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Thermal Contact Resistance and Thermal Conductivity of A Carbon Nanofiber
Thermal Contact Resistance and Thermal Conductivity of A Carbon Nanofiber
Introduction ment was conducted before and after a platinum 共Pt兲 layer was
deposited on the contacts between the CNF and the microdevice
Diamond, graphite, and graphite fibers have been known as
so as to investigate the thermal contact resistance between the
excellent heat conductors with a high thermal conductivity up to CNF and a planar surface. The contact resistance was reduced by
3000 W / m-K 关1–3兴. Recently, the axial thermal conductivity of the platinum coating for about 9–13% of the total thermal resis-
individual multiwalled carbon nanotubes 共CNTs兲 关4兴 has been tance of the nanofiber sample before the Pt coating. At tempera-
found to be higher than 3000 W / m-K at a temperature of 300 K ture 300 K, the obtained axial thermal conductivity of the carbon
关5兴. It was also found that the effective thermal conductivity of nanofibers was about three times smaller than that of graphite
CNT mats 关6兴 and CNT bundles 关7兴 was one or two orders of fibers grown by pyrolysis of natural gas prior to high-temperature
magnitude lower than that of individual defect-free CNTs due to heat treatment.
the large thermal contact resistance between adjacent CNTs in the
bundles.
It has been suggested that CNTs and carbon nanofibers 共CNFs兲 Experimental Methods
can be used as thermal interface materials to enhance contact ther-
mal conductance for electronic packaging applications. Several Nanostructure Growth. CNFs were grown using a plasma en-
groups have reported mixed experimental results from no im- hanced chemical vapor deposition 共PECVD兲 method as
provements to large improvements in the thermal contact conduc- described previously 关13兴. Briefly, silicon substrates with a prede-
tance due to the CNTs and CNFs 关8–12兴. These mixed results can posited 30-nm-thick Ti barrier layer and a 30-nm-thick Ni
be caused by the difference in surface coverage and perpendicular catalyst layer were subjected to a glow discharge at a dc bias of
alignment of the CNTs or CNFs. Moreover, the results can be 585 V, 500 W, and 0.85 A under a total flow of 100 standard
affected by two other factors. First, the CNTs and CNFs grown cubic centimeter per minute 共sccm兲 of 4:1 NH3 : C2H2 process gas
using different methods possess different defect densities and dif- mixture at 4 Torr for 45 min. CNF growth rate under these con-
ferent intrinsic thermal conductivities. Secondly, the contact ther- ditions was approximately 500 nm/ min. Cross-sectional transmis-
mal resistance of the nanometer scale point and line contacts be- sion electron micrographs 共Fig. 1兲 were obtained to investigate the
tween a CNT or CNF and a planar surface can be high due to CNF quality and graphitic microstructure. The CNFs possessed
enhanced phonon-boundary scattering at the nanocontacts. cone angles between 5°–20° with typical cone angles around 10°
We have used a microfabricated device to measure the thermal 共Fig. 1共c兲兲.
