The superlattice (SL) structure, which can efficiently suppress phonon thermal transport, has important implications for materials design in thermal insulating and thermoelectric applications. In this work, we prepare periodic ultra-high-temperature ceramic SLs made of transition metal carbides HfC and TaC with SL interface spacing ranging from 9.5 to 84.5 nm. The measured cross-plane phonon thermal conductivity displays a crossover dependence on SL interface spacing, achieving a minimum value of 0.84 W m−1 K−1 at room temperature. Moreover, the SLs with small interface spacing (9.5 and 14.7 nm) even show higher thermal conductivity than the constituent materials. The interfacial thermal resistance for HfC/TaC interface is determined from both a prepared single-interface double-layer sample and the thermal conductivity data of SLs, which is found to be a considerably large value for ceramic material interfaces. We further resolve the electron and phonon components of the interfacial thermal resistance. Finally, thermal stability of SLs is evaluated at 1200 °C in air, and a thin HfO2 cap layer is shown to effectively protect against high-temperature oxidation and preserve the thermal insulating property to a good extent.

1.
R. M.
Costescu
,
D. G.
Cahill
,
F. H.
Fabreguette
,
Z. A.
Sechrist
, and
S. M.
George
,
Science
303
(
5660
),
989
(
2004
).
2.
C.
Chiritescu
,
D. G.
Cahill
,
N.
Nguyen
,
J.
David
,
A.
Bodapati
,
P.
Keblinski
, and
P.
Zschack
,
Science
315
(
5810
),
351
(
2007
).
3.
X.
Liang
and
D. R.
Clarke
,
Acta Mater.
63
,
191
(
2014
);
X.
Liang
and
D. R.
Clarke
,
J. Appl. Phys.
124
(
2
),
025101
(
2018
).
4.
X.
Liang
,
M.
Baram
, and
D. R.
Clarke
,
Appl. Phys. Lett.
102
(
22
),
5
(
2013
).
5.
X.
Liang
,
L.
Shen
, and
C.
Wang
,
Nano Energy
59
,
651
(
2019
).
6.
J. H.
Perepezko
,
Science
326
(
5956
),
1068
(
2009
);
[PubMed]
N. P.
Padture
,
M.
Gell
, and
E. H.
Jordan
,
Science
296
(
5566
),
280
(
2002
);
[PubMed]
D. R.
Clarke
and
C. G.
Levi
,
Annu. Rev. Mater. Res.
33
(
1
),
383
(
2003
);
D. R.
Clarke
and
S. R.
Phillpot
,
Mater. Today
8
(
6
),
22
(
2005
);
D. R.
Clarke
,
M.
Oechsner
, and
N. P.
Padture
,
MRS Bull.
37
(
10
),
891
(
2012
).
7.
G. J.
Snyder
and
E. S.
Toberer
,
Nat. Mater.
7
(
2
),
105
(
2008
).
8.
R.
Cheaito
,
J. C.
Duda
,
T. E.
Beechem
,
K.
Hattar
,
J. F.
Ihlefeld
,
D. L.
Medlin
,
M. A.
Rodriguez
,
M. J.
Campion
,
E. S.
Piekos
, and
P. E.
Hopkins
,
Phys. Rev. Lett.
109
(
19
),
195901
(
2012
).
9.
C.
Perez
,
L.
Avazpour
,
M. K.
Eryilmaz
,
T.
Earles
,
S.
Ruder
,
V.
Gopalan
,
D.
Botez
,
I.
Knezevic
,
B.
Ramos-Alvarado
,
B. M.
Foley
, and
L. J.
Mawst
,
Appl. Phys. Lett.
121
(
23
),
232201
(
2022
).
10.
X.
Liang
,
H.
Wang
, and
C.
Wang
,
Acta Mater.
216
,
117160
(
2021
).
11.
S. M.
Lee
,
D. G.
Cahill
, and
T. H.
Allen
,
Phys. Rev. B
52
(
1
),
253
(
1995
).
12.
T.
Shang
,
J. Z.
Zhao
,
D. J.
Gawryluk
,
M.
Shi
,
M.
Medarde
,
E.
Pomjakushina
, and
T.
Shiroka
,
Phys. Rev. B
101
(
21
),
214518
(
2020
);
D.
Yan
,
D.
Geng
,
Q.
Gao
,
Z.
Cui
,
C.
Yi
,
Y.
Feng
,
C.
Song
,
H.
Luo
,
M.
Yang
,
M.
Arita
,
S.
Kumar
,
E. F.
Schwier
,
K.
Shimada
,
L.
Zhao
,
K.
Wu
,
H.
Weng
,
L.
Chen
,
X. J.
Zhou
,
Z.
Wang
,
Y.
Shi
, and
B.
Feng
,
Phys. Rev. B
102
(
20
),
205117
(
2020
).
