We report the electrical properties, measured both at the macroscopic and nanometric scales, of epitaxial (110)-Na0.5Bi0.5TiO3 (NBT) thin films grown on (110)Pt/(110)SrTiO3 by pulsed laser deposition (PLD). The influence of the A-site composition (Na and/or Bi excess) on both the structural/microstructural characteristics and the electrical properties is discussed. Whatever the composition of the NBT target, the final layers are systematically epitaxially grown, with NBT crystallites mainly (110)-oriented, and as well (100)-oriented for some minor proportion. Atomic force microscopy (AFM) images reveal the coexistence of two kinds of grains presenting different shapes: namely flat and elongated grains, corresponding to (100)- and (110)-oriented NBT crystallites, respectively. The macroscopic ferroelectric properties were measured at room temperature. A rather well-defined shape of the hysteresis loops was obtained: the incorporation of a Bi excess in the target clearly improves the saturation of the loops. The ferroelectric performances are a remanent polarization (Pr) value, ranging from 7 to 14 μC/cm2, associated with a coercive field (Ec) in the range 68–85 kV/cm. In addition, at 105 Hz, the relative permittivity was about ɛr ∼ 255–410 and the dielectric losses (tan δ) were ∼6%–7%. Finally, the electrical properties at the local scale were investigated by coupling piezoresponse force microscopy (PFM) and tunneling AFM (TUNA) measurements. The collected data reveal that the two types of grains behave differently. The PFM amplitude signal of (110)-oriented grains is very contrasted and such grains are often divided in ferroelectric bi-domains of nanometric sizes, whereas the response of (100)-oriented grains is less contrasted and more homogeneous. The interpretation of the PFM signal is provided. The piezoloop recorded on a (110)NBT grain is strongly distorted and shifted along the vertical axis, in agreement with the vertical drift observed for macroscopic ferroelectric data. Finally, TUNA data clearly indicate that flat grains are leakier than elongated grains, highlighting the anisotropy of the electrical properties at the local scale.

1.
B.
Jaffe
,
W. R.
Cook
, and
H.
Jaffe
,
Piezoelectric Ceramics
(
Academic
,
New York
,
1971
).
2.
F.
Levassort
,
P.
Tran-Huu-Hue
,
E.
Ringaard
, and
M.
Lethiecq
,
J. Eur. Ceram. Soc.
21
,
1361
(
2001
).
3.
EU-Directive 2002/95/EC
, “
Restriction of the Use of Certain Hazardous Substances in Electrical and Electronic Equipment (RoHS)
,”
Off. J. Eur. Union
46
(
L37
),
19
23
(
2003
).
4.
J.
Rödel
,
W.
Jo
,
K. T. P.
Seifert
,
E.-M.
Anton
,
T.
Granzow
, and
D.
Damjanovic
,
J. Am. Ceram. Soc.
92
,
1153
(
2009
).
5.
G. A.
Smolenski
,
V. A.
Isupov
,
A. I.
Agranovskaya
, and
N. N.
Krainik
,
Sov. Phys. Solid State
2
,
2651
(
1961
).
6.
Y.
Hiruma
,
H.
Nagata
, and
T.
Takenaka
,
J. Appl. Phys.
105
,
084112
(
2009
).
7.
G. O.
Jones
and
P. A.
Thomas
,
Acta Crystallogr., Sect. B: Struct. Sci.
58
,
168
(
2002
).
8.
J.
Kreisel
,
A. M.
Glazer
,
P.
Bouvier
, and
G.
Lucazeau
,
Phys. Rev. B
63
,
174106
(
2001
).
9.
T.
Yu
,
K. W.
Kwok
, and
H. L. W.
Chan
,
Thin Solid Films
515
,
3563
(
2007
).
10.
X.-G.
Tang
,
J.
Wang
,
X.-X.
Wang
, and
H. L. -W.
Chan
,
Chem. Mater.
16
,
5293
(
2004
).
11.
J.
Wu
and
J.
Wang
,
J. Phys. D: Appl. Phys.
42
,
195405
(
2009
).
12.
W.
Ge
 et al,
J. Phys. D: Appl. Phys.
41
,
115403
(
2008
).
13.
W.
Qin
,
Y.
Guo
,
B.
Guo
, and
M.
