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EUROPHYSICS LETTERS 1 July 1997
Europhys. Lett., 39 (1), pp. 91-96 (1997)

Magnon spectrum and related finite-temperature

magnetic properties: A first-principle approach

S. V. Halilov, A. Y. Perlov(∗ ), P. M. Oppeneer and H. Eschrig

Max-Planck Research Group “Theory of Complex and Correlated Electron Systems”
University of Technology - D-01062 Dresden, Germany

(received 28 February 1997; accepted 26 May 1997)

PACS. 75.30Ds – Spin waves.

PACS. 75.10Lp – Band and itinerant models.
PACS. 75.30Cr – Saturation moments and magnetic susceptibilities.

Abstract. – It is shown that the magnon spectrum of magnetically ordered crystals can be
calculated using a frozen magnon scheme and spin density functional theory in the local approx-
imation. Ab initio calculated magnon spectra for Fe and Ni are presented. Kohn anomalies
are predicted for the magnon spectrum of Fe. Considering the magnons as true low-lying
thermal excitations and using mean-field semi-classical statistics at elevated temperatures, the
finite-temperature magnetization and Curie temperature TC are calculated, which compare well
with experiment for Fe, Co, and Ni.

One of the present-day foremost challenges in the theory of metallic (itinerant) magnetism
is the description of finite-temperature magnetic phenomena entirely from first principles. To
the most recent achievements in this direction belong the progress in ab initio calculations of
noncollinear magnetism [1], with its impact on the ab initio dynamics of spin moments [2],
the onset of spin-glass behavior [3], calculated Curie temperatures TC [4], [5], and finite
temperature magnetization curves M (T ) [5]. The common aim of these developments is to
describe finite-temperature magnetism on the basis of density functional theory (DFT) in
the local spin density approximation (LSDA) which has been successfully applied to zero-
temperature metallic magnetism.
Along a different access route, previously much research was devoted to the development
of a thermodynamic ensemble theory of finite-temperature magnetism, based on the concept
of long-wavelength exchange enhanced spin fluctuations together with a modeling of the free-
energy functional [6]. Implementations of this concept have been based on various approaches
(see, e.g., [7]-[11]). These approaches have in common that they emphasized the importance of
low-lying spin excitations for finite-temperature properties, which are spin collective modes. In
order to open up the way for first-principles studies of finite-temperature magnetism below TC ,
the evaluation of the spectrum of spin collective modes, i.e. the magnon spectrum is required.

(∗ ) Permanent address: Institute of Metal Physics, Academy of Sciences of Ukraine, 252680 Kiev,
Ukraine.

c Les Editions de Physique
92 EUROPHYSICS LETTERS

In this letter, we show that the “adiabatic” magnon spectrum of arbitrary basis crystal
structures can be calculated ab initio. As an application we present calculated magnon
spectra of Fe and Ni. A particularly interesting point is that we predict a novel feature,
the existence of Kohn anomalies [12] in magnon spectra. As a second important application
we evaluate, on the basis of the derived formalism and the appropriate thermodynamics, the
finite-temperature magnetization M (T /TC), which is in excellent agreement with experiment
on the whole temperature scale from zero to TC . Also the calculated Curie temperatures of Fe,
Ni, and Co are close to the experimental ones.
Before we outline our approach, we mention that earlier calculations of the elementary
magnetic excitations were carried out via the evaluation of the transverse dynamical suscepti-
bility χ−+ (q, ω) [13]-[15]. This is treated in random phase approximation (RPA) with a local
exchange interaction (see, e.g., [6]) and proved to be well able to describe the overall magnon
dispersion as well as the influence of the interband spin-flip continuum; For Ni it seems to re-
produce the experimental spectrum [16] astonishingly well. The “adiabatic” magnon spectrum,
on the contrary, does not comprise the interaction with the interband spin-flip continuum, it
contains, however, all details of intersite exchange interactions of arbitrary range, manifesting,
e.g., in Kohn anomalies.
We proceed in several steps based on the concept
P Rof two time scales. The site spin moment
operators M̂i are introduced as M̂i = −2µB n σ̂ n Vi δ(r − rn )dr, where the sum runs over
all electrons in the crystal and
h Vi is thei volume assigned to the i-th atom. These operators obey
the commutation relations M̂i , M̂j = −2iµB δij εαβγ M̂iγ , (α, β, γ ≡ x, y, z). The adiabatic
α β

