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Journal of Magnetism and Magnetic Materials 2 (1976) 309-318

O North-Holland PublishingCompany

MAGNETOSTATIC M O D E S IN ANTIFERROMAGNETIC RESONANCE *

R.W. SANDERS, J. BARAK ** and V. JACCARINO


Department of Physics, University of California, Santa Barbara, Santa Barbara, California 93106, USA

Received 24 May 1976

Measurements of the antiferromagnetic resonance (AFMR) spectra of MnF2 spheres are reported, and the principal mag-
netostatic modes (MSMs) in these spectra are identified. To interpret the observed spectra it is necessary to take into ac-
count, in addition to the theoretical MSM solution, tl-,e effects of impurities, finite sample size (propagation effects), and
radiation damping. Expressions for the predicted relative intensities of the modes are developed for particular choices of
symmetry of the exc',ing ri field and compared to observations. The observed shifts and intensities are larger than predicted.
This discrepancy ,.'-:explained by analysis of the role of the magnetic susceptibility of a sample near resonance. New observa-
tions are repor~:d which improve the understanding of radiatien damping in AFMR.

1. Introduction In part this may be attributed to the difficulty of


AFMR experiments compared to FMR experiments;
There exist, quite often, numerous lines m the fer- usually low temperatures and high magnetic fields
romagnetic resonance (FMR) spectrum in addition to and/or frequencies are required. Moreover, under the
the uniform mode. These have been shown by Walker usual experimental conditions for AFMR, the MSM
[1 ] to correspond to the solutions of the combined spectrum is altered because of effects of surface im-
magnetization equations of motion and the magneto- perfections, impurities, finite sample size, and radia-
static Maxwell equations with appropriate boundary tion damping. Only comparatively recently has the
conditions for fields at the surface of the (spheroidal) linewidth broadening due to these effects in MnF 2
sample. These magnetostatic modes (MSMs) include been reduced sufficiently to permit resolution of in-
the uniform precession, described by the Kittel equa- dividual MSMs [9]. Any attempt to ,:ompare experi-
tion. The MSM spectrum for the explicit case of fern- mental AFMR spectra with the theory of MSMs must
magnetic resonance in ferrite spheres was recalculated take all these effects into account, Experimentally this
by Fletcher and Bell [2] and by Plumier [3]. The geo- requires the use of very well shaped and polished pure
metric picture and the calculated frequencies of the samples, carefully oriented with respect to the external
modes are well substantiated by experiment [4,5 ]. dc magnetic field and situated in the oscillatory field
However, the theories of MSMs in antiferromagnetic at a point of high symmetry, so that only a small num-
resonance (AFMR), proposed by Beeman [6] and by t, er of narrow MSMs is excited. Under these conditions
Yakovlev and Burdin [7], remain unverified in the lab- it is possible to identify the modes unambigt, ously and
oratory. Although observations of antiferromagnetic to study their frequency shifts, intensities, and line-
MSMs are reported in the l~.erature [8,9], there is no widths.
't . . . . • .3 _ ~ .,,. ; . t ' ~ . - _ ,i.." ~ ~ ~ ~--a2 ~..1 . . . . ..3 . . . . . ".J.'t.. ~ _,t,.." ~ . . I ~ -
c l e a r IL/tI~IILIIIU~II.IUII L/I ~3dl tll,,,Lltldl . I I I U L t I ~ W l l . l I ~.ldt Ll~.Utlgtl

theoretical predictions. cutated in section 2. The shifts due to finite size ("prop-
agation effect") are calculated in section :~ Section 4
* Research supported in part by the National Science Foun- describes the experimental procedure used to observe
dation. and identify the MSMs in spheres of MnF 2. The ~results
** Present address: Solid State Physics Department, Israel
AtomicEnergy Commission, Soreq Nuclear Research Cen- are discussed in section 5, and detailed calculations of
ter, Yavne 70600, Israel. the mode intensities appear in the appendix.

309
310 R. |¢. Sanders et al. / Mag~wtostatic modes in antiferromagnetic resonance

