Chapter 2

Third-Order Nonlinear Effects

2.1Introduction

The book focuses on utilizing the third-order nonlinear effects (including

nonlinear absorption and refraction) to break the diffraction limit and form super-
resolution nanoscale spot. In this chapter, let us give a brief introduction to the
characteristics of the third-order effects.
When a light beam with a frequency of is incident on the isotropic nonlinear
medium, the nonlinear effect occurs, and the second-order nonlinear susceptibility
(2) can beneglectable. The whole polarization is expressed as [1]
 
P[E()] = P(1) + P(3) = 0 (1) + 3 (3) |E()|2 E() (2.1)

where P(1) and P(3) the linear and third-order nonlinear polarization. (1) and (3)
are the linear and third-order nonlinear susceptibility, respectively. The polariza-
tions are marked into the real and imaginary parts as follows

(1) (1)
P(1) = PR + iPI
(3) (3) (3) (2.2)
P = PR + iPI

The (1) and (3) can be also marked into real and imaginary parts as follows

(1) (1)
(1) = R + iI
(3) (3) (3) (2.3)
= R + iI
(1) (3) (1)
where R and R are real part and directly related with the refraction. I and
(3)
I are imaginary parts and related with absorption.

Science Press, Beijing and Springer-Verlag Berlin Heidelberg 2015 13

J. Wei, Nonlinear Super-Resolution Nano-Optics and Applications,
Springer Series in Optical Sciences 191, DOI 10.1007/978-3-662-44488-7_2
14 2 Third-Order Nonlinear Effects

2.2Nonlinear Refraction

For isotropic (homogeneous) materials, the nonlinear refraction can be con-

sidered to be from a four-wave interaction and the third-order nonlinearity is
mainly field dependent. Accordingly, the nonlinear polarization is written as
(3)
P(3) [E()] = 30 R |E()|2 E(). Assuming that the refractive index is meas-
ured using a single laser beam method, such as single beam z-scan technique, the
four-order and higher terms can be neglectable. Then, the total polarization of the
material system is
 
(1) (3) (1) (3)
PR [E()] = PR + PR = 0 R + 3R |E()|2 E() 0 Reff E() (2.4)
(1)
where R is the real part of linear susceptibility. Here, one defines the effective
susceptibility as eff = Reff + iIeff , where the Reff and Ieff are the real and imagi-
nary parts of effective susceptibility, respectively. According to formula (2.4), the
Reff is written as

(1) (3)
Reff = R + eR |E()|2 (2.5)

with

(3) (3)
eR |E()|2 = 3R |E()|2 (2.6)

If all of the nonlinear susceptibility is thought to be effective susceptibility, one

can obtain

(3) (3)
eR |E()|2 R |E()|2 (2.7)

The electric displacement vector is

 
(1) (3)
D = 0 E + P = 0 1 + R + R |E()|2 E() (2.8)

Based on D = E, the total permittivity is

 
(1) (3)
= 0 1 + R + R |E()|2 (2.9)

The relative permittivity is

(1) (3)
r = = 1 + R + R |E()|2 (2.10)
0
The refractive index is defined as

n= r r (2.11)
2.2 Nonlinear Refraction 15

where r is relative permeability and generally equals to 1 for non-magnetic mate-

rials. Thus

n = r (2.12)
Substituting formula (2.10) into formula (2.12), one has

(1) (3)
n = 1 + R + R |E()|2 (2.13)

The linear refractive index is defined as

(1)
n02 = 1 + R (2.14)

Thus, formula (2.13) is rewritten as

 1
(3)
|E()|2 2
n = n0 1+ R 2 (2.15)
n0

Generally, the R(3) |E()|2 /n02 term is much smaller than 1. Using the Taylor series
expansion, the formula (2.15) can be expressed as
(3)
R
n n0 + |E()|2 (2.16)
2n0

Generally, the refractive index can also be written as

n = n0 + n = n0 + I (2.17)
where n is the third-order nonlinear susceptibility-induced refractive index
change and is nonlinear refraction coefficient. I is light intensity and can be
defined as
vr 0
I= E(, t)2 (2.18)
2
where v = c/n0 is light speed in the medium. E(, t) is time-dependent optical
field, and r n02, thus
1
I 0 cn0 E(, t)2 (2.19)
2
If the optical field is of the form [2]
E(, t) = E() exp (it) + c.c., (2.20)
one has

E(, t)2 = 2E()E () = 2|E()|2 (2.21)

