Journal of Semiconductors

COMMENTS AND OPINIONS

Families of magnetic semiconductors — an overview

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 Journal of Semiconductors
(2019) 40, 080301
COMMENTS AND OPINIONS doi: 10.1088/1674-4926/40/8/080301

Families of magnetic semiconductors — an overview

Tomasz Dietl1, 2, †, Alberta Bonanni3, †, and Hideo Ohno4, 5, 2, 6, 7, 8, †
1International Research Centre MagTop, Institute of Physics, Polish Academy of Sciences, Aleja Lotnikow 32/46, PL-02668 Warsaw, Poland
2WPI Advanced Institute for Materials Research, Tohoku University, 2-1-1 Katahira, Aoba-ku, Sendai 980-8577, Japan
3Institut für Halbleiter- und Festkörperphysik, Johannes Kepler University, Altenbergerstrasse 69, A-4040 Linz, Austria

4Laboratory for Nanoelectronics and Spintronics, Research Institute of Electrical Communication, Tohoku University, 2-1-1 Katahira, Aoba-ku,

Sendai 980-8577, Japan

5Center for Science and Innovation in Spintronics (Core Research Cluster), Tohoku University, 2-1-1 Katahira, Aoba-ku, Sendai 980-8577, Japan

6Center for Spintronics Integrated System, Tohoku University, 2-1-1 Katahira, Aoba-ku, Sendai 980-8577, Japan

7Center for Innovative Integrated Electronic Systems, Tohoku University, 468-1 Aramaki Aza Aoba, Aoba-ku, Sendai 980-0845, Japan

8Center for Spintronics Research Network, Tohoku University, 2-1-1 Katahira, Aoba-ku, Sendai 980-8577, Japan

Key words: magnetic and dilute magnetic semiconductors; topological materials; 2D systems

Citation: T Dietl, A Bonanni, and H Ohno, Families of magnetic semiconductors — an overview[J]. J. Semicond., 2019, 40(8),
080301. http://doi.org/10.1088/1674-4926/40/8/080301

Tomasz Dietl obtained his PhD from The interplay of magnetic and semiconducting proper-
the Institute of Physics, Polish Aca- ties has been in the focus for more than a half of the century.
demy of Sciences in Warsaw, where In this introductory article we briefly review the key proper-
he is presently a head of the Interna- ties and functionalities of various magnetic semiconductor
families, including europium chalcogenides, chromium
tional Centre for Interfacing Magnet-
spinels, dilute magnetic semiconductors, dilute ferromag-
ism and Superconductivity with To- netic semiconductors and insulators, mentioning also
pological Matter “MagTop”. He is sources of non-uniformities in the magnetization distribu-
also a P.I. at the Advanced Institute tion, accounting for an apparent high Curie temperature fer-
for Materials Research at Tohoku University in Sendai, Japan. romagnetism in many systems. Our survey is carried out
from today's perspective of ferromagnetic and antiferro-
magnetic spintronics as well as of the emerging fields of
Alberta Bonanni graduated in phys-
magnetic topological materials and atomically thin 2D lay-
ics at the University of Trieste – Italy.
ers.
She worked at the University of Min-
nesota and at the Synchrotron Cen-
ter of the University of Madison-Wis-
Magnetic semiconductors
consin in the US. She is now at the
The discovery of ferromagnetism in some europium chalco-
Johannes Kepler University in Linz –
genides and chromium spinels a half of the century ago[1]
Austria, and her scientific interests
came as a surprise, since insulators typically showed antiferro-
are focused on the physics of nitride compounds and magnetic or ferrimagnetic spin ordering, driven by a superex-
quantum materials. change interaction, whereas ferromagnetism was considered
a domain of metals. However, the Goodenough-Kanamori-An-
Hideo Ohno received his Ph.D. from derson rules indicate in which cases the superexchange can
the University of Tokyo in 1982. He lead to ferromagnetic short-range coupling between local-
ized spins. This mechanism accounts e.g. for Curie temperat-
joined Hokkaido University from
ure TC = 130 K in CdCr2Se4[2]. In the case of EuO and EuS, the anti-
1982 and he was a visiting scientist
ferromagnetic superexchange is overcompensated by a direct
at the IBM T. J. Watson Research f–d ferromagnetic exchange, which results in TC = 68 K and 16 K,
Center for 1.5 years. He was appoin- respectively[3].
ted Professor at Tohoku University in Soon after their discovery, magnetic semiconductors were
1994 and is President since 2018. His found to exhibit outstanding properties, including colossal mag-
netoresistance and magnetooptical effects, assigned rightly to
research interests include spintronics, semiconductor science
the exchange interaction of band carriers and localized spins.
and technology. This sd–f coupling results in a giant spin splitting of bands be-

