Nonstoichiometric NiOx thin films were grown on single crystal substrates of c-plane (0001) sapphires by ion-beam sputter-deposition (IBSD) of a Ni metal target in a mixed argon and oxygen atmosphere. Structural characterization was carried out by X-ray diffraction and scanning electron microscopy. All samples grew (111)-oriented out-of-plane and with a defined in-plane orientation relationship relative to the crystalline substrate. The chemical bonding information of the films was examined by X-ray photoelectron spectroscopy showing that the composition x could be varied by adjusting the oxygen-to-argon ratio in the IBSD process. However, a growth anomaly was detected for a certain range of synthesis parameters, standing out due to an enhanced growth rate, nickel excess, and unusually elongated surface structures. With joint solid-state and plasma diagnostic tools, the underlying processes on the atomic scale were studied. An increased proportion of atomic oxygen species in the intermediate range of the oxygen-to-argon gas flux ratio was identified to be responsible for an enhanced generation of NiOx species. Optical emission spectroscopy was found to be a tool especially well-suited, since the in situ examination of various locations of interest (plasma, ion beam, and vicinity of the target) is feasible nonintrusively.

1.
K.
Kim
, “1.1 silicon technologies and solutions for the data-driven world,” in 2015 IEEE International Solid-State Circuits Conference—(ISSCC) (IEEE, 2015), Vol. 1.
2.
J. U.
Knickerbocker
,
P. S.
Andry
,
B.
Dang
,
R. R.
Horton
,
M. J.
Interrante
,
C. S.
Patel
,
R. J.
Polastre
,
K.
Sakuma
,
R.
Sirdeshmukh
,
E. J.
Sprogis
,
S. M.
Sri-Jayantha
,
A. M.
Stephens
,
A. W.
Topol
,
C. K.
Tsang
,
B. C.
Webb
, and
S. L.
Wright
,
IBM J. Res. Dev.
52
,
553
(
2008
).
3.
H.
Kim
,
S.-J.
Ahn
,
Y. G.
Shin
,
K.
Lee
, and
E.
Jun
, “Memory Workshop (IMW),” in IEEE International (IEEE, 2017), Vol. 1.
4.
C.
Kim
,
D.-H.
Kim
,
W.
Jeong
,
H.-J.
Kim
,
I. H.
Park
,
H.-W.
Park
,
J.
Lee
,
J.
Park
,
Y.-L.
Ahn
,
J. Y.
Lee
,
S.-B.
Kim
,
H.
Yoon
,
J. D.
Yu
,
N.
Choi
,
N.
Kim
,
H.
Jang
,
J.
Park
,
S.
Song
,
Y.
Park
,
J.
Bang
,
S.
Hong
,
Y.
Choi
,
M.-S.
Kim
,
H.
Kim
,
P.
Kwak
,
J.-D.
Ihm
,
D. S.
Byeon
,
J.-Y.
Lee
,
K.-T.
Park
, and
K.-H.
Kyung
,
IEEE J. Solid-State Circuits
53
,
124
(
2018
).
5.
S.
Inaba
, in 2018 IEEE International Memory Workshop (IMW) (IEEE, 2018), Vol. 1.
6.
S. Q.
Liu
,
N. J.
Wu
, and
A.
Ignatiev
,
Appl. Phys. Lett.
76
,
2749
(
2000
).
7.
S.
Seo
,
M. J.
Lee
,
D. H.
Seo
,
E. J.
Jeoung
,
D.-S.
Suh
,
Y. S.
Joung
,
I. K.
Yoo
,
I. R.
Hwang
,
S. H.
Kim
,
I. S.
Byun
,
J.-S.
Kim
,
J. S.
Choi
, and
B. H.
Park
,
Appl. Phys. Lett.
85
,
5655
(
2004
).
8.
Y.
Watanabe
,
J. G.
Bednorz
,
A.
Bietsch
,
C.
Gerber
,
D.
Widmer
, and
A.
Beck
,
Appl. Phys. Lett.
78
,
3738
(
2001
).
9.
M.-J.
Lee
,
Y.
Park
,
D.-S.
Suh
,
E.-H.
Lee
,
S.
Seo
,
D.-C.
Kim
,
R.
Jung
,
B.-S.
Kang
,
S.-E.
Ahn
,
C. B.
Lee
,
D. H.
Seo
,
Y.-K.
Cha
,
I.-K.
Yoo
,
J.-S.
Kim
, and
B. H.
Park
,
Adv. Mater.
19
,
3919
(
2007
).
10.
S.
Oswald
and
W.
Bruckner
,
Surf. Interface Anal.
