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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.
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
(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
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
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
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
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
' =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
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
[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.