VOLUME

17, NUMBER 22

PHYSICAL REVIEW LETTERS

This value is of the order of that

observed by Ahlers and Qrttung' for the entropy under the & spike.
Temperatures' at which side peaks in the nuclear-magnetic-resonance
lines of solid H, appear and disappear upon cooling and warming,
respectively, are plotted also in Fig. 1. These
temperatures appear to be those at which the
H, crystal first starts to change from hexagonal to cubic on cooling or finally complete the
transition from cubic to hexagonal on warming.
When the points are shifted down in temperature by half the &7' over which the structure
change takes place, then the agreement with
Ttr and Tp is quite satisfactory as shown by
the arrows in Fig. 1. It is a reasonable conjecture that the nmr anomaly results because
the cubic symmetry of the crystal favors a splitting of the energy levels.
deg mole.

28 NovEMBER 1966

2R. L. Mills and A. F. Schuch, Phys. Rev. Letters

15, 722 (1965).
3C. S. Barrett, L. Meyer, and J. Wasserman, J.
Chem. Phys. 45, 834 (1966).
4F. Reif and E. M. Purcell, Phys. Rev. 91, 631 (1953).
5G. W. Smith and R. M. Housley, Phys. Rev. 117,
732 (1960).
R. W. Hill and B. W. A. Ricketson, Phil. Mag. 45,
277 (1954).
7R. W. Hill, B. W. A. Ricketson, and F. Simon, in
Conference de Physique des Basses Temperatures,
Paris, 1955 (Institut International du Froid, Paris,
1955), No. 76.
G. Ahlers and W. H. Orttung, Phys. Rev. 133, A1642
(1964).
~C. M. Cunningham,
D. S. Chapin, and H. L. Johnston,
J. Am. Chem. Soc. 80, 2382 (1958).
A. F. Schuch and R. L. Mills, Phys. Rev. Letters
8, 469 (1962).
~E. Cremer and M. Polanyi, Z. Physik. Chem. B21,
459 (1933).
K. Motizuki and T. Nagamiya, J. Phys. Soc. (Japan)
11, 93 (1956).
T. Nakamura, Progr. Theoret. Phys (Kyoto) 14,
135 (1955).
W. H. Orttung, J. Chem. Phys. 36, 652 (1962).
i5J. Jarvis and H.
Meyer, Proceedings of the International Conference on Low Temperature Physics,
Moscow, 31 August-6 September, 1966 (to be published).
~

*Work performed under the auspices of the U. S.

Atomic Energy Commission.
~M. Clouter and H. P. Gush, Phys. Rev. Letters 15,
200 (1965).

ABSENCE OF FERROMAGNETISM OR ANTIFERROMAGNETISM

ISOTROPIC HEISENBERG MODELS*

IN ONE- OR TWO-DIMENSIONAL

N. D. Merminf and H. Wagner'.

Laboratory of Atomic and Solid State Physics, Cornell University,
(Received 17 October 1966)

Ithaca, New York

It is rigorously proved that at, any nonzero temperature, a one- or two-dimensional

isotropic spin-8 Heisenberg model with finite-range exchange interaction can be neither
The method of proof is capable of excluding a vaferromagnetic nor antiferromagnetic.
riety of types of ordering in one and two dimensions.

The number of exact results on the presence

or absence of phase transitions in systems with
realistically short-range interactions is small:
Van Hove has proved that there are no phase
transitions in a one-dimensional classical gas
with hard-core and finite-range interactions,
and Griffiths has proved that the Ising model
is ferromagnetic in more than one dimension. '
More recently Hohenberg has shown that an
inequality due to Bogoliubov~ can be used to
exclude conventional superfluid or superconducting ordering in one or two dimensions.
We have found that a similar application of the
Bogoliubov inequality leads to a surprisingly
elementary but rigorous argument that the one-

isotropic Heisenberg modof finite range can be neiantiferromagnetic at

nor
ther ferromagnetic
These conclusions have
nonzero temperature.
long been suspected, being suggested by calculations of the elementary excitations from
the ordered state, ~ as well as by considerations
of the energetics of domain walls. ' In view
of the present degree of activity in criticalpoint studies, it nevertheless seems worth recording that these very plausible results can
be proved rigorously. 6
We prove that there can be no spontaneous
magnetization or sublattice magnetization in
an isotropic Heisenberg model with finite-range

and two-dimensional
els with interactions

1133

PHYSICAL REVIEW LETTERS

VoLUME 17, NUMBER 22

interactions at temperature 7.', by showing that

for sufficiently small fields h,
Is

Const.
&

Is Ihl

&

'

and, therefore,

(4)

(2 dimensions),

Ihl"'

(1 dimension),

(2)

where sz can be taken as either the infinitevolume limit of the magnetization per particle
in a uniform field h, or the infinite-volume
limit of the difference of the two sublattice
magnetizations per particle, in a field of magnitude h and opposite sign on the two sublattices.
The proof exploits Bogoliubov's inequality, 3

'((A, Aj ))([[C,H], Cj]) - k T I([C, A]) I',

(3)

where H is the Hamiltonian and (X') = TrXe I /

Tre IH with P=1 jkDT'. The following elemen-

tary proof of the inequality is designed to make

it clear that (3) is valid provided only that the
operators A and C are such that the ensemble
averages on the left-hand side of (3) exist.
Define

28 NovEMBER 1966

It is also easily verified that (A, B) satisfies

all the definitions of an inner product necessary to establish the Schwartz inequality
(A, A)(B, B) ~ l(A, B)l2.

