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Optical Fredericks Transition in a Nematic Liquid Crystal Layer Hong Zhou, Eric P. Choate, and Hongyun Wang Abstract: One of the most fascinating aspects of liquid crystals is the Fredericks transition, which can occur when a finite sample of nematic liquid crystal is subjected to an externally applied magnetic or electric field. It is well-known that the director orientation throughout a sample of liquid crystal may be affected by a sufficiently strong magnetic or electric field. More specifically, the director alignment throughout a thin sample of nematic liquid crystal will not be influenced by the external magnetic or electric field when its magnitude is less than the critical field strength or Fredericks threshold, but will be influenced by the external field and start to adjust its orientation whenever the magnitude of the field is above the critical field strength. This change in the director alignment after the magnitude of the field increases beyond the critical field strength is called the Fredericks transition. It is exactly this important aspect of liquid crystals that provides many applications of liquid crystals for displays. In this chapter we first review the classical Fredericks transition in a liquid crystal H. Zhou (corresponding author) Department of Applied Mathematics, Naval Postgraduate School, Monterey, CA 93943, U.S.A. E.P. Choate Department of Mathematics and Statistics, Radford University, Radford, VA 24142, U.S.A. H. Wang Department of Applied Mathematics and Statistics, University of California, Santa Cruz, CA 95064, U.S.A.
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Page 1: Optical Fredericks Transition in a Nematic Liquid Crystal ...hongwang/publications/Fredericks_14.pdf · Optical Fredericks Transition in a Nematic Liquid Crystal Layer. Hong Zhou,

Optical Fredericks Transition in a Nematic Liquid Crystal Layer

Hong Zhou, Eric P. Choate, and Hongyun Wang

Abstract: One of the most fascinating aspects of liquid crystals is the Fredericks

transition, which can occur when a finite sample of nematic liquid crystal is subjected

to an externally applied magnetic or electric field. It is well-known that the director

orientation throughout a sample of liquid crystal may be affected by a sufficiently

strong magnetic or electric field. More specifically, the director alignment throughout

a thin sample of nematic liquid crystal will not be influenced by the external magnetic

or electric field when its magnitude is less than the critical field strength or Fredericks

threshold, but will be influenced by the external field and start to adjust its orientation

whenever the magnitude of the field is above the critical field strength. This change in

the director alignment after the magnitude of the field increases beyond the critical

field strength is called the Fredericks transition. It is exactly this important aspect of

liquid crystals that provides many applications of liquid crystals for displays.

In this chapter we first review the classical Fredericks transition in a liquid crystal

H. Zhou (corresponding author) Department of Applied Mathematics, Naval Postgraduate School, Monterey, CA 93943, U.S.A.

E.P. Choate Department of Mathematics and Statistics, Radford University, Radford, VA 24142, U.S.A. H. Wang Department of Applied Mathematics and Statistics, University of California, Santa Cruz, CA 95064, U.S.A.

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Hong Zhou, Eric P. Choate and Hongyun Wang

layer where analytical solutions can be obtained. After this warm-up, we provide a

detailed analysis in modeling electrically induced Fredericks transition. We conclude

the chapter with some future perspectives.

Keywords: Fredericks transition; nematic liquid crystals; continuum theory; critical

threshold

1. Introduction and Overview

The term "liquid crystals" was first introduced by Otto Lehmann in 1889 and it is

quite self-explanatory. It describes a matter state where materials exhibit many

properties of solid crystals such as anisotropy and symmetry, but flow like fluids or

viscous fluids. This combination of properties makes liquid crystals absolutely unique

and complex materials. There are many different types of liquid crystal phases. One of

the most common phases is the nematic phase where the rod-like molecules tend to be

aligned parallel to each other along some common preferred direction (“anisotropic

axis”). Examples of nematic liquid crystals include p-azoxyanisole (PAA),

4-methoxybenzylidene-4’-butylaniline (MBBA) and 4-pentyl-4’-cyanobiphenyl

(5CB). In a typical nematic such as PAA the molecules closely resemble rigid rods of

length 20oA and width 5

oA (de Gennes and Prost 1993) where 1 angstrom

oA

equals 1010 m− . The state of PAA depends on the temperature. PAA is a solid below

118o C , a nematic liquid crystal between 118o C and 135.5o C , and an isotropic

liquid above 135.5o C (de Jeu 1980). The local direction of the average molecular

alignment in liquid crystals is usually described by a unit vector n , called the

"director". Due to the lack of polarity of liquid crystals the two vectors n and n−

2

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Optical Fredericks Transition in a Liquid Crystal Layer

are indistinguishable.

Liquid crystals have been used in a wide variety of applications because external

perturbation can cause significant changes in the macroscopic properties of the liquid

crystal system. Both electric and magnetic fields can be applied to induce these

changes. In fact, one of the most intensively studied phenomena in the physics of

liquid crystals is the Fredericks transition which has been known for over 80 years. It

refers to a transition from a uniform director configuration to a deformed director

configuration of a homeotropically or planarly aligned nematic liquid crystal (NLC)

layer upon application of a magnetic or electric field of sufficiently large magnitude.

The behavior of a nematic liquid crystal is determined by two competing torques: (1)

the elastic torque within the material that tries to align the NLC molecules along the

easy direction as determined by the anchoring boundary conditions; and (2)

external-field-induced torque that tends to align the NLC molecules either parallel or

orthogonal to the field. A uniform director distribution occurs when only one of these

torques is present. When both torques exist, there is a competition between them.

Once the applied field strength exceeds a threshold value, the uniform NLC

orientation will deform and the Fredericks transition takes place.

The description of how the director is aligned on the boundary surfaces is called

anchoring. The main types of anchoring include strong, weak and conical anchoring.

Strong anchoring occurs when the surface energy is sufficiently large and the director

orientation on the boundary of the sample can be considered simply fixed in a

preferred orientation determined by an alignment technique. In the case of weak

3

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Hong Zhou, Eric P. Choate and Hongyun Wang

anchoring, the director alignment on the boundary is no longer rigidly fixed to the

surface and it is allowed to vary. Conical anchoring refers to the situation where the

director at a boundary makes a fixed angle with the tangent plane of the boundary.

Strong anchoring conditions are commonly used due to their simplicity. There are

several kinds of strong anchoring boundary conditions. For the planar alignment, the

molecules lie parallel to the cell surface. It can be obtained by either rubbing the

alignment layer (usually a polyimide thin film) or by UV photo-alignment. For the

homeotropic alignment, the director is perpendicular to the cell surface. It is obtained

by means of detergents or by applying a surfactant to the alignment surface. It is also

possible to obtain any pretilt angle by evaporating silicon dioxide at different angles

of incidence. Other alignment techniques, such as micron rubbing by microsphere,

micro-contact printing, ion beam bombardment, are available as well (Yilmaz et al.

2008).

