Thermal Expansion
Thermal Expansion
Thermal Expansion
1. INTRODUCTION
Silicon is an ideal reference material for thermal expansion measurements,
because it is isotropic in thermal expansion owing to its diamond-like crys-
tallographic structure and because it is readily available in an ultra-pure
1
Thermophysical Properties Section, National Metrology Institute of Japan, AIST, 1-1-1
Umezono, Tsukuba, Ibaraki 305-8563, Japan.
2
To whom correspondence should be addressed. E-mail: [email protected]
3
International Affairs Department, AIST, 1-1-1 Umezono, Tsukuba, Ibaraki 305-8563,
Japan.
221
addition, there was a possibility that the HTPRT was so long (30 mm in
length) that sufficient temperature uniformity within the sensor could not
be attained. As a result, we could not determine a(T) of silicon below
700 K using LID 2, and the absence of the data below 700 K influences the
reliability of our previous data measured using LID 2.
The objective of the present work is to determine reliable data for
linear thermal expansion coefficients of silicon in the temperature range
293 to 1000 K. This work is a part of a project to establish reference
materials for measurements of thermal expansion of solids. To reduce the
temperature difference between the sample and thermometer, the mea-
surements were undertaken with the sample in helium at an appropriate
pressure. The temperature measurements were corrected for the residual
temperature difference between the sample and thermometer. The sample
temperatures were measured using an elemental thermocouple of which the
achievable accuracy was comparable to that of the HTPRT to avoid the
possible error associated with the size of the thermometer sensor. In addi-
tion, a detailed evaluation of experimental uncertainty was carried out.
2. EXPERIMENTAL
The present interferometric dilatometer (LID 3) was almost the same
as LID 2 [5]. Therefore, we describe here an outline of the measurements
and differences from the operations of LID 2.
In the present work, values of a(T) were calculated by applying
Values of DL, DT, and L 0 were measured with a heterodyne laser Michel-
son interferometer, a gold versus platinum (Au/Pt) thermocouple, and a
linear gauge, respectively. Details of the optical system of the interferom-
eter are described in our previous papers [5–7]. The interferometer
employed a double-path system so that
DL=
l Dhp
4 2p
1 2
, (3)
224 Watanabe, Yamada, and Okaji
where l is the wavelength of laser in the furnace and Dhp is the difference in
the phase of the beat signal for optical heterodyne interferometry measured
on changing the temperature from Tn to Tn+1 .
Two samples of single-crystal silicon in which the crystallographic axes
are oriented in [100] and [110] directions were prepared from an ingot
made using a floating-zone method, which is the same batch as that inves-
tigated in our previous works [3, 5]. Each sample was in the form of a
perpendicular block whose size was 10 mm × 7 mm × 20 mm. The (7 × 20)
surfaces were polished to be flat to within one tenth of a wavelength of
632.8 nm and parallel within 5 arc s. The sample was placed on the flat
base plate, which was also made of single-crystal silicon. The mirror face of
the base plate was polished as was that of the sample. A hole having a
diameter of 4 mm was bored down the symmetry axis through the optical
flats of the sample and the base plate.
The Au/Pt thermocouple consisted of gold and platinum wires having
a diameter of 0.25 mm and an insulation tube made of alumina. The
thermocouple was encased in a fused-quartz tube of 3 mm in diameter, and
it was inserted into the hole of the sample. The equation used to compute
the temperature was deduced from the standard reference function given in
ASTM E 1751, the thermocouple calibration at the metal freezing points of
zinc, aluminum, and silver, and the correction for the temperature differ-
ence (Ds ) between the sample (Ttrue ) and the thermocouple (Texp ). Ds as a
function of temperature was experimentally estimated using a ‘‘dummy’’
silicon sample with a differential thermocouple consisting of two platinum
and one platinum-13 mass% rhodium alloy wires, and a type R thermo-
couple in a mineral-insulated, metal-sheathed (MIMS) configuration.
Figure 1 shows a schematic diagram of the arrangement of the dummy
sample and thermocouples to measure Ds and T. The dummy sample had
two extra holes into which the MIMS thermocouples were inserted. To
attain good thermal contact, the diameter of the holes was made almost the
same as that of the metal sheath (1.6 mm). The following correction func-
tion was given by four repeated measurements of Ds in the temperature
range 293 to 1100 K:
Ds (T)=−0.070+0.00108(T − 293), (4)
which was used to compensate for Ds in the measurements of a(T).
