Chapter 1

INTRODUCTION

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General aspects in nonlinear optics and photonic crystals are presented in this
chapter. A brief overview on the nonlinear optical processes and associated
phenomena, with relevant theory is presented in the first section. The second
section includes details regarding the photonic crystal theory, different types of
photonic crystals and their use in device applications. Transfer matrix formalism
for multilayer structures with an emphasis on application to one dimensional
photonic crystals is also conferred. A literature review on the present work is
included in the end section of this chapter.

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1.1 MOTIVATION

For the last few decades, tremendous research effort has been invested for finding
new materials or methods to realize all-optical signal processing with an ultimate
aim of an efficient, ultrafast communication system. To make information
processing fully in the optical domain, one has to make use of optical
nonlinearities where control of light with light itself is possible. But, in most of
the cases, such nonlinearities are very weak and thus need high operational power.
The problem can be overcome either by finding a material which can show strong
nonlinear optical (NLO) response or by using a structure that can optimize the
nonlinear optical properties of a material. The second method is more efficient
than the former since it is difficult to find NLO materials having instantaneous
response and fast recovery time [1,2]. Photonic crystals (PCs) are found to be very
suitable for this purpose because of their unique features.

1
Photonic crystals are artificially engineered structures, in which two or more
different dielectric materials are arranged in a periodic manner. Due to this
structural periodicity, they exhibit photonic band gap (PBG) – a range of
frequencies for which light propagation is prevented through the crystal [3,4].
Based on the number of directions along which the periodicity can be extended,
PCs are classified as one, two, and three dimensional (1D, 2D and 3D) structures.
Compared to 2D and 3D structures, 1D PCs are easy to fabricate and are thus very
attractive for practical applications. Currently, immense research is going on in the
field of nonlinear optics using 1D PBG structures, and most of the works are
based on theoretical modeling. There is a lot of research scope in the experimental
field when the flexibility in structural engineering of 1D PCs together with the
availability of diverse range of NLO materials are considered. In this work, we
investigate the NLO response of certain porphyrin systems by means of different
1D PC structures.

1.2 NONLINEAR OPTICS

Interaction of highly intense optical field with matter is referred to as nonlinear

optics and here, the polarization of a material system responds in a nonlinear
manner to the electric field of optical radiation. Typically, at low light intensities,
the material properties are found to be independent of the applied input field
intensity. On the other hand, an intense optical field can cause significant
disturbances to the coulomb field of an atom in a material and thus can alter its
properties. Laser sources are needed for this purpose, since they can produce
adequately high radiation intensities to evoke optical nonlinearities even in weak
NLO materials. The first experimental demonstration in nonlinear optics was
happened only after the invention of ruby laser and was in 1961 by Franken and
co-workers when they detected second harmonic generation in quartz crystals [5].
In 1962, Bloembergen [Link] investigated three-wave mixing and four-wave mixing
processes and developed a theoretical framework for treating NLO processes [6].
In the consecutive years, a general scheme for the quantum mechanical
calculation of complex nonlinear susceptibilities was formulated [7]. Thereafter,

2
an enormous growth in the field of nonlinear optics was marked with the
discovery of numerous NLO phenomena such as optical frequency conversion,
self focusing, phase conjugation, stimulated Raman scattering, optical bistability
etc. This field has now become an area of active research with research activities
ranging from the fundamental physics of light-matter interaction to the
technological interest for applications in optical communication systems,
medicine and biotechnology [8].

1.2.1 Basics of nonlinear light-matter interaction

When an electromagnetic wave having frequency ω, is allowed to interact with a

material medium, the atoms or molecules in it start to oscillate in accordance the
electric field of the optical wave. As a result, displacement of electric charges
occurs and thus induced dipole moments are created. The total average dipole
moment per unit volume is considered as the induced electric polarization of the
medium. With small exciting optical intensities, dipole oscillations are nearly
simple harmonic and in this case, a linear relationship exists between the induced
polarization, P and the applied electric field strength, E. To simplify the analysis,
P and E are considered as scalars. The relation can be written as,

P  0 E
(1.1)
where,  0 is the permittivity of free space and χ is linear susceptibility of the

material.

When the excitation field is strong enough, the polarization of the medium, no
longer holds linearity with the applied field. Instead, higher order electric field
dependent terms [9] come into play and in this case, polarization can be expressed
as a power series given by,

P   0   (1) E   (2) E 2   (3) E 3  ................ (1.2)

where χ(1) is termed as linear or first-order susceptibility, χ(2) - second-order

susceptibility, χ(3) - third-order optical susceptibility and so on. In general χ(n) is a
tensor of rank n+1. The magnitude of optical nonlinearity in a material thus

3
depends on the nonlinear susceptibility coefficients and the applied light field
intensity.

