IE EE T RA NS. ELE CT RON. DEVI CE S, VOL . X, NO.

XX, AUGUS T 20 06

Oxide spintronics Manuel Bibes and es Barth el emy

Agn`
Abstrac Concomitant with th e development of metal-based t spintronics in the late 1980s and 1990s, important advances were made on the growth of high-quality oxide thin films and heterostructures. While this was at first motivated by the discovery of high-temperature superconductivity in perovskite Cu oxides, this technological breakthrough was soon applied to other transition metal oxid es, and notably mixed-valence manganites. The discovery of colossal magnetoresistance in manganite films triggered an intense research activity on these materials, but the first notable impact of magnetic oxides in the field of spintronics was th e u se of such manganites as electrodes in magnetic tunnel junctions, yielding tunnel magnetoresistance ratios one order of magnitude larger than what had been obtained with transition metal electrodes. Since then, the research on oxide spintronics has been intense with the latest developments focused on diluted magnetic oxides and more recently on multiferroics. In this paper, we will review the most important results on oxide spintronics, emphasizing materials physics as well as spin-dependent tran sport phenomena, and finally give some perspectives on how the urry of new magnetic oxides could be useful for next-generation spintronics devices. The final version of this review article has been published in IEEE Tran s. Electron. Devices, 54, 1003 (2007) Index Terms multiferroics oxides, spintronics, tunneling, ferromagnets,

This latter family of researchers was mostly focusing on the recently discovered high-critical-temperature superconductors [3] and their growth in thin films using techniques like laser deposition. This experience proved crucial for pulsed the fabrication an d understanding of spintronics structures based on magnetic oxides. the first pioneering TMR results obtained on Since tunnel junctions based on manganese p erovskite oxides [4], the interest for oxides in spintronics has increased at a qu ick pace. research was boo sted by the discovery of This ferromagnetism in diluted magnetic semiconductors like (Ga,Mn)As [5] which triggered an intense activity on oxide semiconductors (ZnO,, etc) doped with magnetic ions. More recently, Ti 2 O the renewed interest in multiferroic materials and their growth in thin film form has provid ed novel op portunities for oxides in spintronics . In this paper, we will review some of the most significant achievemen ts using oxides in spintronics experiments. Even than in the case of spintronics with 3d metals more or semiconductors like GaAs, oxide spintronics is complicated by materials science (g rowth, characterization, materials physics) that have to be properly addressed in order to aspects perform understandable spintro nics exp eriments. In clean and each of this review, a summary of the experimental status part for materials issues will be provided, before getting into the details remark able spintro nics results. Finally, prospects of some on possible future sp intron ics devices using magnetic oxides will ge given. A. Tu nnel magnetoresistance Before surveying recent results on oxide spintronics, us let recall brie y the physics o f tunnel magneto resistance. the tunnel magnetoresistance (TMR) in Although magnetic tunnel junctions (MTJs) is known since the experiments of ere [6] thirty years ago, this phenomena has only Julli ` been under strong focus during the last ten years. This activity,by the possible use of TMR-based devices such pushed as volatile magnetic random access memories (MRAM), non has followed the observation of a large TMR effect (16%) at room temperature in 2 O3 /Co junctions [7]. The last CoFe/Alnot only to improvements in the amplitude of the decade has led TMR but also to advances in its u nderstand ing. Several effect recent report on the TMR effect [1], [8 ], [9]. In the reviews following emp hasize some significant we only aspects. A MTJ is composed of two ferromagnetic metallic electrodes san dwiching a very thin insulating barrier the carriers cross by quantum-mechanical tunneling. The have to TMR is as the variation of resistance between the parallel defined (R the antiparallel and ap ) state of magnetizations of the (R two magnetic electrodes:

N conventional electronics, information is encoded by the electron charge. In sp intron ics, the electron spin is used an as additional degree of freedom to perform logic operations, store information, etc. Spintronics exploits the spindependent properties of magnetic materials and semicond electronic uc- [1]. The first widely studied spintronics effect was tors giant magneto resistance (GMR), discovered in metallic multilayers or Co/Cu superlattices) in the 1980s [2]. (e.g. Fe/Cr Since a large variety of spintronics effects have been then, observed ied [1 ], some of which are reviewed in other and stud articles is Special of th Issue. Another spintronics effect that has given rise to a large number of experimental and theoretical studies is tunn el magnetoresistance (TMR). As we will show in the next part, large effects can be ob tain ed if special magnetic TMR materials (the so-called half-metals), having a finite density of states at level fo r one spin-directio n and a gap for the the Fermi other spin-direction, are used. Many materials that were conjectu red present th is unusual electron ic structure were to magnetic This opportunity of strongly enhancing oxides. spintronics magnetic oxides bridged a gap between the effects using metal spintronics community an d that of tran sition-metal oxides.
M.B. is with the Institut dElectronique Fondamentale, CNRS, Universit Paris-Sud, 91405 Orsay, France. Email : manuel.bibes@ief.u-psud.fr A.B. is with the Unit e Mixte de Physique CNRS-Thales, route d epartementale 128, 91767 Palaiseau, France. Email: agnes.barthelemy@thalesgroup.com e

I. I

NT ROD UCTION

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TMR=R

ap

Rp Rp

(1)

In the early stage of research on TMR, following the approach developed by Meservey and Tedrow [10], [11], this effect has been related to the spin polarization TMR P of the two electrod es by the P2 ere formula Julli` [6 ]: 1 P2 T M R = 2P 1 P 1 P2 with i (i=1,2) defined by the normalized difference P density of states at the Fermi level for the between the majority )) and minority (N i (E F (E F )) spin electrons, i (N i.e. (E F ) N i (E F ) Pi = N i N i (E F ) + N i (E F ) (3) Further ex periments have shown that the spin p olarization determined from tunneling experiments is not an intrinsic of the ferromag netic electrodes but depends on property the barrier [12], [13], i.e. the polarization represents an effective spin polarization of the tunneling probability. Recent theoreti- has clearly put forward the role of interfacial bond cal work ing the importance of symmetry in determining the and hybridizatio n between the Bloch states of the metal and the slowly states in th e insulator [14] [19]. Depending on decaying the barrier material, symmetry rules can select different wave functions for each spin direction and lead to different signs e spin polarization for the same ferromagnetic of th electrode. This effect is even reinforced by the record magnetoresistancebeen obtained recently with epitaxial values that have MgO [20] [24] following theoretical predictions [18], barriers [19]. B. Why oxides ? Another way to o btain very larg e TMR ratio is to use half metallic electrodes. It is indeed very straightforward from the ere formula that materials with o nly o ne spin Julli ` Fermi level (i.e. a to tal spin polarization) should the direction at produce TMR. Among the materials that have been record predicted to be half-metals, many are o xides (for a description and classification of half-metals, see [25], [26]). This triggered an important activity on magnetic oxide thin films, with the main objective o f making oxide tunnel junctions and measure TMR effects. This will be reported in Part II as well as results concerning the search for novel materials with a large spin polarization and a high C . T More recen tly, it was realized that the large number of degrees of freedom existing in transition metal oxides could to design their physical properties according be used to some specific required function. In additio n, the tend ency towards d evice miniaturization has emphasized the need for multifun ctio nal materials, i.e. materials that can perform more one task or that can be manipulated by several than inde- ent stimuli. The larg e variety and the tunability of pend the physical properties exhibited by transition-metal oxides (ferroelectricity, ferromagnetism, antiferromagnetism, metallicity, superconductivity, optical properties, etc) like perovskites thus provide tremendous advantages for spintronics by bring ing

and

(2)

