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An insert for anelastic spectroscopy measurements from 80 K to 1100 K

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IOP PUBLISHING

MEASUREMENT SCIENCE AND TECHNOLOGY

Meas. Sci. Technol. 20 (2009) 015702 (5pp)

doi:10.1088/0957-0233/20/1/015702

An insert for anelastic spectroscopy

measurements from 80 K to 1100 K
F Cordero1 , L Dalla Bella2 , F Corvasce1 , P M Latino1 and A Morbidini3
1
CNR-ISC, Istituto dei Sistemi Complessi, Area della Ricerca di RomaTor Vergata, Via del Fosso del
Cavaliere 100, I-00133 Roma, Italy
2
Tecna, Via Novara 6/A, I-43100 Parma, Italy
3
INAF, Area della Ricerca di RomaTor Vergata, Via del Fosso del Cavaliere, 100, I-00133 Roma, Italy

E-mail: francesco.cordero@isc.cnr.it

Received 13 August 2008, in final form 3 October 2008

Published 13 November 2008
Online at stacks.iop.org/MST/20/015702
Abstract
We describe an insert for measurements of the complex elastic moduli between liquid N2
temperature and over 1000 K. The system has been tested with free flexural vibrations of
bar-like samples suspended on thermocouple wires with electrostatic excitation and capacitive
detection of the vibration, providing excellent measurements with elastic energy loss
coefficients between 3 106 and 0.1. The specially designed system for regulating the
distance between the electrode and the sample would also allow optical detection of the
vibration through optic fibers.
Keywords: anelastic spectroscopy, complex elastic modulus, internal friction

1. Introduction

The insert described here has been realized at Tecna

in Parma with subsequent modifications which are still
ongoing. The construction is as simple as possible and
improvements might be made, especially on the heater, but
the simple design described here keeps the costs low, without
preventing top quality measurements to be made. The system
has been tested between 84 and 1150 K, but the lower
temperature may be further lowered by pumping over the
liquid nitrogen (LN2 ) bath, while the highest temperature
might be increased by using an external furnace and a sample
holder of simpler construction avoiding stainless-steel screws
and Macor insulating pieces. The insert has been used
with a sample holder for free flexural vibrations of samples
shaped as bars suspended on thin thermocouple wires and
electrostatically excited, but might be used for different types
of setups, such as clampedfree vibrations, and we will not
concentrate on the holder.

Anelastic spectroscopy, namely the measurement of the

complex elastic moduli of solids, provides information on the
dynamics of point and extended defects, of domain walls,
on phase transformations, and in general on any dynamic
phenomenon coupled to strain [1, 2]. It is the mechanical
analog of dielectric spectroscopy or magnetic relaxation and,
being insensitive to free charges or spins, it may be used to
study defects and excitations coupled with strain irrespective
of the insulating, conducting, magnetic or ferroelectric state of
the material. We will describe an insert for measurements of
the complex elastic moduli from liquid nitrogen to over 1100 K
in vacuum, which is the result of an ongoing evolution of the
anelastic spectroscopy setups developed in the former Istituto
di Acustica O M Corbino of CNR, starting with Professors
P G Bordoni and M Nuovo and continuing with G Cannelli,
R Cantelli and F Cordero. Many concepts of this setup are
therefore based on the previous ones. The only comprehensive
description of such measurement systems is found in [3] (in
French), with emphasis on the electronics for detecting the
sample vibration and various types of sample mountings.
Of course, similar concepts have been employed in other
laboratories [47] with more or less important differences in
the sample mounting and in the electronics.
0957-0233/09/015702+05$30.00

2. Description
The materials are Inconel 601 and 625 for the tubes, lower
flange F3 and main parts of the sample holder, while the
insulating pieces of the holder are made of Macor. The
maximum operating temperature of Inconel 600 is 1250 K
while that of Macor is 1070 K or 150 K higher for short periods
1