The measurements of a(T) were made while the sample was heated
or cooled successively to constant temperatures between which there were
temperature intervals of approximately 50 or 25 K. In order to improve
thermal contact between the sample and thermocouple, an amount of
helium gas at a pressure of 80 Pa and a temperature of 293 K was sealed
in the furnace. After one measurement cycle of heating to approximately
Linear Thermal Expansion Coefficient of Silicon 225
1050 K and then cooling to 293 K, the gas pressure at 293 K increased by about
30 Pa as a result of gas evolution from the furnace wall. Taking into account the
gas evolution resulting in the pressure increase from 80 to 110 Pa, we con-
sidered the average amount of helium gas during the experiment to be that at
a pressure of 95 Pa and a temperature of 293 K. Thus, the value of l was
calculated to be 632.991 nm using the refractive index of helium gas at 95 Pa
and 293 K. The temperature of the sample changed at a rate of less than
1.7 × 10 −2 K · s −1 from one constant temperature to the next one. The tempera-
ture was kept at each of the temperature steps for a time period longer than
3.6 × 10 3 s to attain thermal equilibrium. The optical window of the furnace was
in contact with a brass plate whose temperature was kept constant using two
thermoelectric transducers in order to reduce the uncertainty due to the tem-
perature distribution within the window through which the laser beams pass.
3. RESULTS
Figure 2 shows the experimental results for a(T) for the two silicon
samples. For each sample, the measurement in the temperature range 293
to 1025 K was repeated six times; three runs were carried out during
heating and cooling, respectively. All of the data were pooled, and the
following fifth-order polynomial function of temperature was obtained by
the method of least squares: at 293 [ T [ 1025
The standard deviation of this fit is 1.1 × 10 −6 with 204 data points.
Linear Thermal Expansion Coefficient of Silicon 227
4. DISCUSSION
where d(DL), d(DT), and dL 0 are the standard uncertainties of DL, DT,
and L 0 , respectively. The magnitudes of uncertainties in Table II were
estimated under the measurement conditions that DT was 50 K, L 0 was
10 mm, a was calculated from Eq. (5) at 1000 K, and DL was given by
On the other hand, the relative combined standard uncertainty (de/e) listed
in Table III is calculated by using
DL=eL 0 . (10)
Measurement conditions
Relative
Original Probability uncertainty
Uncertainty source Type uncertainty distribution Divisor (%) Uncertainty
da/a b
Combined standard uncertainty 0.556 2.41 × 10 −8
Expanded uncertainty (k=2) 1.11 4.82 × 10 −8
a
DL=aL 0 DT.
b
da/a=`; {d(DL)/DL} 2+; {d(DT)/DT} 2+; (dL 0 /L 0 ) 2.
230 Watanabe, Yamada, and Okaji
Table III. Uncertainty Budget of Linear Thermal Expansion, e, for Silicon at 1000 K
Measurement conditions
Relative
Original Probability uncertainty
Uncertainty source Type uncertainty distribution Divisor (%) Uncertainty
de/e b
Combined standard uncertainty 0.126 3.37 × 10 −6
Expanded uncertainty (k=2) 0.252 6.75 × 10 −6
a
DL=L − L 0 =eL 0 .
b
de/e=`; {d(DL)/DL} 2+; (a dT/e) 2+; (dL 0 /L 0 ) 2.
Linear Thermal Expansion Coefficient of Silicon 231
of the wavelength was estimated to be 2.53 × 10 −16 m, which was the stan-
dard deviation of the measured wavelengths from the mean. The instability
of the refraction index of the helium gas in the furnace was caused by the
gas evolution from the inside wall of the furnace. The standard uncertainty
of the laser wavelength due to the change in the refraction index was esti-
mated to be 3.32 × 10 −15 m from the observed pressure change from 80 to
110 Pa after one cycle of heating and cooling. The relative uncertainties
due to the first and second sources are calculated as follows:
d(DL)/DL=dl/(ld), (11)
where dhm is the tilt angle between the sample top surface and the base
plate in radians. The double-path interferometer considerably reduces the
requirement of the parallelism, because the incident and reflected laser
beams are maintained mutually parallel even in the case where there is tilt
of the optical system or nonparallelism between the top and bottom surfa-
ces of the sample [8]. However, the value of dhm in the present work was
limited to 1.88 × 10 −3 rad (0.108 deg) based upon the following inequality:
where l was the distance (600 mm) between the sample and the cube corner
prism used to return the laser beams to the sample, DLB was the diameter
(3 mm) of the laser beams, and DPD was the diameter (6 mm) of the cir-
cular sensing area of the photodetector. The left side of the inequality
equals the distance by which the nonparallelism of dhm makes the reflected
beam shift from parallel. The interference signal dissipates if the distance
becomes greater than that given by the right side of the inequality. There-
fore, the relative uncertainty due to the third source was calculated by
substituting the upper limit of dhm into Eq. (12) on the assumption that the
probability distribution was a rectangular one.