add itional functionalities that do not exist in more conven- u sed materials. In this perspective, research on tionally oxidebased spintronics might well be only at its beginning. Parts III and V will p resent su ch oxide materials that are emerging of sp intron ics, namely diluted magnetic in the field oxides and multiferroic materials. Part IV summarizes the results using the innovative concept of spin filtering obtained using ferromagnetic or ferrimagnetic insulating oxides as th e tunnel barrier. Finally, Part V will discuss the potential of oxides for prospective spintronics applications. II. H A. Manganites Even th ough the term half-metallic ferromagnet was coined in 1983 by de et al for Mn-based Heu ssler Groo predictions of a half-metallic character was extend ed t alloys [27], to double-exchange oxides such as 1984 [28], 3 O4 in 2 Fe 1986 [29] and manganites in 1996 [30]. The halfCrO in metallic of manganites was demonstrated for the first time character by spin-resolved photoemission experiments [31], through which a positive spin-polarization in excess of 90 % was determined. manganite-based mag netic tunnel junctions By that time, with TMR values had already been fabricated and large measured [33] but it was only some years after [4], [32], et al s Park publication [31] that TMR measurements correspondin g to spin-polarizations exceeding this value were measured [34]. Manganites crystallize in the simple perovskite structure. The parent comp ound is an 3 LaMnO antiferromagnetic 3+ charge-transfer insulator. Substituting a fraction of the La by divalent ions such as 2+ ions induces a transition to Sr a ferromagnetic and metallic state for substitution levels of about [35]. Mixed-valence manganites such as 17 % Sr x MnO 3 1x La double-exchange ferromagnets with a maximum are Curie temperature of 360K for x=0.30-0.40. As the literature of manganites is immense and has been extensively reviewed many times, we will refer the reader to such articles [35] and focus in the following on the use of [40] manganites in magnetic tunnel junctions 1) The first TMR measurement on magnetic TMR: with tunnel junctions manganite electrodes was reported by the group of Sun (IBM Yo rktown Heights) in 1996 [4], [32]. The best results were obtained on junction s using optimaldoped Sr 1 /3 MnO 3 (LSMO) electrodes and 3 to 6 2 /3 La nm thick (STO) barriers. The junctions were defined 3 SrTiO by a combination of optical lithography and ion-beam etching. A maximum TMR of 83 % was found [4] (at 4.2K) which, according to ere formula [6], corresponds to a Julli` spinpolarization of 54 % for the LSMO electrodes. et al s Lu pioneering paper also reported several hallmark features of manganite MTJs, such as the early disappearance of TMR increasing temperature and the typical deviation upon from the parabolic behavior found in conductance (G) curves at low bias voltage. A few months after th ese first two p apers, the Sun group reported a TMR of 400 %, co rresponding to P 81% [41]. This was soon followed by et al s Viret that independently reported a 450 % TMR at 4.2K pap er in LSMO/STO/LSMO junctions [33].
IGHLY SPIN

-POLA RIZ ED OXID ES

IE EE T RA NS. ELE CT RON. DEVI CE S, VOL . X, NO. XX, AUGUS T 20 06

(a) (b)

1 60 1 40 1 20 1 00 80 60 40 20 0

1.0 0.8 0.6 0.4

-2-1012

LSMO/ST O LSMO/Ti O LSMO/LA O

H (kOe) Fig. 1. (a) R(H) curves collected on four LCMO/NdGaO 3 /LCMO junctions, corresponding to a maximum TMR of 630 % (with the definition of Eq. 1), measured at 77K (reproduced from reference [42]); the different curves correspond to different junctions. (b) TMR of ~ 1000 % at 4.2K in a LSMO/LAO/LSMO junction (LAO is for LaAlO 3 ) [43].

T*
0.2 0.0
LSMO surface Magnetizatio n

(a)

0 100 200 300 400

T (K)
(b)

Sub sequent publications b y the Sun group and others reported increasingly large TMR values (see figure 1), up to TMR of 1 850 % in a LSMO/STO/LSMO MTJ, as a found by et al in 2003 [34]. This record TMR Bowen correspond s to a spin-polarization of 95 %, i.e. a virtually halfmetallic character for LSMO. 2) Temperature dependence of the TMR: Soon after the first observation s of these large TMR ratios, much attentio n was brough t to the temperature dependence of the TMR. Indeed, in manganite tunnel junctions, the TMR decreased rather rapidly with temperature and d isappeared at a critical temp erature T* (typically 200K in early reports), well below the Curie temperature of the electrod es (maximized at 360K in LSMO). This problem motivated both theoretical [44] and ex perimental manganite-based junctions and also stimulated research on the search for other half-metallic ferromagnets with high . C er T Several explanations have been invoked to explain the differen ce between T* and : defects in the tunnel b C T arrier causin g spin- ips [45], [46 ], non-optimal magn etic proper- manganite/barrier interfaces (either due to ties at oxygen deficiency [33 ], to phase-separation [42], etc). We note that properties of manganite interfaces have been explo the red extensively thro ugh the study of manganite surfaces [47] and manganite/insulator interfaces, in thin films [48], [49] and heterostructures [50], [51]. Disrupted magnetic and electronic (the main features of which are a lower properties C ,a T lower saturation magnetization, a larg er resistivity and a larger low-temperature magnetoresistance) are consistently observed in manganite ultrathin films. It has been suggested that this disruption is due to strain [52], charge-transfer [53] o r atomicscale disorder p romoting charge trapping [54 ]. Recently, systematic studies of interface effects in manganite heterostructures an d manganite tunnel junctions have addressed this issue in greater detail. et al measure Garcia the temperature dependence of the TMR in manganite d tunnel junctions with either STO, LAO or [55 ]. 2 barriers TiO markably, for all these junctions, T* is virtually theResame and to 300K, irresp ective of the barrier material an d thus close of type of manganite/barrier interface. The spinthe polarization not decay very rapidly with temperature actually does (see ure 2a), as opposed to the spin-polarization of a fig manganite

Fig. 2. (a) Temperature dependence of the spin-polarization of several manganite interfaces, as measured by Garcia et [55]. The graph also al includes the temperature dependence of the magnetization of a LSMO film, and that of a LSMO free surface (as reported in [47]). (b) Temperature dependence of the magnetization of several manganite interfaces measured by magneto-optical second harmonic generation (MSH) by Yamada et al [53]. LMO stands for LaMnO and the STO/LMO curve corresponds to a 3 LSMO/LMO(0.8 nm)/STO engineered interface.

free surface [4 7], bu t follows a Bloch law P(T ) = P

0

(1 aT

3 /2

) (4)

with a values only slightly larger than the one found for LSMO (from M(T) data) [55]. Recent mag netobulk optical LSMO/LAO and LSMO/STO interfaces indicate data on that interface magnetization vanishes close to 300K for the both interface types [53] (see figure 2b), in good agreement with Garci et al s a Figure 2b results. also includes the M(T) for a LSMO/STO in interface 2 unit cells of which 3 have been inserted been LaMnOand the STO layers. The purpose o f the LMO layer is the LSMO to compensate for charge transfer that was found to occur at the LSMO/STO interface [56 ], increasing the hole den sity in the LSMO unit-cells. Even though better magnetic last properties for this en gineered interface, the efficiency of are obtained this

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1, 0 0, 8 0, 6 0, 4 0, 2 0, 0

R(H) I(V)

-1,2 -0,9 -0,6 -0,3 0,0 0,3 0,6 0,9 1,2 V (V)
DC

Fig. 3. Bias dependence of the TMR (normalized to its value at 10 mV) in a LSMO/STO(2.8nm)/LSMO junction, at 4.2K [59].

approach to enhance the TMR and its temperature stability to be demonstrated clearly remains [57]. Bias dependence of the TMR: 3) In addition to its temperature dependence, the bias-dependence of the TMR in mang an- MTJs has also received some attention . One of the ite main features of the TMR(V) in manganite-based junctions is the decrease o f the TMR with bias voltage, at least in th e rapid low ( 0.2V) bias range [41], [58], [59]. We note that this behavior is accompanied by a specific zero-bias anomaly (ZBA) in the uctance curves. In magnetic tunn el junctions, a cond ZBA is usually observed and ascribed to the absorption/generation of spin-waves by tunneling electrons [60]. The ZBA in manganitehas been studied theoretically by junctions et al [61] Gu proposed that due to the double-exchange interaction, the who 3 /2 , low- conductance is proportional to bias in V agreement with experimental results [4], [34], [59], [62]. Su ch magnon excitations depolarize the spin of the carriers h ence decreasing spin-polarization and th us the TMR. At the effective larger bias, et al have reported the observation of a Bowen TMR, close to V=0.35 V, followed by anoth er plateau in th e strong beyond 400 mV [59], see figure 3. This in decrease ectioncorresponds to the onset of tunneling into the point spin- co nduction band of LSMO (as predicted by down Bratkovsky position in energy above the Fermi level [63]) whose can be precisely inferred from TMR measurements. The thus value (380 meV) is in good agreement with results from found spinpolarized inverse photoemission [64]. We note that in MTJs on half-metallic Heussler alloys, an analogous in based uence spin-dependent density of states on the TMR(V) of the has reported recently [65]. For further details on the been bias dependence of the TMR in LSMO MTJs and the physics of coherent tunneling in such structures, the reader is referred to Bowen et al [66]. 4) Funda mental tunneling studies with manganite-based junctions: Given their almost total spin-polarization, mang anites are particularly well suited for performing fundamental tunneling studies. For instance, they can be spin-polarized used

