An experimental study was conducted on controlling the growth mode of La0.7Sr0.3MnO3 thin films on SrTiO3 substrates using pulsed laser deposition (PLD) by tuning growth temperature, pressure, and laser fluence. Different thin film morphology, crystallinity, and stoichiometry have been observed depending on growth parameters. To understand the microscopic origin, the adatom nucleation, step advance processes, and their relationship to film growth were theoretically analyzed and a growth diagram was constructed. Three boundaries between highly and poorly crystallized growth, 2D and 3D growth, stoichiometric and non-stoichiometric growth were identified in the growth diagram. A good fit of our experimental observation with the growth diagram was found. This case study demonstrates that a more comprehensive understanding of the growth mode in PLD is possible.

1.
D. B.
Chrisey
and
G. K.
Hubler
,
Pulse Laser Deposition of Thin Films
(
Wiley-Interscience
,
1994
).
2.
H. M.
Christen
and
G.
Eres
,
J. Phys.: Condens. Matter
20
,
264005
(
2008
).
3.
A.
Ohtomo
and
H. Y.
Hwang
,
Nature
427
,
423
(
2004
).
4.
D. P.
Norton
,
Mater. Sci. Eng. R
43
,
139
(
2004
).
5.
H. W.
Jang
,
D. A.
Felker
,
C. W.
Bark
,
Y.
Wang
,
M. K.
Niranjan
,
C. T.
Nelson
,
Y.
Zhang
,
D.
Su
,
C. M.
Folkman
,
S. H.
Baek
,
S.
Lee
,
K.
Janicka
,
Y.
Zhu
,
X. Q.
Pan
,
D. D.
Fong
,
E. Y.
Tsymbal
,
M. S.
Rzchowski
, and
C. B.
Eom
,
Science
331
,
886
(
2011
).
6.
T. J.
Jackson
and
S. B.
Palmer
,
J. Phys. D: Appl. Phys.
27
,
1581
(
1994
).
7.
P. R.
Willmott
and
J. R.
Huber
,
Rev. Mod. Phys.
72
,
315
(
2000
).
8.
P. R.
Willmott
,
Prog. Surf. Sci.
76
,
163
(
2004
).
9.
M. N. R.
Ashfold
,
F.
Claeyssens
,
G. M.
Fuge
, and
S. J.
Henley
,
Chem. Soc. Rev.
33
,
23
(
2004
).
10.
I. V.
Markov
,
Crystal Growth for Beginners: Fundamentals of Nucleation, Crystal Growth and Epitaxy
, 2nd ed. (
World Scientific Publishing Company
,
2003
).
11.
A.
Infortuna
,
A. S.
Harvey
, and
L. J.
Gauckler
,
Adv. Funct. Mater.
18
,
127
(
2008
).
12.
D.
Kan
and
Y.
Shimakawa
,
Appl. Phys. Lett.
99
,
081907
(
2011
).
13.
A.
Ohtomo
and
H. Y.
Hwang
,
J. Appl. Phys.
102
,
83704
(
2007
).
14.
S. K.
Sinha
,
R.
Bhattacharya
,
S. K.
Ray
, and
I.
Manna
,
Mater. Lett.
65
,
146
(
2011
).
15.
S.
Metev
and
K.
Meteva
,
Appl. Surf. Sci.
43
,
402
(
1989
).
16.
W.
Hong
,
H. N.
Lee
,
M.
Yoon
,
H. M.
Christen
,
D. H.
Lowndes
,
Z.
Suo
, and
Z.
Zhang
,
Phys. Rev. Lett.
95
,
95501
(
2005
).
17.
H. Y.
Hwang
,
S.-W.
Cheong
,
N. P.
Ong
, and
B.
Batlogg
,
Phys. Rev. Lett.
77
,
2041
(
1996
).
18.
J. D.
Ferguson
,
Y.
Kim
,
L. F.
Kourkoutis
,
A.
Vodnick
,
A. R.
Woll
,
D. A.
Muller
, and
J. D.
Brock
,
Adv. Mater.
23
,
1226
(
2011
).
19.
X.
Hong
,
A.
Posadas
,
A.
Lin
, and
C. H.
Ahn
,
Phys. Rev. B
68
,
134415
(
2003
).
20.
S.
Brivio
