Introduction to Non-linear Optics
➢Change in Optical Properties and Generation of new
Harmonics
➢Classical expansion in powers of the field induced
Polarization
• Nonlinear optics is the study of phenomena that occur as a
consequence of the modification of the optical properties of a
material system by the presence of light
• Only LASER light is sufficiently intense to modify the optical
properties of a material system
• The beginning of the field of NLO is the discovery of SECOND
HARMONIC GENERATION by Franken et al. in 1961, shortly after the
demonstration of the first working laser demonstrated in 1960
by Maiman.
• Nonlinear optical phenomenon are “Nonlinear”in the sense that
they occur when the response of a material system to an applied
optical field depends in a nonlinear manner on the strength of
the optical field.
• The second harmonic generation occurs as a result of the part of the
atomic response that scales quadratically with the strength of the
applied optical field.
➢That means the intensity of the light generated at the
second harmonic frequency tends to increase as the
square of the intensity of the applied laser light
✓Consider how the dipole moment per unit volume, or polarization,
P(t), of a material system depends on the strength (t), of an applied
optical field
➢In the case of the conventional Linear Optics, the induced
polarization depends linearly on the electric field strength in a
manner that can often be described by the relationship
𝑃 𝑡 = 𝜖𝑜 𝜒 1 𝐸(𝑡)
➢the constant of proportionality 𝜒 1 is known as a linear
susceptibility and 𝜖𝑜 is the permittivity of free space
Nonlinear optics
The optical response can often be described by generalising the equation by expressing the polarization
P(t) as a power series in the field strength E(t) as
✓The quantities χ (2) and χ (3 ) are known as the second and third harmonic nonlinear optical
susceptibilities, respectively
✓For simplicity, taken the fields P(t) and E(t) to be scalar quantities in writing these equations
✓ Treating the vector nature of fields, in such a case, χ (1) becomes a second rank tensor and χ (2)
becomes the third rank tensor and so on
➢ It is also assumed that the polarization at time t depends only on the instantaneous value of electric
field strength
➢The assumption that the medium responds instantaneously also implies (through the Kramers–
Kronig relations) that the medium must be lossless and dispersion less.
➢How to generalize these equations for the case of a medium with dispersion and loss.
➢In general, the nonlinear susceptibilities depend on the frequencies of the applied fields, but under
present assumption of instantaneous response we take them to be constants.
is the second-order nonlinear polarization and
is the third-order nonlinear polarization, and so on for higher-order terms.
✓The physical processes that occur as a result of the second-order
polarization ˜ P(2) are distinct from those that occur as a result of the
third-order polarization ˜ P(3)
✓Also second-order nonlinear optical interactions can occur only in
noncentrosymmetric crystals—that is, in crystals that do not display
inversion symmetry
✓Since liquids, gases, amorphous solids (such as glass), and
even many crystals display inversion symmetry, χ(2) vanishes
identically for such materials, and consequently such
materials cannot produce second-order nonlinear optical
interactions.
✓On the other hand, third-order nonlinear optical interactions
(i.e., those described by a χ(3) susceptibility) can occur for
both centrosymmetric and noncentrosymmetric media.
• How to calculate the values of the nonlinear susceptibilities for various physical
mechanisms that lead to optical nonlinearities.
• For the present, we make a simple order-of-magnitude estimate of the size of
these quantities for the common case in which the nonlinearity is electronic in
origin
• One might expect that the lowest-order correction term ˜ P(2) would be
comparable to the linear response ˜ P(1) when the amplitude of the applied field
˜E is of the order of the characteristic atomic electric field strength),
𝐸𝑎𝑡 = 𝑒/(4𝜋𝜖𝑜 𝑎𝑜2 )
where −e is the charge of the electron and 𝑎𝑜 = 4𝜋𝜖𝑜 ℏ2𝑜 /𝑚𝑒2
is the Bohr radius of the hydrogen atom (here ℏ is Planck’s constant divided
by 2π, and m is the mass of the electron).
Numerically, we find that Eat = 5.14 × 1011 V/m.
• We thus expect that under conditions of nonresonant excitation the
second-order susceptibility χ(2) will be of the order of χ(1)/Eat.
• For condensed matter χ(1) is of the order of unity, and we hence
expect that χ(2) will be of the order of 1/Eat, or that
• Similarly χ(3) to be of the order of χ(1)/E2at,
• For certain purposes, it is useful to express the second- and third-
order susceptibilities in terms of fundamental physical constants.
✓As just noted, for condensed matter χ(1) is of the order of unity.
• This result can be justified either as an empirical fact or can be
justified more rigorously by noting that χ(1) is the product of atomic
number density and atomic polarizability.
• The number density N of condensed matter is of the order of
(𝑎𝑜 )−3 and the nonresonant polarizability is of the order of (𝑎𝑜 )3 . We
thus deduce that χ(1) is of the order of unity.
• Using the expression for E, we similarly find that
and χ(3)=
• The most usual procedure for describing nonlinear optical phenomena
is based on expressing the polarization ˜ P(t) in terms of the applied
electric field strength ˜ E(t),
• The reason why the polarization plays a key role in the description of
nonlinear optical phenomena is that a time-varying polarization can
act as the source of new components
of the electromagnetic field.
✓The wave equation in nonlinear optical media often has the form
where n is the usual linear refractive index and c is the speed
of light in vacuum.
• We can interpret this expression as an inhomogeneous wave equation
in which the polarization ˜ PNLassociated with the nonlinear response
acts as a source term for the electric field ˜E .
• Since
is a measure of the acceleration of the charges that constitute
the medium, this equation is consistent with Larmor’s theorem
of electromagnetism, which states that accelerated charges generate
electromagnetic radiation
• It should be noted that the power-series expansion expressed need
not necessarily converge. In such circumstances the relationship
between the material response and the applied electric field
amplitude must be expressed using different procedures.
• One such circumstance is that of strong resonant excitation of an
atomic system, in which case an appreciable fraction of the atoms can
be removed from the ground state. Saturation effects of this sort can
be described by certain procedures
• Even under nonresonant conditions, the Eq. loses its validity if the
applied laser field strength becomes comparable to the characteristic
atomic field strength Eat, because of strong photoionization that can
occur under these conditions.
• The laser intensity associated with a peak field strength of Eat is given
by
