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EXCITON SCATTERING ON SPIN WAVES IN

QUASI-ONE-DIMENSIONAL ANTIFERROMAGNET

V. Eremenko, V. Shapiro, I. Kachur

To cite this version:

(2)

JOURNAL DE PHYSIQUE

Colloque C8, Supplement au no 12, Tome 49, dkcembre 1988

EXCITON SCATTERING ON SPIN WAVES IN QUASI-ONE-DIMENSIONAL

ANTIFERROMAGNET

V. V. Eremenko, V. V. Shapiro and I. S. Kachur

Institute for Low Temperature Physics and Engineering, Ukr. SSR, Academy of Sciences, 310164 Kharkov, Lenin Avenue, 47, U.S.S.R.

Abstract. - Exciton absorption bandwidths have been measured in a quasi-onedimensional antiferromagnet CsMnC13.2 Hz0 and a three-dimensional MnF2 in magnetic fields oriented along crystal "easy" axes. In one-dimensional antiferromagnets exciton-magnon interaction is shown t o result in a considerable broadening of exciton bands in the vicinity of the critical field of the spin-flop transition.

In one-dimensional (Id) antiferromagnetic (AFM) dielectrics the spin wave dispersion has strong anisotropy: at the wave vector k oriented along the strong exchange interaction direction, the magnon en- ergy changes from EO ("a slit" in the spectrum, i.e. the spin wave energy in the Brillouin zone center) to E,, (the maximum energy at the zone boundary); for transverse directions the energy dispersion is too small. It leads to additional peculiarities in the energy distri- bution of density of magnon states, p (E) : besides the peak near the band Yap"

,

p (srnax)

,

there appears the peak near its "bottom"

,

p (E)

.

In the present work the exciton absorption bandwidth has been studied in Id AFM CsMnCl3.2 H20. It is shown that its be- havior near the orientational phase transition induced by an external magnetic field (the spin-flop transition, H,=1.8 T at T = 1:96 K) is due to exciton scatter- ing on spin waves. In this case the high density of magnon states near the band "bottom" in Id AFM plays a predominant role. For comparison similar stud- -

-

ies of the exciton bandwidth were performed in a three- dimensional (3d) AFM MnF2.

In order t o study experimentally the broadening mechanism of light absorption bands, the temperature dependences of their half-widths are generally inves- tigated [I]. However, for such an experiment, it is difficult to distinguish contributions to the bandwidth from both the interaction of excitons with magnons and their interaction with acoustic phonons. In the present work we fixed temperature (as low as pos- sible, in order to diminish the phonon effect of the bandwidth) and varied the number of thermally ex- cited magnons, thereby decreasing "a slit" in the spin- wave spectrum by an external field H oriented along the crystal "easy" axes.

pendences of band half-widths in CsMnCl3.2 Hz0 (0)

and MnFz (a) on the magnetic field strength oriented along the "easy" axes of these AFM crystals. In the case of manganese fluoride the exciton band half-width increases by about 10 % in a field H H c as com- pared with the initial value. For CsMnCl3.2 Hz0 the band broadens approximately by a factor of 3.5 near the Hc field,. In the spin-flop phase (H

>

Hc) the ex- citon band half-width in CsMnCl3.2 Hz0 takes again its initial value in the absence of an applied field.

Objects of investigation were the exciton band of the Fig. 1. - Relative broadening of exciton bands in

6 ~ 1 g ( 6 ~ ) + 4 ~ 2 g ( 4 ~ ) transition in a CsMnCls.2 HzO ~ s ~ n ~ 1 3 . 2 HzO (o) and MnF2 (;) due to exciton scat-

tering on spin waves versus magnetic field strength; H

//

b, crystal in a field H

//

b at 1.96 K, and the exciton band = for CsMnC13.2 HzO; H

//

C4, = 14

of the 6 A t (6S) -j 4Tlg (4p) transition in MnF2 in for MnF2. Solid curves are calculated for a) Id AFM;

a field H

//

C4 at T = 14 K. Figure 1 gives the de- b) 2d AFM.