2. Magnetostai,c modes in antiferromagnetic spheres equations, where the order is chosen so that increasing
r corresponds to increasing H 0 for resonance at con-
Loudon and Pincus [10] have shown that in a un- stant ~ . The characteristic equations for n :.-gm + 5
iaxial antiferromagnet with applied magnetic field H 0 are tabulated in ref. [3].
parallel to the easy axis, magnons of small wavevector It is convenient to define a parameter X0, = - 2 ]
k are confined to a band of width, in field units, (K + v). The characteristic equations permit valses of
A = 2 r ' 3 f s H A [ H c , with M s the sublattice magnetiza- X 0 only in the range 0 < X 0 < 1 [1,7]. Taking into
tion, H A the anisotropy field, H E the exchange field, account the Lorentz local field [ 11 ], eq. (2) becomes,
and H c = (H2A + 2 H A H E ) l l 2 the spin-flop field, a is to excellent approximation,
constant provided H 0 saisfies Ho(H C - HO)
~- 4rrMsH A . HO = HC _ ~ + 2rtMsHA 411"M S J t A
We fbllow the calculations of Beeman [6] and of nc x0 Hc -'
Yakovlev and Burdin [7] in describing the MSM spec-
trum. As k approaches zero and 1/k becomes com- _ 60. t.
= nc (Xo - (4)
parable to the sample dimensions, the continuum spin
wave approach is no longer appropriate, because the Eq. (4) is written specifically for lower branch AFMR.
magnetic excitations occur at discrete energies. Never- in this form X 0 is readily interpreted as the fractional
theless, the excitations are confined to the same band- part of the bandwidth by which the mode appears
width A [6]. Each MSM is ~pecified by a set of three above the bottom of the band. Since for the uniform
integers (n, m~ r), which indicates the symmetry of mode (110), X 0 = ], H C is the limiting value of H 0 for
the ff magnetization m of the mode. These integers are this mode as ~o -+ 0. For MnF2, the experimental val-
restricted to values such that n i> 1, --n ~< m ~< n, and ue o f H C is 92.94 kOe [12]. TakingM S = 576 Oe and
0 <-<r <<.~(n - Irnl). m is positive for AFMR on the the experimental value of the susceptibility [13}, one
~ower branch and negative on the upper branch [7]. finds HI.: = 536 kOe, H A = 8.00 kOe, and a = 312 Oe.
Y~;e rf magnetization obeys the equations The corresponding values ofX 0 for the MSMs relevant

4 ~ t ' x = s:hx. - ivh v . 4rrm v=ivh~: + Kjl v , m z =0.


Fable 1
(1)
ii~e pa.~ameters ~ and v are related to H 0 and the rf Mode X0 Ho -- H~l ~o) Ot?l

frequency w/2,'r by (Oe)

(110) 0.667 0 1
~H2 8rrMsHA~I/2 +to (2) (21 O) 0.400 -83 1.5
/:°= : -v' (310) 0.258 -127 *
(311) 0.868 63 *
(330) 0.856 59 2.8
SrrmS//A (410) 0.179 -152 **
- "=n: c - e 0 l 2' (3) (41 | ) 0.700 11 **
(430) 0.667 0 **
where -: is the gyromagnetic ratio,, and the plus and
* no theoretical predicti,.,n
mint> sb,,'ts correspond to the upper and iower AFMR ** hllodc ~ t- r"o" t "I L
. t t^C_U
. : tcl:!_ Ilt~t.l
_1

branci:e~, respectively. The magnetostatic Maxweli


Note: T l e resonance positions of several low older antiferro-
equatior~-- V- b = 0 andV × h = 0 a~ld the condition
magnetic MSMs are tabulated fo~ the case of spherical sampks
~at, at ~,~esurface of the spherical sample, h and the satisfying R ,~ h (i.e. in the absence of propagation effects).
con:p:.,nent of b normal to the surface are continuou; X o is the fractional position of a mode above die bottom of
tend to ~,. characteristic equation for each (nm).. This the band The third column indicates the predicted separation
equatio,: is the {hird necessary relation between ~, v, between tile resonance field ot each mode and the (I 10) mode,
taking 312 Oe as the bandwidth in MnF 2. The last column
a qd H 0 *~,r a given w. The index r assumes the values,
contains the values of txn obtained by comparing the dashed
O. ;. 2 . !or r.he different sok~tions of the same (nm~ lines in fig. 2 with the p~'e~lictions o!' eqs. (5).
R. W. Sanders et al. / Magnetostatic modes in antiferromagnetic resonance 311

to the current experiments in the K-band ("-23 GHz) o f M 0 by M s H A / H c ; t h e shifts for tile AFMR modes
are given, together with the predicted separation of become
each mode from the uniform mode (110), in table 1.
~ (~_) = 4rrMsHA 2 n+l
(2n + 1)2
3. Propagation effect

