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Acoustic study of low-energy activation processes in magnetic rare-earth glasses : amorphous holmium
aluminosilicates
F. Lerbet, G. Bellessa
To cite this version:
F. Lerbet, G. Bellessa. Acoustic study of low-energy activation processes in magnetic rare-earth glasses : amorphous holmium aluminosilicates. Journal de Physique, 1987, 48 (12), pp.2111-2118.
�10.1051/jphys:0198700480120211100�. �jpa-00210659�
Acoustic study of low-energy activation processes in magnetic rare-earth glasses : amorphous holmium aluminosilicates
F. Lerbet and G. Bellessa
Laboratoire de Physique des Solides (*), Bâtiment 510, Université Paris-Sud, 91405 Orsay, France
(Requ le 17 juillet 1987, accept6 le 25 août 1987)
Résumé.
2014Nous présentons une étude acoustique de verres d’aluminosilicates de différentes teneurs en
holmium. Les mesures sont faites jusqu’à 100 mK, dans le domaine de fréquences 10-500 MHz et dans des
champs magnétiques compris entre 0 et 60 kOe. Nous observons un pic de l’atténuation en fonction de la
température qui suit une loi d’Arrhenius et qui est sensible au champ magnétique. Nous observons aussi un
petit pic d’atténuation dont la localisation en température ne dépend ni de la fréquence acoustique ni du champ magnétique. Associée au premier pic, une variation de la vitesse du son est observée. Le pic d’activation et la variation de vitesse associée sont bien interprétés dans le contexte de la relaxation par des processus d’activation de systèmes magnétiques à deux configurations. Grâce à l’étude en fonction de la concentration,
nous établissons que ces systèmes ne sont pas les mêmes que ceux observées par d’autres auteurs dans la phase
verre de spin et sont certainement beaucoup plus légers. Nous considérons le modèle d’anisotropie aléatoire
des alliages de terres rares, pour expliquer nos effets.
Abstract.
2014An acoustical study of aluminosilicate glasses with various holmium contents is reported. The
measurements are performed down to 100 mK, in the frequency range 10-500 MHz and in a magnetic field up to 60 kOe. An attenuation peak as a function of the temperature following an Arrhenius law and depending on
the magnetic field is reported. Another small attenuation peak depending neither on the acoustical frequency
nor on the magnetic field is also reported. Connected with the first peak, a sound velocity variation is observed. The activation peak and the connected sound velocity variation are well explained in the framework of the relaxation of two-configuration magnetic systems by activation processes. Thanks to the acoustical study
as a function of the holmium content, we show that these systems are certainly not the same as those observed
by other authors in the spin glass phase and are much lighter. The random anisotropy model of the rare-earth
alloys is considered to explain the observed effects.
Classification
Physics Abstracts
63.20M - 75.50K
-63.50
1. Introduction.
Ultrasonic measurements in metallic spin glasses
have revealed a small dip in the sound velocity near
the freezing temperature [1, 2]. An effect of the
magnetic field on the thermal conductivity of spin glasses has been observed [3, 4]. These authors
proposed that this effect should arise from thermal activation of magnetic clusters. In insulating spin glasses we have reported an acoustical study which
revealed an activation process non-connected with the spin freezing but rather with the reversing of the magnetic ions on their anisotropy axis [5]. Sub- sequently, other acoustical measurements have been
reported [6]. They have been interpreted in terms of dipolar and quadrupolar freezing [7].
We report an acoustical study of aluminosilicate
glasses doped with holmium ions at different concen-
trations. Our preliminary measurements already published were for a concentration of 10 % at. [5].
The low-temperature magnetic study of Chappert et
al. [8] has shown that for this concentration, this insulating amorphous material exhibits a spin glass
behaviour. Hence, it is interesting to vary the
magnetic-ion concentration, mainly below 10 %
(12 % is the concentration from which nearest neigh-
bours appear in a cubic lattice and the interaction between the magnetic moments is dipolar). The
atomic holmium concentrations studied are 10.1 %,
6.7 %, 3.4 % and 1.5 %. The acoustic measurements have been performed down to 100 mK’ and in the
frequency range 10-500 MHz.
