chanakshi=brr
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                                          Journal of Magnetism and Magnetic Materials ] (]]]]) ]]]­]]]
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7     Epitaxial growth, alloying and magnetic structure of interfaces
9                                                  in Fe/Cr (0 0 1) superlattices
11                                            V. Uzdina, W. Keuneb,*, M. Walterfangb
13                              a St. Petersburg State University, ICAPE, 14 linia V.O. 29, 199178, St. Petersburg, Russia
            b Laboratorium f.ur Angewandte Physik, Gerhard-Mercator-Universit.at Duisburg, Lotharstr. 65, D-47048 Duisburg, Germany
15

17
      Abstract
19
         Fe/Cr(0 0 1) superlattices containing two-monolayers thick 57Fe probe layers at the Fe/Cr (Fe-on-Cr) or Cr/Fe (Cr-
21    on-Fe) interfaces were studied using conversion electron M.ossbauer spectroscopy (CEMS). For the interpretation of
      the CEMS data of superlattices annealed at different temperatures, we performed theoretical modeling of their chemical
23    and magnetic structure. Roughness and interface alloying were introduced to the model by algorithms of epitaxial
      growth, which included ballistic deposition with subsequent floating of some atoms on the surface. Self-consistent
25    calculations of magnetic moments within the periodic Anderson model confirmed the proportionality between hyperfine
      fields and magnetic moments. For the explanation of the evolution of CEM spectra versus annealing temperature,
27    the difference in the melting points of bulk Fe and Cr has to be taken into account. r 2001Published by Elsevier
      Science B.V.
29
      Keywords: M.ossbauer spectroscopy; Multilayers; Annealing; Magnetic structure; Fe­Cr
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33
         In Fe/Cr multilayers antiferromagnetic interlayer                       recent calculations of magnetic moments in Fe/Cr              57
35    exchange coupling and giant magnetoresistance                              multilayers with interface alloying [4] did not confirm
      (GMR) were discovered for the first time. Despite the                      the assumption that a large spectral intensity of the 20-T    59
37    large efforts which were undertaken for studying the                       satellite means that the interface is atomically smooth.
      correlation between their interface structure and macro-                   On the contrary, our results showed that this peak            61
39    scopic magnetic and transport properties, many aspects                     corresponds to short-range interdiffused Fe atoms inside
      are still contradictory. In particular, the value of the                   the Cr spacer layers, but not far away from the interface.    63
41    GMR effect was found to correlate with the spectral                        Therefore, its relative spectral intensity has to increase
      contribution (spectral area) of the satellite Zeeman                       upon interface alloying. According to our recent              65
43    sextet in the conversion electron M.ossbauer (CEM)                         findings, earlier conclusions about the role of interface
      spectra [1] that corresponds to a hyperfine field, Bhf; of                 and bulk scattering in the GMR effect should be revised.      67
45    20 T. According to the traditional interpretation for Fe/                  We emphasize in this context that the interpretation of
      Cr multilayers, the peak at 20 T in the hyperfine field                    experimental data is an ambiguous problem, and for the        69
47    (hff) distribution, PðBhfÞ; originates from Fe atoms at                    understanding of real mechanisms of epitaxial growth
      the ideally flat (0 0 1) interface with four nearest                       and interface alloying in Fe/Cr multilayers, experimental     71
49    neighbours
                                                                                                                                               73
51
                                                                                                                                               75
53
        *Correspo         UNCORRECTED PROOF
                      and one second neighbour Cr atoms [1­3].                   and theoretical studies have to be used together to
      This interpretation seems to allow the correlation of                      achieve self-consistency in details.
      transport properties, interface roughness and the ratio                       Here, we present results of a CEMS investigation after
      between interface and bulk scattering [1]. However, our                    isochronal annealing of Fe/Cr(0 0 1) superlattices with
                                                                                 two-monolayers (ML) thick 57Fe probe layers (95%
                     nding author. Tel.: +49-203-379-2387; fax: +49-             enriched) placed either at Fe/Cr interfaces (Fe-on-Cr or      77
55    203-379-3601.                                                              ``lower'' interfaces) or at Cr/Fe interfaces (Cr-on-Fe or
          E-mail address: keune@uni-duisburg.de (W. Keune).                      ``upper'' interfaces), and of theoretical modeling of         79

      0304-8853/01/$ - see front matter r 2001Published by Elsevier Science B.V.
      PII: S 0 3 0 4 - 8 8 5 3 ( 0 1 ) 0 0 8 8 8 - 5



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1     Table 1                                                                                                                                      57
      Position of the fitted Gaussian peaks (satellites) in the hff distribution (first column) and their relative spectral area (in %) for the
3     sample with the 57Fe probe layers at the upper (Cr-on-Fe) and lower (Fe-on-Cr) interfaces after isochronal annealing at different            59
      temperatures
5     B                                                                                                                                            61
           hf (T)         RT                2001C             3001C             4001C              4501C              5001C             5501C

