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Reference
Polarized light studies of ferromagnetic/ferroelectric/ferroelastic domain patterns in NiCl and NiBr boracite
BRUNSKILL, Ian Hedley, SCHMID, Hans
Abstract
Ferromagnetic stripe domains were observed in polarized light along the optic axes of the orthorhombic NiCl and NiBr boracites below ∼9K and ∼30K, respectively. The spontaneous magnetization vector is found to lie along the principal refractive index nγ. Measurements of spontaneous Faraday rotation and spontaneous birefringence down to 4.2K are presented.
BRUNSKILL, Ian Hedley, SCHMID, Hans. Polarized light studies of
ferromagnetic/ferroelectric/ferroelastic domain patterns in NiCl and NiBr boracite.
Ferroelectrics, 1981, vol. 36, no. 1, p. 395-398
DOI : 10.1080/00150198108218137
Available at:
http://archive-ouverte.unige.ch/unige:30824
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POLARIZED LIGHT STUDIES OF FERROMAGNETIC/FERROELECTRIC/FERROELASTIC DOMAIN PATTERNS IN NiCl and NiBr BORACITE
IAN H. BRUNSKILL and HANS SCHMID
Department of Mineral, Analytical and Applied Chemistry, University of Geneva, CH-1211 Geneva 4, Switzerland
Abstract - Ferromagnetic stripe domains have been observed in polarized light along the optic axes of the orthorhombic NiCl and NiBr boracites below ~9K
and ~30K, respectively. The spontaneous magnetization vector is found to lie along the principal refractive index ~· Measurements of spontaneous Faraday rotation and spontaneous birefringence down to 4.2K are presented.
INTRODUCTION
The 3d-metal boraciteGM3B7
o
13x,
abbreviated MX, with the compos1t1ons M=Fe, Co, Ni, Cu and X=Cl, Br, I (except Cui) are known to be weakly ferromagnetic ferroelastic ferroelectricsl,2, being transparent in the visible. So far observations of ferromag- netic domains have been reported for Nii3,4,5 and CoC12 only. In this work the composi- tions remaining cristallographically orthorhombic down to 4.2K, MnCl,MnBr,Mni,NiCl,NiBr, CuCl and CuBr, have been examined with a view to make visib~ ferromagnetic domains. For NiCl and NiBr the search was successful; their respective spontaneous magnetizations Ms at 4.2K were found to be 0.72 emu/g (single crystal)6 and 2.15 emu/g (powder)l. Magneto- clectric7and magnetic torque6 measurements on NiCl yielded a magnetic Curie point of~lO~SPONTANEOUS BIREFRINGENCE
In order to make visible ferromagnetic domains in strongly birefringent NiCl and
NiBr~
Jne has to observe along or close to an optic axis.Tbis isdue to strong interfererce of birefringent phase retardation with Faraday rotation9. Orthorhombic NiCl and NiBr are op!ically positive with ns//Ps//co.r.//<001>cub• na//bo.r.//<110>cub and ny//a0 .r.//
<110>cub with the optic axes lying in the (001)0 .r. plane. With a view to locating the optic axes of NiCl and NiBr in the ferromagnetic range, we have extended the measure- ments of the principal birefringences of NiCl and NiBr from room temperature to 4.2K.
(see Figs. la and b). Using Mallard's approximation formulalO,sinVy=[(ns-na)/(ny-na)Jl/2, where Vy is half the acute optic angle and ns-ny, ny-na are princ1pal birefringences,
the opt1c angles 2Vy of ~79° rtnd ~71° are obtained for NiCl and NiBr at 4.2K, respecti- vely. This means that on (lOO)cub cut platelets with spontaneous polarization within that plane (Fig.2a) one of the two optic axes is coming out at ~5.5° and ~9.5° off the vertical for NiCl and NiBr, respectively. As shown below, these angles and the accom- panying weak birefringence ny-nB proved acceptable for observation of magnetic domains
(compare Figs 4 and 5). For NiCl .J.lso the birefringence section n~ -nB has been measured between 4.2 and 40K (Fig. 3) using a lock-in amplifier together with a photoelastic modulator11. Below lOK a contribution from the Faraday rotation is clearly observed.
FERROMAGNETIC DOMAINS AND ORIENTATION OF SPONTANEOUS MAGNETIZATION VECTOR
For observing ferromagnetic domains in the interiour of the ferroelectric ferro- elasticdomains,(100)cub-cut platelets of NiCl and NiBr were used, allowing in principle,
395
396 IAN H. BRUNSKILL and HANS SCHMID
the simultaneous observation of four different ferroelectric domains having Ps within the plane (see Table 2 of ref,4). At nearly crossed polars, close to extinction, ferro- rnagnetic domains have been observed in NiCl(Fig.4) and NiBr(Fig.5) in the interiour of such ferroelectric domains, In white light brown/bluish contrast was obtained between different states of magnetization. Minimization of magnetostatic energy leads to narrow stripe domains after cooling in the field free state. The stripes are separated by
walls following approximately (001) orth. rh. planes. The NiBr sample (Fig. 5) is particu- larly instructive because it shows ferroelectric domains with four different orienta- tions of Ps and all three types of ferroelectric/ferroelastic domain walls known for NiCl and NiBr 4, i.e. "180°11
Q),
"head-head (tail-tail)"(Y
and "head-tail"@ (Fig. 6) .-
With a view to deducing the orientation of the spontaneous magnetization vector :rv.~
in NiCl and NiBr, stability tests of the stripe patterns in an external field H (~300G~;
permanent magnet rotated around the cryostat) were performed : (i) for rotation of H within the plane ns/na, the stripes are stable for any angular position of H; (ii) for rotation of H within the plane ns/na the stripes are stable for H parallel to ns only;
(iii) for H rotating within the plane nylna the stripes are. stable for H parallel to na only. From (i) to (iii) Ms is found to lie parallel to p. (a0-a.xis of ref. 7)
in good agreement with results from magnetoelectric7and torque 6 measurements on NiCl.