(3)

C8 - 1482 JOURNAL DE PHYSIQUE

The exciton-magnon interaction operator responsi- ble for the exciton scattering on magnons can be rep- resented in the form

J S z

H e - r n , p = ~

C

x

k 1

...

k3

x [@I, (k2, kg) B: (ki

-

k2

+

k3) Bp (ki) b'(k2) 6 (k3)

+62p (k2, k3) B: (ki

+

k2

-

k3) Bp (ki) b (k2) b+ (k3)] (1) Here J is the exchange integral along the a-direction

of a strong interaction, z = 2 the number of nearest neighbours along the &chain; B: (k) and B, (k) exci- ton creation and annihilation operators, respectively, in the p band, and b+ (k) and b (k) those of magnons of the low frequency branch; N the number of crystal lattice sites, S the spin of the ground state.

The interaction amplitudes

a;,

are of the form @ll (k2r k3) = - ( ~ V j c ~ U k ~ ~ k ~

+

eUk2 Uk,; @12 (k2r k3) = -pVk2 U k 3 x 3

+

pUk2 Uk3~k2-k3 ; ( k 2 ~ k3) = -pVk2 U k 3 x 2

+

pVk2 Vk3Yk2 -k3 ; @22 (k2, k3) = -pVk2 U k 3 x 3

+

eVk2 Vk3; where (2)

J'

J'S' J' -1; p=--1; e = - J S J -1;

J' and S' are the exchange integral and the spin in the

excited state, respectively; Uk and Vk coefficients of the u

-

v transformation;

x

=

1

C

exp (ikA,) with

z

Q

the summation over the nearest neighbours of a. The exciton absorption band shape is described by the one-particle delay exciton Green function. Taking into account the exciton-magnon interaction (I), the approximate calculation of this function near the Hc field showed that for a Id AFM a change of the ex- citon band half-width is SHN (1

-

H/H,)-', for a 2d AFM it is SHN-ln (1-H/Hc) and for a 3d AFM SH has a finite limit near a field Hc.

For comparison between the calculation and the experimental results, figure 1 presents two curves (solid lines) corresponding t o theoretical relations: a) SH N (1

-

H/Hc)-l refers to a Id AFM, b) SH

-In

(1

-

H/H,) to a 2d AFM. Experimental points

(0) relating to CsMnCl3.2 Hz0 are concentrated be-

tween the curves and meet mainly the a) dependence corresponding to Id AFM. For a 3d AFM the exciton band broadening is negligible in a field H s Hc that is in agreement with the absence of peaks near the band "bottom" in the magnon state density distribution.

In the spin-flop phase the energy of the spin-wave band "bottom" increases by steps leading to a sharp decrease of magnon occupation numbers. As a result, the exciton band half-width in CsMnCl3.2 H20 takes its initial value for H = 0.

High magnon state density near "the bottom" of the spin-wave band manifests itself in a Id AFM by the shapes not only of pure exciton l~ands, but also of their magnon sidebands [2]. Figure 2 indicates spectral distribution of the light absorption c~oefficient K ( E ) in

CsMnCl3.2 Hz0 in the vicinity of the exciton band studied and its magnon sideband. Unlike 3d AFM in CsMnC13.2 H20, the exciton-magnon absorption is of a band character with the pronounced maximum not only near the frequency correspondi~ig t o the magnon band "top" (E,,-25 cm-l), but also to its "bottom" (EO 2 cm-l). The analysis of exci1,on-magnon band shapes showed that besides high magpon state density p (E) near E O , the significant factor which defines the

band character of the exciton-mapon absorption is the absence of the inversion center ill the location ofd an absorbing magnetic ion (this coiadition is met in CsMnCl3.2 H20).

Fig. 2. - Densitogram of a part of the CsMnC13.2 H 2 0 ab-

sorption spectrum near the exciton-magoon band; the sam- ple thickness is d = 7.1 mm, T = 1.65 F:. Light propagates along the b-axis, the light wave electric: vector is E,

//

c. Count is from the exciton line frequency.

[I] Yen, W. M., Imbush, G. F., Huber, D. L., Optical Properties of Ion Crystals (New York, London, Sydney) Interscience (1967) p. 301.

[2] Novikov, V. P., Kachur, I. S., 13remenk0, V. V.,

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