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091127 「グラフェン・グラファイトとそ の周辺の物理」研究会(筑波大) グラフェンにおけるスピン伝導・ 超伝導近接効果 Akinobu Kanda University of Tsukuba, Japan Collaborators U. Tsukuba H. Goto, S. Tanaka, H. Tomori, Y. Ootuka MANA, NIMS K. Tsukagoshi, H. Miyazaki Akita U. M. Hayashi Nara Women’s U. H. Yoshioka Supported by CREST project. Outline • Brief introduction to graphene • Spin transport in multilayer graphene • Cooper-pair transport in single and multilayer graphene Specialty of multilayer graphene Allotropes of graphite 3D diamond, graphite amorphous carbon (no crystalline structure) 1D carbon nanotubes 0D fullerenes (C60, C70 ...) 2D (graphene) Graphene is a material that should NOT exist! Thermodynamically unstable (Landau, Peierls, 1935, 1937) Atom displacements due to thermal fluctuation is comparable to interatomic distance at any temperature. In 2004, graphene was discovered by Geim’s group. Obtained by mechanical cleavage from bulk graphite. High crystal quality, as a metastable state From Wikipedia Electronic structure of graphene Linear dispersion at K and K’ points. E kvF Charge carriers behave as massless Dirac fermions, described by Dirac eq. Conventional metals and semiconductors have シュレディンガー方程式 parabolic dispersion relation, ruled by Schoedinger eq. parabolicな分散関係 Electrons and holes correspond to electrons and positrons, having charge conjugation symmetry in quantum electrodynamics (QED). Relativistic effects in graphene Klein paradox (propagation of relativistic particles through a barrier) O. Klein, Z. Phys 53,157 (1929); 41, 407 (1927) Geim & Kim, Scientific American, April, 2008 Relativistic Josephson effect Superconducting proximity effect Graphene as a nanoelectronics material K. S. Novoselov et al., Science 306 (2004) 666. – Electric field effect – High mobility – Band gap possible – Stable under ambient conditions – Easy to microfabricate (O2 plasma etching) – Abundance of resource Also good for spintronics Small spin-orbit interaction Small hyperfine interaction Long spin relaxation length Multilayer graphene (MLG) Thickness bilayer bulk graphite semimetal band overlap ~ 40meV single layer graphene Multilayer graphene thickness:1-10 nm (interlayer distance = 0.34 nm) Electric field effect Screening of gate electric field interlayer screening length lSC ~ 1.2 nm (3.5 layers) (Miyazaki et al., APEX 2008) Spin transport in multi-layer graphene FM/MLG/FM sample optical microscope image Cr/Au Co1 Co2 Cr/Au 4 m Scotch tape method Graphene was found in 2004 by Novoselov, Geim et al. (Manchester). Micromechanical cleavage (Scotch tape method) (Geim, Kim, Scientific American (April, 2008)) Scotch tape method Graphene was found in 2004 by Novoselov, Geim et al. (Manchester). Micromechanical cleavage (Scotch tape method) (Geim, Kim, Scientific American (April, 2008), 日経サイエンス(2008年7月)) Scotch tape method Graphene was found in 2004 by Novoselov, Geim et al. (Manchester). Micromechanical cleavage (Scotch tape method) (Geim & Kim, Scientific American (April, 2008), 日経サイエンス(2008年7月)) Repeat