Finally, if one chooses B =[Ct, H], then

j, A j']),

(A, B) = ([C

(B, B) = ([Cj', [H, C]]).

Equation (3) follows from (4)-(6).
To apply the inequality to the Heisenberg
model, let
H=

-Q

J(R-R')S(R) S(R')
~

RR'

-hgs

W. W.
(A, B) =)

(zlAI

j)

(ilB

j)
Z

where the sum is over all pairs from a complete

set of energy eigenstates, excluding pairs with
the same energy; Wz e ~E&/Tre PH. Note
first that
0

&

(R)e

(W. -W. )/(Z. -Z. ) &-,'P(W. + W. ),

To rule out ferromagnetism we will take K to

be 0, and to exclude an iferromagnetism,
we
= 1 when R connects
chose it such that e~
sites in the same sublattice, and -1 when it
connects sites in different sublattices; R and
R' run over the sites of a Bravais lattice with
the usual periodic boundary condit'ion to insure
the presence of just N spins; J(0) =0, J(R)
= J(R), and
is of finite range. 7 Define

g- e

S(k) =Q-e

S(R), S(R) = (1/N)

J(k) =p e

J(R), J(R) = (1/N) Qke

S(k),

J(k)

(where sums over k are always restricted to the first Brillouin zone).
If we take C = S+(k), A = S (-k-K), then (3) gives

2((S (k+K), S

(-k-K) )) ~N2k Ts I(l/N)Q, [J'(k)-J(k'-k)]

x(S ( k') S (k') + ,(S (k'), S (-k') })+ (N/2)h s

where sz (1/N)~R(Sz(R)e~K'R).

1134

The denominator

on the right-hand

side of (8) is positive, being

(8)

VOLUME

PHYSICAL REVIEW LETTERS

17, NUMBER 22

28 NovEMBER 1966

of the form (B, B), and is therefore less than

+ 2Nlhs

(S ( k')S (k)+ 4(s (k'), S (-k')])

)Q,e

(I/N)lg J'(R)(1-e

l(NP IJ(R) l(1-cosk R)s(S+1)+ &Ntks

z
R
~

(-.'N[P-R'IJ{R) IS(S+ I)k'+ lks t].

We have used the fact that

(R)s. (R)) =N'(S. (R )S.(R ))

P-,
k' (s.(k')S. (-k')) =NQ-(s.
0
0
R
S

independent of R, . Replacing the denominator

k, we may conclude that'

by this upper bound and summing

S (S+ 1) & 2k 7's & '(1/N)Q-[S(s+1) Q-R'IJ(R) Ik'+ Iks z

k
R
B
In the infinite-volume

Ts

&

27T

where I/p is the volume per spin and d is the

number of dimensions. This inequality is strengthened if we integrate only over a sphere contained
in the first Brillouin zone, so if ko is the distance of the nearest Bragg plane from the origin in k space, then
1
2wps(s+ 1) (u
kT ln(1+ &u/Iks
k 2

I)

(13)

(2 dimensions),

2kT tan

S(S+ 1)
'lv/lhs

I)

"!)

(14)

(1 dimension),
(u

l]

dk

first zone

both sides of (8) over

limit (11) becomes

2k

S(s+1)

(10)

=Qs(s+ l)k 0 R2IJ(R) I.

In the limit of small k these reduce to (1) and

(2).
The following additional points are of some
interest:
(1) If the coupling is anisotropic the argument
is inconclusive, but if J& Jz WJ, then the
same conclusions are reached for aligning fields
in the s direction.
(2) Our inequality rules out only spontaneous
It
magnetization or sublattice magnetization.
does not exclude the possibility of other kinds

Ik'+
[S(S+1)Q-R'IJ(R)
R

of phase transitions

(12)

Iks I]
g

For example

-0 but (&sz/&h)T = ~ as k
with sz
consistent with (1) or (2).

a state

-0 is not

in-

(3) A very similar argument rules out the

existence of long-range crystalline ordering
in one or two dimensions, without making the
harmonic approximation.
(4) Since our conclusions hold whatever the
magnitude of 8, one would expect them to apply to classical spin systems. We can, in fact,
prove them directly by purely classical arguments in such cases.
This study was stimulated by our hearing
of P. C. Hohenberg's argument in the superfluid case. We have also had very useful conversations with G. V. Chester, M. E. Fisher,
and J. Langer.
*Work supported by the National Science Foundation
under Contract No. GP-5517.
)Alfred P. Sloan Foundation Fellow.
f Permanent address: Max-Planck Institute fur Physik, Munchen, Germany.
I, . pan Hove, Physica 16, 137 (1950); R. B. Qrif-

fiths, Phys. Rev. 136, A437 (1964). See also R. Peierls, Proc. Cambridge Phil. Soc. 32, 477 (1936).
P. C. Hohenberg, to be published.
N. Bogoliubov, Physik. Abhandl. Sowjetunion 6,
1, 113, 229 (1962). See also H. Wagner, Z. Physik
195, 273 (1966).