† Correspondence to: T Dietl, [email protected]; A Bonanni,

[email protected]; H Ohno, [email protected] ©2019 Chinese Institute of Electronics
2 Journal of Semiconductors doi: 10.1088/1674-4926/40/8/080301

low TC, as well as in magnetization fluctuations near TC gener- ors is represented by qubit systems consisting of single magnet-
ated by band carriers[4, 5]. Due to the presence of a sizable sd–f ic ions in single quantum dots[28, 29].
exchange interaction, by electron doping (oxygen vacancies,
Eu substituted by Gd) the magnitude of TC can be enhanced p-type dilute ferromagnetic semiconductors
by about 50 K in EuO, in agreement with the Ruderman-Kittel-
Kasuya-Yosida (RKKY) theory[3]. In these systems, a high density of delocalized or weakly loc-
More recently, EuS and related ferromagnetic insulators alized holes leads to long-range ferromagnetic interactions
have been proposed as functional overlayers that can lead to between transition metal cations, which dominate over the anti-
novel topological properties by exchange splitting of interfa- ferromagnetic superexchange, and are well described by the
cial bands via a ferromagnetic proximity effect[6]. At the same p–d Zener model[30, 31], more universal compared to RKKY-
time, HgCr2Se4 (TC = 110 K) appears to be a Weyl semimetal[7]. type of approaches. The flagship example of this material fam-
Furthermore, antiferromagnetic EuTe constitutes a test-bench ily is (Ga,Mn)As in which Mn ions introduce spins and holes to
for the emerging field of antiferromagnetic spintronics[8]. the valence band[32], but to this category belong also other
Another class of materials that attract considerable atten- types of magnetically doped p-type compounds, in which
tion are van der Waals magnetic semiconductors studied holes originate from point defects, like (Pb,Sn,Mn)Te[33], or
down to the atomically thin limit[9]. A competition between fer- from shallow acceptor impurities, e.g., (Cd,Mn)Te/(Cd,Mg)Te:
romagnetic and antiferromagnetic superexchange accounts N[11] and (Zn,Mn)Te:N[34], rather than from Mn ions. The repor-
for the magnetic properties of CrI3 and related systems as a func- ted magnitudes of Curie temperature TC reach 200 K in
tion of the number of layers, electric field, and strain[9, 10]. In par- (Ga,Mn)As[35–37], (Ge,Mn)Te[38, 39], and (K,Ba)(Zn,Mn)2As2[40] with
ticular, monolayers are ferromagnetic in the case of these com- less than 10% of Mn cations, xeff < 0.1, measured by saturation
pounds in which, similarly to 2D (Cd,Mn)Te[11], the low-temper- magnetization in moderate fields, µ0 H ≲ 5 T. The values of
ature 2D spin order is stabilized by the large magnitude of the Curie temperatures achieved in p-type dilute ferromagnetic
uniaxial magnetic anisotropy[12]. On the other hand, TMPX3, semiconductors are to be contrasted with TC ≈ 0.16 K in n-
where TM is a transition metal and X is either S or Se, are antifer- Zn1–x Mnx O:Al with x = 0.03[41]. Such low values of TC in n-type
romagnetic semiconductors. Their properties as a function of systems reflect the relatively small magnitudes of both s–d ex-
the layer number are under investigations[9]. change integral and density of states. Higher TC values are ob-
served only in specific situations, for instance, at the crossings
of electron Landau levels under quantum Hall effect condi-
Dilute magnetic semiconductors
tions[42].
This material family was initially named semimagnetic semi- Ground breaking spintronic functionalities have been
conductors[13], as it comprises standard semiconductors demonstrated and theoretically described for (Ga,Mn)As and re-