In this paper, we do not consider the effects on the acoustic wave of the tunneling states which always
Article published online by EDP Sciences and available at http://dx.doi.org/10.1051/jphys:0198700480120211100
2112
exist in the amorphous matter [9, 10]. They give rise
in our samples to a logarithmic temperature depen-
dence of the sound velocity and to an acoustic
attenuation variation at the lowest temperatures [5].
A detailed study of these effects are reported
elsewhere [11, 12].
2. Experimental procedure.
The samples studied are aluminosilicate glasses doped with rare earth ions. The ion which interested
us was the Ho3 + magnetic ion. It is easy to obtain
good glasses for a holmium content of 10 % [8]. But,
if one tries to decrease this one, it is no longer possible to obtain a glass from the liquid phase. In
order to overcome this difficulty, we have kept
constant (and equal to 10.1 %) the rare earth ion
content and partly replace the Ho3 + ions by La3 + ions, which are not magnetic. Thus, the
different compositions studied are :
1.5 % at. Ho :
The 10.1 % Ho sample exibits a spin glass behaviour
with a freezing temperature around 0.5 K [8].
The ultrasonic study was made by sending acoustic
wave pulses of various frequencies (10 MHz-
500 MHz) through the samples. The experimental apparatus is phase sensitive and allows measure- ments on both acoustic attenuation and relative variation of sound velocity (with an accuracy better than 10-6 for a reasonnably good signal-to-noise ratio). The very good precision on the ultrasonic attenuation at 10 MHz ( = 10- 3 dB/cm) has been
obtained by studying the n-th echo, in order to lengthen the acoustic path.
The samples are parallepipeds (10 x 4 x 4 mm).
They are cooled in a dilution refrigerator which
works down to 8 mK. A superconducting magnet
can produce a field up to 60 kOe. Its homogeneity is
better than 1 x 10- 5 in the whole sample. The thermometry at low temperatures and high fields has
been achieved with a carbon resistor [13] and a capacitive sensor. At 0 kOe we use also a germanium
resistor in the temperature range 50 mK-10 K.
3. Experimental results : activation processes.
3.1 10.1 % HO GLASS IN ZERO MAGNETIC FIELD [5].
The variations of the ultrasonic attenuation in this
sample as a function of the temperature are shown in figure 1, for different frequencies. A well resolved
peak on the attenuation at 10 MHz clearly appears.
Fig. 1.
-Attenuation variation of longitudinal acoustic
waves as a function of the temperature for various
frequencies and without magnetic field in the 10.1 % Ho
sample. 0 : f = 10 MHz ; * : f= 60 MHz ; + : f =
210 MHz ; x : f = 480 MHz. The vertical scale is arbitrary
and different for every curve.
It becomes a shoulder and its location shifts towards the high temperatures at higher frequencies (between 10 MHz and 480 MHz). Obviously, there
is superposed on these peaks another attenuation variation. The latter arises from the relaxation of the
tunnelling states which exist in our samples [5].
Using the theory [14] and the parameters of the
Fig. 2.
-Attenuation variation of longitudinal acoustic
waves as a function of the temperature at 10 MHz and without magnetic field in the 10.1 % Ho sample. The
asterisk line is the expected attenuation variation due to
the tunnelling states (see text).
tunnelling states in our samples [12], we have displayed in figure 2 the expected attenuation vari- ation. The attenuation peak appears clearly upon this curve (Fig. 2). Our analysis cannot be conducted
at all the frequencies because another contribution appears at higher temperatures (T > a few K) and is
more important at higher frequencies. We can despite this fact, extract a peak at all the frequencies
from the « natural » curve which is also deduced from the results at high magnetic fields (see below).
The variations of the location temperature and of
the amplitude of the peak as a function of the frequency are shown in figure 3 and figure 4, respect- ively. They are easily interpreted in the framework of the relaxation of two-configuration systems (TCS) by activation processes [14, 15]. In this model each system characterized by a barrier V and an asymme- try E interacts with the elastic wave of frequency jf2/2 7T and one calculates the attenuation and the variation of sound velocity using the equations :
where To is a characteristic time. T follows the Arrhenius law of the activation processes and r
depends on the density of states of the TCS and on
their coupling with the elastic strain. r is often called the relaxation strength. We can deduce from these
equations, neglecting the distribution g (V), the
location temperature and the amplitude of the peak :
Fig. 3.
