JOURNAL OF APPLIED PHYSICS 108, 094315 2010

Ultrafast thermoreectance techniques for measuring thermal conductivity and interface thermal conductance of thin lms
Jie Zhu,1,2 Dawei Tang,2 Wei Wang,1 Jun Liu,1 Kristopher W. Holub,1 and Ronggui Yang1,a
1 2

Department of Mechanical Engineering, University of Colorado at Boulder, Colorado 80309, USA Institute of Engineering Thermophysics, Chinese Academy of Sciences, Beijing 100190, China

Received 5 July 2010; accepted 18 September 2010; published online 4 November 2010 The thermal conductivity of thin lms and interface thermal conductance of dissimilar materials play a critical role in the functionality and the reliability of micro/nanomaterials and devices. The ultrafast laser-based thermoreectance techniques, including the time-domain thermoreectance TDTR and the frequency-domain thermoreectance FDTR techniques are excellent approaches for the challenging measurements of interface thermal conductance of dissimilar materials. Both TDTR and FDTR signals on a trilayer structure which consists of a thin lm metal transducer, a target thin lm, and a substrate are studied by a thermal conduction model. The sensitivity of TDTR signals to the thermal conductivity of thin lms is analyzed to show that the modulation frequency needs to be selected carefully for a high precision TDTR measurement. However, such a frequency selection, which is closely related to the unknown thermal properties and consequently hard to make before TDTR measurement, can be avoided in FDTR measurement. We also found out that in FDTR method, the heat transport in a trilayer structure could be divided into three regimes, and the thermal conductivity of thin lms and interface thermal conductance can be obtained subsequently by tting the data in different frequency range of one FDTR measurement, based on the regime map. Both TDTR and FDTR measurements are then conducted along with the analysis to obtain the thermal conductivity of SiO2 thin lms and interface thermal conductance between SiO2 and Si. FDTR measurement results agree well with the TDTR measurements, but promises to be a much easier implementation than TDTR measurements. 2010 American Institute of Physics. doi:10.1063/1.3504213
I. INTRODUCTION

The thermal conductivity k of thin lms and interface thermal conductance G of dissimilar materials play a critical role in the functionality and the reliability of micro/ nanomaterials and devices.1 The measurement of these thermal properties has been very challenging.13 Currently, the most widely used measurement techniques for the thermal conductivity of thin lms can be grouped into frequencydomain and time-domain methods, which are typically represented by the electrically heated 3- method47 and timedomain thermoreectance TDTR method using ultrafast lasers,1,2,8,9 respectively. The 3 method, which uses a metal microbridge deposited on thin lm samples as both an electrical-heater and a temperature sensor, has become a very effective technique for measuring the thermophysical properties of dielectric thin lms.4 However, applications of the 3 method to electrically conducting or semiconducting materials can be challenging in sample preparation because of the need to electrically isolate the metal microbridge from the sample.10 This additional layer of electrical insulation inevitably introduces an additional thermal resistance between the metal microbridge and the sample, which can reduce both the sensitivity and accuracy of the technique.6 Usually a typical frequency range from 5 Hz to 200 kHz is applied for the 3 method.7,11
a

Electronic mail: ronggui.yang@colorado.edu.

Using a typical thermal diffusivity value = 3 106 m2 / s, the thermal penetration depth d can be several to hundreds of microns from the relationship of L = / f .7 As a result, such a quasisteady-state method is insensitive to the interface thermal conductance/resistance, and cannot be used to accurately measure the thermal conductivity of nanoscale thin lms. Ultrafast thermoreectance techniques often employ subpicosecond lasers. Repeated laser pulses are divided into two beams. The pump beam excites a sample and the probe beam measures the changes in the reectivity or diffraction, which is temperature-dependent. In TDTR method, probe beam arrives at the sample surface at different time intervals after the pump beam through a mechanical delay stage. The temporal decay of the measured signals is then used to deduce k and G with a thermal transport model. Since it was introduced in 1980s Refs. 8, 12, and 13 till now, the TDTR technique has been used to measure the thermal conductivity of solids14 and liquids,15 in both bulk and thin-lm formats that spans a range in thermal conductivity from the lowest thermal conductivity ever observed in the fully dense solid16 to very high thermal conductivity of metals and diamond,13,17 and for measuring the interface thermal conductance of dissimilar materials.2,8,1821 The imperfections in the stage motion, the overlap of pump-and-probe pulses, and the divergence of the delayed optical beam could all introduce measurement errors.1,9,13 In recent years, a variety of im 2010 American Institute of Physics