The magnetostatic approximation is valid only as x (5a)


long as the sample is much smaller than the wavelength
of the exciting radiation - i.e. R ~ / c ,~ I, where c is and
the speed of light in vacuo and R is the sample radius. 8 [ ~ _ 41rMsHA 1
When this condition is not fulfilled, the general Max- Hc ( - g ~ ) 2 (2n + 1)2
well equations must be used to determine the correc-
tions due to the propagating characteristics of the
modes. Several authors [3,4,141 have discussed this [e(n "+2) n + 1 ) for(n,n- 1,0) (Sb)
X~,~+3 +2n--] '
problem in connection with FMR, obtaining two prin-
cipal results: (1) the effect of propagation is to shift e, the dielectric constant of the sample, is 6.7 for MnF 2,
the MSMs to lower energies, and (2) the shifts are The experiments reported below detect AFMR on
proportional to Mo(Rto/c)2, where M 0 is the ferromag- the lower branch. In this case, decreasingthe mode en-
netic saturation magnetization. The propagation shifts ergy corresponds to lowering the field required for
were determined experimentally for YIG spheres [4] resonance at fixed frequency. From eqs. (5), the lar-
by exploiting the change ofM 0 with temperature. gest shift is expected for the (110) mode, and the sizes
When the resonance fields are plotted versus 41rMo, of the shifts are expected to decrease with increasing n.
the data fall on straight lines which, extrapolated to
M 0 - 0, intersect the unshifted magnetostatic predic-
tions. These results have been compared to the theor- 4. Experimental procedure
etical values predicted for the simplest modes by
Plumier [31. Although the predicted shifts are of the The experimental arrangement used is virtually
correct order of magnitude, they are consistently identical to that described in ref. [ 1 6 ] - a K-band re-
smaller than the ob:,erved shifts. flection spectrometer in which the sample arm of the
Montarroyos and Rezende [15] have recently magic-tee bridge is terminated by a shorted waveguide
studied the frequency dependence of the propagation section. Microwave propagation in the sample arm is
shift and of the radiation damping contribution to parallel to tbe field in a surrounding superconducting
MSM linewidths in YIG. Although the functional de- solenoid. Th: experiments were carr'.ed out at 4.2 K in
pendence of linewidth on frequency shows excellent fields H 0 ~- 85 kOe and ~/2rr ~- 23 GHz (K-band).
agreement with theory, the magnitudes of the line- Care was taken to avoid the broadening and shifts of
widths and intensities are observed to be much larger the resonances that occur from heating the sample at
tha ~ predicted. Convincing quantitative agreement is high levels of microwave power absorption.
obtained by adopting an effective radius Reff = % R , The samples were spherically shaped single crystals
where the constant % is the same for all modes of a of MnF 2 with radii near 1 mm. After polishing, the
given n. This discrepancy between theory and experi- largest remaining surface llllpel .... : . . . .were
....... "lCl.;tlOilb .
,,,, ....
,v,,,
ment is believed to result from the distortion of the order of 2 - 3 tam, but between these imperfections the
driving field by the reactive effect created by the ex- surfaces were characterized by scratches less than 1 tam
citation of a mode. This idea is treated more extensively in size. Each sample was mounted in polystyrene foam
in the appendix. and centered in the waveguide so that the sample'; cen-
Plumier [3] derived explicit expressions for the fam- ter was located a distance l from the terminating short.
ilies of FMR modes (n, n, 0) and (n, n - 1,0). 3ne may Provision was made for tilting the sample while ob-
adapt his result to the AFMR case by the replacement serving the AFMR, so that the c axis could be care-
?i 2 R.W. Sanders ct al. /Magnctostatic modes in antiferromagnetic resonance

C~ilv aligned with tt o. Field modulation and phase-sen- (311). Table 2 shows that these modes have the largest
sitive delection were used, and H 0 was measured using expected intensities relative to (110), and the observed
l h e 27 Al NMR in a probe placed r~ear the sample. modes are even more intense than predicted. However,
Certain resonance phenomena exhibiit a dependence the positions of these modes with respect to (110)
on ~he ~mple |ocation with respect to the standing agree neither with the predicted positions of the sug-
wave st ructure o4" the microwave fields in the wave- gested modes (table 1) nor with the calculated posi-
guide. The behavior of the width and intensity of the tions of any set of MSMs having n <~ 6. The propaga-
unifoml mode in disk.shaped samples of MnF 2 was ex- tion effect produces shifts of the co; rect sign to ac-
plored in detail in ref. [16]. This behavior, plus a count for these observations, but sin ce eqs. (5) are
knowledge of which MSMs can be excited in an rf limited to modes with n ~< m + 1, they cannot be used
field of a particular symmetry [4], helps to identify for a quantitative interpretation of the observed spec-
the modes observed. Two useful series of high sym- tra.
metD' locations occur in the shorted waveguide. First Faced with a similar situation Fletcher et al. [4]
are the points at i =/max =--:qM2, at which the oscil- were able to measure the slopes of the propagation
lating magnetic field has maximum amplitude. (q is an shifts in YIG by changing M 0 through its temperature
integer, and X is the wavelength of radiation in the dependence. Unfortunately, this approach is not easily
~,aveguide.) Second are the points at l =/node = applied to MnF 2. However, one might expect that,
(2q + i ) X/4, which are nodes in the standing wave since the propagation shifts of the mode positions are
structure. In the appendix we ~ve detailed calcula- proportional to (Rca/c) 2, the coefqcients of propor-
tions of the modes and mode intensities expected tionality of the shifts could be determined experimen.
when the sample is placed a t / m a x o r / n o d e " tally for each mode from measurements in a series of
Our first attempt to excite MSMs in an MnF 2 spheres of various radii. Identification of the modes
sphere near Ima_,~ produced four prominent mcdes, could be made by extrapolating the data to the un-
simi!ar to those in fig. l(b). As I was varied, the largest shifted positions at ~ R = O. This procedure was at-
of these modes exhibited changes iin linewidth and in- tempted on MnF 2 with disappointing results, there
tensity ch,~r_~cteristic of the (110) mode, which was being almost no correlation between mode shift and
s~:di,.~d lr~ Jetai] in vef. [16]. The symmetry of the rf sample size. We realized that traces of impurities pre-
!qeld along tb.e waveguide suggests that the other re- sent in the samples cause large variations in the mo:~e
sonances observed are the modes (210), (3 ~0), and position. That is to say, the field at which resonance