The Fredericks transition plays a fundamental role in the operation of many liquid

crystal displays because the director orientation can be controlled easily by an

external magnetic or electric field. One striking feature is that the magnitude of the

Fredericks threshold voltage is essential to the operation of many liquid-crystal

devices. If the Fredericks threshold voltage could be reduced reliably, this would

make it possible for the manufacture of very low-power liquid crystal displays and

other liquid-crystalline devices. The Fredericks transition can also be employed to

achieve tunable all-optical switching and diode operation in the photonic devices

(Miroshnichenko et al. 2006).

4

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Optical Fredericks Transition in a Liquid Crystal Layer

There have been many studies on the Fredericks transition. For example,

experimental observations include the first observation of the optical-field-induced

Fredericks transition in the nematic liquid crystal 5CB (Durbin et al. 1981), nonlinear

light amplification in MBBA above the Fredericks transition by a magnetic field

(Khoo and Zhuang 1980). A quantitative theory to describe the reorientation of the

director of a nematic liquid crystal induced by the field of a light wave was developed

by Zel’dovich et al. using the geometrical optics approximation (Zel’dovich and

Tabiryan 1980; Zel’dovich, Tabiryan and Chilingaryan 1981). They calculated the

solution for the spatial distribution of the director direction for intensities above and

below threshold. They noted that a Fredericks transition induced by light fields in an

NLC with a positive dielectric anisotropy ( 0aε > ) can occur only when the light wave

is normally incident on an NLC cell with homeotropic orientation. When an ordinary

light wave is normally incident on an NLC cell with planar orientation, Fredericks

transition will not occur. They also predicted that near the threshold the maximum

angle of deviation of the director from the unperturbed direction is proportional to the

square root of the excess of the intensity above the threshold intensity and that for

certain nematic liquid crystals the Fredericks transition in a light field is accompanied

by hysteresis in broad beams, which they believed has no analog in the case of static

fields. In fact, in 1974 Deuling and Helfrich (Deuling and Helfrich 1974) had shown

that a homeotropic nematic layer with negative dielectric (or conductive) anisotropy

enclosed between two metallized glass plates undergoes a Fredericks transition. In

1981 Durbin et al. (Durbin et al. 1981) expressed the total electromagnetic energy

5

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Hong Zhou, Eric P. Choate and Hongyun Wang

density as the ratio of the magnitude of the Poynting vector to the ray velocity and

then used the infinite-plane-wave approximation in which the time average of the

magnitude of the Poynting vector of the optical field was assumed to be a constant

throughout the medium. Minimization of the free energy led to the Euler equation.

The solution of the Euler equation with proper boundary conditions gave the average

molecular reorientation of the liquid crystal. Their theoretical predictions were in

quantitative agreement with their experimental results. These earlier theoretical

studies only took the large anisotropies of nematic liquid crystals into account but

they lack the ability to properly describe the associated nonlinear effects. The

ground-breaking treatment of the optically induced Fredericks transition was given by

Ong (Ong 1983). In this classical work Ong provided a detailed study which includes

the interaction between the optical field and the NLC. An Euler equation, which is

consistent with Maxwell’s equations, is derived for describing the optically induced

spatial reorientation of the director of a homeotropically oriented nematic liquid

crystal for the case of normal incidence. The solution of the Euler equation describes

the deformation angle of the NLC. By examining the maximum deformation angle

near the threshold, Ong obtained the threshold intensity and the criterion for the

physical parameters that indicate whether the Fredericks transition is first order or

second order at the threshold. In contrast to Durbin’s assumption, Ong showed that

the time average of the magnitude of the Poynting vector is not a constant, but the

time average of the z-component of the Poynting vector is a constant, which is

consistent with the geometrical optics approximation (Zel’dovich and Tabiryan 1980;

6

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Optical Fredericks Transition in a Liquid Crystal Layer

Zel’dovich, Tabiryan and Chilingaryan 1981). In 1995 Sugimura et al. (Sugimura,

Luckhurst and Ou-Yang 1995) generalized the Rapini-Papoular formula (Rapini and

Papoular 1969) for the anchoring energy and provided rigorous expressions for the

threshold and saturation fields for a field-controlled twisted chiral nematic slab with

weak boundary coupling. Self, Please and Sluckin (Self, Please and Sluckin 2002)

considered the situation where the electromagnetic field interacts with the liquid

crystal deformation. Assuming strong anchoring at solid surfaces and a

one-dimensional distortion, they identified three dimensionless parameters, which are

related to the elastic anisotropy of the liquid crystal, the anisotropy of the electrical

permittivity of the liquid crystal, and the applied voltage, respectively. They applied

systematic asymptotic methods to determine approximate solutions in five various

regimes defined by physically relevant limiting cases of the parameters. Shi (Shi 2002)

summarized the main results in his two papers (Shi and Yue 2000, Yang, Shi and

Liang 2000) to give the exact criteria for the first order Fredericks transition to occur

in magnetically, electrically or optically driven liquid crystal cells. All these criteria

are in terms of the material parameters, cell geometrical parameters and surface

anchoring parameters where the anchoring strengths at the surfaces are described by

the Rapini- Papoular surface anchoring energy. It was noted that the first order

magnetic or electrical Fredericks transition occurs at surface anchoring conditions that

current technology is not mature enough to achieve. The first order transition cannot

occur for a rigid anchoring condition and this explains why first order transitions in

the magnetic and electrical cases are so difficult to observe. However, the first order

7

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Hong Zhou, Eric P. Choate and Hongyun Wang

transition can be easily realized for a three-dimensional Fredericks transition, as in a

twist liquid crystal cell.

Colloidal suspensions – dispersions of small solid particles in a host liquid

consisting of small molecules -- in nematic liquid crystals can also undergo Fredericks

transition. For a general review on the physics of colloidal dispersions in nematic

liquid crystals, see the article by Stark (Stark 2001). Ferronematics is the name for

suspensions of monodomain ferro or ferromagnetic particles in nematic liquid crystals.

Dispersed ferromagnetic particles greatly enhance the magnetic properties of the

liquid crystals. In 2003 Bena and Petrescu (Bena and Petrescu 2003) considered an

infinite flat layer of ferronematics (FN) between two identical substrates to study the

magnetic field-induced Fredericks transition in a homeotropically aligned FN with

weak anchoring molecules to the walls. They have found a correction to the

Burylov-Raikher expression (Burylov and Raikher 1993) for the magnetic threshold

field, together with an expression for the saturation magnetic field as a function of

material parameters and anchoring conditions. The saturation transition does not occur

in the case of rigid anchoring molecules to the cell walls. In 2009 they extended their

work to analyze the influence of anchoring conditions on the Fredericks transition in

ferronematics subjected to a superposed magnetic static field and an optical field

(Petrescu and Bena 2009). Using the Rapini-Papoular expression (Rapini and

Papoular 1969) for the anchoring energy and the Euler-Lagrange analytical method,

they obtained a correlation between the threshold intensities of the magnetic and the

laser fields, the anchoring strength, the material and device parameters. They found

8

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Optical Fredericks Transition in a Liquid Crystal Layer

that the fields needed for the transition are smaller than those in the rigid anchoring

case.

