Bi2O3缓冲下BiFe0.95Mn0.05O3薄膜的铁磁与压电性能提升
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本研究报道了一种通过溶胶-凝胶法制备的BiFe0.95Mn0.05O3薄膜，该薄膜在Bi2O3缓冲的Pt/Ti/SiO2/Si衬底上展现出显著的铁磁性和压电性能提升。相比于直接沉积在Pt/Ti/SiO2/Si上的薄膜，Bi2O3的存在起到了关键作用。在1到16.7 kHz的宽频率范围内，这两种薄膜都显示出饱和的方形磁滞回线，表明它们具有良好的磁性响应。
在Bi2O3缓冲的BiFe0.95Mn0.05O3薄膜上，压电特性得到了显著增强。其2P（r）值高达156 μC/cm²，这表示薄膜在机械应力下能产生的电荷量较大，适合用于能量转换和传感器应用。同时，2E（c）值减小至510 kV/cm，这意味着在相同的电压下，薄膜能产生更大的位移，这对于提高压电器件的灵敏度至关重要。磁滞回线更加对称，反映出更高的稳定性和较低的非线性效应，而电荷保持能力也更强，即使经过长时间（10^4 s）操作，电荷损耗仅占2%，这证明了薄膜在长期工作中的可靠性能。
此外，该薄膜的耐疲劳性能显著，经过大量的开关循环（达到10^10次）后，压电响应Delta P没有明显下降，这显示了其在实际应用中的持久性。更为重要的是，BiFe0.95Mn0.05O3薄膜能够被压电模式的原子力显微镜均匀极化，显示出64 pm/V的压电系数，这是由于Bi2O3缓冲层有效减少了负电缺陷如(Mn-Fe3+ (2+))复合物以及(Fe-Fe3+ (2+))和氧空位等杂质的影响，从而优化了薄膜的晶体生长，提高了其内部结构的有序性。
这项研究揭示了Bi2O3缓冲层在改善BiFe0.95Mn0.05O3薄膜的铁磁性和压电性能方面的关键作用，这为设计高性能的铁电和压电材料提供了新的思路和方法，可能在微电子、传感器和能量转换等领域具有广阔的应用前景。
Enhanced ferro- and piezoelectric properties of a sol–gel derived
BiFe
0.95
Mn
0.05
O
3
thin film on Bi
2
O
3
-buffered Pt/Ti/SiO
2
/Si substrate
Dehui Li, Xiaoqiang Sun, Xiaohong Chuai
n
, Zhifa Wu, Zijian Cao, Yunfei Yan, Daming Zhang
n
State Key Laboratory on Integrated Optoelectronics, College of Electronic Science and Engineering, Jilin University, Changchun 130012, China
article info
Article history:
Received 3 April 2011
Received in revised form
27 September 2011
Accepted 9 October 2011
Communicated by D.P. Norton
Available online 31 October 2011
Keywords:
A1. Defect complexes
A3. Sol–gel
B1. BiFe
0.95
Mn
0.05
O
3
B2. Ferro-and piezoelectric materials
abstract
The BiFe
0.95
Mn
0.05
O
3
films were fabricated on Pt/Ti/SiO
2
/Si and Bi
2
O
3
/Pt/Ti/SiO
2
/Si substrates using a sol–gel
process. Saturated square P–E hysteresis loops can be observed at frequencies ranging from 1 to 16.7 kHz
for both films. The BiFe
0.95
Mn
0.05
O
3
film on Bi
2
O
3
/Pt/Ti/SiO
2
/Si exhibits a larger 2P
r
(156
m
C/cm
2
), smaller
2E
c
(510 kV/cm), more symmetric P–E loops, stronger charge retaining capability (the loss of
D
P is only
2% after 10
4
s) and fatigue resistance (no loss of
D
P is observed after 10
10
switching cycles) compared to the
film deposited directly on Pt/Ti/SiO
2
/Si. More importantly, the former can be uniformly polarized using a
piezoelectric-mode atomic force microscopic system and exhibits a larger piezoelectric coefficient
(64 pm/V). These results should be due to the Bi
2
O
3
buffer layer, which can favor the grain growth
and hence elimination of defect complexes formed between the negatively charged defects such as
ðMn
2 þ
Fe
3 þ
Þ
0
or ðFe
2 þ
Fe
3 þ
Þ
0
and oxygen vacancies.