Tab],' 2

Mode Site ( 2/D) hnm almt II


a~lmr fin mr/4D2 V
(110) /max 1 1 . _

1
(210) /node kz."3 3p 0.]
(310) 'max -{2k~ k])/72 4.52 p2 2.22(~p 2 - R 2) 2 X 10 -s
(3~ 1) /max -(2k~ - k~::)/72 17.65 o 2 - 17.5 (~p2 ._ R 2) 2 × ln-S
,330> l.r,a x - ( 2 k 2-. + 5k:~)/2160 15 p2 lO-S
;al~ /node - k . I ..~k z2 3k~.)/600
. . 5.6 fi 3 10.9o(5~, 2 R 2) 2.'7 x 10 -v
!,t I I~ [node -kz( 2k2 - 3k2x)/600 23 o3 - 33 Pt~-P
"'7 ~ - R ~-) 6.2 x 10 - 7
,a3q~ ?node k..l,k
"~ z2 + "7k~)/25200.. 21 o3 3.1 x 10 -7

N o w t or each m o d e the "site" column indicates the point of high symmetry in the rf standing wave "'ructuve at which tile mode
is mos~ ir~tense. Also listed for each mode are various coefficients of expansion (defined in the appendix) whi-h lead to the calcu-
i:~;cJ T;a2\i;~um inzensit.~. P~r,,nr V is the sample volume. The values appearing this table do not include the effects of magnetic sus-
.,:",:~i~i.ii~, di,c~,,,~d in the appendix.
R. I41. Sanders et ai. / Magnetostatic modes in anti[erromagnetic resonance 3!3

occurs varies from sample to sample by amounts large


enough to totally obscure the propagation shifts. In I \ (Cl) '~:{MAX

FMR, exchange coupled impurities do not shift the ~ // \


resonances, but, in the case of MnF2, as little as 0.01%
\ \
of Fe 2÷, for example~ causes shifts on the order of
\ J \
100 Oe [9]. Even samples prepared from the same
single crystal exhibit variations of this size, probably
because there is a slight impurity concentration gra- I I , /
I I I n
dient within any boule. 1' ,, I / II \
Because of impurity effects, the values o f H 0 at /'J 'J II ', .
which a mode occurs in different samples cannot
meaningfully be compared. This is also the case when
M
a single sample is examined at several different fre- n- -
quencies; the Zeeman shift is so much larger than the
"- L/ il
propagation shifts that the uncertainty in its calculated _0 [=1.30 ),
value is large enough to conceal the p, pagation shifts.
However, both impurity effects and the Ze,,rnan shifts
displace all the modes of a single spectrum by the
same amount, while the propagation effect shifts dif- ~.
ILl ~ ,