Another system analogous to ferronematics involves ferroelectric rather than

ferromagnetic colloidal particles. The colloidal particles are extremely small and at

low concentrations these submicron colloids macroscopically appear similar to a pure

liquid crystal with no evidence of dissolved particles. These dilute suspensions are

stable because the nanoparticles do not significantly perturb the director field in the

liquid crystals, and interaction between the particles is weak. In these colloidal

suspensions the dielectric response is strongly enhanced and the values of the

effective dielectric functions are higher than those of the analogous pure liquid

crystals. Such systems were first fabricated by Reznikov et al. (Reznikov et al. 2003)

using particles of the ferroelectric thiohypodiphosphate ( )2 2 6Sn P S for the suspension

and have been the subject of many researches (e.g. Li et al. 2006 and Shelestiuk,

Reshetnyak and Sluckin 2011). Shelestiuk et al. (Shelestiuk, Reshetnyak and Sluckin

2011) explored the Fredericks transition in ferroelectric liquid-crystal

nanosuspensions. Their study suggested that doping a nematic liquid crystal with

ferroelectric particles can significantly decrease the electric Fredericks threshold field.

A computational approach to the optical Fredericks transition in a homeotropic

nematic liquid crystal cell has been provided by Ilyina, Cox and Sluckin (Ilyina, Cox

and Sluckin 2006). They combined the popular finite difference time domain (FDTD)

method to solve the Maxwell’s equations with a relaxation algorithm to solve the

Ginzburg-Landau equations for the liquid crystal director.

9

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Hong Zhou, Eric P. Choate and Hongyun Wang

As one can see, it is impossible for us to provide a comprehensive list of all

relevant publications on the Fredericks transition in liquid crystals. For more details

on the theory and application of liquid crystals, please refer to the books by de Gennes

and Prost (de Gennes and Prost 1993), Chandrasekhar (Chandrasekhar 1992), Khoo

(Khoo 1995), Virga (Virga 1994) and Stewart (Stewart 2004).

2. The Classical Fredericks Transitions in a Nematic Liquid Crystal Cell

In general, the classical Fredericks transition in nematics can be fairly

well-explained using continuum theory of nematic liquid crystals developed by Frank,

Ericksen and Leslie. Before we present a detailed analysis on the optical Fredericks

transition, which couples the interaction between the applied electromagnetic field of

a light wave and the orientation of liquid crystals, we would like to briefly review the

classical results (de Gennes and Prost 1993, Virga 1994, Stewart 2004). Many of our

ideas here are borrowed from Stewart (Stewart 2004).

Conventional analytic study of this problem normally considers an

electromagnetic field in which the magnetic component is dominant. Generally the

effect of the nematic orientation does not affect the magnetic field, and so the

electromagnetic field structure decouples from the orientation and the electric field

components can be ignored. To get started, let us consider a nematic liquid crystal

sample confined between two parallel glass plates at 𝑧 = 0 and at 𝑧 = 𝐿. We

assume strong anchoring and impose the same director at each plate. We also assume

the anchoring is uniform in the x- and y-directions so that the orientation is a function

of z only. 10

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Optical Fredericks Transition in a Liquid Crystal Layer

We will consider three common geometries concerning the relationship between

the anchoring conditions and imposed magnetic field: splay, bend, and twist. For the

splay geometry, the director is parallel to the bounding plates where ( )1 0 0) ,( ,z =n

is the uniform equilibrium solution. In this case, the natural choice for the magnetic

field to apply in order to observe the Fredericks transition is ( )0,0,1 ,H H= =H H .

Assuming that the director attempts to reorient itself to be parallel to the magnetic

field and any reorientation of the director only depends on z, we seek solutions for the

director of the form ( ) ( )( )cos ,0,sinz zφ φ=n , where ( )zφ is called the director

angle. The bend geometry reverses these roles with the director anchored

perpendicularly to the plates while the magnetic field is parallel to the plates. We set

the magnetic field ( )1,0,0H=H and seek solutions of the form

( ) ( )( )sin ,0,cosz zφ φ=n . Figure 1 illustrates these three geometries.

We begin by focusing on the twist geometry, in which both the initial director

alignment and the magnetic field are both parallel to the glass plates but are mutually

orthogonal to each other. We impose a magnetic field of the form ( )0,1,0H=H and

search for directors of the form ( ) ( )( )cos ,sin ,0z zφ φ=n . The analysis is easier in the

twist geometry, and we present a detailed derivation of its solution. Afterwards, we

present the splay and bend geometries, which are very similar to each other and reduce

to a form like the twist geometry under a simplifying assumption.

For boundary conditions in all three geometries, we use

11

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Hong Zhou, Eric P. Choate and Hongyun Wang

( ) ( )0 0Lφ φ= = (1)

so that all three have the uniform solution ( ) 0zφ = for all 0 ≤ 𝑧 ≤ 𝐿. Below the

critical field strength 𝐻𝑐 of the Fredericks transition, this uniform solution is stable,

but above the critical value, a stable nonuniform solution appears.

To find the stable solution, we must minimize the free energy of the system, which

balances contributions from elastic and magnetic parts. The Frank elastic free energy

density for nematics is given by

( ) ( ) ( )2 2 21 2 3

12Frankf K K K = ∇ ⋅ + ⋅∇× + ×∇× n n n n n (2)

where the Frank elasticity constants 1 2, ,K K and 3K represent the splay, twist, and bend

moduli, respectively (Virga 1994). The elastic constants depend on temperature and are

commonly of the order 710− to 610− dyn with 3K often being two or three times larger

than 1K and 2K . For example, for PAA, at 120°C the constants are 71 5.0 10K −= × dyn,

72 3.8 10K −= × dyn, and 7

3 10.1 10K −= × dyn, and at 125°C, 71 4.5 10K −= × dyn,

72 2.9 10K −= × dyn, and 7

3 9.5 10K −= × dyn.

For analytical purposes, it is often common to use the simplifying single-constant

assumption with 1 2 3 allK K K K= = = . Under this assumption, the Frank elastic free

energy density simplifies to

1 1 tr( ): ( )2 2

TFrank all allK Kf ∇ ∇ == ∇ ⋅ ∇n n n n . (3)

The free energy density contribution from the magnetic field is

12

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Optical Fredericks Transition in a Liquid Crystal Layer

( )212magnetic af χ= − ⋅n H (4)

where aχ is the anisotropic magnetic susceptibility in Gaussian cgs units. We will

assume 0aχ > . Therefore the total free energy density is Frank magneticf f f= + .

