High-speed switching of nanoscale ferroelectric domains in congruent single-crystal

LiTaO 3
Kenjiro Fujimoto and Yasuo Cho

Citation: Applied Physics Letters 83, 5265 (2003); doi: 10.1063/1.1635961

View online: http://dx.doi.org/10.1063/1.1635961
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 APPLIED PHYSICS LETTERS VOLUME 83, NUMBER 25 22 DECEMBER 2003

High-speed switching of nanoscale ferroelectric domains

in congruent single-crystal LiTaO3
Kenjiro Fujimotoa) and Yasuo Cho
Research Institute of Electrical Communication, Tohoku University, 2-1-1 Katahira, Aoba-ku,
Sendai 980-8577, Japan
共Received 4 August 2003; accepted 30 October 2003兲
The nanodomain reversal characteristics of congruent LiTaO3 共CLT兲 single crystal are investigated.
It is found that fast nanosecond domain switching can be achieved by reducing the sample thickness,
even for CLT, which contains many Li vacancy defects that pin domain-wall movement. As an
example, the authors obtain a polarization inverted domain dot with a radius of 7.9 nm by
application of a 4 ns 10 V pulse. These results demonstrate that the speed of polarization reversal
is closely related to the thickness of the medium. © 2003 American Institute of Physics.
关DOI: 10.1063/1.1635961兴

Recently, ultrahigh-density information storage based on growth of the nucleated spike domain may play a major role
ferroelectric media has attracted considerable interest as a in domain reversal, differing from the switching behavior in
postmagnetic high-density data storage technology. The po- a parallel-plate capacitor, which is driven by a homogeneous
tential of ferroelectric media for such applications stems field.9 However, as yet, there are few reports on polarization
from the much thinner domain walls and smaller minimum reversal under probe tips, with the only examples being
size of domains compared to ferromagnetic materials, which BaTiO3 single-crystal and PZT thin film, which have switch-
are widely used for data storage at present.1 ing times of 1 ␮s and 100 ns, respectively.2,10
Although only preliminary research has been conducted As reported previously by the present authors, CLT has
on ultrahigh-density probe memory using ferroelectrics as a many advantageous characteristics as a high-density record-
data storage medium, scanning probe microscopy has been ing medium.7 However, CLT has been considered to be un-
investigated extensively as a method for forming and detect- suitable for high-speed writing because the material typically
ing small inverted domain dots in ferroelectric thin films, includes many Li vacancy defects, which pin domain-wall
such as lead zirconate titanate 共PZT兲.2 In this technique, do- movement.11 As a further investigation of the potential of
main dots are switched by applying a relatively large dc single-crystal CLT as a recording medium, this study exam-
pulse to the probe, creating an electric field at the tip of the ines the fast nanodomain reversal characteristics of CLT un-
probe cantilever. Recently, the present authors have demon- der a probe tip.
strated 1.50 Tbit/in.2 high-density data storage using a con- First, the characteristics of polarization reversal under
gruent LiTaO3 共CLT兲 single-crystal plate of thickness 70 nm the probe tip were investigated as a function of pulse dura-
with scanning nonlinear dielectric microscopy 共SNDM兲3– 6 tion and amplitude using the previously established SNDM
for the detection of artificial nanodomains.7 domain engineering system. A schematic diagram of the
The recording medium for large-capacity memory de- SNDM domain engineering system is shown in Fig. 1.
vices also requires excellent high-speed writing characteris- SNDM, as described in detail in our previous reports,3–7 de-
tics in addition to high memory density. The switching speed tects the distribution of ferroelectric domains by detecting
of polarization reversal immediately below the tip of the
probe is directly related to the writing time, and of course
should be as fast as possible. Therefore, investigation of the
kinetics of polarization reversal under a probe tip is impor-
tant to estimating the expected writing speed of any record-
ing system, and may also lead to a better understanding of
the polarization reversal process near such tips.
Using PZT thin films with parallel-plate electrodes, po-
larization reversal of 1.8 ns or less has been shown to be
possible.8 However, for actual data storage, it is necessary to
examine the response speed of the nanodomain under the tip
in detail because the domain reversal characteristics beneath
the probe tip differ significantly from those in a parallel-plate
capacitor. For example, the field immediately beneath the tip
is concentrated, and has a quite inhomogeneous distribution.
Therefore, sidewise growth of domains after the forward

a兲
Electronic mail: fujimoto@riec.tohoku.ac.jp FIG. 1. Ferroelectric nanodomain engineering system based on SNDM.