ferent modes by different amounts. It is possible, then,


to study the propagation shifts by abandoning the ab- Q- ,~ /I \ ~l (cl) l= {NOOE
solute measurement of H 0 and mezsuring only the dif- 1 4
f e r e n c e s in H 0 between the modes of each spectrum. .,/j ~ "~ ",-25 OEtRSTEDS
-.%
These spacings between the modes may be compared
from one experimental situation to the next. We ,i.-.---
adopted a ~cheme in which the spacings between the t t 1'
MSMs of a ~,ingle sphere were determined for several 310 210 IIO 311
frequencies. Later similar data from spheres of dif- EXTERNAL FIELD, Ho--)
ferent radii were included in our study. Fig. 1. Th~s series of drawings made from oscilloscope [,hoto-
Our first observation in this new scheme provided graphs illustrates tl~c behavior of the four most prominent
an unexpected clue which conclusively labels the MSMs (labeled at the b o t t o m of the figure) in a single sphere
mode (2 ~0). This mode has m x o: z e i w t , m y = i m x , of Mni"2 as the position of the .sample in the waveguide i.,;
changed with respect to the rf standing wave structure. Tiae
where z is measured along H 0 from the center of the dotted line in each picture is the same spectrum as the corre-
sample. As the frequency is varied, the maxima and sponding solid line, but it was recorded at higher ~,ain. 1"he
nodes of the standing wave structure move wi~h re- vertical scales are only roughly equal t h r o u g h o u t the series.
spect to the sample. Therefore, tl~e condition for the
sample to be precisely at/max ot/node may be achieved ln6de, it is actually broader than the (110) mode, even
by turfing the frequency. When the sample is at lm~Lx though it is nearer to the bottom of the band.
the rf !iel,J in the sample is h x ~ cos(2rrz/;~) e i~°t, In two respects this behavior is an impor:ant ad-
h v = ih x - i . e . almost uniform amplitude within the dendum to previous studies of radiation damping in
sample if R ~ X. As expected, the uniform mode (110) disks [16]. First, in rel. [16] tile measured value for
is very intense and broadened by radiation damping, the maximum radiation damping contributiun to the
while the (210) mode nearly disappears. Conversely, uniform mode linewidth was found to be about two-
a sample at/node experiences fields h x o~ s i n ( 2 n z / ; k ) thirds of the predicted value. It was conjectu~'ed there
eit°t ~_ (constant) ze it°t, h y = ih x . A s shown in fig. 1, that a sample is somewha~ in~hibited in its alfility to
the (110~ mode dramatically disappears and the (210) radiate when it is ~aon-ellipsoidal in shape. Our current
mode becomes very intense. Furthermore, the (210) experiment supports this idea; good agreement with
mode is broadened by radiation damping; close to the predicted radiation damping linewidth (,f the uw.-
314 R. I~: Sanders ct al. / Magnetostatic modes in ant([erromagnetic resonance

form mode is obtained in spherical samples. Second- points in fig. 2 are data from a single sphere with
ly. this is the first clear observation of radiation damp- R = 0.71 mm. Squares represent modes observed in
mg in a non-umfcrm mo~!e. This was not seen in the spheres of different radius, but similar experimental
experinaents on disk-shaped samples, probably because conditions, while X's represent observations of King
~l~e disks were much thirmer in the direction of micro- and Rezende [12] by a different lechnique at much
wave propagation than spheres of the same volume; lower frequencies. These lower fr~:quency spectra were
since the rf magnetization of the (210) mode is prop- measured in a sample of R = 1.2 mm at fixed field and
ortion~ to z, a sample tl'~icker along z can radiate more swept frequency, so these pairs of points do not fall
intensely than a thinner ,ample. on horizontal lines. The points at the lowest values of
Fig. 1 illustrates the behavior of the prominent (RoJ/c) 2 correspond to H 0 close ~.o He; the approxima-
MSMs as the sample site symmetry is changed. In ac- tions leading to eq. (4) no longer hold, and a change in
cordance with the prediction of table 2, the modes the spacing of the MSMs is expected.
(310) and (311) diminish in intensity as I is adjusted The predicted positions of several of the unshifted
from/max to inode. No change in their linewidths was modes are indieat,~d along the abscissa in fig. 3. Excel-
observed. lent agreement with the unshifted positions and with
The observed mode positions are plotted versus a propagation shift proportional to (Rw/c) 2 is ob-
(Roo/c) 2 in fig. 2. Because only the spacing of the tained for the (210), (310) and (311) modes. One of
modes is determined for each set of modes observed the additional modes observed is probably (330). An-
at a particular value of (Roo/c)2; the uniform mode of other weak mode appears at high field in most of the
eaci~ set is arbitrarily placed on the line which repre- spectra, but its slope is not well enough determined to
sents the propagation shift of the (110)mode as pre- permit identification. In a few of the spectra, addition-
dicted by eq. (Sa). The points which comprise a single al weak modes are observed, usually al higher or lower
such set are connected by a horizontal line. Triangular fields than the modes in fig. 3. These a re probably

