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GaN:Gd: A superdilute ferromagnetic semiconductor with a Curie temperature above 300 K PDF

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Preview GaN:Gd: A superdilute ferromagnetic semiconductor with a Curie temperature above 300 K

GaN:Gd: Asuperdilute ferromagnetic semiconductor witha Curie temperature above300K S. Dhar,∗ O. Brandt, M. Ramsteiner, V. F. Sapega,† and K. H. Ploog Paul-Drude-Institut fu¨rFestko¨rperelektronik, Hausvogteiplatz 5–7, D-10117 Berlin, Germany Weinvestigatethemagneticandmagneto-opticpropertiesofepitaxialGaN:Gdlayersasafunctionoftheex- 5 ternalmagneticfieldandtemperature.Anunprecedentedmagneticmomentisobservedinthisdilutedmagnetic 0 semiconductor. TheaveragevalueofthemomentperGdatomisfoundtobeashighas4000m B ascompared 0 toitsatomicmomentof8m B.Thelong-rangespin-polarizationoftheGaNmatrixbyGdisalsoreflectedinthe 2 circularpolarization of magneto-photoluminescence measurements. Moreover, thematerialssystemisfound tobeferromagneticaboveroomtemperatureintheentireconcentrationrangeunderinvestigation(7×1015 to n 2×1019cm−3).Weproposeaphenomenologicalmodeltounderstandthemacroscopicmagneticbehaviorofthe a J system. Ourstudyrevealsacloseconnectionbetweentheobservedferromagnetismandthecolossalmagnetic momentofGd. 9 1 PACSnumbers:75.50.Pp,76.30.Kg,75.50.Dd,71.35.Ji ] i c Efficientspininjectionintosemiconductorstructuresisone beam epitaxy (RMBE). The RMBE system (base pressure: s - ofthemostimportantrequirementstorealizefuturespintronic 2×10−10 Torr) is equipped with conventional effusion cells l r devices. A ferromagneticmaterialcompatiblewith semicon- forGa (purity: 7N)andGd(purity: 4N)[5] andanunheated mt ductorgrowthwhichthuscouldeasilybeintegratedintosemi- NH3 (purity: 7N) gas injector. A substrate temperature of conductordeviceswouldbethebestchoice.Sincethediscov- 810◦C (ourstandardgrowth temperaturefor GaN) was used. . t eryofaCurietemperatureT ashighas110Kin(Ga,Mn)As The Gd/Ga flux ratio was changed in order to adjust the Gd a C m [1],III-Vdilutemagneticsemiconductors(DMS)havegained concentrationinthelayers. Nucleationandgrowthwasmon- alotofattention. GaN-basedDMShavethepotentialforex- itored in situ by reflection high-energy electron diffraction - d hibiting high temperature ferromagnetism which is essential (RHEED). A spotty (1×1) pattern, reflecting a purely three- n fordevelopingfuturespintronicdevices[2]. Severaltransition dimensionalgrowthmode,wasobservedduringnucleationof o metal(TM)dopedGaNDMShavebeeninvestigated. Room- thelayers.Thepatternquicklybecamestreaky,reflectingtwo- c temperatureferromagnetisminthesematerials,however,isof- dimensionalgrowth. [ ten found to result from the formation of precipitates rather TheGdconcentrationofthelayerswasdeterminedbysec- 2 than from a homogeneousalloy [3]. The rare-earth (RE) el- ondaryionmassspectrometryusingaCAMECAIMS4fsys- v 4 ements could be an interesting alternative to transition met- tem, employing 0+2 primary ions with an impact energy of 6 als. REatomshavepartiallyfilled f orbitalswhichcarrymag- 7 keV. Mass interferencedueto parasitic molecularionswas 5 netic moments and may take part in magnetic coupling like avoidedbyselectingpreciselythemassesoftwoGdisotopes 2 in the case of TM with partially filled d orbitals. While it is (155.922and157.924). Theresultingionrateswereidentical 1 expected that the magnetic coupling strength of f orbitals is to within 1%. Measurements at different locations, each of 4 0 muchweakerthanthatofd orbitalsduetothestrongerlocal- whichinvolvedan area of 50×50 m m2, deviatedby nomore / ization of the f electrons, Gd is the only RE element which than5%. Theconcentrationwascalculatedaccordingtomea- t a hasbothpartiallyfilled4f and5d