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Journal of Magnetism and Magnetic Materials 350 (2014) 188198

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Journal of Magnetism and Magnetic Materials


journal homepage: www.elsevier.com/locate/jmmm

Current Perspectives

Radiography and tomography with polarized neutrons


Wolfgang Treimer a,b,n
a
University of Applied Sciences, Beuth Hochschule fr Technik Berlin, Department Mathematics Physics & Chemistry, Luxemburgerstr. 10,
D-13353 Berlin, Germany
b
Helmholtz Zentrum fr Materialien und Energie, Department G GTOMO, Hahn-Meitner-Platz 1,
D-14109 Berlin, Germany

art ic l e i nf o

a b s t r a c t

Article history:
Received 23 June 2013
Received in revised form
2 September 2013
Available online 10 October 2013

Neutron imaging became important when, besides providing impressive radiographic and tomographic
images of various objects, physical, quantication of chemical, morphological or other parameters could
be derived from 2D or 3D images. The spatial resolution of approximately 50 mm (and less) yields real
space images of the bulk of specimens with more than some cm3 in volume. Thus the physics or
chemistry of structures in a sample can be compared with scattering functions obtained e.g. from
neutron scattering. The advantages of using neutrons become more pronounced when the neutron spin
comes into play. The interaction of neutrons with magnetism is unique due to their low attenuation by
matter and because their spin is sensitive to magnetic elds. Magnetic elds, domains and quantum
effects such as the Meissner effect and ux trapping can only be visualized and quantied in the bulk
of matter by imaging with polarized neutrons. This additional experimental tool is gaining more and
more importance. There is a large number of new elds that can be investigated by neutron imaging,
not only in physics, but also in geology, archeology, cultural heritage, soil culture, applied material
research, magnetism, etc. One of the top applications of polarized neutron imaging is the large eld
of superconductivity where the Meissner effect and ux pinning can be visualized and quantied. Here
we will give a short summary of the results achieved by radiography and tomography with polarized
neutrons.
& 2013 Elsevier B.V. All rights reserved.

Keywords:
Radiography and tomography
Imaging
Polarized neutrons
Meissner effect
Flux trapping
Superconductivity
Magnetic domains

1. Introduction
The applications of neutron radiography and tomography
(shortly imaging) cover a large number and quite different
research disciplines, that are all tasked with investigating the
composition of samples under special conditions such as
temperature, pressure, magnetic or electric elds, etc. and
possibly under additional boundary conditions, which inuence the measuring process. The information one obtains from
these experiments can always be distinguished into two large
classes, real space data (e.g. images,) and reciprocal space data
(scattering pattern, scattering curves). Both can be transformed into images or graphs, whereas both presume a (lot
of) theory that predicts and describes the information originally collected. Each light microscope provides real data information, i.e. images from the surface of a sample. On the other
hand, radiography, computer tomography (CT) or nuclear
magnetic resonance yield images from the bulk of a body. But
one realizes the difference between images delivered by a
n

Corresponding author at: University of Applied Sciences, Beuth Hochschule fr


Technik Berlin, Department Mathematics Physics & Chemistry, Luxemburgerstr.
10, D-13353 Berlin, Germany. Tel.: 49 304 5042 428; fax: 49 304 5042 220.
E-mail address: treimer@helmholtz-berlin.de
0304-8853/$ - see front matter & 2013 Elsevier B.V. All rights reserved.
http://dx.doi.org/10.1016/j.jmmm.2013.09.032

microscope and the ones recorded with a CT instrument: both


methods deliver real space images but the data acquisition and
treatment are quite different. A similar situation occurs for
neutron radiography and tomography, where a number of
different imaging techniques have already been realized. The
applicability of neutron imaging depends on the sample and on
the specic technique, which must be used to obtain the
wanted information.
The different neutron imaging techniques are extensively described
in many publications (e.g. [1,5,6,16,17,18,23,24,34,35,3942,5052,
5456]; however, some basic principles will be given here with
emphasis on those that use polarized neutrons.
This rather new tool of neutron scattering has lead to a number of
different techniques, which use absorption-, phase- and spin-based
interactions of the neutron with the samples. Combinations of these
interactions are often wanted and one can distinguish neutron radiography (R) and tomography (CT) into the following topics:
White beam and monochromatic neutron radiography (R) and
tomography (CT):






Absorption R/CT (white beam).


Time resolved R/CT (white beam).
Energy selective R/CT (monochromatic neutrons).
Bragg-edge R/CT (monochromatic neutrons).

W. Treimer / Journal of Magnetism and Magnetic Materials 350 (2014) 188198

Phase-based based neutron radiography (T) and tomography


(CT) are








189

2. Theoretical background
2.1. General remarks

Diffraction enhanced R/CT.


Phase contrast R/CT.
Phase grating R/CT.
Interferometer R/CT.
Refraction contrast R/CT.
Ultra-small angle scattering R/CT.