2.1 Twist Geometry and Single-Constant Assumption

Inserting the form of the twist geometry ( ) ( )( )cos ,sin ,0z zφ φ=n and

( )0,1,0H=H into (2) and (4), we have the total free energy density

222 21 1 sin

2 2 af K H φφ χ= −′ . (5)

The total energy functional of ( )zφ is obtained by integrating the free energy density

over the thickness:

[ ] ( ) ( )( )0

,L

dzF f z zφ φ φ′= ∫ (6)

To look for functions ( )zφ that minimize F , we consider the perturbed solution

( ) ( )z zφ δη+ where ( ) ( )0 0Lη η= = , and write

( )

0

2 2 2 22 2 3

2 2

] ,

22

)[ (L f fF f

f f f dz O

φ δ η ηφ φ

δ η ηη η δφ φ φ

φ

φ

φ ∂ ∂ ′= + + ′∂ ∂

∂ ∂ ∂′ ′+ + + + ′ ′∂ ∂

∂ ∂

∫ (7)

For ( )zφ to minimize [ ]F φ , the first variation must be zero:

0

0L f f dzη ηφ φ∂ ∂ ′+ =

′∂ ∂∫ . (8)

Integration by parts using the boundary conditions ( ) ( )0 0Lη η= = yields

13

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Hong Zhou, Eric P. Choate and Hongyun Wang

0

0L f d f

dzdz

φη

φ ∂ ∂

− = ′∂ ∂ ∫ . (9)

Since η is arbitrary, we obtain the Euler-Lagrange equation

0f d fdzφ φ

∂ ∂− =

′∂ ∂ (10)

Now, substituting (5) obtains the equilibrium equation for the director angle:

22

sin 2 02aK H φχφ +′′ = (11)

This equation is of the form that has been considered by Freedericksz and Zolina

(Freedericksz and Zolina 1933) and Zocher (Zocher 1933).

For any value of H and the boundary conditions (1), ( ) 0zφ = is a trivial but

important solution to (11). This represents a uniform solution in which the nematic

orientation is homogeneous. Its stability can be seen from the second variation in (7). In

order for ( ) 0zφ = to be a minimum, we need

2 2 2

0

2 22 2 02

Ldzf f fη ηη η

φ φ φ φ∂ ∂ ∂′ ′+ + >

′ ′∂ ∂ ∂ ∂∫ . (12)

Integrating by parts and inserting (5) yields

2 2 2

0 2cos 2 0L

a H K dzχ φη η′− + >∫ , (13)

or once we inserting ( ) 0zφ = ,

22

2

0

2 0L

a H K dzηχ η′− + >∫ . (14)

If we assume a representation of 1

( ) sinjj

jzzL

πη η∞

=

=∑ , we find that we must have

14

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Optical Fredericks Transition in a Liquid Crystal Layer

2 2

2 22 0a

jH KL

πχ− + > . (15)

for each 1j ≥ for stability. The most restrictive of these is when 1j = . Therefore, the

homogeneous solution ( ) 0zφ = minimizes the free energy if cH H< where

,uniform2

ca

KL

H πχ

= (16)

The question remains as to whether or not there are other solutions.

Since the free energy density (5) has an even dependence on φ , if ( )zφ

minimizes the free energy, then ( )zφ− also minimizes the free energy. Also, due to the

boundary conditions (1), we expect nontrivial solutions to take the symmetric form

( ) ( ) , 0z L z z Lφ φ= − ≤ ≤ (17)

which implies that

02Lφ ′ =

. (18)

From (11), if 0φ′ = and 02πφ< < , then 0

2Lφ ′′ <

, and so

2Lφ

must be a local

maximum, which we will denote as maxφ .

We now multiply (11) byφ ′ and integrate to get

22

22 sina HK Cχ φφ +′ = . (19)

The constant of integration C may be found by evaluating at 2Lz = :

15

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Hong Zhou, Eric P. Choate and Hongyun Wang

2 222

2 2max

2

sin sina L azC H HK χ φ χφ φ

= + = ′= . (20)

Thus, (19) can be written as

2 2 2m

2a2 xsin sina HK χ φ φφ =′ − . (21)

Since the left side is positive, we can conclude from the right side that max0 φ φ≤ ≤ on the

interval 02Lz≤ ≤ with φ increasing monotonically from 0 to maxφ . Therefore,

2 22 maxsin sinaK H φφ χ φ= −′ . (22)

Upon integration, we can define ( )zφ on 02Lz≤ ≤ implicitly through the equation

2 0 2 2maxsin sin

adKHz

φχ φ

φ φ=

−∫

, (23)

once we have found the value of maxφ , which we may find by first solving the implicit

equation coming from (23) evaluated at 2Lz = and maxφ φ= :

max

2 0 2 2max

2 sin sina

L dH Kφ φ

φ φχ

−= ∫

. (24)

We can then extend the solution to the interval 2L z L≤ ≤ by using the symmetry (17).

To aid us both in analysis and computation, we can rewrite these using elliptic

functions if we first make a change of variables similar to the one used by Zocher

(Zocher 1933)

max max

sin cossin , cossin sin

d dφ φψ ψ ψ φφ φ

= =

. (25)

Eq. (24) can be rewritten as

16

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Optical Fredericks Transition in a Liquid Crystal Layer

( )max2 2max

20

2

sin1 sin s n2 i

aH d KLK

πχ

ψψ φ

φ= =

−∫ (26)

where ( )K k is the complete elliptic integral of the first kind with modulus maxsink φ= .

MATLAB provides a built-in function ellipke to compute complete elliptic integrals of

the first and second kinds. This also allows us to see that in the limit of strong

magnetic fields ( H →∞ ), we must have max 2πφ

→ .

Once maxφ is found, the distorted solution ( )zφ can be found on 0 12

zL

≤ ≤ by

rewriting (23) as

1

max

sinsinsin

2 2max

1max

02

max

1 sin sin

sinsin ,sin ,sinellipt c

a

i

Hz d

F

K

φφ

ψψ

φ

χ

φ

φφ

=−

=

∫ (27)

where , )(ellipticF kψ is the incomplete elliptic function of the first kind with modulus

maxsink φ= , which can be computed in MATLAB with the built-in function ellipticF.

The solution for 1 12

zL

≤ ≤ can then be obtained via the symmetry (17).

This distorted solution, however, does not exist for small values of H . To see this

and find the critical threshold ,distortedcH above which the distorted solution does exist,

we define the function

( )max 2 2max

,1 sin sin

1G ψ φψ φ

≡−

. (28)

Note thatG has the symmetry ( ) ( )max max, ,G Gψ φ φ ψ= . It is straightforward to check

that

17

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( )( )

2max max

3/22 2max max

, sin sin 2

2 1 sin sin

G ψ φ ψ φφ ψ φ

∂=

∂ −. (29)

Thus, for max02πφ< < and 0

2πψ< < ,

( )max

max

,0.

G ψ φφ

∂>

∂ (30)

Consequently, ( )max,G ψ φ is a monotonically increasing function of maxφ for

max02πφ< < . Furthermore, note that

( )max max

max 2 20 0max

lim , lim 11 sin

1sin

Gφ φ

ψ φψ φ+ +→ →

= =−

. (31)

Taking the limit max 0φ +→ on both sides of (26), we find that the critical field

strength ,distortedcH obeys

,distorted

22 2acH

KL χ π

= . (32)

Therefore, we find the same critical value as ,uniformcH from (16), and so we have only

one critical value

2c

a

KHLπ

χ= (33)

such that the uniform solution ( ) 0zφ = is the only solution and is stable if cH H< ,

but for cH H> , the uniform solution is unstable and the distorted solution given by

(26) and (27) exists.