0.20[
\\ _

O.t51 \

".~----~
\

_~, ,,

3 0.~0
1 21
a
\ 63------ ~--~-~, ~_~

0.05

____
ooo!o v
-200 -Ioo o IOO
RELATIVE MAGNETIC FIELD ((;ERSTEDS)
~ig. 2 Plotted here are the obse~ed MSM positions in various spheres of Mli][;'2 vs. (Roo/c) 2. Zero field was chosen to be the un-
shifted position of the (t 10) mode; the solid line is the propagation shift of the (110) mode as predicted by eq. (5a). |t cannot be
c~ er-el~;phasized that this figure was constrac~ed from measurements of the spacing between t h : modes, and that lhe (110) mode in
each spectrum was arbitrarily placed or, the solid line. The dashed curves represent the best choice of straight lines passing through
d~e experimental data and intersecting the preclicted unshifted positions of the modes at (Rto/c) 2 = 0. The unshifted positions of
~e~~:ral b~SMs ar~ plo~*ed elong the abscissa. T t~e use of the various symbols (squares, X's, etc.) is explained in the lext.
R. It;. Sanders et al. / Magnetostatic modes in antiferromagnetic resonance 315

modes (n 1 r) with n > 3, but they are not observed effect can be quantitatively modeled by replacing R i:1
often enough to determine their slopes. They are eqs. (5) by Reff = a n R , where c~n ~> 1. The effect on
omitted from the illustration to make the useful data mode positions is seen to depend on a 2, but the ir~-
easier to see. tensities are shown in the appendix to be propottiom.l
In calculating the propagation shift of the (110) to (R0t) 2(n- 1). This explains why modes with high n
mode, it is assumed that no correction of eq. (5) is are observable. Even small values of a 3 (such as
necessary - i.e. that in a model replacing R in eq. (5) a 3 = 2.8 determined from the shift of the (330) mode)
by Reff = OtnR , o~1 = 1. This assumption is suggested result in an enfiancement of the intensities of the
by YIG experiments [4], in which no correction is modes (310) and (311) t rom the original prediction
necessary for the (l 10) mode, a~,d it is lent further of 2 X 10- 5 of the uniform mode intensity to about
credence by measurements of radiation damped line- 10-3, a value much closer to the observed intensity
widths in YIG [15], wherein parameters o~n were in- ratio of I 0 - 2 . Likewise, one expects more than a two-
voked to account for the observed linewidths, but a 1 fold increase in the intensity of (210), based on the
was determined to be unity. experimental value a 2 = 1.5.
The value of t~1 being fixed, the other t~ for MnF 2 One final remark can be made concerning the MSM
may be determined from the experimental slopes of mtensities. It is known [9] that the lower a MSM ap-
the modes (210) and (330). These values, which appear pears in the band, the narrower is its linewidth. This
in table 1, are surprisingly close to a2 = 1.5 and a 3 = is because the density of final states in two-magnon
3.5 found in the YIG linewidth measurements [15]. relaxation processes decreases as the mode energy is
ot3 cannot be determined from the modes (310)and lowered. In turn, the resonance susceptibilities and cor-
(311) because theoretical predictions do not exist for :esponding a n values take on larger values, thereby en-
these modes. However, a3 determined from the (330) hancing the peak intensib of MSMs near the bottom
mode is helpful in understanding the observed MSM of the band and making t em easier to observe than
intensities of all the modes with n = 3. MSMs with the same sym~aetry higher in the band. Of
the modes too weakly excited to identify clearly,
nearly all occurred near the bottom of the band (to
5. Intensities the extreme left of fig. 3), whille only a few were ob-
served high in the band.
As predicted in the appendix, the observed maxin turn
integrated intensities of the MSMs decrease with i-,-
creasing n. However, the observed intensities are much 6. Conclusions
larger than the predictions in table 2. The intensity of
the (210) mode is about one-fourth that of (110), and The most prominent antiferromagnetic magneto-
me ~ntensities of the modes (310) and (311) are smal- static modes in a sphere are identified with theoretical
ler by a factor of about 100. This may be understood predictions. In addition, the principai effects which
when it is realized that the theories used are descrip- alter the spectrum are defined Among these, the
tions of the modes in the magnetostatic limit as they propagation shift is shown to be proportional to
are subjected to propagative effects in an unperturbed ( R w / c ) 2, and the coefficients of proportionaiity are
rf field, in actuality, one expects appreciable distortion obtained, in general it is found that the observed sh/tts
of the rf field due to the high rf susceptibility of the are larger than predicted by the theory for ferrimag-
sample at ,,..:,,.,....... (¢,~,~.,..oq.. tA-~,..._..,. .Thi.
. . g. . . distortion
... is r~etic propagation shifts adapted to the antiferromag-
understood from early studies of resonance in ferrites net, and that the ratio of observed shift to predicted
[!71 .'Lb.e high susceptibility changes the wavelength shift increases for modes of increasing order. The ob-
of the rf field inside the sample to an effective wave- served intensities of tile MSMs ether lhan the (110)
length which is much shorter than the unperturbed mode are much larger lhan expected. A qualitative
wavelength. Consequently, the wavevectors k x and/~z analysis of the role of the magnetic susceptibility of a
evaluated in table 2 take on correspondingl./larger val- sample near resonance explains these discrepancies.
ues, resulting in higher intensities for the MSMs. This The contribution to the uniform mode AFMR line-
316 R.W. Sanderset aL / Magnetostatic modes in antiferromagneticresonance