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Zhu et al. TABLE I. Comparisons among 3 , TDTR, and FDTR methods. 3 Probing method Sensitive thermal properties Mechanical stage problem Modulation frequency Thermal penetration depth Metal bridge k No 0.05 f 200 kHz 400 L 2 m TDTR Noncontact k,G Yes f 1 10 MHz L 1 0.3 m

J. Appl. Phys. 108, 094315 2010

FDTR Noncontact k,G No 0.1 f 20 MHz 3 L 0.2 m

provements have been done to reduce such imperfections,1,9,13 but the optical alignment involving a moving stage is still rather tedious. A frequency-domain thermoreectance FDTR technique, which has the potential to get rid of the moving stage, has recently been proposed to measure the thermal conductivity and heat capacity of bulk materials22 and then thin metal lm which itself is the transducer layer of pump-andprobe samples.23 The measurement of different materials shows that FDTR has the capability to measure the thermal conductivity of a large range from 1 to 250 W/ mK . In terms of implementation, the FDTR measurement setup is similar as that in TDTR method, but the pump pulses are modulated at variable frequencies and the thermoreectance signals are measured under a xed delay time between the probe and the pump pulses, which avoids all the imperfections that could result from the motion of pump-probe delay stage. Besides the three methods mentioned above, another frequency domain method based on continuous wave laser, called phase sensitive transient thermoreectance technique PSTTR has also been used for thermal conductivity measurement.24 Compared to FDTR method using ultrafast lasers, PSTTR method working at lower frequency range is kind of an optical 3- method, insensitive to interface thermal conductance. Table I shows a comparison among the 3- , TDTR, and FDTR methods. The thermal penetration depth of FDTR method using a frequency of 0.120 MHz is typically from 200 nm to several microns, which makes it very suitable for the thermal conductivity measurement of the nanoscale thin lms. In addition, such FDTR signals also contain the transient heat transfer information that could be used to measure the interface thermal conductance/resistance. We thus expect that the FDTR method has all the advantages of TDTR method over the 3- method, such like it is sensitive to both thermal conductivity of thin lms and interface thermal conductance and is a noncontact method, but also can avoid the problems associated with moving a mechanical stage in TDTR measurements. In this work, we exploit this FDTR method to measure the thermal conductivity of thin lms and the interface thermal conductance between thin lms and their substrates simultaneously. A theoretical model is presented to analyze the thermoreectance signals in a trilayer structure which consists of an aluminum thin lm transducer, a target thin lm, and a substrate. The sensitivity analysis of TDTR signals shows that the modulation frequency needs to be selected carefully for a high precision TDTR measurement. However, such a frequency selection, which is closely related to the

unknown thermal properties and consequently hard to make before TDTR measurement, can be avoided in FDTR measurement. We also found out that in FDTR method, the heat transport in a trilayer structure could be divided into three regimes based on the thickness of the lm and the frequencydependant thermal penetration depth. As a result, the thermal conductivity of thin lms and interface thermal conductance can be obtained subsequently by tting different frequency ranges of one FDTR measurement. Both TDTR and FDTR measurements are conducted along with the analysis to obtain the thermal conductivity of SiO2 thin lms and interface thermal conductance between SiO2 and Si substrate. FDTR measurement results agree well with the TDTR measurements, but promises to be a much easier implementation than TDTR measurements.

II. EXPERIMENTAL METHOD

Figure 1 shows the schematics of the ultrafast thermoreectance setup in our laboratory, which is congured for both TDTR and FDTR measurements. The setup uses a femtosecond laser oscillator and a 0.6 m mechanical delay stage 8 ns optical delay with two round trips and is similar to most setups commonly used for TDTR measurement.1315,18 Comparing to TDTR technique, the FDTR implementation could be much simpler by xing the position of the mechanical stage at a certain delay-time and changing the modulation frequency using electronics. Such FDTR measurement could avoid all the artifacts involved in the delay stage movements of TDTR technique.

FIG. 1. Color online Schematic diagram of the optical paths of our ultrafast pump-and-probe thermoreectance system.