Consider an electromagnetic field represented by E  E0 cos t is interacting with

an NLO medium; then the equation (1.2) takes the form [10],

1  3  1
P   0  (2) E02   0   (1)   (3) E02  E0 cos t   0  (2) E02 cos 2t
2  4  2
1
  0  (3) E03 cos 3t  ... (1.3)
4

Equation (1.3) depicts all the typical phenomena associated with lower order
susceptibilities. The first term in the expression corresponds to the phenomenon of
optical rectification and the second term is the fundamental harmonic of
polarization. The second harmonic and third harmonic generation processes are
represented by the third and fourth term respectively.

In a more generalized form, equation (1.2) can be written as

P  P L  P NL (1.4)

Here, PL and PNL are the linear and nonlinear polarization terms. The nonlinear
polarizations act as the source terms in the nonlinear optical wave equation [11]
given by,
 r 2E 1  2 P NL
 2 E   (1.5)
c 2 t 2  0c 2 t 2

Based on this equation, the processes arising from nonlinear-light matter

interaction can be well described.

1.2.2. Second Order Optical Nonlinearity

The second order susceptibility, χ(2) describes how the polarization changes in the
presence of two interacting fields. It is a third-rank tensor with twenty seven
components and is responsible for second order nonlinear processes that include
sum and difference frequency generation, second-harmonic generation (SHG),
optical parametric amplification and oscillation [12]. For materials possessing

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inversion symmetry, χ(2) becomes zero and in this case, second-order NLO
processes are not possible.

Sum and Difference Frequency generation: Here, two photons having different
frequencies and combine to generate a third photon of frequency . For
sum frequency generation, becomes and the polarization is given by
the equation
P(1 2 )   0  (2) E1E2 (1.6)

Whereas in the process of difference frequency generation, becomes equal to

and the polarization expression in this case is

P(1 2 )   0  (2) E1E2 (1.7)

The processes of sum and difference frequency generation are very useful not only
in generating specific frequencies at new wavelengths but also in generating new
tunable frequencies at new wavelengths in laser systems [13,14].

Second Harmonic generation: The second harmonic generation (SHG) is

considered as the degenerate case of sum frequency generation. Here, two
photons having the same frequency interact with a nonlinear medium and create a
third photon with frequency twice than that of the initial photons. The polarization
equation for SHG can be expressed as

P(2 )   0  (2) E 2 (1.8)

SHG finds applications in laser technology, bio-sensors, imaging microscopy etc

[15,16].

Optical Parametric Amplification and Oscillation: Optical parametric

amplification can be related to the difference frequency generation with a process
of energy transfer from a high intensity beam, known as pump beam having
frequency, say to a lower intensity beam, known as signal beam with
frequency, say within a nonlinear medium. As a result, the signal wave gets
amplified and a third beam, known as idler beam at the frequency, say gets
created in order to meet the energy conservation criteria. With the help of an

5
optical resonator, Suitable feedback to the newly generated beam can be provided
and consequently, the intensity at builds up in the cavity, which in turn
increases the intensity at . This process continues and is thus termed as optical
parametric oscillation [17].

1.2.3. Third Order Optical Nonlinearity

Third order nonlinear optical processes cover a wide and diverse area in nonlinear
optics. They are characterized by means of the third order susceptibility, χ(3)
which is a fourth rank tensor with 81 components. The polarization equation in
this case, is given by,

P(4 )   0  (3) E (1 ) E (2 ) E (3 ) (1.9)

As can be seen, the induced nonlinear polarization is the result of the frequency
mixing process of three interacting fields. Third order nonlinearities mainly
include phenomena such as third harmonic generation (THG), nonlinear refraction
and nonlinear absorption [11]. The real part of χ(3) is directly linked to nonlinear
refraction whereas its imaginary part is responsible for nonlinear absorption.

Third Harmonic Generation: In THG, all the three interacting fields are of the
same frequency, ω and the resultant field will have frequency, 3ω, known as third
harmonic [18]. The process can represented as

P(3 )   0  (3) E 3 ( ) (1.10)

In practice, third harmonic is achieved by adding second harmonic with the

fundamental frequency, since the probability of getting third harmonic from a
three-photon reaction is much weaker than that for a two-photon process.

Nonlinear Refraction: With third order optical nonlinearity, the refractive index
of a material becomes intensity dependent and the change in refractive index is
proportional to the incident intensity. This process is referred to as optical Kerr
effect and the refractive index of the medium is given by,

n  n0  n2 I (r , t ) (1.11)

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Where is the linear refractive index, is the nonlinear refractive index
coefficient which can be either positive or negative and I(r,t) is the input intensity.
The spatial part I(r) results self focusing and the temporal part I(t) give rise to self
phase modulation.

