In order to understand the mechanism of the ferromagnetism in the ferromagnetic semiconductor Ga1xMnxAs [(Ga,Mn)As], we have investigated the magnetic behavior on a microscopic level through systematic temperature (T)- and magnetic field (H)-dependent soft x-ray magnetic circular dichroism (XMCD) experiments at the Mn L2,3 absorption edges. The T and H dependences of XMCD intensities have been analyzed using a model consisting of the ferromagnetic (FM), paramagnetic, and superparamagnetic (SPM) components. Intriguingly, we have found a common behavior for the ferromagnetic ordering process in (Ga,Mn)As samples with different Mn concentrations (4% and 10.8%) and different Curie temperature (TC) values (65, 120, and 164 K). In particular, the SPM component develops well above TC, indicating that local FM regions are formed well above TC. The present findings indicate that the onset of ferromagnetic ordering is triggered by local electronic states around the substitutional Mn ions rather than uniform electronic states considered by mean-field theories. Insight into the most representative ferromagnetic semiconductor, (Ga,Mn)As, provided by the present study will be an important step in understanding the mechanism of ferromagnetic ordering in various ferromagnetic semiconductor families.

1.
H.
Ohno
,
A.
Shen
,
F.
Matsukura
,
A.
Oiwa
,
A.
Endo
,
S.
Katsumoto
, and
Y.
Iye
,
Appl. Phys. Lett.
69
,
363
(
1996
).
2.
T.
Hayashi
,
M.
Tanaka
,
T.
Nishinaga
,
H.
Shimada
,
H.
Tsuchiya
, and
Y.
Otuka
,
J. Cryst. Growth
175-176
,
1063
(
1997
).
3.
A.
Van Esch
,
L.
Van Bockstal
,
J.
De Boeck
,
G.
Verbanck
,
A. S.
van Steenbergen
,
P. J.
Wellmann
,
B.
Grietens
,
R.
Bogaerts
,
F.
Herlach
, and
G.
Borghs
,
Phys. Rev. B
56
,
13103
(
1997
).
5.
D.
Chiba
,
F.
Matsukura
, and
H.
Ohno
,
Appl. Phys. Lett.
89
,
162505
(
2006
).
6.
D.
Chiba
,
M.
Sawicki
,
Y.
Nishitani
,
Y.
Nakatani
,
F.
Matsukura
, and
H.
Ohno
,
Nature
455
,
515
(
2008
).
7.
H.
Saito
,
S.
Yuasa
, and
K.
Ando
,
Phys. Rev. Lett.
95
,
086604
(
2005
).
8.
T.
Kanaki
,
H.
Yamasaki
,
H.
Terada
,
Y.
Iwasa
,
S.
Ohya
, and
M.
Tanaka
,
Jpn. J. Appl. Phys.
57
,
090301
(
2018
).
9.
L.
Chen
,
X.
Yang
,
F.
Yang
,
J.
Zhao
,
J.
Misuraca
,
P.
Xiong
, and
S.
von Molnár
,
Nano Lett.
11
,
2584
(
2011
).
11.
T.
Jungwirth
,
J.
Sinova
,
A. H.
MacDonald
,
B. L.
Gallagher
,
V.
Novák
,
K. W.
Edmonds
,
A. W.
Rushforth
,
R. P.
Campion
,
C. T.
Foxon
,
L.
Eaves
,
E.
Olejník
,
J.
Mašek
,
S.-R. E.
Yang
,
J.
Wunderlich
,
C.
Gould
,
L. W.
Molenkamp
,
T.
Dietl
, and
H.
Ohno
,
Phys. Rev. B
76
,
125206
(
2007
).
12.
K.
Sato
,
P. H.
Dederics
, and
H.
Katayama-Yoshida
,
Europhys. Lett.
61
,
403
(
2003
).
13.
M.
Berciu
and
R. N.
Bhatt
,
Phys. Rev. Lett.
87
,
107203
(
2001
).
14.
P.
Mahadevan
and
A.
Zunger
,
Appl. Phys. Lett.
85
,
2860
2862
(
2004
).
15.
M.
Kobayashi
,
H.
Niwa
,
Y.
Takeda
,
A.
Fujimori
,
Y.
Senba
,
H.
Ohashi
,
A.
Tanaka
,
S.
Ohya
,
P. N.
Hai
,
M.
Tanaka
,
Y.
Harada
, and
M.
Oshima
,
Phys. Rev. Lett.
112
,
107203
(
2014
).
16.
M.
Kobayashi
,
I.
Muneta
,
Y.
Takeda
,
Y.
Harada
,
A.
Fujimori
,
J.
Krempaský
,
T.
Schmitt
,
S.
Ohya
,
M.
Tanaka
,
M.
Oshima
, and
V. N.
Strocov
,
Phys. Rev. B
89
,
205204
(
2014
).
17.
M.
Mayr
,
G.
Alvarez
, and
E.
Dagotto
,
Phys. Rev. B
65
,
241202
(
2002
).
18.
A.