2009 IOP Publishing Ltd Printed in the UK

Meas. Sci. Technol. 20 (2009) 015702

F Cordero et al

under reduced load. The insert (figure 1) has an upper DN100

flange (F1) to be fitted onto a DN100 cross (C1) connected
to the high vacuum system. The lowest port of the cross
is connected to a flange (F2) that allows a quartz tube (Q1)
with an external diameter of 90 mm to be applied with an
O-ring and a compression fitting. If the F2 flange also has
another compression fitting for a dewar (D1) with the external
chamber separately evacuatable, then it is possible to pump
over the LN2 bath in order to lower the minimum temperature
at least down to 60 K. In such a case it is safer to insert a spring
between the bottom of the quartz tube and that of the dewar,
in order to prevent the possible fall of the tube when the dewar
is evacuated.
Three Inconel tubes (T1, 10 1 mm) are soldered to
the upper flange F1 and to the lower flange F3, to which the
sample holder (S1) is fixed; their main purpose is to support the
lower flange solidly enough so that the surrounding vibrations
do not result in excessive oscillations of the sample holder. To
this aim, the three pairs of radiation screens (R1) consist of
0.3 mm thick plates, to which tube pieces 10 mm long (R2)
are attached, and can slide on the insert tubes; pieces of Ta
foils are forced between the tube pairs, in order to make the
junctions rigid and improve the stability of the insert against
flexure. The overall length from the top to lower flange is
83 cm. At the top, the tubes terminate with DN10 flanges
(F4) for various electrical feedthroughs. One of them is for
the thermocouples of the sample and of the heater; another
one is used for the electrical leads of the Pt sensor, used to
calibrate the sample thermocouple and normally dismounted.
A third tube is used for the current leads of the heater. The
wires going to the heater run inside the tubes down to 48 cm
from the top flange, and then come out of the tubes through
apertures, since a junction has to be made in the intermediate
zone where the temperature never exceeds 200 C. These wires
together with those for the calibration of the Pt sensor are
2 0.38 mm2 CuNi wires insulated with kapton. The
thermocouple wires of the sample, instead, run down to the
bottom and are insulated with alumina beads. Other types of
ceramic beads should be avoided since they lose oxygen in
vacuum at high temperature and become conductive.
Through the center of the flanges an Inconel rod (E1,
actually a tube 6.35 1.65 mm) is inserted, which supports
the excitation electrode and allows its distance from the sample
to be regulated during the measurement. The regulation
(figure 2) is accomplished by rotating a knob (E2) connected
to a bellows (E3) with ball bearings (E4) and is screwed onto
a fixed part (E5). The top of the bellows has a DN10 flange to
which an electrical feedthrough (E6) with a BNC connector is
fixed, and which supports the electrode rod E1. This design has
been chosen to allow the possibility of detecting the vibration
by means of a bunch of optic fibers instead of the capacitive
method; in this case, a vacuum tight box would be applied to
the DN10 flange, where the optic fibers are terminated with
emitting laser diode and detecting photodiode; no tests have
been carried out with such a system. Note that the knob must
be made of two pieces attached with screws in order to mount
it on a commercial bellows with DN16 flanges. The lower
flange (F3) is 4 mm thick and is soldered to the three tubes T1,

while in the central hole a flange (F5) is fixed with nuts and
contains two insulating Macor spacers (F6) for maintaining
the electrode rod in a central position; additional holes serve
for attaching the sample holder S1, and four threaded lateral
holes allow the heater to be tightly fixed with M2 screws
(H5). Note that Macor starts becoming conductive above
1000 K; therefore, the cylinders F6 should be combined with
or substituted by alumina cylinders, when working at such
high temperatures.
2.1. The heater
The heater (H1) is made of a 0.3 mm thick Inconel sheet
spot welded to obtain two concentric cylinders sandwiching a
Thermocoax heater (H2) and a chromelalumel thermocouple;
the bottom is closed with a disc from the same sheet. The
Thermocoax with a resistance of 6 ! has an Inconel 600
sheath with 2 mm diameter, a heated part 200 cm long coiled
within the two cylinders plus cold terminals 25 cm long and
cylindrical connectors where the terminals of the current leads
are inserted and pressed with lateral screws. The maximum
temperature that the heater can withstand is 1220 K. The
junction of the thermocouple is fixed at half the height of
the heater, roughly in correspondence with the sample. The
coils of the heater are roughly equispaced, without a particular
study for minimizing the temperature gradients between parts
at different heights and with different heat capacities, although
care has been taken to minimize the masses of all parts while
keeping the structure solid. In fact, the smaller the heater mass
the faster is the cooling to LN2 .
The heater reaches its limit temperature of 1220 K already
by applying 50 V; it is fed by a dc power supply Genesys
Lambda 080 Vdc 09.5 A controlled by a Eurotherm 2604.
Controllers that simply switch on and off a constant current
should be avoided, since at temperatures above 600 K the
variation of heating power during the controller cycle affects
the sample temperature. This becomes a major problem
when measuring phase transitions with steep variation of
the elastic moduli versus temperature; in such cases the
power fluctuations produce changes in the sample resonance
frequency, which in turn give rise to fluctuations of the
vibration amplitude.
In order to reduce the temperature gradients and heat
losses at high temperature, the quartz tube is surrounded by an
insulating box 210 210 440 mm3 into which Carbowool
sheets of 10 mm thickness are fitted (D2). When cooling
below 400 K, the box is lowered and substituted with a liquid
nitrogen dewar (D1).
2.2. The sample holder
The sample holder (S1) that has actually been used with the
present insert is for flexural vibrations of bars 2355 mm
long, 35 mm wide and 0.21.5 mm thick suspended on thin
thermocouple wires and electrostatically excited. Although
the prototype holder allowed excellent measurements to be
made, it is under continuous modification and is still difficult
to use, especially regarding the substitution of the thin
thermocouple wires and the regulation of their parallelism to
2