Also, when cH H> , we can show that the distorted solution given by (26) and

(27) is energetically favorable to the uniform solution ( ) 0zφ = by showing that the

difference in the free energies of the two solutions 18

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Optical Fredericks Transition in a Liquid Crystal Layer

][ [0]F F Fφ∆ = − (34)

is negative. From the energy expression (6) and using (21), we obtain

2 2

2 2 2max

2 2 2 2

22

2ma

0

0

2max

2x0

1 sin21 sin 2sin21 sin 2sin sin 2sin2

a

L

L

L

L

a

L

a

F K H dz

H

dH d

dz

z z

χ φ

χ φ φ

χ φ φ φ φ

φ∆ = −

= −

= − −

+

∫ ∫

(35)

For the second integral, we make the change of variables z L z= − so that

( ) ( )

( ) ( )

2 2 2 2max ma

0

2x

2 2 2 2max max

2

2 20 0

sin 2sin sin 2sin

sin 2sin sin 2sin

LL L

L L

dz L z dz

z dz z dz

φ φ φ φ

φ φ φ φ

− = − − −

= − = −

∫ ∫

∫ ∫

(36)

where the symmetry condition (17) is employed. Thus,

( )

max

max

2 2 2max

2 2 2max

2

20

2max 2 2

ma

2

x

0

0

sin 2sin

(sin 2sin )

sin 2sinsin sin

a

a

L

a

dz

K

F H

dzH dd

H d

φ

φ

φ

χ φ φ

χ φ

φ

φφ

φ φφ

χφ

∆ = −

= −

= −−

(37)

where we have differentiated (23) to get the expression of dzdφ

. Using the substitution

(25), we can rewrite this as

19

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Hong Zhou, Eric P. Choate and Hongyun Wang

( )

2max 2 2

max

2max

max2m

22 0

22 ma0

22 a

x

0x

cos 2

cos 2 ( , )

si

sin1 sin sin

sin

,1 sin2

n 2

a

a

a

F K H

K H

GK H

G

d

d

d

π

π

π

ψ ψχ φφ

ψ ψ φ ψ

ψ

ψ

χ φ

ψ φχ φ ψ

ψ

∆ =−

=

∂= −

(38)

where we have again used (28) and integrated by parts in the last step. Thus, we use (30)

and the fact that sin 2 0ψ > on 02πψ< < to conclude that 0F∆ < for cH H> .

Therefore, the distorted solution is indeed energetically preferred over the

unstable uniform solution, which verifies that the Fredericks transition does occur in

the twist geometry and that

2,twistc

a

KHLπ

χ= (39)

is the critical threshold.

Under the single-constant approximation 1 2 3 allK K K K= = = , the free energy

density takes the same form (5) except that 2K is replaced with allK . Therefore all

the above analysis can be repeated so that the critical threshold is

allc

a

KHLπ

χ= . (40)

When cH H< the uniform solution ( ) 0zφ = is the only stable solution, but for

cH H> , the stable solution is the distorted solution given by

20

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Optical Fredericks Transition in a Liquid Crystal Layer

( )maxsin2

c

KHH π

φ= , (41)

1max

max

sinsin ,sinsin

1el i i

cl pt cFHz

H Lφ

πφφ

− =

, (42)

where K and ellipticF are the complete and incomplete elliptic functions of the first

kind, respectively.

Figure 2 illustrates the distorted solution ( )zφ from (41) and (42) for various

values of the dimensionless magnetic field strength / cH H . As / cH H increases, the

values of ( )zφ in the interior also increase. The transition that we have so far

described analytically can be illustrated by the bifurcation diagram of Figure 3, where

the solid line represents the stable solution and the dashed line represents the unstable

one. For cH H≤ , the trivial solution max 0φ φ= = is the only solution of the

equilibrium equation, and it is necessarily stable. For cH H> , the trivial solution

becomes unstable and a new distorted solution arises, which is stable.

The formulation of the solution terms of elliptic integrals from (41) and (42) can

also be helpful in asymptotic analysis of the solution. As 0,k → the complete elliptic

integral of the first kind has the asymptotic behavior

( ) ( )2 4 41 912 4 64

K k k k o kπ = + + +

. (43)

Therefore, we have an asymptotic expression for how maxφ emerges from the uniform

solution as max 0φ +→ in terms of the normalized field / cH H from

21

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Hong Zhou, Eric P. Choate and Hongyun Wang

( )2 2max max

14

1c

HH

oφ φ= + + (44)

so that as max 0φ +→

max 2 1c

HH

φ ≈ − . (45)

As max 2πφ → , the asymptotic analysis gives (Stewart 2004):

2

max

2 4ln1 sinc

HH π φ

≈ −

(46)

which in turn yields

max 4exp2 2 c

HH

π πφ

≈ − −

. (47)

Thus, when maxφ is close to 2π when

c

HH

is big enough (for example, 3c

HH

> ).

The 1L

dependence in these critical values corresponds with the dependence

found experimentally by Fredericks. Also, from an experimental point of view, they

also provide a way to use the detection of the critical threshold to measure the Frank

elasticity constants if the magnetic anisotropy aχ is known.

2.2 Bend and Splay Geometries

A similar strategy may be followed in the bend and splay geometries, but each

case depends on the two different Frank constants 1K and 3K instead of just one.

We will highlight the differences for the bend geometry, and the splay geometry can

then be found by swapping the roles of 1K and 3K .

22

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Optical Fredericks Transition in a Liquid Crystal Layer

Inserting the bend geometry form of ( ) ( )( )sin ,0,cosz zφ φ=n and

( )1,0,0H=H into (2) and (4), the total free energy density becomes

2 2 22 21 3

1 1sin cos sin2 2 af K K Hφφ φ χ φ −′= + . (48)

The Euler-Lagrange equation for the director angle (10) then becomes

( ) ( )2 2 21 3 1 3

2sin 2 sin 2sin cos 02 2aK K K K Hφ φφ χφ φφ + +′′ ′− + = . (49)

Again, for any value of H and the boundary conditions (1), we have the uniform

solution ( ) 0zφ = . The second variation takes a similar form as (14)

2230

2 0L

a H K dzηχ η′− + >∫ , (50)

so that the uniform solution minimizes the free energy if cH H< where

3,uniformc

a

KL

H πχ

= . (51)

For the distorted solution, we also assume the symmetry (17) and then solve

integral equations first for maxφ and then for ( )zφ on 02Lz< < . Unfortunately, the

forms these integrals take are more complicated and cannot be easily represented with

elliptic functions.

