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Magneto-optical observation of a magnetically induced “ domain spin-flop ” in a cubic antiferromagnet : KNiF3
R.H. Petit, J. Ferré, J. Nouet
To cite this version:
R.H. Petit, J. Ferré, J. Nouet. Magneto-optical observation of a magnetically induced “ domain spin-flop ” in a cubic antiferromagnet : KNiF3. Journal de Physique, 1975, 36 (5), pp.431-436.
�10.1051/jphys:01975003605043100�. �jpa-00208269�
MAGNETO-OPTICAL OBSERVATION
OF A MAGNETICALLY INDUCED « DOMAIN SPIN-FLOP »
IN A CUBIC ANTIFERROMAGNET : KNiF3
R. H.
PETIT,
J.FERRÉ
Laboratoire
d’Optique Physique (*), EPCI, 10,
rueVauquelin,
75231 Paris Cedex05,
France andJ. NOUET
Faculté des
Sciences,
route deLaval,
72000 LeMans,
France(Reçu
le 6 décembre 1974,accepté
le16 janvier 1975)
Résumé. 2014 Sous faible champ magnétique H nous avons observé une variation importante de
l’allure des spectres
magnétooptiques
en fonction de H, pour un composéantiferromagnétique
cubique :KNiF3.
Cephénomène,
examiné ici pour lapremière
fois, est comparé àl’apparition
de la phase oblique, bien connue dans les composés antiferromagnétiques uniaxes. Des calculs spec-
troscopiques nous ont
permis
d’interpréter le spectre de dichroïsme circulaire magnétique observéde part et d’autre d’un champ critique Hcr au-delà duquel il ne subsiste que la phase oblique. La faible
valeur de Hcr nous a conduit à montrer que le déplacement réversible des parois de mâcle
précède
la rotation des spins dans un monodomaine.
Abstract. 2014 We have observed a large change in the field dependence of the
magneto-optical
spectra of cubicKNiF3
at a low magnetic field. This phenomenon, which is beingreported
for thefirst time, is compared to the well-known spin-flop occurring in uniaxial antiferromagnets. Spectro-
scopic
calculations allow us to attribute the magnetic circular dichroism signals that have been observed below and above the critical field, to an antiferromagnetic and aspin-flop phase.
We verifythat in a cubic antiferromagnet, the reversible movement of domain twin-walls occurs at a lower
magnetic field than the rotation of the
spins
inside a single domain.Classification
Physics Abstracts
8.818
1. Introduction. - The
spin-flop phenomenon
ofsublattices of a uniaxial two sublattice antiferroma- gnet is well known
[1].
It occurs when themagnetic
field
applied along
the easy axis exceeds a critical valueHSF
=2 HA Hr, where HA
and HE
are the
anisotropy
and theexchange
fieldsrespectively.
Then,
in a finite interval of field nearHSF,
the anti-ferromagnetic
vector 1 = ml - m2 turns from the direction of the easy axis(antiferromagnetic
AFstate)
to thatperpendicular
to it and since thespins
tilt
slightly
towards the field direction there appearsa net
magnetisation
m = ml + m2(spin-flop
SFstate) [2-4].
In a cubic
antiferromagnet
such asKNiF3,
whichremains cubic below
TN
= 246 K[5],
the situationdiffers
markedly.
We must take account of the factthat in the absence of an extemal
magnetic field,
we
generally
start from a multidomain structure.(*) Equipe de recherches n° 5 du C.N.R.S.
Three kinds of domains must exist in which 1 is
parallel
to one of the fourfold axes[5-6].
The domainstructure is
sample dependent
because it isessentially
related to local
imperfections
associated with internal strains. Twin-walls separate such domains[7]
andcan move
easily
under stress ormagnetic perturba-
tions. When
increasing
themagnetic
fieldapplied along
the fourfold axis z a transition occurs at alow field. In our attempt to
give
aninterpretation
ofthis
transition,
we demonstrate here that it is not due to amicroscopic phenomenon
which involvesHA
and
HF
but rather to a reversible movement of twin- walls at a lowmagnetic field,
this movementbeing
related to the transformation
of dZ
domains intodx
ordy
domains. This agrees withsuggestions
madeearlier
by
Néel[8].
We name this transition domainspin-flop (DSF).
A
spectroscopic study
of the intermediate statewas necessary to demonstrate the coexistence of the two AF and SF
phases
for an uniaxial antiferro-Article published online by EDP Sciences and available at http://dx.doi.org/10.1051/jphys:01975003605043100
432
magnet
[3-4].
