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Imaging of ferroelectric domain walls by force microscopy

F. Saurenbach and B. D. Terris

Citation: Appl. Phys. Lett. 56, 1703 (1990); doi: 10.1063/1.103122

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Imaging of ferroelectric domain walls by force microscopy
F. Saurenbach and B. D. Terris
IBM Research Division, Almaden Research Center, 650 Harry Road, San Jose, Cal(tbmia 95120-6099
(Received 8 December 1989; accepted for publication 13 February 1990)
We have imaged ferroelectric domain walls in the ferroelectric-ferroelastic material
Gd z (MoO4) 3 using force microscopy. By using a mode of imaging developed for the detection
of static surface charge, the force gradient due to the polarization charge at the sample surface
was imaged. The signal was seen to change sign at the domain wall, consistent with the reversal
in sign of the polarization across a wall. By modeling the wall as a step function in the electric
potential, the general features of the force microscope domain wall image could be explained.

Ferroelectric materials are ofinterest both from scientif- normal to the imaged surface. The ferroelectric domain
ic and technological view points because of their switchable walls, therefore, He in the ( 110) plane, and are perpendicular
static polarizations. Numerous measurement probes have to the imaged surface. 14 Prior to imaging, the surface was
been developed to study the electric domain structures in rinsed with isopropanol to remove any static surface charge,
these materials. For example, domains have been imaged by which could obscure the domain wall. However, after
optical microscopy, either directly for transparent materials mounting the sample on the microscope, the surface was
or in combination with decoration I or etching. 2 These meth- seen to accumulate charge slowly. This charge could be com-
ods have resolutions of ~ 10 pm. Using scanning' or trans- pensated for by applying a small dc voltage between the tip
mission4 electron microscopy (TEM), images with nm reso- and an electrode on the back side of the sample (Fig, 1). 9 In
lution have been obtained. These latter methods, however, addition, an ionization source was periodically used to neu-
suffer from electron beam charging effects and, in particular tralize this nonpolarization charge.
for TEM, difficult sample preparation. In addition, the in- Shown in Fig. 2 (a) is the grey-scale image produced by
terpretation of the images is not always straightforward. recording the feedback voltage as the tip was scanned across
We report here the first imaging offerroclectric domain a domain wall. This feedback signa! image, in addition to
walls using a force microscope. These domains are analo- containing numerous surface scratches, shows a broad dark
gous to the ferromagnetic structures, such as magnetic re- stripe across the domain walL Dark (bright) regions in this
cording bits5 ,6 and naturally occurring domains,7 which image indicate a decrease (increase) in the tip-to-sample
have previously been studied using force microscopy. For spacing, resulting from a decrease (increase) in the tip-to-
the case of ferroelcctrics, the microscope is sensitive to the sample force gradient. Although there are several possible
stray electric field emanating from the surface, is non- sources of force gradient, including van der Waals and elec-
destructive, and provides information which is complemen- trostatic forces, we can assume that the only spatially vary-
tary to the techniques mentioned above. ing interaction in the vicinity of the domain waH is that due
The principles of force microscopyX and the imaging of to the ferroelectric polarization P. When P is nonzero, there
electrostatic charge with a force microscope have been de~ will be an associated polarization charge density ifo at the
scribed in detail elsewhere. 9 - 12 Briefly, a lever/tip is mount- surface. In the absence of compensating space or' surface
ed on a piezoelectric bimorph and oscillated at a frequency charge, ifp will induce an image charge Qp in the tip. The
WI just above the resonant frequency of the lever. The lever resulting force gradient will be proportional to the product
motion is detected by an optical fiber based interferometer" of Qp and the external field due to the polarization. The force
and a lock-in amplifier. The lever/tips are, in this case, elec- gradient, therefore, is proportional to the square of the field
trochemically etched tungsten wires, with base diameters and depends only on the magnitude, and not the sign, of the
~ 10 11m and lengths - 700 jIm. The last 50-100 pm of the polarization. As the tip passes over the domain waH, P
wire is bent at a 90° angle to form a tip. Typical spring con- changes sign and passes through zero, and hence the tip ex-
stants are on the order of 5 N/m and resonant frequencies
around 15 kHz. As the tip scans the surface, changes in the Osdllator (Wi)
tip-to-surface force gradient will alter the effective spring
constant ofthe lever, thereby changing its resonant frequen- ~~·~~,--i-.----'
cy and its amplitude of oscillation. Figure 1 shows a block
diagram of the apparatus. A feedback loop adjusts the tip-to-
sample spacing so as to maintain a constant oscillation am- Optical
plitude (constant force gradient). By monitoring the feed- Fiber

Birnorph c::~
Sirw a1
back voltage, labeled "z drive" in Fig. 1, contours of constant
---:::v- Tip
force gradient are measured.
We ha ve imaged ferroelectric domain walls in a polished
_ ··~I· Yl sa~n~··i
~..t' I
crystal of the ferroelectric-ferroeIastic material
Gd 2 (Mo04 )3' or GMO. At room temperature, GMO is or- Z Drive
thorhombic and has a uniaxial electric polarization parallel
to the crystallographic c axis. 13 The c axis was aligned to be FI G. 1. Block diagram of the force microscope.