7     Upper interface: Cr on Fe                                                                                                                    63
      33.7(%)             17.8              21.6              21.9              22.2               23.3               21.4              22.5
9     31.3(%)             16.1              13.3              12.8              12.1               12.5               20.2              28.3       65
      28.5(%)             13.9              13.9              14.7              16.3               14.0               17.1              30.4
      25.6(%)             11.3              12.9              12.0              12.6               13.0               10.6
11    23.1(%)             11.3              12.0              13.1              10.1               11.2                8.5                         67
      20.3(%)             15.1              11.1              10.0               9.9               11.2               11.9              15.5
13    16.5(%)                               12.1              12.4              13.9               12.2                8.2                         69

15    Lower interface: Fe on Cr                                                                                                                    71
      33.8(%)             29.6              30.7              30.4              32.3               31.3               30.0              25.6
17    31.4(%)             15.8              13.9              15.3              14.5               14.9               18.1              21.9       73
      28.7(%)             11.3              12.9              13.1              13.9               13.2               15.1              17.2
19    25.5(%)             10.9              11.6              10.5               9.8                9.7               10.1              13.6       75
      23.0(%)             10.4               9.7               9.6               8.9               11.1                7.2
21    20.0(%)             10.7              11.1              11.9              13.7               10.4               11.1              17.4       77

23                                                                                                                                                 79

25    interface alloying in these systems during the sample                   to the sum of the areas of the fitted Gaussian peaks)                81
      preparation and annealing process.                                      obtained for each annealing temperature is only slightly
27          Superlattices of composition MgO(0 0 1)/Cr(50 (A)/                less than 100% of the total experimental spectral area               83
      [57Fe(2 ML)/natFe(12 ML)/Cr(8 ML)]15 (lower interfa-                    according to Table 1.
29    ces) or MgO(0 0 1)/Cr(50 (A)/[natFe(12 ML)/57Fe(2 ML)/                    The hff distributions for the two types of interfaces              85
      Cr(8 ML)]15 (upper interfaces) were epitaxially grown                   prove to be remarkably different (Table 1). For the Fe-
31    at Ts ¼ 433 K by ultrahigh-vacuum (UHV) depo-                           on-Cr interface, the relative area of the ``bulk'' peak              87
      sition of the metals on epipolished MgO(0 0 1) sub-                     (near 33.8 T) is found to be about 30%, whereas for the
33    strates, as described in detail in Ref. [4]. (natFe=Fe                  Cr-on-Fe interface it is only about 20%. Other satellite             89
      metal of natural 57Fe abundance, 2.1%). Characteriza-                   peaks are narrower and generally yield less contribution
35    tion by low and high angle X-ray diffraction demon-                     (except for the peak near 31.4 T) to the total spectrum              91
      strates the high-quality superlattice structure of our                  for the lower interface as compared with the upper
37    samples [4].                                                            interface. The largest difference was detected for the               93
            CEM spectra were measured at room temperature as                  peak near 20 T: before annealing it contributes less than
39    described in Ref. [4]. Typical CEM spectra and hff                      11% of the total spectral area for the lower interface and           95
      distributions before annealing of samples with either                   more than 15% for the upper one. An additional peak
41    ``upper'' or ``lower'' interfaces were shown in Fig. 2(a) of            corresponding to a hff of 16.5 T appears in PðBhfÞ of the            97
      Ref. [5]. One-hour isochronal annealing of the samples                  upper interface after annealing at 2001C and above. In
43    was performed in UHV in steps of increasing tempera-                    general, for the upper interface the low-field distribution          99
      tures between 2001C up to 5501C, when strong bulk                       was found to be essentially broader and the amplitude of
45    diffusion starts. The CEM spectra and hff distributions                 the 20 T peak itself was smaller than that for the lower             101
      (not shown here) are of similar statistical quality as                  interface. Annealing of the samples up to a temperature
47    those displayed in Refs. [4] (Figs. 4 and 5) and [5]                    of 4501C does not crucially modify the CEM spectra. A                103
      (Fig. 2(a)). The obtained hff distributions have been                   small increase of the ``bulk'' contribution (33.8 T peak)
49    decomposed                                                                                                                                   105

51                                                                                                                                                 107
53                     UNCORRECTED PROOF
                      by least-squares fitting into several (here:            and of the low-field contribution (20 T peak for the
      six or seven) Gaussian functions (satellites) with                      lower interface, and the sum of the 20.3 and 16.5 T peaks
      individual widths and spectral areas. Our results, i.e.                 for the upper interface) up to a temperature of 4001C
      the average position of the Gaussian satellite lines and                reflects the weak (short-range) diffusion of 57Fe atoms
      the corresponding relative spectral areas (in %, relative               from the interface towards the inside of the Fe and Cr               109
      to the total experimental spectral area), obtained after                slabs, respectively. A similar result concerning a weak
55    annealing both types of samples at different tempera-                   increase in area of the 20 T satellite line after annealing          111
      tures, are given in Table 1. The total area (corresponding              at 3001C was reported by Kopcewicz et al. [3]. Their



