Incorporation of functional metal oxides in organic devices enables the creation of electronic devices that have both the advantages of organic materials, such as flexibility and light weight, as well as those of metal oxide materials, such as optical transparency and stability against ambient air. However, developing high-performance organic/metal-oxide hybrid devices is challenging, because the deposition of a metal oxide onto an organic semiconductor layer severely damages the device for reasons that are not well understood. In this study, we clarified that the internal stress of the metal oxide is the cause of this damage. A hybrid device composed of an organic semiconductor layer sandwiched between two indium tin oxide electrodes was investigated as a typical organic/metal-oxide hybrid device. The internal stress in the metal oxide layer causes the formation of nanometer-order clearances at the weak bonding interface in the device; this damage reduces the electrical conductivity of the device by over two orders of magnitude. A method to control the internal stress of the metal oxide layer by introducing a gas that affects crystal growth during metal oxide deposition was developed, and an undamaged hybrid device was demonstrated by controlling the internal stress of the metal oxide. High-performance organic/metal-oxide hybrid devices without the damage may be key devices that open up electronics with features beyond those possible with the organic electronics and metal oxide electronics.

1.
S.
Kim
,
H.
Kwon
,
S.
Lee
,
H.
Shim
,
Y.
Chun
,
W.
Choi
,
J.
Kwack
,
D.
Han
,
M.
Song
,
S.
Kim
,
S.
Mohammadi
,
I.
Kee
, and
S. Y.
Lee
, “
Low-power flexible organic light-emitting diode display device
,”
Adv. Mater
23
,
3511
3516
(
2011
).
2.
D.
Di
,
A. S.
Romanov
,
L.
Yang
,
J. M.
Richter
,
J. P. H.
Rivett
,
S.
Jones
,
T. H.
Thomas
,
M. A.
Jalebi
,
R. H.
Friend
,
M.
Linnolahti
,
M.
Bochmann
, and
D.
Credgingtonet
, “
High-performance light-emitting diodes based on carbene-metal-amides
,”
Science
356
,
159
163
(
2017
).
3.
S.
Khan
,
L.
Lorenzelli
, and
R. S.
Dahiya
, “
Technologies for printing sensors and electronics over large flexible substrates
,”
IEEE Sens. J.
15
,
3164
3185
(
2015
).
4.
M.
Zirkl
,
A.
Haase
,
A.
Fian
,
H.
Schön
,
C.
Sommer
,
G.
Jakopic
,
G.
Leising
,
B.
Stadlober
,
I.
Graz
,
N.
Gaar
,
R.
Schwödiauer
,
S.
Bauer–Gogonea
, and
S.
Bauer
, “
Low-voltage organic thin-film transistors with high-k nanocomposite gate dielectrics for flexible electronics and optothermal sensors
,”
Adv. Mater.
19
,
2241
2245
(
2007
).
5.
T.
Someya
and
M.
Amagai
, “
Toward a new generation of smart skins
,”
Nat. Biotechnol.
37
,
382
(
2019
).
6.
G.
Schwartz
,
B. C.-K.
Tee
,
J.
Mei
,
A. L.
Appleton
,
D. H.
Kim
,
H.
Wang
, and
Z.
Bao
, “
Flexible polymer transistors with high pressure sensitivity for application in electronic skin and health monitoring
,”
Nat. Commun.
4
,
1859
(
2013
).
7.
C.
Wang
,
D.
Hwang
,
Z.
Yu
,
K.
Takei
,
J.
Park
,
T.
Chen
,
B.
Ma
, and
A.
Javey
, “
User-interactive electronic skin for instantaneous pressure visualization
,”
Nat. Mater.
12
,
899
904
(
2013
).
8.
A.
Bauer
,
T.
Wahl
,
J.
Hanisch
, and
E.
Ahlswede
, “
ZnO:Al cathode for highly efficient, semitransparent 4% organic solar cells utilizing TiOx and aluminum interlayers
,”
Appl. Phys. Lett.
100
,
073307
(
2012
).
9.
A.
Colsmann
,
A.
Puetz
,
A.
Bauer
,
J.
Hanisch
,
E.
Ahlswede
, and
U.
Lemmer
, “
Efficient semi-transparent organic solar cells with good transparency color perception and rendering properties
,”
Adv. Energy Mater.
1
,
599
603
(
2011
).
10.
H.
Schmidt
,
H.
Flügge
,
T.
Winkler
,
T.
Bülow
,
T.
Riedl
, and
W.
Kowalsky
, “
Efficient semitransparent inverted organic solar cells with indium tin oxide top electrode
,”
Appl. Phys. Lett.
94
,
243302
(
2009
).
11.
T.
Yokota
,
P.