1703 Appl. Phys. Lett. 56 (17),23 April 1990 0003-6951/90/171703-03$02,00 © i 990 American Institute of Physics 1703

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r?,. ::::;Q1EL. + -V~2 . ~
SIn-(uht) - .
After substituting the expression for Q, from above, we ob-
tain the force gradient
F'=, JF,

= -
sm-(o)"t) - -
a2 e
2 /. az?
, (. iJC
- V;) sm (i)2 t E z a; + C" 3EJz z ) iJ ,
- iJz (QpE,).
If the region being imaged has no net polarization,
(al E z = Qp = 0, then only the sin 2 (u]t term is nonzero and the
force gradient will oscillate at 2(i)2' This 2U)2 oscillation in the
force gradient will cause the envelope of the U)I tip oscillation
to be modulated at 2u)]. For electrically polarized samples,
Hz #0, the force gradient has a sin (():.t term and thus the
envelope of the (i) I tip oscillation will be modulated at (i)2' As
shown in Fig. 1, this U)2 signal is detected at the output of the
feedback loop lock-in amplifier with a second lock-in, and is
referred to as the "charge signaL" The phase of the detected
signal will indicate the sign of the charge.
The charge signal, shown in Fig, 2(b), changes sign as
the tip passes over the ferroelectric domain walL To reveal
the details of the data, a line scan of the charge image from
another section of the wall is shown in Fig. 3. On approach-
ing the wall, the signal is seen to first increase slightly, then
(bJ change sign as the tip passes over the waH, and finally go
through a minimum. To understand this line shape, we mod-
10Jim el the wall as a potential step fUllction. As discussed above,
the charge signal is
FIG. 2. (al fccdba\:k voltage image and (b) ch~,rgc image ofa ferroelectric
domain wall in GMO. ..
Vo sm(ril 2 t) E z (iJC + CiJEz)
-- .
iJz iJz
periences a minimum in the force gradient. To maintain a Shown in Fig. 4 are the calculated E z and JEzlaz for tip
constant force gradient, the feedback loop reduces the tip-to- heights of 0.5 and LO ,um. Ifwe assume the tip-to-electrode
sample spacing, thus producing the minimum seen in the capacitance has a liz dependence, such as from a parallel-
image of Fig. 2(a). The small bright spots in the feedback plate capacitor, then the charge signal becomes
image are results of tip "crashes" as the field passes through
. (aEz
CV;) sm(UJ 2 t) - - ~~ - )
Ez \
zero making it difficult for the feedback loop to servo off the
(}z z
minimum in force gradient.
In order to more clearly image the ferroelectric domain and is shown in Fig. 4 for the same two tip heights.
wall, we have used a more sensitive imaging mode developed While the general shape of the domain wall image is
for imaging static charge on insulators. I 1.12 This mode of
imaging responds only to charge and can distinguish the sign
of the charge. An ac bias voltage, V;) sin (il 2 t, is applied
bctweeen the tip and the electrode behind the ferroelectric
sample, with (i)2 chosen to be higher than the feedback loop
response frequency but much lower than uJ I' This
ac voltage induces an oscillating charge on the electrode,
Qc = CVo sin 0)21, where C is the tip-to-electrode capaci-
tance, and an equal and opposite charge on the tip. The total
tip charge for a ferroelectric sample is therefore
Q, = - (Qp + Q" ). To calculate the force on the tip. we
treat the tip-surface force as due to a point charge in a field o 10 20 30 40
x (11m)
E z = Pj(E - 1 )£0' where E is the sample dielectric con-
stant, and the tip-electrode force as from a capacitor. The FIG. 3. Single line scan of the charge signal across a ferroelectric domain
electrostatic force on the tip can then be approximated by wall.

1704 Appl. Pllys. Lett., Vol. 56, No. 17,23 April 1990 F. Saurenbach and B. D. Terris 1704

Downloaded 09 Sep 2012 to Redistribution subject to AIP license or copyright; see
'""' L._--' --'...._ L

-6 -4 -2

FIG. 4. One-dimensional step

fUllction in the (a) potential, with
the calculated (b) normal compo-
nent of the electric field Be and (c)
dE,I(iz. The (d) force gradient F'
is calculated assuming a paralJel-
plate capacitor modeL In the [ower
three figures, the solid lines were
calculated assuming a tip height of
O.S 11I1l and the dashed lines with a
tip height of l.D ,urn. FIG. 5. Charge image of a lO-flm-wide ferroelectric domain.