-Location temperature of the activated peak as a
function of the frequency for two magnetic fields. 0 : H = OkOe; +: H= 5k0e.
Fig. 4.
-Amplitude variation of the activated peak with-
out magnetic field as a function of the frequency.
and
Our results can be interpreted in the framework of this model. Hence, we obtain :
In fact, the description with only one barrier height
is not satisfying with regard to the width of the peak
which is better (but not perfectly) fitted with a
constant distribution of barriers between 2 K and 8 K. In this case the Arrhenius law is still followed in
our frequency range 10 MHz-480 MHz. Since the basic line is not perfectly known, there is no more meaning to search for a better fit of the attenuation
peak, with unknown parameters. However, a broad distribution of relaxation times is not surprising in glasses [16-19] and does not change fundamentally
our interpretation.
According to equation (2), there is a variation of the sound velocity correlated with the attenuation
peak. However, the experimental results are more
2114
difficult to interpret due to another source of vari-
ation for the sound velocity [5]. Nevertheless, in figure 5 which displays the variations of the sound
velocity at 110 MHz, it appears a diminution of the
velocity around the peak temperature Tp, as ex- pected from equation (2) [5]. The relaxation
strength r’ deduced from figure 5 using equation (2)
and assuming an additional logarithmic variation,
is :
It agrees very well with the one obtained from the attenuation peak.
Fig. 5.
-Relative velocity variation of the acoustic waves as a function of the temperature at 110 MHz without
magnetic field in the 10.1 % Ho sample. The solid line is
only a guide for the eyes. Tp is the location temperature of the attenuation peak for the same frequency.
3.2 10.1 % Ho GLASS IN MAGNETIC FIELD [5].
-We
have observed an attractive effect, which is the
displacement of the attenuation peak induced by a magnetic field. The attenuation peak (and correla- tively the characteristic variation of the sound vel-
ocity) shifts towards the high temperatures as the magnetic field increases (Fig. 6). Restricting us to
the range [0-10 kOe], where the deformation of the attenuation peak is not too large, we show this shift at 10 MHz. In figure 6, the vertical shifts of the
curves are arbitrary for a clearer display, but we can experimentally adjust them with respect to each other, since we are able to measure for the same temperature and frequency the variations of the attenuation (and of the sound velocity) as a function
of the magnetic field. Thus, can we find a right basic
line for the results without magnetic field as it is
shown in figure 7. The variations of the ultrasonic attenuation for two different magnetic fields at
110 MHz are shown without any arbitrary shift with respect to each other. Since the attenuation is the
same for the two magnetic fields above 4 K, the
Fig. 6. - Attenuation variation as a function of the temperature at 10 MHz for different magnetic fields in the 10.1 % Ho sample. The vertical shifts of the curves with respect to each other are arbitrary for clarity. 0 : H
=0 kOe ; * : H
=5 kOe ; x : H
=10 kOe.
disappearance of the activation peak as the high magnetic field is set up, is obvious in figure 7 (we
shall consider later the attenuation peak which
appears at low temperature in high magnetic field).
Fig. 7. - Attenuation variation as a function of the temperature at 110 MHz for two different magnetic fields
in the 10.1 % Ho sample. Here, there is no arbitrary
vertical shift of the curves. 0 : H
=0 kOe ; * : H
=60 kOe.
If we restrict now our study to a single relaxation time, we can perform the same analysis as in paragraph 3.1, but for various magnetic fields be- tween 0 kOe and 10 kOe. For all the magnetic fields,
we have found that the peak follows an Arrhenius
law with the parameters :
The first remarkable result is that To does not change
with the magnetic field (Fig. 3). This means that the
wells neither change. The shift of the attenuation
peak towards the higher temperatures (Fig. 6 and Fig. 3) has to be interpreted as an increase of the barrier height. This one increases linearly with increasing magnetic field up to 10 kOe (Fig. 8). If we
write a
=Kgj Jg B, using the values of the Ho3 + ion
(J = 8 and gj = 1.25), we find that K - 1. This result will be examined below.
