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TMP 18 D1
TMP 18 D1
TMP 18 D1
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013511-2 Lee et al. J. Appl. Phys. 104, 013511 共2008兲
共HRTEM兲 was carried out using the JEOL JEM-ARM1250 is also apparent that the volume fraction of the a-axis do-
operated at 1.25 MV with 0.12 nm point-to-point resolution. mains increased and their aspect ratio decreased with anneal-
In analyzing TEM results, the a- and c-axis directions were ing temperature.
distinguished from each other. However, since the YBCO
structure is known to be heavily twinned,11,12 the a- and IV. DISCUSSION
b-axis directions were not distinguished from each other, and
hence the orientation of grains whose c-axis directions are The initial YBCO films deposited on the substrate at
parallel to the surface is referred to as the a-axis orientation. 780 ° C possibly had a tetragonal structure with the c-axis
direction normal to the film surface because the substrate
temperature is above the tetragonal-orthorhombic transition
III. RESULTS temperature, about 700 ° C at ⬃1 atm of oxygen. The sub-
strate temperature of 780 ° C is thought to be high enough to
The plan-view TEM images from the YBCO annealed at activate volume diffusion of the deposit, and so the orienta-
500 ° C and from those annealed at 500 ° C and subsequently tion of the deposit could be dominated such that the mini-
annealed at 400 ° C or 200 ° C are shown in Fig. 1. The film mum surface-energy plane of the film is parallel to the film
annealed at 500 ° C was c-axis oriented and revealed many surface.13 The minimum surface-energy plane of tetragonal
twin boundaries 关Fig. 1共a兲兴. However, in the film annealed at YBCO is not known. On the other hand, the minimum
500 ° C and subsequently annealed at 400 ° C for 3 h, as surface-energy plane of superconducting orthorhombic
shown in Fig. 1共b兲, the a-axis domains developed in the YBCO is known to be the 共001兲 plane.10 A slight difference
c-axis matrix. The a-axis domains assumed a rectangular in structure between the two phases leads us to suppose that
shape and in some areas two domains met each other at 90°. the tetragonal YBCO has the minimum surface energy along
The selected area diffraction pattern 共inset兲, whose zone axis the 共001兲 plane. The c-axis orientation could be inherited to
was nearly parallel to the c-axis direction of the matrix orthorhombic YBCO deposits after annealing at 500 ° C for
共关001兴兲, included both an a-axis domain and the c-axis ma- 1 h in oxygen in agreement with the observed result 共Fig. 1兲.
trix within the selected area indicated by “O.” Two extra However, when the c-axis YBCO deposits were an-
spots between the fundamental reflections arose from the nealed at 400 or 200 ° C, the a-axis domains developed in
a-axis domain, the d spacing between the nearest spots cor- the c-axis YBCO matrix, as already mentioned. This is con-
responding to the interplanar spacing of the 共001兲 planes tradictory to the surface-energy minimization criterion. We
共1.17 nm兲. The pattern indicates that the long edges of the attribute the evolution of the a-axis domains to the strain
a-axis domains are parallel to their 共001兲 planes and run energy developed in the deposits during cooling from the
along the a-axis direction of the c-axis matrix. The c-axis deposition temperature and the postdeposition heat treat-
direction of the a-axis domains is indicated by arrows. The ments. Since the thermal expansion coefficient of YBCO
plan-view HRTEM image of two a-axis domains meeting 共13.4⫻ 10−6 / K兲 共Ref. 14兲 is higher than that of SrTiO3 共11
each other at 90° 关Fig. 1共c兲兴 clearly shows the interplanar ⫻ 10−6 / K兲 共Ref. 14兲, the YBCO film would be tensile
spacing of the 共001兲 planes, d = 1.17 nm. After annealing at stressed when cooled from the elevated temperatures. An-
200 ° C, the a-axis domains formed a clear network struc- other source of stress is a possible temperature gradient be-
ture, as shown in Fig. 1共d兲, and the width of the a-axis do- tween the substrate/film interface and the film surface. Actu-
mains was approximately 150 nm, which is smaller than that ally, Westerheim et al.15 measured the temperature of the
of the specimen annealed at 400 ° C 共280 nm on average兲. It surface of a 200-nm-thick YBCO film grown on LaAlO3 to
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013511-3 Lee et al. J. Appl. Phys. 104, 013511 共2008兲
TABLE I. Young’s modulus 共GPa兲 as a function of angle ␥ 共deg兲 along the 共001兲 plane.
