J 12 J 23 J 34. Driving forces in the nano-magnetism world. Intra-atomic exchange, electron correlation effects: Inter-atomic exchange: MAGNETIC ORDER
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1 Driving forces in the nano-magnetism world Intra-atomic exchange, electron correlation effects: LOCAL (ATOMIC) MAGNETIC MOMENTS m d or f electrons Inter-atomic exchange: MAGNETIC ORDER H exc J S S i j ij i j J 1 J 3 J 34 Hund s rules Spin-Orbit Coupling: MAGNETOCRYSTALLINE ANISOTROPY: K Dipolar Interaction: SHAPE ANISOTROPY r m m 1 H s.o. LS s i l i H dip m 1 m ( m1 )( ) 3 r m r 3 5 r r
2 The He atom: intra-atomic exchange H p 1 Ze 1 e H i He H 0 i1 m 4 0 i1 ri 4 0 r r1 ee r r 1 He atom Ground state -> the two electrons occupy the 1s orbital -> the spatial part of the wavefunction is symmetric (electrons have identical quantum numbers nlm=100) -> the spin part must be antisymmetric (electrons are fermions) 1 ground sym (r 1,r ) antisym (s 1,s ) [ 100 (r 1 ) 100 (r ) 100 (r 1) 100 (r )][ ] From the previous Hamiltonian we can calculate the energy of the ground state. Because H He does not contain spin terms, the spin part of the wavefunction only needs to satisfy the antisymmetric condition Excited state -> one electron occupies the 1s orbital (nlm=100); the second electron is in an excited state nlm 1) the spatial part of the wavefunction is symmetric and the spin part is antisymmetric S sym (r 1,r ) antisym (s 1,s ) [ 100 (r 1 ) nlm (r ) nlm (r 1) 100 (r )][ ] Singlet S=0 exci 1 ) the spatial part of the wavefunction is antisymmetric and the spin part is symmetric T 1 exci antisym (r 1,r ) sym (s 1,s ) [ 100 (r 1) nlm (r ) nlm (r 1) 100 (r )] sym (s 1,s ) ; sym (s 1,s ) ; ; ( ) Triplet S=1
3 The exchange interaction The singlet and triplet wavefunctions applied to H 0 give the same energy; the H e-e contribution can be calculated with the perturbation theory e I (r ) (r ) dr dr nlm r1 r e J (r ) (r ) (r ) (r )dr dr * * nlm 100 nlm 4 0 r1 r 1 1 E I J S ee E I J I is the Coulomb integral -> electrostatic repulsion between the electrons ((r) -> r electron density) J is the exchange integral -> energy associated with a change of quantum states between the electrons T ee Origin of Exchange interaction: -> Coulomb repulsion between electrons -> total anti-symmetric wave function (Pauli exclusion principle) J is positive -> triplet ground state S=1 -> parallel spins J is negative -> singlet ground state S=0 -> antiparallel spins Note: we get the exchange energy from an Hamiltonian not including spin terms!!!!!
4 The H molecule: inter-atomic exchange r 1 r R Atom1 Atom Atom1 Atom
5 The H molecule
6 Inter-atomic exchange
7 The H molecule Ground state depends on the relative strength of J 1 (always > 0) in respect to -4l (I 1 +I +K 1 ) J 1 > 4l (I 1 +I +K 1 ) -> ground state is magnetic (triplet) J 1 < 4l (I 1 +I +K 1 ) -> ground state is non magnetic (singlet) Ex: H molecule J 1 < 0 -> singlet ground state The molecule magnetic ground state depends on the interaction between electrons belonging to two different atoms
8 The Heisenberg Hamiltonian The Heisenberg Hamiltonian is an effective Hamiltonian extending to larger atoms the electronelectron interaction seen in the He atom H H H H Heisenberg 0 Coulomb exchange H J s s ; N exchange ij i j i j e J (r ) (r ) (r ) (r )dr dr 4 r r * * ij i i j j i j j i i j 0 i j a) The Heisenberg Hamiltonian is used to describe: -> coupling of individual spins located on the same atom (intra-atomic exchange) -> coupling of atomic spin moments on different atoms (inter-atomic exchange) BUT Intra-atomic (a,c) and inter-atomic (b) exchange have different energies b) a),c) -> intra-atomic V e-e in the isolated atom (Hund s rules) or Stoner band approach [Stö06] c)
9 Magnetic coupling between atoms: inter-atomic exchange Generalization to N-atoms system: Coulomb interaction + Pauli s principle The spins of the electrons are correlated i.e., there is a magnetic splitting in the energy spectrum of electrons in systems of atoms with open el. shells, true for systems of any size, doesn t tell what type of magnetic coupling The energy spectrum is represented by a model system of pairwise interacting spins H J S S i j ij i j correct to nd order in the overlap orbitals, cannot be proven rigorously Heisenberg model There are many possible exchange-interaction Hamiltonians H J z S S J S S S S z z x x y y i j i j i j ij ij Anisotropic Heisenberg model and XY model (J z =0) H J z i j SS z i z j Ising model