Spin based radiography and tomography with polarized neutrons combines, absorption (attenuation) and phase based interactions, i.e. with the option of polarized neutrons enormously
enlarges the eld of applications. Additionally new techniques are
emerging that reach higher resolution and exibility such as the
Larmor Labeling neutron imaging, which uses the Larmor precession of the neutron spin in magnetic elds (see e.g. Ref. [9])
Investigations of matter by thermal and cold neutron beams
are very popular, especially if magnetism comes into play. Neutrons have some very specic properties that make them superior
to other probes such as X- or gamma rays, electrons, protons,
molecular beams, light and laser if one wants to investigate not
only surface but also the bulk of a sample. The interaction of
(thermal and cold) neutrons with matter is described by the
nuclear interaction potential, given by the special isotopedifferentiating scattering lengths and there is no dependency on
the atomic number. The low attenuation of neutrons by most
elements, with some exceptions, allows for investigating large
samples (in comparison to electrons or X-rays). The spin interaction with the magnetism of a sample together with their low
velocities (for time of ight measurements) make thermal and
cold neutrons a unique probe for condensed matter research. The
interaction of neutrons with magnetically ordered matter includes
the interaction with the nuclei (coherent scattering length bc) and
with the electronic magnetic moments of incompletely lled
3d-. 4d-, 4f- and 5f-shells (see e.g. [31]). The interaction with
magnetic elds H is described by the neutron spin (and the

resulting magnetic moment m) and the Larmor frequency L LH,


with

L the gyromagnetic ratio of the neutron. One can determine

the number of spin rotations in a magnetic eld modulo 2 and


thus calculate back the amount of H if the path length of the
neutrons in H is known (see below).
The investigation of samples with respect to their magnetic
properties therefore benets from polarized neutron beams. The
knowledge of the initial and nal states of the neutrons, i.e. the
detection of the polarization after the transmission of neutrons
through a sample, is a valuable information and determines
contrast of an image (Fig. 1). In this eld last few years witnessed
the development of new polarizers/analyzers (e.g. the so-called
benders based on supermirrors), which combine high transmission with high polarization.

Fig. 1. Layout of an instrument for imaging with polarized neutrons: neutrons from
a source are polarized and guided to the sample, which e.g. depolarizes the beam,
which is spin-analyzed and then 2D-detected.

Principally there are two different optical geometries for


neutron imaging. The rst method uses the pin hole technique,
i.e. the neutron beam is collimated by an entrance aperture D and
a long ight path L of approximately 5 m up to more than 10 m.
The better the collimation here given as the L/D ratio the better
is the spatial resolution at the 2D detector (see Fig. 2). With such a
setup one can use the whole white neutron spectrum (0.051.5
nm) and thus an intense beam for strong-absorbing or timeresolved radiography or tomography. This can be a disadvantage
for wavelength dependent radiographies and tomographies that
appear smeared and blurred at the 2D detector; however very
often the absorption contrast by some details in a sample is the
important information, which is to be visualized. Using a high
neutron ux (e.g. 107108 neutrons/cm2) one must be aware of
sample activation issues, which may even destroy it.
The pin hole technique is easily explained, as shown in Fig. 2.
The L/D is the inverse beam divergence and determines the spatial
distance of two points at a given distance ld. If the distance ld of
two points in a sample to the detector is e.g. enlarged, i.e. the
detector is placed at ld x1 or ld x2, then at a certain distance ld
the points in the image cannot be distinguished from each other as
shown in Fig. 3.
The second kind of neutron imaging uses a single crystal or a
double crystal monochromator, the latter maintains the ight direction of the neutron beam while selecting the wavelength [53]. In the
case of a single or double monochromator crystal (often pyrolytic
graphite) a main wavelength and a certain wavelength band is Bragg
reected (thus selected) depending on the divergence of the incident
neutron beam and the mosaic spread of the monochromator. The
selected wavelength band denes the momentum resolution Q/Q
(Q 4 = sin ), the L/D ratio denes the spatial resolution, and
both must be adapted and optimized to the imaging problem to be
solved [57,58].
In the case of a crystal monochromator the circumstances are a
little bit more complicated, than for the pin hole technique,
because the simple law of L/D l/d does not hold any more [57].
The crystal monochromator can be seen as consisting of many
pin holes (mosaic blocks). From each of these a beam is reected
with the divergence of the incident beam. Under certain boundary
conditions it is possible to optimize D and L with respect to the
given mosaic spread and gain neutron intensity because L can be
reduced and at the same time the spatial resolution can be
improved, as shown by Fig. 4. One sees that despite decreasing
L, P1 and P2 can be better resolved on the detector screen. This
technique is very successfully applied to radiography and tomography especially with polarized neutrons [59,61,62].
In the case of a double crystal monochromator two graphite
crystals are operated in the parallel arrangement [53]. The rst
crystal selects a wavelength band out of the incident neutron
beam and the second one reects it back to the initial direction.
So one can continuously change the wavelength between e.g.
0.2 nm and 0.62 nm, depending on the wavelength distribution of

Fig. 2. Pin hole geometry: D diameter of the aperture, L distance of D from two
points, ld distance of the points from detector (screen), and d1 and d2 blurred
images of point 1 and point 2 respectively (see text).

190

W. Treimer / Journal of Magnetism and Magnetic Materials 350 (2014) 188198

which inuence the Larmor precession of the analyzed spins and


thus the detected image.
2.2. Theoretical background for imaging with polarized neutrons

Fig. 3. For a given L/D, the distance ld of the detector screen from P1 and P2
inuences the resolution to distinguish the two points. At ld P1 and P2 can be
separated, as well as at ld x1; at ld x2 no separation is possible.

