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Physica 11~ B (l9K.') lfill71 Nonh·HoIland Publishing Company
ON THE MAGNETOSTRICTIVE
PHENOMENA IN MET AMAGNETISM
J.A. TUSZYNSKI and H. COFTA"
Depanmen: of
Pll}'.flCS.
The UniUfsity of ("algcm\ Calgorv. AB. COlIQda
Received I~ April 19R2 Revised 21 June 11.»1.2
A semiclassical model of a merarnagnet comparison with the Mn~GaC compound the mechanisms involved are generalized and investigated. Both cases are free of possibilities of applications of this model
exhibiting nonlinear temperature expansion is presented and analyzed. A direct as an example displaying such a phenomenon is made. Earlier predictions about and refined. Two distinct cases of the feasible metamagnetic behaviour are found internal contradictions and paradoxes. in contrast 10 the previous models. The to other types of magnetic substances are outlined.
1. Introduction In this paper we are primarily concerned with the role rnagnetostrictive phenoraena play in the spontaneous (i.e. temperatureinduced) metamagnetic phase transitions. Spontaneous metamagnets (in a broader sense) are defined as such substances which exhibit first order phase. transitions between two magnetically ordered phases under the variation of temperature alone and even in the absence of external magnetic field. The particular case of the transitions between the ferromagnetic (F) and antiferromagnetic (AF) phases is termed the collinear metamagnetism. The following substances can be listed as examples of the temperatureinduced metamagnets:  perovskitelike carbide MnJGaC [14];  binary metallic system FeRh {5];  chromium modified Mn2Sb, i.e. Mn2.Cr~Sb with O.06~ x ~O.lO [69J,  Frl.9S_xMn"Aswith L19~x ~ 1.28 [101. These compounds represent the four main types of metamagnetic transitions: AF""'"F, F ~ AF, AF ~ Fi, Fi _".AF, respectively (the symbol Fi denotes the ferrimagnetic phase). A number of mechanisms have been proposed
• Institute or Physics, The A. Mickiewicz University. Poznan. Poland.
as a possible source of these orderorder magnetic transitions. First, Smart Ill] suggested the linear dependence on temperature of the magnetic sublattice molecular field constants:
I
A.. = A~(1 + aaT) ,
(1)
where a denotes the sub lattice index. Then, Neel [1213] assumed the anisotropy constants K~ and K4 as the cause of spontaneous metamagnetism provided they depend on temperature in two distinct manners: and
(2)
Other authors [1418] further modified the Neel model to include the exchange interactions. Still another group [1921] claimed the interactions between localized and collective electron spins in the itinerant magnetism theory to be responsible for the phenomenon under consideration. Recently, Onyszkiewicz [22261 has published a series of papers wherein he has developed a microscopic theory based on the fourspin couplings. It has also been attempted to describe metamagnetism in terms of the Landau theory of phase transitions with two interacting order parameters [27]. None of the abovementioned theories. however, fully explains the magnetostrictive effects associated with spontaneous metamag
03784363/83/(XX)().O()()O/$03.00 1983 NorthHolland ©
162
J.A. Tus:)·nski. H. Cofta I
MQKIlt'lo.~triClil~
pht'nomt'non
'" mt'IQmagnf'tism
netism. The discovery of abrupt lattice parameter discontinuities (without any structural changes in the crystal lattice) accompanying all these transitions at the metamagnetic temperature TM led Kittel 1281 to believe that the magnetoelastic mechanisms govern the temperature metamagnetism. All other papers that followed the idea of Kittel's 12931. 1. 21 employed the socalled exchange inversion hypothesis which asserts that the intersublattice exchange constant A inverts (i.e. changes its sign) at TM• or that A(T= TM)=O. (3)
Such a behaviour is supposed to result from the dependence of A on the interionic separation simultaneously with the thermal expansion of the crystal lattice. However, in the case of the Mn3GaC compound the interpretation of experimental data by the means of the Kittel model has proven unsatisfactory. Unlike other metamagnets, this substance displays unambiguously observed [14] lattice contraction at
tinuity in the exchange constant A at T,.. appears to have a negative sign making the transition to the Fphase impossible. Second. the quadratic thermal expansion of the crystal lattice of the Mn.,GaC 1141 has never been fully exploited in the theoretical investigations. It is very attractive, however. to take a close look at the thermal expansion coefficients as they contain the information about the strength of magnetoelastic interactions. In this paper we propose a semiclassical theory of the thermally expansible twosublattice magnet. The magnetic sublattices are assumed to be equivalent but the generalization to the case of nonequivalent sublattices is straightforward. By the means of statistical analysis we intend to replace the approximate and contradictive conditions (4H6) with a more plausible set of forrnulas.of higher accuracy and free of paradoxes. A diJct reference tp the experimental data of the Mn3GaC compound will also be made.