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FIG. 2. Color online Schematic diagram of a trilayer sample that ultrafast thermoreectance techniques are used to measure the thermal conductivity of the thin lm in the middle layer: a sectional view; and b top view, where the bigger circle is the pump spot with Rpump as the radius and the smaller circle is the probe spot with radius Rprobe.

for the pump beam and the temperature transducer for the probe beam. In our measurements, the focuses radii of the pump and probe beams on the surface of the samples are 10 m and 5 m, respectively. The heat of the pump laser beam is absorbed by the surface of the transducer layer, and then diffused through the layers and the interfaces in the multilayer structure. The thermoreectance signal of the probe beam is picked up by a lock-in amplier. The heat transfer model based on the transform matrix method of heat transfer through a single layer and an interface has been presented by other authors before,9,22,2527 and here we present some of the key equations simply for the easiness of the readers to understand the rest of the paper.
A. Single layer and interface

The Spectra-Physics Tsunami femtosecond Ti-sapphire laser, pumped by a 10 W diode laser, emits a train of 150 fs pulses at a repetition rate of 80 MHz. The central wavelength is 800 nm and the power per pulse is roughly 19 nJ. The laser pulse is split into pump and probe beams. The pump beam passes through an electro-optic modulator EOM that modulates the beam at a frequency between 0.1 and 20 MHz. The modulation frequency serves as the reference for a lock-in amplier which extracts the thermoreectance signal from the background. The second-harmonic generator is used to double the frequency of the probe pulses, which produces a light train with a central wavelength of 400 nm and are timedelayed relative to the pump pulses with the mechanical stage. Such a near infrared-blue two-color system has signicant advantages over a single-color one since it is easier to isolate the scattered pump light from the detector by using dielectric mirrors and color lters which could have a transmission of 109 at the wavelength around 800 nm, much more efcient than a polarization arrangement. This also allows us to use a simple coaxial geometry where pump and probe beams are focused by the same objective lens, simplifying the overlap of pump and probe pulses and producing less deformation of the laser prole. In the TDTR measurement, an inductor is placed between the output of the photodiode and the lock-in amplier to maximize the response at the modulation frequency and remove the higher harmonic components in the measured signal.25 For the FDTR method, instead of this method, we adjust a sinusoidal wave form driving the EOM to minimize the higher harmonic components to make the measurement procedure easier.22 Also, in both the TDTR and FDTR measurement, the signal needs a phase correction by adjusting the phase of the lock-in until the out-of-phase component of the signal is constant as the stage moves across the zero delay time.22,25 This phase correction should be obtained under each applied frequency in FDTR measurements.
III. HEAT TRANSFER MODEL AND LOCK-IN SIGNAL

In each layer, the heat conduction equation can be written as the following considering a cylindrical heating spot on the surface:
2 kr r + kz 2 = c r z r r

l , t

where r is the radial coordinate, z is the cross-plane coordinate in the depth direction , t is time, is the temperature, is the density, c is the specic heat, and kr and kz are the in-plane and cross-plane thermal conductivity, respectively. Taking the zeroth-order Hankel transform of Eq. 1 yields
2

k rl 2 l + k z

l z
2

= c

l , t

where l is the transform variable, and is the temperature in Hankel transform. In the thermoreectance measurement, the heating pulses are modulated by a frequency 0, and the response are extracted from the probe laser beam at the frequency 0 by a lock-in amplier, so we seek a solution of Eq. 2 in the frequency domain = u exp i t , 3

where u is a function of z only, and is an arbitrary constant. This solution will have periodicity 2 / . Substituting Eq. 3 into Eq. 2 , we have
2

,z z2

= q2

,z ,

where q= k rl 2 + i c . kz 5

The general solution of Eq. 4 is z = exp qz + exp qz , 6 7

Figure 2 shows the schematics of a typical tri-layer sample used in TDTR or FDTR techniques to measure the thermal conductivity of thin lms. Such trilayer structure consists of a 50120 nm thick aluminum Al thin lm, a thin lm with unknown thermal properties to measure, and a substrate. The aluminum lm serves as an energy absorber

F z = kzq exp qz + kzq exp qz ,

where and are constants, and z and F z are the temperature and heat ux at the point z. Let and F be the temperature and heat ux at the face z = 0 and let and F

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be their values at the face z = d. The relation between these four quantities , F, , and F can be expressed as F =
1 3 2 4

2Qpump 2r2 Ipump r = , exp 2 2 Rpump Rpump which after taking the Hankel transform will give F1 l = Ipump l =
2 l2Rpump Qpump exp , 8 2

16

. and

8 can be

By substituting Eqs. 6 and 7 into Eq. 8 , eliminated, and we can easily get
1

17

4 3

= cosh qd ,

= sinh qd / kzq , 9

= kzq sinh qd .

