We report molecular beam epitaxy growth of Sr-doped Bi2Se3 films on the (111) BaF2 substrate, aimed to realize unusual superconducting properties inherent to SrxBi2Se3 single crystals. Despite the wide range of the compositions, we do not achieve superconductivity. To explore the reason for this, we study the structural, morphological, and electronic properties of the films and compare them with the corresponding properties of the single crystals. The dependence of the c-lattice constant in the films on the Sr content appears to be more than an order of magnitude stronger than that in the crystals. Correspondingly, all other properties also differ substantially, indicating that Sr atoms get different positions in lattices. We argue that these structural discrepancies arise from essential differences in growth conditions. Our research calls for more detailed structural studies and novel growth approaches for the design of superconducting SrxBi2Se3 thin films.

1.
Y. S.
Hor
,
A. J.
Williams
,
J. G.
Checkelsky
,
P.
Roushan
,
J.
Seo
,
Q.
Xu
,
H. W.
Zandbergen
,
A.
Yazdani
,
N. P.
Ong
, and
R. J.
Cava
, “
Superconductivity in CuxBi2Se3 and its implications for pairing in the undoped topological insulator
,”
Phys. Rev. Lett.
104
,
057001
(
2010
).
2.
K.
Matano
,
M.
Kriener
,
K.
Segawa
,
Y.
Ando
, and
G.-Q.
Zheng
, “
Spin-rotation symmetry breaking in the superconducting state of CuxBi2Se3
,”
Nat. Phys.
12
,
852
(
2016
).
3.
S.
Yonezawa
,
K.
Tajiri
,
S.
Nakata
,
Y.
Nagai
,
Z.
Wang
,
K.
Segawa
,
Y.
Ando
, and
Y.
Maeno
, “
Thermodynamic evidence for nematic superconductivity in CuxBi2Se3
,”
Nat. Phys.
13
,
123
(
2017
).
4.
J.
Shen
,
W.-Y.
He
,
N. F. Q.
Yuan
,
Z.
Huang
,
C.-W.
Cho
,
S. H.
Lee
,
Y. S.
Hor
,
K. T.
Law
, and
R.
Lortz
, “
Nematic topological superconducting phase in Nb-doped Bi2Se3
,”
NPJ Q. Mater.
2
,
59
(
2017
).
5.
M. P.
Smylie
,
K.
Willa
,
H.
Claus
,
A. E.
Koshelev
,
K. W.
Song
,
W.-K.
Kwok
,
Z.
Islam
,
G. D.
Gu
,
J. A.
Schneeloch
,
R. D.
Zhong
, and
U.
Welp
, “
Superconducting and normal-state anisotropy of the doped topological insulator Sr0.1Bi2Se3
,”
Sci. Rep.
8
,
7666
(
2018
).
6.
T.
Asaba
,
B. J.
Lawson
,
B. J.
Tinsman
,
L.
Chen
,
P.
Corbae
,
G.
Li
,
Y.
Qiu
,
Y. S.
Hor
,
L.
Fu
, and
L.
Li
, “
Rotational symmetry breaking in a trigonal superconductor Nb-doped Bi2Se3
,”
Phys. Rev. X
7
,
011009
(
2017
).
7.
Z.
Liu
,
X.
Yao
,
J.
Shao
,
J.
Zuo
,
L.
Pi
,
S.
Tan
,
S.
Zhang
, and
Y.
Zhang
, “
Superconductivity with topological surface state in SrxBi2Se3
,”
J. Am. Chem. Soc.
137
,
10512
10515
(
2015
).
8.
A. Y.
Kuntsevich
,
M. A.
Bryzgalov
,
V. A.
Prudkoglyad
,
V. P.
Martovitskii
,
Y. G.
Selivanov
, and
E. G.
Chizhevskii
, “
Structural distortion behind the nematic superconductivity in SrxBi2Se3
,”
New J. Phys.
20
,
103022
(
2018
).
9.
Y.
Pan
,
A. M.
Nikitin
,
G. K.
Araizi
,
Y. K.
Huang
,
Y.
Matsushita
,
T.
Naka
, and
A.
de Visser
, “
Rotational symmetry breaking in the topological superconductor SrxBi2Se3 probed by upper-critical field experiments
,”
Sci. Rep.
6
,
28632
(
2016
).
10.
Z.
Li
,
M.
Wang
,
D.
Zhang
,
N.
Feng
,
W.
Jiang
,
C.
Han
,
W.
Chen
,
M.
Ye
,
C.
Gao
,
J.