Consider the propagation of a Gaussian profiled beam through a nonlinear

material. As the beam passes, refractive index changes are induced in the material
in such a way that the refractive index becomes larger at the center of the
Gaussian beam than its periphery. As a result, the material acts as a positive lens,
making the beam to focus within the material. This phenomenon is known as self
focusing effect. In this case, the value of will be positive. On the other hand,
if , the system will behave as a negative lens and thus try to diverge the
beam [19]. Nonlinear refraction (NLR) can also impose a phase modulation in the
beam, causing changes in its frequency spectrum and this phenomenon is known
as self phase modulation.

Nonlinear Absorption: Transmission properties of a material can be changed

considerably when the medium is exposed to high intensity illumination and this
is referred to as nonlinear absorption (NLA). Simultaneous multiphoton
absorption or cumulative multi step absorption can happen with high intensity
radiation and consequently, the optical transmittance of the material can either be
increased or decreased due to NLA. The major mechanisms of NLA are discussed
below.

Two-Photon Absorption

In the two-photon absorption (TPA) process, two photons get simultaneously

absorbed by the material system by means of an intermediate virtual state. When
an intense beam propagates through a nonlinear medium supporting TPA, the
variations in the beam intensity is given by,
dI
   0 I  I 2 (1.12)
dz

where β is known as the two-photon absorption coefficient and z is the

propagation distance in the material media. In general, for a multi-photon

7
absorption process where the simultaneous absorption of n photons ( ) takes
place, the nonlinear propagation equation can be written as [20,21]

dI
dz

   0  ( n 1) I n I  (1.13)

where is the (n+1)th photon absorption coefficient.

If the linear absorption of the system is negligibly small, the second term (TPA) in
the equation (1.12) dominates, and propagation equation now becomes,

dI
  I 2 (1.14)
dz
With I0 being the input light intensity, the above equation yields the solution given
by,
I0
Iz  (1.15)
1  I 0 z

Saturable Absorption

Materials exhibiting strong electronic absorption can favour saturable absorption

(SA) if the rate of populating the excited state becomes greater than that of the
ground state. In this process, the optical transmittance of the material increases
significantly, upon increasing the incident light intensity.
Consider a two-level system in which N1 and N2 are the ground state and excited
state population respectively, and σ is the absorption cross section. Under
equilibrium condition, for the incident intensity I,

dN 2  I N
  N1  N2   2  0 (1.16)
dt h 

where is the excited state life time and is the incident photon energy. The
linear absorption coefficient, α is related to N1 and N2 as, α = σ (N1-N2).
Considering the ground state linear absorption as, α0 = σN1, the intensity-
dependent linear absorption coefficient can be written as

1 1
  I   0  0 (1.17)
 I I
1 1
h Is

8
where Is=hυ/τσ is known as the saturation intensity, at which α(I) reduces to half
of α0 [22,23]. Saturable absorbers find applications in Q-switching, mode-locking
and pulse compression. When a saturable absorber is used in combination with an
optical limiter, temporally compressed and symmetrically shaped pulse can be
produced [24].

Reverse Saturable Absorption

When a material system having multiple energy levels is irradiated with a high
intense light, the atoms/molecules which are initially got excited to the first
excited state, can move to subsequent higher energy levels with the absorption of
more number of photons. This excited state absorption (ESA) can cause
substantial drop in the light transmittance through the material and the
phenomenon is designated as reverse saturable absorption (RSA).

Fig.1.1 Energy level description of RSA

Unlike TPA, ESA is a sequential two-photon absorption process involving real

intermediate levels with finite life times [25,26]. The process is schematically
shown in Fig.1.1 in which Ng is the ground state population, N1 and N2 represent
population in the two excited states and σg1, σ12 are the absorption cross sections
corresponding to the transitions from ground to first excited state and that from
first excited to second excited state respectively. With the assumption that
Ng>>N1, the propagation equation in this process take the form,

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 dI
  0 I   ' I 2 (1.18)
dz

Where, α0 = and β’ = , with b, being a constant. The equation

(1.18) is analogous to the equation for two-photon absorption and hence similar
formalism can be applied in solving the equation for obtaining the relevant
parameters.

1.2.4. Optical Limiting

Reduction in optical transmission at higher input fluences is often referred to as

optical limiting (OL) and is considered as a characteristic behaviour exhibited by
most of the NLO materials. The scope of optical limiters lies in the diversity of
applications ranging from the protection of human eye and optically sensitive
components from high intense radiation, to all-optical switching [27-29]. The
performance of an optical limiter is often determined by its limiting threshold,
value at which the optical transmittance drops to half of the linear transmittance.
The lower the threshold value, the better will be the limiting action. Besides low
limiting threshold, the other characteristics of a good optical limiter are high
optical damage threshold, broadband response and fast response time. Typically,
there are different mechanisms that promote OL action in a material media and
they include RSA, TPA, nonlinear scattering, free carrier absorption etc [30].
Optical limiters that make use of NLO materials is often referred to as passive
optical limiters in which OL action is a part of their physical characteristics and
thus, due to their inherent properties, passive optical limiters are fast and less
complex [31].

