Atomic resolution ptychographic phase contrast imaging of polar-ordered
structures in functional oxides
Ian MacLaren
1
, Hao Yang
2
, Lewys Jones
2
, Peter D. Nellist
2
, Henning Ryll
3
, Martin Simson
4
, Heike
Soltau
4
, Yukihito Kondo
5
, Ryusuke Sagawa
5
, Hiroyuki Banba
5
1.
SUPA School of Physics and Astronomy, University of Glasgow, Glasgow G12 8QQ, UK
2.
University of Oxford, Department of Materials, Parks Rd, Oxford, UK
3.
PNSensor GmbH, Otto-Hahn-Ring 6, 81739 München, Germany
4.
PNDetector GmbH, Sckellstraße 3, 81667 München, Germany
5.
JEOL Ltd., 3-1-2 Musashino, Akishima, Tokyo 196-8558, Japan
Scanning transmission electron microscopy (STEM) imaging has traditionally relied on (mostly)
incoherent imaging using electrons scattered to high angles [1,2]. This gives strong contrast for imaging
heavier atoms, but is only an incomplete technique for in ferroelectrics or polar-ordered functional
oxides, since the oxygens are invisible in the presence of the dominant scattering from the heavy cations.
In recent years, however, there has been a resurgence in the use of low angle scattered electrons using
modes like annular bright field imaging [3] and standard bright field imaging [4,5]. This allows the
direct imaging of oxygen atoms, which can be used for a full quantification of the local polarization [5],
as has previously been performed using negative C
S
imaging using high resolution TEM [6].
In principle, however, it is possible to reconstruct the phase at atomic resolution using ptychographic
methods from suitable diffraction patterns with overlapping diffraction discs recorded at each scan point
in a STEM image [7]. However, to do so practically requires the rapid recording of diffraction data,
both to allow the acquisition of images with reasonable numbers of pixels in a sensible time scale, as
well as to minimize the distortion images in real-space due to sample-drift. We show that this has now
become possible by exploiting a direct electron detector running at 1000 frames per second (fps) or
greater, which is a massive improvement over earlier CCDs running at < 30 fps.
This was applied to an unusual antiphase boundary in Nd,Ti codoped BiFeO
3
, which has been well-
characterised previously by conventional atomic resolution STEM [8,9] and HRTEM techniques. The
atomic structure and chemistry of this boundary is consequently well-understood making this an ideal
test object for atomic resolution ptychography. Atomic resolution datasets were recorded using a JEOL
ARM200F, equipped with a cold FEG source and fitted with a PNDetector pnCCD (S)TEM camera
running at up to 2000 fps. Reconstructions were performed using algorithms published previously [7].
The resulting phase image is shown in Figure 1 (top) and is compared to the HAADF image acquired
simultaneously. The phase image shows a contrast similar to that previously seen in negative C
S
images
of the same structure and can be assigned to atoms by comparison with the HAADF image. The strong
red peaks in the phase image are coincident with the green peaks in the HAADF image and must be
mixed B-site (Fe/Ti) / O columns. The broad yellow/orange peaks in the phase image are coincident
with the bright red peaks in the HAADF image and must be A-site (Bi/Nd) columns. Finally, the
weaker yellow peaks in the phase image are not seen in the HAADF image, but sit in positions which
would fit expectations for pure O columns. It will clearly be possible to determine the atom positions
quantitatively from such images and therefore perform atomic resolution polarization calculations,
which will be reported at the conference and compared with the results calculated from atomic
Paper No. 0610
1221
doi:10.1017/S1431927615006893 © Microscopy Society of America 2015
Microsc. Microanal. 21 (Suppl 3), 2015