Kaminski
and
S.
Das Sarma
,
Phys. Rev. Lett.
88
,
247202
(
2002
).
19.
A.
Kaminski
and
S.
Das Sarma
,
Phys. Rev. B
68
,
235210
(
2003
).
20.
S.
Souma
,
L.
Chen
,
R.
Oszwaldowski
,
T.
Sato
,
F.
Matsukura
,
T.
Dietl
,
H.
Ohno
, and
T.
Takahashi
,
Sci. Rep.
6
,
27266
(
2016
).
21.
J.
Kanski
,
L.
Ilver
,
K.
Karlsson
,
I.
Ulfat
,
M.
Leandersson
,
J.
Sadowski
, and
I. D.
Marco
,
New. J. Phys.
19
,
023006
(
2017
).
22.
M.
Kobayashi
,
S.
Ohya
,
I.
Muneta
,
Y.
Takeda
,
Y.
Harada
,
J.
Krempasky
,
T.
Schmitt
,
M.
Oshima
,
V. N.
Strocov
,
M.
Tanaka
, and
A.
Fujimori
, “Alternative interpretation of the recent experimental results of angle-resolved photoemission spectroscopy on GaMnAs [Sci. Rep. 6, 27266 (2016)],” arXiv:1608.07718 (2016).
23.
M.
Sawicki
,
D.
Chiba
,
A.
Korbecka
,
Y.
Nishitani
,
J. A.
Majewski
,
F.
Matsukura
,
T.
Dietl
, and
H.
Ohno
,
Nat. Phys.
6
,
22
(
2010
).
24.
Y.
Nishitani
,
D.
Chiba
,
M.
Endo
,
M.
Sawicki
,
F.
Matsukura
,
T.
Dietl
, and
H.
Ohno
,
Phys. Rev. B
81
,
045208
(
2010
).
25.
Y.
Yuan
,
M.
Wang
,
C.
Xu
,
R.
Hübner
,
R.
Böttger
,
R.
Jakiela
,
M.
Helm
,
M.
Sawicki
, and
S.
Zhou
,
J. Phys. Condens. Matter
30
,
095801
(
2018
).
26.
Y.
Yuan
,
C.
Xu
,
R.
Hübner
,
R.
Jakiela
,
R.
Böttger
,
M.
Helm
,
M.
Sawicki
,
T.
Dietl
, and
S.
Zhou
,
Phys. Rev. Mater.
1
,
054401
(
2017
).
27.
L.
Gluba
,
O.
Yastrubchak
,
J. Z.
Domagala
,
R.
Jakiela
,
T.
Andrearczyk
,
J.
Żuk
,
T.
Wosinski
,
J.
Sadowski
, and
M.
Sawicki
,
Phys. Rev. B
97
,
115201
(
2018
).
28.
K.
Edmonds
,
G.
van der Laan
, and
G.
Panaccione
,
Semicond. Sci. Technol.
30
,
043001
(
2015
).
29.
Y.
Takeda
,
M.
Kobayashi
,
T.
Okane
,
T.
Ohkochi
,
J.
Okamoto
,
Y.
Saitoh
,
K.
Kobayashi
,
H.
Yamagami
,
A.
Fujimori
,
A.
Tanaka
,
J.
Okabayashi
,
M.
Oshima
,
S.
Ohya
,
P. N.
Hai
, and
M.
Tanaka
,
Phys. Rev. Lett.
100
,
247202
(
2008
).
30.
These two samples (S1 and S2) were also used in the previous RIXS measurement.15
31.
Y.
Saitoh
,
Y.
Fukuda
,
Y.
Takeda
,
H.
Yamagami
,
S.
Takahashi
,
Y.
Asano
,
T.
Hara
,
K.
Shirasawa
,
M.
Takeuchi
,
T.
Tanaka
, and
H.
Kitamura
,
J. Synchrotron Radiat.
19
,
388
(
2012
).
32.
K. W.
Edmonds
,
N. R. S.
Farley
,
R. P.
Campion
,
C. T.
Foxon
,
B. L.
Gallagher
,
T. K.
Johal
,
G.
van der Laan
,
M.
MacKenzie
,
J. N.
Chapman
, and
E.
Arenholz
,
Appl. Phys. Lett.
84
,
4065
4067
(
2004
).
33.
D.
Wu
,
D. J.
Keavney
,
R.
Wu
,
E.
Johnston-Halperin
,
D. D.
Awschalom
, and
J.
Shi
,
Phys. Rev. B
71
,
153310
(
2005
).
34.
Y.
Ishiwata
,
M.
Watanabe
,
R.
Eguchi
,
T.
Takeuchi
,
Y.
Harada
,
A.
Chainani
,
S.
Shin
,
T.
Hayashi
,
Y.
Hashimoto
,
S.
Katsumoto
, and
Y.
Iye
,
Phys. Rev. B
65
,
233201
(
2002
).
35.
K. W.
Edmonds
,
P.