doped with magnetic impurities that are randomly distrib- lated systems[31, 43]. They rely on the strong p–d coupling
uted, electrically inactive, and do not show any long-range spa- between localized spins and hole carriers, as well as on sizable
tial spin ordering[14, 15]. Typical representatives are (Cd,Mn)Te, spin-orbit interactions in p-like orbitals forming the valence
(Zn,Co)O, and (Pb,Eu)S. Here, the short-range antiferromagnet- band or originating from inversion asymmetry of the host crys-
ic superexchange between Mn[16, 17] and heavier 3d transition tal structure. Numerous functionalities of (Ga,Mn)As and other
metal ions (e.g. Co) or long-range dipolar interactions p-type dilute ferromagnetic semiconductors (electrical spin in-
between rare earth magnetic moments[18] lead to spin-glass jection[44], magnetization control by an electric field[45–47], cur-
freezing at Tf < 1 K for x < 0.1. Magnetooptical and quantum rent-induced domain-wall motion[48, 49], anisotropic tunneling
transport experiments have allowed to reveal and quantify the magnetoresistance[50, 51], and spin-orbit torque[52, 53]) have
influence of sp–d coupling upon the exciton, polariton, and triggered the spread of spintronic research over virtually all ma-
Landau level spectra, quantum Hall effects, one-electron and terials families. In particular, they are now explored in multilay-
many-body quantum localization, universal conductance fluctu- ers of transition metals supporting ferromagnetism above
ations, and carrier spin dynamics in dilute magnetic semicon- room temperature[54]. At the same time, the search for high TC
ductor systems of various dimensionalities realized in bulk, 2D ferromagnetic semiconductors led to the discovery of Fe-
quantum structures, nanowires, and quantum dots[15, 19–21], as based superconductors, whereas theoretical approaches to
well as made it possible to optically detect electrical spin injec- the anomalous Hall effect in (Ga,Mn)As in terms of the Berry
tion[22]. Conversely, the dynamics of localized spins has been phase[55, 56] and studies of spin-orbit torque in the same com-
probed by the Faraday effect[23] or quantum noise spectro- pound[52, 53] have paved the way to spintronics of topologi-
scopy[24]. The physics of bound magnetic polarons, single elec- cal[57, 58] and antiferromagnetic systems[59].
trons interacting with spins localized within the confining po-
tential of shallow impurities or quantum dots, has been ad-
Dilute ferromagnetic insulators
vanced in dilute magnetic semiconductors[25]. While the major-
ity of experimental results can be explained within virtual crys- As mentioned, the Goodenough-Kanamori-Anderson
tal and molecular field approximations, strong coupling ef- rules indicates in which cases superexchange can lead to ferro-
fects show up in the case of oxides and nitrides doped with magnetic short-range coupling between localized spins. Accord-
transition metal impurities[26, 27]. ing to experimental and theoretical studies, such a mechan-
Most of the end binary compounds, for instance MnSe ism operates for Mn3+ ions in GaN and accounts for TC values
and EuTe, are insulating antiferromagnets and, therefore, at- reaching about 13 K at x ≈10 % in semi-insulating wurtzite
tract attention from the point of view of antiferromagnetic spin- Ga1–x Mnx N[60], an accomplishment preceded by a long series
tronics. Another ultimate limit of dilute magnetic semiconduct- of material development stages[61, 62]. Since there is no compet-

