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Submitted on 1 Jan 1978

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EXCITATIONS IN THE ISING COMPOUND

RbFeCl3-2H2O

Q. van Vlimmeren, C. Swüste, W.J.M. de Jonge

To cite this version:

(2)

JOURNAL D E PHYSIQUE

Colloque

C6,

supplPment au

no

8, Tome 39, aoiit 1978, page C6-743

EXCITATIONS

IN THE

ISING COMPOUND RbFeC13.2 H20

Q.A.G. van Vlimmeren, C.H.W. Swiiste and W.J.M. de Jonge

Department of Physics, Eindhoven U n i v e r s i t y

of

TechnoZogy, Eindhoven, The N e t h e r Z a d s .

RBsum6.- La rlsonance de cluster de spin (SCR) a dt8 observ6e dans l'antiferromagn6tique

pseudo unidimensionnel d'Ising RbFeC13.2H20. L'inclinaison des moments conduit

2

des

rlsultats caract8ristiques aussi bien d'une chalne ferromagnltique que d'une chalne anti-

ferromagnctique.

Abstract.- Spin cluster Resonance (SCR) is observed in the pseudo one-dimensional canted

Ising antiferromagnet RbFeC13.2H20. Due to the canting of the moments the SCR experiments

show characteristics of both a ferromagnetic and an antiferromagnetic chain.

Recent reports on RbFeC

13.

2H20 (RFC)

/

1 ,

E

=

-

2Ja

+

m {aJb

+

BJc

+

yJbc>

2

2mC.b for %//c

2,3/ have indicated that this compound can be con-

(1)

sidered as a good realization of an Ising system.

E = -

2Ja

+

m {aJb

+

BJc

+

yJbc}

+

26mc.'it for'it//a

The specific heat

/ I /

can be descirbed both above

and below the ordering temperature (TN

11.96 K)

with Onsagers rectangular S

= 1

Ising model with

( ~ / k l

=

39 K and ( ~ ' / k (

=

0.3

K. At T

=

4.2 K

application of a megnetic field along the c axis

results in two metamagnetic phase transisitons at

8.1 and 12.4 kOe /1,3/, respectively. The increase

in the magnetization is equal at both phase tran-

sitions. The basic excitations in Ising-like sys-

tems can be treated as localized spin reverseals.

In pseudo one-dimensional systems, like W C , the

excitation energy of a spin cluster depends mainly

on the intrachain interaction. For RFC these exci-

tations will be located in the far infrared (FIR)

region. Indirect excitations starting from a ther-

mally excited spin cluster, spin cluster resonance

(SCR), are much lower in energy since only inter-

chain and Zeeman interactions areinvolved. Given

the magnitude of

J'

and the rather pronounced

Ising-like properties it was anticipated that SGR

should be observable in the

GHz

region. As a con-

sequence of the canting of the moments in the ac

plane the experimental SCR results exhibit charac-

teristics of both a ferromagnetic (H//c) and an

antiferromagnetic chain (Hlla).

We assume three different interchain in-

( 2 )

with a

=

2,O or -2, 6

=

2,O or -2,

y =

4,2,0,

-2 or -4, 6

= 0

for even m and

6 = 1

for

m

m

odd m. The actual values of a, 6 and

y

depend on

the orientation of the spins in the neighbouring

chains. The expressions for the SCR frequencies

are obtained by taking the difference of spin clus-

ter energies with different

m.

The SCR data for H//c (Figure

1)

can be

fitted very well on basis of this pure Ising

mo-

del (Equation I), with Jb/k

-0.76 K, Jc/k

=

0.21 K, Jbc/k

-

-0.13 K,

;.2/l3l

=

1 . 5 0 ~ ~ .

Reson-

nances which involve an increase of the cluster-

size up till 9 spins are observed.

The SCR spectrum for H//a (Figure 2) shows

a nonlinear field dependence of the frequencies,

which is not predicted by the pure Ising model

(Equation 2). A detailed study of the SCR frequen-

cies shows that this curvature may be explained by

1

the splitting of the lowest doublet

( S = T )

by the

crystal field and spin-orbit coupling.

A

crystal

field study shows that the full splitting of the

spin quintet (S=2), may be described by the Harnil-

tonian

/ 7 / .