1.3. PHOTONIC CRYSTALS

Photonic crystals are artificially structured dielectric media, capable of

manipulating the flow of light by means of a periodically modulated refractive
index profile. This spatial periodicity creates forbidden energy regions in the
photon dispersion relation, preventing propagation of photons with frequencies
falling in this range, through the crystal. The forbidden frequency range is then

10
referred to as photonic bandgap, in analogous to the bandgap in semiconductors.
Thus PCs influence the flow of light in a similar way as semiconductors control
the flow of electrons and due to this reason, PCs are sometimes called
‘semiconductors of light’. PBG appears whenever there is a difference in
dielectric constants of the materials constituting the PC. The smaller the contrast
in dielectric constants, the smaller is the gap. In general, PBGs are polarization-
dependent and a complete PBG is one which prevents the propagation of
electromagnetic waves irrespective of their polarization and direction of travelling
through the crystal for some frequency range [32].

PBG structures exist in nature in the form of structural coloration and the
examples include peacock feather, butterfly wings, opals, beetle shells etc. The
glittering colours of these are not due to pigmentation, instead due to light
interaction with the structural pattern seen on their exoskeletons [33,34]. In 1887,
Lord Rayleigh investigated the properties of periodic multilayers using
electromagnetic theory and predicted the reason behind the iridescent colors
exhibited by butterfly wings and beetle shells [35]. Almost hundred years later, in
1987, Eli Yablonovitch and Sajeev John in an independent work [36,37],
predicted the properties of high dimensional periodic optical structures which are
now known as photonic crystals and the periodic multilayer structures are now
termed as one dimensional photonic crystals.

1.3.1 Basic theory of photonic crystals

The light propagation through photonic crystals can be well described by using
Maxwell’s equations in material media [32]. Assuming no free charges or current
in the dielectric materials constituting the photonic crystal, Maxwell equations
becomes,

B
E   (1.19)
t
D  0 (1.20)
D
H  (1.21)
t

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 B  0 (1.22)
where E and H are the electric and magnetic fields respectively, D is the electric
displacement field and B is the magnetic induction field. The parameters D and E
are related as,

D(r, t )   0 (r) E(r, t ) (1.23)

where is the vacuum permittivity and (r) is the spatially dependent dielectric
constant also called relative permittivity. In the case of photonic crystal, the
dielectric constant (r) becomes a periodic function and takes the form
 (r)   (r  R) (1.24)
where R is the lattice vector of the photonic crystal.
Assuming unit relative magnetic permeability for dielectric materials, B and H are
related through the vacuum permeability 0 as,

B(r, t )  0 H(r, t ) (1.25)

Consider an incident electromagnetic field for which electric and magnetic fields
are represented as follows:

E(r, t )  E(r)eit (1.26)

H(r, t )  H(r)eit (1.27)

Using equations (1.23), (1.25), (1.26) and (1.27), the Maxwell’s equations (1.19-
1.22) becomes modified as,
  H(r)  0 (1.28)

 E(r)  i0 H(r) (1.29)

 
   (r ) E(r )   0 (1.30)
 

 H(r)  i 0 (r) E(r) (1.31)

Substituting for E(r) from (1.31) into (1.29) and using c  0 0 , we can get,

 1   
2

   H(r)     H(r) (1.32)

  (r )  c

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This equation is considered as the ‘master equation’ [32] since it delivers all the
details regarding the propagation of an electromagnetic wave in a photonic
crystal. Now, by putting
 1 
H(r )     H(r )  , (1.33)
  (r ) 

the master equation can be represented in the form of an eigenvalue equation in

quantum mechanics as

 
2

H(r )    H(r ) (1.34)

c
where is considered an operator acting on H(r). As can be seen, the equation
(1.34) looks similar to the Schrödinger equation describing the electron
propagation through a semiconductor crystal

 p2 
  V (r )  (r)  E (r) (1.35)
 2m 
where p is momentum of the electron, m is the mass of the electron, E is the
energy value and is the wave function for the electron. The term V(r) is the
periodic potential formed by the periodic arrangement of atoms, which takes the
form, V(r) =V(r+R) and is responsible for the bandgap formation in
semiconductor crystals. Since the equation (1.34) is in resemblance with the
Schrödinger equation (1.35), similar type of solutions can be assumed for equation
(1.34). Due to the presence of periodic dielectric function (r), the solutions to the
master equation yields a photonic band structure depicting allowed and forbidden
energy states for photons and the forbidden energy range is termed as the PBG.