spin moment of an atom on site Ri is defined as Mi = hM̂i i, where the quantum average is
over the fast electronic degrees of freedom. The Mi are obtained from LSDA calculations,
whereby their directions are fixed at each atom site by constraints. Our approach adopts
similar assumptions as those made previously for the description of noncollinear magnetism, in
which the spin density matrix defines the local magnetic orientation [1]. Any spin configuration
can be obtained as a superposition of individual spin spirals which would be given as Mi ∼
(sin θi cos φi , sin θi sin φi , cos θi ) with φi = q · Ri + φ0i . The total energies of a set of static spin
spirals may be used to represent the total energy as a function of the moments to be
1X
E = E0 {Mi2 } − Jij Mi Mj + . . . , (1)
2
i6=j

with Jij ≡ J(Ri − Rj ) the exchange constants. The first term contributes to the on-site part
of the exchange energy, and the second term rules the transversal spin motion.
To obtain the spin modes from these LSDA results, it is assumed that the time scale of the
spin vibrations is much larger than that of the electron motion. For the average over the latter
we assume

hM̂i M̂j i = hM̂i ihM̂j i, for i 6= j. (2)

These assumptions result in a similarity to the adiabatic, or frozen phonon, approach for the
lattice vibrational modes, and we would therefore label it a “frozen magnon” scheme. The
calculations of the frozen magnons were performed self-consistently using the linear muffin tin
method [17]. In particular, the spin-orbit interaction has been neglected, and advantage of
the Bloch theorem in spinor representation has been taken to reduce the magnetic supercell
to the crystalline unit cell [18]. We emphasize furthermore that we did not put a constraint
on the length of the moment. The latter was obtained self-consistently for each spiral. We
note, however, that the part of the phase space {θ, q} where the length of the adiabatic moment
varies (large θ and q) has vanishingly small statistical weight below TC , even for Ni.
s. v. halilov et al.: magnon spectrum and related etc. 93

On account of the assumption (2), the expression (1) with the same Jij is now treated as
an effective Hamiltonian for the adiabatic transversal motion, which leads to the following
equations of motion:
∂φi X
sin θi =γ Jij Mj [cos θi sin θj cos φij − sin θi cos θj ] ,
∂t
j6=i
∂θi X
=γ Jij Mj sin θj sin φij . (3)
∂t
j6=i

Of course, although M̂2i is not varying in time, yet the relevant quantum states are not
eigenstates of M̂2i . The prefactor γ ≡ 2µB /h̄ is the gyromagnetic ratio, and φij ≡ φi − φj .
These equations describe the complete spin dynamics up to those temperatures at which the
magnitudes of the moments begin to change. In a single spatially extended magnon mode the
precession angles θi are small at all sites and one can linearize eq. (3) with respect to θi . In
addition, translational symmetry can be used to rewrite eq. (3) in reciprocal space, which leads
to the following set of equations (in complex notation):
X
θµqλ ωqλ = γ Jqµν θνqλ Mν exp[iφ̃0q µν ] , (4)
ν

with φ̃0q µν ≡ q · (τ µ − τ ν ) + φ0µν , and Jqµν is (up to an additive constant) the Fourier transform
of the exchange constants. The indices µ, ν run over all Na basis atoms in the unit cell, τ µ are
their positions. Equation (4) represents an Na -dimensional eigenvector, eigenvalue problem
for the frequencies ωqλ of the normal spin modes and their amplitudes θµqλ . The evaluation
of eq. (4) requires the knowledge of the exchange coupling constants, Jqµν ≡ |Jqµν | exp [iψqµν ],
which can be determined from the second derivatives of the energy function Ecell [θµ , φ0µν , q, Mν ]
per unit cell for a single spiral array
1X
Ecell = E0 + Re{Jqµν exp [iφ̃0q µν ]}θµq θνq Mµ Mν , (5)
2 µν