36
,
17
(
2004
).
11.
D. G.
Hwang
,
C. M.
Park
, and
S. S.
Lee
,
J. Magn. Magn. Mater.
186
,
265
(
1998
).
12.
S.-S.
Lee
,
D.-G.
Hwang
,
C. M.
Park
,
K. A.
Lee
, and
J. R.
Rhee
,
J. Appl. Phys.
81
,
5298
(
1997
).
13.
D.-H.
Han
,
J.-G.
Zhu
,
J. H.
Judy
, and
J. M.
Sivertsen
,
J. Appl. Phys.
81
,
340
(
1997
).
14.
M.-H.
Lee
,
S.
Lee
, and
K.
Sin
,
Thin Solid Films
320
,
298
(
1998
).
15.
J. X.
Shen
and
M. T.
Kief
,
J. Appl. Phys.
79
,
5008
(
1996
).
16.
C.-H.
Lai
,
T. C.
Anthony
,
E.
Iwamura
, and
R. L.
White
,
IEEE Trans. Magn.
32
,
3419
(
1996
).
17.
M. J.
Carey
,
F. E.
Spada
,
A. E.
Berkowitz
,
W.
Cau
, and
G.
Thomas
,
J. Mater. Res.
6
,
2680
(
1991
).
18.
W.
Cao
,
G.
Thomas
,
M. J.
Carey
, and
A. E.
Berkowitz
,
Scr. Metall. Mater.
25
,
2633
(
1991
).
19.
D.-H.
Han
,
J.-G.
Zhu
, and
J. H.
Judy
,
J. Appl. Phys.
81
,
4996
(
1997
).
20.
C.-H.
Lai
,
H.
Matsuyama
,
R. L.
White
, and
T. C.
Anthony
,
IEEE Trans. Magn.
31
,
2609
(
1995
).
21.
C.-H.
Lai
,
T. J.
Regan
,
R. L.
White
, and
T. C.
Anthony
,
J. Appl. Phys.
81
,
3989
(
1997
).
22.
R. P.
Michel
,
A.
Chaiken
,
C. T.
Wang
, and
L. E.
Johnson
,
Phys. Rev. B
58
,
8566
(
1998
).
23.
J. R.
McNeil
,
J. J.
McNally
, and
P. D.
Reader
, “Ion beam deposition,” in Handbook of Thin Film Deposition, edited by K. Seshan (William Andrew, 2012).
24.
C.
Bundesmann
and
H.
Neumann
,
J. Appl. Phys.
124
,
231102
(
2018
).
25.
M.
Becker
,
M.
Gies
,
A.
Polity
,
S.
Chatterjee
, and
P. J.
Klar
,
Rev. Sci. Instrum.
90
,
023901
(
2019
).
26.
M.
Becker
,
A.
Polity
, and
P. J.
Klar
,
J. Appl. Phys.
122
,
175303
(
2017
).
27.
M.
Becker
,
F.
Michel
,
A.
Polity
, and
P. J.
Klar
,
Phys. Status Solidi B
255
,
1700463
(
2017
).
28.
M.
Becker
,
A.
Polity
,
P. J.
Klar
, and
B. K.
Meyer
,
Phys. Status Solidi RRL
9
,
326
(
2015
).
29.
I.
Hotový
,
J.
Huran
,
L.
Spiess
,
Š.
Haščík
, and
V.
Rehacek
,
Sens. Actuators B
57
,
147
(
1999
).
30.
S. J.
Han
,
S.
Kim
,
J.
Ahn
,
J. K.
Jeong
,
H.
Yang
, and
H. J.
Kim
,
RSC Adv.
6
,
71757
(
2016
).
31.
D. A.
Shirley
,
Phys. Rev. B
5
,
4709
(
1972
).
32.
A. N.
Mansour
,
Surf. Sci. Spectra
3
,
231
(
1994
).
33.
M.
Schulze
,
A.
Yanguas-Gil
,
A.
von Keudell
, and
P.
Awakowicz
,
J. Phys. D
41
,
065206
(
2008
).
34.
J. B.
Boffard
,
R. O.
Jung
,
C. C.
Lin
, and
A. E.
Wendt
,
Plasma Sources Sci. Technol.
18
,
035017
(
2009
).
35.
J.
Kaupe
,
D.
Coenen
, and
S.
Mitić
,
Plasma Sources Sci. Technol.
27
,
105003
(
2018
).
36.
J.
Kaupe
,
P.
Riedl
,
D.
Coenen
, and
S.
Mitić
,
Plasma Sources Sci. Technol.
28
,
065012
(
2019
).