Characterization of photonic bandgap: In general, the PBG properties are

determined by means of dispersion diagram and/or transmittance/reflectance
spectrum. The master equation is solved for obtaining all possible energy
eigenvalues and when these values are plotted against wavevector, k, dispersion
diagram can be obtained. For each value of k, a series of optical modes with a
discrete set of eigenfrequencies exist and this forms the pass band for a PC. The
frequency range between two adjacent pass bands, where no eigenmodes exist, is
considered as the PBG [38]. PBG can also be characterized using transmittance

13
spectrum of the PC, where the PBG appears as a deep dip in the spectrum.
Assuming no intrinsic absorption for materials constituting the PC, the
transmittance value for the frequency range in the PBG can fall to zero with 100%
transmittance for the pass bands. PBG appear as a pronounced peak in the
reflectance spectra, with 100% reflection for frequencies within the PBG. In this
ideal case, pass band frequencies approach to zero reflectance value.

1.3.2 Types of Photonic Crystals

Fig.1.2. Schematic of 1D, 2D and 3D photonic crystals

(Image courtesy: Ref. 32)

Depending on the spatial periodicity that can be extended along one or more
principal axes, PCs are categorized as one, two, and three dimensional structures
as shown in Fig.1.2. A one-dimensional photonic crystal is a multilayer structure
that can be formed by the periodic stacking of materials having different refractive
indices, over one another. An example for this includes Bragg grating. Two
dimensional photonic crystals are those in which the periodicity extends in two
dimensions. They can be fabricated by drilling holes in a suitable substrate and
often triangular/square lattices of holes are employed. Photonic crystal fibers
belong to this category. Three dimensional photonic crystals can have full control
over light signals due to the periodicity in all the three axes. Various geometries
are possible for 3D PCs (Fig.1.3) and some of which as discussed below [39-42].

Yablonovite: This structure constitutes a dielectric medium in which cylindrical

holes drilled along the lattice vectors of an FCC lattice. It is considered as the first

14
experimentally demonstrated 3D photonic crystal with a complete photonic band
gap.

The Woodpile Structure: It consists of a number of dielectric rods that are stacked
in alternating orthogonal orientations. They can be fabricated by deposing and
patterning a sequence of layers using lithographic techniques.

Inverse Opals: it consists of an FCC lattice of air holes in a dielectric background

and this inverse structure can have a complete photonic bandgap when FCC lattice
of dielectric spheres in air is considered. They can be realized by the method of
colloidal self assembly.

Fig.1.3. Different structures of 3D photonic crystals

(Image courtesy: Ref. 4 & Ref. 32)

1.3.3. Defects in Photonic Crystals

As in the case of ordinary crystals, defects can be introduced in PCs. The presence
of defects violates the symmetry of the crystal and as a result, new allowed photon
modes are created within the band gap. Defects can mainly be of two types- point
defects and line defects (Fig. 1.4). Point defects also referred to as cavity defects
are of paramount importance in the light localization process. Any kind of
imperfection in the actual PC structure such as, removal of one of the building
blocks, modification in its refractive index or dimensions etc constitutes a point
defect[43,44]. The point defect can act as a resonating cavity, in which any light
inside the defect gets trapped. Line defect is considered as the set of consecutive

15
point defects along a line. Line defects within a PBG structure enable
waveguiding through the crystal for photons of frequencies lying within the band
gap[45,46]. The advantage of PC waveguides over conventional waveguiding
systems is that in the former case, photon confinement does not rely on index-
guiding (total internal reflection) and hence transmission losses are negligible.

Fig.1.4. Defects in photonic crystals

(Image courtesy: Ref. 32)

1.3.4 Applications of Photonic Crystals

Owing to their peculiar characteristics, PCs find numerous potential applications

in various fields. 1D PCs are used for applications in thin-film optics which
include high reflection dielectric mirrors, optical filters, distributed feedback
lasers, sensors, optical diodes, optical switches etc [47-56]. Some of the possible
applications of 2D PCs include photonic crystal fibers, waveguides, super-lens
[57,58]etc. Due to the ability for light confinement in hollow cores, photonic-
crystal fibers are used in optical communication systems, high-power transmission
area, fiber lasers, nonlinear optical devices etc. PCs can be designed to achieve
super-lenses via all-angle negative refraction. The main advantage of super lenses
is that the diffraction limit present in conventional lenses can be effectively
overcome in super lenses. Due to the complexity in the fabrication process and
difficulties in making strict control over the disorders, waveguiding and light
localization in 3D PCs has not much developed as in 2D. If these major hurdles
can be overcome, 3D structures will be potentially useful in novel photonic

16
circuits. They exhibit features for realizing optical transistors which are expected
to bring revolution in the field of integrated optics. Super prism effects, self
guiding, negative refraction etc are the phenomenon, demonstrated using 3D
photonic crystals, aiming at applications mainly in telecommunication area[59].

In this research work, one dimensional photonic crystal structures are utilized in
investigating enhanced optical nonlinearities for NLO applications.