resistance of an individual CNF from a vertically aligned CNF Measurement Procedure. The measurement was conducted
film for applications as thermal interface materials. The measure- with the use of a previously reported method based on a microde-
vice. A detailed description of the measurement method can be
1
Current address: Materials Sciences Division, Lawrence Berkeley National found in Ref. 关7兴. In brief, the microdevice consists of two sym-
Laboratory, Berkeley, CA 94720. metric silicon nitride 共SiNx兲 membranes suspended by long SiNx
2
Author to whom correspondence should be addressed; e-mail: beams, as shown in Fig. 2共a兲. A Pt serpentine line was patterned
lishi@mail.utexas.edu
Contributed by the Heat Transfer Division of ASME for publication in the JOUR-
on each membrane and used as a heater and resistance thermom-
NAL OF HEAT TRANSFER. Manuscript received December 20, 2004; final manuscript eter 共RT兲. A nanofiber deposited from a suspension was trapped
received September 18, 2005. Review conducted by C. P. Grigoropoulos. between the two membranes. When a dc current 共I兲 was supplied
234 / Vol. 128, MARCH 2006 Copyright © 2006 by ASME Transactions of the ASME
冑冉 冊 冉 冊
= 0.01% Tr including both random and systematic errors. Due to a
2
small temperature gradient in the cryostat, there was a less than B Gm B Gm B Gb B共⌬Th+⌬Ts兲 BQ 2
0.2% difference between the temperature readings of the two di- = = = + 艋 0.24% 共5兲
Gm Gm Gb ⌬Th + ⌬Ts Q
odes that were located 4.5 cm apart from each other. The RT on
the microdevice was located between the two diodes and the diode
Reduction of the Thermal Contact Resistance. The measured
right next to the RT was used as the reference in the temperature
calibration. The difference between Tr and the actual temperature thermal resistance of the sample 共Rm = Gm−1
兲 consists of the intrin-
of the RT should be less than 0.2% because the distance between sic thermal resistance of the nanofiber 共Rn兲 and the total contact
the RT and the reference diode was much shorter than that be- thermal resistance between the nanofiber and the two membranes
tween the two diodes. Thus, the systematic error in the calibration 共Rc兲, i.e.,
of the RT was calculated to be BT 艋 0.2% T. Because BTh共I兲 and Rm = Rn + Rc 共6兲
BTh共I=0兲 arise from the same calibration error and are thus perfectly
To reduce Rc, we used a focused electron beam deposition
correlated, the propagation of BTh共I兲 艋 0.2% Th共I兲 and BTh共I=0兲 method to deposit a thin Pt layer locally on the contacts from
艋 0.2% Th共I = 0兲 results in B⌬Th共I兲 艋 0.2% ⌬Th共I兲 关14兴. In other precursor gases in a dual beam focused ion beam 共FIB兲 tool. The
words, because Th共I兲 and Th共I = 0兲 were distorted by the same deposited Pt layer is shown in Figs. 5共a兲 and 5共b兲. The effective
percent of the reading due to the same calibration error, ⌬Th共I兲 contact area between the nanofiber and the membranes was in-
was distorted by the same percent of the reading. Similarly, creased by the Pt layer.
B⌬Ts共I兲 艋 0.2% ⌬Ts共I兲. Because Th and Ts were calibrated using the
same Tr and thus BTh and BTs arise from the same calibration error,
BTh and BTs are also perfectly correlated and propagate into Measurement Results and Discussions
B共⌬Th−⌬Ts兲 艋 0.2% 共⌬Th − ⌬Ts兲 and B共⌬Th+⌬Ts兲 艋 0.2% 共⌬Th + ⌬Ts兲. Figure 6 shows the measured thermal resistance 共Rm兲 before
The Joule heat Q was obtained as a product of the measured and after the Pt coating on the contacts. The difference in Rm is
voltage 共V兲 and current 共I兲. The systematic error of the second caused by the reduction in the thermal contact resistance by the Pt
type in the V measurement, i.e., BV, was specified in the instru- layer, and the reduction of the contact resistance 共Rc兲, i.e., ⌬Rc, is
ment manual to be less than 0.05% of the reading, and this error shown in the inset of Fig. 6. The uncertainty in ⌬Rc is calculated
共BI兲 in the I measurement was less than 0.1% of the reading. as the root-sum-square of the uncertainty in Rm before the Pt
Hence, the same type of error in Q was calculated as BQ coating and that after the Pt coating. The contact resistance was
= 共BI2 / I2 + B2V / V2兲1/2Q = 0.125% Q. reduced by the Pt coating for about 9–13% of the Rm value ob-
The dominant uncertainty source is the random fluctuation in tained before the Pt coating.