orbitals. Togethertheseor- surementsofanion-implantedstandard(sampleI),whichwas m bitalscantakepartina newcouplingmechanismproceeding implantedwith a Gd dose of1015 cm−2. The detectionlimit - viaintra-ion4f-5dexchangeinteractionfollowedbyinter-ion wasfoundtobe2×1015cm−3. d 5d-5dcouplingmediatedbychargecarriers[4]. Magnetization measurements up to 360 K were done in a n o Here,weperformasystematicstudyofthemagneticprop- Quantum Design superconducting quantum interference de- c erties of the DMS GaN:Gd. The magnetization measure- vice (SQUID) magnetometerwith the sample held in a plas- v: ments reveal an unprecedented magnetic moment of up to tic straw providedby Quantum Design. The response of the Xi 4000 m B per Gd atom. This colossal magnetic moment can magnetometerwascalibratedwithepitaxialFeandMnAslay- beexplainedintermsofalong-rangespin-polarizationofthe ersonGaAsforwhichthemagnetizationisaccuratelyknown. r a GaN matrix by Gd. This conclusion is independently con- The magnetization of undoped GaN layers was found to be firmedbythepronouncedchangesofthecircularpolarization indistinguishablefromthatofbareSiCsubstrates.Magnetiza- inmagneto-photoluminescencemeasurementsuponlightGd- tionloopswererecordedatvarioustemperaturesformagnetic doping. Moreover,allsamplesarefoundtobeferromagnetic fieldsbetween±50kOe. Themagneticfieldwasappliedpar- above room temperature. A phenomenologicalmodel is de- allel to the sample surface, i. e., perpendicular to the c-axis, velopedtoexplainthemacroscopicmagneticbehaviorof the forallmeasurements. Alldatapresentedherewerecorrected system, suggesting a close connection between the observed forthediamagneticbackgroundofthesubstrate. ferromagnetismandthecolossalmagneticmomentofGd. For magneto-PL, the sample was excited by a He-Cd ion The 400–700 nm thick GaN layers with a Gd concentra- laser at a wavelength of 325 nm. The laser power densities tion ranging from 7×1015 to 2×1019 cm−3 were grown di- focused on the sample were in the range between 200 and rectly on 6H-SiC(0001) substrates using reactive molecular- 250 Wcm−2. The experiments were carried out in the tem- 2 samples. Figure 2 (b) and (c) show the temperature depen- F 1019 G denceofthe magnetizationundera magneticfield of100Oe forsamplesAandC,respectively.Priortomeasuringthetem- E -3m) 1018 D SIMS profile : sample C pcoeroalteudrefrodmeperonodmentceemopfetrhaetumreatgon2etKizaetiitohne,rtuhnedsearmapslaetuirsafitirosnt (cd1017 C -3m) 1017 fieldof20kOe(Field cooled: FC) oratzerofield (zerofield NG1016 A B (cNGd1015 cZoFoClecdu:rvZeFsCar)e. IqtuiaslictaletiavrelfyrosmimtihlaersfeorfibgoutrhessatmhaptlethsefeFaCturainndg 10130 300 600 adoublesteplikestructurebelow100KintheFCcurves. In Depth (nm) 1015 thecaseofsampleC,thetwocurvesremainseparatedthrough- 10-6 10-5 10-4 10-3 10-2 outthe entire temperaturerange (2–360K), while they coin- Flux ratio J /J Gd Ga cide at around 360 K for sample A. The separation between theFCandZFCcurvesindicatesahystereticbehaviorwhich FIG. 1: Gd concentration as measured by SIMS as a function of is consistent with our previous observation from Fig. 2 (a). Gd/Gafluxratio(solidsquares). Thesolidlineisalinearfittothe ThetwocurvescoincideattheCurietemperatureT ,whenthe datarepresentingsampleC,EandF.TheGdconcentrationforsam- c ple A, B and D (open squares) is obtained from the corresponding hysteresisdisappears. Clearly,Tc isaround360Kforsample Gd/Gafluxratiobyextrapolation. Theinsetofthefigureshowsthe A while it is much larger for sample C. The separation be- SIMSprofileobtainedforsampleC. tweentheFCandZFCcurvesmeasuredat360Kisplottedas afunctionofGdconcentrationintheinsetofFig.2(c),andis seentoincreasewithincreasingGdconcentrationrevealinga peraturerange5–100K,inacontinuousHe-flowcryostat,and shift of T towardshigher temperatures. We