to probe the spin-dependent density of states of a material used electrode, as in the previous example. One can as an replace the manganite counter-electrode by some other ferromagnetic some insight on the electronic properties metal and get of metal, as well as on those of the barrier material, this via analysis of the junction cond uctance curves and the TMR(V) is exemplified by the results of de data. This e Teresa [13] on LSMO/STO/Co junctions. In such t al [12], the MTJs, at low bias is negative (i.e. the spinTMR polarization interface with STO is negative) and shows of Co at the a negative maximum at about V=0.4V for electrons tunneling from LSMO to Co. Upon further increasing the voltage, the changes sign to become positive at V -0.8V. TMR These were qualitatively confirmed by results et al i Hayakawa /STO/LSMO junctions [67], [68]. It was argued n Co 9 0 Fe 1 0 that this very peculiar dependence arises from specific bon ding effects at the STO/Co interface, favoring the tunn el transmis- Co d states that have a negative spinsion of polarization at calculations also predicted the appearance EF . Theoretical of a sizeable magnetic moment on the Ti ions adjacent to the interface, antiparallel to the Co magnetization [16]. However, recent experiments have been u nable to confirm this prediction [69]. Experimentally, a negative spin-polarization for Co at the interface with epitaxial [70] and 3 [71] 2 TiO also reported. The TMR(V) of Co/LAO/LSMO LaAlO barriers was junctions is strikingly similar to that of Co/STO/LSMO junctions. This strongly suggests that wave function symmetry selection by epitaxial barrier is a key parameter in determining the the tunnel current in these junctions. Unfortunately, the structure of p erovskite insulatin g oxides that are traditionally used as tunnel barriers , , etc) is more 3 3 (SrTiO of rock-salt MgO and this maycomplicated LaAlO than that ex plain why so complex electronic stru cture calculations are few available oxides compared to the MgO case [19], [72] for these [74]. So far, only the complex band structure of 3 has been SrTiO calculated and pub lished [75], [76], even though preliminary results exist concerning indicating a 3 [77], LaAlO negative spin-polarization for a Co/LAO interface, in agreement with experiments [71]. B. Double perovskites Even though the study of manganite-based MTJs has deepened our understanding of spin -polarized tunneling and interface properties of these complex oxides, the the of initial of using them for room-temperature spintronics hopes appli- have not been fulfilled . Devices exploiting cations some of the transport properties o f manganites at or close to room temperature have however been proposed, such as contactless potentiometers based on the colossal magnetoresistance effector bolometers [79], [80] bu t none of these are [78] strictly speaking spintronics devices. other hand, the remarkab le low-temperature On the spintronics prop erties of manganites soon motivated the search half-metals with higher Curie points. Several for new high-compounds had b een predicted to b e half-metallic in TC the 1980s, like [28] and Heussler alloys [27] but 3 O4 Fe the

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first spin-polarization measurements on these systems with a structure were disappointin g [81]. Much effort for complex the discovery of new highfocused on C half-metals T which a great experienceperovskites accumulated for had been through the study of manganite films and heterostructures. of double-perovskites first received The family theattention[82][85] but it is only in 1998 that it was 1960s in first conjectured that 2 FeMo 6 (SFMO) should be halfSr [86]. This compound O indeedmetallic of the required had some proper- a good half-metal, such as an almost integer ties of magneticand, remarkably a moment of 420K and an C T magneto resistance slowly decaying intergrain with temperature (which was though t to re ect better interface properties than those of manganites [87]). research on double-perovskites such as SFMO Most has focused on bulk samples and aimed at u nderstand ing betterstructural, electronic an d mag netic properties, and their the ection between them. The magnetic interaction is a conn special type of dou ble exchange in which the metallic band is formed by the overlap of Fe states, O 2p states and Mo 2g 2g t states [8 8]. The spin of thet itinerant electrons is antiparallel moment of the Fe ions and parallel to the to the local small moment carried by the Mo ions, and thus the spinpolarization to be negative. A first ev idence for this is expected mechanism was provided by et al [89]. With in the doubleBesse exchange picture, the Curie temperature d epend s on band filling and attempts to increase the of SFMO by La doping at C T sites have been successful [90 ]. Unfortunately the the Sr magne- of these do ped systems decreases with doping as tization the introduction of dopant ions enhances the Fe/Mo disorder [90], [91]. Nevertheless, a few undoped double-perovskites have C T above 500K such as FeReO 6 [92], [93] and CrReO 6 2 2 Ca Ca FeReO has an insulating behaviour but Sr [94]. 2 6 2 CrReO 6 Sr is metallic [93]. The possible half-metallic character of this compound is still deb ated [95], [9 latter 6]. The advantages of SFMO and other metallic doubleperovskites are thwarted by some severe problems. The first is that optimal magnetic properties require a perfect one threedimensional ordering of the magnetic ions at the perovskiteand Mo in the case of SFMO. When cationic sites, Fe B disorder the magnetization decreases systematically due is present, to antiferro magnetic coupling between Fe neighbors at antiph ase boundaries [97], [98]. Diso rder is also detrimental to the spinpolarization [99]. Another one is its strong reactivity to air water, which makes pro cessing and storage p and roblematic [100] . Despite these difficulties, the growth of doubleperovskite thin films was carried out in several laboratories. Different growth techniques have been used [101], [102], the more being pulsed laser deposition (PLD) [103][107]. popular To obtain single-phase SFMO films by PLD is very difficult. The growth pressure mu st be kept very low because at higher pres- the more stable sure 4 compoun d forms [103 ], SrMoO [108]. Conversely, at such low pressures, metallic Fe and 3 O4 Fe tend to appear [108], [109], and thu s yield overestimated values. In addition, high growth magnetization temperatures (typically above 8 50 C) are required to obtain a good Fe/Mo ordering .

5.5x10 5.0x10 4.5x10 4.0x10 3.5x10

(a)

T=4 K =10 V DC mV

-2 -1 0 1 2

H (kOe)

(b)

Fig. 4. TMR curves measured at 4.2K on a SFMO/STO/Co tunnel junction [110] (a) and a SFMO/I/Co tunnel junction [111] (b). In this last structure I is the native oxide appearing at the surface of SFMO layers.

Several grou ps have attempted to measure the spinpolarization of SFMO, mostly in thin films. Values of 60 % have been estimated throug h point-contact to 75 spectroscopy measurements [112], [113 ]. Given the poor compatibility of SFMO with typical perovskite barrier materials (like ) and its reactivity to water, SFMO-based 3 SrTiO junctions are tunnel extremely challenging to fabricate and specific lithography processes need to be developed. Using a special nan oindentation-based lithography technique [114 ], it h as been possible to define Co/STO/SFMO nanometric ( 20 nm in diameter) tunnel jun ctio ns and to measure their TMR at low temperature, see figure 4a. The TMR of such jun ctio ns is positive and rang es from 10 to 50 % [110]. As Co/STO/LSMO TMR of up to -50 % [13], the observation junctions give a ofTMR of +50 % in Co/STO/SFMO indicates that the a spinpolarization of SFMO is comparable to that of LSMO, but with an opposite sign, i.e. at least -80 %. Mo re recently Asano also reported the observation of a positive TMR al have 10 of at 4K in SFMO-based junctions, using a native % oxide tunnel barrier and Co as the top electrode [111] as the (see figure 4b). Other doub le-perovskite compounds have also been

e t

grown in thin films, especially CrWO 6 [115], [116] and 2 Sr recently CrReO 6 [117] that has a more of 635K [94]. 2 C Sr data concerning the T spin-polarization of No these compounds is yet available. Finally, we wo uld like to point out that the physics of double perovskites have been recently rev iewed by et al [118] Serrate .