10 Magnetic coupling between atoms: FM and AFM coupling H S S J J ij i j i j J 0 0 ferromagnetic coupling antiferromagnetic coupling (10-50 mev in Fe, Co, Ni) ( mev in Mn, Cr; 0 mev in NiO superexchange) J < 0, depending on formula unit, system dimensions, topology: fully compensated AFM ferrimagnetism (uncompensated AFM) frustrated AFM Cr(100) surface
11 Exchange energy All spins in the grain must be ferromagnetically aligned exchange energy J coupling spins H exc J S S i j ij i j H exc << kt Coupling is destroyed and the net magnetic moment is zero Domain formation -> magnetic moment is strongly reduced S i is the atomic spin Gain in the magnetostatic energy at the expenses of the exchange energy
12 Weiss-Heisenberg model Which is the origin of the aligned atomic spin moments in a ferromagnetic domain (spontaneous magnetization)? Weiss -> molecular field H W (or mean field theory) of unknown origin Heisenberg -> molecular field originating from the interaction of the atomic spin moment with the spin sea of all the other atoms Ei sijijs j mih W; HW Jijs j g j B j Example: single spin s=1/ Two energy levels: +/- B H with an occupation probability given by exp(+/- B H/kT) x x e e BH M(H,T) M M Ng B( ) N x x x x Btanh(x); x e e e e k T B Sea of spin s=1/ x B(H M(T)) kt B M(T) -> molecular field Curie temperature: temperature at which the spontaneous magnetization (H=0) goes to zero M(T) ->0 when tanh(x) -> 0 when x-> 0 i.e. tanh(x) = x ( M(T )) N M(0) M(T ) N x N T B c B c B B C B kbtc kb kb The magnetization goes to zero when the thermal energy (k B T C ) equals the energy of a single spin in the molecular field (gs B H W = gs B M0
13 Curie and Neel temperatures For a general spin value s and moment m=-g B s s J T ; J J NJ 0 C 0 ij 01 3kB j H W s J 3 m 0 Neel temperature: is the equivalent to the Curie temperature for an antiferromagnet A few Neel temperatures NiO T N = 55 K CoO T N = 90 K FeO T N = 98 K oxigen metal
14 Curie temperature size dependence T C depends on the atomic coordination s J T ; J J NJ 0 C 0 ij 01 3kB j S. Bornemann et al. Phase Transitions 78, 701 (005) J ij as a function of distance T c nanostructures < T c bulk The number of magnetic neighbours (N) is reduced in a thin film interface: N i bulk-like: N b t layers N zb interface: N i b i t = t b + t i t N t N N N b b i i b i t t t 1/t dependence
15 Curie temperature size dependence Phys. Rev. B 1, 35 (1970) T ( ) T ( t) t, =1 C C Experiments and finite-size scaling model: TC( ) T ( t) t T ( ) C C t0 C. Domb, J. Phys. A 1, 196 (1973); Y. Li et al. Phys. Rev. Lett. 68, 108 (199); etc. ' ', 11.6 This model accounts for the decrease of T C with t down to a critical thickness t 0 4 monolayers. t is a continuous parameter -> in the ultra thin limit t becomes discrete (number of atomic layers) Ultra thin limit: linear decrease TC( ) TC( t) T ( ) R. Zhang et al. Phys. Rev. Lett. 86, 665 (001) C A ( n 1) / N 0 N o is the spin-spin coupling range (typically a few atomic sites) A takes into account the observation that for n=1 ferromagnetism can exist
16 Curie temperature and band structure Paramagnet the magnetic moments are randomly oriented due to thermal fluctuations T>T C T<T C Ferromagnet unlike the moments in a paramagnet, these moments will remain parallel even when a magnetic field is not applied Antiferromagnet Adjacent magnetic moments from the magnetic ions align antiparallel to each other without an applied field. T>T C T<T C Spin resolved inverse photoemission spectroscopy for 3d bands as a function of temperature for Ni(110) T=T C -> spin transition from minority and majority states are equal -> D=0 [Stö06] E - E F
17 Where exchange energy gets in play Curie (Neel temperature) -> magnetic order in a ferromagnetic (antiferromagnetic) nanostructure Super-exchange -> mediated interaction between magnetic atoms Bias exchange -> interaction at the interface of FM AFM structures Kondo effect -> interaction between a magnetic impurity and the conduction band electrons RKKY interaction -> interaction between magnetic impurities mediated by the conduction band electrons
