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Patterson, Bailey - Solid State Physics Introduction to theory

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7.4 Magnetic Resonance and Crystal Field Theory

447

 

 

Table 7.7. The character table of D3

 

C1

 

C2

 

 

C3

 

 

 

 

 

 

 

g5

 

 

g1

 

g2

g3

g4

g6

 

χ(1)

1

1

1

1

1

1

 

χ(2)

1

1

1

1

1

1

 

χ(3)

2

1

1

0

0

0

Below we summarize some important rules for constructing the character table for the irreducible representations. These results will not be proved, since they are readily available.29 These rules are:

1.The number of classes s in the group is equal to the number of irreducible representations of the group.

2.If ni is the dimension of the ith irreducible representation, then ni = χi(E), where E is the identity of the group and ∑sl ni2 = h, where h is the order of the group G. For small finite groups, this rule obviously greatly restricts what the ni can be.

3.If Bk is the number of group elements in the class Ck, then the characters for each class obey the relationship

s = Bk χ(l) (Ck )χ( j) (Ck ) = hδ j , k 1 l

where δlj is the Kronecker delta. This relation is often called the orthogonality relation for characters.

4.Suppose the order of a group element g is m (i.e. suppose gm = E). Further suppose that the dimension of a representation (which need not be irreducible) is n. It then follows that χ(g) equals the sum of n, mth roots of unity.

5.The one-dimensional representation is always present.

Finally it is worth giving the criterion for determining the irreducible representations in a given reducible representation. The rule is if

R = i CiRi ,

(7.288)

then Ci (which is the number of times that irreducible representation i appears in the reducible representation R) is given by

Ci′ = (1/ h)k Bk χ(i) (Ck ) χ(Ck ) ,

(7.289)

where χ denotes character relative to R and the sum over k is a sum over classes. When a reducible representation is expressible in the form (7.288) it is said to be in, reduced form. Putting it into such a form as (7.288) is called reduction.

29 See Mathews and Walker [7.47].

448 7 Magnetism, Magnons, and Magnetic Resonance

A frequent use of these results occurs when the representation R is formed by taking direct products (see Sect. 1.2.1 for a definition) of the representations R(i). We can then evaluate (7.289) by remembering that the trace of a direct product is the product of the traces.

There are many ways that group theory has been used as an aid in actual calculations. No doubt there remain other ways that have not yet been discovered. The basic ideas that we will use in our physical calculations involve:

1.The physical system determines a symmetry group with irreducible representations that can be found by group theory.

2.Except for what is called by definition “accidental degeneracy” we have a distinct eigenvalue for each (occurrence of an) irreducible representation. (It is possible for the same irreducible representation to occur many times. The meaning of the word “occur” will be given later.)

3.The dimension of the irreducible representation is the degeneracy of each corresponding eigenvalue.

For a brief insight into the above, let the eigenfunctions of H corresponding to the eigenvalue En be labeled ψni(i → 1 to d). En is thus d-fold degenerate. Thus

ni = Enψni .

(7.290)

If g is an element of the symmetry group G, it follows that

 

[g,H ] = 0 .

(7.291)

From this,

 

H (gψni ) = En (gψni ) .

(7.292)

Comparing (7.290) and (7.291), we see that

 

gψni = id=1Cinψin .

(7.293)

It can be shown that Cni matrices are a representation of the group G. We thus have the desired connection between energy levels, degeneracy, and representations.

Let us consider the physically interesting problem of an atom with one 4f electron. Let us place this atom in a potential with trigonal symmetry. The group appropriate to trigonal symmetry is our old friend D3. We want to neglect spin and discover what happens (or may happen) to the 4f energy levels when the atom is placed in a trigonal field. This is a problem that could be directly attacked by perturbation theory, but it is interesting to see what type of statements can be made by the group theory.

If you think a little about the ideas we have introduced and about our problem, you should come to the conclusion that what we have to find is the irreducible representations of D3 generated by (in previous notation) ψ(4f)i. Here i runs from 1 to 7. This problem can be solved by using (7.289).