When heat diffuses through an interface, there should be a temperature difference between its two sides, and the only necessary property is the interface thermal conductance G, which could be dened by F=F =G . 10

where Qpump is the power absorbed from pump laser, and Rpump is the 1 / e2 radius of pump intensity distribution as a Gaussian spot. Inserting Eq. 17 to Eq. 15 yields the surface temperature
1

l =

2 l2Rpump D Qpump exp . 8 C 2

18

In matrix form Eq. 10 will become F = 1 1/G 0 1 F , 11

Eqs. 8 and 11 are the heat transfer solutions for a single layer with thickness of d and an interface, respectively.

The surface temperatures are measured by thermoreectance, i.e., the change in the reectivity which depends on temperature change. This change in reectivity is measured by changes in the reected intensity of a probe laser beam. Let Qprobe be the power of probe beam and let Rprobe be the 1 / e2 radius of probe intensity distribution as a Gaussian spot. The thermoreectance response H l contained in reected probe beam should be the product of surface temperature 1 and thermoreectance coefcient , and weighted by the probe intensity distribution, considering the cylindrical spreading effects, Hl = =
2 l2Rprobe Qprobe exp 8 2 1

B. Multilayer structure

In a multilayer structure with n parallel layers inside, from Eqs. 8 and 11 , we can see that for either a lm or an interface at jth j = 1 , . . . , n layer, the temperature j+1 and heat ux F j+1 on the bottom side of the layer should be the product of the temperature j and heat ux F j on the top side with a matrix M j, like
j+1

l . 19

2 2 l2 Rpump + Rprobe D QpumpQprobe exp 2 8 C 4

F j+1

Aj Bj = Cj Dj

Fj

= Mj

Fj

12

The frequency-domain response H of the surface temperature change in real space can then be found by taking the inverse Hankel transform of Eq. 19 H = QpumpQprobe 2 exp l
0

Multiple layers are handled by multiplying the matrices for individual layers like Eqs. 8 and 11 together. Therefore, the temperature n+1 and heat ux Fn+1 of the bottom side of the multilayer stack can be expressed by
n+1

D C dl. 20

Fn+1 where

A B = C D

2 2 l2 Rpump + Rprobe 8

F1

13
C. Lock-in amplier response

A B = M nM n1 . . . M 1 , C D

14

and 1 and F1 are the temperature and heat ux on the top side of the multilayer stack. If the heat ux is applied to the top surface of the rst layer, and the nth layer is assumed to be semi-innite, which means Fn+1 = 0, the top surface temperature will be given as
1

A lock-in amplier picks up the fundamental harmonic component of the probe signal 0 at the modulation freZ quency 0 and rejects all other components. In the case of pulsed pump and probe beams, at each individual delay time between pump and probe pulses, 0 could be given as Z Z
0

=
m=

+m

exp im

21

D F1 , C

15

from Eq. 13 , where C and D are calculated via Eq. 14 . The pump pulse heats the top surface and gives the top boundary condition as the cylindrical heat ux distribution

by applying the sampling theorem.9,13,25 Here s is the probe pulsing frequency or sampling frequency 80 MHz in our experiment , is the delay time between probe and pump is the sample frequency response obtained pulses, and H by Eq. 20 . The outputs of lock-in amplier are the real part

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and imaginary part of the fundamental component of the probe signal with respect to the reference wave exp i 0t , which correspond to in-phase signal Vin and out-of-phase signal Vout Vin = Re Z Z Vout = Re
0

exp i exp i

0t

, ,

22 23

0t

respectively. This result assumes the sample responds as a linear system and behaves as a continuum; these conditions are usually met for small temperature excursions and delay times greater than 100 ps, when the phonon-electron coupling does not need to be considered.18 The ratio of the inphase and out-of-phase signal Vin / Vout is used for obtaining the thermophysical properties by tting the measurement data to the theoretical model since it is a more robust quantity than amplitude signal.14 The model presented above describes the heat transfer process though multilayer structures in both time-domain and frequency-domain, and the only difference for the application is which one is the variable in the implementation, the delay time time-domain or the modulation frequency 0 frequency-domain . In TDTR measurement, the modulation frequency 0 is xed and the signal is obtained with changing the delay-time . In FDTR measurement, the signal is obtained with changing 0 while is xed.