Fig. 4. Using a crystal monochromator the spatial resolution depends on L and on


the mosaic spread of the crystal. Note, that decreasing L improves the visibility of
P1 and P2, in contrast to the classical pin hole technique.

the incoming beam or geometric restrictions. The distance of the


second crystal to the sample determines, as mentioned above, the
spatial resolution.
The 2D image at the detector is smeared by several contributions: once there is the nite size of a detector pixel, another one
the geometrical smearing due to the beam divergence and
the distance of the object from the detector (screen),1 furthermore
additional smearing effects occur due to the nite thickness of the
detector (scintillator screen). This blurring and the resolution of an
imaging set-up are quantied by the point spread function PSF
PSFx; z

2 =2
1 fx x0 2 z  z0 2 g3=2
2

here is the slope of the tangent in x0 and z0, and x0 and z0 are the
coordinates of the center of the image point. Often it is better (and
easier) to determine the edge spread function E(x) which can be
tted to the measured data (background and amplitude must be
tuned to the data),
Ex

1
1 ex  x0 

The determination of smearing effects involves the determination


of the spatial resolution of an imaging system, which is usually
performed by measuring the modulation transfer function (MTF).
This can be done either by using absorption gratings with varying
lattice spacing and measure the contrast of the transmitted
intensity as the function of the line pairs per unit length (e.g.
lp/mm); or by measuring the edge spread function and t the
image of the edge to the function E(x). The Fourier transform of the
derivative of E(x), FT{E(x)}, yields the modulation transfer function
and thus at 10% FT{E(x)} the spatial resolution of the image [5052,
54,55]. In the case of polarized neutrons, where an analysis of the
neutron spin occurs, two further sources of blurring must be
considered, one is the analyzer itself, which causes blurring
because its transmission can inuence the geometry, and another
is due to small gradients of magnetic elds around the analyzer,
1
Note that points at or close to the surface of the object lay closer or further far
from the screen.

The use of polarized neutrons for imaging can be traced back to


1996, when at the Berlin research reactor (BER II reactor) of the
Helmholtz Zentrum Berlin Wannsee (former Hahn Meitner Institute) the rst tomography of the stray eld of a small permanent
magnet could be reconstructed. However it took several years
before this experiment was published [5052]. The basic layout,
however, remained the same and is very similar to that used in
modern instruments for radiography and tomography with polarized neutrons such as PONTO II at the BER II (Fig. 5).
When comparing the existing instruments, several differences
exist in the layout. Some use a white beam and polarize neutrons
with 3He lters reaching polarizations up to 90% for a large
wavelength band. Other instruments are situated at spallation
sources such as PSI (Switzerland), SNS (USA), JPARC (Japan), ISIS
(GB) or at the future European Spallation Source (ESS) in Lund
(Sweden). Some others are designed for special uses [7,19,39,57].
Radiography and tomography with polarized neutrons utilize
both the low attenuation by most of the elements and the strong
interaction with magnetic elds. Imaging with polarized neutrons
is therefore suitable for the investigation of magnetic eld distributions in the bulk of materials as was shown in last years.
When using polarized neutrons not only for imaging one
must consider the physics of interaction of neutrons with magnetic elds and the microscopic magnetic moments. In neutron
physics the technique of spin rotation and spin analysis is well
established. First of all one has to determine the initial spin state
with respect to a given direction in space. This is achieved by using
polarizing devices, i.e. and for the polarization of a neutron beam
several options are available. For neutron radiography and tomography so-called benders, 3He-lters [20,12] or periscope-type
polarizer guides are used [34,35,7]. Benders use the different
angles of total reection for spin up ad spin down neutrons at a
magnetized surface [15]. The geometry of such devices can be kept
very compact (  30 mm length) which is benecial for spin
analyzers, because the distance of the detector from the sample
should be kept as small as possible, much less than 100 mm
(ignoring stray elds). 3He polarizers use different cross-sections
for spin up and down neutrons when they pass a spin polarized
3
He gas. Neutron periscope work similarly to the double crystal
monochromators, but they consist of two parallel polarizing
neutron supermirrors that preserve both the beam collimation
and the spatial resolution [34,35]. The use of one of these methods
depends on the problem to be solved.
The spin analysis is done either with a bender or with polarized
3
He gas. Here several (competing) conditions must be optimized.
The distance from the sample to the detector shall be as short as
possible (cf. Figs. 2 and 3), on the other hand, the change of the
spin orientation caused by the sample must be analyzed, i.e. the
spin analyzer must be placed between sample and detector and it
must not inuence the magnetism of the sample under investigation, i.e. stray elds (of the spin analyzer) must be kept as low as
possible. External magnetic elds applied to the samples must not
overlap with the stray eld of the spin analyzer because they may
change the direction of magnetic eld at the analyzer and thus its
direction along which the neutron spin is analyzed.
The description of the neutron spin in a magnetic eld can be
treated rather classically. A neutron with a energy of some meV
behaves like a classical particle thus the motion of the spin can be
described like a magnetic moment in a magnetic eld. Starting
with circling motions of charges that produce a magnetic moment
one can imagine an electron for which motion creates a magnetic