7.4 Magnetic Resonance and Crystal Field Theory

449

 

 

The first thing we need to know is the character of our rotation group. This is given by [61] for the lth irreducible representation

χ(l) (φ) =

sin[(l +

1

)φ]

 

 

 

 

 

2

 

.

(7.294)

sin(φ / 2)

 

 

 

In (7.294), φ is an appropriate rotation angle. Since we are dealing with a 4f level we are interested only in the case l = 3:

χ(3) (φ) = sin(7φ / 2) .

(7.295)

sin(φ / 2)

 

By (7.289), we need to evaluate (7.294) D3. Since the classes of D3 correspond two-fold rotations, we have

only for φ in each of the three classes of to the identity, three-fold rotations and

χ(3) (0) = 7 ,

(7.296a)

χ(3) (2π / 3) = +1,

(7.296b)

χ(3) (π) = −1 .

(7.296c)

Table 7.13. Character table for calculating Ci

 

C1

C2

C3

Bk

1

2

3

χ(1)

1

1

1

D3 χ(2)

1

1

1

χ(3)

2

1

0

Rotation Group χ(3)

7

+1

−1

We can now construct Fehler! Verweisquelle konnte nicht gefunden werden.. Applying (7.289) we have

C1′ = 16 [(7)(1)(1) + 2(+1)(1) + 3(1)(1)] =1,

C2′ = 16 [7(1)(1) + 2(+1)(1) + 3(1)(1)] = 2,

C3′ = 16 [7(1)(2) + 2(+1)(1) + 3(1)(0)] = 2 .

Thus

R = 2R(3) + R(1) + 2R(2) .

(7.297)

By (7.297) we expect the 4f level to split into two doubly degenerate levels plus three nondegenerate levels. The two levels corresponding to R(3) that occur twice and the two R(2) levels will probably not have the same energy.

450 7 Magnetism, Magnons, and Magnetic Resonance

7.5 Brief Mention of Other Topics

7.5.1 Spintronics or Magnetoelectronics (EE)30

We are concerned here with spin-polarized transport for which the name spintronics is sometimes used. We need to think back to the ideas of band ferromagnetism as contained for example in the Stoner model. Here one assumes that an exchange interaction can cause the spin-up and spin-down density of states to split apart as shown in the schematic diagram (for simplicity we consider that the majority spinup band is completely filled). Thus, the number of electrons at the Fermi level with spin up (Nup) can differ considerably from the number with spin down

(Ndown). See (7.242) and Fig. 7.32 (spins and moments have opposite directions due to the negative charge of the electron – the spins are drawn in the bands). This

results in two phenomena: (a) a net magnetic moment, and (b) a net spin polarization in transport defined by

P =

Nup Ndown

.

(7.298)

Nup + Ndown

 

 

 

Fe, Ni, and Co typically have P of order 50%.

In the figures, the D(E) describe the density of states of up and down spins. As shown also in Fig. 7.33 one can use this idea to produce a “spin valve,” which preferentially transmits electrons with one spin direction. Spin valves have many possible device applications (see, e.g., Prinz [7.55]). In Fig. 7.33 we show transport from a magnetized metal to a magnetized metal through a nonmagnetic metal.

E

E

EF

EF

T > Tc

T < Tc

D(E)

D(E)

D(E)

D(E)

non-magnetic metal

magnetized metal

Fig. 7.32. Exchange coupling causes band ferromagnetism. The D are the density of states of the spin-up and spin-down bands. EF is the Fermi energy. Adapted from Prinz [7.55]

30 A comprehensive review has recently appeared, Zutic et al [7.73].

7.5 Brief Mention of Other Topics

451

 

 

The two ferromagnets are still exchange coupled through the metal separating them. For the case of the second metal being antialigned with the first, the current is reduced and the resistance is high. The electrons with moment up can go from

(a) to (b) but are blocked from (b) to (c). The moment-down electrons are inhibited from movement by the gap from (a) to (b). If the second magnetized metal were aligned, the resistance would be low. Since the second ferromagnet’s magnetization direction can be controlled by an external magnetic field, this is the principle used in GMR (giant magnetoresistance, discovered by Baibich et al in 1988). See Baibich et al [7.4].