have also inves- c in magnetic fields up to 12 T using the backscattering Fara- tigateda Gd-implantedGaN sample(sampleI)with a higher day geometry. In all measurements, the magnetic field was Gdconcentrationthanwecouldreachbyincorporationduring oriented parallel to the c-axis of the samples. The magnetic growth.Thissamplealsoexhibitsferromagnetismatandwell fieldinducedcircularpolarizationofthe(D0,X)transitionwas above room-temperature. These observations are consistent analyzed by passing the emitted light through a photoelastic withtheresultsobtainedbyTeraguchietal., whoobserveda modulator(PEM),aquarter-wave-plate,andalinearpolarizer. Curie temperaturelargerthan 400K in Ga Gd N alloys 0.94 0.06 GaN:GdlayersA–GweregrownwiththeGd/Gafluxratio [6]. increasingfromAtoGinalphabeticorder.Theconcentration TheeffectivemagneticmomentperGdatomp canbeob- eff of Gd (NGd) in samples C, E, F and G is measured by sec- tainedfromthevalueofthesaturationmagnetizationMs (peff ondaryionmassspectrometry(SIMS).InFig.1,N asmea- =M /N ). InsampleC, p isfoundtobe935and737m at Gd s Gd eff B suredbySIMSisplottedasafunctionoftheGd/Gafluxratio 2Kand300K,respectively.Thesevaluesareabouttwoorder f . SamplesC, EandF(solidsquares)arelyingonastraight ofmagnitudeslargerthanthe puremomentof Gd. In Fig. 3, line with a slope of unity indicating a linear dependence of p obtainedatdifferenttemperaturesisplottedasafunction eff Gdincorporationonf . TheGdconcentrationofsampleGis ofN . DataobtainedfromsampleIarealsoincludedinthis Gd smallerthanexpectedfromthislineardependence.Infact,we figure(solidsquares).Bothat2K[Fig.3(a)]and300K[Fig. haveobservedastronglyfacetedsurfaceforsampleG,indicat- 3(b)], p isfoundtobeextraordinarilylarge,particularlyfor eff ingthatGdisaffectingthegrowthmodeatthesehighconcen- lowGdconcentrations.AthighGdconcentrations,p isseen eff trations.N forsampleA,BandD(opensquares)isobtained to saturate. It is interesting to note that at 300K, the satura- Gd bylinearlyextrapolatingthecurvepassingthroughsamplesC, tionvalueisclosetothatoftheatomicmomentofGd(8m ), B E and F. The inset of the figure shows the SIMS profile ob- while at 2 K, it is clearly higher. This is true even for sam- tained for sample C. The concentrationof Gd is found to be pleI.Suchacolossalmomentcanbeexplainedintermsofa constantovertheentiredepthforsampleCandallothersam- veryeffectivespin-polarizationof the GaN matrix bythe Gd plesinvestigatedbySIMS,rulingoutanyaccumulationofGd atoms. In fact, in certain diluted metallic alloys, the solute onthesurfaceduringgrowth. Allsamplesweresubjecttoan atoms exhibit an average magnetic moment larger than their extensiveinvestigationbyhigh-resolutionx-raydiffractionin atomic value. This effect is called giant magnetic moment. a wide angular range. No reflections related to a secondary There are severalreportson a giant magneticmomentof Fe, phase was detected. Furthermore, we have investigated one Mn and Co when they are either dissolved in or residing on sample(C)bytransmissionelectronmicroscopy. Noclusters the surface of Pd [7, 8, 9]. This effect is explained in terms orprecipitateswereobserved.Electrically,allGddopedsam- of a spin polarization of the surroundingPd atoms. Very re- plesarefoundtobehighlyresistive. cently, a giant magnetic moment was observed in Co doped Figure 2 (a) shows the magnetization loops obtained for SnO2−d [10], a DMS. High-temperatureferromagnetismand sampleCat2Kand300K.Atbothtemperatures,themagneti- an unusually large magnetic moment were observed also in zationsaturatesathighmagneticfields(unlikesuperparamag- Fe-dopedSnO ,whichwasarguedtooriginatefromferrimag- 2 neticmaterials)andexhibitsaclearhysteresisatlowerfields. netic coupling mediated by electrons trapped on bridging F- Thesetwo featuresclearlyindicatea