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optical effects
Magnetooptics deals with phenomena arising as a result of interaction between light and matter when the latter is subjected to a magnetic field. In the case of magnetically ordered matter (ferromagnets, ferrimagnets, etc) magnetooptical effects may appear in the absence of an external magnetic field as well. The presence of a magnetic field changes the dispersion curves of the absorption coefficient and leads to the appearance or variation of optical anisotropy. A great number of magnetooptical phenomena are the direct or indirect outcome of the splitting of system energy levels in an external magnetic field. This splitting is the Zeeman effect'. Essentially, all other magnetooptical effects are consequences of the Zeeman effect. Basic magnetooptical phenomena can be classified according to the relative orientation of the wave vector of the light emission k and the magnetic field H . Two basic geometries are distinguished (figure 1.1): and
(1) Faraday geometry: the light travels along the field direction
(k 11 H ) ;
(k IH ) .
In both cases the Zeeman effect is observed-longitudinal in the Faraday geometry and transverse in the Voigt geometry. In an absorption spectrum the optical anisotropy of a magnetized medium manifests itself as dichroism, i.e. the difference between the absorption coefficients for the two orthogonal polarizations. Dichroism is defined as the difference between the absorptions of the circularly polarized components
I In 1896. P Zeeman, Dutch physicist and Nobel prize winner. discovered that, when a sodium flame is placed between the poles of an electromagnet. the two yellow lines are considerably broadened. Shortly afterward, Lorentz presented a simple theory for these observations, based upon the electron theory of matter.
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Copyright 1997 IOP Publishing Ltd
Introduction
( k , - k - ) in the case of the Faraday geometry (so-called magnetic circular dichroism (MCD)),and in the Voigt geometry it is determined from the difference between the absorptions of components polarized parallel and perpendicular to the magnetic field (the magnetic linear dichroism (MLD)). These effects are analogues of the transverse and longitudinal Zeeman effects. From the Kramers-Kronig relations it follows that the splitting of the dispersion curves of the absorption coefficient (i.e. MCD or MLD) is connected with the splitting of the dispersion curves of the refractive index. In this case it shows up as a difference between the refractive indices for the two circularly polarized components (the magnetic circular birefringence or Faraday effect) in the Faraday geometry and for the two linearly polarized components (the magnetic linear birefringence) in the Faraday geometry.
L k
Figure 1.1. Magnetooptical effects resulting from the interaction of optical radiation with the medium: magnetic circular birefringence ((a), (b)), magnetic circular dichroism ((c). (d)). magnetic linear birefringence (e), and magnetic linear dichroism ( f ) .
The constant V , called the Verdet constant, is defined as the rotation per unit path, per unit field strength. The Verdet constant depends upon the properties of the medium, the frequency of light, and the temperature T . The sign of the angle 8 depends on the sign of H . Therefore if the light travels twice through a field, first along the field direction, and then after normal
reflection from a mirror in the opposite direction, the value of 8 is doubled. This is a phenomenological distinction of the Faraday effect from the effect of natural optical activity. In the latter case, when light returns, 8 = 0. The circular anisotropy of the magnetized medium is explained by the fact that magnetic field splitting of the energy levels of the ground and excited states creates energy non-equivalence of quantum states with different eigenvalues of the angular momentum. From a phenomenological point of view, the Faraday effect is explained as has been pointed out above by the fact that the refractive indexes. i t + and n- for the left-hand and right-hand circularly polarized light in the case of an originally inactive substance, become different when the latter I S placed in a magnetic field. Linearly polarized light with a given plane of polarization can be represented as a superposition of the right-hand and the left-hand circularly polarized waves with a definite phase difference. As a consequence of the difference between n+ and n-, the right-hand and the lefthand circularly polarized waves propagate with different velocities, c/n+ and c / n - . The plane of polarization of the linearly polarized light therefore rotates through the angle w 8 = -(n+ - n - ) L (1.2) 2c where w is the angular frequency, c is the velocity of light, and L is the path length of an optical beam in the medium. The magnetic-field-induced Larmor precession of electron orbits is the simplest mechanism for the Faraday effect. Instead of one eigenfrequency of the electron ( w ) , two ( U + and w - ) arise, corresponding to the right-hand and the left-hand circular oscillations when there is a magnetic field in the medium. Theory shows that