In our case, theabsorption
isonly slightly
modified at the DSF and we have thereforeused a more sensitive
method,
i.e.magnetic
circulardichroism
(MCD).
The apparatus described earlier
[9]
is able to detectdichroism of about
10-6
in absorbance. Here the field isprovided by
asuperconducting
solenoid whichgives
anhomogeneity
better than one per cent.2. Evidence for AF and SF
phases by
MCD2. 1 ON EXCITONIC TRANSITIONS. - 2. 1. 1
Antiferroma- gnetic phase : dz
domains. -First,
we consideronly dz
domains. We suppose that when weapply
a weakmagnetic
fieldalong
z, thespins
of the a and b sublat- tices remain orientedantiferromagnetically
andparal-
lel to z.
We can write the wave
function 1 G >
of theground
state of the entire
crystal [10]
n and m refer to the unit cells in the two sublattices.
A is the
antisymmetrisation
operator. Note that thespins
arequantised along
the z axis.The exciton
corresponding
to the electronic tran-sition
’A2g --+ 1 Eg
in thesublattice J1 (a
orb),
forthe wave vector k is
if we suppose that the intersublattice interaction is
negligible.
Here 1 Eny >
stands for the excited state in which thenpth
ion is excited.a is the
component
e or 0 of1 Eg
in theOh
group.In order to calculate the
MCD,
we must consider thecomponents fl à
± 1 of themagnetic dipolar
moment
operator
m.For the excitonic
transition,
k =0,
then :By considering
the second member of the above expres-sions,
we deduce that Q+polarised light
in the a sublat- ticecorresponds
to Q-polarised light
with the sameintensity
in the b sublattice. Then the observed MCD in a lowmagnetic
field arises from the difference in energy between theup-spin
anddown-spin sublattices,
i.e. 2
9/ÀB H (g
= Landé factor of3A2g,
/lB = Bohrmagneton).
For an isolated transition whichgives
riseto an
absorption
line(bandwidth y)
and when9JIB H y,
the MCDAAc(u)
looks like the first derivative of theabsorption
curve, i.e.d/(y)/dcr [11 ].
In this case, we shall
speak
of adf(u)/du
term. Abovethe
DSF,
thedf(u)/du
term vanishes because themagnetic
energy of the two sublattices is identical.2.1.2
Spin-flop phase : dx
anddy
domains. -For
KNiF3,
insided, and dy
domains thespins
tendto
align
themselvesalong
the field direction. Then thespin configuration
is the same as in thespin-flop phase
of a uniaxialantiferromagnet.
So that the method of our calculations is valid whatever thecrystal
symmetry.We shall use the
Wigner
functions forspin
rotationin order to write the wave functions of the entire
crystal
under amagnetic
field. Wekeep
z as thequantisation axis,
and consider that under the magne- ticfield,
thespins
of the a(or b)
sublattice deviatethrough
theangle n -
0(or 0)
from the z directionin the
ground
state of thecrystal (cos
0 =H/2 HE).
Then
stands for the
ground
state of thecrystal,
with :The excited
state lEg )nll
of then,uth
ion is not modi-fied
by
aspin
rotation because itsspin equals
zero.The
exciton 1 E4, k y
is obtainedby replacing 1 3A2 +
1)na and ! 1 3A2 - 1 >mb by I 3A2 +
1>’na and 1 3 A2 -
1):nb
in theexpression (2.2).
Herewe
keep
the sameangle
0 in the exciton wave functionas in the
ground
state. We should have taken 0’depending
upon theexchange
between an excitedion and
surrounding ground
state ions while 0depends only
upon theexchange
in theground
state.Therefore,
we are
assuming
that the excitation of one ion does notmodify
thespins
of the others.Petrov
[12]
has demonstrated that thespin-flop phase
is characterisedby
the removal of thedegene-
racy between the excitonic levels
The
splitting,
which is called the Davidovsplitting
at k =
0,
isproportional
to the energy of transfer of the excitation to1 Eg
from one sublattice to theother ;
itdepends
upon theexchange
interaction and isproportional
tocos’
0[12].