K

=

D(S~

z

-

LS(S+I))

3

+

E

(

S

:

-

):S

(3)

teractions /2,3/ J in the b direction, Jc in the

b

when D<O an

(EI

I D /

a pseudo doublet is lowest

c direction, and J

diagonally in the bc plane.

bc

in energy with an energy splitting of

A

=

12D(1-

When all the interactions are taken to be Ising,

JI

+

3(E/D)

)I

.

the excitation enargy of m neighbouring spins in

The data for H//a (Figure 2) can be explai-

a

chain can be expressed as

ned satisfactorily on basis of a S

=

-

1

model

2

(3)

+ - P

w i t h A = 0.76 K,

U.H/(%~

= 4 . 3 p and t h e same

B s e t o f i n t e r c h a i n exchange p a r a m e t e r s a s used f o r H//c. F i g . 1 : Observed r e s o n a n c e f r e q u e n c i e s p l o t t e d v e r s u s f i e l d H, f o r H a l o n g c . A l l t h e i n s e r t e d l i n e s a r e t h e o r e t i c a l p r e d i c t i o n s f o r t h e p u r e I s i n g model ( E q u a t i o n I ) . The l i n e s a r e l a b e l e d w i t h t h e number o f e x c i t e d s p i n s and t h e c o n f i - g u r a t i o n o f t h e c h a i n s i n t h e a n t i f e r r o m a g n e t i c , i n t e r m e d i a t e and f e r r o m a g n e t i c phase.The t h e o r e - t i c a l p r e d i c t i o n s o f SCR of o t h e r c o n f i g u r a t i o n s a r e r e p r e s e n t e d b y b r o k e n l i n e s . F i g . 2 : Observed r e s o n a n c e f r e q u e n c i e s p l o t t e d v e r s u s f i e l d H, f o r H a l o n g a . The c u r v e s a r e t h e t h e o r e t i c a l p r e d i c t i o n s f o r SCR when t h e e f f e c t of t h e pseudo d o u b l e t s p l i i t t i n g A i s t a k e n i n t o a c c o u n t . Open c i r c l e s r e p r e s e n t SCR d a t a b e l o n g i n g t o t h e a n t i f e r r o m a g n e t i c o r d e r i n g . Closed c i r c l e s r e p r e s e n t SCR i n o t h e r c o n f i g u r a t i o n s . o n l y t r a n s i s i t o n s between l a r g e c l u s t e r s a r e o b s e r v e d . The v a l u e of A c a n a l s o b e i n f e r r e d from t h e h i g h t e m p e r a t u r e s u s c e p t i b i l i t i e s . T h i s y i e l d D = -20

+

5 K and E

-

2

+

I K g i v i n g A = 0 . 6 K, which i s c o n s i s t e n t w i t h t h e v a l u e d e t e r m i n e d by SCR. P r e l i m i n a r y measurements i n t h e FIR r e g i o n show t h a t a l s o d i r e c t e x c i t a t i o n s o f s p i n c l u s t e r s c a n b e o b s e r v e d . These e x p e r i m e n t s y i e l d a n i n t r a - 1 c h a i n i n t e r a c t i o n J a / k = 35 K (S =

?),

which i s i n r e a s o n a b l e agreement w i t h J J , / I C ~ = 39 K d e t e r m i n d from s p e c i f i c h e a t measurements. More d e t a i l e d e x p e r i m e n t s i n t h e FIR r e g i o n a r e i n p r o g r e s s .

T h i s i n v e s t i g a t i o n i s p a r t o f t h e r e s e a r c h program o f t h e " S t i c h t i n g v o o r Fundamenteel Onder- zoek d e r M a t e r i e @OM)".

Re£ e r e n c e s

/ I / Kopinga, K . , Van Vlimmeren, Q . A . G . , B o n g a a r t s , A.L.M., and De J o n g e , W.J.M., P h y s i c a 86-88 B+C (1977) 803.

/ 2 / Van V l i m e r e n , Q . A . G . , De J o n g e , W.J.M., and S c h u i l w e r v e , M.S.J., 1 3 t h IUPAP Conf. S t a t . Phys. H a i f a (1977).

/ 3 / B a s t e n J . A . J . , Van Vlimmeren, Q.A.G. and D e

J o n g e , W.J.M., t o b e p u b l i s h e d .

/ 4 / T o r r a n c e , J.B. and Tinkham, M., Phys. Rev.= (1969) 587-595. N i c o l i , D.F. and Tinkham, M. Phys. Rev. B

2

(1974) 3126. T o r r a n c e , J.B. and Hay, K.A., Phys. Rev. L e t t .

2

0 9 7 3 ) 163.

151'

Date, M., and Motokawa, M., H. Phys. Soc. J a p n

24 (1968) 41.

-

1 6 1 Thornton, D.D., Phys. Rev. B 1 (1970) 3193. / 7 / Schriempf, J.T. and F r i e d b e r g , S . A . Phys. Rev.

136A (1964) 518.

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