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1990-2010. Magnetismo
       cuántico
   Javier Tejada Palacios
Qué es el magnetismo?


• Interacción electrostática+ Mecánica Cuántica
                         2
                     e
                                     Solapamiento de
                     r12             las funciones de
                                     onda
               2
           e
                   es diferente     S    0 and S   1
           r12     para
                                                       Heisenberg
                         s i s j Hamiltoniano          Hamiltoniano
Interacción de intercambio
• Interacción en función de operadores de espín


                       Solapamiento de f.o. decae
                       exponencialmente




                                     Suma se hace sobre
                                     los primeros vecinos
                  J ~ TC
Anisotropía Magnética
• Origen relativista                   p
                                   v
   – Orden de magnitud                     , siendo p par.
                                   c
• Clásicamente:
   – Altura de la barrera de energía:
          U         kV
              Constante de   volumen
              anisotropía

• Cuánticamente:

        Eje fácil        Eje difícil
Del sólido magnético a la partícula
          monodominio
• Dominios y paredes de dominio           E ex
                                                  a
                                          EA
                                           E ex        3        5
                                                  10       10
                                           EA
                                          nm
• Si tamaño partícula R<λ:
  – No hay paredes de dominio
  – Partícula monodominio!
  – Probabilidad de invertir un espín
                 E ex
      exp                     0 Para T (<< TC): S=cte
                  T
¿Realidad de SDP?
• Distribución de tamaños y de orientaciones:
                  f R      f V       f U




   • Sus momentos magnéticos se alinean con el campo
     magnético externo
   • Si anulamos el campo, los momentos magnéticos
    tienden a recuperar su orientación inicial y eso hace
       que el valor de la magnetización que medimos
         decrezca logarítmicamente con el tiempo:
Dependencia de la viscosidad con
        la temperatura
• Partículas relajan hacia su estado de equlibrio:
             M       M0 1            S ln t
                        Viscosidad
                        magnética

• Comportamiento clásico               S      T
   – A temperaturas elevadas es más fácil saltar la barrera
• Cuánticamente (independent of T)
   – Relajación debida al efecto túnel
Blocking temperature
• Flipping between ↓ and ↑ states occurs in a
  certain characteristic time that depends on
  temperature:
                                   U
                tf       t 0 exp
                                   k BT
                                          T > TB
• Below the blocking temperature TB the magnetic
                 T<T B

  moment cannot flip above the barrier
• Above the blocking temperature the magnetic
  moment can flip, following a Curie law:
             SUPERPARAMAGNETIC state
Moleculas magnéticas
• Identicas a SDP
• Objetos cuánticos




• M(H,T) univocally determined by D and E
Magnetization curve
• Application of an external field: Zeeman Term
                          H S
  – Longitudinal field (H || easy axis)
     • Moves levels
  – Transverse field (H     easy axis)
     • Allows tunneling
• Tunneling is possible at resonant fields
Spin resonant tunnel effect



                  -2-1 0 1 2
                -3           3
              -4               4
            -5                   5
          -6                       6
        -7                           7
       -8                                8
  -9                                         9

 -10                                         10
                                                  Magnetic field
  B=0
Spin resonant tunnel effect



                   -1 0 1
               -3-2       2
                            3
             -4               4
           -5
                                5
         -6
                                  6
       -7
                                      7
   -8
                                          8
  -9
                                              9
 -10
                                              10   Magnetic field
B = 0.5B0
Spin resonant tunnel effect



                -3-2   12
              -4            3
            -5                  4
          -6                        5
        -7                              6
    -8                                      7
   -9                                           8
  -10                                               9
   B = B0                                           10
                                                         Magnetic field
Spin resonant tunnel effect



             -3-2-10 1
           -4          2
         -5              3
       -6                  4
     -7                      5
    -8                         6
   -9                              7
  -10                                  8

                                           9
 B = 2B0                                        Magnetic field
                                           10
Relaxation in Molecular Magnets
• After a certain time, relaxation goes
  exponential

      M t      M   eq
                        t 1   exp     H t

• Peaks of the relaxation rate Γ(H) at
  resonances
A.C. measurements
• TB depends on measuring frequency
                        K V0
             TB
                    ln 1 /     0
New trends in magnetism
• Magnetic deflagration
• Superradiance
• Rotational Doppler Shift
Magnetic Deflagration
                            Deflagration is a technical term describing subsonic combustion that
                            usually propagates through thermal conductivity
            Energy Barrier
                                  •   There are two characteristic timescales which are
AF                                    important here. The first is the thermal diffusion
                                      timescale is approximately equal to