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C. CrO

Chromium dioxide ) is a metallic binary oxide 2 (CrO in the tetragonal rutile structure. The crystallizing moments oforder ferromagnetically below the Cr ions 395K. At C T low temperature, the satu ration magnetic moment is B /f.u., as 4 + ions with a 2 2 expected for a collinear ordering of the 2g Cr t electronic configuration. The Fermi level lies in the half-full band dyz dz x and 2 is a proto typical doubleCrO exchange system. The low-temperature resistivity is on the order of.cm in high q uality thin films [119]. More details on 1 the properties of 2 can be found in reference CrO [25]. CrO films can be grown by chemical vapor d eposition (CVD) [120], [121], thermal decomposition [122] or pulsed laser deposition (PLD) [123]. A large spin-po larization can be expected for 2 from its electronic structure and the CrO large powder magnetoresistance observed in polycrystalline samples [124], ascrib ed to spin-dependent tunneling between grains. techniques have been used to measure d irectly Several the spin-polarization. Andreev re ection experiments with 2 CrO superconducto r point contacts [125][127] have indicate a very P, up to 97 %, at low temperature. Spin-dependent large tun- experiments using a supercon ducting Al spinneling detecting (Meservey-Tedrow technique) confirmed this electrode result Despite these record spin-polarization values, [128]. rather TMR effects have been reported in small 2 -based MTJs. CrOto now, three groups have published results on the Up fabri- and characterization of such MTJs, using cation 2 as one CrO electrode and Co as the other [129][131]. The selection of barrier material is a problem as a native oxide the 2 O3 ) (Cr metric layer forms at the surface of the nano 2 films. Th CrO can nevertheless be used as a tunnel barrier, is layer yielding a maximum TMR of -8% [130]. We note that 2 O3 is a Cr multiferroic material [132]. Depositing Al to form a composite CrO x barrier has allowed to increase this value x AlO ]. These TMR values are far too small in to 24 % [131 view almost total spin -polarization measured in of the Andreev and Meservey-Tedrow experiments, likely re ection due a modified electronic structure of at the interface 2 CrOnative barrier. The presence of impurity states inside with the the barrier, making inelastic tunneling processes dominant, is also a likely explanation as pointed out by et al [131] Parker . D. Fe
3 2

is indeed indicated by electronic structure calculations [28], [134] [136].

(a)

(b )

Fig. 5. (a) TMR curve measured at 4K in a Co/Al (from [137]. (b) TMR curve of a Fe 3 O4 /MgTi (from [138]).

O 4 junction 2 O 3 /Fe 3- x O 4 /LSMO junction, at 50K

O4

Magnetite O4 ) is the oldest known magnetic 3 (Fe ferrimag net with material. temp erature of It is a a critical C =858 T O crystallizes in the spinel structu re whose A sites K. Fe 3 4 3+ 2+ occupiedare by ions an d B sites by a mixture of Fe Fe 3 + ions. As Fe and in most spinel ferrites, the ferrimagnetic ordering arises from the strong antiferromagnetic coupling the A and B sublattices. Within the B sublattice, between the ions are coupled ferromagnetically. Given the mixed Fe Fe valence in this sublattice, double-exchange interaction can take as was theoretically described by Loo s and Novak place, [133]. A half-metallic state with a total negative spinpolarization is conduction band being formed by the expected, the overlap of spin-down Fe 2 g states with O 2p states. This is t what

At room temperature, magnetite is a bad cond uctor, with a metallic behavior o ccurring in the 320-800K range [139]. room-temperature the resistivity is th ermally Below activated, with a transition to a charge-ordered insulatin g state below the Verwey transition temperature 1 20K). The V (T precisea long-stan nature o f the electronic properties below is V T ding problem in solid-state physics that is still strongly debated as by the contradictory review articles published illustrated by Walz [140] and et al [141] Garcia growth of magnetite thin films has been carried . The by out many groups, by a large number of deposition techniques such as sputtering [142], molecu lar-beam epitaxy [143] and laser deposition [144]. It is a consistent trend in pulsed the literature that the properties of magnetite thin films d eviate those of the bulk. In particular, their from magnetization is hard to saturate and often lower than the bulk o ne [142], [145]. These effects are exacerbated by thickness reduction , and films as a few nm become superparamagnetic [146], as thin [147]. disrupted magnetic properties are accompanied by These an increase in the electrical resistivity and a blurrin g or even disappearance of the Verwey transition [148], [149]. This has been convincingly related to the films micro stru cture and the presence of an tiphase boundaries [149], [150]. spin-polarization of magnetite measured by The spinpolarized photoemission spectroscopy is generally found to be negative, ranging from -40 to -80 % [151][155]. This is lower than what is expected from band structure calculations and several explanation s have been put forward to explain this discrepancy (surface reco nstruction [156], surface etc). The spin-polarization values deduced from defects, spin- enden t tunneling experiments show a large dep dispersion ure 5). (see fig et al [137] have found a Seneor spin-polarization of about 50 % frompositive TMR experiments on Fe 3 x O4 / 2 O3 /Co junctions (see figure 5a). This Al positive sign, also observed by et al [157], et al Aoshima Yoon [160], [158], et al [1 59] an d et al Bataille Reisinger spin-polarization stands in contrast with the negative calculated or measured by spin-polarized photoemission. A negative spin-polarization was also found by the Suzuki gro up in LSMO/CoC 2 O4 /Fe 3 O 4 [161], (see 2 O4 /Fe3 O4 r LSMO/MgTi O jun ctio ns [162]. figure 5b) and 2 O 4 /Fe 3 4 LSMO/FeGa cently, et al have also measured Re- negative a Parkin spinpolarization of -48 % for [163]. 3 O4 / x interfaces Fe AlO This

IE EE T RA NS. ELE CT RON. DEVI CE S, VOL . X, NO. XX, AUGUS T 20 06

large dispersion in the sign and values of the spinpolarization be related to the strong sensitivity of the is likely to electronic of iron oxides to oxy gen stoichiometry properties [14]. few other spintronics dev ices b ased on A 3 O4 have Fe fabricated. This is the case of magnetic tunnel also been transistors using a magnetite emitter, an alumin a barrier and a Si collector [164]. Current-in-plane (CIP) GMR structures with Au or Pt spacer lay ers have also been studied by van et al [165 Dijken ] and et al [166]. A maximum MR ratio of 5 % Snoeck measu red at was low temperature. integrate Efforts to O 4 into semiconductor 3 Fe [167][170] have not permitted yet structures devices to fabricate that exploit the spintronics properties of would 3 O 4 . Surface Fe interface properties of and are still under 3 O4 Fe n to understand spin-polarization measurements and investigatio their ection with predictions from ab-initio calculations conn [156], Another issue is the ro le o f antiphase bound aries [171]. [149]. devices with lateral sizes in the deep sub 100 Defining nm might permit to avoid the contribution to antiph range ase boundaries and define better their role on transport properties. we note th at Finally, O4 is a magnetoelectric material 3 Fetemperature, see for in stance [172], [173]. This at low potentiality for spintro nics (discussed in part V) has not been exploited yet. E. 2 O4 NiFe Apart from 3 O4 , all other bulk spinel ferrites are Fe insulating. This is the case of that has an 2 O4 [174] NiFe structure in its bulk form and shows ferrimagnetic inverse spinel order 850K and an insulating character with a room below temperature resistivity of 1k .cm [175]. Its magnetic structure of two antiferromagnetically coupled consists sublattices. A is formed by ferromagnetically ordered 3+ first sublattice Fe 5 , magnetic moment (M) : 5 (3d ) ions occupy ing B tetragonal A sites of the spinel Othestructure, while 2 4 2+ AB the second sublattice contains ferromagnetically ordered Ni 8 , M=2 (3d ) and Fe 3 + (3d 5 , M= B ) ions occupy B 5 ing the octahedral B sites. This type of ordering results in a saturation magnetization of 2 B /f.u. (f.u. : formula unit) 3 . Recent electronic or 300 structure calculations emu.cm have smaller gap values for spin-down consistently estimated than spin-up [176] for [178]. Remarkably, O4 can be turned into a 2 NiFe in thin films grown by spu ttering on conductive material substrates 3 SrTiO in a pure Ar atmosphere. This conductive behavior [179] (room temperature resistivity: 100 m .cm [180]) is likely to be related to oxygen vacancies promoting a mixed valence for the Fe ions [181] as occurs in magnetite. In addition, these films exhibit magnetic properties that radically differ from those of bulk O4 [182], namely a saturation magnetization 2 NiFe to 300 % [179]. Preliminary X-ray magnetic larger by up circular indicate that this enhanced magnetic moment dichroism is great extent due to cationic inversion between the ions at a to the A and B site [181]. Cation ic inversion is known to occur ferrite thin films [183 ], [184] and has also been spinel in reported in nanoparticles [185] [187]. Such conductive 2 O4 films have been used as NiFeelectrodes in mag- /LSMO netic magnetic 2 O4 / 3 NiFe SrTiO tunnel