with respect to the variable θνq for each wave vector q. The practical step, which effectively
enables the determination of the Jqµν , is to compute the LSDA total energy for frozen magnons,
and to demand that its second derivatives are equal to those of eq. (5). The initial phases of the
spin waves φ0µν may be chosen to be given by Im{exp[i(ψqµν + φ̃0q µν )]} = 0. Once the
exchange force constants and site moments are known, the magnon spectrum can be computed
from eq. (4).
In figs. 1, 2 we present the calculated magnon dispersion curves and densities of states for
bcc Fe and fcc Ni, respectively. We note that the displayed spectra are distinctly different from
those of the Heisenberg model in nearest-neighbor approximation [19]. Genuine band effects
are to be expected for itinerant metallic systems, already because their potentials exhibit
long-range Friedel oscillations. In particular, we predict Kohn anomalies [12] to be present in
the calculated spectrum of Fe due to pronounced Fermi surface nesting of flat Fermi surface
regions of the Γ -centered electron surface for both spin directions. Magnon Kohn anomalies,
already anticipated in the original paper by Kohn [12], were never discovered experimentally.
In the case of Fe, rather sharp magnons in large parts of the BZ were obtained from the
RPA susceptibility [14], but, lacking theoretical predictions, no particular experimental search
for Kohn anomalies has been undertaken up to now, although several investigations of the
high-energy magnon spectrum were undertaken [20], [21]. Particularly in the Γ -P direction
where magnons are experimentally seen at the location of our predicted Kohn anomaly, a
careful investigation is highly encouraged.
94 EUROPHYSICS LETTERS

400 ....
. .......... ..........
. . .....
Energy (meV)
300
. .. .
.. .... ..
.. ...
..
200

. .
..
.. ...
100
.. . ... ..
... ......
H N P N0 1

Fig. 1. – Magnon dispersions of bcc Fe for high-symmetry directions. Experimental data, for pure Fe
at 10 K:  [20], and for Fe (12 % Si) at room temperature: [22]. Calculated dispersions are depicted
by solid circles and line. The right-hand panel shows the calculated magnon total density of states (in
states/(meV∗cell)×10−2 ). Note the Kohn-like anomalies (“cusps”) in the theoretical spectrum.

There is overall agreement with experiment [20], [22] for Fe, but for Ni we do not find the
additional structure measured [16] along Γ -X. Since the “optical magnon branch” found for Ni
as a shallow ridge of Im{χ−+ } [14] and also indicated experimentally [16] is most likely due to
interband spin-flip excitations, it is not obtained in our approach. The same is true for similar
but less distinct structures of Im{χ−+ } found in ref. [14] for Fe, which, however, have not been
confirmed in experiment [20].
To describe finite-temperature magnetic properties, we consider the thermodynamics of
magnons. At low temperatures the magnons are the appropriate thermal excitations, the statis-
tics of which is described by the Planck distribution. At elevated temperatures the occupation
numbers and hence the amplitudes hθµqλ i of long-wavelength modes become large. The modes
start to interact both kinematically (deviation from bosonic character) and anharmonically, and
finally the magnon picture is to be replaced by a picture of strong long-wavelength transverse
spin fluctuations. For 3d metals, only above TC longitudinal spin fluctuations may come into
the game and we shall neglect them. We, therefore, divide the temperature scale into two parts,

.
.. ................ .... ........
300

. . ......
Energy (meV)

. .
. . ..
200
. . .
100
. . ..
. . .
.. ...
X W K L W 0 1

Fig. 2. – As fig. 1, but for fcc Ni. The experimental data () are those of ref. [16].
s. v. halilov et al.: magnon spectrum and related etc. 95

M(T)/M(0)
Theory
Expt.