                         FM       •   The second is the burning timescale that strongly
                                      decreases with temperature, typically as
       Energy released

      Thermal diffusion

            Ignition
     (barrier overcoming)
From Magnetisation jumps to magnetic
                            deflagration.
                                                                                    Manganites
                                                                                    Field jumps 1999
                                                                                    Deflagration-like description 2007
                                                                                                              T=3K
                                                                                                    1.0

  Molecule magnets
  Field jumps 1999




                                                                                                S
                                                                                              M/M
                                                                                                    0.5

  Deflagration-like description 2005

                                                                                                    0.0
                                                                                                          0           10              20   30
                T = 1.8 K                                                                                                       H (kOe)
       1.0


       0.5                                                 Intermetallic compounds
                                                           Field jumps 2002
M/Ms




       0.0
                                                           Deflagration-like description 2009
       -0.5
                                                                      1.0
       -1.0
                                                                      0.8

          -30     -20       -10      0      10   20   30              0.6
                                  H (kOe)
                                                               M/MS




                                                                      0.4

                                                                      0.2

                                                                      0.0

                                                                            0   5   10   15     20        25   30    35    40    45   50
                                                                                                    H (kOe)
Molecule Magnets
                                                          H

                                                                              ΔE
                                                            Magnetic deflagration:
                                                   Propagation of a front of reversing spins
                                                     at constant velocity along the crystal


A. Hernández-Mínguez et. al. PRL 95 17205 (2005)




                                                       Problem: Sweeping H we cannot
                                                       control the magnetic field at
                                                       which it occurs.

 Y. Suzuki et. al. PRL 95, 147201 (2005)
Igniting avalanches with SAW
Surface acoustic waves (SAWs) are low frequency acoustic phonons (below 1 GHz)


The coaxial cable is connected to an Agilent microwave signal generator.

The change of the magnetic moment is registered by a rf-SQUID magnetometer.


                                                Hz
     coaxial cable
                                    IDT     Mn12 crystal
                                                    c-axis




                     conducting                          LiNbO3
                     stripes                             substrate
Quantum magnetic deflagration in nanomagnets




                                                                   κ          U(H)
                                                           v           exp
                                                                  τ0         2k B T f

                                                           This velocity is well fitted:
                                                                κ = 0.8·10-5 m2/s
• The speed of the avalanche                                Tf (H = 4600 Oe) = 6.8 K
                                                           Tf (H = 9200 Oe) = 10.9 K
increases with the applied
magnetic field.

• At resonant fields the       •   The ignition time shows peaks at the
velocity of the flame front        magnetic fields at which spin levels
presents peaks.                    become resonant.
Associated to the deflagration...
• Superradiance emission (?)
  – All spins decay to the fundamental level
    coherently, with the emission of photons.

                           -3-2-10 1
                         -4          2
                       -5              3
                     -6                  4
                   -7                      5
                 -8                          6
                -9                             7
               -10                                 8
                                                       9
             B = 2B0
                                                       10
Linear Doppler
Shift on frequency due to relative velocity between
emitter and observer (non relativistic case): Relative
                                                      velocity
                             v
                         1
  Frequency                  c
  seen by the
  observer                             Frequency of
                                       the emitter




                             v
                             c
Rotational Doppler
Shift on frequency due to relative rotation between
emitter and observer (circularly polarized light):
                                         Relative rotation

  Frequency
  seen by the                        Frequency of
  observer                           the emitter
Rotational Doppler Effect
EPR results
EPR results
Rotational Doppler Effect
                                           2       B


FMR        0
                    H                          
                                                   n
                                                       I

                                   n
            Hn                 0
                                       I
                                                   2
                                              
      H        Hn   1
                        Hn   
                                   I       2       B
                                                       I

          measured           H ~ 2 . 5 Oe
      produced by r ~ 1nm particles
Rotational Doppler Effect
          Occupied states
          L L     1
     En                n n       1   B
                                             H
             2I
                  2     En
                 n ~
                       B
                             H
                                                     1/ 2
                                         k BT
    E n ~ k BT               n~
                                         B
                                                 H
    T ~ 2K
                                         n       100
B
    H ~ 0 . 17 mK
Rotational Doppler Effect
• Change in frequency observed due to rotation:


• RDE in GPS systems (resonance of an LC
  circuit)
   – Resonant frequency insensitive to magnetic fields
                Resonance

• RDE in Magnetic Resonance systems
   – Resonant frequency sensitive to magnetic fields
                 Resonance
Rotational Doppler Effect
• Article by S. Lendínez, E. M. Chudnovsy, and J.
  Tejada:
      arXiv:1008.2142v1 [cond-mat.other]