Fig. 8.
-Activation energy of the peak as a function of
magnetic field.
3.3 Ho GLASSES AT 0 k0e AND LOWER CONCEN- TRATIONS.
-We have extended our study with the
concentration of magnetic ions from a rather concen-
trated regime (10.1 % at. ; at this concentration there is a spin glass behaviour with a freezing temperature around 0.5 K [8]) to a more dilute one ( = 1.5 %). The other concentrations studied are :
6.7 %, 3.4 %, 1.5 %. We may believe, that with decreasing the magnetic-ion content the freezing temperature decreases strongly, since the ion interac- tion is dipolar. Thus, we can check whether the attenuation peak here reported is directly connected
with the spin glass phase or not. It is this last hypothesis we have made previously [5].
Figure 9 displays the ultrasonic attenuation in two
Fig. 9.
-Attenuation variation as a function of the temperature at 110 MHz without magnetic field and for two Ho contents. The solid lines are only guides for the
eyes. 0 : cHo
=0.101 ; * : cHo
=0.067.
aluminosilicate glasses with a holmium content of
6.7 % and 10.1 % respectively, at the same frequency (110 MHz). Whereas the phenomena related to the
T9 are certainly moving towards the lower temperat-
ures for this diminution of Ho content, it appears that the peak temperature does not change and that
the peak amplitude decreases. In view of the natural basic line, the peak amplitude is :
/-1 (10.1 %) = 0.8 X /-1 (6.7 %) .
At lower concentration, the attenuation peak is no longer clearly discernible due to its decrease and also to the large increase of the effect of the tunnelling
states on the acoustic propagation which changes significantly the basic line [12]. Nevertheless, as it
can be seen in figure 10, the correlated effect on the
Fig. 10.
-Relative variation of the sound velocity as a
function of the temperature without magnetic field and for different Ho contents. The solid lines are only guides for
the eyes. The arrow points the location temperature of the attenuation peak. V : cHo
=0.101, f
=110 MHz ; 0 :
cHo
=0.067, f = 110 MHz ; * : cHo
=0.034, f
=60 MHz.
2116
sound velocity (Eq. (2)) is still present in the 3.4 % Ho glass. Its temperature location does not change perceptibly and the amplitude of the effect decreases with decreasing concentration from 10.1 % to 3.4 %.
This confirms that the activation processes here
reported have energies which do not vary sensibly
between 10.1 % and 3.4 % and are not directly
connected with the spin glass phase [5].
4. Non-Arrhenius attenuation peak [5].
Another interesting experimental observation is the appearance of a second peak at a lower temperature
(T -- 370 mK) when a magnetic field is set up. One
can see it in figure 7. Its main features are :
- The location temperature of the peak does not change with the frequency, the magnetic field and
the Ho3 + content. The independence of this tem- perature with respect to the acoustical frequency
excludes Arrhenius processes.
- The peak amplitude increases with the fre- quency, the magnetic field and the Ho3 + content.
We have displayed in figure 11 this attenuation
peak at 470 MHz and 60 kOe (the experimental
Fig. 11. - Attenuation variation as a function of the temperature at 470 MHz and 60 kOe for different Ho contents. The solid lines are only guides for the eyes. x : CH.
=0.101 ; V : CH.
=0.067 ; 0 : CH.
=0.034 CHo
=0.015.
conditions which give the largest peak), for different holmium contents. It vanishes at low concentration of holmium and its location temperature does not change sensibly with varying the concentration. The correlated effects on the sound velocity, if they exist,
are hidden by the rather complicated behaviour of the sound velocity in high magnetic field [5].
Although it is obvious that this peak is due to the magnetic ions, we have presently no satisfactory explanation for it.
5. Discussion on the activation processes.
We have seen that the main attenuation peak and
the correlated effect on the sound velocity can be interpreted with activated processes involving mag- netic entities. The activation barriers are low (height
=