Meas. Sci. Technol. 20 (2009) 015702

F Cordero et al

Figure 2. Detail of the upper flange with the system for regulating
the electrode vertical position.

electrode (E7) is regulated; this is necessary since during the

temperature ramps the length of the long rod (E1) changes
with respect to that of the tubes T1, even if the electrode
rod is not inserted into a central tube, to avoid excessive
temperature gradients between it and the tubes. The sample
(S5) is fixed to the thermocouple suspension wires (S6) with
drops of conductive paint, to improve the mechanical stability
and the electrical contact with the thermocouple (note that in
figure 3 the longest edges of the sample are perpendicular
to the page). If the sample is not conductive, its upper
face is completely covered with conductive paint, in order
to allow the electrostatic excitation through the electrode
(one of the thermocouple wires is grounded) and to close
the thermocouple circuit. In addition, the thermal gradients
along the sample are minimized. Note that Ag paint is
definitely cheaper and more convenient than Pt paint, but
above 850 K in vacuum Ag starts evaporating and depositing
on the cooler parts of the insert, and one is bound to use Pt
paint. The thickness of the conductive layer must be such that
the resistance between the two suspension wires is not more
than few ohms; a thicker layer may also be applied in order to
protect the sample when accidental sparks are formed between
the sample and the electrode. The evaporation of the solvent
and curing of the conductive layer causes additional elastic
energy dissipation during the first heating (up to 500 K for
Ag paints), but afterward no contributions to the elastic losses
are noted.
The thermocouple wire is thin (0.025 mm diameter)
only in the sample region, and is joined to the thick one
(0.5 mm diameter) by pressing the wires against each other

Figure 1. General view of the insert.

each other; therefore it will not be described in detail here. We

will just mention that the suspension wires are maintained in
tension by the cantilever L pieces (S2) with variable number
of counterweights (S3). This method gives very good results
and elastic energy loss coefficients from 3 106 to 0.1 have
been measured. The distance between the wires is always
regulated at 0.55 times the sample length, corresponding to
the nodes for the first and fifth free flexural vibration modes
[1]. The parallelism between the sample and the electrode
is very important in order to maximize the sampleelectrode
capacity; it is achieved through the nuts (S3) that regulate
the position of the holder plate (S1) with respect to the fixed
plate (S7). During the measurement, only the height of the
3

Meas. Sci. Technol. 20 (2009) 015702

F Cordero et al

Figure 4. Elastic energy loss coefficient, Q1 = E /E , and

relative variation of the Youngs modulus, E , of a hydrated sample
of BaCe0.85 Y0.15 O3 , measured on fast heating and on cooling. The
insert shows an enlargement of the Q1 curves, which coincided
even if the heating rate reached 10 K min1 .

3. Test of the apparatus

Figure 3. Lower part of the insert with heater and sample holder.

Over 100 measurements have been done up to now with

the described insert, 40 of them at temperatures above 700
K, and no major deterioration of the setup occurred yet;
even the stainless-steel screws have never been changed.
The measurements can be made in vacuum in the whole
temperature range, but cooling below 400 K at a reasonable
rate requires the introduction of some He as exchange gas
within the quartz tube. The sample is fixed to the thermocouple
wires with drops of conductive paint in correspondence with
the nodes for the first and fifth flexural modes, which are
nearly coincident at 0.225l from the sample ends; sometimes,
also the third mode may be measured in such a configuration.
This is especially useful when measuring anelastic spectra
with high dissipation values, where the excitation of the fifth
mode becomes problematic or impossible, and the fact that
the sample is not fixed at the nodes of the third mode is of
minor importance. Therefore, when the dissipation is low,
the first and fifth modes are measured with the third one
generally producing double or multiple resonances. When the
dissipation is high and the width of the multiple resonances
becomes broader than their separation, the third mode can also
be reliably measured.
The major problem is the minimization of temperature
gradients; in fact, the thermal conductivity of the ensemble
is rather low and the contacts between the heater coil and
walls and between the latter and the lower flange are poor. In
addition, the electrode is very close to the sample surface
and its temperature during ramps lags behind that of the
less massive sample. As a result, the temperature difference
between the center and the ends of an insulating sample may
exceed 10 K during fast cooling or heating. The problem may