FIG. 3. Color online TDTR signals Vin / Vout of a 110 nm and b 518 nm thick SiO2 thin lms and the best-t to the theoretical thermal conduction model with different modulation frequencies. The dashed lines are analytical results using the thermal conductivity of the thin lm with 20% and +20% changes to the best-t value, respectively.

A. TDTR method

IV. RESULTS AND DISCUSSIONS

We prepared SiO2 thin lms grown on Si wafers by thermal oxidation with thickness in the range of 100500 nm for measurements. In the trilayer structure as shown in Fig. 2, the interface thermal conductance between Al and SiO2 GAlSiO2 , the thermal conductivity of SiO2 thin lm layer kSiO2 , and the interface thermal conductance between SiO2 and Si GSiO2Si are the free parameters in our data analysis. Because the thickness of Al lm and the spot size of the laser have strong effects on the measurement results,23 we veried Al lm thicknesses using prolometer every time after deposition. We usually place a piece of silicon substrate next to the sample in the deposition chamber which can be used to calibrate the thickness of the Al layer. To build measurement condence, we have also calibrated the system and the data tting procedure by measuring many samples of well-known materials, such as silicon, sapphire, and glass. The spot size of laser was measured by knife edge method with an accuracy of 1 m. We obtained the signals on four different locations of every sample. The errors of the signals due to the uncertainties in thicknesses of Al lms and the thin lms to be measured as well as the spot size are always within 10%. The nal data presented here for the tting are the mean of these four sets of signals. Both TDTR and FDTR methods are applied in the measurement, and the sensitivity of the signals, depending on thin lm thickness, thermophysical properties, and modulation frequency, are analyzed by the theoretical model presented in Sec. III for comparison.

Figure 3 shows the TDTR signals on a 110 and b 518 nm thick SiO2 thin lm samples with different modulation frequencies, as well as the best-t curves and solutions obtained by varying the thermal conductivity of SiO2 by 20%. From each set of the measurement data, the thermophysical properties are obtained by comparing to the aforementioned thermal model and the tted results are listed in Table II. To achieve an effective measurement, high sensitivity of the signal to the parameter is needed, which means the further the 20% curves depart from the experimental data the better. Both Figs. 3 a and 3 b show that using different modulation frequencies results in different sensitivities of TDTR measurement. It can be clearly seen in Fig. 3 a that if 1.34 MHz was selected as the modulation frequency, the sensitivity of the TDTR signal of 110 nm thick SiO2 sample will be too low for obtaining a good measurement of the thermal conductivity. A higher modulation frequency of 2 MHz gives a higher sensitivity for the 110 nm thick SiO2 thin lm sample. However the situation showed in Fig. 3 b is in the opposite, where lower modulation frequency 1 MHz gives a higher sensitivity for the 518 nm thick SiO2 sample. The thermal penetration depth in TDTR method is related to the modulation frequency and thermal diffusivity = k / c of
TABLE II. Best-t values obtained from the TDTR experimental data. Thickness nm Modulation frequency MHZ kSiO2 W/m K GAlSiO2 108 W / m2 K GSiO2Si 108 W / m2 K 110 1.34 1.33 1.2 0.15 2 1.31 1.1 0.14 1 1.27 1.5 0.15 518 4 1.30 1.5 0.12

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FIG. 5. Color online Sensitivity of FDTR Vin / Vout signals to: a thermal conductivity of the SiO2 thin lm kSiO2, and b interface thermal conductance GSiO2Si with different modulation frequencies for 100, 200, and 500 nm SiO2 thin lms.