,
C.
Magen
,
A. A.
Sidorenko
,
D.
Petti
,
M.
Cantoni
,
M.
Finazzi
,
F.
Ciccacci
,
R.
De Renzi
,
M.
Varela
,
S.
Picozzi
, and
R.
Bertacco
,
Phys. Rev. B
81
,
94410
(
2010
).
21.
D.
Sun
,
L.
Yin
,
C.
Sun
,
H.
Guo
,
Z.
Gai
,
X.-G.
Zhang
,
T. Z.
Ward
,
Z.
Cheng
, and
J.
Shen
,
Phys. Rev. Lett.
104
,
236602
(
2010
).
22.
A.
Chen
,
Z.
Bi
,
C.-F.
Tsai
,
L.
Chen
,
Q.
Su
,
X.
Zhang
, and
H.
Wang
,
Cryst. Growth Des.
11
,
5405
(
2011
).
23.
A.
Chen
,
Z.
Bi
,
C.-F.
Tsai
,
J.
Lee
,
Q.
Su
,
X.
Zhang
,
Q.
Jia
,
J. L.
MacManus-Driscoll
, and
H.
Wang
,
Adv. Funct. Mater.
21
,
2423
(
2011
).
24.
F.
Tsui
,
M. C.
Smoak
,
T. K.
Nath
, and
C. B.
Eom
,
Appl. Phys. Lett.
76
,
2421
(
2000
).
25.
H.-Y.
Zhai
,
J. X.
Ma
,
D. T.
Gillaspie
,
X. G.
Zhang
,
T. Z.
Ward
,
E. W.
Plummer
, and
J.
Shen
,
Phys. Rev. Lett.
97
,
167201
(
2006
).
26.
T. Z.
Ward
,
S.
Liang
,
K.
Fuchigami
,
L. F.
Yin
,
E.
Dagotto
,
E. W.
Plummer
, and
J.
Shen
,
Phys. Rev. Lett.
100
,
247204
(
2008
).
27.
See supplementary material at http://dx.doi.org/10.1063/1.4811187 for more detailed information of nucleation, diffusion and step advance, thermodynamics of phase transition and features of poorly and well crystallized growth.
28.
A.
Thompson
,
I.
Lindau
,
D.
Attwood
,
Y.
Liu
,
E.
Gullikson
,
P.
Pianetta
,
M.
Howells
,
A.
Robinson
,
K. J.
Kim
,
J.
Scofield
,
J.
Kirz
,
J.
Underwood
,
J.
Kortright
,
G.
Williams
, and
H.
Winick
,
X-Ray Data Booklet
(
Lawrence Berkeley National Laboratory
,
2009
).
29.
See http://www.veeco.com/pdfs/mbe/vapor-pressure-Chart-1.pdf for information about vapor pressures of different elements as a function of temperature.
30.
I.
Ohkubo
,
H. M.
Christen
,
S. V.
Kalinin
,
J. G. E.
Jellison
,
C. M.
Rouleau
, and
D. H.
Lowndes
,
Appl. Phys. Lett.
84
,
1350
(
2004
).
31.
M.
Volmer
and
A.
Weber
,
Z. Phys. Chem.
119
,
277
(
1926
).
32.
F. C.
Frank
and
J. H.
van der Merwe
,
Proc. R. Soc. London, Ser. A
198
,
205
(
1949
).
33.
I.
Stranski
and
L.
Krastanov
,
Sitzugnsber. Akad. Wiss. Wien, Math.-Naturwiss. Kl., Abt. 2B
146
,
797
(
1938
).
34.
M.
Kareev
,
S.
Prosandeev
,
B.
Gray
,
J.
Liu
,
P.
Ryan
,
A.
Kareev
,
E. J.
Moon
, and
J.
Chakhalian
,
J. Appl. Phys.
109
,
114303
(
2011
).
35.
W.
Wang
,
Z.
Gai
,
M.
Chi
,
J. D.
Fowlkes
,
J.
Yi
,
L.
Zhu
,
X.
Cheng
,
D. J.
Keavney
,
P. C.
Snijders
,
T. Z.
Ward
,
J.
Shen
, and
X.
Xu
,
Phys. Rev. B
85
,
155411
(
2012
).
36.
G. H.
Lee
,
B. C.
Shin
, and
B. H.
Min
,
Mater. Sci. Eng., B
95
,
137
(
2002
).
37.
J.
Shin
,
S. V.
Kalinin
,
A. Y.
Borisevich
,
E. W.
Plummer
, and
A. P.
Baddorf
,
Appl. Phys. Lett.
91
,
202901
(
2007
).
38.
M.
Koubaa
,
A. M.
Haghiri-Gosnet
,
R.
Desfeux
,
P.
Lecoeur
,
W.
Prellier
, and
B.
Mercey
,
J. Appl. Phys.
93
,
5227
(
2003
).

Supplementary Material

You do not currently have access to this content.