2. The model
Consider the following Hamiltonian: (7) where HL describes the crystal lattice interactions and HM denotes the magnetic part of the Hamiltonian. Since we intend to account for the quadratic temperature expansion of the lattice, the crystal potential ought to include at least the terms up to the sixth power in the lattice spacing
rij:
TM•
It is our belief that the shortcomings of the latter theory can be easily eliminated if only some oversimplifications are removed. First, the linear dependence of the exchange constant on the lattice spacing: (A(x»
3: A(i).
(4)
seems to be too crude an approximation. It implies the form of the condition for the AF + F transition as d(A) = a . aA(i) > 0 dT P ai . (5)
(8) where Uq = Irq  rtl denotes the displacement from the twoion zerotemperature separation r~ "" r? rJ. We assume the magnetic Hamiltonian HM to consist of the Heisenberg exchange and the magnetic anisotropy term which determines the easy magnetization axis x: HM =
(j3 is the thermal expansion coefficient), which is contradictory to the requirement that the lattice parameter be contracted at TM:
(6) where K stands for the compressibility constant. Moreover. within this framework, the discon
~LJM + L [Kz(Sr)2+
iJlri i
K4(S:t].
(9)
16..1
Since the easy magnetization axis in the collinear metamagnetism is found to be fairly constant with temperature. from now onwards we utilize the quasionedimensional description of the system with the xcornponent of denoted by Xii' being the only one present in the pseudoHamiltonian. Moreover. we expand the exchange integral J'J in terms of Xi) up to the second order
"<r
(in particular. the lattice contraction at T"f). we now investigate the statistical properties of the model. Due to the noncommutation of HL and HM• both the density matrix p
(15)
and the partition
function
Z
(16)
Z
(10) where
=
tr p
cannot be contained in the exact analytical form. In the previous paper [31]. the approximation for the density matrix has been adopted in the zeroth order: (lOa) (17) and the Bogolyubov principle for the free energy calculation has then been applied. In order (0 improve our accuracy we presently use the BakerHausdorffCampbell formu1a exp{Hl
The expansion coefficients are assumed to be independent of the choice of a pair of ions. Note. that since Jij depends on Xii. the two operators HM and HI,. do not commute with each other. For the sake bf convenience. let us separate two distinct contributions to the magnetic Hamiltonian:
+ H2) = exp(H1) exp(H2) x exp{~[Hh
I
h[H1[HI,
H2}
H2]J
(18)
H~ == and
2
1. LJaSrS,
i'"
+ TIlH2[H2, HI]] + ... },
(11) where HI and H2 win be chosen depending on the specific case considered. When calculating the average of an arbitrary positiondependent function !(Xii), we take and (13) (19)
(12) according to their commutation relations
IH~,Hd =0
and [HLM'
and notice that [H" H2] "" o. On the other hand. for the calculations of a spindependent function g(S,) we make another choice: and (20)
Hd
;eo,
(14)
as well as the roles they play in the phenomenon.
3. Statistical
averages concentrates around of the metamagnet
Since our major interest the macroscopic properties
and neglect the third exponent of (18). Such separations as (19) and (20) allow us to obtain the averages over the spin and lattice variables in dependently . Before proceeding any further. however, we assume the mean field approximation (MFA) neglecting fluctuations within each of the mag
164
netic sublattices, Consequently, we introduce new magnetic variables  the mean sublattice magnetizations Mo:
U(X) the crystal the magnetoelastic
6
lattice potential couplings:
modified
by
where a is the sublattice label. We also employ the MFA exchange constants: the intrasublattice parameter

V(X) (21)
= L CtX· + [(AI cos ¢J t2
Bt)(M)2]X (26)
(22)
and the intersublattice 1
=22
one
where A" A2• 810 B2 are the exchange derivatives analogous to those of (10) and 4J the angle between the sublattice magnetizations. It is clearly seen that the static lattice properties (e.g, the average spacing) are strongly dependent on both sublattice and total magnetizations. Similarly, the average of an arbitrary magnetizationdependent function (e.g. magnetization itself) can be expressed as (g(M»
A
Lioa.ja,B L
(JiiX5iX~)
.
