S.

1 Magnetic signals in MFM images

To understand the origin of the image contrasts in MFM images, we performed systematic MFM

observations by changing the magnetization directions of the tip. The MFM images in Fig. S.1a, b

are obtained with tip magnetized in the opposite directions. Moreover, a lift-up height of 20 nm was

used here. The sample was magnetized at a magnetic a field of 14 T. In the MFM phase image, the

phase shift is known to show negative correlation to a force gradient [1]. Consequently, a dark spot

(negative phase shift) should be observed when an attractive force is applied to the tip, while a bright

spot (positive phase shift) should be observed when a repulsive force is applied. In the present case,

we observe bright contrasts at the dislocations, which indicate that the repulsive forces are detected

at the dislocations. The tip for the MFM measurements is considered to detect several force

components: an atomic force, an electrostatic force and a magnetic force. The atomic force is always

attractive when the tip is lifted up for more than tens of nanometers [1]. The sign of the electrostatic

force is determined by the charge states of the tip and the sample surface. In the present case, charge

state of the tip is dominated by the surface charge because no bias is applied to the tip. The sample

charge induces opposite charge on the tip, and then the tip detects an attractive force. Thus, only

magnetic force can be repulsive. Here, we can observe MFM image contrast reversals under opposite

tip magnetization directions. The fact that the force directions are switched by changing the

magnetizing directions of the tip indicates that the magnetization direction of the NiO dislocations

should be constant. If the contrasts in MFM images reflect the paramagnetic or electrostatic

behaviors, the contrasts should be always attractive irrespective of the magnetized direction of the

tip. Thus, the contrasts in the MFM images are mainly originated from the ferromagnetic property of

the dislocations.

To support the conclusions drawn from the MFM images, we perform the measurements after

applying a magnetic field of -14 T. Thes MFM with oppositely magnetized tips are shown in Fig. S1

1
c, d. These images reveal the same result as what was concluded from Fig. S1 a and b. These provide

further evidence that local magnetization is responsible for the contrasts in the MFM images.

Figure S.1|MFM images with opposite magnetization directions of a tip and the sample. a-d
AFM topographic and MFM phase images with changing the magnetization of the tips and the
samples. In each image, left panel is the topographic AFM image and right one is the MFM phase
image of the same area. Switching the magnetization directions of tip or sample reverses the contrast
in the MFM images. e A schematic showing the direction of applied magnetic field. Arrows show
“+” direction.

2
S.2 Electrostatic component in MFM images

To provide further evidences to the above discussions, EFM was measured at the same area where

the AFM topographic image was taken (Fig. S.2a), as shown in Fig. S.2b. A scan height of 20 nm

was adopted, as in the MFM case. Attractive forces are observed at the dislocations in EFM image

according to the polarization at the sample surface or topographic cross-talk. The MFM images

consist of magnetic force, atomic force and electrostatic force, while the EFM images consist of the

atomic and electrostatic forces only. The magnetic force component can hence be acquired by

subtracting the forces in the EFM image from those in the MFM images.

One could expect the electrostatic force component in MFM images by the aforementioned

measurements, but the electrostatic effect can be eliminated from the MFM images using the

following method [2]. An Au thin film of 10 nm was coated on the NiO film by plasma etching

coating. Such conductive coating averages the local polarization at the NiO film surface and the

electrostatic force component becomes uniform background. Hence, the MFM images for the sample

with conductive coating includes only magnetic and atomic force component. The topographic

cross-talk can be ignored by taking MFM images with up and down magnetized tips. Figures S2 c

and d show the MFM phase images of the NiO film with Au coating, which clearly unveil that the

dislocations have spontaneous magnetizations.

3
Figure S.2| Electrostatic force microscopy image and MFM image for Au coated sample. a,
AFM topographic image of the NiO film surface. b, EFM phase image without bias observed at the
same area as in a. The tip was lifted up for 20 nm to obtain the image. c, AFM topographic image of
the NiO film with Au coating. d, MFM phase image taken at the same area. e and f are the MFM
images taken with the tip magnetized to opposite directions.

4
S.3 Tip stray field effect on sample magnetization

Tips for the MFM observations possess spontaneous magnetizations, where there is a stray magnetic

field around the tips. This field can affect magnetizations of a sample. If the stray magnetic field

around the tips surpasses the coercivity of the sample, then opposite directional magnetization will

be formed on the sample. In this case, tip sample interaction must always be attractive and dark

contrast should be observed in MFM images. Therefore, bright contrast in the MFM image can be an

evidence for the existence of spontaneous magnetization.

To confirm this point further, we performed the MFM imaging with up and down magnetized

low-moment tips. Low-moment tips can reduce stray magnetic field in comparison to the normal

MFM tips. The AFM topographic images are shown in Fig. S.3 a and c and the MFM phase image

with up and down magnetized tips are shown in Fig. S.3 b and d. The results are the same as those

obtained using the normal tips, which indicates that spontaneous magnetization of the sample is not

affected by the tip stray field.