cleavage Scotch tape method Graphene was found in 2004 by Novoselov, Geim et al. (Manchester). Micromechanical cleavage (Scotch tape method) (Geim, Kim, Scientific American (April, 2008), 日経サイエンス(2008年7月)) Si Substrate with 300 nm of SiO2 Scotch tape method Graphene was found in 2004 by Novoselov, Geim et al. (Manchester). Micromechanical cleavage (Scotch tape method) (Geim, Kim, Scientific American (April, 2008), 日経サイエンス(2008年7月)) Under optical microscope Scotch tape method Graphene was found in 2004 by Novoselov, Geim et al. (Manchester). Micromechanical cleavage (Scotch tape method) (Geim, Kim, Scientific American (April, 2008), 日経サイエンス(2008年7月)) Optical microscope image No need for MOCVD... FM/MLG/FM sample AFM image optical microscope image Cr/Au substrate UGF SEM image I H I Co1: 200 nm L = 290 nm Co2: 330 nm Co1 Cr/Au Co2 V 4 m 1 m –+ V thickness ~ 2.5 nm (AFM) Highly doped Si substrate is used as a back gate. (4 - 5 layers) Nonlocal measurement F. J. Jedema et al. Nature 416, 713 (2002) FM/MLG/FM sample AFM image optical microscope image Cr/Au substrate UGF SEM image I H I Co1: 200 nm L = 290 nm Co2: 330 nm Co1 Cr/Au Co2 V 4 m 1 m –+ V thickness ~ 2.5 nm (AFM) Highly doped Si substrate is used as a back gate. (4 - 5 layers) Nonlocal measurement Ferro1 F. J. Jedema et al. Nature 416, 713 (2002) Ferro2 Parallel alignment of magnetization positive voltage FM/MLG/FM sample AFM image optical microscope image Cr/Au substrate UGF SEM image I H I Co1: 200 nm L = 290 nm Co2: 330 nm Co1 Cr/Au Co2 V 4 m 1 m –+ V thickness ~ 2.5 nm (AFM) Highly doped Si substrate is used as a back gate. (4 - 5 layers) Nonlocal measurement Ferro1 F. J. Jedema et al. Nature 416, 713 (2002) Ferro2 Parallel alignment of magnetization positive voltage Antiparallel alignment of magnetization negative voltage Nonlocal measurement 0.55 0.4 g R P 0.1 0.40 Rs 0 R: 4-terminal resistance of MLG -0.1 200 R -0.2 -0.3 0.45 0.35 AP -2000 -1000 0 1000 2000 H (Oe) RP ~ -RAP > 0 R () V/I () 0.2 Rs () 0.3 Rs: spin signal 0.50 V =0V 4K 150 100 50 -100 -50 0 V (V) g Rs: spin accumulation signal (spin signal) 50 100 Nonlocal measurement 0.55 0.4 g R P 0.1 0.40 Rs 0 R: 4-terminal resistance of MLG -0.1 200 R -0.2 -0.3 0.45 0.35 AP -2000 -1000 0 1000 2000 H (Oe) RP ~ -RAP > 0 R () V/I () 0.2 Rs () 0.3 Rs: spin signal 0.50 V =0V 4K 150 100 50 -100 -50 0 V (V) g Rs: spin accumulation signal (spin signal) 50 100 Nonlocal measurement 0.6 0.4 0.3 g 0.5 0.2 V <V n n P 0.4 0.1 -0.1 R -0.2 AP -2000 -1000 0 1000 2000 H (Oe) RP ~ -RAP > 0 Rs: spin accumulation signal (spin signal) s Rs 0 -0.3 g g R R () V/I () V >V V =0V 4K 0.3 0.2 Spin signal is a linearly decreasing function of resistance. 