== O~
(23)
L
Mo
g(M)
e"("
<u4+S>W1
dM
(27)
g It B
io".i.oJi(5iXSj)
Notice that these fotmulas contain the averages of the exchange integral over p of (15). Assuming homogeneity of the crystal lattice sites at equilibrium, we apply the same mean field approximation to the lattice Hamiltonian HL which results in dropping of all subscripts in the position variable and using the uniform lattice spacing X instead. Furthermore, our computations will be carried out in the semiclassical limit, so as to factor out the kinetic energy contribution in the partition function (24) where ON is the N particle configuration integral. Under the present circumstances. the average of an arbitrary positiondependent function I(x) can be calculated as
with 0,... denoting the magnetic partition function, Mo the sublattice saturation magnetization, A the average intersublattice constant: (28) and B the constant: average intrasublattice exchange
(29) Conversely. the static magnetic properties are considerably influenced by both the lattice dilatation (X) and the oscillations (X). The meaning of (25) can best be described as regarding the elastic lattice as the one with "frozen spins" on its sites. Eq, (27). in turn, views the spins as the ones placed on the sites of the rigid crystal lattice. Note, however, that since both equations are coupled, the two subsystems are allowed to dynamically interact with each other. Moreover. by obtaining a system of selfconsistent equations we do not have to consider the internal energy and entropy separately. The importance of the outlined averages is particularly transparent when we study the magnetic phase transitions of the system. Within the MFA theory. the Curie temperature Tc is
(f(X»
where
== OJ_1
I leX)
eIIU(X) dX •
(25)
Oi. is the lattice configuration
integral and
16.5 determined by (30) from (32) Since eqs. (30}(32) contain the average exchange constants A and B. all these transition temperatures Te, TN and TN win be affected not only by the tirst order magnetostrictive terms proportional to (X) (customarily considered), but also by the higher order ones with the lowest such term being proportional to the magnitude of lattice oscillations (Xl). In this work, special regard to the intersublattice interactions is given and, therefore, the intrasublattice exchange constant B is assumed to vary negligibly in the vicinity of TN. We . realize, however, that if the region of critical temperatures Tc and TN were focussed, this assumption would no longer be valid.
If the lowtemperature phase is AF, then the Neel temperature TN is given by
(31) In virtue of (25}(26), however, not only may these temperatures be modified due to magnetoelasticity, but the transitions themselves may no longer be of the second but of the first order (for the conditions see (27)). In the case when the two ordered phases exist in the neighbouring temperature ranges, the metamagnetic temperature TM can be found
4. Thermal expansion
Basing on the formulas given in the preceding section and using the quasiharmonic approximation in the semiclassical limit, we obtain the following explicit expression for the average lattice spacing: (33) with
ao 
_
AIM2COS~ 2(C2 A2M2COS~)'
(34)
(35)
(36) and the average lattice oscillations
(37) with (38)
166
l.A.
Tuszyriski. H. wfto
I MQg~IOSlrictiVf! phntOmmon
in m~ro,"QIf"f!rism
(39)
(40)
(41)
For the details of the derivation of the above formulas. see Appendix. In terms of the above coefficients. the average intersublattice exchange constant can be expressed as a polynomial function of temperature:
(42)
or. when the cubic term is neglected, from (32) one obtains a close form expression for the rnetamagnetic temperature:
T,  (alAI
M
+ dIA2)±V(atA1 + dlA2f  4(a2AI + d2A2)(Ao + A1ao+ A2do)
2(Ao+ A1ao+ Azdo)
(43)
I
In order for the model to be consistent we require that two additional conditions be satisfied: (i) for the AF + F (F + AF) transition A must be an increasing (decreasing) function of temperature. which implies that
(al'"
+ 2af' . T)AI + (dfF + 2df' . T + 3d~ . T2)A2 > 0 .
(44)
or (if F > AF takes place)
(45) (ii) if the transition is accompanied by the lattice contraction it follows that (46)
or. otherwise.
(47)
These conditions and the expressions for the phenomenological parameters will be confronted with the experimental data in the next section.
(i) the Curie temperature
5. Comparison with experiment Utilizing the measurements of [14] for the Mn3GaC compound we restate the important experimental data:
is (48)
Tc=(246±2)K; (ii) the metamagnetic temperature T Pot
as
J.A. Tus:~'ri.ski.H. Co(lO I MaSltt'roslriclit'!t'ph~ltom~_
in mtramag~ti5m
167
I
found by the extrapolation of data obtained in the magnetic field which was necessary to remove the magnetic domain structure equals TM= (l50z.5)K: (49)
3.•
S X
(:I
3.86
Af PI1.lst
(iii) the values of the sublattice magnetizations at TM relative to the saturation magnetization are
G ~
en
Z
3.84
3.82
3.80 3.18 3.7S+.,..,....r"T"T~ ......... ........ ...,..., ...,..,..T"T",......., .........
fairly close in both phases (for the plot of magnetization, see fig. 1).
m AF
o ~
III
5
== (MMAF)
o
=:; TTM
0.859 ,
(50)
40
80
120 160 200 240 280
TEMPERATURE (·K)
(51)
Fig. 2. Dilatational curve for the MnJGaC.