13.
C.
Li
,
N. K.
Ravichandran
,
L.
Lindsay
, and
D.
Broido
,
Phys. Rev. Lett.
121
(
17
),
175901
(
2018
).
14.
M. V.
Simkin
and
G. D.
Mahan
,
Phys. Rev. Lett.
84
(
5
),
927
(
2000
).
15.
B.
Yang
and
G.
Chen
,
Phys. Rev. B
67
(
19
),
195311
(
2003
).
16.
Y.
Chen
,
D.
Li
,
J. R.
Lukes
,
Z.
Ni
, and
M.
Chen
,
Phys. Rev. B
72
(
17
),
174302
(
2005
);
A.
Chernatynskiy
,
R. W.
Grimes
,
M. A.
Zurbuchen
,
D. R.
Clarke
, and
S. R.
Phillpot
,
Appl. Phys. Lett.
95
(
16
),
161906
(
2009
);
J.
Ravichandran
,
A. K.
Yadav
,
R.
Cheaito
,
P. B.
Rossen
,
A.
Soukiassian
,
S. J.
Suresha
,
J. C.
Duda
,
B. M.
Foley
,
C.-H.
Lee
,
Y.
Zhu
,
A. W.
Lichtenberger
,
J. E.
Moore
,
D. A.
Muller
,
D. G.
Schlom
,
P. E.
Hopkins
,
A.
Majumdar
,
R.
Ramesh
, and
M. A.
Zurbuchen
,
Nat. Mater.
13
(
2
),
168
(
2014
);
[PubMed]
R.
Cheaito
,
C. A.
Polanco
,
S.
Addamane
,
J.
Zhang
,
A. W.
Ghosh
,
G.
Balakrishnan
, and
P. E.
Hopkins
,
Phys. Rev. B
97
(
8
),
085306
(
2018
).
17.
J.
Garg
and
G.
Chen
,
Phys. Rev. B
87
(
14
),
140302
(
2013
).
18.
Y.
Wang
,
H.
Huang
, and
X.
Ruan
,
Phys. Rev. B
90
(
16
),
165406
(
2014
).
19.
H. J.
Cho
,
Y.
Wu
,
Y.-Q.
Zhang
,
B.
Feng
,
M.
Mikami
,
W.
Shin
,
Y.
Ikuhara
,
Y.-M.
Sheu
,
K.
Saito
, and
H.
Ohta
,
Adv. Mater. Interfaces
8
(
7
),
2001932
(
2021
).
20.
B.
Latour
,
S.
Volz
, and
Y.
Chalopin
,
Phys. Rev. B
90
(
1
),
014307
(
2014
);
T.
Juntunen
,
O.
Vänskä
, and
I.
Tittonen
,
Phys. Rev. Lett.
122
(
10
),
105901
(
2019
);
[PubMed]
Z.
Zhang
,
Y.
Guo
,
M.
Bescond
,
J.
Chen
,
M.
Nomura
, and
S.
Volz
,
Phys. Rev. Lett.
128
(
1
),
015901
(
2022
).
[PubMed]
21.
M. N.
Luckyanova
,
J.
Garg
,
K.
Esfarjani
,
A.
Jandl
,
M. T.
Bulsara
,
A. J.
Schmidt
,
A. J.
Minnich
,
S.
Chen
,
M. S.
Dresselhaus
,
Z.
Ren
,
E. A.
Fitzgerald
, and
G.
Chen
,
Science
338
(
6109
),
936
(
2012
).
22.
K.
Shinokita
,
K.
Reimann
,
M.
Woerner
,
T.
Elsaesser
,
R.
Hey
, and
C.
Flytzanis
,
Phys. Rev. Lett.
116
(
7
),
075504
(
2016
).
23.
J.
Chen
,
X. F.
Xu
,
J.
Zhou
, and
B. W.
Li
,
Rev. Mod. Phys.
94
(
2
),
50
(
2022
);
E. T.
Swartz
and
R. O.
Pohl
,
Rev. Mod. Phys.
61
(
3
),
605
(
1989
);
A.
Giri
and
P. E.
Hopkins
,
Adv. Funct. Mater.
30
,
1903857
(
2020
).
24.
C.
Monachon
,
L.
Weber
, and
C.
Dames
,
Annu. Rev. Mater. Res.
46
(
1
),
433
(
2016
).
25.
M.
Ruxandra
,
M. A.
Costescu
,
D. G.
Wall
,
J. P.
Review
, and
B.
Cahill
,
Phys. Rev. B
67
(
5
),
054302
(
2003
).
26.
Y.
Kan Koh
,
Y.
Cao
,
G.
David
, and
D.
Cahill
,
Adv. Funct. Mater.
19
(
4
),
610
(
2009
).
27.
S.
Ali
,
T.