0.1 Quite different from conventional spin signals 0 0 50 100 150 200 R () 250 General expression for spin signal Takahashi and Maekawa, PRB 67, 052409 (2003) PJ Rii pF RRFF 2 R R i 1 1 PJ N 1 pF2 RN N L / lN RS 4 RN e 2 2 Ri 2 RRFF 2 L / lN 1 e 2 R 2 R R i 1 1 PJ NN 1 pF NN 2 PJ: interfacial current polarization pF: current polarization of F1 and F2 L: separation of F1 and F2 General expression for spin signals Takahashi and Maekawa, PRB 67, 052409 (2003) PJ Rii pF RRFF 2 R R i 1 1 PJ N 1 pF2 RN N L / lN RS 4 RN e 2 2 Ri 2 RRFF 2 L / lN 1 e 2 R 2 R R i 1 1 PJ NN 1 pF NN 2 Two limiting cases are well studied. Tunnel junctions R1,R2 >> RN >> RF Co/Al2O3/Al Jedema et al., Nature 416, 713 (2002). RS PJ2 RNN eL / lN General expression for spin signals Takahashi and Maekawa, PRB 67, 052409 (2003) PJ Rii pF RRFF 2 R R i 1 1 PJ N 1 pF2 RN N L / lN RS 4 RN e 2 2 Ri 2 RRFF 2 L / lN 1 e 2 R 2 R R i 1 1 PJ NN 1 pF NN 2 Two limiting cases are well studied. Tunnel junctions R1,R2 >> RN >> RF Co/Al2O3/Al Jedema et al., Nature 416, 713 (2002). RS PJ2 RNN eL / lN Transparent junctions RN >> RF >> R1,R2 Py/Cu RS Jedema et al., Nature 410, 345 (2001). 4 pF2 (1 pF2 ) 2 RF e L / lN 1 RN 2 L / lN RNN R RRNN 1 e 2 General expression for spin signal Takahashi and Maekawa, PRB 67, 052409 (2003) PJ Rii pF RRFF 2 R R i 1 1 PJ N 1 pF2 RN N L / lN RS 4 RN e 2 2 Ri 2 RRFF 2 L / lN 1 e 2 R 2 R R i 1 1 PJ NN 1 pF NN 2 Two limiting cases are well studied. Tunnel junctions R1,R2 >> RN >> RF Co/Al2O3/Al Jedema et al., Nature 416, 713 (2002). Transparent junctions RN >> RF >> R1,R2 Py/Cu Jedema et al., Nature 410, 345 (2001). Intermediate interface RN >> R1,R2 >> RF RS a bRN RS PJ2 RNN eL / lN RS 4 pF2 (1 pF2 ) 2 RF e L / lN 1 RN 2 L / lN RNN R RRNN 1 e 2 General expression for spin signal Takahashi and Maekawa, PRB 67, 052409 (2003) PJ Rii pF RRFF 2 R R i 1 1 PJ N 1 pF2 RN N L / lN RS 4 RN e 2 2 Ri 2 RRFF 2 L / lN 1 e 2 R 2 R R i 1 1 PJ NN 1 pF NN Linearly decreasing asymptotic form R1R2 2 P 2 R1R2 2 2 P R RsRs (1) 2 2 R 1 P R1 R2 ( R1 R2 ) 2 only under the following condition, ( R1 R2 ) RN 2 R1 R2 R R . N 1 P2 (1 P 2 )2 (2) From the fitting and condition (2), Interface resistance: R1+R2 = 540 (c.f. 490 from independent estimation) Current polarization: PJ = 0.047 (c.f. PJ ~ 0.1 in Co/graphene[*]) Fitting parameters take reasonable values, justifying the fit to eq. (1). [*] Tombros et al. Nature 448, 571 (2007). General expression for spin signal Takahashi and Maekawa, PRB 67, 052409 (2003) PJ Rii pF RRFF 2 R R i 1 1 PJ N 1 pF2 RN N L / lN RS 4 RN e 2 2 Ri 2 RRFF 2 L / lN 1 e 2 R 2 R R i 1 1 PJ NN 1 pF NN Linearly decreasing asymptotic form R1R2 2 P 2 R1R2 2 2 P R RsRs (1) 2 2 R 1 P R1 R2 ( R1 R2 ) 2 only under the following condition, ( R1 R2 ) RN 2 R1 R2 R R . N 1 P2 (1 P 2 )2 (2) From the fitting and condition (2), Interface resistance: R1+R2 = 540 (c.f. 490 from independent estimation) Current polarization: PJ = 0.047 (c.f. PJ ~ 0.1 in Co/graphene[*]) Spin relaxation length: lN >> 8 m Longer than lN of SLG, Al, and Cu. RN >> R1,R2 >> RF Intermediate interface Long spin relaxation length in MLG graphite 1. Nearly perfect crystal free of structural defects 2. Origins of scattering MLG SLG on SiO2 charged impurities J. H. Chen et al. Nature Nanotech. (2008) Long spin relaxation length in MLG graphite 1. Nearly perfect crystal free of structural defects 2. Origins of scattering contaminant MLG (multilayer) graphene lSC SLG on SiO2 charged impurities adsorbed molecules modulation of carrier density charge impurities, phonon SiO2 layer J. H. Chen et al. Nature Nanotech. (2008) Smaller scattering Longer spin relaxation length lSC: interlayer screening length lSC ~ 1.2 nm (3.5 layers) (Miyazaki et al., APEX 2008) Distance from contaminant and c.f. lN = 1.5 - 2 m in SLG adsorbed molecules becomes larger. Tombros et al. Nature 448, 571 (2007). Ripple becomes smaller. Contact resistance in thick MLG devices c1 c2 c3 c4 Ni c1 (L = 180 nm) c2 (L = 290 nm) c3 (L = 380 nm) c4 (L = 490 nm) thickness: 5 nm lSC C4 C1 contact resistance Contact resistance in thick MLG devices c1 c2 c3 c4 Ni c1 (L = 180 nm) c2 (L = 290 nm) c3 (L = 380 nm) c4 (L = 490 nm) thickness: 5 nm lSC C4 C1 contact resistance Contact resistance in thick MLG devices c1 c2 c3 c4 Ni c1 (L = 180 nm) c2 (L = 290 nm) c3 (L = 380 nm) c4 (L = 490 nm) thickness: 5 nm lSC C4 C1 contact resistance Contact resistance in thick MLG devices c1 c2 c3 c4 Ni c1 (L = 180 nm) c2 (L = 290 nm) c3 (L = 380 nm) c4 (L = 490 nm) thickness: 5 nm lSC Gate-controllable intrinsic contact C4 resistance in thick C1 MLG Layered structure Screening of gate electric field contact resistance Contact resistance in thick MLG devices c1 c2 c3 c4 Ni lSC Gate-controllable intrinsic contact resistance in thick MLG Layered structure Screening of gate electric field Contact resistance in thick MLG devices c1 c2 c3 c4 lSC Gate-controllable intrinsic contact resistance in thick MLG Layered structure Screening of gate electric field Ni R1,2 contact Rc intrinsic Rc (Vg ) Rccontact can be reduced. Contact resistance in thick MLG devices c1 c2 c3 c4 Ni c1 (L = 180 nm) c2 (L = 290 nm) c3 (L = 380 nm) c4 (L = 490 nm) Rccontact thickness: 5 nm C4 Rcintrinsic (Vg ) Rgraphene(Vg ) C1 contact resistance slope: graphene resistance If one can sufficiently reduce Rccontact, Ri const. RN Contact resistance and spin signal Takahashi and Maekawa, PRB 67, 052409 (2003) PJ Rii pF RRFF 2 R R i 1 1 PJ N 1 pF2 RN N L / lN RS 4 RN e 2 2 Ri 2 RRFF 2 L / lN 1 e 2 R 2 R R i 1 1 PJ NN 1 pF NN 2 Tunnel junctions R1,R2 >> RN >> RF L / lN RS PJ2 RN RN Ne Transparent junctions (Rccontact) with MLG, Transparent junctions RN >> RF >> R1,R2 RF e L / lN 1 RS R N N 2 L / lN RNN R (1 pF2 ) 2 RRNN 1 e 4 pF2 2 (RF ~ 1m) Ri const. RN RS RN Sample for local measurement I + _V Thickness: 9 nm Spin valve effect parallel – small R R MLG antiparallel – large R H 46.50 V =0V g 46.49 46.48 -1500-1000 -500 0 500 1000 1500 Magnetic field (Oe) Gate voltage dependence 4K 46.50 V =0V g 46.48 V = 80 V g 37.72 37.71 V = -80 V 29.86 1200 Oe 0 Oe 46.49 37.73 spin induced magnetoresistance (SIMR) g 29.85 29.84 -1500-1000 -500 0 500 1000 1500 Magnetic Field (Oe) R ( H ) R ( H )dH Gate voltage dependence 4K 46.50 V =0V g spin induced magnetoresistance (SIMR) 1200 Oe 0 Oe 46.49 R ( H ) R ( H )dH 46.48 37.73 V = 80 V g 37.72 37.71 V = -80 V 29.86 g 29.85 29.84 -1500-1000 -500 0 500 1000 1500 Magnetic Field (Oe) Might indicate Rs proportional