magnetized metal

non-magnetic metal

magnetized metal

 

E

 

E

E

 

 

 

Blocked

 

electrons

electrons

EF

 

 

 

 

(a)

(b)

(c)

Fig. 7.33. Due to preferential transmission of spin orientation, the resistance is high if the second ferromagnet is antialigned. Adapted from Prinz [7.55]

One should note that spintronic devices are possible because the spin diffusion length that is the square root of the diffusion constant times the spin relaxation time can be fairly large, e.g. 0.1 mm in Al at 40 K. This means that the spin polarization of the transport will typically last over these distances when the polarized current is injected into a nonmagnetized metal or semiconductor. Only in 1988 was it realized that electronic current flowing into an ordinary metal from a ferromagnet could preserve spin, so that spin could be transported just as charge is.

We should also mention that control of spin is important in efforts to achieve quantum computing. Quantum computers perform a series of sequences of unitary transformation on sets of “qubits” – see Bennett [7.5] for a definition. In essence, this holds out the possibility of something like massive parallel computation. Quantum computing is a huge subject; see, e.g., Bennett [7.5].

Hard Drives (EE)

In 1997 IBM introduced another innovation – the giant magnetoresistance (GMR) read head for use in magnetic hard drives – in which magnetic and nonmagnetic materials are layered one in the read head, roughly doubling or tripling its sensitivity. By layering one can design the device with the desired GMR properties. The device works on the quantum-mechanical principle, already mentioned, that

452 7 Magnetism, Magnons, and Magnetic Resonance

when the layers are magnetized in the same direction, the spin-dependent scattering is small, and when the layers are alternatively magnetized in opposite directions, the electrons experience a maximum of spin-dependent scattering (and hence much higher resistivity). Thus, magnetoresistance can be used to read the state of a magnetic bit in a magnetic disk drive. The direction of soft layer in the read head can be switched by the direction of the magnetization in the storing media. The magnetoresistance is thus changed and the direction of storage is then read by the size of the current in the read head. Sandwiches of Co and Cu can be used with the widths of the layers typically of the order of nanometers (a few atoms say) as this is the order of the wavelength of electrons in solids. More generally, magnetic multilayers of ferromagnetic materials (e.g. 3d transition metal ferromagnets) with nonferromagnetic spacers are used. The magnetic coupling between layers can be ferromagnetic or antiferromagnetic depending on spacing. Stuart Parkin of IBM has been a pioneer in the development of the GMR hard disk drive [7.52]

Magnetic Tunnel Junctions (MTJs) (EE)

Here the spacer in a sandwich with two ferromagnetic layers is a thin insulating layer. One difficulty is that it is difficult to make thin uniform insulators. Another difficulty, important for logic devices, is that the ferromagnetic layers need to be ferromagnetic semiconductors (rather than metals with far more mobile electrons than in semiconductors) so that a large fraction of the spin-aligned electrons can get into the rest of the device (made of semiconductors). GaMnAs and TiCoO2 are being considered for use as ferromagnetic semiconductors for these devices.

The tunneling current depends on the relative magnetization directions of the ferromagnetic layers. It should be mentioned here that in the usual GMR structures the current typically flows parallel to the layers (but electrons undergo a random walk, and sample more than one layer so GMR can still operate), while in a MTJ sandwich the current typically flows perpendicular to the layers.

For the typical case, the resistance of the MTJ is lower when the moments of the ferromagnetic layers are aligned parallel and higher when the moments are antiparallel. This produces tunneling magnetic resistance TMR that may be 40% or so larger than GMR. MTJ holds out the possibility of making nonvolatile memories.

Spin-dependent tunneling through the FM-I-FM (ferromagnetic-insulator-ferro- magnetic) sandwich had been predicted by Julliere [7.34] and Slonczewski [7.61].

Colossal Magnetoresistance (EE)

Magnetoresistance (MR) can be defined as

MR =

ρ(H ) ρ(0)

,

(7.299)

ρ(0)

 

 

 

where ρ is the resistivity and H is the magnetic field.