1 .0

400

350 300

TMR : 120% PNFO : ~40%

0 .8 0 .6 0 .4 0 .2 0 .0 1 .0

(b)

250 200

(c)

0 .8

(a)

4K

0 .6 0 .4 0 .2 0 .0 0 5 0 1 00 1 50 2 00 25 0 30 0 P
LS M O

150 - 4 0 0 0 -2 0 0 0 0 2 0 0 0 4 0 0 0

No r mal ize d TMR

H (Oe)

T (K)

Fig. 6. (a) TMR curve measured at 4K for a magnetic tunnel junction with one LSMO and one conductive NiFe 2 O 4 electrodes (from [180]). (b) Temperature dependence of the conductive NiFe 2 O 4 spin-polalarization, as deduced from TMR vs temperature measurements (c) and the temperature dependence of the spin-polarization of LSMO/STO interfaces (from [188]).

junctions, see figure 6. A TMR ranging in 15 to 140 % has measured at low temperature [180], [188], co been rresponding to a maximum spin-p olarization of 45 % for the NiFe Significantly, this value is clo se to the largest layer. spinpolarization measured for mag netite by tu nneling experiments. as visible in figure 6b , this spinIn addition, polarization is virtually constant up to 300K, in agreement with the high T of O4 . 2 NiFe n ote that recently, condu ctive We O4 films 3 (Mn,Fe)fabricated [189]. Evidence for a finite have also been spinpolarization at room temperature has been provided by anomalous Hall effect [189] and p reliminary TMR measurements in Co/Al x / 3 O4 junctions O (Mn,Fe) [190]. F. SrRuO
3

O4

SrRu 3 is a metallic ferromagnet C =160K) O (T in the perovskite structure [191]. Its goodcrystallizing electrical conductiv- it a material of choice as electrode for ity makes ferroelectric capacitor measurements. The conduction band is formed by overlap of Ru the and O 2p orbitals. It is not a 2g t doubleexchange system but an itinerant ferromagnet [192] [194]. Electronic structure calculations have predicted a neg atively spin-polarized state, with P -60 % [195]. first measurement of the spin-polarization of The SrRuO was performed by Worledge and Geballe using a MeserveyTedrow techn ique [196]. A negative number was found, in agreement with theoretical predictions, but with a much value (-9%). Subsequent Andreev re ection smaller experi-reported a value of 50 % [197] (Andreev re ection ments is sensitive to the sign of the spin-polarization). The not spinpolarization of 3 has also b een determined from SrRuO TMR experiments in tunnel junctions 3 /STO/LSMO SrRuO These two studies [198], a negative TMR, as [199]. found expected the ere model [6] and inferred a spin-polarization from Julli` ut -10 of for abo % 3 , in agreement with reference SrRuO It is interesting to note that[196]. the spin-polarization of SrRuO roughly like the magnetization [198], i.e. it does decays not vanish prematurely like that of manganite does. This observation confirms the robustness of interface 3 to SrRuO disorder, as inferred fro m magnetotransport data through artificial grainboundaries [200].

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III. D

IL UTE D MAGNE TIC OX IDES

The search for novel magnetic materials, with ideally large spin-polarization, high C and possib ly multifunctional T characteristics has triggered an intense activity on doping nonmagnetic semiconducting oxides with magnetic ions. To a extend the ch oice of oxide hosts was motivated by great the prediction b y et al of a T C above 300K in MnDietl [201]. This prediction opened a way to achieve doped ZnO roomtemperature operation with diluted magnetic semiconductors even nowadays is impossible with (DMS), which (Ga,Mn)As, the prototypical DMS [202]. we will not review extensively the quickly g Here ingrow- of diluted magnetic oxides (for more details field see references [203][20 6]) but focus on some asp ects most re- to their relevance for spin tronics. The first lated important experimental repo rt on diluted magnetic oxides was by Matsumot et al [207] who observed a ferromagnetic o room temperature in Co-d oped (7%) behavior at . This was 2 TiO soon followed by papers rep orting ferromagnetism in Codoped and V-doped ZnO [209]. Later on, [208] ferromagnetism several other diluted magnetic oxides, was reported in with differen t oxide hosts 2 , In 2 O3 , HfO 2 , 2 O, etc). It (SnO proved very difficult to unambig uously demonstrate Cu soon that ferromagnetic behavior, typically observed using the standard metry techniq ues (e.g. SQUID, AGFM, VSM), magneto was intrinsic (e.g. due to so me exchange mechanism resulting from the substitu tion of some cation of th e matrix by the magneticrather than extrinsic (due to the formation of dopant) parasitic or ferrimagnetic p hases, in the form of ferro nanometric clusters, filaments, etc). Actually, little unambiguous evidence for intrinsic ferromagnetism in dilu ted magnetic oxides exists.accumulation of experimental results has also The challenged imagine interaction mechanisms compatible theorists to withdata. This has led to the development of novel the conceptsF-center exchange [210] and 0 ferromagnetism such as d ferromag netism without ions having partially filled d [211], i.e. or f shells. Despite these efforts, the physics o f diluted magnetic not well understood and still the object of oxides is intense experimental and theoretical activity. following, we present some relevan t results In the in obtainedmagnetic oxides over the last few diluted years. A. 2 TiO Ferromagnetism in transition-metal-doped was first 2 TiO observed in anatase films grown by 0 .9 3 Co 0 .0 7 O2 Ti laser deposition by et al pulsed [207]. A few Matsumoto months later, et al also reported room temperature Chambers in Co-doped ferromagnetism anatase 2 films grown by oxyg TiO enplasma-assisted mo lecular-beam epitaxy [212], [213]. A ferromagnetic behavior was also found fo r sputtered Codoped TiO anatase 2 films [214], and in Co-doped rutile 2 [215] TiOthe origin of ferromagnetism in this . Controversy on system appeared early after th ese first reports with the observation of clusters by several groups [216][218 ]. These Co Co clustersferromagnetic or superparamagnetic and give rise can be to anomalous Hall effect [218]. Subsequent reports an have nevertheless provided strong indications that ferromagnetism

is possible in cluster-free films in which the Co dopants are homogeneously distributed within the material (see for instance [219]). It thus appears that only in a narrow range of growth conditions (i.e. dopant concentration, growth temperature, growth pressure and growth rate) can cluster-free films be produced. This obviou sly makes comparisons between films in different systems grown a fortiori with different and growth techniq ues very difficult, if possible at all.The origin of ferromagnetism in doped has been 2 TiO the object of much theoretical [220], [221] and experimental [223]. As before, it is hard to summarize efforts [222], the whole literature as contradictory reports have been published. Nevertheless, the Kawasak i group has provided indications for carrier-mediated ferromagnetism in Co-doped 2 throug TiO h systematic studies of transport properties like the anomalous [224] and X-ray photoemission spectrosco py Hall effect experiments [225]. In this system, carriers are usually provided vacancies and their concentration adjusted by by oxygen the oxygen partial pressure during growth (see for instance [226]). the ro le of oxygen vacancies is n ot restricted However, to electron doping as their presence was found to in uence the nucleation of metallic clustered phases [227]. Furthermore, oxygen vacancies alo ne (i.e. in the absence of magnetic could give rise to ferromagnetism. For instance, dopants) Yoon et al recently reported a ferromagnetic behavior in 2d TiO films [228]. In addition, other typ es of defects (e.g. structuralco uld also be relevant for ferromagnetism defects) [229]. thoug h the observation of anomalous Hall effect Even be may taken as evidence that charge carriers are spinpolarized,direct proof is provided by spin-dependent a more tunneling experiments. Recently, et al repo rted the Toyosaki characterization of tion and Fe 1 0 / fabrica-.9 5 Co 0 .0 5 O 2 d / 0 90 x Co AlO Ti R(H) magnetic tunnel junctions [230], [2 31]. Hysteretic curves were observed at low temperature (see figure 7), with a maximum MR of 11 %. The MR disappeared at about 20 0K, was attributed to the p resence of defects in the b which arrier. preliminary results remain to be confirmed by These further experiments on better-quality junctions. we note that a reversible electric-field Finally, themodulation of of a magnetization Co0 . 0 7 O2 film was reported in 0 .9 3 Ti a structure PbZr 0 .2 T 0 . 8 5 O3 / 0 .9 3 Co0 . 0 7 O2 / [232]. 3 i of th is effect in MTJs based on Co-doped Ti SrRuO The exploitation TiO ld allow the design of n ovel multifunctional cou spintronics devices . B. ZnO Ferromagnetism in transition-metal-doped ZnO was first reported by et al in 2001 [208]. The measured Ueda magnetic Co moment was 2 in 0 .8 5 films. Another B /Co 0.15 O Zn in V-dop ed ZnO was also early report of ferromagnetism published by the same group [209]. Since these first papers, ZnO films with different 3d ions have been grown by a doped number of techniques, the most popular being pulsed laser dep osition. of the research status o f doped ZnO films h ave Reviews been ed recen tly [205], [233]. As with publish the 2 , TiO of ferromagnetism is not clearly established but precise origin several theoretical models have been put forward to describe the