to RN? Contact resistance and spin signal Takahashi and Maekawa, PRB 67, 052409 (2003) PJ Rii pF RRFF 2 R R i 1 1 PJ N 1 pF2 RN N L / lN RS 4 RN e 2 2 Ri 2 RRFF 2 L / lN 1 e 2 R 2 R R i 1 1 PJ NN 1 pF NN 2 Tunnel junctions R1,R2 >> RN >> RF L / lN RS PJ2 RN RN Ne Transparent junctions (Rccontact) with MLG, Transparent junctions RN >> RF >> R1,R2 RF e L / lN 1 RS R N N 2 L / lN RNN R (1 pF2 ) 2 RRNN 1 e 4 pF2 2 (RF ~ 1m) Ri const. RN RS RN Gate controllable Cooper pair transport in single and multi-layer graphene Why Cooper-pairs in graphene? Single layer graphene (SLG) relativity superconductivity Injection of Cooper-pairs by proximity effect Andreev reflection Intraband A. R. Interband A. R. Beenakker, Rev. Mod. Phys. 80, 1337 (2008). Why Cooper-pairs in graphene? Multilayer graphene (MLG) semimetal Usual proximity effect Large gate electric field effect (-1012cm-2 < n < 10-12cm-2) Never obtained in other SNS systems S/graphene/S junctions superconductor superconductor graphene Mechanical exfoliation of kish graphite followed by e-beam lithography and metal deposition. Electrode: Pd(5 nm)/Al(100 nm) or Ti(5 nm)/Al(100 nm)/Ti(5 nm) Gap of electrodes d ≈ 0.2 - 0.6 m Doped Si is used as a back gate. graphene Josephson effect in SLG Gate voltage dependence gap: d = 0.22 m IV characteristics 0.2 V (mV) 0.1 T=200mK, B B=0.00mT =0 Vg -75V -50V -25V 8V Magnetic field dependence 0.0 -0.1 -0.2 -3000 -2000 -1000 sweep 0 I (nA) 1000 2000 3000 Temperature dependence of critical supercurrent Vg = -75 V -50V 75V 50V -25V 25V 0V 8V gap: d = 0.22 m Conventional theory for Ic(T) Long junctions (d >> xN) Ic exp(d / x N ) exp((T / T0 ) ) 0.5 1 Clean limit: l x N Dirty limit: l x N Conventional theory for Ic(T) Long junctions (d >> xN) Ic exp(d / x N ) exp((T / T0 ) ) Clean limit: l x N Dirty limit: l x N 0.5 1 (l: mean free path) Short junctions (d << xN) Two kinds of Kulik-Omel’yanchuk theory ballistic, ideal interface diffusive, ideal interface Conventional theory for Ic(T) Long junctions (d >> xN) Ic exp(d / x N ) exp((T / T0 ) ) Clean limit: l x N 0.5 1 Dirty limit: l x N Short junctions (d << xN) Two kinds of Kulik-Omel’yanchuk theory ballistic, ideal interface diffusive, ideal interface Ambegaokar-Baratoff result Temperature dependence of critical supercurrent Vg = -75 V -50V 75V 50V -25V 25V 0V 8V gap: L = 0.22 m Temperature dependence of critical supercurrent Vg = -75 V -50V 75V KO1 theory (short junction dirty limit: l << d << xN) 50V -25V 25V 0V 8V I. O. Kulick and A. N. Omel'yanchuk, JETP Lett. 21, 96 (1975). Temperature dependence of critical supercurrent Injection of Cooper pairs into graphene Vg = -75 V 75V Ic KO1 theory (short junction dirty limit: l << d << xN) Ic(T=0) 1500 Ic(T=0) (nA) -50V 2000 1000 500 0 -75 -50 -25 0 25 50 75 Vg (V) 50V -25V 1.0 Tc 0.8 Tc (K) 0.6 0.4 0.2 25V 0V 8V 0.0 -75 Tc -50 -25 Never seen in other SNS systems 0 25 50 75 Vg (V) Ballistic junction is needed for relativistic Josephson effect! I. O. Kulick and A. N. Omel'yanchuk, JETP Lett. 21, 96 (1975). Making ballistic junctions