Juntunen
,
S.
Sintonen
,
O. M. E.
Ylivaara
,
R. L.
Puurunen
,
H.
Lipsanen
,
I.
Tittonen
, and
S.-P.
Hannula
,
Nanotechnology
27
(
44
),
445704
(
2016
).
28.
S.-M.
Lee
,
D. G.
Cahill
, and
R.
Venkatasubramanian
,
Appl. Phys. Lett.
70
(
22
),
2957
(
1997
).
29.
E.
Ziade
,
J.
Yang
,
G.
Brummer
,
D.
Nothern
,
T.
Moustakas
, and
A.
Schmidt
,
Appl. Phys. Lett.
107
,
091605
(
2015
).
30.
R. B.
Wilson
,
B. A.
Apgar
,
W.-P.
Hsieh
,
L. W.
Martin
, and
D. G.
Cahill
,
Phys. Rev. B
91
(
11
),
115414
(
2015
).
31.
J. T.
Gaskins
,
G.
Kotsonis
,
A.
Giri
,
S.
Ju
,
A.
Rohskopf
,
Y.
Wang
,
T.
Bai
,
E.
Sachet
,
C. T.
Shelton
,
Z.
Liu
,
Z.
Cheng
,
B. M.
Foley
,
S.
Graham
,
T.
Luo
,
A.
Henry
,
M. S.
Goorsky
,
J.
Shiomi
,
M.
Jon-Paul
, and
E.
Patrick
,
Nano Lett.
18
(
12
),
7469
(
2018
).
32.
N.
Ye
,
J. P.
Feser
,
S.
Sadasivam
,
T. S.
Fisher
,
T.
Wang
,
C.
Ni
, and
A.
Janotti
,
Phys. Rev. B
95
(
8
),
085430
(
2017
).
33.
G. T.
Hohensee
,
R. B.
Wilson
, and
D. G.
Cahill
,
Nat. Commun.
6
(
1
),
6578
(
2015
).
34.
B. F.
Donovan
,
C. J.
Szwejkowski
,
J. C.
Duda
,
R.
Cheaito
,
J. T.
Gaskins
,
C.-Y. P.
Yang
,
C.
Constantin
,
R. E.
Jones
, and
P. E.
Hopkins
,
Appl. Phys. Lett.
105
(
20
),
161103
(
2014
).
35.
R. J.
Stevens
,
A. N.
Smith
, and
P. M.
Norris
,
J. Heat Transfer
127
(
3
),
315
(
2005
).
36.
X.
Qian
,
P.
Jiang
, and
R.
Yang
,
Mater. Today Phys.
3
,
70
(
2017
).
37.
R.
Cheaito
,
J. T.
Gaskins
,
M. E.
Caplan
,
B. F.
Donovan
,
B. M.
Foley
,
A.
Giri
,
J. C.
Duda
,
C. J.
Szwejkowski
,
C.
Constantin
,
H. J.
Brown-Shaklee
,
J. F.
Ihlefeld
, and
P. E.
Hopkins
,
Phys. Rev. B
91
(
3
),
035432
(
2015
).
38.
P. E.
Hopkins
,
P. M.
Norris
, and
R. J.
Stevens
,
J. Heat Transfer
130
(
2
),
022401
(
2008
).
39.
R. B.
Wilson
and
D. G.
Cahill
,
Nat. Commun.
5
(
1
),
5075
(
2014
).
40.
R. B.
Wilson
and
D. G.
Cahill
,
Phys. Rev. Lett.
108
(
25
),
255901
(
2012
).
41.
B. C.
Gundrum
,
D. G.
Cahill
, and
R. S.
Averback
,
Phys. Rev. B
72
(
24
),
245426
(
2005
).
42.
B. M.
Clemens
,
G. L.
Eesley
, and
C. A.
Paddock
,
Phys. Rev. B
37
(
3
),
1085
(
1988
).
43.
A.
Majumdar
and
P.
Reddy
,
Appl. Phys. Lett.
84
(
23
),
4768
(
2004
).
44.
H.-K.
Lyeo
and
D. G.
Cahill
,
Phys. Rev. B
73
(
14
),
144301
(
2006
).
45.
S. R. S.
Kumar
,
M. N.
Hedhili
,
D.
Cha
,
T. M.
Tritt
, and
H. N.
Alshareef
,
Chem. Mater.
26
(
8
),
2726
(
2014
);
P.
Chen
,
T.
Etzelstorfer
,
F.
Hackl
,
N. A.
Katcho
,
H.-T.
Chang
,
L.
Nausner
,
S.-W.
Lee
,
T.
Fromherz
,
J.
Stangl
,
O. G.
Schmidt
,
N.
Mingo
, and
A.
Rastelli
,
Phys. Status Solidi (a)
213
(
3
),
533
(
2016
).
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