Jia
,
J.
Li
,
S.
Qiao
,
D.
Qian
,
B.
Xu
,
H.
Tian
, and
B.
Gao
, “
Possible structural origin of superconductivity in Sr-doped Bi2Se3
,”
Phys. Rev. Mater.
2
,
014201
(
2018
).
11.
T. P.
Ginley
,
Y.
Wang
, and
S.
Law
, “
Topological insulator film growth by molecular beam epitaxy: A review
,”
Crystals
6
,
154
(
2016
).
12.
N.
Koirala
,
M.
Brahlek
,
M.
Salehi
,
L.
Wu
,
J.
Dai
,
J.
Waugh
,
T.
Nummy
,
M.-G.
Han
,
J.
Moon
,
Y.
Zhu
,
D.
Dessau
,
W.
Wu
,
N. P.
Armitage
, and
S.
Oh
, “
Record surface state mobility and quantum Hall effect in topological insulator thin films via interface engineering
,”
Nano Lett.
15
,
8245
8249
(
2015
).
13.
J.
Moon
,
N.
Koirala
,
M.
Salehi
,
W.
Zhang
,
W.
Wu
, and
S.
Oh
, “
Solution to the hole-doping problem and tunable quantum Hall effect in Bi2Se3 thin films
,”
Nano Lett.
18
,
820
826
(
2018
).
14.
Y.-L.
Wang
,
Y.
Xu
,
Y.-P.
Jiang
,
J.-W.
Liu
,
C.-Z.
Chang
,
M.
Chen
,
Z.
Li
,
C.-L.
Song
,
L.-L.
Wang
,
K.
He
,
X.
Chen
,
W.-H.
Duan
,
Q.-K.
Xue
, and
X.-C.
Ma
, “
Structural defects and electronic properties of the Cu-doped topological insulator Bi2Se3
,”
Phys. Rev. B
84
,
075335
(
2011
).
15.
Y.
Takagaki
,
B.
Jenichen
,
U.
Jahn
,
M.
Ramsteiner
, and
K.-J.
Friedland
, “
Weak antilocalization and electron-electron interaction effects in Cu-doped Bi2Se3 films
,”
Phys. Rev. B
85
,
115314
(
2012
).
16.
T.
Shirasawa
,
M.
Sugiki
,
T.
Hirahara
,
M.
Aitani
,
T.
Shirai
,
S.
Hasegawa
, and
T.
Takahashi
, “
Structure and transport properties of Cu-doped Bi2Se3 films
,”
Phys. Rev. B
89
,
195311
(
2014
).
17.
M.
Brahlek
,
N.
Koirala
,
M.
Salehi
,
N.
Bansal
, and
S.
Oh
, “
Emergence of decoupled surface transport channels in bulk insulating Bi2Se3 thin films
,”
Phys. Rev. Lett.
113
,
026801
(
2014
).
18.
H. D.
Li
,
Z. Y.
Wang
,
X.
Kan
,
X.
Guo
,
H. T.
He
,
Z.
Wang
,
J. N.
Wang
,
T. L.
Wong
,
N.
Wang
, and
M. H.
Xie
, “
The van der waals epitaxy of Bi2Se3 on the vicinal Si(111) surface: An approach for preparing high-quality thin films of a topological insulator
,”
New J. Phys.
12
,
103038
(
2010
).
19.
N.
Bansal
,
Y. S.
Kim
,
E.
Edrey
,
M.
Brahlek
,
Y.
Horibe
,
K.
Iida
,
M.
Tanimura
,
G. H.
Li
,
T.
Feng
,
H. D.
Lee
,
T.
Gustafsson
,
E.
Andrei
, and
S.
Oh
, “
Epitaxial growth of topological insulator Bi2Se3 film on Si(111) with atomically sharp interface
,”
Thin Solid Films
520
,
224
229
(
2011
).
20.
N.
Bansal
,
Y. S.
Kim
,
M.
Brahlek
,
E.
Edrey
, and
S.
Oh
, “
Thickness-independent transport channels in topological insulator Bi2Se3 thin films
,”
Phys. Rev. Lett.
109
,
116804
(
2012
).
21.
A. A.
Taskin
,
S.
Sasaki
,
K.
Segawa
, and
Y.
Ando
, “
Achieving surface quantum oscillations in topological insulator thin films of Bi2Se3
,”
Adv. Mater.
24
,
5581
5585
(
2012
).
22.