ferromagneticbehavior. centers[11]. Wehaveobservedqualitativelysimilarhysteresisloopsforall The above conclusion of a long-rangespin-polarizationof 3 0.6 2 K (a) 104 2 K 300 K 3m) 10 3m) 0.3 103 mu/c (emu/cM-00..30 3 (emu/cm)M 00..03 mp ()eB102 (eMS0.11 N1G01d7 (cm-3)1019 -0.3 -2 0 2 -0.6 H (kOe) 101 (a) -30 0 30 H (kOe) 1016 1017 1018 1019 1020 N (cm-3) 0.08 FC (b) Gd 300 K 103 3m) 10 c 3) u/ m m 1 (emu/cM0.04 mp ()eB102 (eMS0.1 10N17Gd (cm1-03)19 ZFC 101 (b) 0.00 0 100 200 300 T (K) 1016 1017 1018 1019 1020 0.12 N (cm-3) FC (c) Gd T = 360 K FIG. 3: Magnetic moment per Gd atom (p ) as a function of Gd ) MZFC3cm) 10-2 concentrationat(a)2Kand(b)300K.Theseaffturationmagnetization 3cm0.09 - MFC emu/ 10-3 t(hMesr)easspaecftuinvectiinosneotsf.GOdpceonnscqeunatrreastioarnearte2praensden3t0in0gKthiseaelxspoesrhimowenntianl u/ ( dataforsampleA–GandsolidsquaresforsampleI.Solidlinesare m (eM ZFC 1016 1N0G17d (1c01m8-31)019 thetheoreticalfitobtainedfromourmodel(discussedinthetext). 0.06 neticfield. Figure4showsthePLspectraforaGaNreference 0 100 200 300 sample [Fig. 4 (a)] and sample C [Fig. 4 (b)] under a mag- T (K) netic field of B=10 T. The transition is polarized for both samples,whichisevidentfromthedifferenceinintensitiesof FIG.2: (a)MagnetizationloopsobtainedforsampleCat2K(solid line)and300K(dottedline).Theinsetof(a)showstheloopsatsmall thetwocircularlypolarizeds + (opensquares)ands − (solid fields.Temperaturedependenceofmagnetizationatfield-cooled(FC) squares) components. Most importantly,the polarizationhas andzero-field-cooled(ZFC)conditionsatamagneticfieldof100Oe opposite sign for sample C when compared to the reference for(b)sampleAand(c)sampleC.ThedifferencebetweenFCand sample,whichclearlyindicatesthattheexcitonicgroundstate ZFCmagnetizationmeasuredat360KisplottedasafunctionofN Gd insampleCissubjectedtoaninternalmagneticfieldwhichis intheinsetof (c). Thesolidcurve through thedataisguide tothe effectivelystrongerthantheexternalfieldandisactinginthe eye. oppositedirection. ConsideringthatthemeanGd-Gdsepara- tionin sampleCis 25nm, andthatthe averagedistanceofa the GaN matrix by the Gd atomsis independentlyconfirmed (D0,X)sitefromaGdatomwillthusbeaslargeas12nm[13], bymagneto-PL.Intheabsenceofanexternalmagneticfield, thisfindingdirectlyconfirmsourpreviousconclusionthatthe Gdatomsareintroducingalongrangespinpolarizationinthe the PL spectra of all samples are characteristic for undoped epitaxialGaN layersin thattheyaredominatedby a neutral- GaN matrix. We also observethatthe relative changeof po- donor bound exciton (D0,X) transition at ∼3.458 eV. The larizationwithrespecttothereferencesampleincreaseswith lowerenergyofthistransitionwhencomparedtohomoepitax- the Gd concentration, as intuitively expected. These results, ial GaN is consistent with the tensile in-plane strain in these togetherwithaquantitativeanalysisofthedependenceofthe layers of 0.15% [12]. In all cases, the donor responsible for polarization on the magnetic field, will be reported in detail thistransitionisOwithaconcentrationofabout1018cm−3as elsewhere[14]. measured by SIMS. However, clear differences between un- Inordertogetaquantitativeunderstandingoftherangeof dopedandGd-dopedGaN layersareevidentwhenanalyzing thespinpolarization,wehavedevelopedaphenomenological the circular polarization of the PL in the presence of a mag- modelas explainedin the following. The polarizationof the 4 N (a) + (cid:2)p0−(p0+p1NGdv)e−vNGd(cid:3) 0 (3) Reference GaN N Gd AtlowGdconcentrations,mostofthespheresarewellsep- aratedand p hasits maximumvalue. As the concentration s - ofGdisincreeaffsed,moreandmorespheresoverlapandp de- eff ts) s + creases.Finally,ataveryhighGdconcentrationtheentirema- ni trix becomespolarized, and p approachessaturation. Note u eff