vddth due to radiation damping is found to agree well h z = hnmpn- l(n + m) Y~nn_1 " (A2)
with 'he theory, and radiation damping of a non-uni-
form magnetostatic mode in an antiferromagnet is re- The rf magnetization m of the mode is proportional
p.~ted fo~ fl~e first time. to (2n + l)hnm/E, where E is the characteristic equa-
It is believed that this improved understanding of tion of the mode. The explicit expressions for m when
the AFMR spectrum will be useful not only in studies n <~ m + 3 are tabulated by Plumier. In general, f o r
of AFMR linewidths, but also in the study of any lower branch ~FMR with ir -- vl "< Ix + ~'1,m is given
phenomenon whicla couples magnetic excitations of by
antiferromagnet to external electromagnetic fields.
1 hmn
mx - 21r X - X 0
Acknowledgements

It is a pleasure to thank Drs. A.R. King and X I


[anmr(P) in ~ + ...] ,
Ynm - - I + a~mr(O),m-
$31. Rezende, not only for the use of their unpublis-
hed data, but also for their many helpful discussions my = im x , m z '-- 0 , (A3)
and suggestions throughout the course of this work.
We are also grateful to Dr. J.P. Kotthaus, whose early where X - X 0 is, in units of the bandwidth A, the de-
work on this problem stimulated and directed our parture from the field at which the resonance peak oc-
o ~ interest and involvement. curs. For the experimental conditions described in
section 4, ~ - v = 0.04 and X 0 = ½(r + v). The calcu-
Appendix lated values of altar (p) for the lowest order modes are
given in table 2. Relaxation of m can be phenomenol.
ogicady included by adding to X 0 an imaginary part,
Following the analysis of Plumier [3], the rf scalar
ma~etic potential inside the sample is expanded in X 0 ~ X 0 + i/i; it follows that lm(mx) is a Lorentzian
with full width at hrlf-maximum 2~5.
(unnormalized) spherical harmonics. In the frame of
The response to the rf field given by eqs. (A3) ex-
reference rotating with angular velocity co, the poten-
tial is hibits a complicated susceptibility which changes the
shape of the rf field both inside and near the sample.
However, as a function o f H 0 (ol X), it has the usual
6tp} 3 " x~ resonance form. The mode absorbs ene,gy from the
n=l rft = - n
driving field at a rate

p - _. f re(p). dh(p) d p , (A4)


=n~= ~ hn,n p , , y m (o,¢) (A1)
I r ~ = - - t~ rt '
Vsample

' =pm(cos
,,'here ~'~(0, 6) n
0)e imO, Pff:(cos 0)are as- where the integration is over the volume of the sample.
sociated Legendre functions, and p, O, ¢~are respec- From eqs. (A2) anti ( ~ ) the intensity of a particular
tively the radial, polar, and azimuthal coordinates of mode (n,m,r) is
position vector p. hnm are real coefficients of expan-
sion The mode (n, m, r) is excited by an rf field h Pnmr(X) = 4hnmf(X ) f 1
~ven by h V~nm(P). From eq. (A1), the components
=
Vsample
of h are (omitting the arguments of the Y function,=
!,:)r brevic.y)
+ aUnmr(P) r nm - ~ + ...]hx(P ) d p , (AS)
hx=~',~o°nm~'~'' 1 [-Y~,_+~+(n+m)(n+m- l ) ] n,rrj,-I _~
~]'
where

i~, : ~- n- 1 [+ym+l , m-- 8 1


~h,,~p n -1 + (n + m) (n + m - 1),r,, ~] , f(A9 (A6)
-rr (X- X0)2 + 8 ~
R.W. Sanders et al. / Magnetostatic modes in antiferromagnetic resonance 317

The coefficients hnm are found by analyzing the rf site symmetry are predicted to be the modes (110),
field in the rectangular waveguide, operating in the (310), (311) and (330).
TEl0 mode. z is the spatial coordinate measured from
the center of the sample along the direction of micro- A2. lnode site spectra
wave propagation, while x is measured from the center
of the sample in the direction parallel to the longer By the same procedure used for Imax, eq. (A9) be-
cross-sectional width of the waveguide, which is taken comes
to be of width a. For a sample centered in the wave-
guide at distance I from the terminating short, the h x -- 1] D [1 - ~(XxX)
t, 2 l tkzz ~(kzz)3l
transverse components of the rf field are

h x = D cos(kxx ) cos[kz(z - / ) 1 cos o~t, =- Dtk:rO - 03k2kz r2 - la3k2kzr3 2

hy = 0 , (A7) ,03(i!6 k2xkz _ l.~k3z) yO _ i!603kz(k 2 , k 2) vO] .