L. N.
Oveshnikov
,
V. A.
Prudkoglyad
,
E. I.
Nekhaeva
,
A. Y.
Kuntsevich
,
Y. G.
Selivanov
,
E. G.
Chizhevskii
, and
B. A.
Aronzon
, “
Magnetotransport in thin epitaxial Bi2Se3 films
,”
JETP Lett.
104
,
629
634
(
2016
).
23.
F.
Bonell
,
M. G.
Cuxart
,
K.
Song
,
R.
Robles
,
P.
Ordejon
,
S.
Roche
,
A.
Mugarza
, and
S. O.
Valenzuela
, “
Growth of twin-free and low-doped topological insulators on BaF2(111)
,”
Cryst. Growth Des.
17
,
4655
4660
(
2017
).
24.
G.
Springholz
,
S.
Wimer
,
H.
Groiss
,
M.
Albu
,
F.
Hofer
,
O.
Caha
,
D.
Kriegner
,
J.
Stangl
,
G.
Bauer
, and
V.
Holy
, “
Structural disorder of natural BimSen superlattices grown by molecular beam epitaxy
,”
Phys. Rev. Mater.
2
,
054202
(
2018
).
25.
X.
Chen
,
H. D.
Zhou
,
A.
Kiswandhi
,
I.
Miotkowski
,
Y. p.
Chen
,
P. A.
Sharma
,
A. L.
Lima Sharma
,
M. A.
Hekmaty
,
D.
Smirnov
, and
Z.
Jiang
, “
Thermal expansion coefficients of Bi2Se3 and Sb2Te3 crystals from 10 K to 270 K
,”
Appl. Phys. Lett.
99
,
261912
(
2011
).
26.
A. A.
Melnikov
,
K. N.
Boldyrev
,
Y. G.
Selivanov
,
V. P.
Martovitskii
,
S. V.
Chekalin
, and
E. A.
Ryabov
, “
Coherent phonons in a Bi2Se3 film generated by an intense single-cycle THz pulse
,”
Phys. Rev. B
97
,
214304
(
2018
).
27.
M.
Wang
,
F.
Zhang
,
W.
Jiang
,
Z.
Li
,
C.
Han
,
J.
Jia
,
J.
Li
,
S.
Qiao
,
D.
Qian
,
H.
Tian
, and
B.
Gao
, “
Growth and structural characterisation of Sr-doped Bi2Se3 thin films
,”
Sci. Rep.
8
,
21992
(
2018
).
28.
A. Y.
Kuntsevich
,
A. A.
Gabdullin
,
V. A.
Prudkogliad
,
Y. G.
Selivanov
,
E. G.
Chizhevskii
, and
V. M.
Pudalov
, “
Low-temperature Hall effect in bismuth chalcogenides thin films
,”
Phys. Rev. B
94
,
235401
(
2016
).
29.
B. A.
Aronzon
,
V. A.
Oveshnikov
,
V. A.
Prudkoglyad
,
Y. G.
Selivanov
,
K. I.
Chizhevskii
,
K. I.
Kugel
,
I. A.
Karateev
,
A. L.
Vasiliev
, and
E.
Lahderanta
, “
Magnetic and magnetotransport properties of Bi2Se3 thin films doped by Eu
,”
J. Magn. Magn. Mater.
459
,
331
334
(
2018
).
30.
Y. A.
Aleshchenko
,
A. V.
Muratov
,
V. V.
Pavlova
,
Y. G.
Selivanov
, and
E. G.
Chizhevskii
, “
Infrared spectroscopy of Bi2Te2Se
,”
JETP Lett.
99
,
187
(
2014
).
31.
P. F.
Fewster
,
X-Ray Scattering from Semiconductors
(
Imperial College Press
,
London
,
2003
).
32.
Shruti
,
V. K.
Maurya
,
P.
Neha
,
P.
Srivastava
, and
S.
Patnaik
, “
Superconductivity by Sr intercalation in the layered topological insulator Bi2Se3
,”
Phys. Rev. B
92
,
020506(R)
(
2015
).
33.
S.
Hikami
,
A. I.
Larkin
, and
Y.
Nagaoka
, “
Spin-orbit interaction and magnetoresistance in the two dimensional random system
,”
Progr. Theor. Phys.
63
,
707
710
(
1980
).
34.
J.
Wang
,
A. M.
DaSilva
,
C.-Z.
Chang
,
K.
He
,
J. K.
Jain
,
N.
Samarth
,
X.-C.
Ma
,
Q.-K.
Xue
, and
M. H. W.
Chan
, “
Evidence for electron-electron interaction in topological insulator thin films
,”
Phys. Rev. B
83
,
245438
(
2011
).