thatthevalueofsaturationislargerthanthemagneticmoment . b ar ofbareGdatomsbyanamountof p1N0v. WeuseEqn.3tofit ( ourexperimentaldatawithpGd=8m Bandp0, p1andrasfree y parameters. The agreement is quite satisfactory as shown in nsit Sample C (b) Fig.3. Thefityields p0=1.1×10−3m B, p1=1.0×10−6m B, e and r=33 nm at 2 K and p = 8.4×10−4 m , p ≈0, and t 0 B 1 n r=28nmat300K.Thefinitevalueofp at2Kexplainswhy I 1 s - peff saturates at a value which is still higher than the atomic momentofGd. Mostimportant,however,isthatthevaluefor s + rissufficientlylargetoaccountforthestrongeffectofGdon theexcitonicgroundstateoftheGaNmatrix(cf. Fig.4). The second remarkable property of our GaN:Gd layers is thehigh-temperatureferromagnetismobservedinallsamples (wellaboveroomtemperature,comparedtoaT of289Kfor c 3.42 3.44 3.46 3.48 bulkGd).Webelievethattheferromagnetismandthecolossal Photon Energy (eV) moment of Gd observed in these samples are in fact closely related. An overlap of the spheres of influence establishes a (long-range)couplingbetweentheindividualspheres. Within FIG. 4: Circularly polarized PL spectra for (a) the reference GaN sampleand(b)sampleC,measuredat6Kunderamagneticfieldof the framework of percolation theory, ferromagnetism is ex- B=10TinFaradayconfiguration(Bkc-axis). pected to occur at the percolation threshold, when an ”infi- nite cluster” spanning macroscopic regions of the sample is formed. The percolation threshold is reached for our model GaNmatrixbytherandomlypositionedGdatomsisdescribed at v = 0.28955 [15, 16]. With increasing Gd concentration, asarigidsphereofinfluencearoundeachGdatom,meaning weewouldthusexpectaphasetransitionfromparamagneticto that all the matrix atoms within the sphere are polarized by ferromagneticbehavior. Furthermore,T whichdependsupon c anequalamountwhereasmatrixatomsfallingoutsideofthis thestrengthoftheoverlapisexpectedtoincreasewiththeGd spherearenotaffected.Letusassociateaninducedmomentof concentration.Thisisclearlyconsistentwiththeresultsshown p witheachofthematrixatomslyingintheregionoccupied 0 intheinsetofFig.2(c). byonesphere. Asoneshouldexpectanincreaseofthepolar- Unfortunately, the well-established percolation formalism izationofmatrixatomsiftheybelongtoaregionwheretwo(or cannotbe straightforwardlyadoptedto quantitativelyexplain more)spheresofinfluenceoverlap,weattributeanadditional the currentproblem. Itis intuitivelyclear thatthe spheresof momentnp tomatrixatomsoccupyingsitesinregionswhere 1 influence are not hard but soft, i. e., the polarization of the n (n=2,...N ) spheres overlap. Since their radius r is pre- Gd matrix induced by the Gd atoms must decay with increasing sumablymuchlargerthanthelatticespacinginGaN,wefur- distance.Theonsetofferromagneticordernowdependsupon therassumethatthespheresarerandomlyarrangedinathree- the precise shape of this polarizationcloud as well as on the dimensionalcontinuum(continuumpercolation). Within this overlap of two or more of these clouds. A quantitative pre- framework,thesaturationmagnetizationcanbeexpressedas diction of the onset of ferromagnetism in this situation thus N(cid:229) Gd requires a detailed understanding of the nature of the ferro- Ms=pGdNGd+p0vN0+p1N0 nvn (1) magneticcouplinginthismaterial. e n=2 e Regardingthemicroscopicoriginofthiscoupling,itisclear whereN0istheconcentrationofmatrixatomsperunitvolume, that it cannot be explained simply in terms of direct, double v is the volume of each sphere, v =1−exp(−vNGd) is the or superexchange between Gd atoms since the average Gd- volumefractionoccupiedbythespeheres,and Gddistanceistoolargeforsuchacouplingtoexist. Further- (vN )n more,allsamplesarefoundtobeelectricallyhighlyresistive, vn= Gd e−vNGd (2) ruling out free-carrier mediated RKKY (Rudermann–Kittel– e n! Kasuya–Yosida)typelong-rangecoupling. Finally, also