Zalar
,
M.
Kaltenbrunner
,
H.
Jinno
,
N.
Matsuhisa
,
H.
Kitanosako
,
Y.
Tachibana
,
W.
Yukita
,
M.
Koizumi
, and
T.
Someya
, “
Ultraflexible organic photonic skin
,”
Sci. Adv.
2
,
e1501856
(
2016
).
12.
H.-K.
Kim
,
D.-G.
Kim
,
K.-S.
Lee
,
M.-S.
Huh
,
S. H.
Jeong
, and
K. I.
Kim
, “
Plasma damage-free sputtering of indium tin oxide cathode layers for top-emitting organic light-emitting diodes
,”
Appl. Phys. Lett
86
,
183503
(
2005
).
13.
S.
Dangtip
,
Y.
Hoshi
,
Y.
Kasahara
,
Y.
Onai
,
T.
Osotchan
,
Y.
Sawada
, and
T.
Uchida
, “
Study of low power deposition of ITO for top emission OLED with facing target and RF sputtering systems
,”
J. Phys.: Conf. Ser
100
,
042011
(
2008
).
14.
A. P.
Ghosh
,
L. J.
Gerenser
,
C. M.
Jarman
, and
J. E.
Fornalik
, “
Thin-film encapsulation of organic light emitting devices
,”
Appl. Phys. Lett
86
,
223503
(
2005
).
15.
J. S.
Hong
,
S. M.
Kim
, and
K.-H.
Kim
, “
Preparation of SiO2 passivation thin film for improved the organic light-emitting device life time
,”
Jpn. J. Appl. Phys., Part 1
50
,
08KE02
(
2011
).
16.
J.-G.
Kim
,
J.-H.
Lee
,
S.-I.
Na
,
H. H.
Lee
,
Y.
Kim
, and
H.-K.
Kim
, “
Semi-transparent perovskite solar cells with directly sputtered amorphous InZnSnO top cathodes for building integrated photovoltaics
,”
Org. Electron.
78
,
105560
(
2020
).
17.
K.
Suemori
,
S.
Hoshino
,
N.
Ibaraki
, and
T.
Kamata
, “
Effect of positively charged particles on sputtering damage of organic electroluminescent diodes with Mg:Ag alloy electrodes fabricated by facing target sputtering
,”
AIP Adv.
7
,
045014
(
2017
).
18.
W. J.
Boettinger
,
C. E.
Johnson
,
L. A.
Bendersky
,
K.-W.
Moon
,
M. E.
Williams
, and
G. R.
Stafford
, “
Whisker and hillock formation on Sn, Sn–Cu and Sn–Pb electrodeposits
,”
Acta Mater.
53
,
5033
5050
(
2005
).
19.
C. F.
Ma
,
F.
Wang
,
P.
Huang
,
T. J.
Lu
, and
K. W.
Xu
, “
Hillock growth in CuZr metallic glass
,”
Thin Solid Films
589
,
681
685
(
2015
).
20.
E.
Nishimura
,
T.
Sasabayashi
,
N.
Ito
,
Y.
Sato
,
K.
Utsumi
,
K.
Yano
,
A.
Kaijo
,
K.
Inoue
, and
Y.
Shigesato
, “
Structure and internal stress of tin-doped indium oxide and indium–zinc oxide films deposited by DC magnetron sputtering
,”
Jpn. J. Appl. Phys., Part 1
46
,
7806
7811
(
2007
).
21.
J.
Jou
,
M.
Han
, and
D.
Cheng
, “
Substrate dependent internal stress in sputtered zinc oxide thin films
,”
J. Appl. Phys.
71
,
4333
(
1992
).
22.
V.
Raghuwanshi
,
D.
Bharti
, and
S. P.
Tiwari
, “
Flexible organic field-effect transistors with TIPS-pentacene crystals exhibiting high electrical stability upon bending
,”
Org. Electron.
31
,
177
182
(
2016
).
23.
P.
Sony
,
P.
Puschnig
,
D.
Nabok
, and
C.
Ambrosch-Draxl
, “
Importance of van der Waals interaction for organic molecule-metal junctions: Adsorption of thiophene on Cu(110) as a prototype
,”
Phys. Rev. Lett.
99
,
176401
(
2007
).
24.
K.
Braun
and
S.
Hla
, “
Probing the conformation of physisorbed molecules at the atomic scale using STM manipulation
,”
Nano Lett.
5
,
73
76
(
2005
).
25.
L. S.
Hung
,
C. W.
Tang
,
M. G.
Mason
,
P.
Raychaudhuri
, and
J.
Madathil
, “
Application of an ultrathin LiF/Al bilayer in organic surface-emitting diodes
,”
Appl. Phys. Lett.