Bogusławski
,
K. Y.
Wang
,
R. P.
Campion
,
S. N.
Novikov
,
N. R. S.
Farley
,
B. L.
Gallagher
,
C. T.
Foxon
,
M.
Sawicki
,
T.
Dietl
,
M.
Buongiorno Nardelli
, and
J.
Bernholc
,
Phys. Rev. Lett.
92
,
037201
(
2004
).
36.
B. T.
Thole
,
P.
Carra
,
F.
Sette
, and
G.
van der Laan
,
Phys. Rev. Lett.
68
,
1943
(
1992
).
37.
P.
Carra
,
B. T.
Thole
,
M.
Altarelli
, and
X.
Wang
,
Phys. Rev. Lett.
70
,
694
(
1993
).
38.
J.
Stöhr
and
H.
König
,
Phys. Rev. Lett.
75
,
3748
(
1995
).
39.
Y.
Teramura
,
A.
Tanaka
, and
T.
Jo
,
J. Phys. Soc. Jpn.
65
,
1053
(
1996
).
40.
We proportionally converted the peak intensity of the XMCD spectrum at the Mn L3 edge [indicated by the arrow in Fig. 2(h)] into the magnitude of the magnetic moment in μB/Mn because the spectral shapes are not changed with T and H.
41.
K. M.
Yu
,
W.
Walukiewicz
,
T.
Wojtowicz
,
I.
Kuryliszyn
,
X.
Liu
,
Y.
Sasaki
, and
J. K.
Furdyna
,
Phys. Rev. B
65
,
201303
(
2002
).
42.
M.
Dobrowolska
,
K.
Tivakornsasithorn
,
X.
Liu
,
J. K.
Furdyna
,
M.
Berciu
,
K. M.
Yu
, and
W.
Walukiewicz
,
Nat. Mater.
11
,
444
(
2012
).
43.
Note that the choice of MMAX value does not affect the common behavior of the magnetic ordering process obtained from the fitting results significantly.
44.
O.
Proselkov
,
D.
Sztenkiel
,
W.
Stefanowicz
,
M.
Aleszkiewicz
,
J.
Sadowski
,
T.
Dietl
, and
M.
Sawicki
,
Appl. Phys. Lett.
100
,
262405
(
2012
).
45.
M.
Sawicki
,
O.
Proselkov
,
C.
Sliwa
,
P.
Aleshkevych
,
J. Z.
Domagala
,
J.
Sadowski
, and
T.
Dietl
,
Phys. Rev. B
97
,
184403
(
2018
).
46.
Y. K.
Wakabayashi
,
S.
Sakamoto
,
Y.-h.
Takeda
,
K.
Ishigami
,
Y.
Takahashi
,
Y.
Saitoh
,
H.
Yamagami
,
A.
Fujimori
,
M.
Tanaka
, and
S.
Ohya
,
Sci. Rep.
6
,
23295
(
2016
).
47.
S.
Sakamoto
,
L. D.
Anh
,
P. N.
Hai
,
G.
Shibata
,
Y.
Takeda
,
M.
Kobayashi
,
Y.
Takahashi
,
T.
Koide
,
M.
Tanaka
, and
A.
Fujimori
,
Phys. Rev. B
93
,
035203
(
2016
).
48.
We started the fitting procedure from the highest T, where the MH curves can be reproduced by a straight line, corresponding to PLinear = 1 well above TC. Since all the parameters are obviously functions of T, we naturally assumed that they vary continuously with T. The fitting analysis was sequentially conducted toward the next lower T so that the T dependence of the parameters becomes smooth. After that, the reproducibility of the fitting results was carefully checked by both increasing T and decreasing T. In addition, the value of MSPM was restricted to be less than MMAX.
49.
S. R.
Dunsiger
,
J. P.
Carlo
,
T.
Goko
,
G.
Nieuwenhuys
,
T.
Prokscha
,
A.
Suter
,
E.
Morenzoni
,
D.
Chiba
,
Y.
Nishitani
,
T.
Tanikawa
,
F.
Matsukura
,
H.
Ohno
,
J.
Ohe
,
S.
Maekawa
, and
Y. J.
Uemura
,
Nat. Mater.
9
,
299
(
2010
).
50.
S.
Ohya
,
K.
Takata
, and
M.
Tanaka
,
Nat. Phys.
7
,
342
(
2011
).
51.
I.
Muneta
,
S.
Ohya
,
H.
Terada
, and
M.
Tanaka
,
Nat. Commun.
7
,
12013
(
2016
).
52.
J.
Fujii
,
M.
Sperl
,
S.
Ueda
,
K.
Kobayashi
,
Y.
Yamashita
,
M.
Kobata
,
P.
Torelli
,
F.
Borgatti
,
M.
Utz
,
C. S.
Fadley
,
A. X.
Gray
,
G.
Monaco
,
C. H.
Back
,
G.
van der Laan
, and
G.
Panaccione
,
Phys. Rev. Lett.
107
,
187203
(
2011
).
53.
J. C.
Ododo
,
Solid State Commun.
25
,
493
(
1978
).
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