FIG. 4. Color online Sensitivity of TDTR Vin / Vout signal to the thermal properties of thin lms: a sensitivity to kSiO2 of 100 nm SiO2 on silicon substrate with different modulation frequencies; b sensitivity to kSiO2 of different thicknesses of SiO2 thin lms at 4 MHz modulation frequency; and c sensitivity to kSiO2 of 100 nm SiO2 on silicon substrate with different kSiO2 and GSiO2Si.

the material. As a result, the sensitivity of the measurement signal to the thermal conductivity has a signicant difference when applying different modulation frequencies on various thin lm materials. In order to illustrate this limitation of TDTR method for measuring the thermophysical properties of thin lms, we further analyze the sensitivity of TDTR signals as a function of lm thickness, thermophysical properties, and modulation frequency. We take the sensitivity of our measurement to a parameter x as28 Sx = d Vin/Vout / Vin/Vout , dx/x 24

optimal modulation frequency in TDTR measurement. However, the sensitivity also depends on the thickness and the thermophysical properties of the thin lm. As shown in Fig. 4 b , the TDTR sensitivity on SiO2 thin lm sample with a thickness of 100 nm is obviously higher than those on the other two, no matter thicker or thinner. Figure 4 c shows that the changes on the thermal conductivity of the thin lm and the interface thermal conductance can signicantly alter the sensitivity curves. In conclusion, the sensitivity of TDTR signals to the thin lm thermal conductivity depends on the modulation frequency, the thickness, and the thermophysical properties of the thin lm. On samples with different thicknesses and the thermophysical properties, the modulation frequency needs to be selected carefully for a high accuracy and sensitive TDTR measurement. Unfortunately, such a frequency selection is closely related to the unknown themselvesthermal conductivity and interface thermal conductance which we are interested in measuring.
B. FDTR method

where d Vin / Vout / Vin / Vout is the uctuation of Vin / Vout signal and x is the property that we are interested in measuring. Property x could thus be thermal conductivity or interface thermal conductance in the multilayer structure presented in Fig. 2. Figure 4 a shows the sensitivity of the TDTR signal to the thermal conductivity kSiO2 on 100 nm thick SiO2 lm sample. It can be clearly seen that the signal with modulation frequency of 4 MHz has a higher sensitivity than those with 1 and 8 MHz signals, which conrms our conclusion from the Fig. 3 that for each thin lm sample, there should be an

The FDTR method, which employs a large modulation frequency range from 0.1 to 20 MHz in each measurement, will avoid the limitation of frequency selection. Figure 5 a shows the sensitivity of the Vin / Vout signal to the thermal conductivity of SiO2 thin lm kSiO2 with different modulation frequency for 100, 200, and 500 nm SiO2 thin lms on the Si substrate. Here we chose 500 ps as the xed delay time. As mentioned above, the delay time should be longer than 100 ps when the electro-phonon coupling effect dies out, and shorter than 1 ns since the experimental data would be less noisy and more sensitive to the thermal conductivity of the thin lm. It can be seen from these curves that the optimal sensitivity can usually be captured when the modulation frequency is in this range. Not only on the measure-

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FIG. 6. Color online Comparison of FDTR Vin / Vout signal sensitivity to thermal conductivity of the SiO2 thin lm and interface thermal conductance between the SiO2 thin lm and the Si substrate.

ment of thermal conductivity, but also on that of interface thermal conductance, has FDTR technique avoided the limitation of bad choice on modulation frequency, as is shown in Fig. 5 b . The heat transport in a trilayer system could be divided into three regimes when the thickness of the thin lm d is smaller than, close to, or larger than the thermal penetration depth L according to the modulation frequency. Figure 6 shows the comparison of the sensitivity to the thermal conductivity of 500 nm SiO2 thin lm and the interface thermal conductance between SiO2 thin lm and Si substrate. In regime I d L , the modulation frequency is relatively high, the sensitivity of the signal to the interface thermal conductance is close to zero and the main information deduced from the signal is the thermal conductivity of thin lm; regime II d L is the transition regime where the interface thermal conductance begins to become important; and in regime III d L , the interface thermal conductance has large enough effect on the measurement data, which makes the sensitivity high enough for data tting. In the FDTR method, based on this three-regime plot in Fig. 6, the thermal conductivity of thin lm could be obtained by tting the experimental data in regime I to the theoretical model without the inuence from the interface between thin lm and substrate. The interface thermal conductance could then be obtained optimally by tting the data in regime III. The thermal conductivity of SiO2 thin lm and interface thermal conductance between SiO2 and substrate used in Figs. 5 and 6 are 1.3 W/ mK and 0.15 108 W / m2K , respectively. The Al lm thickness used in Figs. 46 for the analysis is 100 nm.
C. Measurements

FIG. 7. Color online FDTR Vin / Vout signals of SiO2 thin lms with different thickness at 500 ps delay-time and the best-t to the theoretical model of thermal transport: a 110 nm, b 304 nm, and c 518 nm.