7.5 Brief Mention of Other Topics

453

 

 

Typically, MR is a few per cent, while GMR may be a few tens of per cent. Recently, materials with so-called colossal magnetoresistance (CMR) of 100 per cent or more have been discovered. CMR occurs in certain oxides of manganese – manganese perovskites (e.g. La0.75Ca0.25MnO3). Space does not permit further discussion here. See Fontcuberta [7.23]. See also Salamon and Jaime [7.58].

7.5.2 The Kondo Effect (A)

Scattering of conduction electrons by localized moments due to s-d exchange can produce surprising effects as shown by J. Kondo in 1964. Although, this would appear to be a very simple basic phenomena that could be easily understood, at low temperature Kondo carried the calculation beyond the first Born approximation and showed that as the temperature is lowered the scattering is enhanced. This led to an explanation of the old problem of the resistance minimum as it occurred in, e.g., dilute solutions of Mn in Cu.

The Kondo temperature is defined as the temperature at which the Kondo effect clearly appears and for which Kondo’s result is valid (see (7.301)). It is given approximately by

Tk = EF

 

1

(7.300)

J exp

,

 

 

 

nJ

 

where Tk is the Kondo temperature, EF is the Fermi energy, J characterizes the strength of the exchange interaction, and n is the density of states. Generally Tk is below the resistance minimum that can be estimated from the approximate expression giving the resistivity ρ,

ρ = a b ln(T ) + cT 5 .

(7.301)

The ln(T) term contains the spin-dependent Kondo scattering and cT5 characterizes the resistivity due to phonon scattering at low temperature (the low temperature is also required for a sharp Fermi surface), and a, b and c are constants with b being proportional to the exchange interaction. This leads to a resistivity minimum at approximately

 

 

b 1/ 5

 

TM

=

 

.

(7.302)

 

 

 

5c

 

In actual practice the Kondo resistivity does not diverge at extremely low temperatures, but rather at temperatures well below the Kondo temperature, the resistivity approaches a constant value as the conduction electrons and impurity spins form a singlet. Wilson has used renormalized group theory to explain this. There are actually three regimes that need to be distinguished. The logarithmic regime is above the Kondo temperature, the crossover region is near the Kondo temperature, and the plateau of the resistivity occurs at the lowest temperatures. To discuss this in detail would take us well beyond the scope of this book. See, e.g., Kirk WP,

454 7 Magnetism, Magnons, and Magnetic Resonance

“Kondo Effect,” pp. 162-165 in [24] and references contained therein. Using quantum dots as artificial atoms and studying them with scanning tunneling microscopes has revived interest in the Kondo effect. See Kouwenhoven and Glazman [7.41].

7.5.3 Spin Glass (A)

Another class of order that may occur in magnetic materials at low temperatures is spin glass. The name is meant to suggest frozen in (long-range) disorder. Experimentally the onset of a spin glass is signaled by a cusp in the magnetic susceptibility at Tf (the freezing temperature) in zero magnetic field. Below Tf there is no long-range order. The classic examples of spin glasses are dilute alloys of iron in gold (Au:Fe, also Cu:Mn, Ag:Mn, Au:Mn and several other examples). The critical ingredients of a spin glass seem to be (a) a competition among interactions as to the preferred direction of a spin (frustration), and (b) a randomness in the interaction between sites (disorder). There are still many questions surrounding spin glasses such as do they have a unique ground state and if the spin glass transition is a true phase transition to a new state (see Bitko [7.7]).

For spin glasses, it is common to define an order parameter by summing over the average spin’s squared:

q =

1

iN=1 Si

2 ,

(7.303)

 

N

 

 

 

and for T > Tf, q = 0, while q ≠ 0 for T < Tf. Much further detail can be found in Fischer and Hertz [7.22]. See also the article by Young [7.8 pp. 331-346].

Randomness and frustration (where two paths linking the same pair of spins do not have the same net effective sign of exchange coupling) are shared by many other systems besides spin glasses. Or another way of saying this is that the study of spin glasses fall in the broad category of the study of disordered systems, including random field systems (like diluted antiferromagnets), glasses, neural networks, optimization and decision problems. Other related problems include combinatorial optimization problems, such as the traveling salesman problem, and other problems involving complexity. For the neural network problem see for example, Muller and Reinhardt [7.50]. The book by Fischer and Hertz, already mentioned has a chapter on the physics of complexity with references. Another reference to get started in this general area is Chowdhury [7.12]. Mean-field theories of spin glasses have been promising, but there is no general consensus as to how to model spin glasses.