We find these integrals by multiplying (49) byφ ′ and integrating with the same

constant of integration as (20) so that

( )2 2 2 2 21 3 m x

2asin cos sin sinaK K Hφ φ χ φ φφ ′ + = − . (52)

Taking the square root and integrating, we can define the distorted solution with

23

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Hong Zhou, Eric P. Choate and Hongyun Wang

2 2 2

1 3 1 32 2 2 20 0

max max

3sin cos (sin sin sin s n

)sinia

K K K K Kd dHzφ φφ φ φ

φχ φ φ

φ φ φ+ −

=−

=+

−∫ ∫

, (53)

with maxφ having been found from

max2

12 2

max

3 30

( K sin2 sin

)sina

K KLH dφ φχ φ

φ φ+ −

=−∫

. (54)

Or, using the change of variables (25), we have

( )1

max

2 2sinsin 3 1 3 maxsin2 2

m0

ax

sin sin1 sin sina

K K KHz d

φφ

ψ φχ

ψ φψ

+ −=

−∫ (55)

( ) 2 23 1 3 max

2 20ax

2

m

sin sin2 1 sin sina

K K KLH dπ ψ φ

χ ψψ φ

+ −=

−∫ (56)

We can find the critical field strength above which this distorted solution exists

through a similar argument as the twist geometry by observing that the integrand in (55)

and (56) is an increasing function of maxφ so that

( ) ( )max max

2 23 1 3 max

max 32 20 0max

sin sinlim , lim

1 sin sinK K K

G Kφ φ

ψ φψ φ

ψ φ+ +→ →

+ −= =

− (57)

Thus, taking the limit max 0φ +→ of (56) shows that

,distorted 32 2a cLH Kπχ = , (58)

and again we have only one critical value

3,bendc

a

KHLπ

χ= , (59)

which has the same dependence on the Frank constant as the twist (33) and

single-constant approximations (40). A similar argument to the one above shows that

24

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Optical Fredericks Transition in a Liquid Crystal Layer

when ,bendcH H> , the distorted solution is energetically preferable to the uniform

solution.

The critical value for the splay geometry is

1,c splay

a

KHLπ

χ= , (60)

and the distorted solution is given by

( )1

max

2 2sinsin 3 1 maxsin2 2

1

m0

ax

sin sin1 sin sina

K K KHz d

φφ

ψ φχ

ψψ

φ

+ −=

−∫ (61)

( ) 2 21 3 1 max

2 20ax

2

m

sin sin2 1 sin sina

K K KLH dπ ψ φ

χ ψψ φ

+ −=

−∫ . (62)

2.3 Extension to Electric Fields

The above discussion of the Fredericks transition can be extended to include (1)

pretilt at the boundaries where the boundary conditions ( ) ( )0 0Lφ φ= = are replaced

by ( ) ( ) 00 Lφ φ φ= = ; (2) the tilted fields where the magnetic field is applied across the

sample at a fixed angle; (3) weak anchoring where the director is weakly anchored to

both boundary plates. A more detailed discussion can be found in Stewart (Stewart

2004) and Virga (Virga 1994).

The Fredericks transition also occurs under the influence of an electric field E .

From a mathematical perspective, the above analysis can be repeated with the magnetic

free energy density (4) replaced by an electric free energy density

25

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Hong Zhou, Eric P. Choate and Hongyun Wang

( )212electric af ε= − ⋅n E , (63)

where aε ε ε⊥= −

is the dielectric anisotropy of the liquid crystal where ε

and ε⊥

are the relative permittivities or dielectric constants of the liquid crystal when the field

and director are parallel and perpendicular, respectively. The analogous critical field

strengths for the splay, twist and bend geometries are (Stewart 2004)

31 2, , ,, ,c splay c twist c bend

a a a

KK KE E EL L Lπ π π

ε ε ε= = = . (64)

However, this formulation is known to be less accurate than the magnetic field

approximation. So far, we have assumed that the electromagnetic fields are unaffected

by the orientation of the liquid crystal medium. For magnetic fields, this assumption

works well, but for electric fields, the coupling of the field and the liquid crystal

orientation cannot be ignored.

3. Optical Fredericks Transition with Coupled Orientation and Electromagnetic

Fields

We now extend our analysis in two ways to better model the optical Fredericks

transition. That is, the reorientation of a nematic liquid crystalline cell by a light wave

passing the layer allowing for the coupling of the electromagnetic field and the nematic

orientation field. We use the bend geometry from Section 2 with the director

(sin ( ),0,cos ( ))z zφ φ=n , but the electromagnetic field consists of a normally incident

beam of light with the polarization parallel to the xz-plane, as illustrated in Figure 4. In

order to focus on the effect of the NLC, we assume the supporting plates have the same

optical properties as the medium outside the cell, which we treat as vacuum. 26

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Optical Fredericks Transition in a Liquid Crystal Layer

3.1 Maxwell Equations

The governing equations of the electromagnetic field are given by Maxwell's

equations (see, for example, Yeh 2005) which in Gaussian units are

1c t∂

∇× + =∂BE 0 (65)

1 4c t c

π∂∇× − =

∂DH J (66)

4πρ∇⋅ =D (67)

0∇⋅ =B (68)

for the electric field E , the magnetic field H , the electric displacement D , the

magnetic induction B , and the speed of light c . We include the electric current

density J and the charge density ρ for the moment, but we will soon assume they are

zero.

In order to close the system, it is necessary to specify constitutive relations that

describe the macroscopic properties of the medium. The magnetic constitutive equation

is

µ=B H , (69)

where the relative permeabilityµ is assumed to be 1 so that the NLC has no effect on

the magnetic field. The constitutive equation for the electric field is

= ⋅D ε E (70) for the symmetric relative permittivity tensor ε , which is also known as the dielectric

tensor. If εwere a scalar, the system would be isotropic. Outside the NLC cell, we use

1ε = . Inside the cell, the NLC is anisotropic with two different values of the relative

permittivity. In the direction parallel to the director n , we have the extraordinary

27

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Hong Zhou, Eric P. Choate and Hongyun Wang

relative permittivityε

, but in the directions perpendicular to n , we have the ordinary

relative permittivity ε⊥ . Typical values for these constants for the nematic PAA at

125°C are 3.3ε ≈

and 2.3ε⊥ ≈ . The relative permittivity tensor is

2

2

sin 0 sin cos0 0

sin cos 0 cos

a a

a

a a

ε ε φ ε φ φε ε ε

ε φ φ ε ε φ

⊥ ⊥

+ = + = +

ε I nn (71)

where I is the identity tensor and aε ε ε⊥= −

measures the dielectric anisotropy.