To validate the above analysis, we have used FDTR technique to measure the thermal conductivity and interface thermal conductance of SiO2 thin lms with different thicknesses grown on commercial Si wafers by thermal oxidation. Figure 7 shows the room-temperature FDTR measurement signal of SiO2 thin lms with the thicknesses of a 110 nm, b 304 nm, and c 518 nm, respectively, at a xed delay

time of 500 ps. The measurement signal is then tted using the previously mentioned thermal model for the thermal conductivity of the thin lm kSiO2 and the interface thermal conductance GAlSiO2 and GSiO2Si. A nonlinear least-squares routine was used to minimize the error between the theoretical model and measurement data. Consistent with Fig. 6, the measured Vin / Vout signal for 518 nm thick SiO2 sample is sensitive to the thermal conductivity of the lm kSiO2 but not sensitive at all to the interface thermal conductance GSiO2Si in the frequency range 420 MHz. This phenomenon is clearly shown in Fig. 7 c , where the two curves with 20% GSiO2Si almost overlap with the best-t curve, but the other two 20% kSiO2 curves separate from it when frequency is over 4 MHz. Therefore, for the measurement of 518 nm SiO2, the thermal conductivity could be obtained without signicant inuence from interface thermal conductance in this frequency range. Then GSiO2Si could be obtained in the frequency range 0.11 MHz, where the signal is relatively sensitive to GSiO2Si, with known thermal conductivity. Similarly, for the 110 nm and 304 nm SiO2 sample, kSiO2 and GSiO2Si can be subsequently obtained by tting different frequency ranges of the FDTR measurement curve, too. We also noted that, in the FDTR measurement on 110 nm SiO2 sample see Fig. 7 c , the 20% kSiO2 and 20% GSiO2Si curves hardly depart from each other only except when

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TABLE III. Best-t values obtained from the FDTR experimental data. Thickness nm kSiO2 W/m K GAlSiO2 108 W / m2 K GSiO2Si 108 W / m2 K 110 1.30 1.0 0.17 304 1.31 1.2 0.15 518 1.35 1.2 0.16

method is used to roughly estimate k and G rst, an optimal frequency range could be identied for subsequent TDTR measurements that could render much better precision of TDTR measurements.
ACKNOWLEDGMENTS

modulation frequency is close to 20 MHz. For even thinner samples 100 nm , these two parameters should be unable to be obtained at the same time by FDTR method. The reason is, if the thickness d of the thin lm is much smaller than the thermal penetration depth L d 0.1L , this lm is thin enough to be treated as a thermal interface with a total thermal resistance as its only thermal property. As a result, the thermal conductivity of the thin lm and the interface thermal resistance on its both sides are included in this total thermal resistance,14 and cannot be separated in the analysis of the measurement data. TDTR method also has this limitation since it shares the same thermal model with FDTR method. The best-t parameters of these three measurements are listed in Table III. The FDTR measurement results of the thermal conductivity of the nanoscale SiO2 thin lms agree well with the accepted literature values measured of bulk materials5 and our TDTR measurements on the same samples. The interface thermal conductance between SiO2 thin lms and silicon substrates were also measured, and the value agrees well with the results recently presented by Hopkins et al.29
V. SUMMARY AND OUTLOOK