w+ = WO
f ---
1 e H 2m c
where e and m are the electron charge and mass. The appearance of two resonance frequencies (0- and U + ) in a medium placed in a magnetic field gives rise to the splitting of the absorption line. The difference between the resonance frequencies in the Zeeman doublet, w+ and w - , results in a displacement of the curves n+(w) and n - ( w ) relative to each other on the frequency scale:
rt+(w)
dn e H n ( w ) f -dw 2nzc
( 1.4)
where n(o)is the refractive index in the absence of the field H . Substituting (1.4) and (1.2) into ( I . 1 ) yields the well-known Becquerel formula
where k = 2rrc/w is the wavelength of light. Formula ( 1 S ) is consistent with experimental data for diamagnetic media. Complete analysis of the phenomenon
Copyright 1997 IOP Publishing Ltd
Introduction
has to be carried out on the basis of quantum mechanics (chapter 5 ) . Figure 1.2 shows that formula ( 1 . 1 ) describes with high accuracy the Faraday rotation in paramagnetic glasses in magnetic fields up to 7 MOe (Pavlovskii et a 1980). f
4 0.54
4 0.972
4
2.6
H (MOe)
6.3
Figure 1.2. The Faraday effect for the glass TF-5 ( V = 0.0495' cm-' Oe, I = 5 mm). The intervals between minima are 180'. The numbers correspond to the magnetic field measured in MOe. After Pavlovskii et a1 (1980).
Giant values of rotation -1-10' cm-' Oe-I were observed for the magnetic semiconductor Cdo 95MnoosTe (Gaj et a1 1993).
(b)
ic 1
Figure 1.3. Magnetooptical Kerr effects taking place when light is reflected from the surface of a magnetized material: polar (a); longitudinal (meridional) (b); and transverse (equatorial) (c) effects (the subscripts p and s in E,, and E , indicate p and s polarization of the wave).
1.4
Optical anisotropy of a magnetized medium manifests itself also in the reflection of light from its surface. Phenomena arising here are generally referred to as the magnetooptical Kerr effect. It consists in an influence of the magnetization of the medium on the reflected light2. Depending on the orientation of the magnetization vector relative to the reflective surface and the plane of incidence of the light beam, three types of magnetooptical effect in reflection are distinguished: the polar, longitudinal (meridional), and transverse (equatorial) Kerr effects. The magnetization vector M is oriented perpendicularly to the reflective surface and parallel to the plane of incidence in the polar effect (figure 1.3(a)). The geometry of the longitudinal Kerr effect is shown in figure 1.3(b). The influence of magnetization in both of these effects is reduced to a rotation of the plane of polarization and the appearance of ellipticity of the reflected linearly polarized light. The general feature of the polar and longitudinal effects is the presence of a non-zero projection of the wave vector k of the electromagnetic wave on the magnetization direction M . The polar Kerr effect is of great importance for optical data storage, since it is the basis for reading information from magnetooptical disks. The geometry of the transverse (equatorial) Kerr effect is depicted in figure 1.3(c). It is observed when the magnetization vector is oriented perpendicularly to the plane of incidence of the light, and it is revealed in the change of intensity and phase of the linearly polarized light reflected by the magnetized medium. This effect corresponds to the transverse magnetooptical effect since the projection of the light wave vector in the magnetization direction is here equal to zero. The transverse Kerr effect, unlike the Cotton-Mouton effect, is odd in
The magnetooptical Kerr effect was discovered by the Scottish physicist John Kerr in 1888. He observed that when plane-polarized light is reflected at normal incidence from the polished pole of an electromagnet, it becomes elliptically polarized with the major axis of the ellipse rotated with respect to the plane of polarization of the incident beam.
lntroductioti
E (eV)
1
2
I
3
I
L
I
U U
-0.2
e -0.3
-0.4
-0.5
-0.6
Figure 1.4. The spectral dependence of the polar Kerr rotation in Ni (dotted curve ( I ) : Krinchik and Artemev ( 1968); solid curve (2): van Engen ( 1983)) and the ellipticity of Nio.92Auo,,~X (chain curve (3): Buschow (1988)); of the polar Ken rotation in CO alloy (dotted curve (4):Krinchik and Artemev (1968); solid curve ( 5 ) : van Engen (1983); chain curve (6): Carey et a1 (1983)); and of the polar Kerr rotation in Fe (dotted curve (7): Krinchik and Artemev (1968); solid curve (8): van Engen (1983); dashed curve
(9): Carey et
U/
(1983)).