It is worth looking at a few experimental results to show real spin glass properties. Figure 7.34 shows the cusp in the susceptibility for CuMn. The true Tf occurs as the ac frequency goes to zero. Figure 7.35 shows the temperature dependence of the magnetization and order parameter for CuMn and AuFe. Figure 7.36 shows the magnetic specific heat for two CuMn samples.

 

 

 

 

 

 

 

 

 

 

 

 

 

 

7.5 Brief Mention of Other Topics

455

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

Fig. 7.34. The ac susceptibility as a function of T for CuMn (1 at %). Measuring frequencies: □, 1.33 kHz; o, 234 Hz, ■, 10.4 Hz; and , 2.6 Hz. From Mydosh JA, “Spin-Glasses – The Experimental Situation” Magnetism in Solids Some Current Topics, Scottish Universities Summer School in Physics, 1981, p. 95, by permission of SUSSP. Data from Mulder CA, van Duyneveldt AJ, and Mydosh JA, Phys Rev, B23, 1384 (1981)

 

0.48

 

 

 

 

0.43

 

 

 

 

0.38

 

CuMn

 

M(T)

0.33

 

 

 

 

 

 

 

 

0.28

 

AuFe

 

 

 

 

 

 

0.23

 

 

 

 

0.180

10

20

30

 

1.0

 

 

 

Q(T)

0.5

 

AuFe

 

CuMn

 

 

0

10

20

30

 

 

Temperature (K)

 

Fig. 7.35. The temperature variation of the magnetization M(T,H) and order parameter Q(T,H) with vanishing field (open symbols) and with 16 kG applied external magnetic field (full symbols) for Cu–0.7 at% Mn and Au–6.6 at% Fe; M(T,H=0) is zero. After Mookerjee A and Chowdhury D, J Physics F, Metal Physics 13, 365 (1983), by permission of the Institute of Physics

456 7 Magnetism, Magnons, and Magnetic Resonance

K)(mJ/mole

M C

80

Cu0.988Mn0.012

60

40

20

0

5

10

15

20

25

30

 

 

 

T(K)

 

 

 

K)(mJ/mole

M C

160

Cu0.976Mn0.024

120

80

40

0

5

10

15

20

25

30

T(K)

Fig. 7.36. Magnetic specific heat for CuMn spinglasses. The arrows show the freezing temperature (susceptibility peak). Reprinted with permission from Wenger LE and Keesom PH, Phys Rev B 13, 4053 (1976). Copyright 1976 by the American Physical Society

7.5.4 Solitons31 (A, EE)

Solitary waves are large-amplitude, localized, stable propagating disturbances. If in addition they preserve their identity upon interaction they are called solitons. They are particle-like solutions of nonlinear partial differential equations. They were first written about by John Scott Russell, in 1834, who observed a peculiar stable shallow water wave in a canal. They have been the subject of much interest since the 1960s, partly because of the availability of numerical solutions to relevant partial differential equations. Optical solitons in optical fibers are used to transmit bits of data.

Solitons occur in hydrodynamics (water waves), electrodynamics (plasmas), communication (light pulses in optical fibers), and other areas. In magnetism the steady motion of a domain wall under the influence of a magnetic field is an example of a soliton.32

In one dimension, the Korteweg–de Vries equation

u + A 3u + B (u2 ) = 0 t x3 x

(with A and B being positive constants) is used to discuss water waves. In other areas, including magnetism and domain walls, the sine-Gordon equation is encountered

2u

2u

C

 

2πu

A

2 B

 

2 = −

 

 

 

 

x

u0

sin

 

 

t

 

 

 

u0

31See Fetter and Walecka [7.20] and Steiner, “Linear and non linear modes in 1d magnets,” in [7.14, p199ff].

32See the article by Krumhansl in [7.8, pp. 3-21] who notes that static solutions are also solitons.

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