where k x = ~r/a, k z = 2rr/X, and D is a constant repre- (A12)


senting the strength of the rf field. In the rotating Values of hnm at/node appear in table 2. Unlisted
frame, eq. (A7) becomes modes with n K 4 have Pnmr = 0. The principal modes
excited in this site symmetry are predicted to be; the
h x = ~D cos(kxx ) cos(kxZ ), when l = lmax , (A8)
modes (21 0), (4 10), (41 1) and (430).
and Since at/node the rf electric field is maximum, the
dielectric constant e of the sample acts to distort the
h x = t D cos(kxx ) sin(kzZ), when 1 =/node • (A9) rf field. Qualitatively, this is equivalent to having a
sample larger in size by e 1/2. Consequently, Pnmris
larger by £n/2. The values o f ffnrnrgNen in table 2 in-
A1. lmax site specYa
clude this effect, taking e = 6.7 in MnF 2.

To find the components of eq. (A8) in terms of


spherical harmonics when R '~ a, R ~- X; eq. (A8) is Refi~rences
approximated as
[1] L.R W',fiker, Phys. Rev. 105 (1957} 390;
h x = ~D[I - ~(kxx)2l [1 - ½(kzz)2l L.R. Walker, in Magnetism, Voi. I, eds. G.T. Rado and
H. Suhl (Academic Press. Inc., New Yerk, 1963) ch, 8.
[2] P.C. Fletcher and R.O. Bell, J. Appl. Phys. 30 (1959)
=½ofyO_ ½02[ (2k2 _ k 2 ) + 6k 2 687.
(A10) [3] R. Plumier, Physica 28 (1961) 423.
[41 P.C. Fletcher, I.H. Solt, Jr. and R. Bell, Phys. Rev. 114
1 x2 + k 2) Y00]}+ higher n terms.
+ 2 k 2 y ~ 2 + ~(k (1959) 739.
[5] J,F. Dillon, Jr. and J.P. Remeika, Appl. Phys. Letters 2
The hnm values found by comparing eqs. (A1 O) and (1963) 38;
J.F. Dillon, Jr., H. Kamimura and J.P. Reme~a, J. Appl.
(A2) are listed in table 2. For our experiments in the
Phys. 34 (1963) 1240.
K.band X = 1.6 cm, R = 0.072 cm, k z = 3.9 era- 1, [61 D.E. Beeman, J. Appl. Phys. 37 (1966) 1136.
and k x = 2.9 cm- 1. Table 2 lists the integrated in- [7] Yu. M. Yakovlev and Yu. N. Burdin, Soy. Phys. Solid
tensities of the lines found from these values and State i0 (i968) i284.
[8] D.E. Beeman, H.J. Fink and D. Shaltiel, Phys. Rev. 142
oo
(1966) 454.
ff nmr --- f Pnmr (X) dX " (All) [9] J.P. Kotthaus and V. ]accarino, Phys. Rev. Letters 28
__oo (1972) 1649; i

J.P. Kotthaus, Ph.D. Thesis, University of California at


All the MSMs with n ~< 4 which are not tabulated for Santa Barbara, (1972) unpublished.
Imax h a v e Pnmr= 0. The modes best excited at this [lOl R. Loudon and P. Pincus, Phys. Rev. 132 (1963) 673.
318 R. W. Sanders et al. /Magnetostatic modes in antiferromagnetic refonance

[I I ] R.M. White, J. Appl. P~ys. 36 (1965) 3653; [ 15] E. Montarroyos and S.M. Rezende, tD be published.
A. Brooks Harris, Phys. Rev. 143 (1966) 353. [16] R.W. Sanders, D. Paquette, V. Jacca~.-ino and S.M. Re2:ende,
[12] A.R. King and S.M. Rezende, unpublishe¢t d~ta. Phys. Rev. BIO (1974) 132.
[13] C. Trapp and J.W. Stout, Phys. Rev. Letters ~0 (1963) [ 17] See, for example, B. Lax and K.J. Button, Microwave
157. Ferrites and Ferrimagneties (McGraw-Hill Co., New York,
[14] R.A. Hurd, Can. J. Phys. 36 (1958) 1072; 1962) p. 480.
J.E. Mercereau and R.P. Feynman, Phys. Rev. 104 (1956)
63.

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