1.4 THEORY OF 1D PHOTONIC CRYSTALS: TRANSFER MATRIX

METHOD

1D PCs exhibit the configuration of a multilayer stack of different dielectric

materials arranged in a periodic manner so that the dielectric function in this case
follows the relation [60]

 ( x, y, z)   ( x, y, z  m) (1.36)

where m is an integer and is the period. Here, is assumed to be

periodic along the z direction (direction perpendicular to the plane of the layers)
and uniform in the other two directions. The commonly used form of a 1D PC is a
periodic multilayer composed of two types of layers with dielectric constants
and . In this case, the PBG emerges in accordance with the contrast in the
dielectric constants of the materials. When an electromagnetic wave having
wavelength , enters into such a structure, it undergoes partial reflection,
refraction and transmission at the interfaces of the dielectric layers. The partially
reflected (transmitted) waves can then interfere constructively (destructively) at
some specific wavelength , according to the lattice spacing and refractive indices
of the layer materials and this defines the spectral region of the PBG [51]. The
situation is analogous to X-ray Bragg reflections at different crystal planes and
therefore 1D PCs are sometimes referred to as dielectric Bragg reflectors (DBR)
or simply Bragg mirrors.

The optical response of 1D PCs can be well described using transfer matrix
method (TMM) [61,62]. Here, the propagation of an electromagnetic wave at each
interface is characterized by a 2Х2 matrix and the as obtained each matrix is then

17
multiplied in a sequential order to form a single characteristic matrix for the entire
multilayer system. In this thesis work, theoretical modeling on the reflectance and
transmittance of 1D PC structures are accomplished using TMM which is
described below.

1.4.1 Transfer matrix formalism

Fig.1.5. A dielectric multilayer system

Consider the multilayer configuration as shown in Fig.1.5. Let the multilayer be

composed of ‘N’ number of layers in which di and ni represent the ith layer (where
i=1, 2,…,N) thickness and refractive index respectively. The z-axis is taken as
normal to the plane of the multilayer structure and the propagation of the
electromagnetic wave is assumed to be in the xz-plane.

Now, the electric field in each layer can be represented as,

E j (r)  [ E j  eikz z  E j eikz z ]ei ( kx x t ) (1.37)

where and are the components of wave vector along x and z axes
respectively and and represent the amplitudes of the forward and
backward travelling waves.

At the interface between the ith and jth layers, the tangential components of electric
and magnetic fields of the plane wave is continuous. Applying these boundary

18
conditions, the electric field amplitudes in the ith and jth layers, ie., and
can be conveniently related with the help of matrices as

Ei  M ij E j (1.38)

E   E j 
Where Ei   i   , E j    (1.39)
 Ei    E j 

and is a 2Х2 matrix, called the boundary matrix for the interface between ith
and jth layers.

In terms of reflection and transmission coefficients, takes the form,

1 1 rij 
M ij  r 1 
(1.40)
tij  ij
Depending on the polarization of the electromagnetic field, the elements of M ij

can be expressed as,

ni cos i  n j cos  j 2ni cos i
for s-polarization rij , s  , tij , s  (1.41)
ni cos i  n j cos  j ni cos i  n j cos  j

n j cos i  ni cos  j 2ni cos i

for p-polarization rij , p  , tij , p  (1.42)
ni cos  j  n j cos i ni cos  j  n j cos i

where and are the refraction angles in the ith and jth layer respectively. Thus,
boundary matrix tells what happens to the electromagnetic wave at different
interfaces when it travels though a multilayer media.

Between each interfaces, the phase of the wave changes during its transmission
and this phase change can be characterized by means of propagation matrices.

The electric field propagation in the ith layer can be expressed using propagation
matrix  i as

Ei ( zi  di )  i Ei ( zi ) (1.43)

19
The propagation matrix is given by
ei 0 
i    (1.44)
0 ei 

 
where   1 2 ni di cos  .

Now, the transfer matrix of the entire multilayer system can be calculated by the
multiplication of boundary and propagation matrices in a sequential order as given
below
TN  M N , N 1 N 1M N 1, N 2 N 2 ...2 M 21 (1.45)

The transfer matrix TN contains all the information regarding the propagation of an

optical wave through a multilayer media. The field amplitudes in the first and the
Nth layer can thus be related as,

 EN   T11 T12   E1 

 0   T T   E  (1.46)
   21 22   1 

where E1 , E1 and EN  are the incident, reflected and transmitted waves. The total

reflection and transmission coefficients then become,

E1 T E det(T )
r   21 and t  n   (1.47)
E1 T22 E1 T22
The reflectance and transmittance through the multilayer sample can be calculated
using the relation,

R  r and T  t .
2 2
(1.48)

1D PCs can be considered as a special case of the multilayer system considered

above, in which two different materials are arranged N-times in a repeating
manner (ie., the total number of layers in this case, is an even integer). For the 1D
PC configuration air/(high index layer/low index layer)2N/substrate where optical
thickness of each high index and low index layers are optimized as λ/4, all the
partially reflected beams emerging from the structure, will be in phase and
consequently reflectance will get enhanced. The reflectance and transmittance can

20
be calculated by solving transfer matrix (1.45) and the calculation become much
simpler in this case. At normal incidence, for a quarter wave stack, reflectance
becomes maximum at ‘λ’, according to the relation [63],
2
 (n n )(n n ) 2 N  1 
Rmax   0 s L H 2N  (1.48)
 (n0 ns )(nL nH )  1 

where nL and nH represent the refractive indices of the low index and high index
layers respectively.