Gu
,
J. Alloys Compd.
513
,
154
158
(
2012
).
14.
Y.
Guo
,
D.
Akai
,
K.
Sawada
, and
M.
Ishida
,
Solid State Sci.
10
,
928
(
2008
).
15.
Y. P.
Guo
,
D. S.
Akai
,
K.
Sawada
,
M.
Ishida
, and
M. Y.
Gu
,
Solid State Commun.
149
,
14
(
2009
).
16.
M.
Dinescu
,
F.
Craciun
,
N.
Scarisoreanu
,
P.
Verardi
,
A.
Moldovan
,
A.
Purice
,
A.
Sanson
, and
C.
Galassi
,
J. Phys. IV
128
,
77
(
2005
).
17.
N.
Scarisoreanu
,
F.
Craciun
,
V.
Ion
,
S.
Birjega
, and
M.
Dinescu
,
Appl. Surf. Sci.
254
,
1292
(
2007
).
18.
M.
Abazari
,
A.
Safari
,
S. S. N.
Bharadwaja
, and
S.
Trolier-McKinstry
,
Appl. Phys. Lett.
96
,
082903
(
2010
).
19.
C. H.
Yang
,
Z.
Wang
,
Q. X.
Li
,
J. H.
Wang
,
Y. G.
Yang
,
S. L.
Gu
,
D. M.
Yang
, and
J. R.
Han
,
J. Cryst. Growth
284
,
136
(
2005
).
20.
H.-W.
Cheng
,
X.-J.
Zhang
,
S.-T.
Zhang
,
Y.
Feng
,
Y.-F.
Chen
,
Z.-G.
Liu
, and
G.-X.
Cheng
,
Appl. Phys. Lett.
85
,
2319
(
2004
).
21.
J.-R.
Duclère
,
C.
Cibert
,
A.
Boulle
,
V.
Dorcet
,
P.
Marchet
,
C.
Champeaux
,
A.
Catherinot
,
S.
Députier
, and
M.
Guilloux-Viry
,
Thin Solid Films
517
,
592
(
2008
).
22.
M.
Bousquet
 et al,
J. Appl. Phys.
107
,
034102
(
2010
).
23.
In this paper, NBT crystal structure is considered as a pseudo-cubic cell. Thus, we index the XRD patterns using the corresponding nomenclature. The International Centre for Diffraction Data® provides the Joint Committee on Powder Diffraction Standards (JCPDS) files related to both the NBT cubic structure and to the real NBT rhombohedral structure, which are referenced, respectively, as follows: (Ref.: 01-389-3109) and (Ref.: 01-070-9850).
24.
T.
Harigai
,
Y.
Tanaka
,
H.
Adachi
, and
E.
Fujii
,
Appl. Phys. Express
3
,
111501
(
2010
).
25.
H.
Adachi
,
Y.
Tanaka
,
T.
Harigai
,
M.
Ueda
, and
E.
Fujii
,
Appl. Phys. Express
4
,
051501
(
2011
).
26.
S. O.
Leontsev
and
R. E.
Eitel
,
Sci. Technol. Adv. Mater.
11
,
044302
(
2010
).
27.
R.
Zuo
,
S.
Su
,
Y.
Wu
,
J.
Fu
,
M.
Wang
, and
L.
Li
,
Mater. Chem. Phys.
110
,
311
(
2008
).
28.
M.
Spreitzer
,
M.
Valant
, and
D.
Suvorov
,
J. Mater. Chem.
17
,
185
(
2007
).
29.
Y. S.
Sung
,
J. M.
Kim
,
J. H.
Cho
,
T. K.
Song
,
M. H.
Kim
, and
T. G.
Park
,
Appl. Phys. Lett.
96
,
202901
(
2010
).
30.
Y. S.
Sung
,
J. M.
Kim
,
J. H.
Cho
,
T. K.
Song
,
M. H.
Kim
,
H. H.
Chong
,
T. G.
Park
,
D.
Do
, and
S. S.
Kim
,
Appl. Phys. Lett.
96
,
022901
(
2010
).
31.
D. Y.
Wang
,
N. Y.
Chan
,
S.
Li
,
S. H.
Choy
,
H. Y.
Tian
, and
H. L. W.
Chan
,
Appl. Phys. Lett.
97
,
212901
(
2010
).