This work is supported by the National Science Foundation CAREER Grant No. CBET-0846561 , the AFOSR Discovery Challenge Thrust Grant No. FA9550-08-1-0078 , and National Natural Science Foundation of China Grant No. 50876103 .
D. G. Cahill, W. K. Ford, K. E. Goodson, G. D. Mahan, A. Majumdar, H. J. Maris, R. Merlin, and S. R. Phillpot, J. Appl. Phys. 93, 793 2003 . 2 D. G. Cahill, K. Goodson, and A. Majumdar, ASME J. Heat Transfer 124, 223 2002 . 3 G. Chen, D. Borca-Tascuic, and R. Yang, in Encyclopedia of Nanoscience and Nanotechnology, edited by H. S. Nalwa American Scientic Publishers, California, 2004 , Vol. 7, pp. 429459. 4 D. G. Cahill and R. O. Pohl, Phys. Rev. B 35, 4067 1987 . 5 D. G. Cahill, Rev. Sci. Instrum. 61, 802 1990 . 6 T. Borca-Tasciuc, A. R. Kumar, and G. Chen, Rev. Sci. Instrum. 72, 2139 2001 . 7 Y. K. Koh, S. L. Singer, W. Kim, J. O. Zide, H. Lu, D. G. Cahill, A. Majumdar, and A. C. Gossard, J. Appl. Phys. 105, 054303 2009 . 8 R. J. Stoner and H. J. Maris, Phys. Rev. B 48, 16373 1993 . 9 A. J. Schmidt, X. Chen, and G. Chen, Rev. Sci. Instrum. 79, 114902 2008 . 10 S. M. Lee and D. G. Cahill, J. Appl. Phys. 81, 2590 1997 . 11 C. E. Raudzis, F. Schatz, and D. Wharam, J. Appl. Phys. 93, 6050 2003 . 12 C. A. Paddock and G. L. Eesley, J. Appl. Phys. 60, 285 1986 . 13 W. S. Capinski and H. J. Maris, Rev. Sci. Instrum. 67, 2720 1996 . 14 R. M. Costescu, M. A. Wall, and D. G. Cahill, Phys. Rev. B 67, 054302 2003 . 15 A. J. Schmidt, M. Chiesa, X. Chen, and G. Chen, Rev. Sci. Instrum. 79, 064902 2008 . 16 C. Chiritescu, D. G. Cahill, N. Nguyen, D. Johnson, A. Bodapati, P. Keblinski, and P. Zschack, Science 315, 351 2007 . 17 J. C. Zhao, X. Zheng, and D. G. Cahill, Mater. Today 8, 28 2005 . 18 R. J. Stevens, A. N. Smith, and P. M. Norris, ASME J. Heat Transfer 127, 315 2005 . 19 P. E. Hopkins, R. N. Salaway, R. J. Stevens, and P. M. Norris, Int. J. Thermophys. 28, 947 2007 . 20 P. M. Norris and P. E. Hopkins, ASME J. Heat Transfer 131, 043207 2009 . 21 D. G. Cahill, A. Bullen, and S. M. Lee, High Temp. - High Press. 32, 135 2000 . 22 A. J. Schmidt, R. Cheaito, and M. Chiesa, Rev. Sci. Instrum. 80, 094901 2009 . 23 A. J. Schmidt, R. Cheaito, and M. Chiesa, J. Appl. Phys. 107, 024908 2010 . 24 T. Tong, Y. Zhao, L. Delzeit, A. Kashani, M. Meyyappan, and A. Majumdar, IEEE Trans. Compon. Packag. Technol. 30, 92 2007 . 25 D. G. Cahill, Rev. Sci. Instrum. 75, 5119 2004 . 26 A. Feldman, High Temp. - High Press. 31, 293 1999 . 27 H. S. Carslaw and J. C. Jaeger, Conduction of Heat in Solids Oxford University Press, New York, 1959 . 28 B. C. Gundrum, D. G. Cahill, and R. S. Averback, Phys. Rev. B 72, 245426 2005 . 29 P. E. Hopkins, J. R. Serrano, L. M. Phinney, S. P. Kearney, T. W. Grasser, and C. T. Harris, ASME J. Heat Transfer 132, 081302 2010 .
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The FDTR method, which can avoid the limitations of TDTR technique involving mechanical delay stage, has been extended for measuring the thermal properties of thin lms. A trilayer structure which consists of a metal transducer, a thin lm with unknown thermal properties, and a substrate is introduced as a theoretical model for analyzing the sensitivity of TDTR and FDTR signals. The FDTR measurement results of the thermal conductivity of the nanoscale SiO2 thin lms and the interface thermal conduction between SiO2 and Si agree well with literature and the TDTR measurements on the same samples. From the sensitivity analysis of TDTR and FDTR methods, we can expect that a combination of these two methods will render additional advantages on the thermal property measurements of thin lms. The combination can be taken in two ways: 1 tting two curves obtained by FDTR and TDTR measurement simultaneously on the same sample can be used to characterize more unknown parameters, such as specic heat, thermal conductivity of thin lm and its substrate, and interface thermal conductance. 2 If the FDTR

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