(iv) the lattice parameter discontinuity at TM has been measured as flX
e
and in the Fphase: Xo+
(XF X"hT),I =.O.059A.
o
ao= 3.885 A ,
106 A KI. (54)
;
(52)
al
= 1694 x
Moreover, using the dilatational analysis curve plotted in [3} we have found from the quadratic regression the following sets of thermal expansion coefficients, in the AFphase (see fig. 2): Xo+
a]
=
a2 = 648 x 108(~.K2• revealing a significant difference between the magnetoelastic effects in the two phases. It comes as no surprise that these values provide us with the correct sign and magnitude of the lattice parameter diminution at TM as in (52), since they are obtained from the experimental points. However, they produce an astonishing result when substituted into the theoretical expression for the lattice spacing. From (33) we obtain flX TM+ lla2' T~ sflXo+ flX1 + flX1
Aal'
ao= 3.831 A,
252 x 106 A K1
8
,
(53)
a2 = 192 x 10
A K
2,
~ ~
70 60
50
• E"I*1_ poinII 01 (2. Totel"""l .... """"'"
= A~+
:)
E
•. lil. + il~1
(55)
Z
0
~
40
30 20 10 0 0
E z
~
(!) 0:(
N
~.
00 100
150 200 250
T.1$O"I<
and upon substitution of eqs. (53)(54) and (49) we arrive at the numerica1 values of the three separate contributions towards the discontinuity of the lattice spacing flX at TM: AXo = +0.054
A,
(56)
300
AX1
flX2
of the
TEMPERATURE (41<) Fig. 1. Thermal
dependence MIhGaC compound. of the total magnetization
A, = +0.1026 A,
=
0.216
which bear important
consequences on the in
168
J.A. Tuszyriski. H. Co/la I MlIgl1r/osl7ictit~
pltmollltl1M
in mrramIJ8n"rism
terpretation of the phenomenon: P) Contrary to what has been believed until now. the zeroth order contribution ~Xn (caused by the harmonicity of the lattice) is not the one responsible for the lattice contraction at TM since it is of the positive sign. (2) It is the change in the linear temperature expansion coefficients between the two phases which makes the substance contract at TM• Unlike in previous theories. however, this condition does not lead 10 any contradictions. The coefficients C2, C3, C4. CS. Cit and Al and A~ are in no way predetermined except for the requirements (44)(47). still none of them contradictory to another. (3) The contribution due to the discontinuity of the quadratic thermal expansion coefficient ~X2' although of the positive sign. is large in magnitude (greater than ~Xo) and thus should not be neglected. (4) It follows from (34) that AI >0 and therefore eq. (46) indicates that the effect of nonlinearity of the exchange integral around Ttol is greater than that of the first order
(57)
<
~""'2
<
~
~1l4 u WI.fi
X
~
~I.8
41
8il
120
1611
10
246
28il
TOIP£RATURE: H
Fig. 3. Schematic plot of the inte~.sublaltice exchange constant with temperature.
We conclude that both the anharmonicity of the crystal lattice and the nonlinear distance dependence of the exchange integral are essential factors in the explanation of the Mn3GaC case. (5) From (44) and (46) we deduce that there are two distinct ways in which the metamagnetism of the MnJGaC may be realized: (a) the zerotemperature ground state without magnetoelastic couplings is antiferromagnetic (Ao < 0). The Arterm in (44) mayor may not increase with temperature but in the latter case the lower bound on A2 is imposed: (58) (b) the zerotemperature ground state without magnetoelastic couplings is ferromagnetic (~> 0) and the Arterm must decrease with temperature more slowly than the A Iterm increases.
Both these terms oppose each other. For the plot of the possible temperature dependence of A. see fig. 3. The first option seems more feasible than the other one since it does not imply too odd a position dependence of the exchange integral and has more flexibility in the choice of parameters. The second one has been recently suggested by Cofta and Pawlicki [33} as an explanation of the negative lattice parameter discontinuity. Our rough estimates show that at T M both terms are close in magnitude and of the same sign, thus favouring the first possibility.