18 Super-exchange oxigen metal in many materials (oxides), magnetic atoms are separated by non-magnetic ions (oxygen) (ex: MnO) Indirect interactions through oxygen atoms In the antiferromagnetic configuration, electrons of atoms A and B can both hybridize with 1 p-electron of Oxygen energy depends on the relative spin orientation
19 Kondo effect impurity S J S s << k B T K Screening S - s host J s 1/ J S s >> k B T K Non screening S The Kondo interaction J S s couples itinerant electrons of the host with spin s 1/ to a magnetic impurity with spin S. For exchange interaction J < 0, antiferromagnetic (AFM) coupling of the spins of the conduction electrons screens the impurity spin. The ground state at temperatures T below the Kondo temperature T K is a spin S - s (red area). For J > 0, the ferromagnetic (FM) coupling tends to create a cloud of spins aligned parallel to the impurity spin, which becomes asymptotically free at low temperatures. For S = ½ complete screening For S > 1 under-screening Kondo NATURE COMMUNICATIONS 4:110 DOI: /ncomms3110
20 RKKY interaction Indirect exchange couples moments (in impurities or magnetic layers) over relatively large distances Impurity 1 (layer 1) Impurity (layer ) FM coupling J(r) = J 0 cos( k F r)/( k F r) D D represent the system dimensionality F = /k F Fermi wave length (in metal is of the order of a few nm) AFM coupling
21 Co/Pt(111): RKKY interaction J(r) = J 0 cos( k F r)/( k F r) F = /k F 3 nm F. Meier, et al., Science, 8, 30 (008)
22 Read for exercise
23 Bias exchange a) In an external field and above the Néel temperature T N, antiferromagnetic spins located at the interface with the ferromagnet are aligned, like the ferromagnet, with the external field. b) Once cooled below T N, these interface spins keep their orientation and appear "pinned" because they are tightly locked to the spin lattice in the bulk of the antiferromagnet, which is not sensitive to external fields. Consequently these pinned spins produce a constant magnetic field at the interface that causes the hysteresis loop of the ferromagnet to shift. H c c) This intuitive picture overestimates the magnitude of the loop shift by orders of magnitude. H b / H c W / ev / 50 mev 30 When T < T N you need several tens of tesla to reverse the AFM coupled spins ( pinning ) H c H b J. Nogués et al., J. Magn. Magn. Mater. 19, 03 (1999)
24 Bias exchange: real case only a small fraction (5%) of interfacial spins is actually pinned, and these cause the horizontal hysteresis loop shifts. H. Ohldag et al., Phys. Rev. Lett. 91, (003)
25 Exchange braking layer: Magnetic recording technology The exchange break layer is need to decouple the recording layer from the soft underlayer (necessary to close the magnetic flux lines)
26 Exchange braking layer: oxide phase for grain decoupling R. Araki, et al. IEEE Trans. Magn. 44, 3496 (008). D. E. Laughlin, et al. J. Appl. Phys. 105, 07B739 (009). The inter-grain exchange interaction is stopped by the oxide layer
27 GMR: giant magneto resistance DR/R(%) Pinned FM NM spacer (metallic or insulating ) Free FM Electric current DR / R R R R
28 Science 8, 1660 (1998); Nat. mater. 6, 813 (007) GMR: why is working Available states with the same spin: Low resistance 1 0 Absence of states with the same spin: High resistance
29 Pinned layer: bias exchange M (arb. un.) DR/R (%) Electric current H E Pinned layer Free layer J. Appl. Phys. 69, 4774 (1991) AFM Pinned FM Free FM
30 Role of the NM spacer: decoupling the two FM layers The atom spins are coupled together In non magnetic materials H ex = J S i S j = 0 Inter-atomic exchange: MAGNETIC ORDER H exc J S S i j ij i j J 1 J 3 J 34 Domain wall between two pinned ferromagnetic materials with opposite orientation of the magnetization Without the spacer two (negative) scenarios depending on the strength of the exchange force in respect to the pinning force: a) The free layer magnetization always aligns parallel to the magnetization of the pinned layer b) A domain wall forms which produces the spin current depolarization J. Appl. Phys. 69, 4774 (1991)
31 GMR applications: MRAM Magnetic random access memory (MRAM) Ferromagnetic (FM) - nonmagnetic (NM) - ferromagnetic (FM) junction Science 8, 1660 (1998); Nat. mater. 6, 813 (007)
32 GMR applications: reading head Reading-writing head in HDD Reading: the bit stray field defines the magnetization direction of the free layer
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