W. Treimer / Journal of Magnetism and Magnetic Materials 350 (2014) 188198

191

in a eld B is determined by the path integral of the magnetic eld B


over the neutron trajectory, i.e. one gets
Z

m
L t L Bt L Bds L Bs
7
h
v
where v is the velocity of the neutron, B is the magnetic eld, m is
the neutron mass, s is the path length of the neutron in the magnetic
eld B, is the neutron wavelength and h is the Planck constant. The
velocity and the wavelength are related to each other (de Broglie) as
h/p, pmv, mmass of the neutron, and vvelocity. h/
m3.956034  10  7 m2/s, for v3956 m/s, the wavelength
1  10  10 m0.1 nm1 . The neutron spin performs Larmor
precessions L also when the neutron passes through an (inhomogeneous) magnetic eld B, and thus the path integral depends on the
particular path through the eld. The angle of rotation is given by Eq.

Fig. 5. Layout of Polarized Neutron Tomography II (PONTO). A graphite monochromator reects neutron wavelength between 0.28 nm and 0.47 nm to the optical bench
which can be rotated around the C-monochromator. Length of the instrument  4 m,
items on the optical bench are displayed in an exaggerated manner.

(7), i.e. one has to know , s and B to determine . The knowledge of


is always a number modulo 2, but the strength of B can be
derived (locally) from small changes of s s, and B(s) and B(s s),
for the assumption that o2 for B(s)-B(s s). Determining for
B(s) and B(s s) yields B for a larger region (due to continuity of B).

moment m. For this idea one has to consider the magnetic moment
m, which is classical derived from a rotating electric charge e on a
circle with the radius r and the velocity v as
 
ev
e !
!
jl j
3
r2  
2 r
2m
!
and analogous with this, in quantum mechanics the spin S is
!
connected with angular momentum l as

From Eq. (7) one also realizes that the slower neutrons, the more
Larmor precession are performed in B.
For the visualization of the magnetism of a sample the beam
must be polarized and analyzed with a spin polarizer and an
analyzer and a 2D-detector (Fig. 1). The sensitivity of the spin
direction on B is quite high: For e.g. B 1 mT and a neutron
velocity of 103 m s  1 (wavelength 0.3956 nm) the spin rotates in

!
!
l
S
!
and !
m s g s mk
m l g l mk

e
meV
mk
3:1525  10  14
2mP
T

wavelength spread of 0.05 (70.025) causes a spread of the


spin rotations of 5.251 which changes nearly negligibly the beam
polarization, thus one can work with a rather large wavelength
4

where mP is the mass of a proton, mk is the nuclear magneton


(mk 5.05078343  10  27 J/T), h is the Planck constant
(6.6260755  10  34 J s) and h/2. The gl,s are the g-factors
distinguishing protons and neutrons. For protons gp,l 1 and
gP,s 5.5857, whereas for neutrons gn,l 0 and gn,s  3.826085.
Thus the magnetic moment of the neutron mn  1.9130427mK, i.e.
mn  9.662364  10  27 J/T. The time-dependent motion of the
spin of a neutron S S(t) in a magnetic eld B is described by
!
!
!
dSt 

5
 k g n S t  B tj j x; y; z
dt 
h
j

The motion of the spin can be seen as follows. If the spin S S(t) is
given in an rectangular coordinate system, where the magnetic eld
B is parallel to the z-axis, S(t) can be written as (see also small sketch)

0
1
cos
!
B
C
St S@ sin A
0

The circling motion of the spin has a so-called Larmor frequency


L LB. L is the gyromagnetic ratio of the neutron, L gmN/
1.83247  108 rad s  1 T  1. L is independent of the neutron
wavelength, but a neutron (spin) passes magnetic elds which have
certain extents, thus the time a neutron needs to pass specic
magnetic elds depends on its velocity, i.e. its wavelength. With
L t the angle of rotation is given by Lt, with t is the time the
spin moves in the magnetic eld B. Thus the number of spin rotations

a path length of 10 mm by an angle

1051. At the same time a

spread of up to  10%. Note, that at 0.3956 nm and e.g. a Bragg


angle

 36.21 the pure mosaic spread 70.21 0.41 of a

monochromator crystal (graphite) causes a  0.01. This has


to be taken into account for the measured intensity I I(x,z)
(Eq. (8)) after the sample, which depends on the incident intensity
I0, the attenuation due to the sample and the spin orientation in front
of the spin analyzer. The different transmission factors of the spin
polarizer, collimators and spin analyzer are combined in the factor T
and the intensity measured with a 2D-detector can be written as
 Z

1
Ix; z I 0 x; zT exp 
sds 1 cos x; z
8
2
path
|{z}|{z}
I att x;z

I spin x;z

where is the linear attenuation coefcient of the sample. Ispin is the


amplitude of an oscillating cosine function and describes intensity
oscillations due to spin precession in the magnetic eld B. The path
integral in the exponential function yields the attenuation of the
neutron beam by the sample, the cosine-term determines the
spatial-dependent oscillations due to spin rotation in the sample.
The path integral is calculated with the Radon transform of the crosssection of the sample (cp. Fig. 6) which yields the path lengths of a
neutron through the sample.
To calculate Ispin one has to determine all possible paths of
R
neutron spins through the sample and calculate Bds. The solution
of this problem is known from computerized tomography, but the
way to nd a solution depends also on the problem to be solved.
For the investigations of e.g. magnetic domains a special reconstruction method as used [22,25] utilizing tting routines that are
applied to incomplete data sets. Another method (preferred by
these authors) is to assume a reasonable B-eld model and t this
model to the measured data. This means that the measured
projections (two-dimensional depolarization images) are

