International Journal of Heat and Mass Transfer 137 (2019) 263–267

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International Journal of Heat and Mass Transfer

journal homepage: www.elsevier.com/locate/ijhmt

Thermal conductivity tensor of NbO2

Hai Jun Cho a,b,⇑, Gowoon Kim b,c,1, Takaki Onozato b,1, Hyoungjeen Jeen c, Hiromichi Ohta a,b
a
Research Institute for Electronic Science, Hokkaido University, N20W10, Kita, Sapporo 001-0020, Japan
b
Graduate School of Information Science and Technology, Hokkaido University, N14W9, Kita, Sapporo 060-0814, Japan
c
Department of Physics, Pusan National University, Busan 46241, South Korea

a r t i c l e i n f o a b s t r a c t

Article history: Among several transition metal oxides showing metal to insulator transition, NbO2 has attracted atten-
Received 8 January 2019 tion as the active material of memory devices due to its high thermal stability. Although clarification of
Received in revised form 18 March 2019 thermal conductivity (j) is essentially important for optimizing the NbO2 device performance, it has not
Accepted 23 March 2019
been reported thus far probably due to the anisotropic crystal structure. Here we show the thermal con-
Available online 27 March 2019
ductivity tensor of NbO2 crystal. We measured the thermal conductivities of (1 1 0)-, (0 0 1)-, and (1 1 1)-
oriented NbO2 films and found h1 1 1i -direction shows 1 W m1 K1 higher thermal conductivity com-
pared with the other directions (3 W m1 K1). Using the measured j-values, we successfully deter-
mined thermal conductivity tensor components j11, j13, and j33. The diagonal components of the
thermal conductivity tensor were 2.5 W m1 K1 while the nonzero off-diagonal component was
1 W m1 K1. We believe that the present results are of great value in optimizing the performance of
NbO2 based devices.
Ó 2019 Elsevier Ltd. All rights reserved.

1. Introduction group of I41/a with the lattice parameters of a = 1.37 nm and

Transition metal oxides exhibiting metal-to-insulator transi-
tions (MIT) are considered to be promising candidates for next gen-
eration non-volatile resistive random-access memory (RRAM)
applications [1–4]. As memory devices are constantly exposed to
read/reset pulses, they are always exposed to high heat accumula-
tion rates, and thermal stability is one of the key issues in the
materials selection [5]. For this reason, NbO2 is gaining interest
in the RRAM community [6–10] since it has high MIT temperature
( 1080 K) [11,12] and therefore high thermal stability. The
approaches vary from local joule heating [13,14] to utilizing elec-
troforming current to change its oxidation states [15,16]. In all
cases, understanding the thermal conductivity of NbO2 is essential
for the device optimization. However, it has been largely over-
looked compared to the electrical properties because there is a lack
of studies in literature on the thermal conductivity characteriza-
tion of NbO2.
One of the difficulties in measuring the thermal conductivity of
NbO2 comes from its anisotropic crystal structure. Fig. 1 schemat-
ically represents the unit cell of NbO2 crystal at room temperature.
The crystal structure of NbO2 is tetragonal and belongs to the space
⇑ Corresponding author at: Research Institute for Electronic Science, Hokkaido
University, N20W10, Kita, Sapporo 001-0020, Japan.
E-mail address: joon@es.hokudai.ac.jp (H.J. Cho).
1
Equally contributed to this work.
c = 0.599 nm [12]. In NbO2, the NbO6 octahedrons are connected
at their edges (side lines) along [0 0 1] direction whereas they
are connected at their corners (end points) in the other directions.
Very recently, Kim et al. [17] reported that epitaxial NbO2 films
grown on a-Al2O3 substrates exhibit anisotropic electron trans-
h i
port: the carrier effective mass (m*) in 1 1 2 direction is
h  i
0.05 m0 whereas that in 1 1 0 and [0 0 1] directions are much
h  i
heavier ( 1 1 0 : 1 m0, [0 0 1]: 0.8 m0). The electron trans-
portation in semiconducting oxides is strongly affected by the elec-
tron–phonon collisions, which is related to the vibrational
properties of the lattice. In addition, the elasticity tensor of NbO2
shows anisotropy along its major axes and nonzero off-diagonal
terms [18,19]. All physical properties of NbO2 suggest that its ther-
mal conductivity would be anisotropic.
In this study, we measured the thermal conductivities along
[1 1 0]-, [0 0 1]-, and [1 1 1]-directions using the (1 1 0)-, (0 0 1)-,
and (1 1 1)-oriented NbO2 films and found [1 1 1]-direction shows
1 W m1 K1 higher thermal conductivity compared with the
other directions. In order to clarify the heat conduction in NbO2
crystal, we extracted the full thermal conductivity tensor ( j b ) from
the observed thermal conductivities. j b has 6 independent terms. In
case of NbO2, this can be reduced to 3 independent terms because
of its 4-fold symmetry in the ab-plane. In a matrix representation,
it looks as follows:

