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Ferromagnetic ordering in (Ga,Mn)As related zincblende semiconductors Tomáš Jungwirth Institute of Physics ASCR University of Nottingham František Máca, Jan Mašek, Jan Kučera Josef Kudrnovský, Alexander Shick Karel Výborný, Jan Zemen, Vít Novák, Miroslav Cukr, Kamil Olejník, et al. Bryan Gallagher, Tom Foxon, Richard Campion, Kevin Edmonds, Andrew Rushforth, Devin Giddings et al. in collaboration with Hitachi Cambridge Polish Acad. of Sci. UT & Texas A&M Jorg Wunderlich David Williams, et al. Tomasz Dietl Mike Sawicki Allan MacDonald Jairo Sinova Univ. Wuerzburg Laurenc Molenkamp Charles Gould, et al. Spintronics in (Ga,Mn)As dilute moment ferromagnetic semiconductor Spintronic transistor Huge hysteretic low-field MR Sign & magnitude tunable by small gate valtages Wunderlich, et al., PRL (2006) Current driven magnetization reversal Magnetic race track memory 2 orders of magnitude lower critical currents in dilute moment (Ga,Mn)As than in conventional metal FMs Sinova, Jungwirth et al., PRB (2004) Parkin, US Patent (2004) Yamanouchi et al., Nature (2004) OUTLINE 1. Mn-doped GaAs material - only a factor of 2 short room-T otherwise outstanding properties 2. Mn-doped (Al,Ga)As and Ga(As,P) - useful materials to compare with and Ga(As,P) could lead to higher Tc 3. Mn-doped LiZnAs - still very closely related to (Ga,Mn)As and might heal its key problems (Ga,Mn)As material Mn As Ga - Mn local moments too dilute (near-neghbors cople AF) - Holes do not polarize in pure GaAs - Hole mediated Mn-Mn FM coupling 5 d-electrons with L=0 S=5/2 local moment moderately shallow acceptor (110 meV) hole Ohno, Dietl et al. (1998,2000); Jungwirth, Sinova, Mašek, Kučera, MacDonald, Rev. Mod. Phys. (2006), http://unix12.fzu.cz/ms Universal scaling of (Tc / Mn-moment) vs. (hole / Mn-moment) theory expectations Robust mean-field-like ferromagnet experiment hole density / Mn-moment density Jungwirth, Wang, et al. PRB (2005) coupling strength / Fermi energy Magnetism in systems with coupled dilute moments and delocalized band electrons band-electron density / local-moment density (Ga,Mn)As More Mn - interstitial incorporation Covalent SCs do not like doping self-compensation by interstitial Mn Interstitial MnInt is detrimental to magnetic order charge and moment compensation defect Yu et al., PRB ’02; Blinowski PRB ‘03; Mašek, Máca PRB '03 + Mnsub As MnInt Mnsub Can be annealed out MnInt Tc 95K in as-grown (9% Mn) theory & exp. to 173 in annealed (6% Mnsub) Ga but MnGa < nominal Mn Jungwirth, Wang, et al. PRB (2005) More Mn - problem with solubility - Effective concentration of uncompensated MnGa moments has to increase beyond 6% of the current record Tc=173K sample. A factor of 2 need (12% Mn is still a DMS). - Low solubility of group-II Mn in III-V-host GaAs makes growth difficult Low-temperature MBE A startegy: Find DMS system as closely related to (Ga,Mn)As as possible to with • larger hole-Mn spin-spin interaction • lower tendency to self-compensation by Mnint • larger Mn solubility • independent control of local-moment and carrier doping (p- & n-type) lattice constant (A) (Al,Ga)As & Ga(As,P) hosts 5.7 (Al,Ga)As Mn As 5.4 0 Ga(As,P) Ga 1 conc. of wide gap component local moment - hole spin-spin coupling Jpd S . s Mn d - As(P) p overlap GaAs & (Al,Ga)As Mn d level - valence band splitting d5 Ga(As,P) GaAs d5 (Al,Ga)As & Ga(As,P) (Al,Ga)As p-d coupling and Tc in mixed (Al,Ga)As and Ga(As,P) theory 10% Mn Ga(As,P) Smaller lattice const. more important for enhancing p-d coupling than larger gap Mixing P in GaAs more favorable for increasing mean-field Tc than Al 10% Mn Ga(As,P) Up to a factor of ~1.5 