the magnetization. Therefore it is widely employed in magnetic investigations, particularly for observations of magnetic domains at the surface of a magnetized sample. Also, this effect allows the design of transversely magnetized mirrors as non-reciprocal optical devices. In general the Kerr effects are small; for example, the polar Kerr angles for perpendicular incidence for iron, cobalt, and nickel are typically less than a degree in the visible range of the spectrum, and the transverse effect is 0.01 or less (figure 1.4j. Transition metal compounds containing Mn and Pt are known to show a giant magnetooptical Kerr effect. Van Engen et a (1983b) discovered the giant f Kerr effect in the Heusler compound PtMnSb, which has a maximum Kerr
rotation of 1.2 at 1.7 eV photon energy. There is a huge Kerr rotation of I . 18 in MnPt3 (Kato et a1 1983b).
1.5
The formal description of magnetooptical effects is based on consideration of the influence of a magnetic field on the dielectrical permittivity tensor of the medium c l , . If E;,, is symmetric (c;k = ~ k , at H = 0, it becomes non-symmetric ) (E,~(H) = cki(-H)) in the presence of a magnetic field H . In this case the requirement of reality of the cik-tensor for a transparent medium is replaced with the requirement of its hermiticity:
From the present considerations it follows that the symmetric part of the tensor c I k of a transparent magnetized medium is real, and the antisymmetric part is imaginary. Besides which, the real components of c,k have to be even functions of the magnetic field. A second and most important point which must be made in relation to magnetooptical calculations is as regards the choice of sign convention, for the form of the permittivity tensor and also the sense of magnetooptically induced rotations and ellipticities. There are advantages and disadvantages to all of the basic sign schemes and, in the final analysis, that adopted may be a question of personal taste or may have been chosen for historical reasons. However, whatever choice is made with regard to the sign convention, the scheme must be clearly stated and, where possible, justified as being an appropriate and reasonable choice. To begin with. assume that the plane-wave solutions to the Maxwell equations are taken to have a negative time exponent e-w, and take the form of the skew-symmetric permittivity tensor as
[E]
= n2
-iQ
+;Q
; ;]
0
where the complex index of refraction n and the so-called magnetooptical parameter Q are
and the magnetization lies along the z-direction. The form of the permittivity given in equation (1.6) ensures that the signs of the Kerr and Faraday rotations and ellipticities are positive for a clockwise rotation of the axes of the polarization ellipse and a clockwise rotation of the E vector respectively, when viewed along the positive z-direction (see section 2.2).
Copyright 1997 IOP Publishing Ltd
Introduction
It is perhaps worth making a number of points in relation to other schemes, so that the reader familiar with an alternative convention can easily convert from one scheme to another (Atkinson and Lissberger 1992). First, it is equally valid in the plane-wave solution to the Maxwell equations to take the positive time exponent as The consequence of doing this is that the complex refractive index must now be written as n - in, again to ensure an exponential decay of the wave amplitude with increasing propagation distance. On choosing the same form for the magnetooptical parameter, namely Q - iQ, all other transformations between this scheme and the preferred one are simply obtained by changing the sign associated with all of the imaginary quantities. This applies throughout the whole of any magnetooptical analysis, including, for example, the Kerr or Faraday ellipticities which may be regarded as imaginary components of the complex Kerr of Faraday rotations. Second, a commonly used form for the permittivity tensor has the signs of the off-diagonal elements reversed compared to those shown in equation ( 1.6). The transposition from one scheme to the other is effected quite simply by multiplying any terms in Q by minus one.