192

W. Treimer / Journal of Magnetism and Magnetic Materials 350 (2014) 188198

Fig. 6. (a) Polarized neutrons and a homogeneous magnetic eld create an image of non-equidistant fringe pattern, and (b) theory and experimental result (neutron images)
of the increasing B-eld in the copper coil.

compared with calculated Radon transforms of the model. The


path integrals are projections of the Radon Transform R{f} [6062]
Z 1 Z 1
 
f x; zp  x cos  z sin dx dz
R f f^ p;
1

1

9
where p is the scanning variable over the 2D function {f} and the
angle under which the sample is scanned. For investigations of
ux trapping the samples were scanned under 01 and 901 with

respect to the neutron ight direction, yielding for 0 and for


901 the Radon transform for the sample orientations 01
(parallel to the neutron beam) and 901 (perpendicular to the
neutron beam). However, the neutrons are polarized in front of
the sample and spin analyzed after the sample. The spin-analyzed
neutron intensity measured behind a sample, orientated parallel
and perpendicular to the neutron ight direction is given by
Z

1
Ix; z I 0 T exp 
sds 1 cos x; z
2
path
|{z}|{z}
I att x;z

I spin x;z

1
Iy; z I 0 T exp 
sds 1 cos y; z
2
path
|{z}|{z}
I att y;z

10

I spin y;z

3. Imaging with polarized neutrons of superconductors


The rst image of a magnetic eld of a small magnet was
realized already in 1997 at the BER II and later published [5052].
Neutron radiography and tomography with polarized neutrons
became more prominent when instruments and detector systems
for neutron imaging were improved and more than 10 years later
much better radiographies with polarized neutrons were published. Remarkable, progress was achieved using phase contrast,
mainly pushed forward by the development of grating interferometers [28,29,4345] and its application to imaging magnetic
domains [25]. The potential applications of imaging with polarized
neutrons are very large; therefore the focus here is put on the very
rst use of this method in superconductivity. It is well known that
superconductors exhibit zero electrical resistance and the Meissner effect (magnetic eld expulsion). However, it is less known
that magnetic elds can be trapped or pinned in superconductors.
All these effects occur in the superconducting state of a material,
i.e. when it is cooled below its individual critical temperature Tc,
when the electrical resistance disappears and magnetic elds
are expelled. Innumerable investigations about the expelled and
trapped magnetic eld have been published since Landau [21]
tried to explain the magnetic pattern on the surface of a

superconducting sample and the magnetism inside it. An interesting physics is the co-existence of two phases, superconducting
and normal conducting especially in superconductor type I samples, because, in contrast to type II superconductors, these should
not exhibit any ux trapping or ux pinning. Thus investigations of
the bulk of samples that are in the superconducting state unveils
size, shape and structure of these trapped or pinned magnetic
elds and give answers on how this can happen.
3.1. Imaging magnetic elds of superconducting samples
The main purpose of experiments with polarized neutrons was
to visualize expelled and trapped magnetic elds of samples in the
superconducting state. The samples were lead (superconductor
type I) and niobium (superconductor type II). The suppressed
Meissner effect and ux trapping are better known from superconductor type II; however as mentioned above they were also
observed in type I superconductors, such as in lead. To explain and
underline the precision of the experimental results, the starting
point was the image of the magnetic eld created by a Cu coil.
An electric current in the coil creates an homogeneous magnetic
eld B, as is known from fundamental electrodynamics. The
strength of B is given by the current I [Amperes] (varied from
4 A up to 6 A), the length of the coil (90 mm) and the number of
windings (205). With Eq. (7) the number of the Larmor precessions can be calculated for each path through the coil, which yields
an image as shown in Fig. 6.
The spin analyzer behind the sample is transparent for parallel
spins (spin up) and opaque for anti-parallel spins, i.e. for a spin
rotation of (spin down). The spin rotation angle (Eq. (7)) is
proportional to Bs, and s is the path length through the sample
as shown in Fig. 6. Due to different s (and given B) the spin

rotation angle changes, which is analyzed with the spin analyzer


in front of the detector.
The images of Fig. 6 hold for a magnetic eld which is
homogeneously distributed in the volume under investigation
(coil). A similar behavior was expected in the case of the partially
suppressed Meissner effect, i.e. occurance of ux trapping in the
intermediate phase, a state where normal and superconducting
volumes occupy simultaneously different parts of a cylindrical
sample.
The samples used for the investigations of ux trapping in
superconductors were crystalline and polycrystalline lead, both
having a high purity (99.9999 wt% Pb) and the same dimensions.
The crystal samples were o110 4 orientated, the mosaic spread
was 1.71, the diameter 12 mm and the length 30 mm. The critical
magnetic eld Bc depends on the sample temperature according

W. Treimer / Journal of Magnetism and Magnetic Materials 350 (2014) 188198

to [8]
"
Bc T Bc 0 K 1 

T
Tc

2 #
1  N

11

For Pb, Bc (0)80 mT. N is the so-called demagnetization factor


which depends on the geometry of the sample and is given by
N 1

1
1 a=hq

12

where a ( 6 mm) and h ( 15 mm) are the radius and the half
length of the cylinder, respectively, and q is given by as
q

4
2

 tan 1:27  h=a  ln 1 a=h


3 3

13

Fig. 7. Temperature dependence of the critical magnetic eld for the used Pb
sample geometry 01. At T 5.5 K the applied external magnetic eld was
Bext 6.4 mT, which is well below Bc 25 mT (blue curve). (For interpretation of
the references to color in this gure legend, the reader is referred to the web
version of this article.)