␥ 0 10 20 30 40 45 50 60 70 80 90
E共001兲 163 166 173 184 192 195 196 193 186 181 178
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013511-4 Lee et al. J. Appl. Phys. 104, 013511 共2008兲
FIG. 3. 共Color online兲 共a兲 A cube whose edge has unit length in the c-axis V. CONCLUDING REMARKS
YBCO deposit for the calculation of the strain energy per unit volume. 共b兲
Young’s modulus along the 共001兲 plane is Ē共001兲. 共c兲 Now the cube is re- In summary, the strain energy minimization leads to the
placed by another cube of the same YBCO with a different orientation. nucleation and growth of the a-axis domain and its aniso-
Young’s modulus along both the edge of the new cube and the deposit tropic shape. It explains consistently the thickness and tem-
surface must be Ē共001兲. Let the Young’s modulus along the deposit surface perature dependence of the texture evolution previously re-
and normal to Ē共001兲 be E. ported. Our results suggest that the elastic anisotropy of the
orthorhombic YBCO should be considered as an important
Ē共001兲 be E. 关see Fig. 3共c兲兴. Then the strain energy of the cube factor in controlling the morphology and texture of the depo-
sition structure.
becomes w2 = 21 共Ē共001兲 + E兲2. The strain energy released by
the replacement process is thus
The strain-energy release ⌬w can be maximized when E is We thank Ms. Ute Salzberger for the TEM specimen
the lowest. The lowest value of E is Ec. In other words, the preparation. The help at the ARM of Mr. Rainer Höschen is
strain-energy release can be maximized when Ec of the sub- acknowledged. This work was supported by the Korea Re-
stituted cube is parallel to the deposit surface or, in other search Foundation Grant funded by the Korean Government
words, a-axis-oriented domains form in the c-axis matrix 共MOEHRD兲 共KRF-2007-314-D00107兲.
关Fig. 3共c兲兴.
When the a-axis and b-axis of the c-axis YBCO are par-
allel to the a-axis and b-axis of the substituted cube, the APPENDIX: ELASTIC ANISOTROPY OF
boundary energy between the c-axis YBCO matrix and the ORTHORHOMBIC YBa2Cu3O7
new cube will be minimized, resulting in the evolution of
rectangular grains shown in Fig. 1. However, the growth rate The elastic compliance matrix of YBCO crystals with
of the new grains depends on their elastic anisotropy. The orthorhombic symmetry is given by
冤 冥
metastable high-energy matrix is subjected to the higher S11 S12 S13 0 0 0
strain energy in the higher Young’s modulus directions of the
stable low-energy grains, resulting in the higher growth rate S12 S22 S23 0 0 0
along the higher Young’s modulus direction.18,19 This is the S13 S23 S33 0 0 0
. 共A1兲
reason why the low energy grains have longer dimensions in 0 0 0 S44 0 0
the Ē共001兲 direction than that in the Ec direction as shown in 0 0 0 0 S55 0
Fig. 1 and as previously observed.7,8
0 0 0 0 0 S66
The larger aspect ratio of the low energy grains devel-
oped during annealing at 200 ° C than that developing at Compliances of orthorhombic YBCO crystals are as fol-
400 ° C can be attributed to the higher elastic anisotropy at lows: S11 = 0.006 147, S22 = 0.005 614, S33 = 0.013 029, S12 =
the lower temperature. The lower volume fraction of the −0.000 779, S13 = −0.004 489, S23 = −0.004 285, S44
grains developing at 200 ° C is due to the lower atomic mo- = 0.016 393, S55 = 0.021 277, and S66 = 0.010 309 共in
bility. GPa−1兲.16
At relatively high temperatures, the lattice diffusion is so If calculating the Young’s modulus E along the arbitrary
high that the strain energy cannot dominate the film energy, direction, x1⬘ can be calculated using the following relation:
and the surface energy minimization determines the film
⬘ ,
E = 1/S1111 共A2兲
texture,6,13 resulting in the c-axis orientation because the
minimum surface plane is along the ab plane or the 共001兲 ⬘ is expressed in terms of the com-
where the compliance S1111
plane.10 On the other hand, as temperature decreases, the pliances Sij referred to the symmetry axes of the crystal.