As in the case of the
antiferromagnetic phase,
we have calculated the MCD for the excitonic tran- sitions
(1 EI B) and 1 EI (J »). For 1 E- B)
and1 E- (J)
the MCD is zero.For 1 E+ B, (J)
we findan MCD term
proportional
to theabsorption
curvef(a),
theamplitude
of which is :where mo is
proportional
to the reduced matrixelement of the
magnetic dipole
momentThe
exchange interaction,
thespin
orbitcoupling
and the
applied magnetic
field do not lift thedegene-
racy of
1 Eg e
and’Eg 0
levels. Then for the pure excitonic transition we obtainAAc/Am
= - cos 0where
Am
=4 mÕ/3
stands for the maximum absor- bance of the line in the absence of themagnetic
field.2.2 ON EXCITON-PHONON TRANSITIONS. - We now
consider the
exciton-phonon
transitions inducedby
one odd
parity phonon.
We make thehypothesis
that the MCD and
absorption
spectra can be inter-preted by considering
that thephonons tlu
at k = 0are the most influential
[13].
Then it ispossible
toestimate the MCD in the
antiferromagnetic [14]
and in the
spin-flop phases.
For the latter case, in the same way as for the excitontransition,
we cal- culateAAc{u)/Am = ! cos O.f(u)
for the exciton-onephonon tiu
transition.It is
interesting
to compare our results to those ofa pure
ferromagnetic phase
whereWe deduce the MCD for the
zero-phonon
transition :AAc(u)fAm
=(- 1) f(J)
and for the exciton-onepho-
non t lu at k = 0 :
AAc(u)fAm = 1 f (a).
We note thatin the spin-flop phase
or fordx and dy domains,
theMCD
isonly
due to theferromagnetic component.
2.3 GENERAL EXPRESSION FOR MCD. - In conclu-
sion,
the MCD allows us to separate the effects dueto dZ
domains from those due todx and dy
domains.In an ideal case and without
perturbation,
threekinds of domains
(dx, dy, JJ
must exist. Amagnetic
field
Hz favours dx and dy
domains.We have demonstrated
that,
ifNz
represents theproportion
ofthe dz domains,
the MCD isexpressed by :
in the
rigid
shiftapproximation.
The a and c coeffi-cients
(Table 1) depend
on theoptical
transition.TABLE 1
a and c theoretical
values for
excitonicand
exciton-phonon (t1u
atk =0) ’A2 g --+ ’Eg
transition2.4 EXPERIMENTAL RESULTS. - 2.4.1 General considerations. - The MCD
signals
may be alteredby
linearmagnetic birefringence
and linear dichroism due to theinequivalency
of the numberof dx
anddy
domains.
Such a stray
magnetic birefringence depends
upon thequality
and the thickness of thecrystal
and alsoupon the orientation of its fourfold axis z with respect
to the
light
and themagnetic
field directions. Small internal strains of severalkg/cm2
orientedalong
one ofthe x or y axes, lead to a
large
linear dichroism[5].
The most reliable
spectra
are obtained forcrystals
with
only
a fewimperfections, impurities
and internal strains.We have obtained
the
spectra for a thincrystal (e
= 0.195mm) of good quality.
Before eachexperi-
ment, we verified that no linear dichroism
appeared
at low
temperature
and in order to be sure that we observed the realMCD,
we have also verified that itssign
reverses onreversing
H.Note that we obtained better results when we
cooled the
sample
in the absence of anapplied
field.This is consistent with the fact that near
TN
thespins
orienteasily
themselvesperpendicular
to asmall
magnetic
field.2 . 4.2 Field
dependence of
the spectra. - The spec- tra for the’A2g -+ ’Eg
transition aregiven
infigure
1.Note that the DSF has been observed for all
optical
transitions but the
3 A2g -+ 1 Eg
transition has been chosen because of thesimplicity
of the excited state.We observe MCD
(Fig. 1) temperature independent
terms
(5
K T 25K) proportional
todf(u)/du
for low
magnetic
fields and tof(u)
forhigh
fields(H
= 37kOe),
on the firstabsorption peaks
whichare well isolated in the spectrum. The
high
field spectrum is consistent with the MCDshape dispersion
434
FIG. 1. - Absorption at H = 0 (bottom) and MCD spectra (top)
for the
3A2g -> ’E’ 9
transition in KNiF3 at 15 K. We have shownthe MCD spectra for H = 6.25 kOe (2013), H = 19 kOe (- - -),
H = 37 kOe (-.-). The thickness of the sample is 0.195 mm.
The bandwidth used is 3 cm -1.
for the
ferrimagnetic RbNiF3 [13]
where the ferro-magnetic component aligns along
the field.Then we have followed the variation of MCD terms when
slowly varying
themagnetic
field(25 Oe/s).