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8.0

70.5

7.5 70.0 7.0 69.5 6.5

(a) (b)
6.0 -4 0 0 0 - 20 0 0 0 2 00 0 4 0 00

H (O e)

69.0 -1 0 0 0 - 5 0 0 0 5 0 0 1 00 0 H (O e )

Fig. 7. Resistance vs field curves measured at different temperatures in a Ti0. 95 Co 0. 05 O2 - d /AlO x /Co 0. 9 Fe 0. 1 junction. (from [230]).

Fig. 8. (a) TMR curve measured at 4K and 10 mV on a CoLSTO/LaAlO 3 /Co/CoO tunnel junction (see reference [254]. (b) TMR curve measured at 4K and 10 mV on a Co-LSTO/SrTiO 3 /Co nanojunction defined by the process described in [114].

physics of transition-metal-doped ZnO. They can be divided in two categories: (i) models b ased on Zener double-exchange or RKKY interactions [201], [234]; (ii) models based on Fcenter exchange [210]. Reports of the presence of ferromagnetic Co clusters [235] or parasitic phases [236] have questioned the possib ility of an intrinsic ferromagnetic behavior. Nevertheless, some reports have evidenced a strong spd coup ling, indicative of a coupling between the magnetic d carriers [237]. More recently, a detailed dopant an analysis of Co-doped ZnO and Mn-doped ZnO films [238] has shown that ferromagnetism is carrier-related. The introduction of p- carriers by N dopants induces ferromag netism in type Mn- ZnO, and n-type carriers provided by interstitial Zn doped are necessary for ferromagnetic Co-doped ZnO [239]. These experimental results are in agreement with theoretical predictions [240], [201], [241 ]. search for a finite spin-polarization of carriers The nothas been very successful but recently et al [242] Xu et al [243] have measured anomalous Hall effect in and Peng doped ZnO. CoMagnetic tunnel junctions using a Co-doped ZnO electrode and giving rise to a magnetoresistance effect have measured by been et al [244]. However, the in Rode of Co-clusters present in the ZnO uence has to be films clearly before drawing conclusions on a possible studied intrinsic spinpolarization. C. 3 (La,Sr)TiO When is doped with La, a transition from 3 SrTiO to a metallic state occurs for a La an insulating concentration % [245][247]. as low as 5 Sr x Ti 3 is a 1x La metal with a low-temperature resistivity ofOabout paramagnetic 200.cm for the x=0.5 compoun d. The temperature dependence of its resistivity is dominated by electron-electron scattering mechanisms, evidencing the strong electronic correlations atsystem. The importance of correlations play in this become particularly visib le as x increases [248] and the system iscloser to the driven 3 end compound that is a LaTiO prototypical antiferromagnetic Mottinsulator. Epitaxial films of have been grown by 0 . 5 Sr 0 .5 Ti 3 La O a few groups [249], [250], mostly motivated by its possible use electro de for ferroelectric capacitors or as a as transparent

con ductor. The idea of doping (LSTO) films 3 (La,Sr)TiO with et al . As a magnetic ions was introduced by Zhao [251] host material, LSTO differs from most oth er systems by its strongly-correlated character and its large carrier density. Its perovskite structure is an advantage for film growth and for combining it with other functional oxides like manganites or A ferromagnetic behavior with a Curie multiferroics. temper- the 500K range was found by ature in et al [251], Zhao for a doping level of only 1.5 %. The films resistivity was very sensitive to oxygen pressure during growth, and a metallic 4 mbar, indicating state found for pressures lower than was 10 clear role o f oxygen vacancies in transport. a This was confirmed by annealing studies [252]. A ferro magnetic behavior was also found for Co-doped LSTO films by et al [253]. Ranchal Auger electron spectroscopy or high-resolution transmission electron microscopy with electron energy loss analyses did n ot identify phases nor Co-rich clusters [254]. Preliminary Xparasitic ray absorption spectroscopy experiments indicate that the Co ions are in a 2+ state in a octahedral environment [255]. a high As ferromagnetic metal, Co-d oped LSTO is C T an interesting material for spin-injection. To determin e its spinpolarization, et al fabricated /Co3 Herranz Co/LaAlO magnetic tun nel junctions and measured their LSTO magnetotransport ch aracteristics [254]. A typical TMR curve obtained on junctions is represented in figure 8. The an alysis of such the bias dependence of the TMR in several /Co3 Co/LaAlO junctions in terms of defect-assisted tunneling yields a LSTO value % for the spin-polarization of Co-LSTO. We of -80 note a TMR was also observed on junctions with that 3 , SrTiOa lower value [256], see figure 8b. The TMR but with decreases with temperature and disappears around 200K, likely due to spin-depolarization inside the barrier or to the impossibility of achieving an antiparallel state above this temperature. Despite these encouraging tunneling results, the phy sics of Co-doped LSTO remains unclear. Recent studies of transition- doped metal 3 films, showing a p aramagnetic SrTiO 7], suggest that thebehav- of La and of hence ior [25 presence a large carrier density is required for ferromagnetism. Many issues are still unadd ressed, like the role of oxygen vacan- the dopant type. On this latter point, the cies or studies of (La,Sr) et al [258] 3 bulk samples b y In (Ti,Cr)O et al [259] aba and Iwasawa might bring interesting insight.

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10

IV. S

PI N -FILTE RI NG

18

The concept of spin filter relies on the use of a or ferromagnetic ferrimagnetic insulating tunnel barrier. In a ferromagnetic material, the conduction bands are spin and insulating split by exchange leading to two different barrier heights for spin- spin-down electrons. The combin atio n of a up and nonmagnetic electrode with a ferromagnetic barrier yields two different currents fo r spin-up and spin-d own very electrons exponential dependence of the transmission with due to the the barrier heigh t, resulting theoretically in a very large spin polarization. Such a non-magnetic-metal/ferromagneticinsulatorconstitutes a kind of artificial half metal. bilayer Following early experiments by et al [260 ], the validation of Esaki the spin-filter co ncept and the determination o f its efficiency in spin-polarizing the current was reported by Mooderas group In these first experiments the spin polarizatio n of [261]. the current was measured by a supercon ducting counter electrode temperature. The spin polarisation can also at very low be checked by a metallic ferromagnetic counter-electrode whichacts as a spin analyser also [262]. Several ferromagnetic or ferrimagnetic oxides, EuO [263], NiF 2 O 4 [180], [264], 2 O4 [265], 3 [266] e BiMnO La 0. 1 B 0 .9 CoFe 3 [267], [268] have been used as and MnO i magnetic sp in insulating barriers in such filters. A. EuO The efficiency in spin polarizing the current by an EuO barrier has been measured using the Meservey and Tedrow techniqu e in Al/EuO/Ag and Al/EuO/Y/Al structures [263]. A spin polarisation of 29% at low temperature has been measured where a thin Y layer (5 nm) is in troduced at the in samples top interface in order to obtain a purer EuO phase. B. Spinel ferrites The spinel oxide family has been most widely studied. First experiments by the group of Suzuki using a ferrimagnetic O 4 barrier in O4 /CoCr 2 O4 /La 0 .7 Sr 0 .3 MnO 3 2 3 CoCr junctions didFe t clearly demonstrate a spintunnel no filter by the barrier due to the u se of two effect mag- materials as electrode and counter-electrode netic [161]. L ders et al u [180], [264] observed a large TMR fect of 52% atef-4K in O4 /La 0 .7 Sr 0. 3 MnO 3 and 2 Au/NiFe O / Au/NiF 2 4 /La 0 .7 Sr 0 .3 MnO 3 tunnel junctions. In 3 e SrTiO the latter h eterostructures, th e STO spacer is introduced to induce magnetic decoupling between LSMO and a better 2 O4 . NiFe 9a represents the magnetoresistance curve of such Figure a spin filter. When the co nfiguratio n of the magnetizations of the 2 O 4 barrier and the LSMO counter-electrode NiFe an antiparallel to a parallel state, a large drop in goes from the resistance is observed . The positive TMR observed, with a resistance larger in the antiparallel state than in the parallel one corresponds to a positive spin filtering efficiency of 23%. is in contrast with the negative spin polarization that This could be expected from band structure calculations (conduction band fo r sp in down than for spin up) for the inverse and smaller the normal spinel structure [176], [269]. The positive spin filtering