Fig. 8. External magnetic eld orientation with respect to the sample and neutron
ight direction.

193

Thus the demagnetization factor N of the Pb samples was equal to


0.8837. The external eld Bext was 6.4 mT and at T5.5 K it was
well below the critical Bc 25 mT (see Fig. 7).
Because the Pb samples had the same cylindrical shape as the
copper coil, one would expect in the case of a partial Meissner
effect an homogeneous ux trapping/pinning. The Pb samples,
however, showed very different images. For the measurements
with polarized neurons they were kept in a special Al holder in a
cryostat and cooled stepwise from room temperature down to 8 K.
The magnetic eld (from Helmholtz coils) applied to the sample
was 6.4 mT, orientated as shown in Fig. 8. When the sample was
further cooled down to 5.5 K radiographs (without and without
the external magnetic eld) were recorded rst at T 8 K and then
at T 5.5 K (with and without the external magnetic eld). The
critical temperature Tc of lead is 7.19 K.
The axis of the lead sample was adjusted parallel to the neutron
ight direction, and at the presence of the external magnetic eld
images were recorded at T8 K and 5.5 K. At T5.5 K a characteristic fringe pattern appears, which is attributed to the expulsion of
the magnetic eld (Fig. 9). The asymmetry of the pattern can be
explained (and calculated) by a small disorientation of the sample
with respect to the neutron propagation direction. When increasing
the temperature to T8 K (i.e. above Tc) the fringe pattern disappears. Fig. 9 also shows that a fraction of the applied eld may be
trapped in the sample, i.e. ux trapping is possible. At a second step
the sample was again cooled down to T5.5 K and in the presence
of the external magnetic eld was rotated by 901 perpendicular to
the neutron propagation direction. In this conguration the eld
was switched off and images were recorded as shown in Fig. 10.
If the rod axis is horizontally perpendicular to the incident
neutron beam direction, the path length through the cylinder
depends only on the height (z-value) of the beam, and is at most 2r
if it passes through the middle of the cylinder (cf. Fig. 6). Thus the
image of the projection of the magnetic eld was assumed to be
similar to the image of the magnetic eld of the coil. Fig. 10 shows
the 2D-spin-analyzed images at T 5.5 K, 6.8 K and 8 K. One sees a
nearly perfect horizontal nearly equidistant fringe pattern at
T 5.5 K, which changes when the temperature is raised to 6.8 K.
At T 8 K, i.e. above Tc 7.19 K, the fringe pattern disappears.
In order to explain the observed images the trapped eld must
fulll several boundary conditions. The Radon transforms must
yield a fringe pattern as the one shown in Figs. 9 and 10. In
addition the trapped eld must be less than the applied Bext and
the sum of expelled and trapped elds must be less or equal the
applied magnetic eld (energy conservation). At the inside at the
surface of the sample B must become small because no fringe
patterns were observed. On the other hand, outside of the sample
the expelled eld must follow an exponential law.
The solution to this problem was a Gaussian shaped eld,
where only two parameters were tted to the experiment, the
FWHM of the function and the amount of the trapped eld
[61,62]. Fig. 11 shows a series of calculated radiographs varying

Fig. 9. Pb polycrystalline sample, polarized neutron images of a partial Meissner effect: rod axis 01 with respect to the neutron beam direction: (a) T 5.5 K and (b) overlap
calculated image and experiments, at T 7.4 K the fringes disappear (see text) (courtesy PRB).

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W. Treimer / Journal of Magnetism and Magnetic Materials 350 (2014) 188198

Fig. 10. Pb polycrystalline sample: rod axis 901 with respect to the neutron ight direction: (a) T 5.5 K, (b) T 6.8 K, and (c) T 8 K. No further images processing was
applied to see these rst original images of a trapped magnetic eld which is not homogeneously distributed in the homogeneous sample (permitted reuse, by courtsey of
Phys. Rev. B).

Fig. 11. (a) Variation of the trapped eld B, FWHM is kept constant, the eld was adapted to the geometry of the lead cylinder; note the sensitivity of B on the fringe pattern,
tuning further the FWHM of the Gaussian function the calculation agree perfectly with the pattern for both, the suppressed Meissner effect (Fig. 9 and ux trapping
((Fig. 10b) [61], permitted reuse, by courtesy of Phys. Rev. B).