The time constant used was 2.5 s. As an
example figure
2a shows the variation of the extremum of adf(u)/du
term for the firstabsorption peak
withfield. Because of the smallness of the MCD
signal
at
high field,
we alsogive
the field variation for the extremum of thef(u)
term for alarger peak
locatedat 15 485
cm-1 (Fig. 2b).
In a
magnetic
field thespin
insidedx
ordy
domainsshould tilt and
give af(u) signal.
The absence of sucha
signal
at low field indicates analmost dZ type crystal.
Between 12 kOe and 20
kOe,
thedf(u)/du
termdecreases and it reaches zero at
Hcr
= 20 kOe(Fig. 2a)
meanwhile the
f(a)
term increases. This is consistent with the fact thatthe dz
domainsdisappear
at theexpense
of dx or dy
domains. Between 12 and 20kOe,
the MCD behaviour
(Fig. 1)
indicatesclearly
thecoexistence of all
phases.
AboveHcr
thereonly remain dx and dy
domains. Since the linear dichroism issmall,
we conclude thatthey
havepractically equal importance.
At the same time we have observed a
rapid
variationof the
absorption
for allpeaks
around 15 kOe : ifwe increase the
magnetic field,
the firstabsorption peak
located at 15 347cm -1
decreasesby
about20
%
and the others increaseby only
a few per cent, whatever thepolarisation
of thelight.
We cannotFIG. 2. - a) Experimental (-) and calculated field dependence
of the peak to peak amplitude of the df«(1)/d(1 MCD term for the magnetic dipole
’A2, 1Eag
transition (7o = 15 347 cm-’) for Her = 20 kOe, Hl = 0 (...), Hl = 11.6 kOe (-.-), Hl = 14 kOe (- - -) ; b) Field dependence of the magnitude of the f«(1) MCDterm for the first exciton-phonon (tlu) peak which is located at
15 485 cm-1. For the (a) and (b) experimental curves the error does
not exceed AA,, = 2 x 10- 5.
attribute this variation to
birefringence
and theassociated linear dichroism because these have been verified to remain small
(f1AL/Am 10-3).
Theabsorption
transitionprobabilities
may thus be alteredby
thechange
in the site group symmetry fromC4h
toC2h,
related to thechange
in themagnetisation
direc-tion.
2.5 DIsCUSSION. - 2 . 5 .1 At low
magnetic field (H
12kOe).
- The weakdipole strength
of thefirst
absorption peak
located at 15 347cm -1
and thesign
of its MCDdf(u)/du
term under amagnetic
field confirm its
magnetic dipolar origin.
From the avalue we can
estimate g
= 2.3 ±0.1,
which is close to g = 2.28predicted theoretically (Table I).
The
energies
of the other nearabsorption peaks,
the
sign
andamplitude
of thecorresponding a
values
[14], a
= 1.1 ±0.2,
allow us to attribute themto
tlu phonon
lines at k = 0(Table I).
These results confirm that at low field almost all the
spins
are orientedalong
z.2. 5.2 Above the critical
field (20 kOe).
- Weverify (Fig. 2)
that the MCD varieslinearly
with Habove the
transition,
which confirms the fact thatf1AclAm
varies as cos 0 =H/2 HE.
This fact supportsour
hypothesis
6 = 0’. If we had(J’ =1=
0 the MCD would bemultiplied by
new termsdepending
onH,
such as the
overlap
of the wavefunctions of the ions which are not excited. Forexample
Moreover,
we find the propersign
for the exciton line(negative dichroism)
and for the two first exciton-phonon (t1J
lines(positive MCD).
Theexperimental
values of the
corresponding f(u)
terms are very small since9PB H (1-5 cm -1 )
9PBHE
whichimplies
cos 0to be very small. These values agree with those pre- dicted
theoretically by taking
Thus we
verify
that the appearence of MCD in thespin-flop phase
isonly
related to the netferromagnetic
component m.
3. Evidence of a twin-wall movement. - We remark that the
phenomenon
seems to be reversible whenincreasing
ordecreasing
themagnetic
field(0-45 kOe).
At low
temperature (6 K)
thesharpness
of the transi- tion is greater than athigher temperatures (210 K).
We
give
some evidence which arguesagainst
thehypothesis
of aspin-flop
transition similar to thephase
transition in uniaxialantiferromagnets :
-
Hcr depends
on thecrystal shape
and on itsthickness and varies from 8 to 22 kOe for our
samples (0.2
to 14mm).