The fourth uncertainty is associated with the uncertainty of the mea-
surement of the phase (hp ) of the beat signal with the lock-in amplifier used
232 Watanabe, Yamada, and Okaji
in the present work. The magnitude of the fourth original uncertainty (dhp )
was reported as 1.75 × 10 −2 rad (1 degree) from the manufacturer of the
lock-in amplifier (SRS, Model SR830). The phase shift (Dhp ) correspond-
ing to DL is obtained by the two determinations of hp , and thus dhp mul-
tiplied by `2 equals the uncertainty of Dhp . Therefore, the relative uncer-
tainty is calculated using
d(DL)
DL
=
`2 l dhp
d DL 4 2p
. 1 2 (14)
was repeated two times during heating and cooling. The value of the
original uncertainty was calculated as follows:
where dL A and SA were the respective average values of the instability and
the magnitude of the zero drift obtained during the four measurement runs.
identical to the uncertainty due to the resolution of the linear gauge (Sony,
Model DZ521).
uniformly heat the bulk sample and thermometer using radiant image fur-
naces. A fairly large temperature difference between the sample and ther-
mometer or a serious nonuniformity in temperature within the sample
would exist in the measurement. Compared to the Au/Pt thermocouple
and HTPRT, type R thermocouples are sufficiently sensitive but lack long-
term stability. It is considered that the use of a Zeeman laser as the light
source of the heterodyne interferometry in LID 1 increased the periodic
nonlinearity, more or less. In the operations of the later interferometers
(LIDs 2 and 3), the probe and reference laser beams were generated using
the combination of a stabilized He-Ne laser unit and a pair of acousto-
optical modulators to reduce the periodic nonlinearity. From the concerns
about the significant error, we can conclude that the standard reference
data should be reevaluated without the data measured using LID 1 at
temperatures above 600 K, although the difference between the present
data and CODATA 2 is within the magnitude of the expanded uncertainty
in the present work.
5. CONCLUSIONS
Linear thermal expansion data, a(T) and e(T), on single-crystal
silicon in the temperature range 293 to 1000 K have been determined using
a laser interferometric dilatometer. The expanded uncertainties (k=2) of
a(T) and e(T) in the measured temperature range were estimated to be
3.8 × 10 −8 to 4.8 × 10 −8 K −1 and 1.6 × 10 −6 to 6.7 × 10 −6, respectively. The
respective standard deviations of the measured a(T) and e(T) were esti-
mated to be 7.5 × 10 −9 K −1 and 1.1 × 10 −6, which were within the mag-
nitudes of their expanded uncertainties.
The present results are in good agreement with the most recently
reported data [5] but not with the earlier reported data at temperatures
above 700 K [3], both of which were measured with the dilatometers
similar to that used in the present work. The poor agreement with the
earlier reported data, which were used to estimate the present CODATA
recommended values [1], suggests the need for a reevaluation of the stan-
dard reference values of a(T) on silicon at temperatures above 600 K.
ACKNOWLEDGMENTS
The authors wish to thank Dr. Jun Ishikawa of the Time and
Frequency Division of our institute, who calibrated the wavelength of the
laser used in this work. This work is a result of the national research
program ‘‘Research on Measurement Technology and Reference Materials
for Thermophysical Properties of Solids’’ which was financially supported
236 Watanabe, Yamada, and Okaji
REFERENCES
1. G. K. White, in CINDAS Data Series on Material Properties, Vols. 1–4: Thermal Expansion
of Solids, R. E. Taylor, ed. (ASM International, Materials Park, OH, 1998), Chap. 11,
pp. 269–285.
2. C. A. Swenson, J. Phys. Chem. Ref. Data 12:179 (1983).
3. M. Okaji, Int. J. Thermophys. 9:1101 (1988).
4. M. Tanaka, T. Yamagami, and K. Nakayama, IEEE Trans. Instrum. Meas. 38:552 (1989).
5. H. Watanabe, N. Yamada, and M. Okaji, Int. J. Thermophys. 23:543 (2002).
6. N. Yamada and M. Okaji, High Temp. High Press. 29:89 (1997).
7. H. Watanabe, N. Yamada, and M. Okaji, Int. J. Thermophys. 22:1185 (2001).
8. M. Okaji and H. Imai, Prec. Eng. 7:206 (1985).
9. M. Okaji and H. Imai, J. Phys. E 20:887 (1987).