& 2011 Elsevier B.V. All rights reserved.
1. Introduction
BiFeO
3
(BFO) has been demonstrated to be a promising lead-
free candidate for the high-density ferroelectric random access
memories (FeRAMs) and piezoelectric devices due to its large
remanent polarization and piezoelectric coefficient in thin film
form [1–3]. It is well known that BFO suffers from high leakage
current, which leads to that the intrinsic ferro- and piezoelectric
properties are difficult to be obtained especially in BFO thin films
fabricated using the chemical solution deposition methods (e.g.
sol–gel or metal organic decomposition). To solve the leakage
problem of BFO thin films, several groups have attempted to form
double-layered films consisting of a BFO layer and a ferroelectric
layer with lower leakage current [4–7]. Although the insulating
properties of such double-layered structure can be enhanced, the
square shape of the P–E loops was inevitably degraded. This
indicates that domain backswitching may occur in the asym-
metric double-layered thin films.
Lanthanides (Nd, La, Gd, Pr, Sm and Tb) substitution for A sites
[8–12] and high-valence-ion (Ti
4 þ
,Nb
5 þ
and W
6 þ
) doping at B
sites [13–16] have been utilized to reduce the leakage current of
BFO films. Unfortunately, saturated P–E hysteresis loops can only
be obtained at frequencies higher than 10 kHz. Singh et al. have
reported the leakage current in BFO thin films can be reduced to a
great extent by Mn doping at Fe
3 þ
sites [17]. More importantly,
well saturated P–E hysteresis loops with large remanent polariza-
tion (100
m
C/cm
2
) can be obtained at 1 kHz in BiFe
0.95
Mn
0.05
O
3
(BFMO) thin films deposited on Pt/Ti/SiO
2
/Si substrates. Wen et al.
found that, in addition to the Mn doping content, the annealing
process has strong influence on the ferroelectric properties of
BFMO films [18]. Particularly, an evident asymmetric coercive
field can be observed in the film annealed layer-by-layer. The
authors attributed this phenomenon to the aging effect as in the
Zn-doped BFO films [19,20].
The aging effect has been demonstrated to be related to the
domain backswitching induced by the electrostatic force asso-
ciated with the defect complexes formed between oxygen vacan-
cies and negatively charged defects such as ðMn
2 þ
Fe
3 þ
Þ
0
or ðFe
2 þ
Fe
3 þ
Þ
0
[21], which will be strongly dependent on the crystallinity of
BFMO thin films. In this work, we report on the effects of a
15-nm-thick Bi
2
O
3
buffer layer on the ferroelectric properties of
a (110)-preferred BFMO thin film prepared using a metal organic
decomposition method. Our results suggest that the Bi
2
O
3
buffer
layer can favor the grain growth and hence elimination of defect
complexes, which in turn leads to enhanced ferro-and piezo-
electric properties in the BFMO film.
2. Experimental
Both the Bi
2
O
3
buffer layer and BiFe
0.95
Mn
0.05
O
3
(BFMO) films
were fabricated using the same sol–gel method. For the prepara-
tion of the precursor solutions, bismuth nitrate [Bi(NO
3
) 5H
2
O,
Contents lists available at SciVerse ScienceDirect
journal homepage: www.elsevier.com/locate/jcrysgro
Journal of Crystal Growth
0022-0248/$ - see front matter & 2011 Elsevier B.V. All rights reserved.
doi:10.1016/j.jcrysgro.2011.10.010
n
Corresponding authors.
E-mail addresses: xhchuai@jlu.edu.cn (X. Chuai),
zhangdm@jlu.edu.cn (D. Zhang).
Journal of Crystal Growth 338 (2012) 85–90
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