From this result the schematic representation of the stripe domains follows (Fig.2b) and which - together with Fig.2a-explains the magnetic domain patterns of Figs.4 and 5.
The angles between Ms on either side of the ferroelectric walls @'®and G) (Fig. 2) are 90°, 60° and 60°, respectively. Whereas across the walls ~the magnetic domains seem to be joined both by magnetic head-head and head-tail junctions, the continuity of the stripes across the walls
(V
seems to indicate that in the latter case the magnetic stripes -while 11bending11 around 90° - are joined by head-head junctions.FARADAY ROTATION
In Figure 6 the apparent Faraday rotation versus temperature of NiCl and NiBr is shown for observation perpendicularly to (100)cubcuts containing Ps within the plane
and characterized by the birefringence ny-lla· By 'apparent' we mean that the plotted ,~
rotation is the angle formed by the plane of the initial linearly polarized wave and the major axis of the elliptically polarized wave leaving the crystal. For measurement a conventional technique using a polarizer, an analyser and a microphotometer was used in conjunction with a photoelastic modulator acting as a high frequency polarization chopper.
CONCLUSIONS
The domain studies of NiCl and NiBr lead to the deduction of Aizu spec~es
43m1'Fm'm2' for both compositions at 4.2K, with Ms lying in both cases along ny.Further work is needed for separating the intrinsic Faraday rotation from birefringent
phase retardation.
ACKNOWLEDGMENTS
Warm thanks are extended toR. Boutellier, E. Burkhardt, R. Cros and Mrs. 0. Birth for drawings, photographs, samples preparation and typing, resp. and to the Fonds
National Suisse de la Recherche Scientifique for financial support.
C") 2 4 ··· · · .. · · · .. · · ... fY·r~ -~~-.. .
NiCI
~20
Q)
g16
~ ... --~~-n,· ...
·· .. "
\
.£12
~ ... -~~~-~~~
ffi8
4
0o~-1~oo~2~o~o...~...::-3o~o~4~oo~s~oo~~soo~
Temperature [K]
20r---~
.. ... . '"!v-n.
C") 16~
... .
0 ...-;
Q)
g12 · .... · ...
ny-n11Q) . . .
0'1 ~
Ea~ c ... Q)
4
. . . . ~-n. ...
NiBr
. ...
'"-
..
··.
. ..
I I
50 100 150 200 250 300 350 400 Temperature [KJ
FIGURE Principal spontaneous birefringences versus temperature, (a) NiCl,(b) NiBr (A
=
546nm; tilting compensator)a.--G--
~-G-d.
-~~-ny'
M's-G-
FIGURE 2 Schematic domains on a (100)cubcut
r~~) ferroelectric/ferroelastic single Jmain, (b) ferromagnetic stripe domains occuring in (a)
194 r
~193
Q)~
r0'1 c
;£:192
Q)
m
L. r 191·• • ....,. ... -... ·I •..
...
··· ...
... _NiCl
··-
0 5 10 15 20 25 30 35 40 Temperature [K)
FIGURE 3 Spontaneous birefringence ny-nS of NiCl versus temperature
(photoelastic modulator).
Sample thickness1 244~m
FIGURE 4 Ferromagnetic stripe domains of NiCl, (a) narrow stripes, as-cooled without magnetic field; T
=
4.2K, (b) large stripes after repeated switching; T=
4.2K.Sample thickness, 244~m.
398
IAN H. BRUNSKILL and HANS SCHMIDFIGURE 5 Ferromagnetic stripe domains of NiBr, (a) as-cooled without field, T = 12K, (b) ferroelectric/ferroelastic domains of Fig. 5-:t; G,) , (y , @ , are 180°,
head-head and head-tail domain walls, resp. (compare Fig. 6). Sample thickness) 77~m
180'- DOMAINS
it7i'
. .
tllfu~ [
0 g
HEAD- HEAD <TAIL-TAIL) DOMAINS
. . 0 ; -
' . t i . ' i.~. ...
HEAD- TAIL DOMAINS
FIGURE 6 Three types of ferroelectric/
ferroelastic domain wall occur~ng ~n
NiCl an NiBr4 REFERENCES
]140
""'
2'120.!2.
510o
1j 0 80
0:::
"0 ~60
~ 40
LL 0
. I .
• •• NiBr
.
lNiCl
2o- ~~., ... I .
oo~~~~~~~~~~~~
10 20 30 40
Temperature [K]
FIGURE 7 Apparent Faraday rotation of NiCl and NiBrJl(ny-ns);
A=
546mn; samplethicknesses 244~m and 145~m, resp.
l. G. Quezel and H. Schmid, Solid State Comm. 6, 447 (1968) 2. H. Schmid, Int.J.Magnetism, 4, 337 (1973)
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9. W.J. Tabor and F.S. Chen, J.App1.Phys. 40, 2760 (1969)
10. C. Burri, Das Po1arisationsmikroskop (Birkhauser, Easel, 1950), p. 48 11. J.C. Kemp, J.Opt.Soc.Amer. 59, 950 (1969)