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0003-6951/2003/83(25)/5265/3/$20.00 5265 © 2003 American Institute of Physics
141.212.109.170 On: Mon, 08 Dec 2014 20:10:36
 5266 Appl. Phys. Lett., Vol. 83, No. 25, 22 December 2003
FIG. 2. SNDM images of inverted domain dot arrays (5⫻6) on single-
crystal CLT plates of thickness 共a兲 83, 共b兲 71, 共c兲 63, and 共d兲 55 nm. Pulse
amplitude was varied from 12 to 7 V in 1 V steps from the left- to the
right-hand side and pulse application time was varied from 100 ␮s to 10 ns
in 10⫻ steps from top to bottom.
the nonlinear dielectric constant. The measured change in
capacitance, induced by a change in the nonlinear dielectric
response under an alternating applied electric field, is con-
verted to a frequency deviation in a frequency modulation
signal to extract the polarization at that point. The point is
then redetected using frequency demodulation and lock-in
techniques. In this study, an electrically conductive PtIr-
coated cantilever with a tip radius of 25 nm is employed as
the probe. In order to minimize pulse reflection problems and
to obtain a well-defined pulse, the load resistance was
matched to the characteristic impedance of the pulse appli-
cation system by inserting a 50 ⍀ terminal resistance in par-
allel between the tip 共ground兲 and the back electrode of the
specimen 共metal stage兲. The polarization of the medium im-
mediately under the probe tip was reversed by applying a
pulse of relatively high voltage across the probe and the
metal stage of the SNDM. The resulting features were then
imaged by SNDM.
The sizes of the domain dots were measured as a func-
tion of pulse amplitude and duration for various sample
thicknesses. Figures 2共a兲–2共d兲 show SNDM images of the
inverted domain dot array formed on single-crystal CLT
plates with thicknesses of 83, 71, 63, and 55 nm, respec-
tively. An array of 5⫻6 pulses was applied to each sample.
From the left- to the right-hand side in Fig. 2, the pulse
amplitude was varied from 12 to 7 V in 1 V steps, and from
top to bottom, the pulse application time was varied from
100 ␮s to 10 ns in 10⫻ steps. Both the pulse amplitude and
the application time required to achieve reversal of polariza-
tion vary significantly with even small variations in sample
thickness. Very fast domain switching of less than 100 ns
was achieved for the plates of single-crystal CLT with a
thickness of less than 63 nm. This strong thickness depen-
dence originates from the inhomogeneous distribution of
electric field immediately beneath the tip. The domain
switching speed heavily depends on the electric-field
strength. And it rapidly decreases along the depth direction
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because the field is highly concentrated just beneath the tip.
141.212.109.170 On: Mon, 08 Dec 2014 20:10:36
K. Fujimoto and Y. Cho
FIG. 3. Radius of inverted domain dots as a function of voltage application
time.
Therefore, only when the thickness of the sample becomes
less than the penetration depth of the field high-speed switch-
ing is possible. As a result, a small variation in sample thick-
ness affects the nanodomain reversal characteristics materi-
ally.
Figure 3 shows the relationship between the inverted do-
main radius 共half width at half maximum of the SNDM sig-
nal兲 and voltage application time for the 55 nm thick CLT
plate. The radius of the inverted domain formed with these
very short pulses also depends logarithmically upon the volt-
age application time, similar to the case reported previously
for relatively longer pulses.2
The shortest pulse duration for polarization switching of
a nanodomain was 4 ns, and this speed was limited by the
performance of the pulse generator used in this study. As an
example, Fig. 4 shows a SNDM image of a inverted nan-
odomain dot of with radius of 7.9 nm formed by application
of a 4 ns 10 V pulse.
These experimental results appear to contradict the re-
sults reported by Kim et al.12 From a detailed investigation
of the domain switching mechanism in very thick lithium
tantalate single-crystal 共thickness 250 ␮m兲, Kim et al.12 con-
cluded that a very long voltage application time of 1 s or
more was required to stabilize inverted domains in CLT.
FIG.to4.the
SNDM of an inverted domain 共radius 7.9 nm兲 formed
termsimage