Tc enhancement 5% Mn theory Mašek, et al. preprint (2006) Microscopic TBA/CPA or LDA+U/CPA Mnint formation in mixed (Al,Ga)As and Ga(As,P) higher in (Al,Ga)As and Ga(As,P) than in GaAs smaller interstitial space only in Ga(As,P) No reduction of Mnint in (Al,Ga)As Mixing P in GaAs more favorable for suppressing Mnint formation theory Limits to carrier-mediated Weak hybrid. Delocalized holes long-range coupl. ferromagnetism in (Mn,III)V InSb, InAs, GaAsTc: 7 173 K d5 Similar hole localization tendencies in (Al,Ga)As and Ga(As,P) Strong hybrid. GaP Tc: 65 K d5d4 Impurity-band holes short-range coupl. Scarpulla, et al. PRL (2005) no holes d (GaN ?) d4 III = I + II Ga = Li + Zn GaAs and LiZnAs are twin SC Wei, Zunger '86; Bacewicz, Ciszek '88; Kuriyama, et al. '87,'94; Wood, Strohmayer '05 LDA+U sais that Mn-doped are also twin DMSs Masek, et al. preprint (2006) No solubility limit for group-II Mn substituting for group-II Zn theory Additional interstitial Li in Ga tetrahedral position - donors n-type Li(Zn,Mn)As Electron mediated Mn-Mn coupling n-type Li(Zn,Mn)As similar to hole mediated coupling in p-type (Ga,Mn)As EF Ga s-orb.L As p-orb. As p-orb. Comparable Tc's at comparable Mn and carrier doping and Li(Mn,Zn)As lifts all the limitations of Mn solubility, correlated local-moment and carrier densities, and p-type only in (Ga,Mn)As Conclusions 1. Relatevily small technological investment in Mn-doped (Al,Ga)As useful info about trends in III-V's and for Ga(As,P) 2. More tech. difficult Mn-doped Ga(As,P) - could lead to higher Tc 3. Adventureous Mn-doped LiZnAs - might heal key problems in (Ga,Mn)As & n-type FS super-exchange (anti-ferro) kinetic exchange (RKKY) Intrinsic properties of Ga1-xMnxAs Mn Mn As Mn Ga room-Tc for x=10% hole density (nm-3) hole density / Mn density Effective kinetic-exchange Hamiltonian, microscopic TBA or LDA+U • Tc linear in MnGa local moment concentration • Falls rapidly with decreasing hole density in more than 50% compensated samples • Nearly independent of hole density for compensation < 50%. Extrinsic effects - covalent SC do not like doping self-compensation by interstitial Mn Interstitial MnI is detrimental to magnetic order: compensating double-donor – reduces carrier density attracted to substitutional MnGa acceptor and couples antiferromagnetically to MnGa even at low compensation Yu et al., PRB ’02; Blinowski PRB ‘03; Mašek, Máca PRB '03 MnGa - As + MnI Ga Tc in as-grown and annealed samples Open symbols as-grown. Closed symbols annealed 180 140 0.1 M[110](T) / MSat(5K) 160 8% (Ga,Mn)As T = 172 K 0.0 120 -0.1 -1 Magnetic 0 Field 1 [ Oe ] 180 180 160 80 40 1.7% Mn 2.2% 1.7% Mn 3.4%Mn Mn 2.2% 4.5%Mn Mn 3.4% 5.6%Mn Mn 4.5% 6.7%Mn Mn 5.6% 9%Mn Mn 6.7% Mn 8% 9% Mn C 20 160 140 140 180 120 1.7% Mn 120 160 2.2%100 Mn 100 3.4% Mn 140 80 4.5%80 Mn 120 5.6% 60 Mn 66.7%60 7 Mn 1005 40 9% Mn 40 80 doping (%) Mn 20 total 20 60 TC(K) T (K) 60 0 0 1 2 3 4 Mn Total TC(K) TC(K) 100 Tc=173K (%) 8 9 10 A A A A Linear increase of Tc with effective Mn moment doping Mneff = MnGa-MnI 180 160 MnGa - 140 As MnI Ga 120 TC(K) + Closed symbols are annealed samples 100 80 60 High compensation 40 20 0 0 1 2 3 4 5 (%) EffectiveMn Mn eff doping (%) Tc increases with Mneff when compensation is less than ~40%. No saturation of Tc at high Mn concentrations 6 7 (III,Mn)V materials: Microscopic picture of Mn-hole coupling in (Ga,Mn)As Mn GaAs d5 Mn As Ga Ga s-orb. L 1 Mn 0.1eV acceptor As p-orb. many Mn As 4p - Mn 3d hybridization d5 Mixed (Al,Ga)As and Ga(As,P) hosts Mn d level Ed Ed Mn d level |Vpd|2 ~ alc-7 1/|Ed| + 1/|Ed| ~ const. Hole - local moment Kondo coupling: Mean-field Curie temperature: = 50% in GaP 4% in GaP and AlAs