6. Conclusions
We have derived theoretical expressions for the interpretation of magnetostrictive phenomena involving the anharmonic crystal lattice and a twosublattice spins system (the extension to onesublattice magnets and/or harmonic lattices seems fairly straightforward). The presented model removes deficiencies exis
Hi9
ting in the previous phenomenological theories of spontaneous metamagnetism. It also reveals two distinct ways in which the metamagnetism of the Mn~GaC compound can be realized without getting into internal contradictions. It is emphasized that the anharmonicity of the lattice is the major reason for the abrupt lattice contraction of the Mn~GaC at TM• Furthermore. the nonlinear exchange integral dependence on the interionic distance plays also a crucial role in the model. The theory developed in this paper can be easily adapted to describe other types of magnetic transitions associated with magnetostrictive phenomena. We believe that a refinement of the theory of first and second order AF + P and F + P transitions accompanied by magnetoelastic effects [34.35] may also be accomplished. The translation of the formulas (34),(35) and (38)(41) to embrace these cases poses no difficulty.
!
We think that the inclusion of higher order anharmonic terms as well as the influence of the lattice oscillations on the exchange integral may result in the modification of the expressions for critical temperatures and lattice parameter discontinuities (first order transitions) or thermal expansion coefficient jumps (second order transitions). Finally. we hope that the recently reported case of a ferromagnetic spontaneous magnetostriction (36] which has been encountered with some interpretative difficulties may be elucidated with the help of our model.
Acknowledgement This work has been partly sponsored by the Institute for Low Temperature and Structure Research. Polish Academy of Sciences. Wroclaw, Poland. i
Appendix Treating the lattice distribution function PL in the quasiharmonic approximation. we expand it as
where {3 = (kTf
1,
Making the substitution
of variables (A.2)
in a similar fashion to that used for the harmonic lattice coupled to the spins with the exchange proportional to the displacement [321. the PL becomes
integral
•
f
(A3) Above we have introduced the magnetically modified elasticity constant
c;:
(A.4)
as well as other lattice coefficients
changed
by presence of magnetic
interactions: (A.S) (A.6)
170 (A.7) (A.S) (A.9) (AW)
(All)
Due to the small magnitude of E itself and the decrease in value of the lattice coefficients with high subscripts. we have discarded all the terms which are nonlinear in E. Note also that the approximate canonical transformation (A.2) provides us with effective fourspin terms in the magnetic Hamiltonian and thus yields correspondence with the Onyszkiewicz fourion model (2226). The analysis of such a model from the point of view of the Landau theory of phase transitions has been carried out elsewhere [27] and showed that the use of two interacting order parameters is necessary. With the distribution function (A3) we calculate the average lattice separation and keep in mind that X denotes the distance relative to the zerotemperature lattice spacing (X)
=
2
f
(y
+ e)p(y)dy
== e + 2
I
I
0
yp(y)dy Gaussian integrals:
fI\.12)
The integration
is carried out with the help of the following
(A. 13)
o
J
o
x
2~+1
e
1U2
d
x  2a~+1'
~
(A 14) thermal expansion of the lattice
if only a> O. This leads to the quadratic
(A15)
where the expansion coefficients are functions of both M and
4>:
(A. 16)
•
(A.17)
(A.IB) Similarly, the calculation of the second moment dy of X2
(X2) = 2
f
o
(y
+ efp(y)
== 2(X)£'

£2
+2
J
0
y~p(y)dy
(A19)
171
yields the cubic temperature
dependence of the averaged lattice oscillations (A20)
with the following coefficients: (A.21)
d,
=!
k
2 (C2 A2M2
[1_ 15(C2 A2M cos t/J1#1'1 _ 3 (C2  A2M2cos ~)" ] • cJA.M cos c.(A M cos 1#1) 4 cos 1#1'1
2 I 2 2
(A 22)
d2 = _15
8 (C2  A2M2
k2
cos tfJ 'f
[c + Z c AIM· cos 1#1 +(A.W cos tfJ 'f ] ~ 2 5 C2 A2M'l cos tfJ 3C6 (C2  A2M2 cos 1#1 'f
•
(A. 23)
(A.24)
Note that the terms in the brackets in (A.16}(A.18) and (A21}(A24) are written in the decreasing order. .
References
[1] M Guillot, (2) M. Guillot These, Grenoble (1966). and R. Pauthenet, c.R.
[18] KJ. Michalski. W. Reich and H. Cotta, Phys. Stat. Sol.
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