regions with slightly reduced E z , such as that in Fig. 2 (b),

would result.
As with magnetic domains, it is also possible to image
complete ferroelectric domains as well as isolated walls.
Shown in Fig. 5 is the charge image of a 1O-flm-wide domain.
As was the case with the single domain walls, the images of
accounted for by the simple model, the measured charge the walls are much broader than their atomic dimensions,
signal decays with increasing distance from the wall much due to the scan height and the size of the tip.
slower than the calculated force gradient. The calculated In conclusion, the force microscope provides informa-
value is neady zero within 5 /-tm of the wall, while the charge tion on the domains and domain walls which is complemen-
signal is still approximately half its peak value at a distance tary to other techniques. The microscope is nondestructive
of 20 flm from the wall, This apparent enhancement of the and detects the electric field above the sample surface. With
signal may arise from at least two sources. First, the true refinements to this technique, such as working in vacuum to
capacitance is unknown, and thus the relative weighting of eliminate some of the non polarization charge, it may be pos-
the two contributions to the force gradient is unknown. A sible to investigate the detailed field behavior at a ferroelec-
capacitance which decreases faster with distance than the tric surface.
assumed liz would favor the E z term more, and thus the We thank S. Meeks for providing the GMO sample and
calculated F' would be in better agreement with the data. for useful discussions.
Second, since we have assumed a point charge interaction
between the tip amI the polarization, the size and shape of Iy. P. Konstantinova, N. A. Tichomirova, and M. Glogarova, Ferroelec-
the tip have not been accounted for. As the electrostatic tries 20, 259 (1978).
2F. (hlletta, Pllys. Status Solidi 11, 721 (1972).
force is long range, the measured field will not be the field at 'R. LeBihan and M. Maussion, J. Phys. 33, C2-215 (1972).
the end of the tip but will be an average over some volume of 4PcngJu Lin and L. A. Bursill, Philos. Mag. A48, 251 (19g3); L A. Bursill
the tip. This will broaden any sharp changes in field. There- and Peng Iu Lin, l'hilos. Mag. A 48,953 (1983).
fore, the signal peak near the domain wall will be reduced in 'H. J. Mamin, D. Rugar, J, E. Stern, B. D. Terris, and S. E. Lambert, App!.
Phys. Lett. 53, 1563 (1988).
amplitude, and the relative magnitude ofthe signal far from ('D, Rugal', H. J. Mamin, R. Erlandsson, J. E. Stern, and B. D. Terris, Rev.
the wall will be increased. This long-range nature of the elec- Sci. Instrum. 59, 2337 (l928).
trostatic force may also account for the fact that the curve lH. J. Mamin, D. Rugar, J. E. Stern, R. E. Fontana, Jr., ,md P. Kasiraj,
for the 111m tip height is in better agreement with the data AppL Phys. Lett. 55, 31 R ( 1989); P. Grutter, E. Meyer, H. Heinzelmann,
L Roscnthalcr, H.-R. Hidber, and H.-J. Guntherodt, J. Ya.::. Sci. Techno!.
than the curve for 0.5,um tip height. Although the actual tip A 6,279 (\988).
height was ~O.l ,urn, the effective charge centroid will be "G. Binllig. C. F. Quate, and Cll. Gerber, Phys. Rev. Lett. 56, 930 (1986);
located farther from the surface. An anaiogous increase of Y. Martin, C. C. Williams, and H. K. Wickramasinghe, J. Appl.l'hy,. 61,
the apparent tip height has also been seen in the magnetic 4723 (1987); G. M. McClelland, R. Erlanc\sson, and S. Chiang, in Review
of Progress in Quantitative Nondestructive Evaluation, edited by D. O.
imaging. s Thompson and D. E. Chimenti (Plenum, New York, 19( 7 ), Yol. 6B, p.
The domain wall image occasionally contained features 3D7.
which could not be accounted for by such a simple model. 9J. E. Stem, B. D. Terris, H. J. Mamin. and D. Rugal', App!. Phys. Lett. 53,
2717 (l9RR).
One such structure is the elliptical region at the upper part of "'Y. Martin, D. W. Abraham, and H. K. Wickramasinghe. App!. Phys.
the domain wan in Fig. 2 (b). This structure is unexpected, Lett. 52,1103 (1987).
as only domain walls in the (110) plane have been found in I'R D. Terris, J. E. Stern, D. Rugar, and H. J. Mamin, Phys. Rev. Lett. 63,
unstressed GMO. It is possible that irregularities in the do- 2669 (19R9).
12B, D. Terris, J. E. Stern, D. Rugar. and H. J. Mamin, J. Yac. Sei. Techno\.
main orientations could result from crystallographic imper- A 8,374 (1990),
fections near the surface. If the polarization of these domains "n. J. Borchardt and P. E. Bierstedt, 1. App\. Phys. 38, 2057 (1967).
were not oriented perfectly normal to the crystal surface, 14A. Kumada, Phys. Lett. A 30, 186 (1969).

1705 Appl. Phys. Lett., Vol. 56, No. i 7, 23 April 1990 F. Saurenbach and 8. D. Terris 1705

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