5
Figure S.3| MFM images with up and down magnetized low-moment MFM tip. a and c, AFM
topographic image. b and d, MFM phase image taken with up and down magnetized tip, respectively.
Dislocations show dark and bright contrast in b and d, respectively. The results are the same as those
achieved using the normal magnetic coating. Bright contrasts in a are magnetic impurities. Magnetic
sensitivity is low in LM tip, and the bright contrasts in b are very weak. It is evident that the
dislocations show the bright contrast.

6
S .4 The atomic structure model of spinel type Ni1-xO

The periodic introduction of Ni vacancies to the rock salt NiO structure results in formation of the

spinel type Ni1-xO. The structure model of spinel type Ni1-xO and comparison with the rock salt NiO

structure are shown in the following figure.

Figure S. 4| a A schematic of the rock-salt, antiferromagnetic NiO. b A schematic of the spinel type

NiO. Introduction of Ni vacancies to the specific sites result in the formation of spinel type NiO

structure.

7
S. 5 Calculation methodology and results on the bulk NiO

Calculations of structures and electronic properties were performed using Vienna ab initio

simulation package (VASP) within the framework of DFT [3]. The projector augmented wave

approach [4] was applied for electron-ion interactions with a regular Monkhorst-Pack grid of 8×8×4

k points for the bulk and 4×1×1 k points for the dislocations [5]. The single-particle Kohn-Sham

wave function was expanded using plane waves with a cutoff energy of 400 eV. The generalized

gradient approximation (GGA) of Perdew et al. (PW91) [6] plus U-method was used with U = 6.3

and J = 1.0 eV for the Ni-d states (where U is effective on-site Coulomb repulsion and J is the

exchange parameter), which have been validated on NiO in earlier studies [7,8]. The optimum lattice

constant of bulk NiO calculated using the above method is 100.25% of experimental value. The

calculated energy band is 2.5 eV, which is less than the experimental value of 3.8~4.0 eV but close to

the calculated value of 2.6 eV by Nolan et al. [9]. Deviation from the experimental value is

attributed to the well-known drawback of DFT. In the calculations, the rock-salt structure was taken

for NiO. The ground state of NiO is AFM and the AFM type-II ordering is shown schematically in

Fig. S.5a, with successive (111) planes showing an alternating spin. The AFM ordering for NiO is

confirmed in the density of states (DOS) shown in Fig. S.5b. It is found that the valence top is

hybridized character between Ni 3d and O p orbitals, while the conduction bottom is mainly

composed of Ni 3d orbitals in spin minority, indicating that the band gap is a charge-transfer type. As

for the dislocation, the predominant slip systems in the rock-salt structure were determined to be

<110>{110} both experimentally and theoretically [10,11], in which we adopted the [110](1 1 0)

system. To simulate a realistic dislocation, we imposed periodic boundary conditions along the

dislocation-line ([001]) and Burgers-vector ([1 1 0]) directions, and embedded a sufficient region of

vacuum (12 Å) in the supercell along the [110] to avoid unwanted interactions between dislocations.

All of the atoms except those in the two layers proximal to vacuum were allowed to relax. To shed

8
light on the impact of point defects on electronic properties of NiO dislocations, we introduced a Ni

vacancy into the core site in view of the facts that impurities or vacancies favor segregations at the

dislocation core and that the cation vacancy is dominant in NiO. The NiO dislocation supercells

which contain one vacancy underwent the structural relaxation again. The introduction of a single Ni

vacancy to the core site corresponds to 0.26% atom concentration.

a b 10
Total-DOS
O-PDOS
DOS (arb. units)

5 Ni-PDOS

z
-5

Ni
y
-10
O x -6 -4 -2 0 2 4 6
Energy (eV)

Figure S.5| a, Rocksalt structure of bulk NiO with a schematic illustration of its AFM ordering. b,

Total DOS and PDOS plots of O and Ni atom contributions for the optimized bulk NiO with the

AFM type-II ordering. The contribution to the valence band top comes from the hybridization

between O p and Ni d states, while the conduction band bottom is dominated by the Ni d states. The

EF position is aligned to zero.

9
S. 6 High temperature MFM measurements

We carried out the MFM measurements at high temperatures to investigate the Curie temperature of

the ferromagnetic dislocations. Figure S.6 shows AFM topographic images and MFM images

measured at 300, 400, 500, 520 and 540 K. The sample is magnetized in a magnetic field of 14 T

before heating. The images taken below 520 K show a clear dark contrast. However, such contrast

disappears in the image taken at 540 K. This indicates that the Curie temperature is in between 520

and 540 K. To confirm this point, we further carry out the MFM imaging after cooling the sample, as

shown in Fig. S.6f. The dislocations show a bright contrast in the MFM image, suggesting that the

magnetization is switched during heating. Hence, Curie temperature of the dislocations is determined

to be between 520 and 540 K. This temperature almost corresponds to the Curie temperature of the

spinel type NiO (523K) [12] and the Neel temperature of NiO (525K).

10
Figure S.6| MFM images at high temperature. AFM topographic and MFM phase images at high
temperatures. The same area is adopted for taking images at 520 K and 540 K. Dark contrasts are
observed at the dislocations below 520 K, yet are disappeared at 540 K. Images taken after cooling
show that bright contrasts, which mean that the magnetization at the dislocation, have switched
between 520 K and 540 K.

11
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