冑 冉冑 冊
be calculated from the contact force. Rc = 共7兲
Bahadur et al. calculated the contact force between a nanowire k储D2 4
tanh l
and a substrate to be the van der Waals force. The calculation 4R⬘c k储D2R⬘c
requires the knowledge of the Hamaker constant 共A兲 that can be
where k储 is the axial thermal conductivity of the nanofiber, and lc
calculated from Lifshitz-van der Waals coefficient 关18兴. For the
is the contact length in the axial direction. The radial or cross-
contact between Pt and carbon 共C兲 in vacuum, the Hamaker con-
stant can be estimated from those of Pt–Pt and C–C interfaces to plane thermal conductivity of the nanofiber, i.e., k⬜, is needed for
the calculation of R⬘c . Although the cross-plane thermal conduc-
be APt–C ⬇ 冑APt–PtAC–C 关18,19兴. We could not find the Hamaker
tivity of graphite is given in the literature to be k⬜ = 5.7 W / m-K at
constant for Pt–Pt and graphite-graphite interfaces in the litera-
300 K 关2兴, the value for the nanofiber can be different because of
ture, and have used the values for Au-Au and diamond-diamond
different crystalline structure and quality. More importantly, the
interfaces to approximate APt–Pt and AC–C and obtained APt–C ⬇ 4
effective thermal conductivity at a point contact of a Knudsen
⫻ 10−19 J for the contact between the nanofiber and the mem-
number 共K兲 of the order of unity or larger, where K is the ratio
brane. In the calculation, we have used Van der Waals radii for Pt
and carbon found in Ref. 关20兴. Based on these alternative between the phonon mean free path and the contact width, can be
properties, we calculated that the contact width 共2b兲 between the substantially reduced 关21兴. This reduction needs to be taken into
account in the calculation of the contact resistance based on the
152-nm-diameter nanofiber and the Pt surface was approximately
continuum model when the contact width is comparable to or
10 nm.
smaller than the mean free path. On the other hand, the axial or
Because the temperature of the nanofiber segment in contact
in-plane thermal conductivity k储 can be calculated from the mea-
with the membrane varies along the nanofiber as a result of heat
sured thermal resistance of the nanofiber after the Pt coating. Us-
transfer to the membrane, the portion of the nanofiber in contact
ing the obtained k储 values at 150 K and 300 K, we have calculated
with the membrane should be treated as a fin. The thermal contact
the contact thermal resistance as a function of k⬜ for different
resistance between the nanofiber and the sensing membrane is
thus the fin resistance. Assuming adiabatic boundary condition at contact widths of 2b = 0.1 nm, 1 nm, 10 nm, 50 nm, and 100 nm.
The results are shown in Fig. 7.
Without the Pt coating, a contact width of 2b = 50 and 100 nm
is rather unlikely because the diameter of the nanofiber is only
152 nm. With the Pt coating, on the other hand, a contact width of
2b 艌 50 nm is possible. If 2b 艌 50 nm with the Pt coating and
2b ⬇ 10 nm without the Pt coating, the calculated ⌬Rc can match
the measurement value when k⬜ ⬍ 0.6 W / m-K for 150 K and
k⬜ ⬍ 2 W / m-K for 300 K. For this case, the residual Rc after the
Pt coating is comparable to the measure ⌬Rc shown in the inset of
Fig. 6.
We have used the thermal resistance results measured after the
Pt coating to calculate the axial thermal conductivity of the
nanofiber. The results are shown in Fig. 8. As a comparison, Fig.
8 also shows the measured thermal conductivity of a graphite fiber
grown by pyrolysis prior to heat treatment. The thermal conduc-
tivity of the PECVD nanofiber increases nearly linearly with the
temperature in the temperature range between 150 K and 310 K
and the value at 300 K is about three times smaller than that of the
graphite fiber. Note that the thermal conductivity of the graphite
fiber and the specific heat 共C兲 of graphite 关22兴 increase nearly
Fig. 6 Measured thermal resistance of the nanofiber sample
before a Pt layer was deposited „solid black circles… and after a linearly with temperature in the temperature range between 150 K
Pt layer was deposited with the use of the electron beam „open and 310 K. Using the specific heat of graphite and a sound veloc-
circles…. The inset shows the reduction in contact resistance, ity of v = 10000 m / s, we have calculated the phonon mean free
⌬Rc, after the Pt coating. path 共l兲 according to the thermal conductivity formula, i.e., k