• Expression for ω’Res are found for ESR, NMR and
  FMR.
              Resonance

         • Exact expression depends on type of resonance
         (ESR, NMR or FMR)
         • Depends on anisotropy
Rotational Doppler Effect
• Ω ≈ 100 kHz
• ESR and FMR: • ωRes ≈ GHz       Ω << ωRes << Δω
               • Δω ≈ MHz
                                             BUT
                                Position of maximum can be
            With free rotors:   determined with accuracy of
                                100 kHz ≈ Ω
          • ω Ω≈ 100 Ω ≈ Δω
              ≈ MHz  MHz
• NMR:      Res
          • Δω ≈ kHz                          Gyromagnetic
                                   ESR and    tensor
• κ ≠ 1 needed     anisotropy      FMR:       (shape,...)

                                   NMR:      Hyperfine
                                             interactions

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1990-2010 - Magnetismo Cuántico

  • 1. 1990-2010. Magnetismo cuántico Javier Tejada Palacios
  • 2. Qué es el magnetismo? • Interacción electrostática+ Mecánica Cuántica 2 e Solapamiento de r12 las funciones de onda 2 e es diferente S 0 and S 1 r12 para Heisenberg s i s j Hamiltoniano Hamiltoniano
  • 3. Interacción de intercambio • Interacción en función de operadores de espín Solapamiento de f.o. decae exponencialmente Suma se hace sobre los primeros vecinos J ~ TC
  • 4. Anisotropía Magnética • Origen relativista p v – Orden de magnitud , siendo p par. c • Clásicamente: – Altura de la barrera de energía: U kV Constante de volumen anisotropía • Cuánticamente: Eje fácil Eje difícil
  • 5. Del sólido magnético a la partícula monodominio • Dominios y paredes de dominio E ex a EA E ex 3 5 10 10 EA nm • Si tamaño partícula R<λ: – No hay paredes de dominio – Partícula monodominio! – Probabilidad de invertir un espín E ex exp 0 Para T (<< TC): S=cte T
  • 6. ¿Realidad de SDP? • Distribución de tamaños y de orientaciones: f R f V f U • Sus momentos magnéticos se alinean con el campo magnético externo • Si anulamos el campo, los momentos magnéticos tienden a recuperar su orientación inicial y eso hace que el valor de la magnetización que medimos decrezca logarítmicamente con el tiempo:
  • 7. Dependencia de la viscosidad con la temperatura • Partículas relajan hacia su estado de equlibrio: M M0 1 S ln t Viscosidad magnética • Comportamiento clásico S T – A temperaturas elevadas es más fácil saltar la barrera • Cuánticamente (independent of T) – Relajación debida al efecto túnel
  • 8. Blocking temperature • Flipping between ↓ and ↑ states occurs in a certain characteristic time that depends on temperature: U tf t 0 exp k BT T > TB • Below the blocking temperature TB the magnetic T<T B moment cannot flip above the barrier • Above the blocking temperature the magnetic moment can flip, following a Curie law: SUPERPARAMAGNETIC state
  • 9. Moleculas magnéticas • Identicas a SDP • Objetos cuánticos • M(H,T) univocally determined by D and E
  • 10. Magnetization curve • Application of an external field: Zeeman Term H S – Longitudinal field (H || easy axis) • Moves levels – Transverse field (H easy axis) • Allows tunneling • Tunneling is possible at resonant fields
  • 11. Spin resonant tunnel effect -2-1 0 1 2 -3 3 -4 4 -5 5 -6 6 -7 7 -8 8 -9 9 -10 10 Magnetic field B=0
  • 12. Spin resonant tunnel effect -1 0 1 -3-2 2 3 -4 4 -5 5 -6 6 -7 7 -8 8 -9 9 -10 10 Magnetic field B = 0.5B0
  • 13. Spin resonant tunnel effect -3-2 12 -4 3 -5 4 -6 5 -7 6 -8 7 -9 8 -10 9 B = B0 10 Magnetic field
  • 14. Spin resonant tunnel effect -3-2-10 1 -4 2 -5 3 -6 4 -7 5 -8 6 -9 7 -10 8 9 B = 2B0 Magnetic field 10
  • 15. Relaxation in Molecular Magnets • After a certain time, relaxation goes exponential M t M eq t 1 exp H t • Peaks of the relaxation rate Γ(H) at resonances
  • 16. A.C. measurements • TB depends on measuring frequency K V0 TB ln 1 / 0