(a 16 )

14 12 10 -4 -2 0 2 4

H (kOe)
(b)

Fig. 9. (a) TMR curve measured at 4K and 10 mV on a Au/NiFe spin-filter (from [264]). (b) Minor TMR loop measured at 300K on a Au/CoFe 2 O 4 /MgAl 2 O4 /Fe 3 O 4 spin-filter (from [265]).

O4 /LSMO

efficiency has been attributed to the different symmetry of the up and spin down conduction ban d and to the spin resulting filtering [264]. More recently, Chapline and symmetry Wang have claimed to have observed a sizeable filtering [265] effectroom temperature in at O4 / O 4 /Fe 3 O 4 . The 2 2 Au/CoFe layer has been introd uced to decouple the MgAl MgA 2 O4 l zations of magnetithe spin-filter barrier O4 ) and the 2 (CoFe ). Measurements are performed by electrodea (Fe 3 O4 using conducting tip AFM. Fig. 9b shows the minor loop magnetoresistan ce curve obtained wh ile reversing the 3 O4 magnetization. Fe positive magnetoresistance of 24% is observed at A room temperature. The corresponding positive filtering efficiency has attributed to the lower energy of the been 2 g conduction 2+ t band of the ions in antisites. Such a change of sign in Co the filtering efficiency by cation inversion is in co ntrast with the d structure calculations of ban et al [176], [269] Szotek the preservation of a minority gap smaller than that suggest the majority one in the normal spinel structure as for the inverse structure of spinel 2 O4 . NiFe C. BiMnO
3

Large TMR effects have also been reported for barriers of some ferromagnetic-insulating manganites 3 [266] (BiMnO MnO (LBMO) [267], [268]). Due to the and La 0 .1 B 0 .9 3 i multiferroic character of these materials results are reported in the following Part. end this Part on spin-filtering by mentioning that We the

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11

bias-dependence of the TMR in spin-filters has not been properly addressed yet. Few papers report on ex perimental on calculations [270]. A very rapid decrease of results o r the TMR at low bias followed by a less pronounced variation reported by have been uders et al [264] and L Gajek [266], which could be due to ex citation of spin waves in the magnetic insulating b arrier as found with NiO ferro barriersTheoretical input of this idea has not been [271]. published yet. V. M

et al

ULTIFE RROICS

Multiferroics is an emerging family of materials in the field of spintronics. Th ese multifunctional materials present more ferroic orders among ferromag netic, two or ferroelectric, ferro elastic or ferrotoroidic. Magnetoelectricmultiferroics in which ferromagnetic (bu t it is also a general trend to in clude antiferro magnets or weak ferromagnets in this definition) and electric o rders coexist with a magnetoelectric ferro coupling th em, open the possibility of controlling the between polarization by a magnetic field or the magnetization by an field. This should allow the design of, for electric examp le, ferro electric memories which can be magnetically recorded or, more interestingly, to MRAM recorded electrically. Whereas the reversal of the po larization by a magnetic field or even the induction of a ferroelectric order by a magnetic field have reported in several materials (see for example been [272]and figure 10), literature is extremely scarce as to [275] the reciprocal effect, which may b e due to the small number of ferro - (or ferri-) magnetic ferroelectrics. The small abundance of single-phase multiferroic materials [276] is circumvented by the emerging field of artificial multiferroics combinelectric and magnetic materials in a same ferro ing heterostructure [73], [277]. of the work reported on multiferroics has been Most performed o n bulk materials but an increasing effort is made to obtain high-quality th in films. The purpose of this chapterto make an exhaustive review on multiferroics is not but to highlight a few experiments on thin films of interest in the of spintronics. For furth er information on field multiferroic reader is referred to recent reviews [278] materials, the [280]. most studied multiferroic material is The which 3 , BiFeO is one of the few multiferroics with both critical temperatures an d ferroelectric) much larger than 300K (i.e. magnetic [281], Its antiferromagnetic [283][285] character has [282]. been to induce an exchange bias on a soft ferromagnetic used layer at room temperature [286 ], [287]. Th is capability, together preservation of the ferroelectric character of with the this material down to 2 nm [288] as well as the observation of a tunnel magnetoresistance through [287] 3 barriers BiFeO make this material very promising in the field of spintronics and should allow the desig n of tunnel magnetoresistancebased devices controlled electrically [289]. potential of multiferroic materials is fu rther The illustrated by two very recent results. The first one is the first demonstration of the electric field control of the exchange bias in hexagonal heterostructures [290]. 3 based YMnO magnetic character of The compound has been antiferro the used

Fig. 10. Reproducible reversal of the ferroelectric polarization by an external magnetic field in the spin-spiral compound CoCr O 4 . The upper panel shows 2 the geometrical relationship between M, P and T (toroidal moment), from [275].

to exchange bias a thin [291] o r 8 0 Fe 2 0 [290] 3 SrRuO Ni . Applying a dc voltage on the antiferromagneticferroelectric YMnO 3 layer causes a modification of the exchange bias and reversal of the magnetization of the 8 0 Fe 2 0 layer Ni a Ni 8 0 Fe 2 0 /YMn O 3 /Pt heterostructure, as shown o n Fig. in The exploitation of 11. multifu nctional character of the these multiferroic materials is also exemplified by the recent results of Gajek and coworkers in and LBMO-based 3 BiMnO heterostructures [268]. is an established 3 BiMnO [292][29 4]. In ad dition, a ferroelectric ferromagnetic insulator character claimed by several groups [295][2 97]. has been e Gajek t al have proposed to use a ferromagnetic and ferroelectric material as a tunnel barrier in order to obtain a four resistance level device. Thin ferromagnetic insulating layers of 3 BiMnO B and La 0 . 1 0 .9 MnO 3 have been used as ferromag netic barriers i in 1 x Btunnel 3 /LSMO spin filters [266], MnO x Au/La ifiltering efficiency respectively. [267] with 22% and 35% spin By lying a magnetic field, switching the configuration of app the magnetizations of the barrier and the LSMO counterelectrode from antiparallel to parallel produced two distin ct resistance states related to the tu nnel magnetoresistance effect. The polarization of the ferroelectric 0 .1 B 0 .9 Mn O3 barrier La ad ditional degree of freedom and accordingly two gives i an other resistance states are obtained, corresponding to an electrore- phenomena of 20% [268] (for details on sistance ferroelectric tunnel junctions, see [2 98]). VI. S
PINTRONICS DEV ICES WI TH OXIDE MATE RIALS

Research on half-metallic oxides has allowed to measure record TMR values [34] and to get a better understanding of

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12

Fig. 11. Magnetization of a Ni in which an 8 0 Fe 2 0 /YMnO 3 bilayer, exchange bias is induced on Ni 8 0 Fe 20 by YMnO 3 , as a function of the voltage applied across the YMnO 3 layer (from [290]).