Fig. 12. 3D model of the trapped magnetic eld. The strength of B increases towards the rod axis and decreases to zero at the inner side of the sample surface [61] (permitted
reuse, by courtesy of Phys. Rev. B).

the amount of trapped eld. This series did not result in the best
t with respect to the FWHM, which also had to be adapted.
The Gaussian shaped eld is constant, parallel to the rod axis,
but squeezed around the rod axis, the FWHM was estimated to be
1.45(5) mm. The expelled eld was also tted by a Gaussian
function, which has its maximum at the rod axis but is zero inside
the sample. The t was compared with the experimental images as
shown in Fig. 11, a model of the calculated trapped eld is shown
in Fig. 12.

Besides the rst experiments with crystalline, pure and medium


pure Pb samples one should mention recent experiments of composite samples, i.e. samples which contain other elements and have
different critical temperatures. The question was, how do expelled
and trapped magnetic elds behave if in the superconducting phase
of the main body of a sample (Pb) parts of lead were replaced by
non-superconducting parts (e.g. Al, special steel, air). For this reason
a lead sample was modied by inserting aluminum and iron screws
and creating a hole, which remain normally conducting T7.19 K,

W. Treimer / Journal of Magnetism and Magnetic Materials 350 (2014) 188198

195

Fig. 13. Observation of partial Meissner effect and ux pinning in a composed Pb sample (left sketch), [62] (permitted reuse, by courtesy of Appl. Phys. Lett.).

Fig. 14. (a) Magnetic ux trapping in a Nb sample, Tc 9.25 K. The sample was not treated (chemically polished). One recognizes a temperature dependence of ux
trapping (T 5.5; T 9 K) that vanishes at T 11 K 4Tc 9.25 K. Only less than a quarter of the disc is shown (diameter 45 mm). (b) Nb sample with holder for the cryostat.

Fig. 15. Images obtained from the same sample as in Fig. 14, but the surface of the sample was this time chemical polished. This treatment removes (mosaic) surface
structures and apparently inuences the trapped ux. For T 4Tc the patterns disappear.

where lead is superconducting. The interesting result was, that the


squeezing effect again could be observed but not in all parts of the
lead sample. Calculations (assuming non-symmetric eld sources)
could partially prove this effect [63,64]; however further, detailed
measurements are necessary (Fig. 13).
A similar behavior of anisotropic ux trapping but a completely
suppressed Meissner effect was observed in disc shaped niobium
samples. Niobium is a type II superconductor with Tc 9.25 K. As a
part of detailed investigations, Nb samples were tested with polarized neutrons [2]. Radiographies with polarized neutrons and spin
analyzed images should reveal the effect of surface polishing on the
suppressed Meissner effect as well as on the amount of ux trapping,
Figs. 14 and 15 show the (surprising) results. The procedure of the
measurement was the same as for the lead samples, i.e. the samples
were cooled by a cryostat down to T11 K (i.e. above Tc 9.25 K) and
then images were recorded with and without an external magnetic
eld at the temperatures as shown in Figs. 14 and 15.
Fig. 14 (and other images, not presented here) shows that a
complete suppression of the Meissner effect could be imaged, which
was conrmed by other magnetic eld measurements. It could also be

conrmed that surface treatment has a great inuence on the


magnetic eld distribution, as shown in Fig. 15. Comparing the images
for T5.5 K and T9 K in Fig. 14 (untreated) with the same ones in
Fig. 15 (treated) one realizes, once the visualized position resolved
difference of ux trapping and then more homogeneous distribution
of the trapped eld, seen as a decrease of the fringe pattern and fringe
contrast in the radiographs of Fig. 15.
For this eld distribution up to now no unique description of
the expelled and trapped magnetic eld could be found as for the lead
sample. One problem stems from the absorption, i.e. one could not
image the bulk of the samples when their surfaces were parallel to the
neutron ight direction (cf. Fig. 14b, 901 position). Additional problems
arise from the geometry and size of the samples. This work will be
continued with other geometries and magnetic elds. Internal stress
and strain may also an impact that can be unveiled with imaging.
3.2. Imaging magnetic domains
As a second eld of applications the investigations of
magnetic domains shall be given. Magnetic domains are the

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W. Treimer / Journal of Magnetism and Magnetic Materials 350 (2014) 188198

building blocks of macroscopic magnetism and they play a


fundamental role in the theory of micro-magnetism. Therefore
besides industrial and economical demands for low energy
loss magnetic devices the study of domains by means of
neutrons has already a long tradition [3]. With X-rays and by
means of Lang topography high resolution images of
magnetic domain structures in thin samples (spatial
resolution 10 mm) could be already realized [30]. The rst
neutron topographies of magnetic domains were published by
Schlenker and Baruchel [36,37]. Neutrons would be much
better suited but due to the much lower uxes which were
available at neutron sources and also due to the lack of suitable
and optimized setups different techniques were used to
explore details of magnetic domains [3,4]. The rst work with

Fig. 16. Design of a grating interferometer ([25], permitted reuse, by courtesy of


Nat. Commun.).