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V 4 ns pulse application with a 60 nm thick CLT plate.
 Appl. Phys. Lett., Vol. 83, No. 25, 22 December 2003
FIG. 5. P – E hysteresis loops of single-crystal CLT plates of thickness 共a兲
6.5 ␮m and 共b兲 500 nm. Loops illustrated as solid lines were measured
quasi-statically with 共a兲 10 mHz and 共b兲 100 mHz triangular voltage wave
forms. Loops indicated by dashed–dotted and dotted lines were measured
using a high-frequency field with 1 kHz triangular voltage wave form for
upward and downward initial polarization states, respectively.
Therefore, nanosecond domain switching in CLT has been
thought to be impossible. To attempt to explain this remark-
able discrepancy, the polarization reversal of a very thin CLT
capacitor was examined using parallel-plate electrodes to
achieve switching. Measured P – E hysteresis loops of very
thin CLT single-crystal plates of thicknesses 6.5 ␮m and 500
nm are shown in Figs. 5共a兲 and 5共b兲. In Figs. 5共a兲 and 5共b兲,
the hysteresis loops indicated by solid lines were measured
quasi-statically 关applying Fig. 5共a兲 10 mHz and Fig. 5共b兲 100
mHz triangular voltage wave forms兴. The loops denoted by
dashed and dotted lines in Figs. 5共a兲 and 5共b兲 were measured
using a high-frequency field 共applying a 1 kHz triangular
voltage wave form兲. The initial polarization states were fixed
positive 共upward兲 or negative 共downward兲 by applying an
adequately long and large dc pulse prior to loop measure-
ment.
In the case of quasi-static measurements, the two hyster-
esis loops obtained for different initial polarization states are
almost the same. Although the loops are shifted horizontally
due to the intrinsic internal field,12,13 P – E hysteresis loops
for the two samples with different thicknesses of 6.5 ␮m and
500 nm have the characteristics of general ferroelectrics. In
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141.212.109.170 On: Mon, 08 Dec 2014 20:10:36
K. Fujimoto and Y. Cho 5267
contrast, the shapes of the hysteresis loops obtained by mea-
surement under a high-frequency field differ significantly
from those obtained through quasi-static measurement, and
vary according to sample thickness. For the sample of thick-
ness 6.5 ␮m, the loops were narrower and shifted horizon-
tally to the opposite direction of each other depending on the
initial state of polarization. Therefore, under a high-
frequency field, CLT exhibits remanent polarization in only
one direction. For example, if the initial state of polarization
is negative 关dotted line Fig. 5共a兲兴, the polarization will be
inverted upward when the electric field is increased, but will
switch to downward upon reducing the electric field before
the voltage reaches zero. This phenomenon is called
‘‘backswitching.’’ 13 In this example, the remanent polariza-
tion has only a negative value, preventing the polarization
from being inverted with a short voltage pulse. Due to this
backswitching, it has been considered that a domain created
by the application of an electric field requires a certain
amount of time to stabilize and persist after voltage
application.12 However, for a sample of 500 nm thick, the
loops become wider, and the electric field at which back-
switching occurs decreases. In particular, when the initial
polarization is upward, the loop has two values of remanent
polarization, despite measurement under high-frequency
conditions. These results indicate that fast domain reversal in
CLT is possible by reducing the sample thickness, and is the
most likely explanation for the observation of nanosecond
switching in quite thin 共⬃100 nm兲 CLT. However, further
detailed investigation of this specific phenomenon will be
required to verify the physical mechanism of nanodomain
switching using nanosecond pulses.
In summary, the authors have demonstrated nanodomain
dot formation by nanosecond voltage application 共4 ns兲 using
very thin single-crystal CLT 共⬍63 nm兲. The 4 ns switching
time obtained in the study is suitable for the development of
high-speed ferroelectric data storage systems, potentially
supporting writing rates of 250 Mbps per probe and memory
densities of more than 1 Tbit/in.2
The authors would like to thank A. Onoe of R&D Labo-
ratories, Pioneer Corporation for valuable technical help.
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