1135

VoLUME 17, NUMBER 22

PHYSICAL RKVIK%' LETTERS

4F. Bloch, Z. Physik 61, 206 (1930). Bloch discusses only the ferromagnetic case, but in spite of some
suggestions to the contrary t see D. Mattis, The Theory of Magnetism (Harper and Row Publisher, Inc. ,
New York, 1965), p. 244], his analysis leads to similar conclusions in the antiferromagnetic case.
5See C. H. Herring and C. Kittel, Phys. Rev. 81, 869
(1951), footnote on p. 873, and also G. Wannier, Elements of Solid State Theory (Cambridge University
Press, Cambridge, England, 1959), pp. 111-113.
For example, the doubts recently raised by H. E.

EVIDENCE FOR RESONANT-MODE

28 NOVEMBER 1966

T. A. Kaplan, Phys. Rev. Letters 17, 913

(1966), on the validity of Wannier's conclusions can
now be laid to rest, although their alternative suggestion of a transition to a state without spontaneous magnetization is not inconsistent with our theorem.
~Actually it is enough that QR R2~J(R) converge.
We have not hesitated to sacrifice better bounds for
simpler expressions [e.g. , tSx2(RO)+S& (Ro)) &S(S+1)],
but such crudities affect only the constants in (1) and
Stanley and

(2) and not the dependence on Q and T.

~N. D. Mermin and H. Wagner, to be published.

SIDEBANDS IN ALKALI HALIDES*

G. Benedek and G. F. Nardellif

Istituto di Fisica dell'Universita di Milano, Milano, Italy
(Received 17 October 1966)
Recently sidebands of a local-mode absorption peak were observed in alkali halides doped
by a very light negative impurity. '& They were
recognized to be produced by the combination
of the local mode itself with an odd mode of
the vibrational quasicontinuum, '&3 through the
anharmonic interaction. Hereafter, we cail
odd the modes whose displacements are antisymmetrical with respect to the defect site,
i.e., u(-f) = u(l). The experimental observation of the sidebands represents a direct method to detect the spectral density of the impurity-induced odd modes. Nevertheless, this
method has been applied only in the case of
the U center, the only case as yet known in
which the defect is able to produce a local mode.
Our purpose here is to give theoretical support to the existence of sidebands for low-frequency resonant modes also, and to suggest
how to detect them by stress experiments.
%e will show, indeed, that the application of
an external stress makes one able to divide
out the harmonic lattice absorption in the total absorption spectrum. One should then be
able to extend to a good number of impurityhost lattice systems the experimental study
on the odd-mode spectral densities. Since the
coupling coefficients responsible for the sideband absorption are simply related to the cubic anharmonic coefficients in the defect-hostlattice interaction, stress experiments on the
resonant as well as local-mode absorption peak
are also suggested in order to deduce such coupling coefficients.
Consider an infrared (IR)-active resonant
mode (I" symmetry) which produces a narrow

1136

absorption peak in the low acoustic-frequenLi+ in KBr). The

cy region (for example,
two-phonon absorption processes which can
occur below the reststrahl region are schematically shown in Table I. 0 denotes the frequency of the absorbed light; ~e and ~0, the frequency of the even (1,5) and odd phonons, respectively. The statistical weight for the process
is reported in the last column, where n(u)
= [exp(hu/k T)-1] ~ denotes the phonon occupation number at absolute temperature T. Since
we are concerned with low-temperature
absorption spectra, we consider the contribution coming from the first process (Stokes sideband)
and the small contribution coming from the
second process (photon-resonant phonon annihilation with odd-symmetry phonon production),
while we neglect the third process (anti-Stokes
reststrahl sideband). Furthermore, we assume
that the resonant mode does not extend appreciably beyond the first neighbors of the impurity, and we retain only terms of the type
C 's'(0, 0, f):u(0)u(0)u(l) in the local anharmonic interaction [0 denotes the impurity site; E,
the nearest neighbors (nn) ].
By using the method given by Nguyen, the
sideband contribution to the IR absorption coTable I. Two-phonon absorption
ing sidebands below the reststrahl

processes generatregion.

Process

Weight

=~o+cue (resonance)

1+n(~e) +n(~o)

0 =no-~e (resonance)
~ = ~e (reststrahl)-mo