very is the volume fraction of the regions contained within n recentproposalsaimedatexplainingagiantmagneticmoment spheres. The average magnetic moment per Gd atom p is eff and/or high-temperature ferromagnetism in various material thenobtainedas systems [7, 8, 9, 10, 11] do not apply to the currentrequire- p = p +p N v ment of a long-range coupling. An actual understanding of eff Gd 1 0 5 thephenomenonobservedinthepresentpaperwillrequirede- AcademyofSciences,194021St.Petersburg,Russia tailed ab initio studies, particularly of the f-d coupling be- [1] H.Ohnoetal.,Appl.Phys.Lett.69,363(1996). tween Gd and Ga. Considering the long spatial range of the [2] T.Dietl,H.Ohno, F.Matsukura, JCibertandD.Ferrand,Sci- ence287,1019(2000). couplingevidentfromourexperiments,suchcalculationsare [3] S.Dharetal.,Appl.Phys.Lett.82,2077(2003). computationallyverydemandingandarethereforebeyondthe [4] T.Storyetal.,Phys.Rev.Lett.77,3447(1996). scopeofthepresentpaper.Animportantresultforanytheoret- [5] ThepurityoftheGdingothasbeendeterminedbythemanufac- icalapproachwasrecentlyobtainedbyHashimotoetal.,who turer(StanfordMaterialsCorporation) viainductively-coupled showedthatGdoccupiesprimarilyGasitesinGaNevenata plasmamassspectroscopy. Thedatasheet ofouringotcertifies concentrationashighas6%(twoordersofmagnitudehigher that the ferromagnetic elements Fe, Ni and Co are present in thanthehighestconcentrationinvestigatedhere)[17]. residualtracesof≪100ppm,≪50ppm,andbelowthedetec- tionlimit(0.5ppm), respectively. Notethat the magnetization Our study has revealed an extraordinarily large magnetic observedinthisworkfor,e.g.,samplesAandCwouldrequire moment of Gd in GaN which can be explained in terms of anFe(Ni,Co)concentrationof1019cm−3andabove,threeor- a long-range spin-polarization of the GaN matrix by the Gd dersofmagnitudehigherthantheGdconcentration.Alsonote atoms. Thematerialisfoundtoexhibitferromagnetismabove thatthevaporpressureofalltheseelementsisalmostidentical room temperature even with a Gd concentration less than tothatofGd. 1016 cm−3. Thisfindingoffersanexcitingopportunity,since [6] N.Teraguchietal.,Sol.StateCommun.122,651(2002). GaN:Gd maybe easily dopedwith donors(acceptors)with a [7] G.Bergmann,Phys.Rev.B23,3805(1981). [8] J. Flouquet, O. Taurian, J. Sanchez, M. Chapellier, J. L. Tho- concentrationexceedingthatofGdtogeneratespinpolarized lence,Phys.Rev.Lett.38,81(1977). electrons(holes)intheconductionband(valenceband). Gd- [9] J.CrangleandW.R.Scott,J.Appl.Phys.36,921(1965). dopedGaNwithitsT aboveroomtemperaturemightthusbea c [10] S.B.Ogaleetal.,Phys.Rev.Lett.91,077205(2003). veryattractivecandidateasasourceofspin-polarizedcarriers [11] J.M.D.Coey,A.P.Douvalis,C.B.Fitzgerald,M.Venkatesan, forfuturesemiconductor-basedspintronics[18]. Appl.Phys.Lett.841332(2004). We are indebted to A. Trampert, K. J. Friedland and U. [12] P.Waltereitetal.,Appl.Phys.Lett.74,3660(1999). Jahnforimportantcontributionstothiswork.Furthermore,we [13] It can be easily shown that the average distance of an exciton thankJ.Herfort,M.BowenandR.Kochforvaluablediscus- bindingsitefromitsnearestGdatomis=0.480296a,wherea istheaverageGd-Gdseparation sionsandsuggestions. Wealsoacknowledgepartialfinancial [14] V.Sapegaetal.,unpublished. support of this work by the Bundesministerium fu¨r Bildung [15] R. Consiglio, D. R. Baker, G. Paul, H. E. Stanley, Physica A undForschungoftheFederalRepublicofGermany. 319,49(2003). [16] D.R.Baker,G.Paul,S.Sreenivasan,H.E.Stanley,Phys.Rev. E66,046136(2002). [17] M.Hashimotoetal.,phys.stat.sol.(c)7,2650(2003).Seealso Ref.6. ∗ Electronicaddress:[email protected] [18] S.A.Wolfetal.,Science294,1488(2001). † Permanent address:Ioffe Physico-Technical Institute, Russian

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