Supplemental Material to
Native defect induced charge and ferromagnetic spin ordering and coexisting
electronic phases in CoO epitaxial thin film
D. S. Negi,1,2,a) B. Loukya,1,2 and R. Datta1,2,a)
1
International Centre for Materials Science, Jawaharlal Nehru Centre for Advanced Scientific Research, Bangalore
560064, India.
2
Chemistry and Physics of Materials Unit, Jawaharlal Nehru Centre for Advanced Scientific Research, Bangalore
560064, India.
In this supplementary document we are providing supplemental experimental HRTEM images
with dark diffuse contrast areas, diffraction patterns, various types of electronic phases,
experimental EMCD of the samples. Schematic of various structures considered for the
theoretical calculation along with complete details of calculate atom specific XMCD spectra,
density of states, electron occupancy, magnetic moments obtained via mBJGGA and GGA+U
based calculations.
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FIG.S1. (a) - (c) HRTEM images from dark diffused contrast areas at different magnifications,
(d) - (f) HRTEM images from the same dark diffused contrast from different areas showing
difference in lattice parameters. The increase and decrease in lattice parameter has no
relationship with the type of contrast encountered.
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FIG.S2. Local FFT from different areas showing the strength of superlattice spots are varying
from place to place.
FIG.S3. (a) Supperlattice spots along another zone axis <011>. Commensurate reciprocal vector
0.5 <11-1> and incommensurate reciprocal vector 0.33 <-11-1>, 0.67 <-11-1>, 0.81 <-11-1>
with spots are labeled as a′, b′ and c′ in Fig.S3(b).
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FIG.S4. (a) & (b) Example experimental EMCD spectra from two different areas shoing a
variation in dichroic signal. Calculated XMCD spectra for (a) stoichiometrc CoO with two
different Co atoms in AFM configurations show no dichroic signal, (d) & (e) XMCD signal for
HS and LS individual Co atoms in VCo(16.6%), almost zero dichoric signal for LS Co atoms, (f)
XMCD spectra for VCo(4.16%) supercell.
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FIG.S5.
Schematic
structures
of
(a)
stoichiometric
VCoAFM(4.16%):CoO, (d) VCoFM(16.6%):CoO, and (e) VCo
CoO,
(4.16%):CoO
(b)
VCo(16.6%):CoO,
(c)
considered for theoretical
calculations with type-II AFM arrangements are shown.
Table S1. Cohesive energy of CoO and CoO with various defect concentrations and
configurations.
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FIG.S6. Comparative total DOS calculated by mBJGGA and GGA+U for (a) & (d) CoO, (b) &
(e) VCo(16.6%):CoO and (c) & (f) VCo(4.16%):CoO. GGA+U calculation predicts metallic state for
VCo(16.6%) and insulating state by mBJ. Experimentally the sample is insulating. Whereas both the
calculations predicts half metallicity for VCo(4.16%) case. The band gap values for both up and
down spin electrons are labeled in the respective figures.
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Table S2. Coparative electronic charges at the interstitial regions for CoO and CoO with two
different Co vacancy concentrations. With vacancy there is a significant increase in charge in the
interstitial regions suggesting charge transfer due to compensation the hole formation.
Following diagrams compare electron occupancy, magnetic moments of different atoms in CoO,
VCo(16.6%) and VCo(4.16%) obtained both by GGA+U and mBJGGA calculations.
FIG.S7. magnetic moments and electron occupancy for CoO for both Co and O atoms
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FIG.S8. magnetic moments and electron occupancy for VCo(16.6%):CoO for both Co and O atoms.
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FIG.S9. magnetic moments and electron occupancy for VCo(4.16%):CoO for both Co and O atoms
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