https://doi.org/10.1016/j.ijheatmasstransfer.2019.03.135
0017-9310/Ó 2019 Elsevier Ltd. All rights reserved.
264 H.J. Cho et al. / International Journal of Heat and Mass Transfer 137 (2019) 263–267
Fig. 1. Schematic crystal structure of NbO2 at room temperature. Projection along the normal to (a) (0 0 1), (b) (1 1 0), (c) (1 1 1), and (d) [1 1 2]. The space group is I41/a and
the lattice parameters are a = 1.37 nm and c = 0.599 nm [12]. Note that the NbO6 octahedrons are connected at their edges (side lines) in [0 0 1] direction whereas they are
connected at their corners (end points) in other directions.
0 1 0 1
j11 j12 j13 j11 0 j13
B C B C
jb NbO2 ¼ @ j12 j22 j23 A ! @ 0 j11 j13 A
j13 j23 j33 j13 j13 j33
where the subscripts 1, 2, and 3 refer to a-, b-, and c-axis of NbO2,
respectively. Using the thermal conductivities in three different
directions of [1 1 0], [0 0 1], and [1 1 1], we successfully determined
j
b NbO2 . The components of j b NbO2 were converted to the total thermal
conductivity (jtot) using tensor coordinate transformations (Sup-
plementary), and the resulting system of non-linear equations
were solved to obtain all components of j b NbO2 (Eq. (1)). We believe
the present results are significantly important for understanding
the heat accumulations in NbO2 based devices, which are critical
for enhancing their performance.
2. Materials and methods
Using RF magnetron sputtering, NbO2 films with three different
crystallographic orientations were grown on (0 0 0 1) a-Al2O3, (1 0
 
1 0) a-Al2O3 and (1 1 0 2) a-Al2O3 substrates (Crystal Bank at Pusan
National University), respectively. The films were grown at 650 °C
under 2.5–5 mTorr of Ar/H partial pressure. The details of our NbO2
film growth condition are described elsewhere [17]. The film thick-
nesses (t) and crystallographic orientations were analyzed by X-ray
diffraction (HRXRD, Cu Ka1 radiation, ATX-G, Rigaku Co.). The total
thermal conductivity (jtot) of the resultant NbO2 films were mea-
sured in the out-of-plane direction with time-domain thermo-
reflectance (TDTR, pump beam wavelength: 775 nm, probe beam
wavelength: 1550 nm, pulse duration: 1 ps, pulse frequency:
20 MHz method, PicoTR, PicoTherm Co.) at room temperature.
Metallic Mo films (100 nm), which were used as the transducer,
were deposited on the top surface of the NbO2 films by d.c. mag-
netron sputtering method at room temperature.
3. Results and discussion
Fig. 2 shows the out-of-plane XRD patterns [Fig. 2(a)] and the
rocking curves (OXRCs) [Fig. 2(b)] of the resultant NbO2 films. Only
intense diffraction peaks of 1 1 0 (top), 0 0 1 (middle), and 1 1 1
ð1Þ (bottom) NbO2 are seen together with the a-Al2O3 diffraction
peaks in Fig. 2(a), indicating that highly oriented single phase
NbO2 films were grown on the a-Al2O3 substrates. Full-width at
half maximum (FWHM) of the OXRCs of 4 4 0 NbO2 (top) and
2 2 2 NbO2 (bottom) are 0.02°, which corresponds to the resolu-
tion of our X-ray diffractometer, indicating strong 1 1 0 and 1 1 1
orientation of the films while that of 004 NbO2 (middle) is a bit
broader (0.76°). From these results, the out-of-plane orientation
of the resultant films were clarified as [(1 1 0) NbO2k(0 0 0 1) a-
 