1.6 Other physical aspects
1.6.1 Time-reversal symmetry, and circular anisotropy in a rotating medium The origin of circular birefringence and dichroism is evident from a symmetry viewpoint. Magnetic field. which is an axial vector, has the symmetry of a circular current set out in a plane perpendicular to the vector of the magnetic field. In a medium placed in a magnetic field, the rotation directions in a plane oriented perpendicularly to the magnetic field are non-equivalent. Therefore the optical properties of a magnetized medium for light propagating along the field direction with right-hand and left-hand circular polarization have to be different. By analogy we can assert that a mechanically rotating medium ought to reveal circular anisotropy along its rotation axis. This follows from the fact that angular velocity, like magnetic field. is an axial vector. The effect of rotation q f t h e plane of polarization on a rotating medium predicted by J J Thomson in 1885 was recently discovered experimentally (see Jones 1976). The Faraday rotation and the Kerr effect can be assigned as non-reciprocal effects. They are characterized by different phase velocities and/or attenuations of light waves travelling along the same optical path but in opposite directions. Non-reciprocal optical effects are usually observed in magnetized media. A magnetic moment can be induced by a magnetic field in paramagnets and diamagnets or can arise spontaneously, as in ferromagnets or ferrimagnets. In
This effect is a close analogue of the Barnette effect. i.e. magnetization appears in a rotating medium. The latter is in its turn related to the Einstein-de Haas effect consisting in the sample twisting during its magnetization in a reverse sense.
all of these the time-reversal symmetry (T) is broken. A number of attempts have been made to detect the non-reciprocal optical effects due to time-parity violation in high-T,. superconductors predicted within some theoretical models (see, e.g., Spielman et a1 1990). All of these attempts failed, but meanwhile non-reciprocal optical rotation was observed in a conventional antiferromagnet (Krichevtsov et a1 1993).
1.6.2
Effects in which emission not only probes the magnetic state of a medium but also changes it in an active way are referred to as magnetooptical effects. It is well known that an elliptically polarized wave has angular momentum. Therefore, circularly (and elliptically) polarized light giving rise to electronic transitions of the atoms induces orientation of their moments relative to the light beam direction. These effects are most conspicuous in magnetic semiconductors. From this point of view it is interesting to consider the photo-induced change in magnetization of solid or gas-like paramagnets effected by circularly polarized emission. This phenomenon was discovered in 1952 by A Kastler and it is known as optical orientation. Atomic absorption of circularly polarized photons results in a change of magnetization of the medium. In principle, optical orientation can appear as a result of emission of sufficiently small intensity if the magnetization relaxation times are sufficiently large. It should be noted that angular momentum exchange between circularly polarized emission and a medium may also produce macroscopic angular momentum in the medium, i.e. a twist of the sample (the Sadovskii effect predicted in 1899). This effect is rather small, but was observed experimentally (see Rosenberg 1950, Santamato et a1 1986). 1.6.3 Non-linear magnetooptical effects Different effects arise in transparent media. It is known from electrodynamics that a rotating electric field acts as an effective magnetic field, whence it immediately follows that a medium becomes magnetized under the action of an intense circularly polarized wave. The magnetization direction is defined by the sign of the circularly polarized light. This effect is called the inverse Faraday effect. This non-linear optical effect can be observed if the amplitude of the electromagnetic field is fairly large. The inverse Faraday effect has been observed in crystals doped with paramagnetic centres and in metal vapours. Non-linear magnetooptics-in particular, magnetism-induced secondharmonic generation (MSHG)-is of general interest, and is becoming an important tool in the investigation of fundamental problems of magnetic films, multilayers, and surfaces. MSHG derives its sensitivity from the breaking of the symmetry at the surface or at interfaces. Because the optical penetration length
Copyright 1997 IOP Publishing Ltd
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lntroductiori
is of order 50-100 nm, not only surfaces but also buried interfaces can be studied by this method. There is a large enhancement of the non-linear MOKE (Aktsipetrov et a/ 1990, Reif et a1 1991, Spierings et a1 1993, Pustogowa et a1 1994, Vollmer et a/ 1995) in comparison with the linear MOKE. Magnetism-induced MSHG was also observed in the magnetoelectric materials CrzO3 (Fiebig et a1 1994) and BiFeO3 (Agaltsov et a1 1989).
Is - I I+ + I-
can be assigned as a spectrum of the magnetic circular luminescence. The luminescence spectrum carries information about the magnetization of the excited ions (Zapasskii and Feofilov 1975).