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1     interpretation is based on the assumption that this hff            between atoms of different chemical elements, and gives            57
      corresponds to Fe atoms in the ``flat'' interface, and they        a natural explanation of the change of the hff distribu-
3     had to conclude that there is in-plane diffusion inside the        tion on 119Sn atoms in V/Cr superlattices versus the               59
      superlattice during annealing which leads to smoothing             position of the 119Sn probe layer inside the Cr spacer [10].
5     of the interfaces. However, this is an unlikely process,              We conclude that the difference between the hff                 61
      and our finding that the 20 T peak (as well as the 16.5 T          distributions from lower and upper interfaces in Fe/Cr
7     peak) originates from Fe atoms embedded in the Cr                  superlattices can be explained without consideration of            63
      spacer near the interface [4] gives a more natural                 Fe and Cr melting points. However, the different melting
9     explanation of the annealing experiment.                           points play an important role in the evolution of PðBhfÞ           65
        Another problem is the explanation of the differences            versus annealing, especially at high temperature, when
11    in PðBhfÞ for lower and upper interfaces. This difference          bulk diffusion starts. After annealing at 5001C, we                67
      was reported earlier [5,6], and it was assumed that                observe a remarkable increase of the spectral area of the
13    interface alloying is governed by the binding energies             second satellite line (31.3 T­31.4 T ) in both types of            69
      between the substrate and ad-atom material, which, as a            interfaces. This means that individual Cr atoms start to
15    first approach, are proportional to the melting points of          penetrate into the Fe layers. There is no similarly                71
      the solids [6]. The melting point of Cr is higher than for         remarkable increase of the low-field contribution at
17    Fe and, therefore, interface mixing for the lower                  5001C, which would correspond to isolated Fe atoms in              73
      interface might be less significant as compared with the           the Cr spacer. The latter process starts only after
19    upper one [6]. However, recent investigations of epitaxy           annealing at 5501C for the lower (Fe-on-Cr) interface              75
      of Fe on Cr [7] and Cr on Fe [8] using scanning                    whereas for the upper (Cr-on-Fe) interface, the total
21    tunneling microscopy demonstrate the occurrence of                 low-field contribution (at 20.3 and 16.5 T) decreases              77
      alloying on both interfaces. Modeling of the epitaxial             strongly with annealing at 5501C. Consequently 57Fe
23    growth with the algorithm of simple ballistic deposition           atoms at the upper interface do not penetrate deeply (far          79
      cannot reproduce the differences between interfaces [4].           away from the interface) into the Cr spacer even at such
25    Now, we developed a new algorithm [9] for interface                a high annealing temperature. Although the observed                81
      alloying, which includes ballistic deposition with con-            starting temperature of 500­5501C for bulk diffusion is
27    sequent rising up of some atoms on the surface. It allows          remarkably lower then the melting points of bulk Fe and            83
      to reproduce the main differences between lower and                Cr, it is closer to the Fe melting point. That is why Cr
29    upper interfaces. We assume that site exchange of atoms            atoms can diffuse into the Fe slabs, which are nearer to           85
      and their diffusion take place only at the surface during          the liquid state, but Fe atoms do not diffuse into the
31    the epitaxial growth and there is no internal bulk                 solid Cr spacer. This conclusion is in agreement with              87
      diffusion. We start from the structure obtained by the             recent calculations of vacancy formation energies which
33    algorithm of simple ballistic deposition. Then in every            are found to be larger for Cr than for Fe [11].                    89
      layer, we choose a definite fraction (B) of atoms using a
35    random procedure, and layerwise, starting from the                    V.U. appreciates financial support from the Alexan-             91
      bottom, this fraction of atoms was exchanged in every              der von Humboldt foundation and the MML01
37    pair of neighbouring layers. The parameter Bo1                     symposium organizers.                                              93
      determines the intensity of interface alloying. Such a                This work was partially supported by the Russian
39    scenario automatically leads to the asymmetry of the               Ministry of Higher Education (grant E00-3.4-547), the              95
      interface: atoms could float up on several layers, but did         program ``Universities of Russia: fundamental re-
41    not move down due to suppression of diffusion in the               searches'' (project 015.01.01.083) and the Deutsche                97
      inner layers below the surface. For the probe layer at the         Forschungsgemeinschaft (SFB 491Bochum/Duisburg).
43    lower (Fe-on-Cr) interface, 57Fe atoms will float and                                                                                 99
      move into the natFe slab, thus increasing the intensity of         References
45    the bulk-like peak in PðBhfÞ: At the upper (Cr-on-Fe)                                                                                 101
      interface, these 57Fe atoms will float and move into the            [1] R. Schad, P. Belien, G. Verbanck, K. Temst, V.V.
47    Cr spacer, thus increasing the low-field contribution in                Moshchalkov, Y. Bruynseraede, B. Bahr, J. Falta,              103
      PðBhfÞ: Self-consistent calculations of the magnetic                    J. Dekoster, G. Langouche, Europhys. Lett. 44 (1998) 379.
49    moment                                                              [2] F.      Klinkhammer,    Ch.    Sauer,    E.Yu.    Tsymbal,    105

51                                                                                                                                          107
53                   UNCORRECTED PROOF
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                     UNCORRECTED PROOF