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the most general case third-order nonlinear processes can relate up to four different frequency
components, . The 3rd-order nonlinear susceptibility is a tensor of rank 4,
described in the most general case by independent components. The 3rd-order nonlinear
polarization can be given by following a similar procedure developed for the description of the 2nd-
order effects. The polarization at frequency is given by
(5.1)
The description of the general four-wave mixing (FWM) process involves the solution of four coupled
wave equations.
In this chapter we will consider a few practically important specific examples. These include third-
harmonic generation (THG) and the Kerr effect. As a special case of the latter the intensity-dependent
refractive index is considered.
(5.2)
(5.3)
By substituting the Fourier amplitudes of the above two-component field into this expression and
selecting the terms contributing to the polarization at the 3rd harmonic the following expression is
obtained:
(5.4)
By writing out the coordinate indices explicitly this gives:
(5.5)
where can take the values . Please note the change in the meaning of the indices
(denoting Cartesian coordinates rather than the frequency component) and the arguments of the field
quantities (denoting the frequency rather than the propagation distance ). The -dependence and
the order of nonlinearity are not written out explicitly.
THG can be treated similarly to SHG, described by two coupled wave equations. In the limiting case
of negligible pump depletion we get similar result for the 3rd harmonic field:
(5.6)
The phase-mismatch parameter is defined as . The intensity of the third harmonic
beam is given by
(5.7)
Notice the cubic dependence of the THG intensity on that of the fundamental.
In this Section structurally isotropic media will be assumed for simplicity. Gases, liquids, and
amorphous solids are examples of such media. Please note that cubic crystals are optically isotropic
but not structurally. For structurally isotropic media only 21 out of 81 elements of are non-zero,
which can be grouped in four types . The following relations hold:
(5.8)
(5.9)
(5.10)
(5.11)
(5.12)
Hence, a structurally isotropic medium has 3 independent components. The tensor nature of the
linear and nonlinear susceptibilities will be discussed in more detail in Chapter 6.
DC Kerr effect
(5.13)
Let us assume that the DC field is in the direction and the optical field propagates
in the direction. The nonlinear polarization at the optical frequency can be written
as
(5.14)
(5.15)
The induced change of the refractive index is different for light polarized parallel and
perpendicular to the applied DC field. This means that the birefringence of the
medium is changed (or a birefringence is induced) as
(5.16)
(5.17)
with . The DC Kerr effect can be used for optical switching. This requires
that the optical beam propagates a half-wave distance through the medium placed
between crossed polarizers:
(5.18)
In the optical or AC Kerr effect an intense optical beam at frequency modulates the refractive
index for a co-propagating weak probe beam at frequency . This effect is also called as cross-
phase modulation (XPM). Let us assume that both fields are polarized in the direction. The
nonlinear polarization is:
(5.19)
(5.20)
In case of -polarized probe beam and -polarized strong beam, the type 4 coefficient becomes
effective rather than the type 1:
(5.21)
By substituting the corresponding Fourier amplitude into the general expression of the 3 rd-order
polarization given above one obtains
(5.23)
where intrinsic permutation symmetry (IPS) was taken into account. For a beam polarized in the
direction the nonlinear polarization is given by:
(5.24)
(5.25)
where is the low-intensity refractive index and is called the nonlinear refractive index.
In case of circularly and elliptically polarized light the effects of IDRI become more complex.
(5.26)
(5.27)
(5.28)
As a consequence of this feature, for elliptically polarized light, the axes of the ellipse rotate during
propagation. For linearly or circularly polarized light the polarization state remains unchanged. The
above expression giving the refractive index change illustrates this for linearly polarized light: the
expression does not contain the coefficient . For circularly polarized light the corresponding
equation is:
(5.29)
Self-focusing
IDRI has important practical relevance. One consequence is self-focusing. Self-focusing of light is the
process in which an intense beam modifies the refractive index of the medium such that the beam is
caused to come to a focus within the material (Fig. 5.2a). Here we have assumed that is positive.
As a result, the laser beam induces a refractive index variation within the material with a larger
refractive index at the center of the beam than at its periphery (Fig. 5.3). Thus the material acts as if it
were a positive lens, causing the beam to come to a focus within the material.
Figure 5.2. Schematic illustration of three self-action effects: (a) self-focusing of light, (b) self-trapping
of light, and (c) laser beam breakup, showing the transverse distribution of intensity of a beam that
has broken up into many filaments.
Figure 5.3. Distortion of the phase front of a collimated laser beam due to IDRI.
Another self-action effect is the self-trapping of light (Fig. 5.2b). In this process a
beam propagates with a constant diameter as a consequence of an exact balance
between self-focusing and diffraction. Self-trapping can occur only if the power
carried by the beam is exactly equal to the so-called critical power for self-trapping.
(5.30)
Self-focusing can occur only if the beam power is greater than . The exact value of
depends on the precise beam profile, and is usually close to 2.
The final self-action effect shown in Figure 5.2c is laser beam breakup. This process occurs only
for and leads to the breakup of the beam into many components each carrying
approximately power . This process occurs as a consequence of the growth of imperfections of
the laser wavefront by means of the amplification associated with the forward four-wave mixing
process.
A simple model of the self-focusing process can be given by ignoring the effects of diffraction. The
neglect of diffraction is justified if the beam diameter or intensity (or both) is sufficiently large. Figure
5.4 shows a collimated beam of characteristic radius and an on-axis intensity falling onto a
nonlinear optical material with positive . Fermat’s principle can be used to determine the
distance from the input face to the self-focus. It states that the optical path length of
all rays traveling from a wavefront at the input face to the self-focus must be equal. As a first
approximation, we take the refractive index along the marginal ray to be the linear refractive
index and the refractive index along the central ray to be . According to Fermat’s
principle:
(5.31)
where the angle is defined in the Figure. Solving the approximate expression for , we find
that
(5.32)
This quantity is known as the self-focusing angle and in general can be interpreted as the
characteristic angle through which a beam of light is deviated as a consequence of self-action effects.
The ratio of nonlinear to linear refractive index is invariably a small quantity, thus
justifying the use of the paraxial approximation. In terms of the self-focusing angle, we can calculate
the characteristic self-focusing distance as or as
(5.33)
Figure 5.4. Prediction of the self-focusing distance by means of Fermat’s principle. The curved
ray trajectories within the nonlinear material are approximated as straight lines.