Al2O3], [(0 0 1) NbO2k(1 0 1 0) a-Al2O3] and [(1 1 1) NbO2k(1 1 0
2) a-Al2O3]. From the X-ray reflection measurements (data not
shown), the film thickness of the (1 1 0)-, (0 0 1)-, and (1 1 1)-
oriented films were clarified 68, 52, and 72 nm, respectively, which
were sufficiently thick for the films to behave like bulk materials
(30 nm, Supplementary Table S1) [20].
Fig. 3 summarizes the thermo-reflectance signals from the
NbO2 films grown on a-Al2O3 substrates at room temperature.
Sharp increase and decay curves before 2 ns are due to the Mo
transducer. The decay of (1 1 1)-oriented NbO2 film is slightly fas-
ter than (1 1 0)- and (0 0 1)-oriented NbO2 films, clearly indicating
that jtot in the (1 1 1) direction is higher than that in the (1 1 0)
and (0 0 1) directions. We analyzed the thermo-reflectance decay
curves with the software package provided by the manufacturer
and obtained the jtot of 3.0 W m1 K1 for (1 1 0), 2.9 W m1 K1
for (0 0 1), and 4.0 W m1 K1 for (1 1 1), respectively.
Acoustic longitudinal phonons usually dominate the lattice
thermal conductivity [21–23]. While the presence of soft phonons
in the phonon dispersion relations makes it challenging to obtain
detailed phonon transport characteristics of NbO2 [24], the speed
of acoustic longitudinal phonons can be estimated with the its
elastic stiffness constants [18,19]. According to our calculations,
the speed of elastic longitudinal waves along [1 1 1], [1 1 0], and
[0 0 1] are 8476 m s1, 7978 m s1, and 8109 m s1, respectively
(Supplementary). Therefore, the high thermal conductivity
observed from the (1 1 1) oriented film is attributed to the speed
of acoustic longitudinal phonons. We would like to note that the
observed thermal conductivities are not proportional to the calcu-
lated acoustic longitudinal phonon speeds, and the calculation
 H.J. Cho et al. / International Journal of Heat and Mass Transfer 137 (2019) 263–267 265

Fig. 2. Crystallographic orientation of the resultant NbO2 films. (a) Out-of-plane X-ray Bragg diffraction patterns and (b) corresponding out-of-plane X-ray rocking curves
(OXRCs) of the resultant NbO2 films. Only intense diffraction peaks of 1 1 0 (top), 0 0 1 (middle), and 1 1 1 (bottom) NbO2 are seen together with the a-Al2O3 diffraction peaks
in (a), indicating that highly oriented single phase NbO2 films were grown on the a-Al2O3 substrates. FWHM of the OXRCs of 4 4 0 NbO2 (top) and 222 NbO2 (bottom) are
0.02°, which corresponds to the resolution of our X-ray diffractometer, indicating strong 1 1 0 and 1 1 1 orientation of the films, while that of 0 0 4 NbO2 (middle) is a bit
broader (0.76°).