  • 17. New trends in magnetism • Magnetic deflagration • Superradiance • Rotational Doppler Shift
  • 18. Magnetic Deflagration Deflagration is a technical term describing subsonic combustion that usually propagates through thermal conductivity Energy Barrier • There are two characteristic timescales which are AF important here. The first is the thermal diffusion timescale is approximately equal to FM • The second is the burning timescale that strongly decreases with temperature, typically as Energy released Thermal diffusion Ignition (barrier overcoming)
  • 19. From Magnetisation jumps to magnetic deflagration. Manganites Field jumps 1999 Deflagration-like description 2007 T=3K 1.0 Molecule magnets Field jumps 1999 S M/M 0.5 Deflagration-like description 2005 0.0 0 10 20 30 T = 1.8 K H (kOe) 1.0 0.5 Intermetallic compounds Field jumps 2002 M/Ms 0.0 Deflagration-like description 2009 -0.5 1.0 -1.0 0.8 -30 -20 -10 0 10 20 30 0.6 H (kOe) M/MS 0.4 0.2 0.0 0 5 10 15 20 25 30 35 40 45 50 H (kOe)
  • 20. Molecule Magnets H ΔE Magnetic deflagration: Propagation of a front of reversing spins at constant velocity along the crystal A. Hernández-Mínguez et. al. PRL 95 17205 (2005) Problem: Sweeping H we cannot control the magnetic field at which it occurs. Y. Suzuki et. al. PRL 95, 147201 (2005)
  • 21. Igniting avalanches with SAW Surface acoustic waves (SAWs) are low frequency acoustic phonons (below 1 GHz) The coaxial cable is connected to an Agilent microwave signal generator. The change of the magnetic moment is registered by a rf-SQUID magnetometer. Hz coaxial cable IDT Mn12 crystal c-axis conducting LiNbO3 stripes substrate
  • 22. Quantum magnetic deflagration in nanomagnets κ U(H) v exp τ0 2k B T f This velocity is well fitted: κ = 0.8·10-5 m2/s • The speed of the avalanche Tf (H = 4600 Oe) = 6.8 K Tf (H = 9200 Oe) = 10.9 K increases with the applied magnetic field. • At resonant fields the • The ignition time shows peaks at the velocity of the flame front magnetic fields at which spin levels presents peaks. become resonant.
  • 23. Associated to the deflagration... • Superradiance emission (?) – All spins decay to the fundamental level coherently, with the emission of photons. -3-2-10 1 -4 2 -5 3 -6 4 -7 5 -8 6 -9 7 -10 8 9 B = 2B0 10
  • 24. Linear Doppler Shift on frequency due to relative velocity between emitter and observer (non relativistic case): Relative velocity v 1 Frequency c seen by the observer Frequency of the emitter v c
  • 25. Rotational Doppler Shift on frequency due to relative rotation between emitter and observer (circularly polarized light): Relative rotation Frequency seen by the Frequency of observer the emitter
  • 29. Rotational Doppler Effect 2 B FMR 0 H  n I n Hn 0 I 2   H Hn 1 Hn  I 2 B I measured H ~ 2 . 5 Oe produced by r ~ 1nm particles
  • 30. Rotational Doppler Effect Occupied states L L 1 En n n 1 B H 2I 2 En n ~ B H 1/ 2 k BT E n ~ k BT n~ B H T ~ 2K n 100 B H ~ 0 . 17 mK
  • 31. Rotational Doppler Effect • Change in frequency observed due to rotation: • RDE in GPS systems (resonance of an LC circuit) – Resonant frequency insensitive to magnetic fields Resonance • RDE in Magnetic Resonance systems – Resonant frequency sensitive to magnetic fields Resonance
  • 32. Rotational Doppler Effect • Article by S. Lendínez, E. M. Chudnovsy, and J. Tejada: arXiv:1008.2142v1 [cond-mat.other] • Expression for ω’Res are found for ESR, NMR and FMR. Resonance • Exact expression depends on type of resonance (ESR, NMR or FMR) • Depends on anisotropy
  • 33. Rotational Doppler Effect • Ω ≈ 100 kHz • ESR and FMR: • ωRes ≈ GHz Ω << ωRes << Δω • Δω ≈ MHz BUT Position of maximum can be With free rotors: determined with accuracy of 100 kHz ≈ Ω • ω Ω≈ 100 Ω ≈ Δω ≈ MHz MHz • NMR: Res • Δω ≈ kHz Gyromagnetic ESR and tensor • κ ≠ 1 needed anisotropy FMR: (shape,...) NMR: Hyperfine interactions