78
,
544
(
2001
).
26.
G.
Gu
,
V.
Bulović
,
P. E.
Burrows
,
S. R.
Forrest
, and
M. E.
Thompson
, “
Transparent organic light emitting devices
,”
Appl. Phys. Lett.
68
,
2606
2608
(
1996
).
27.
P.
Chaudhari
, “
Hillock growth in thin films
,”
J. Appl. Phys.
45
,
4339
4346
(
1974
).
28.
F.
Pei
,
N.
Jadhav
,
E.
Buchovecky
,
A. F.
Bower
,
E.
Chason
,
W.
Liu
,
J. Z.
Tischler
,
G. E.
Ice
, and
R.
Xu
, “
In-situ synchrotron micro-diffraction study of surface, interface, grain structure, and strain/stress evolution during Sn whisker/hillock formation
,”
J. Appl. Phys.
119
,
105302
(
2016
).
29.
W. K.
Man
,
H.
Yan
,
S. P.
Wong
,
I. H.
Wilson
, and
T. K. S.
Wong
, “
Grain size and hillock growth of vacuum evaporated SnO2 thin films
,”
J. Vac. Sci. Technol. A
14
,
1593
(
1996
).
30.
M.
Nie
,
A.
Bikowski
, and
K.
Ellmer
, “
Microstructure evolution of Al-doped zinc oxide and Sn-doped indium oxide deposited by radio-frequency magnetron sputtering: A comparison
,”
J. Appl. Phys.
117
,
155301
(
2015
).
31.
J. A.
Thornton
and
D. W.
Hoffman
, “
Stress-related effects in thin films
,”
Thin Solid Films
171
,
5
31
(
1989
).
32.
C. C.
Fang
,
F.
Jones
, and
V.
Prasad
, “
Effect of gas impurity and ion bombardment on stresses in sputter-deposited thin films: A molecular-dynamics approach
,”
J. Appl. Phys.
74
,
4472
4482
(
1993
).
33.
T. J.
Vink
,
W.
Walrave
,
J. L. C.
Daams
,
P. C.
Baarslag
, and
J. E. A. M.
Meerakker
, “
On the homogeneity of sputter-deposited ITO films Part I. Stress and microstructure
,”
Thin Solid Films
266
,
145
151
(
1995
).
34.
M.
Ando
,
E.
Nishimura
,
K.
Onisawa
, and
T.
Minemura
, “
Effect of microstructures on nanocrystallite nucleation and growth in hydrogenated amorphous indium–tin–oxide films
,”
J. Appl. Phys.
93
,
1032
1038
(
2003
).
35.
H.
Morikawa
and
M.
Fujita
, “
Crystallization and electrical property change on the annealing of amorphous indium-oxide and indium-tin-oxide thin films
,”
Thin Solid Films
359
,
61
67
(
2000
).
36.
H.
Hosono
,
Y.
Yamashita
,
N.
Ueda
,
H.
Kawazoe
, and
K.
Shimidzu
, “
New amorphous semiconductor: 2CdO⋅PbOx
,”
Appl. Phys. Lett.
68
,
661
663
(
1996
).
37.
H.
Hosono
,
N.
Kikuchi
,
N.
Ueda
,
H.
Kawazoe
, and
K.
Shimidzu
, “
Amorphous transparent electroconductor 2CdO⋅GeO2: Conversion of amorphous insulating cadmium germanate by ion implantation
,”
Appl. Phys. Lett.
67
,
2663
2665
(
1995
).
38.
M.
Schaer
,
F.
Nüesch
,
D.
Berner
,
W.
Leo
, and
L.
Zuppiroli
, “
Water vapor and oxygen degradation mechanisms in organic light emitting diodes
,”
Adv. Funct. Mater.
11
,
116
(
2001
).
39.
S.
Hoshino
,
M.
Yoshida
,
S.
Uemura
,
T.
Kodzasa
,
N.
Takada
,
T.
Kamata
, and
K.
Yase
, “
Influence of moisture on device characteristics of polythiophene-based field effect transistors
,”
J. Appl. Phys.
95
,
5088
(
2004
).
40.
J.
Jeong
and
H.
Kim
, “
Al2O3/Ag/Al2O3 multilayer thin film passivation prepared by plasma damage-free linear facing target sputtering for organic light emitting diodes
,”
Thin Solid Films
547
,
63
(
2013
).
41.
Y.
Noh
,
J.
Kim
,
S.
Kim
,
H.
Kim
, and
S.
Na
, “
Efficient semi-transparent perovskite solar cells with a novel indium zinc tin oxide top electrode grown by linear facing target sputtering
,”
J. Power Sources
437
,
226894
(
2019
).

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