strain energy increasingly dominates the film energy and the From the transformation law,
Tensor 11 22 33 23 or 32 13 or 31 12 or 21
Contracted 1 2 3 4 5 6
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013511-5 Lee et al. J. Appl. Phys. 104, 013511 共2008兲
⬘ = a1ia1ja1ka1lSijkl
S1111 共A3兲 ⬘ = a11
1/E = S1111 4 4
S11 + a12 4
S22 + a13 2 2
S33 + a11 a12共2S12 + S66兲
The compliances 共in the tensor notation兲 Sijkl in the above 2 2
+ a11 a13共2S13 + S55兲 + a12
2 2
a13共2S23 + S44兲, 共A6兲
equation are converted to the contracted notation Smn accord-
ing to Eq. 共A4兲 and Table II. where E is Young’s modulus.
Let the symmetric axes a, b, and c of the orthorhombic
pSijkl = Smn with ij = m and kl = n, 共A4兲 YBCO crystal be x1, x2, and x3. For the x1 tension, a11 = a12
where = 0 and a13 = 1. Therefore, for the orthorhombic YBCO crys-
tal,
p = 1 when both m and n are 1,2 or 3 共S1111
⬘ 关001兴 = S33 = 0.01303 GPa−1 or Ec = 76.75 GPa.
S1111
= S11, S1122 = S12 ¯兲,
Similarly,
p = 2 when either m or n is 1,2 or 3 共2S1123
⬘ 关010兴 = S22 = 0.005614 GPa−1 or Eb = 178.1 GPa.
S1111
= S14, 2S1113 = S15 ¯兲,
⬘ 关100兴 = S11 = 0.006147 GPa−1 or Ea = 162.7 GPa.
S1111
p = 4 when both m and n are 4,5 or 6 共4S1223
= S64, 4S1212 = S66 ¯兲, 1
T. R. Dinger, T. K. Worthington, W. J. Gallagher, and R. L. Sandstrom,
Phys. Rev. Lett. 58, 2687 共1987兲.
Nonzero compliance components for an orthorhombic 2
Y. Enomoto, T. Murakami, M. Suzuki, and K. Moriwaki, Jpn. J. Appl.
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Phys., Part 2 26, L1248 共1987兲.
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⬘ = a11a11a11a11S1111 + a11a11a12a12S1122
4
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5
+ a12a12a12a12S2222 + a12a12a13a13S2233 A. Cassinese, A. Di Chiara, F. M. Granozio, S. Saiello, U. S. di Uccio, and
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+ a13a13a11a11S3311 + a13a13a12a12S3322 6
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+ a13a13a13a13S3333 + a12a13a12a13S2323 7
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+ a12a13a13a12S2332 + a13a12a12a13S3223 8
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+ a13a12a13a12S3232 + a11a13a11a13S1313 9
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10
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11
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12
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+ a12a11a12a11S2121 , 共A5兲 13
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14
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15
where a1i are the direction cosines with the subscripts 1 and A. C. Westerheim, A. C. Anderson, and M. J. Cima, Rev. Sci. Instrum. 63,
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16
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D. N. Lee, Thin Solid Films 434, 183 共2003兲.
Taking into account that S21 = S12, S31 = S13, and S32 = S23, 18
S. B. Lee, D. K. Choi, and D. N. Lee, J. Appl. Phys. 98, 114911 共2005兲.
Eq. 共A5兲 reduces to 19
D. N. Lee, Adv. Mater. Res. 26–28, 623 共2007兲.
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