are mainly populated near P point (Brillouin Zone edge along

Fig. 3. Thermo-reflectance signal of the NbO2 films grown on a-Al2O3 substrates at
room temperature. Sharp increase and decay curves until 2 ns are due to the Mo
transducer. The decay of (1 1 1)-oriented NbO2 film is slightly faster than (1 1 0)-
and (0 0 1)-oriented NbO2 films, clearly indicating that jtot in the (1 1 1) direction is
higher than that in the (1 1 0) and (0 0 1) directions. Using these thermo-reflectance
decay curves, we obtained the jtot of 3.0 W m1 K1 for (1 1 0), 2.9 W m1 K1 for
(0 0 1), and 4.0 W m1 K1 for (0 0 1), respectively.
results only explain why (1 1 1) film shows the highest thermal
conductivity. To fully explain the observed thermal conductivities,
it is necessary to understand the coupling of soft phonons, which
[1 1 1]). Since these phonons are shear waves along [1 1 1] with
large displacement fields [7], one possibility is anisotropic soft
phonon scattering effect. In this scenario, soft phonon scattering
would reduce the thermal transport properties along [0 0 1] and
[1 1 0] films whereas its effect on the [1 1 1] longitudinal waves
will be relatively small since their displacement fields ([1 1 1] lon-
gitudinal and transverse) are perpendicular. At elevated tempera-
tures, as phonon softening will be compensated by an increase in
the phonon population, the soft phonon effect will be enhanced,
and the anisotropy will likely increase.
The observed thermal conductivity jtot is sum of the lattice
thermal conductivity (jlat) and the electron thermal conductivity
(jele). In order to estimate the maximum contribution of carrier
electrons (jele) to the observed jtot, we measured the in-plane
electrical resistivity (q) of the NbO2 films by the d.c. four-probe
method in van der Pauw electrode configuration at room temper-
ature (Table 1). The q values of (1 1 0)-, (0 0 1)-, and (1 1 1)-
oriented films were 51, 2, and 51 X cm, respectively. Using these
q values, we estimated jele assuming the Wiedemann-Franz law
(jele = LrT, where L is the Lorenz number of a free electron gas
(2.45  108 W X1 K2) [25], r is the electrical conductivity
(=q1), and T is the absolute temperature). While the
Wiedemann-Franz law is often not suitable for describing mobile
electrons in oxides [26], it does offer reasonable estimations for
the upper bound for jele. Note that the jele values are negligibly
small (<4  104 W m1 K1) as compared with jtot. Therefore,
we concluded that the heat transportation in NbO2 crystal is
mostly dominated by lattice vibrations (phonons, jlat).
266 H.J. Cho et al. / International Journal of Heat and Mass Transfer 137 (2019) 263–267

Table 1
Anisotropic thermal conductivity of the NbO2 films at room temperature. Total thermal conductivity (jtot) in the out-of-plane direction, in-plane resistivity (q), and electron
thermal conductivity (jele) assumed with Wiedemann-Franz law of the (1 1 0)-, (0 0 1)-, and (1 1 1)-oriented NbO2 films are listed. (1 1 1)-oriented film shows higher jtot
compared with (1 1 0)- and (0 0 1)-oriented films. Note that the jele values are negligibly small compared to jtot.

Orientations t (nm) jtot (out-of-plane, Wm1K1) q (in-plane, Xcm) jele (Wm1K1)

(1 1 0) 68 3.0 51 1.4  105
(0 0 1) 52 2.9 2 3.7  104
(1 1 1) 72 4.0 51 1.4  105

The q of (1 1 0) and (1 1 1) oriented NbO2 films are within Eqs. (4a)–(4c) have two different sets of solutions: (k11 ,
agreements with our previous studies [17]. However, the q of k13 ; k33 Þ= (2.60, 1.06, 2.48) W m1 K1 and (1.60, 1.79, 1.41) W
(0 0 1) film was noticeably lower than that of the other two films. m1 K1. In this case, elasticity can be used to choose a more
This implies the presence of oxygen vacancies [27], which may be appropriate solution since propagation of elastic waves can be rea-
attributed to the large lattice mismatch (1.75% and 10.6%) between sonable estimations for the propagation of phonons. According to