Since these are linear equations, they apply to both real and complex

electromagnetic vectors. However, since the real part of the product of two complex

vectors is not equal to the product of their real parts, care must be taken to distinguish

between the real and complex electromagnetic vectors in their products. The simplest

form of light is a monochromatic, linearly polarized plane wave. So we assume a

monochromatic complex form with angular frequency ω , and for the rest of this

section, we use a tilde to denote the real, time-varying vectors. Vectors without tildes

represent complex vectors that may depend on z but not t . That is,

( ) ( ) ( ) ( )Re , Re , Re , Rei t i t i t i te e e eω ω ω ω− − − −= = = =E E D D H H B B . (72)

We can now use (69) and (70) to rewrite Faraday’s Law (65) and Ampere’s Law

(66) as

,icω

⋅− = ∇×ε E H (73)

.icω

= ∇×H E (74)

These allow us to condense the electromagnetic field equations into a single vector

equation with E and n , which appears through ε , as

28

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Optical Fredericks Transition in a Liquid Crystal Layer

c ii c

ωω

∇× ∇× = − ⋅

E ε E (75)

or

( )2

2cω

∇× ∇× ⋅=E ε E (76)

which, with the help of the vector identity ( ) ( ) 2∇× ∇× = ∇ ∇⋅ −∇E E E , can be

expressed as

( )2 20k∇ −∇ ∇⋅ + ⋅ =E E ε E 0 (77)

for the wavenumber 00

2kcω π

λ= = , where 0λ is the free space wavelength of the

incident beam.

This can be simplified further under our assumptions that the NLC and

electromagnetic fields are homogeneous in both the x- and y-directions and the

polarization of the incident beam has the electric field in the x-direction. From the

z-component of (73), we observe that

13 1 33 32 1)( 0E E H Hi

c x yε εω ∂ ∂

− + = − =∂ ∂

(78)

which implies that 13 1 33 3 0E Eε ε+ = . This allows us to write the z-component of the

electric field as a function of the x-component as

133 1 12

33

sin coscos

a

a

E E Eε ε φ φε ε ε φ⊥

= − = −+

(79)

A similar argument from (74) shows that 3 0H = .

Also, the y-component of (73) is

29

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Hong Zhou, Eric P. Choate and Hongyun Wang

2

220 22 0E k E

zε⊥

∂+ =

∂, (80)

and given the polarization of the incident beam, we can conclude that 2 0E = .

Furthermore, since 3 2 21

E E Ei Hc y z zω ∂ ∂ ∂

= − = −∂ ∂ ∂

from (74), it follows that 1 0H = .

Returning to (73), the x-component is

( )2

210 11 1 13 32 0d E k E E

dzε ε+ + = (81)

Substituting (79), this yields an equation connecting the x-component of the electric

field and the director angle as

||2

210 12 2 0

cosa

d E k Edz

εε ε φ

ε⊥⊥

+ =+

. (82)

Once 1E is known, we can find the y-component of the magnetic field from (74) to be

12

0

1 dEHik dz

= . (83)

3.2 Free Energy Minimization

Now we need to minimize the free energy of the system to determine the

preferred orientation of the system. The elastic free energy density Frankf is the same

as (2). However, the electromagnetic contributions are more complicated due to the

time-varying fields. The electric contribution is

( ) ( )

( )

( )

* *

2 * * * * 2

2 *

1 18 321

321 Re

16

i t i t i t i telectric

i t i t

i t

f e e e e

e e

e

ω ω ω ω

ω ω

ω

π π

π

π

− −

= ⋅ + ⋅ +

= ⋅ + ⋅ + ⋅ + ⋅

= ⋅ + ⋅

=E D E E D D

E D E D E D E D

E D E D

(84)

because *⋅E D is real. Similarly, we also have the magnetic contribution

30

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Optical Fredericks Transition in a Liquid Crystal Layer

( ) 221 1 Re8 16

i tmagneticf e ω

π π−⋅ = ⋅ = + B H B H H . (85)

The time-varying Poynting vector, which represents the directional energy flux density

of the electromagnetic field, is

( ) ( )2 *Re Re4 8

i tc c e ω

π π− = × = × + × S E H E H E H . (86)

The magnitude of the Poynting vector is the irradiance.

According to the energy conservation law Poynting’s theorem, the work done by

the electric field is

14

ctπ

∂⋅ = − + ∇× ⋅ ∂

DJ E H E (87)

with the insertion Ampere’s law (66). The first term can be written using the identity

( )

2 2ji iij j i ij ij j

EE EE E Et t t t t t t

ε ε ε∂∂ ∂∂ ∂ ∂ ∂

⋅ = ⋅ + ⋅ = + = = ⋅∂ ∂ ∂ ∂ ∂ ∂ ∂

E D DE D D E E

(88)

where we have used Einstein summation convention and the fact that ε is symmetric.

The second term can be rewritten with the identity ( ) ∇⋅ × = ⋅∇× − ⋅∇×E H H E E H ,

so that we can rewrite (87) as

( ) ( )( )( )

( )

1 14 2

1 1 ˆ4 2

( .)electric magneticf f

ct

D ct t

t

π

π

∂ ⋅ = − ⋅ + ⋅∇× −∇⋅ × ∂ ∂ ∂

= − − ⋅ − ∇ ⋅ × ∂ ∂ ∂

= − −∇

⋅∂

+

J E E D H E E H

BE H E H

S

(89)

Under our assumption that the current density J is zero, then we have

( 0)electric magneticf ft∂

+ =+ ∇⋅∂

S . (90)

For time-periodic sinusoidal electromagnetic fields, the average power flow per unit

time is often more useful. We assume the timescale of the reorientation of the liquid

crystal is much slower than the electromagnetic timescale defined by the frequency ω31

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Hong Zhou, Eric P. Choate and Hongyun Wang

of our monochromatic incident beam. We therefore approach the liquid crystal part as a

steady-state by averaging the appropriate electromagnetic quantities over one period.

Therefore we need the time-average free energy densities over one period for the free

energy minimization for the φ equation:

2*1 1,16 16electric electric magnetic magneticf f f fπ π

= = ⋅ = =E D H (91)

Also, to define the intensity below, we will also need the time-average of (90), or

( ) ( )

( )

2 *

*

0 ( )

Re Re8

Re .8

i tm

electric magnetic

ele agneticctric

ft

cf f et tc

f

ω

π

π

−∇

∂= + +∇⋅

∂ ∂ = + + × + × ∂ ∂

= ∇ ⋅ × = ∇ ⋅

S

E H E H

E H S

(92)

From the perspective of the free energy density of the orientation, the optical

energies are treated as negative quantities so that the free energy density is

Frank electric magneticf f f f= − − . (93)

However, since magneticf does not contain the director angle φ , its contribution to the

free energy does not affect the minimization process, and so we omit it.

We now proceed to minimize the free energy function in a manner similar to that of

Section 2, except that it will contain the unknown 1E . The free energy density is

( ) ( )( ) ( ) ( ) ( )

( )( )

22 21 3

21

2

1, sin cos2

16 cosa

f z z K z K z z

E zz

φ φ φ φ φ

ε επ ε ε φ

′ ′ = +

−+

(94)

Substituting this into the Euler-Lagrange equation (10), we find

32

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Optical Fredericks Transition in a Liquid Crystal Layer

( ) ( )

( )

222 2

1 3 1 32

2122

sin cos sin cos

sin 20.