mean free path shorter junctions Angle deposition of metals 300 Resist mask 250 mfp (nm) 200 graphene 150 Substrate 100 50 0 -60 l 50 nm -40 -20 0 20 Vgate(V) 40 60 h 2e 2 k F cleaner graphene kF Vg Vn 7.2 1014 m 2 V 1 K.I. Bolotin et al., SSC 146, 351 (2008) Multilayer graphene Temperature dependence of resistance (Inset: Vg dependence of normal-state resistance) Tc of Pd/Al Current-voltage (I-V) characteristics hole supercurrent 0.2 K electron supercurrent Vgp Ic supercurrent dV/dI at 0.06 K Critical supercurrent Ic depends on the gate voltage. Ambipolar behavior was observed. I-V curves do not show hysteresis due to small Rn, in clear contrast to the single layer graphene Josephson junctions. Electron and hole supercurrents Relation between Ic and Rn Electron and hole supercurrents Temperature dependence of resistance (Inset: Vg dependence of normal-state resistance) Tc of Pd/Al Asymmetry in electron and hole supercurrents Temperature dependence of Ic Vg=75V 60V 45V d 2 Ic dT 2 0 Ic exp((T / T0 ) 2 ) Conventional theory for Ic(T) Long junctions (d >> xN) Clean limit: l x N Ic exp(d / x N ) Dirty limit: l x N exp((T / T0 ) ) 0.5 1 Short junctions (d << xN) (l: mean free path) In our measurement, = 2. Two kinds of Kulik-Omel’yanchuk theory measurement ballistic, ideal interface diffusive, ideal interface Ambegaokar-Baratoff result d 2 Ic dT 2 0 d 2 Ic dT 2 0 Possible origin of exp(T/T0)2 behavior MLG lSC ~ 3.5 layers SiO2 (300 nm) Si (Back gate) In thick MLG, when large Vg is applied, the carriers at the bottom of the MLG increases due to the screening of the gate electric field. Assumption: The number of superconducting layers increases with decreasing temperature. Model for Ic(T) of multilayer graphene Assumptions Regard each layer as independent single-layer graphene with different carrier density. Model for Ic(T) of multilayer graphene Assumptions Regard each layer as independent single-layer graphene with different carrier density. Critical supercurrent of each layer follows the KO1 theory. (Note that the results are almost the same for Ambegaoker-Baratoff or KO2 theory.) Model for Ic(T) of multilayer graphene Assumptions Regard each layer as independent single-layer graphene with different carrier density. Critical supercurrent of each layer follows the KO1 theory. (Note that the results are almost the same for Ambegaoker-Baratoff or KO2 theory.) The onset temperature TC(n), and zero-temperature critical supercurrent IC0(n) of n-th layer becomes infinitesimally small when the carrier density of the layer is small enough: For example I C 0 (n), TC (n) N gate (n) Ngate: gate-induced carrier density Numerical result A, B, C... : Onset of supercurrent in 1st, 2nd, 3rd... layers Ic exp((T / T0 ) 2 ) is reproduced in a wide temperature range. Message • Multilayer graphene is also an attractive material! Screening of gate electric field leads to – Large spin relaxation length – gate-dependent contact resistance Good for spintronics – Large modulation of supercurrent Good for superconducting transistors