- We find the same
Hcr
value for alltemperatures
between 6 K and 210 K.- Our
Hcr
value does notcorrespond
to theexperimental
one-magnon(k
=0)
Ramanfrequency :
4.5
cm-1 [15].
- No new transition appears at the theoretical
spin-flop
field at 4.5cm-1 [15].
We have continuedexperiments
up to 45.6 kOe(4.84 cm-1 ).
- As the MCD
presents
novarying
noise at thetransition,
we deduce[16]
that there is nospin
fluc-tuation at the DSF.
Thus we are
going
to show that the reversible movement of twin-wallsprecedes
thespin flopping
of the
spins
inside thedomains,
whenincreasing
the
magnetic
field in cubicantiferromagnets,
ashas been
suggested by
Néel[8].
So we want to
explain theoretically
the DSF.For a domain
(with
direction cosines of thespins
a,fl,
y, withrespect
to thecrystallographic axes),
thefree energy per unit volume due to the interaction with an
applied magnetic
field H(direction
cosines ,u, v,p)
can be defined as[6] :
where X_L
andx
1, stand for theperpendicular
andparallel susceptibilities
of thecrystal.
Here J1 = v = 0, p = 1.
We consider adisplace-
ment x of the wall between
a dZ
domainand dx or dy
domains,
whichcorresponds
to a rotation of thespins
from the(a
=fl
=0,
y =1)
to the(a’, fi’, y’
= cos({J)
direction. The variation of free energy per area unit due to the volume variation may be writtenas : - 2 x(xl - x I I )
H2sin2
({J.The variation AF of the total energy, in which we
must include the effect of the
restoring
forcekx2/2,
has been minimized with
respect
to x and ({J. We deducedThese results indicate that the walls move
gradually
with H and
disappear
when x reaches the value C of the width nf the d domains- at a fieldThis agrees with the
gradual
fielddependence
of theMCD terms
(Fig. 2)
between 12 and 20 kOe. Thisbehaviour is very different from the brutal SF tran- sition in a uniaxial
antiferromagnet.
Thesample dependence
of theBer
values is related to thedisper-
sion of k and C due to the
poor-definition
of thedomains in cubic
antiferromagnets.
We have looked more
carefully
at the fielddepen-
dence of the MCD terms
(Fig. 2).
In the formula(2. 5), Nz
isproportional
to the width(L - x)
ofthe dz
domains. Then we have
compared
the fielddepen-
dence of the
df(u)/du
term to theexpression
1
(Fig. 2a)
and that of theI(u)
term toH(H 2/H i)
(Fig. 2b).
Infigure
2b we observe that there is novariation of the MCD term below 12
kOe,
whichdisagrees
with theH(H2IH;r)
law.Thus,
we haveintroduced
phenomenologically
a new term in theexpression
of AF :xB sin2 qJ
and we have deducedand
For H
Hl, x
is zero and there is nochange
in thedomains structure. For
A
comparison
between theexperimental
andcalculated values of the
d/((r)/dy
term(Fig. 2a)
hasled us to estimate a threshold field
Hl
=(12
±2) k0e.
The threshold field value
depends
upon thesample
and varies from 0 to 15 kOe for our
crystals.
We haveverified that the
application
of a stressalong
z,which
favours dz
domains[5],
increases theHl
value.
Thus,
we have concluded thatB,
which is smallcompared
to theanisotropy
energy ofKNiF3,
may be the difference ofanisotropy
between the z and the x or y directions.436
4. Conclusion. - We have shown that MCD expe- riments allow us to follow
accurately
thespin-flop
transition. The MCD is related in a
simple
way to the tiltangle
0 between themagnetic
moments fortwo
opposite
sublattices inKNiF3
under amagnetic
field. In some
antiferromagnets
wemay.have
the sameconfiguration
of a weakferromagnetism,
due to aDzialoshinski
exchange.
Circular dichroism could be used in order to determineprecisely
theangle
0in these materials.
For the cubic
antiferromagnet KNiF3
we haveshown the occurrence of a
spin-flop
transition.Its
description
differsmarkedly
from that of the sametransition in uniaxial
antiferromagnets
because it isdue to the reversible
displacement
of twin-walls.This work also illustrates some difficulties which
can be encountered in
magnetooptical
measurementson cubic
antiferromagnets.
Suchexperiments
mustobviously
be undertaken with great care.We wish to thank Dr. F. Moch for fruitful dis- cussions and we
acknowledge
the assistance of Mrs. Vemazza(Département
de RecherchesPhy- siques,
Université ParisVI)
who oriented andpolished
the
samples.
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