1.6.5
The transmission and reflection magnetooptical effects considered above constitute the foundation of established methods for studying the magnetic materials in the visible, infra-red and ultra-violet regions. There are analogous magnetooptical effects in the x-ray region. Although the x-ray polarizability of materials is very slight (see chapter 6), there is great scientific interest and progress in the use of x-ray magnetooptical effects as a probe of magnetic materials. This has become possible due to both theoretical advances in describing near-x-ray-absorption-edge phenomena and great experimental progress achieved with the use of synchrotron radiation (SR). Broad-spectrum, high-brightness sources, which provide intense monochromatic beams of 1010l3 photons per second, and the unique polarization properties of SR permit the realization of experimental methods involving the production, monitoring, and detection of polarized x-rays. Magnetic x-ray dichroism (MXD) was predicted by Erskine and Stern (1975) and Thole et a/ (1985a, b) and observed using both linearly (van der Laan et a1 1986) and circularly (Schutz et a / 1987) polarized synchrotron radiation. Magnetic circular x-ray dichroism (MCXD) is mainly used as a tool at the x-ray absorption edges of 3d or 4f elements, where large asymmetries in the white lines upon reversal of either the sample magnetization or the photon spin are observed. MXD has opened up the possibility for element-specific analysis of magnetic materials.
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MXD is also lattice site specific, because the final electron states are disturbed by the crystal field, and this disturbance is different when the same ions occupy different lattice sites. This method supplements neutron diffraction because it does not require a large volume of material (it could determine for example the orientation of the moment on impurities). In addition it can determine the orientation of the magnetic moments absolutely. MXD has all the versatility of x-ray absorption spectroscopy: one can study bulk spectra by measuring the fluorescence of the core hole, or just the first few atomic layers by measuring the intensity of the Auger electrons. This makes MXD especially suitable for studying the magnetism of surfaces and thin films. Moreover, the sum rule for MCXD spectra allows a quantitative determination of the orbital contribution to the total magnetization. This direct measurement of orbital angular momentum is highly desirable for probing spin-orbit interaction and macroscopic phenomena originating from it (e.g. magnetocrystalline anisotropy). In general, MXD attracts great interest as a tool for studying phenomena (spin-orbit coupling, exchange interaction, hybridization, and crystal-field splitting) affecting the electronic structure of a sample. Many alloy surfaces and multilayers exhibiting unusual magnetic properties have been probed by MCXD. Somc other phenomcna connected with the interaction of x-rays and magnetic structure such as the Kerr effect (Bonarski and Karp 1989) and Faraday rotation (Siddons er a1 1990) have also been observed using SR.
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Introduction
1.7.1 Dielectrics
In chapter 8 the magnetooptical properties of different classes of magnetic dielectric, such as orthoferrites, manganites, spinel ferrites, magnetoplumbite, barium hexaferrite, chalcogenide spinels, chromium trihalides, europium oxide and monochalcogenides. ferric borate. and ferric fluoride, are described. For most of these compounds the spectral dependencies of the Faraday and Kerr effects are presented, and the nature of the magnetooptical activity of magnetic dielectrics is discussed.
Applied magnetooptics
1.7.3 Metals and alloys
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In chapter I O the experimental results obtained on ferromagnetic metals and compounds are presented. Included in this section will also be a discussion of magnetooptical properties of alloys based on simple metals, binary intermetallics including Copt, MnBi and pseudo-binary compounds, ternary compounds including PtMnSb and Heusler alloys. amorphous fiims of rare-earth-transition metal alloys used in magnetooptical disk memories, and low-temperature uranium- and rare-earth-containing compounds with outstanding magnetooptical properties including U(Sb, Te), CeSb and others.
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Introduction
the devices that control the intensity of optical radiation in optical communication and data-processing systems by applying a magnetic field. Low-frequency modulators based on domain wall movement and high-frequency modulators based on the rotation of the magnetization vector of a saturated sample are described. Development of optical fibres with extremely low losses has stimulated development of non-reciprocal elements (optical isolators), which are used in communication systems for the suppression of reflected signals, which appear in fibre-optic connectors and other contact elements of functional optical devices and which have adverse effects on the optical performance of laser sources.
Applied magnetooptics
15
The thin-film magnetooptical isotropic and anisotropic waveguides, and the problems of optical losses, induced optical anisotropy and mode conversion are examined in chapter 15. Integrated magnetooptical waveguide modulators, and non-reciprocal elements and structures are also described in chapter 15. Special attention is paid to a new branch of integrated magnetooptics at the interface of microwave technology and integrated optics, which is based on waveguide mode interaction with magnetostatic waves.