According to formulas (2.19) and (2.21), one has

16 2 Third-Order Nonlinear Effects

Table2.1Typical values of and response time for linearly polarized light [2]
Mechanism (m2 /W ) Response time (s)
Electronic polarization 1020 1015
Molecular orientation 1018 1012
Electrostriction 1018 109
Saturated atomic absorption 1014 108
Thermal effects 1010 103
Photorefractive effectsa Large Intensity
dependent
a The photorefractive effect can cause large nonlinear effect, which cannot usually be described
with nonlinear susceptibility (3) (or ). The nonlinear polarization process of the photorefractive
effect is not the same as the other physical mechanisms listed

1
|E()|2 = I (2.22)
0 cn0
Substituting formula (2.22) into formula (2.16), one obtains
(3)
R
n n0 + I (2.23)
20 cn02

Based on formulas (2.17) and (2.23), the nonlinear refraction coefficient is written as
(3)
R
= (2.24)
20 cn02

According to formula (2.24), one can obtain value. The different physical mecha-
nisms can cause different values. The typical value andresponse time are listed in
Table 2.1. In formula (2.24), < 0 corresponds to self-defocusing effect and > 0
can lead to self-focusing effect. The self-focusing effect can generate the nanoscale
spot, which is very useful for nanolithography and high-resolving light imaging, etc.

2.3Nonlinear Absorption

Similar to the real part of polarization, the imaginary part of polarization is

 
(1) (3) (1) (3)
PI [E()] = PI + PI = i0 I + I |E()|2 E() (2.25)

For isotropic medium, on the basis of the slowly varying-envelope approximation,

one has
dE i
= PI (2.26)
dz 20 cn0
Substituting formulas (2.22) and (2.25) into formula (2.26), one has
2.3 Nonlinear Absorption 17

 
dE (1) (3)
= + I E (2.27)
dz 2cn0 I 20 c2 n02 I

One defines the following

0 (1) (3)
= + = + I I (2.28)
2 2 2 2cn0 I 2 2
20 c n0

From the formula (2.28), the formula (2.27) is rewritten as

dE
= E (2.29)
dz 2
So
 
E(L) = E0 exp L (2.30)
2
where L is medium thickness. The intensity decaying accordingly is
I(L) = I0 eL (2.31)
Thus,
(1)

0 = cn0 I
= (3)
I (2.32)
0 c2 n02 I

Thus, 0 is defined as linear absorption coefficient, and is nonlinearity-induced

intensity-dependent absorption coefficient change and is
= I (2.33)
where is nonlinear absorption coefficient and is
(3)
= (2.34)
0 c2 n02 I

For some materials, such as semiconductors, < 0 is saturation absorption, and

> 0 means reverse saturation absorption or multi-photon absorption.
As described in formula (2.31), the light goes through the nonlinear materials,
and the intensity changes with the traveling distance z inside the materials. The
intensity decaying process can be rewritten as
I
= 0 I I 2 (2.35)
z
The exiting light intensity from the materials is [3]
I0 exp(0 L)
Ie = (2.36)
1 + I0 Leff
18 2 Third-Order Nonlinear Effects

with
1 exp(0 L)
Leff =
0
For 0 0, the linear absorption of materials is neglectable, and the third-order
nonlinear absorption is dominant. In this case, exp (0 L) (1 0 L), thus
Leff L. Based on formula (2.36), the exiting light intensity becomes
I0
Ie (2.38)
1 + I0 L
An alternative way to obtain the exiting light intensity is through the formula
(2.35) with 0 = 0, which yields
I
= I 2 (2.39)
z
Formula (2.38) can be solved by the separation of variables, which yields
I0
I(z) = (2.40)
1 + I0 z
Formula (2.40) is consistent with formula (2.38) and can be used to calculate the
light spot intensity profile after passing through the nonlinear absorption materials
with weak linear absorption characteristics (0 0).
The nonlinear refraction can induce self-focusing super-resolution effect (for
> 0), and the nonlinear absorption can lead to the generation of aperture-type
super-resolution effect (for < 0), or subwavelength energy absorption region
(for > 0), which can be applied to the nanolithography and nanoscale optical
data storage, etc.

References

1. D. L. Mills, Nonlinear OpticsBasic Concepts, (Springer, Berlin, 1998)

2. R. W. Boyd, Nonlinear Optics, Academic (2003)
3. M. Sheik-Bahae, A. A. Said, T. H. Wei, D. J. Hagan, E.W. Van Stryland, Sensitive measurement
of optical nonlinearities using a single beam. IEEE J. Quantum Electron. 26, 760769 (1990)
http://www.springer.com/978-3-662-44487-0