T Dietl et al.: Families of magnetic semiconductors — an overview

 Journal of Semiconductors doi: 10.1088/1674-4926/40/8/080301 3

ing antiferromagnetic interactions and due to high atom dens- Heterogeneities in magnetic semiconductors
ity, an unusually high magnitude of magnetization for the dilu- It becomes increasingly clear that spatial inhomogeneit-
tion x = 0.1 is observed in Ga1–x Mnx N[62]. In contrast to ran- ies in the magnetization distribution account for a number of
dom antiferromagnets (such as II–VI dilute magnetic semicon- key properties of magnetic semiconductors, including the mag-
ductors), there is no frustration in the case of ferromagnetic nitude of TC. We discuss here three distinct mechanisms ac-
spin-spin interactions. Furthermore, according to the tight-bind- counting for the non-uniform distribution of magnetization
ing theory, the interaction energy decays exponentially with and describe their consequences.
the spin-spin distance[60]. Accordingly, the dependence of TC (1) According to the percolation theory applicable to di-
on x cannot be explained within the mean-filed approxima- lute systems with short-range spin-spin interactions, critical tem-
tion, but corroborates the percolation theory[63], and can be perature TC corresponds to the formation of a percolative
quantitatively described by combining tight-binding theory cluster that incorporates typically about 16% of the spins in
and Monte Carlo simulations[60]. the 3D case. This cluster extends over all spins at T = 0, imply-
The significant inversion symmetry breaking specific to ing that at T > 0 ferromagnetism co-exists with superparamag-
wurtzite semiconductors and the insulating character of the sys- netism produced by not percolative clusters[73]. Presumably
tem allow controlling the magnetization by an electric field via this effect accounts for thermal instabilities of the quantum an-
a piezoelectromagnetic coupling in (Ga,Mn)N. As shown experi- omalous Hall effect even at T ≪ TC, and shifts below 100 mK
mentally and confirmed theoretically[64], the inverse piezoelec- the operation range of the potential resistance standards
tric effect changes the magnitude of the single-ion magnetic an- based on this phenomenon[74, 75].
isotropy specific to Mn3+ ions in GaN, and thus the magnitude (2) A specific feature of conducting magnetic semiconduct-
of magnetization. ors is the interplay of carrier-mediated ferromagnetism with car-
rier localization, which results in spatial fluctuations of magnetiz-
Dilute magnetic topological materials ation and superparamagnetic signatures generated by the critic-
al fluctuations in the carrier density of states in the vicinity of
In these systems[57, 58], there are novel consequences of
the metal-to-insulator transition. This effect has been extens-
magnetization-induced giant p–d exchange spin-splittings of
ively discussed in the context of both ferromagnetic[5, 76] and di-
bulk and topological boundary states. In particular, in thin lay- lute ferromagnetic semiconductors[77–79].
ers of 3D topological insulators, this splitting turns hybridized (3) The magnetic properties discussed above have con-
topological surface states into chiral edge states. Striking con- cerned systems with a random distribution of cation-substitu-
sequences of this transformation include: (i) the precise quantiz- tional magnetic impurities. A major challenge in dilute magnet-
ation of the Hall conductance σxy = e2/h demonstrated for thin ic materials is the crucial dependence of their properties on
layers of ferromagnetic (Bi,Sb,Cr)2Te3 at millikelvin temperat- the spatial distribution of magnetic ions and their position in
ures[65], as predicted theoretically[66]; (ii) the efficient magnetiza- the crystal lattice. These nanoscale structural characteristics de-
tion switching by spin-locked electric currents in these ferro- pend, in turn, on the growth and processing protocols, as well
magnets[67]. In the case of 3D Dirac materials with magnetic im- as on doping with shallow impurities[80, 81]. By employing a
purities coupled by antiferromagnetic superexchange, such as range of photon, electron, and particle beam methods, with
(Cd,Mn)3As2 or strained (Hg,Mn)Te, the magnetic field-in- structural, chemical, and spin resolution down to the nano-
duced formation of Weyl semimetals with non-zero topologic- scale, it has become possible to correlate the surprising magnet-
al charges has been predicted[68]. ic properties with the spatial arrangement and with the elec-
Furthermore, inverted band ordering specific to topologic- tronic configuration of the magnetic constituent[82, 83]. In partic-
al matter enhances the role of the long-range interband Bloem- ular, the aggregation of magnetic cations which are either intro-
bergen-Rowland contribution to spin-spin interactions, result- duced deliberately or present due to contamination, accounts
ing in higher spin-glass freezing temperatures Tf in topologic- for the high TC values observed in a number of semiconduct-
al semimetals, such as (Cd,Mn)3As2 and (Hg,Mn)Te, compared ors and oxides[84, 85]. The symmetry lowering associated with
to topologically trivial II–VI Mn-based dilute magnetic semicon- this aggregation is also responsible for remarkable magnetic
ductors[17]. This spin-spin exchange mechanism, taken into con- and magnetotransport anisotropy properties of (Ga,Mn)As[86]
sideration within the p–d Zener model[69] and named Van and (In,Fe)As[87].
Vleck's paramagnetism, was proposed to lead to ferromagnet-
ism in topological insulators of bismuth/antimony chalcogen-
Outlook
ides containing V, Cr, or Fe[66], a proposal discussed earlier in
the context of zero-gap (Hg,Mn)Te[70]. However, according to Semiconductors and insulators doped with magnetic im-
ab initio studies and corresponding experimental data, the su- purities, in addition to showing fascinating physics, have well
perexchange in the case of V and Cr, and the RKKY coupling in established applications as semi-insulating substrates and lay-
Mn-doped films appear to contribute significantly to ferromag- ers, and as building-blocks for solid state lasers, optical insulat-
netism in tetradymite V2–VI3 compounds[71]. It appears that ors, and detectors of high energy photons. More recent works
the co-existence of ferromagnetic superexchange with ferro- have revealed surprising materials science features, such as a
magnetic Bloembergen-Rowland and RKKY interactions ac- dependence of the spatial distribution of magnetic impurities
counts for TC as high as 250 K in (Crx Sb1–x )2Te3 with x = 0.44[72]. on the Fermi level position. At the same time, studies of dilute
Ferromagnetic coupling between magnetic impurities medi- ferromagnetic semiconductors have led to discoveries of break-
ated by carriers residing in surface or edge Dirac cones is through functionalities, like for instance spin-orbit torque and
rather weak for realistic values of spatial extension of these magnetization manipulation by an electric field, which are on
states into the bulk[31]. the way of recasting the concept of computer hardware. The

T Dietl et al.: Families of magnetic semiconductors — an overview

 4 Journal of Semiconductors doi: 10.1088/1674-4926/40/8/080301

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T Dietl et al.: Families of magnetic semiconductors — an overview