the (1010) a-Al2O3 substrate and (0 0 1) NbO2 [12,28]. As oxygen previous studies, the terms in the elasticity of NbO2 representing
vacancies can affect the thermal conductivity [29,30], their effects compression/tension are always greater than the terms represent-
ing shear [19]. This suggests the latter solution needs to be dis-
must be quantified to avoid mischaracterizing j b NbO2 . To examine
carded since its off-diagonal term is greater than the two
the effect of oxygen vacancies on jtot of our NbO2 films, we slightly
diagonal terms, which is highly unlikely. Therefore, if a-, b-, and
adjusted the sputter deposition condition to fabricate oxygen defi-
cient NbO2x films and measured their thermal conductivities c-axes of the NbO2 unit cell are used as the Cartesian axes, jb NbO2
(Supplementary Table S1). The q values of NbO2x films were is expressed by the following matrix:
orders of magnitude lower than the q values in Table 1, but jtot 0 1
2:60 0 1:06
values remained almost unchanged. These results confirm that
b NbO2 ¼ B
j @ 0
C
2:60 1:06 A W m1 K1 ð@300 KÞ ð4Þ
the effect oxygen deficiency on the jtot of our NbO2 films is negli-
gibly small. 1:06 1:06 2:48
Here we show the thermal conductivity tensor, j b NbO2 . Eq. (1)
Using the j
b NbO2 , one can calculate the heat flux in NbO2 along
describes j NbO2 when the c-axis of the film is perpendicular to its
b
any directions, which is useful for understanding the heat flux in
top surface. Since the orientations of the NbO2 films are not iden- NbO2 based devices.
tical, j
b NbO2 needs to be transformed accordingly to properly inter-
pret jtot observed from differently oriented films. The following
4. Conclusion
matrices represent j b NbO2 of (1 1 0) and (1 1 1) oriented films in a
Cartesian coordinate when b z -axis is perpendicular to the substrate
In summary, we successfully clarified the full thermal conduc-
(See Supplementary information):
tivity tensor of NbO2 for the first time using the thermal conductiv-
0 pffiffiffi 1
j33 0 2j13 ity values of (0 0 1)-, (1 1 0)-, and (1 1 1)-oriented NbO2 films
B C
jb NbO2 ;ð110Þ ¼@ 0 j11 0 A ð2aÞ grown on a-Al2O3 substrates. Using the (1 1 0)-, (0 0 1)-, and
pffiffiffi (1 1 1)-oriented NbO2 films, we measured the thermal conductivity
2j13 0 j11 of [1 1 0]-, [0 0 1]-, and [1 1 1]-directions and found [1 1 1]-

 pffiffi pffiffi
jb NbO2 ;ð111Þ ¼ 1
3
ð j11  4j13 þ 2j33 Þ0 32 ðj11  j13  j33 Þ0j11 0 32 ðj11  j13  j33 Þ013 ð2j11 þ 4j13 þ j33 ÞÞ ð2bÞ

where j b NbO2 ;ðhklÞ represents the thermal conductivity tensor of the direction shows 1 W m1 K1 higher thermal conductivity com-
! pared with the other directions (3 W m1 K1). The diagonal
(hkl)-oriented NbO2 film. The heat flux j in the film induced by
! components of the thermal conductivity tensor were 2.5 W m1
the temperature gradient r T across the film can be written as: K1 while the nonzero off-diagonal component was 1 W m1
! ! K1. These results will be essential for understanding the flow of
j ¼ j
b NbO2 ;ðhklÞ r T ð3Þ
heat in NbO2 based devices, which is critical for their design and
During TDTR measurements, the pump laser creates a tempera- efficiency optimization.
ture difference across the film, and the resulting signal reflects the
!
total heat flux leaving the top surface. Therefore, r T = (0, 0, rT) Conflicts of interest
!
 
and jtot ¼  j =rT. This yields 3 different coupled non-linear equa-
There are no conflicts of interest to declare.
tions (See Supplementary information):

qffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi Acknowledgements
jtot½001 ¼ k33 þ 2k13 ¼ 2:9Wm1 K1
2 2
ð4aÞ
H.J. and H.O. are supported by the Korea-Japan bilateral program
qffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
funded from following programs of each country: International
jtot½110 ¼ k11 þ 2k13 ¼ 3:0Wm1 K1
2 2
ð4bÞ
cooperation program by the NRF (NRF-2018K2A9A2A08000079)
rffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
  and JSPS. H.O. is supported by Grants-in-Aid for Scientific Research
1
jtot½111 ¼ 2 k11  k13  k33 Þ þ 2k11 þ 4k13 þ k33 Þ ¼ 4:0Wm1 K1
2 2 A (17H01314) from the JSPS, the Asahi Glass Foundation, and the
3 Mitsubishi Foundation. Student aids from JSPS (T. Onozato, No.
ð4cÞ 17J01281) is also greatly appreciated.
 H.J. Cho et al. / International Journal of Heat and Mass Transfer 137 (2019) 263–267
Appendix A. Supplementary material
Supplementary data to this article can be found online at
https://doi.org/10.1016/j.ijheatmasstransfer.2019.03.135.
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