1.5 A BRIEF REVIEW ON EARLIER WORK

The research on photonic crystals started in the late 1980s when Eli Yablonovitch
and Sajeev John popularized the concept of photonic band gap (PBG) structures
[36,37]. This concept led to a stunning growth in the research field of optics.
Photonic crystals have attained considerable attention of researchers in both
experimental as well as theoretical sciences, because of the large variety of
structures that can be tailored using PCs.

Much of the initial works in the field of PCs is focused on one dimensional PBG
structures, since they are simply multilayer systems and are easy to fabricate. In
the early 1990s, most of research works were based on the mechanism of photonic
bandgap formation, localized state of photons, optical nonlinearity in photonic
crystals etc [38,64,65]. The analysis of a more general class of nonlinear photonic
crystals began with a paper by Scalora et al. in 1994 [65]. Concept of all-optical
switching using photonic crystals was discussed in the paper and third order
nonlinearities were identified as the essential basis for all-optical switching
devices. In 1997, Toshiaki Hattori et al. studied theoretically the enhancement of
optical nonlinearity using one dimensional photonic crystal structures having
defect states [66]. They considered quarter wave stacks of silica and titania as the
model structure and introduced a defect layer of an NLO material in this basic
multilayer structure. They theoretically calculated the enhancement in the
absorption saturation and four wave mixing efficiency of the defective multilayer
in comparison with a simple monolayer nonlinear optical film and they predicted

21
the possibility of optical bistability in purely absorptive NLO materials. The
propagation of ultra short laser pulses in linear as well as nonlinear PBG structures
was theoretically investigated by Koroteev et al in 1999 [67]. It was demonstrated
that photonic crystals incorporated with optical nonlinearity provided an efficient
way to achieve laser pulse compression on a sub-millimeter spatial scale.

In the final stage of 1990s, significant efforts were made towards the development
of various techniques for photonic crystal fabrication. The traditional methods to
fabricate 1D PCs were by means of molecular beam epitaxy, chemical vapour
deposition, pulsed laser deposition, sputtering technique etc which are highly
expensive [68]. These techniques follow complex procedures and are highly time-
consuming. In the earlier research, inorganic dielectric materials, such as SiO 2,
TiO2 and Al2O3 were extensively used for making the periodic structures because
of their high refractive index contrast. Fabrication of a one dimensional photonic
crystal consisting of TiO2 and Al2O3 layers using UHV RF magnetron sputtering
system ,was presented in a paper authored by Kim et al. and a complete photonic
bandgap was achieved [69].

In the early years of 21st century, the research was centered on the fabrication of
high quality PBG structures, studies on the physical processes within photonic
crystals and the realization of photonic devices using photonic crystals, and the
trend continues. The methods such as dip coating, spin coating etc have been
developed for the fabrication of multilayer structures. These methods are less
expensive and make the fabrication process simpler. Another advantage is that
with these techniques, 1D PCs can be prepared using inorganic as well as organic
materials. Using the sol-gel technology and dip coating method, Ewa Gondek, and
Pawel Karasinski fabricated 1D PC consisting of silica and titania layers and
achieved a reflectance of 96.7% for five bilayers[70].

With the advancement in fabrication process, 1D photonic crystals have then been
started to use with optical nonlinearity for optical device applications. Currently
there are many research groups working in this field and several exciting results
have been reported. Hideto Shirai et al. demonstrated the terahertz emission and
detection using a 1D photonic crystal microcavity embedded with a

22
semiconductor material. The efficiencies of THz emission and detection were
found to be enhanced and ultrafast switching effects were observed [71]. Sangbum
Kim et al. reported efficient second harmonic generation in 1D photonic crystals
composed of GaAs and AlAs using quadratic optical nonlinearity [72]. Vincenti et
al. investigated the NLO properties of 1D PC with a Graphene based defect and
observed that the third harmonic signal obtained using the modified periodic
structure was nearly five orders of magnitude larger than the signal produced by
free standing Graphene [73]. Valligatla et al. reported optical field enhanced
nonlinear optical absorption and optical limiting properties of a 1D photonic
crystal having ZnO as defect material, fabricated by RF sputtering technique and
4-fold increment in the nonlinear optical absorption coefficient, relative to the
single layer ZnO film is achieved [74]. Liao et al. demonstrated enhancement in
the nonlinear optical absorption coefficient and nonlinear refractive index of
Colloidal CdSe/ZnS core/shell nanocrystals by means of the band-edge shift
mechanism in a nonlinear 1D PC in which the nanocrystals are embedded in
alternate layers [75].