32.
D.
Alonso-Sanjosé
,
R.
Jiménez
,
I.
Bretos
, and
M. L.
Calzada
,
J. Am. Cer. Soc.
92
,
2218
(
2009
).
33.
J.
Wang
,
Z.
Zhou
, and
J.
Xue
,
Acta Mater.
54
,
1691
(
2006
).
34.
F.
Rémondière
,
A.
Wu
,
P. M.
Vilarinho
, and
J. P.
Mercurio
,
Appl. Phys. Lett.
90
,
152905
(
2007
).
35.
D. Y.
Wang
,
D. M.
Lin
,
K. S.
Wong
,
K. W.
Kwok
,
J. Y.
Dai
, and
H. L. W.
Chan
,
Appl. Phys. Lett.
92
,
222909
(
2008
).
36.
J.
Xu
,
Y.
Liu
,
R. L.
Withers
,
F.
Brink
,
H.
Yang
, and
M.
Wang
,
J. Appl. Phys.
104
,
116101
(
2008
).
37.
A.
Boulle
,
O.
Masson
,
R.
Guinebretière
,
A.
Lecomte
, and
A.
Dauger
,
J. Appl. Crystallogr.
35
,
606
(
2002
).
38.
B.
Gautier
,
J.-R.
Duclère
, and
M.
Guilloux-Viry
,
Appl. Surf. Sci.
217
,
108
(
2003
).
39.
M.
Bousquet
, Ph.D. dissertation,
University of Limoges
, France,
2010
.
40.
N. D.
Scarisoreanu
,
F.
Craciun
,
A.
Chis
,
R.
Birjega
,
A.
Moldovan
,
C.
Galassi
, and
M.
Dinescu
,
Appl. Phys. A
101
,
747
(
2010
).
41.
J.
Wu
and
J.
Wang
,
J. Appl. Phys.
106
,
104111
(
2009
).
42.
I. B.
Misirlioglu
,
M. B.
Okatan
, and
S. P.
Alpay
,
J. Appl. Phys.
108
,
034105
(
2010
).
43.
J. F.
Scott
,
J. Phys.: Condens. Matter
20
,
021001
(
2008
).
44.
Z. H.
Zhou
,
J. M.
Xue
,
W. Z.
Li
,
J.
Wang
,
H.
Zhu
, and
J. M.
Miao
,
Appl. Phys. Lett.
85
,
804
(
2004
).
45.
A.
Ferri
,
A.
Da Costa
,
R.
Desfeux
,
M.
Detalle
,
G. S.
Wang
, and
D.
Rèmiens
,
Integr. Ferroelectr.
91
,
80
(
2007
).
46.
D. V.
Taylor
and
D.
Damjanovic
,
Appl. Phys. Lett.
76
,
1615
(
2000
).
47.
S. V.
Kalinin
, “
Nanoscale electric phenomena at oxide surfaces and interfaces by scanning probe microscopy
,” Ph.D. dissertation,
University of Pennsylvania
, USA,
2002
.
48.
A. L.
Kholkin
,
S. V.
Kalinin
,
A.
Roelofs
, and
A.
Gruverman
, in
Scanning Probe Microscopy: Electrical and Electromechanical Phenomena at the Nanoscale
, edited by
S.
Kalinin
and
A.
Gruverman
(
Springer
,
2007
).
49.
A.
Wu
,
P. M.
Vilarinho
,
D.
Wu
, and
A.
Gruverman
,
Appl. Phys. Lett.
93
,
262906
(
2008
).
50.
A.
Gruverman
,
B. J.
Rodriguez
,
A. I.
Kingon
,
R. J.
Nemanich
,
A. K.
Tagantsev
,
J. S.
Cross
, and
M.
Tsukada
,
Appl. Phys. Lett.
83
,
728
(
2003
).
51.
A. L.
Kholkin
,
K. G.
Brooks
,
D. V.
Taylor
,
S.
Hiboux
, and
N.
Setter
,
Integr. Ferroelectr.
22
,
525
(
1998
).
52.
Y.
Rozier
,
B.
Gautier
,
G.
Hyvert
,
A.
Descamps
,
C.
Plossu
,
F.
Ducroquet
, and
C.
Dubourdieu
,
Thin Solid Films
517
,
1868
(
2009
).
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