37.
T.
Tsutsumi
,
A.
Greb
,
A. R.
Gibson
,
M.
Hori
,
D.
O’Connell
, and
T.
Gans
,
J. Appl. Phys.
121
,
143301
(
2017
).
38.
R. E.
Walkup
,
K. L.
Saenger
, and
G. S.
Selwyn
,
J. Chem. Phys.
84
,
2668
(
1986
).
39.
X.-M.
Zhu
and
Y.-K.
Pu
,
J. Phys. D
43
,
015204
(
2010
).
40.
O.
Zatsarinny
and
K.
Bartschat
,
J. Phys. B
37
,
4693
(
2004
).
41.
H. W.
Nesbitt
,
D.
Legrand
, and
G. M.
Bancroft
,
Phys. Chem. Miner.
27
,
357
(
2000
).
42.
K. S.
Kim
and
N.
Winograd
,
Surf. Sci.
43
,
625
(
1974
).
43.
N.
Fairley
, see http://www.casaxps.com/ebooks/ebooks.htm for “CasaXPS Webmanual,” Casa Software Ltd. (last accessed August 26, 2019).
44.
J. A.
Thornton
,
Ann. Rev. Mater. Sci.
7
,
239
(
1977
).
45.
U.
Fantz
,
Nucl. Fusion
46
,
297
(
2006
).
46.
V. N.
Ochkin
,
Spectroscopy of Low Temperature Plasma
(
John Wiley & Sons
,
2009
).
47.
X.-M.
Zhu
and
Y.-K.
Pu
,
Plasma Sources Sci. Technol.
17
,
024002
(
2008
).
48.
D. L.
Crintea
,
U.
Czarnetzki
,
S.
Iordanova
,
I.
Koleva
, and
D.
Luggenhölscher
,
J. Phys. D
42
,
045208
(
2009
).
49.
G. D.
Stancu
,
F.
Kaddouri
,
D. A.
Lacoste
, and
C. O.
Laux
,
J. Phys. D
43
,
124002
(
2010
).
50.
J. P.
Booth
,
O.
Joubert
, and
J.
Pelletier
,
J. Appl. Phys.
69
,
618
(
1991
).
51.
W.
Low
,
Phys. Rev.
109
,
247
(
1958
).
52.
R.
Newman
and
R. M.
Chrenko
,
Phys. Rev.
114
,
1507
(
1959
).
53.
R. J.
Powell
and
W. E.
Spicer
,
Phys. Rev. B
2
,
2182
(
1970
).
54.
V.
Propach
,
D.
Reinen
,
H.
Drenkhahn
, and
H.
Müller-Buschbaum
,
Z. Naturf.
33b
,
619
(
1978
).
55.
K. M.
Miedzinska
,
B. R.
Hollebone
, and
J. G.
Cook
,
J. Phys. Chem. Solids
49
,
1355
(
1988
).
56.
K. D.
Becker
and
F.
Rau
,
Ber. Bunsenges. Phys. Chem.
96
,
1017
(
1992
).
57.
T.
Tsuboi
and
W.
Kleemann
,
J. Phys. Condens. Matter
6
,
8625
(
1994
).
58.
R.
Tsu
and
L.
Esaki
, in Proceedings of 10th Internatioonal Conference on Physics of Semiconductors (US Atomic Energy Commission, 1970), pp. 282–285.
59.
C.
Díaz-Guerra
,
A.
Remón
,
J. A.
García
, and
J.
Piqueras
,
Phys. Status Solidi A
163
,
497
(
1997
).
60.
D.
Adler
and
J.
Feinleib
,
Phys. Rev. B
2
,
3112
(
1970
).
61.
A.
Gorschlüter
and
H.
Merz
,
Phys. Rev. B
49
,
17293
(
1994
).
62.
B.
Fromme
,
M.
Möller
,
Th.
Anschütz
,
C.
Bethke
, and
E.
Kisker
,
Phys. Rev. Lett.
77
,
1548
(
1996
).
63.
C.
Díaz-Guerra
and
J.
Piqueras
,
Solid State Commun.
104
,
763
(
1997
).
64.
D.
Jiménez-Rey
,
B.
Zurro
,
G.
García
,
A.
Baciero
,
L.
Rodríguez-Barquero
, and
M.
García-Munoz
,
J. Appl. Phys.
104
,
064911
(
2008
).
65.
V.
Veligura
,
G.
Hlawacek
,
R.
van Gastel
,
H. J. W.
Zandvliet
, and
B.
Poelsema
,
J. Lumin.
157
,
321
(
2015
).
You do not currently have access to this content.