between insulating Macor pieces with a screw and a spring

washer. All the threads and moving parts are covered with
the lubricating MoS2 Molikote powder to prevent gripping at
high temperature. In order to avoid excessive dispersion of the
powder, the latter may be applied with a brush after dispersing
it into alcohol. Before using the equipment for the first time,
all the hot metal parts must be heated in vacuum in order to
let them evaporate any impurities that would contaminate the
sample and the insulating ceramics parts.
2.3. The measurement method
The vibration is detected through a frequency modulation
method that has been described in earlier literature [3]. In brief,
the sampleelectrode capacitor is part of a high frequency
resonating circuit, whose resonance frequency f0 10 MHz is
modulated by the sample vibration; the frequency modulation
is in turn transformed into amplitude modulation by means of
a resonating circuit accorded through a variable capacitor in
order that one of the sides of its resonance curve corresponds
to f0 . The resulting signal is rectified and sent to a lock-in
amplifier for the detection of the vibration amplitude. The real
part of the elastic Youngs modulus E , or of its reciprocal,
the elastic compliance s , is measured from the resonance
frequency; in the case of free flexural vibrations through
the relationship E = (0.973f l 2 / h)2 where , l, h and f
are the density, length, thickness and fundamental resonance
frequency of the sample, respectively. The elastic energy loss
coefficient Q1 = E /E = s /s is measured from the free
decay of the vibration after switching off the excitation or from
the width of the resonance curve when the decay is too fast or
short.
4

Meas. Sci. Technol. 20 (2009) 015702

F Cordero et al

Figure 5 presents a measurement on the first and fifth

flexural modes of a crystal of SrTiO3 with the 100
directions parallel to the edges, so that the measured
compliance is s11 . The thermally activated peaks (shifted
to higher temperature at higher frequency) above 200 K are
related to O vacancies, while the steep rise of the compliance
below 97 K is the antiferrodistortive transition to the tetragonal
phase [9]. The purpose is to show that at least four full orders
of magnitude of the elastic energy loss, from 3 106 to
3 102 in this case, can be measured at both frequencies
even on a sample with non-optimal shape (only 26 mm long
and with slightly irregular cuts).

4. Conclusion
A relatively simple and cost effective insert for the
measurement of the elastic moduli between liquid nitrogen
and at least 1150 K has been presented. The heater might
be improved, e.g., by increasing the length of the heated
part and the number of windings and by improving the
thermal contact with the walls of the shield; yet, the thermal
gradients constitute no problem if the sample is conductive or
is made such with conductive paint. It is shown that reliable
measurements can be obtained even at heating rates as fast as
10 K min1 , at least as far as the measurement of temperature
is concerned. It is also shown that elastic energy losses over
a range of at least four orders of magnitude can be reliably
measured.

Figure 5. Elastic energy loss coefficient, Q1 = s /s and relative

variation of the compliance of a crystal of SrTiO3 , measured on
the first and fifth flexural modes.

be solved by applying conductive paint over the whole upper

surface of the sample. The best test is the comparison between
curves measured on heating and cooling, since in the two
cases the temperature gradients within the insert and especially
in the sample and thermocouple wires are opposite, and any
inaccuracy in the temperature measurements would appear as
a shift of the curves with respect to each other. Figure 4 shows
a measurement of a hydrated sample of BaCe0.85 Y0.15 O3 ,
where the peaks in Q1 (T ) at room temperature and below
are due to H motion [8], while the kink in the Youngs modulus
E near 500 K is due to a structural phase transition.
The continuous line is a measurement taken on cooling
at 0.7 K min1 , while the empty circles are measured
on subsequent heating at a very fast rate, between 4 and
10 K min1 , therefore in the presence of very strong
temperature gradients. The Q1 (T ) curves are perfectly
coincident (see the enlargement in the inset), while there is
a hysteresis of nearly 5 K between heating and cooling in
the E(T ) curves, due to the first-order nature of the phase
transformation. It can be concluded that the application of
a conductive layer is sufficient to neutralize the effect of the
temperature gradients present in the insert.

References
[1] Nowick A S and Berry B S 1972 Anelastic Relaxation in
Crystalline Solids (New York: Academic)
[2] Schaller R, Fantozzi G and Gremaud G 2001 Mechanical
Spectroscopy Q1 2001 (Totton, UK: Trans Tech
Publications)
[3] Nuovo M 1961 Ric. Sci. 31 212
[4] Simpson H M and Sosin A 1977 Rev. Sci. Instrum. 48 1392
[5] Weller M and Torok E 1987 J. Physique 48 C8371
[6] Coluzzi B, Biscarini A and Mazzolai F M 1996 Rev. Sci.
Instrum. 67 4240
[7] Bonetti E, Campari E G, Pasquini L and Savini L 2001 Rev. Sci.
Instrum. 72 2148
[8] Cordero F, Craciun F, Deganello F, La Parola V, Roncari E and
Sanson A 2008 Phys. Rev. B 78 054108
[9] Cordero F 2007 Phys. Rev. B 76 172106