Recently, organic polymeric materials have attained considerable attention of

researchers, because they are advantageous over conventional inorganic materials
in many ways. Polymers offer easier processing, flexibility and better resistance to
chemical attack. They can be easily transferred into thin film by low cost coating
methods such as spin coating, dip coating etc. This is possible because of their
lower thermal properties that include glass transition and melting temperatures
which open up lower temperature processing windows[76]. Spin casted multilayer
using poly(vinyl Carbazole) (PVK) and poly(vinyl alcohol) was successfully
fabricated by Alvarez et al. in 2003 and a photonic bandgap at 532 nm was
obtained[77]. By making use of polystyrene and poly(vinyl pyrolidone), infrared
dielectric mirrors with 94% reflection were realized by James Bailey and James S
Sharp [78]. The introduction of polymeric materials into photonic crystal research
has made a great step towards the realization of all-optical integration. Although
nonlinear optical effects in inorganic 1D PCs have been well demonstrated, only a
few number of works have reported the use polymeric PCs for NLO applications.
Ultrafast optical switches operating at 1064 nm have been successfully fabricated

23
by Katouf et al. using polymeric 1D PC structures in which layers were doped
with second and third order NLO chromophores [79]. By making use of band edge
effects in PCs, Zhu and coworkers have observed enhanced optical performances
from nonlinear PBG structures made up of Co 3O4 nanoparticle doped poly(vinyl
alcohol) and poly(9-vinyl- carbazole) [80]. Husaini et al. have reported improved
nonlinear absorption behaviour in a 1D PC composed of alternate layers of a silver
nanocomposite and a passive polymer layer [81]. Although, experimentation with
polymeric PCs is challenging when comparing with their inorganic counterparts,
polymeric PC structures accompanied with optical nonlinearities can offer
extraordinary opportunities towards the realization of practical all-optical devices
and the research scope towards this direction is numerous.

1.6 PRESENT WORK

The present work is focused on the enhancement of nonlinear optical effects of

certain porphyrin samples by means of different 1D photonic crystal structures. As
an initial step nonlinear optical studies on certain sets of porphyrin systems are
conducted.

Porphyrins are versatile organic two-dimensional nano-materials that offer

unprecedented opportunities towards the optimization of desired molecular and
material properties by means of structural diversification. Optical nonlinearities
exhibited by these systems are widely noted in literature and are greatly
appreciated from the fundamental science as well as application point of view.
The conjugated 18π-electron bonding networks [82] present in the porphyrin
macrocycle consisting of four pyrrole units linked by methine groups, serve as the
basis of observed NLO activities in these molecules. The porphyrin macrocycle
can be modified by central metal coordination and by attaching peripheral
substituents at the pyrrolic free positions without compromising its chemical
stability [83]. Considering the porphyrin metal complexes, incorporation of
transition metal ions into the macrocycle cavity seems to contribute in extending
the π-electron delocalization and thereby improving the NLO effects. Additional
control over the photophysical properties are possible by changing the axial

24
ligands attached to the central metal ions and also by varying the metal oxidation
states[82,84]. In this thesis, two sets of porphyrin systems: (i) tin(IV) porphyrins
with peripheral modifications and (ii) fluorinated pyridyl porphyrins with Zn(II)
and Cu(II) derivatives and its dications are selected in order to investigate the
NLO properties. Third order NLO effects in these molecules are evaluated by
means of Z-scan experimental techinque with 7ns pulses at 532nm and the results
are presented in chapter 3.

From among the studied compounds, three porphyrin molecules with specific
NLO properties are selected for embedding into different 1D photonic crystal
structures and the results are presented in consecutive chapters. The first structure
used is a 1D photonic crystal microcavity in which cavity layer is doped with the
material dihydroxy(5,10,15,20-tetraphenyl porphyrinato)tin(IV) or SnTPP.
Nonlinear optical absorption and optical limiting properties of SnTPP are found to
be enhanced significantly with the cavity structure when comparing with the bare
SnTPP sample. The results are presented in chapter4. A plasmonic 1D photonic
crystal is used as the second structure and the NLO effects in 5,15-
di(pentafluorophenyl)-10,20-bis(4-N-methylpyridyl)Zn(II) porphyrin, abbreviated
as ZnP+ are investigated by means of Tamm plasmon polaritons. The Tamm
resonance mode created at the z-scan experimental wavelength, lying within the
photonic band gap is found to play the key role in improving the NLO response of
ZnP+. The third structure is simply 1D photonic crystal in which alternating layers
are doped with a nonlinear material. We call such a structure as nonlinear
distributed Bragg reflector (DBR) and the NLO material used in this case, is a
freebase porphyrin namely, 5,15-di(pyridyl)-10,20-bis(pentafluorophenyl)
porphyrin. Enhanced NLO activity of this molecule when incorporated in
nonlinear DBR is identified as due to the photonic band-edge effects.

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