Fig. 17. Measured transmitted intensity with the grating interferometer ([25],
permitted reuse, by courtesy of Nat. Commun.).

neutrons used refraction of (unpolarized) neutrons by Bloch


walls, i.e. by the boundaries between two different orientated
magnetizations. Pioneering work was done by Schrpf [32,33],
who applied dynamical diffraction to domain wall systems and
gave the formulae for the scattered intensities. These rst
experiments (performed at the low-ux research reactor of
the PTB Braunschweig) were continued with the high angular
resolving double crystal setups at the BER II reactor (Berlin),
where the (zig-zag) structure and thickness of Bloch walls in
o 110 4 Fe4 at% Si single crystals could be determined
uniquely and with high accuracy [38]. With the use of a double
crystal diffractometer other details such as mosaic block distributions and Bloch wall junctions [4648], Bloch wall thickness [13,14] and the shape of Bloch walls in the bulk of Ni
samples could be determined ([14,26,27]) and thus contribute
to the understanding of the interplay of external magnetic
elds and forces on the domain structures in the samples.
All studies of magnetic domains required either thin crystals (for
topography) or well orientated samples for spin-dependent refraction of neutrons by the Bloch walls. Very recently another attempt
was done using the special technique of a grating interferometry.
This method was rst introduced to X-rays [28,29] later on applied
to neutrons [10,11,4345] and used for three dimensional imaging
of magnetic domains in a Fe 12.8-at% Si single crystals [25].
The principle of a grating interferometer is based on the
Talbot effect. Three gratings, GS, GPh and GA, (see Fig. 16) are
matched to each other at distances L1 and l1 and have periodicities pS, pPh and pA. A source grating GS provides a (partially)
coherent wave front (with periodicity pS), illuminating the phase
grating GPh which is placed downstream at L1 (  5 m). The
periodicities pPh and pA of the gratings GPh (phase) and GA
(absorption) are related to each other as pA pPH/2. Using the
(Talbot) condition pSl1 pAL1, GA is at the rst fractional Talbot
distance l1 .The rst fractional Talbot distance l1 is given by
pA 2 =2. Thus the wavelength determines the periodicities of
pPh and pA and of course L1. The phase grating modulates the
beam causing a phase shift of /2 between neighboring beams in
the rst fractional Talbot distance. The absorption (analyzing)
grating GA scans the pattern, which is modulated by the sample.
The imaging signals are absorption, refraction and ultra-small
angle scattering, measured as a damping, a phase shift and
smearing of the oscillating curve, when GA or GS is moved
perpendicular to the beam.
Therefore, a tomography consisting of many radiographies of a
sample obtained using phase grating interferometry involves a quite
complicated scanning and reconstruction. The idea can be explained
by experiments with a special double crystal diffractometer, where
absorption, refraction and small angle scattering could be determined
simultaneously and so 2D and 3D reconstruction of samples from

Fig. 18. TalbotLau neutron radiographies of magnetic domains. (a) Sketch of the FeSi sample. (b)(f) Radiographic projection images at different external magnetic elds.
(c)(f) Equal eld strength in (c) and (h), (white bar 3 mm), ([25], permitted reuse, by courtesy of Nat. Commun.).

W. Treimer / Journal of Magnetism and Magnetic Materials 350 (2014) 188198

197

Fig. 19. Reconstruction from a TalbotLau neutron tomography of a FeSi wedge. (a) and (b) Sketches of the FeSi wedge ((a) front view and (b) side view). (c) Horizontal slices
at different wedge thicknesses as indicated in (b). (d)(g) Cross-sections through the TalbotLau neutron tomogram along different planes (dotted by (d)(g) in (a) and (b))
that show the high complexity of the 3D shape of magnetic domains. (h) Horizontal slice (as in (c)). (i) Enlargement of the area marked in red in (h) ([25], permitted reuse, by
courtesy of Nat. Commun.). (For interpretation of the references to color in this gure legend, the reader is referred to the web version of this article.)

projections could be achieved [49,40,41]. In this case, the scanning


procedure is more complicated because for each projection the phases
had to be scanned over one period (Fig. 17).
The achieved results are shown in Figs. 18 and 19. Different
slices could be extracted and magnetic domains identied.
With these measurements it could be demonstrated that randomly orientated magnetic domains could be detected even in the
bulk of massive samples. It must be mentioned that the limited
spatial resolution allowed for imaging of rather large domains,
smaller ones could not be detected but in comparison with
standard, classical methods, phase grating interferometry is a good
step forward in this eld. This technique is very young and therefore as happened in other disciplines many new experiments
will bring new results and deeper understanding of matter.

4. Summary
Imaging with polarized neutrons is widely used [23] and the eld
of applications is increasing, because of the large potential of this
method. Up to now imaging with polarized neutrons is still something exotic, it requires knowledge about radiography and

tomography, about neutron scattering in general and about polarized


neutron scattering in detail. Furthermore it requires good polarization and spin-analyzing components (P495%) to achieve a good
spin-upspin-down ratio (spin contrast), a well collimated beam to
avoid smearing effects due to different depolarization effects, no
magnetic stray elds from other devices (sample magnet, etc.). The
beam collimator, polarizer and spin-analyzer also reduce the intensity of the neutron beam. So for certain experiments sometimes the
use of 3He polarizer is a big advantage because it allows for using the
full neutron spectrum. For a detailed analysis of the bulk magnetism
of a sample, monochromatic neutrons yield simpler results because
they allow a dened analysis of the transmitted neutron spin. Up to
now there are a lot of new ideas what can be realized with polarized
neutron imaging, and in the future there will certainly be a polarized
neutron imaging instrument at the European Spallation Source (ESS)
in Lund, Sweden, where most of the fascinating new ideas will be
realized and lead to exciting new physics and results.
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