35.
Y.
Onose
,
R.
Yoshimi
,
A.
Tsukazaki
,
H.
Yuan
,
T.
Hidaka
,
Y.
Iwasa
,
M.
Kawasaki
, and
Y.
Tokura
, “
Pulsed laser deposition and ionic liquid gate control of epitaxial Bi2Se3 thin films
,”
Appl. Phys. Express
4
,
083001
(
2011
).
36.
N. V.
Tarakina
,
S.
Schreyeck
,
M.
Luysberg
,
S.
Grauer
,
C.
Schumacher
,
G.
Karczewski
,
K.
Brunner
,
C.
Gould
,
H.
Buhmann
,
R. E.
Dunin-Borkowski
, and
L. W.
Molenkamp
, “
Suppressing twin formation in Bi2Se3 thin films
,”
Adv. Mater. Interfaces
1
,
1400134
(
2014
).
37.
X.
Guo
,
Z.
Xu
,
H.
Liu
,
B.
Zhao
,
X.
Dai
,
H.
He
,
J.
Wang
,
H.
Liu
,
W.
Ho
, and
M.
Xie
, “
Single domain Bi2Se3 films grown on InP(111)A by molecular-beam epitaxy
,”
Appl. Phys. Lett.
102
,
151604
(
2013
).
38.
H.
Lind
,
S.
Lidin
, and
U.
Haussermann
, “
Structure and bonding properties of (Bi2Se3)m(Bi2)n stacks by first-principles density functional theory
,”
Phys. Rev. B
72
,
184101
(
2005
).
39.
A. I.
Figueroa
,
G.
van der Laan
,
L. J.
Collins-McIntyre
,
G.
Cibin
,
A. J.
Dent
, and
T.
Hesjedal
, “
Local structure and bonding of transition metal dopants in Bi2Se3 topological insulator thin films
,”
J. Phys. Chem.
C119
,
17344
17351
(
2015
).
40.
G.
Du
,
J.
Shao
,
X.
Yang
,
Z.
Du
,
D.
Fang
,
C.
Zhang
,
J.
Wang
,
K.
Ran
,
J.
Wen
,
H.
Yang
,
H.
Zhang
, and
H.-H.
Wen
, “
Drive the dirac electrons into Cooper pairs in SrxBi2Se3
,”
Nat. Commun.
8
,
14466
(
2017
).
41.
P.
Shang
,
X.
Guo
,
B.
Zhao
,
X.
Dai
,
L.
Bin
,
J.
Jia
,
Q.
Li
, and
M.
Xie
, “
Nanoclusters of CaSe in calcium-doped Bi2Se3 grown by molecular-beam epitaxy
,”
Nanotechnology
27
,
085601
(
2016
).
42.
L. N.
Oveshnikov
,
Y. I.
Rodionov
,
K. I.
Kugel
,
I. A.
Karateev
,
A. L.
Vasiliev
,
Y. G.
Selivanov
,
E. G.
Chizhevskii
,
I. S.
Burmistrov
, and
B. A.
Aronzon
, “
Magnetism of Bi2Se3 thin films with Eu-rich flat inclusions
,”
J. Phys. Condens. Matter
30
,
445801
(
2018
).
43.
H. M. D. N.
Vasconcelos
,
M.
Eddrief
,
Y.
Zheng
,
D.
Demaille
,
S.
Hidki
,
E.
Fonda
,
A.
Novikova
,
J.
Fujii
,
P.
Torelli
,
B. R.
Salles
,
I.
Vobornik
,
G.
Panaccione
,
A. J. A.
de Oliveira
,
M.
Marangolo
, and
F.
Vidal
, “
Magnetically hard Fe3Se4 embedded in Bi2Se3 topological insulator thin films grown by molecular beam epitaxy
,”
ACS Nano
10
,
1132
1138
(
2016
).
44.
E. D. L.
Rienks
,
S.
Wimmer
,
P. S.
Mandal
,
O.
Caha
,
J.
Ruzicka
,
A.
Ney
,
H.
Steiner
,
V. V.
Volobuev
,
H.
Groiss
,
M.
Albu
,
S.
Khan
,
J.
Minar
,
H.
Ebert
,
G.
Bauer
,
A.
Varykhalov
,
J.
Sanchez-Barriga
,
O.
Rader
, and
G.
Springholz
, “Large magnetic gap at the Dirac point in a Mn-induced Bi2Te3 heterostructure,” e-print arXiv:1810.06238 (
2018
).
You do not currently have access to this content.