netoelectric co upling [301] might allow to switch electrically the resistance of a spin-valve or MTJ adjacent to a BFO layer near future. This achievement would represent a in the major breakthro ugh for spintronics since it would allow to write a magnetic bit electrically, with very little power co nsumption. might then arise as to the integration of Questions devices multiferroics into CMOS tech nology. Goodbased on quality BFO films can be grown on to Si substrates epitaxial [302]. regard, it is also important to note that In this perovskite already been integ rated to CMOS techno oxides have logy information storage ap plicatio ns. Ferroelectric for memories (FERAMs) [303] using ferroelectric 3 (PZT) have Pb(Zr,Ti)O been fabricated by Fujitsu using a 0.5 m CMOS process and integrated as 4kbit memory elements in each Sony Play station have been sold to over 100 millions units 2 (that worldwide). Samsung are now shipping 32 Mb and 64 Panasonic and Mb FERAM chips, respectively. tly, Fujistu announced in July 2006 that their Significan nextgen eration FERAMs will be based on a 3 , BiFeO free ferroelectric [304]. A multiferroic material will thus be soon in a wide-scale microelectronic product. CMOS used industryalready exploiting the potential of complex is thus oxides for applications and wide-scale fabrication processes to define p erovskite oxide layers with lateral dimensions in active the nm ran ge are 100 available.longer timescale, the development of reliable On a high magnetic oxides with large spin-polarization at diluted T roomtemperature and above, and electrically tunable magnetic and electronic properties might play a role in future spintronics devices. ZnO is a particularly promising candidate (duelo ng spin lifetime [305]) and prospectives its to spintronics s based on ZnO would benefit from the huge app lication effort that is currently being made to use ZnO in optoelectronics and fabricate low-dimension ZnO structures to [233]. VII. C
O NCLUSION S AN D PE RSPE CT IVE S

lead-

spin-dep enden t tu nneling. However, manganite-based tunnel junctions show a vanishingly small TMR at 300K and are thus usable for applications. Room temperature results not using magnetic oxides with higher such as Fe 3 O4 are C T [137], with TMR ratios one order of magnitude smaller modest than o btained on last-generation MgO-based MTJs those [299]. However, some very recent developmen ts permit some optimism as to the possible future use of magnetic oxides in spintronics devices. important observation is that the vast majority A first of magnetic oxides with high critical temperatures are (i) Fe- and (ii) insulating. One might thus arg ue that based future device-oriented research sho uld focus on these sy stems. Such insulating Fe oxides exist in many structural families (perovskites, garnets, spinels, corundum, etc) and can be anti- magnetic or ferrimag netic. So far, mostly two ferro groups of insulating Fe oxides have been studied for spintronicssp inel ferrites as spin-filter barriers and purposes: BiFeO derived compounds) as multiferroic elements. Spin-filters have th e potential to gen erate currents with spinpolarization approaching 100%, which seems to be difficult by using epitaxial diamagnetic barriers such as MgO, because of finite tu nneling probability for states of all sy the mmetries.very highly spin-polarized current sources If such become for example using spinel ferrite tunnel barriers, available, the of po ssible applications for spintronics devices range might rapidly to logic in addition to data extend storage. Another promising family of materials for spintronics

(and

applications are multiferroics, and especially 3 that has BiFeO very high critical temperatures and has alread y been studied extensively in thin film form. Since not 3 is BiFeO but antiferromagn etic (in addition to ferromagnetic being ferroelectric), spintronics could be for exchangeits interest for biasing Robust and large exchange bias effects has purposes. been recently demontrated at room temperature in 3 / BiFeO [300]. The combin atio n of exchange bias with CoFeB bilayers mag-

The use of magnetic oxides in spintronics architectures dates back from only 10 years ago. Since that time, this field has developing quickly. Record spin-p olarization and been TMR have been rep orted in several systems, confirming values the predicted half-metallic character of manganites, 2 CrO SFMO. New families of magnetic oxides, namely diluted magnetic oxides and multiferroics, have emerged and started their potential for spintronics. Even tho ugh this h as reveal to been a leitmotif goal for many years, the observation of a large spinpolarization at room temperature has not been possible until while in the meantime epitaxial MgO-based now, junctions have reached TMR values as high a 400 % [24 ] at 30 0K. However, the recent discovery of novel C spinhigh-T oxides [230], [254] and the observation of large polarized magnetic spinfiltering effects with spinel ferrites [264], [265] bring hopes of large TMR effects at room temperature and achieving beyond, magnetic using oxide materials. In addition, the relevance of ox ides for spintronics notdoes restrict to generating highly spin -polarized currents. Approaches to exploit their multifunction al character are pro mis- and reveal new or p oorly add ressed physical ing phenomena.

and

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Efforts towards an electrical control of magnetization are being pursued by several original approaches exploiting for instance the in uence of carriers on magnetization in Co-doped TiO magnetoelectric coupling [290] or strain effects [232], [306]. Current-induced magnetization switching, due to spintransfer, observed in manganite-based tunnel junctions, has been with a poor reproducibility [307]. This approach certainly deserves furth er attention, from both experimentalists an d theorists. We also note that bilayers consisting o f a ferroelectric/piezoelectric oxide and a ferromagnet (either oxide or metal) are currently being investigated [306]. Electric mod- of the magnetic properties of the ferromagnet by ulations the electric or piezoelectric layer have been rep orted ferro [308], [309]. While most ex perimental work has fo cused on epitaxial perovskite bilayers such as 3 [309], LSMO/BaTiO also been predicted for important [310] effects have 3 /Fe BaTiO thus be observable at roo m temperature and and should above. promising approaches for oxide-based electronics Other

and spintronics rely on engineering interfaces between two oxides, two-dimensional phases with novel electronic to design prop- An interesting example in provided by the erties. observation of a metallic beh avior at a / interface, i.e. a 3 3 LaTiO SrTiO ) system combinin g a Mott insulator and a band 3 (LaTiO ) [311], [312]. Theoretically calculations on this insulator (SrTi 3 O interfaces predict a rich variety of n ovel prop erties type of [313] like a ferromagnetic state [313]. Interesting [318], charge- effects have also been observed at transfer / 3 3 LaAlO SrTiO [319] interfaces, but the reported transport properties may be dominated by the conductive electron-doped sub strate 3 SrTiO The large Hall mo bilities observed in such [320]. 3 SrTiO systems [321], [322] as well as in ZnO films based [323] are promising for spin-transp ort experiments in fieldeffect transistor samples [324], [325]. Future research directions in oxid e spintronics may also exploit the new physical properties of oxides in further reduced dimensions, i.e. one- and zero-dimensional objects. It is inter- to note that nanowires or nanotubes of several esting magnetic oxides have been synthesized [326], [3 27], 3 O4 (Fe LSMO case [328], Co-doped 2 [329], etc), with in some TiO unexpected and promising highly properties [330 ]. To perform spindependent transport in gated structures using these nanotubes challenge experimentalists and might unveil [331] will novel physical effects. Optimism is p ossible in view of the recent enden t transport measurements in planar devices spin-dep com- LSMO spin-injecting an d spin-detecting electrodes bining with carbon nanotubes [332], [333]. ACKN OWLED GME NT The authors would like to thank J.M.D. Coey, A. Fert, V. Garcia, G. Herranz, N.D. Mathur, J.S. Moodera, F. Petroff, T.S. and J.F. Scott for help ful comments on the manu Santos script. R EFERE NCES
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es-Herrera, Nature ,

Manuel Bibes was born in 1976 in Sainte-Foy-la-Grande, France. He received his Ph.D. degree in 2001 from the Universitat Aut` onoma de Barcelona, Spain and the Institut National des Sciences Appliqu ees, Toulouse, France after a joint Franco-Spanish thesis on interfaces in manganites at the Institut de Ci` encia de Materials de Barcelona, under the supervision of J. Fontcuberta and J.-C. Ousset. After a two-year postdoc in A. Ferts group in Orsay, France he became a CNRS research scientist at the Institut dElectronique Fondamentale, Orsay, France in 2003. His current research interests include spin-dependent tunneling, spin-filtering, multiferroics and diluted magnetic oxides.

Agn`es Barth elemy received her Ph.D. in 1991 from the University of ParisXI, Orsay, France, under the supervision of A. Fert. She became an assistant professor at this university that same year, carrying out her research activity in the Unit e Mixte de Physique CNRS-Thomson. During her Ph.D. and the following years, her main research subject was giant magnetoresistance in metallic multilayers. In 1998, she began working on magnetic tunnel junctions based on magnetic oxides such as manganites. She became a Professor of Physics in 2004 and is now leading the Multifunctional Oxides group at the Unite Mixte de Physique CNRS-Thales. Her research focuses on the physics of such oxides and their integration in spintronics architectures.