0
0.2 0.4 0.6 0.8
T/TC

Fig. 3. – Temperature-dependent magnetization of Ni given as a function of T /TC . Experimental data

after ref. [23].

i.e. the harmonic regime, with well-defined quantum excitations, and the non-harmonic regime.
In the harmonic regime, the average mode amplitude hθνqλ 2
i is obtained by putting the
2
mode energy (∼ θνqλ ) equal to h̄ωqλnqλ in accordance with the Planck distribution nqλ =
[exp [h̄ωqλ /kB TP ] − 1]−1. The thermal reductionPof the sublattice magnetization is then obtained
as ∆Mν = Mν qλ [1 − hcos(θνqλ )i] ≈ Mν 12 qλ hθνqλ
z 2
i.
At higher temperatures a mean-field approach may be used to evaluate M (T ) using the
force constants and moments of the adiabatic LSDA total-energy expression (1). However,
the mean-field approach has to be applied with caution. As ωmax /TC  1, even for Ni,
the moment dynamics is rather a cluster dynamics up to temperatures well above TC . The
cluster moment is large compared to 1µB , but the interaction with an effective Weiss field
for an ensemble of the clusters J0,c Mc2 will not too much change compared to that of atoms
J0 Ma2 . For this reason we use the Langevin approach instead of the Brillouin one, i.e. hMaz i =
Ma cth [Ma J0 hMaz i/TR] − T /J0 hMaz i. Here, J0 is determined from the Fourier-transformed force
−1
constants J0 = VBZ dq Jq , with VBZ the BZ volume. This describes the dependence of the
hMa i on T at the high temperatures as well as the Curie temperature TC . With respect to TC
z

our treatment results simply in omitting a factor (S + 1)/S, which has been done previously
(see, e.g., [11]).
In fig. 3 we show the temperature dependence of the magnetization of Ni, which we calculated
with the above-given approach, together with experiment [23]. The crossover of the harmonic
and non-harmonic region occurs approximately at TC /2. The present parameter-free calculation
yields an almost perfect agreement with experiment, if the scaled temperature T /TC is used
as variable. The same quality of agreement was obtained for Fe and Co. The theoretical
Curie temperature of Ni itself, however, is calculated here to be 430 K, which is too small
in comparison to the experimental 627 K. For bcc Fe and fcc Co, on the other hand, we do
obtain better agreement: TC (Fe) = 1037 K, TC (Co) = 1250 K, as compared to the experimental
TC ’s of 1043 K and 1388 K [19]. We mention further that our calculated TC ’s correspond to
those obtained recently with other first-principles descriptions of spin-fluctuations [4], [11], [5].
The M (T /TC ) curve calculated in the present approach, however, compares much better with
experiment, particularly at low temperatures, than the recent result of Uhl and Kübler [5]. The
reason for this stems from the fact that we adopt the Planck distribution as the appropriate
statistical description for quantized magnons at low temperatures, whereas in ref. [5] a semi-
classical thermal averaging approach was used. With respect to TC of Ni, we also note that in
all presently available calculations on the basis of the LSDA, TC (Ni) is systematically too small
by about 200 K. Apparently, this is connected to the known deficiency of the LSDA yielding
too small a total-energy difference of only 473 K between the ferromagnetic and paramagnetic
states of Ni.
96 EUROPHYSICS LETTERS

To summarize, we have first shown that magnon spectra can be calculated ab initio within
the framework of the LSDA total-energy formalism. Our ab initio calculated magnon spectrum
of Fe exhibits Kohn anomalies, a novel feature which as yet was not known to exist for
magnons. Experimental investigations by means of high-resolution neutron-scattering mea-
surements would be of urgent interest for the verification of this prediction. Second, we
have proposed a thermodynamical formalism which enables the first-principles description of
those finite-temperature magnetic properties which are related to exchange coupled magnetic
vibrations. As an application, we have calculated the finite-temperature magnetization of Ni
and TC ’s of Fe, Co, and Ni, which are close to experimental data (with the exception of the TC
for Ni). Our results particularly highlight that accurate ab initio studies of finite-temperature
magnetic properties are becoming feasible.

***
This work was supported financially by the State of Saxony under Contract No. 4-7541.82-
MP2/502. One of the authors (SVH) additionally acknowledges financial support by the
Max-Planck Institut für Physik komplexer Systeme.

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