16 cosa

a

d dK K K Kdz dz

E

φ φφ φ φ φ

ε ε ε φ

π ε ε φ⊥

+ + −

+ =+

(95)

3.3 Boundary Conditions and Intensity

We now have a coupled second-order system (82) and (95) for the director angle

φ and the x-component of the electric field 1E . We need boundary conditions for

this system and a way to quantify the intensity of the electromagnetic field that will

drive the optical Fredericks transition. For the anchoring conditions, we use

( ) ( ) .0, 00 Lφ φ == (96)

The electromagnetic boundary conditions are more complicated.

When the middle layer ( )0 z L< < is homogeneous and isotropic, boundary

conditions have been given in (Yeh 2005). In our study here, the middle layer is an

NLC so we cannot directly use the boundary conditions in (Yeh 2005). However, we

can borrow ideas from there. Outside the liquid crystal layer, 1E is assumed to take the

forms

( )0 0

01, 0

,

ik z ik zin ref

ik zout

E e E e zE z

E e z L

− + <=

> (97)

where the unknown complex constants inE , refE , and outE represent, respectively, the

incident beam, the beam that reflects off the front of the NLC cell, and the transmitted

beam that passes through the cell. From (83), the corresponding magnetic field outside

the layer is

33

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Hong Zhou, Eric P. Choate and Hongyun Wang

( )0 0

02, 0

,

ik z ik zin ref

ik zout

E e E e zH z

E e z L

− − <=

> (98)

Ideally, we would like to impose inE and then solve for refE and outE . However,

it is not possible to do this since it would not assign a boundary condition to the system

(82) and (95). We can get this around in the following way. From the time-average

Poynting vector (92), it follows that

( )*3 1 2Re 0

8d c dS E Hdz dzπ

= = . (99)

Thus, ( )*3 1 2Re

8cS E Hπ

= is constant throughout the domain, both inside and

outside the NLC cell. Note that it is only the time-average of the z-component of the

Poynting vector that is constant throughout the domain, not the overall Poynting vector,

its magnitude, or 3S itself. We define the intensity I as this constant so that

( )( )22

*1 2

2

, 08Re

8 ,8

in ref

out

c E E zcI E H

c E z L

ππ

π

− <= = >

(100)

Thus, we can conclude that 22 2

in ref outE E E= + , as is required to conserve energy.

We shall choose 8out

IEcπ

= but choose I as our control variable.

For discontinuous media, the components of the electromagnetic fields that are

tangential to the surfaces of the discontinuities must be continuous. For our NLC cell,

this means that 1E and 2H must be continuous at both 0z = and z L= . This gives

us both boundary conditions for (82) and way to solve for the unknowns inE and refE .

For 1E , we have 34

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Optical Fredericks Transition in a Liquid Crystal Layer

( )( )0

1

1

0in ref

ik Lout

E E E z

E e E z L

+ = =

= = (101)

For 2H , (83) gives us

( )

( )0

12 0

0

12

0

10

1

in ref z

ik Lout z L

dEE E H zik dz

dEE e H z Lik dz

=

=

− = = =

= = = (102)

Since (82) is linear in 1E , we use the rescaling

( ) ( )

( ) ( )

01

2 21

8

ik LoutE z E e u z

IE z u zcπ

=

= (103)

so that our solution proceeds as follows.

For a given for a given intensity I , we first define 8out

IEcπ

= . Then we solve

( ) ( )

( )

22

02 2

222 2

1

||

3 1 32

222

0,cos

1sin cos sin 22

sin 20,

2 cos

a

a

a

d u k udz

d dK K K Kdz dz

Iu

c

εε ε φ

φ φ

ε

φ φ φ

ε ε ε φ

ε ε φ

+ =+

+ + −

+ =+

(104)

subject to the four boundary conditions

( )

( ) 0( )

0 0,

1, .0, z Lduu LL ikdz

φ

φ =

=

= == (105)

Then, we may write

35

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Hong Zhou, Eric P. Choate and Hongyun Wang

( )

( )

0

0

00

00

1 10 ,2

1 10 .2

ik Lout

ik Lout

in z

ref z

duE E uik dz

duE Ei

e

udz

ek

=

=

= +

= −

(106)

As in Section 2, for any value of I, we have the solution with the uniform

orientation ( ) 0zφ = . The corresponding electric field is the same as the case of an

isotropic layer with permittivity ε⊥ . This solution is only stable for values of I less

than some critical intensity 2I . There is a second nonuniform solution that only exists

for a values of I greater than a critical intensity 1I . Unlike the problem in Section 2,

these critical values are not the same, and we have hysteresis with two stable solutions

in the region 1 2I I I< < .

4. Numerical Method and Results

We approximate the orientation angle profile ( )zφ using a truncated Fourier sine

expansion:

( ) ( )0 01

sinK

L kk

z k zz wL L

πφ φ φ φ=

= + − +∑ (107)

In this formulation, the orientation angle profile is represented by a vector of K

components 1 2, , , Kw w w w=

. As a result, the free energy is a function of the vector

w .

To calculate the free energy ( )F w defined as [ ] ( ) ( )( )0

,L

dzF f z zφ φ φ′= ∫ with

the free energy density ( ) ( )( ),f z zφ φ′ given in (94), we first calculate functions

( )zφ and ( )zφ′ from vector 1 2, , , Kw w w w=

on a fine numerical grid.

Next, ( )u z is solved from (104) and (105) on the same numerical grid using the

fourth order Runge-Kutta method. The free energy density ( ) ( )( ),f z zφ φ′ is

36

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Optical Fredericks Transition in a Liquid Crystal Layer

evaluated on the numerical grid from functions ( ) ( ),z zφ φ′ and ( )u z . Finally, the free

energy ( )F w is calculated by integrating the free energy density ( ) ( )( ),f z zφ φ′

given in (94) on the numerical grid.

Once we have a numerical method for calculating ( )F w at each value of beam

intensity I and for each coefficient vector w , we solve numerically ( ) 0F w∇ =

for

steady states. The stability of each steady state is determined by examining whether or

not the Hessian matrix ( )( )H F w is positive definite. In numerical simulations, both

the gradient ( )F w∇ and the Hessian matrix ( )( )H F w are calculated using

numerical differentiation.

The problem is specified by parameters below.

• the anchoring conditions at the two boundaries, 0 , Lφ φ

• the ordinary relative permittivity, 2.45ε⊥ =

• the extraordinary relative permittivity, 3.346ε =

• two Frank elasticity constants, 71 4.5 10 dynK −= × , 7

3 9.5 10 dynK −= ×

• thickness of the layer, 200nmL =

• wavelength of the beam, 0 1.5μmλ =

• light speed, 103 10 cm/sc = ×

• intensity of the beam, ( )2 160.1 0.7GW/cm 0.1 0.7 10 dyn/ cmsI = = ×

The derived parameters are

• aε ε ε⊥= −

• 00

2k πλ

= wavenumber of the beam

37

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Hong Zhou, Eric P. Choate and Hongyun Wang

• 8out

IEcπ

=

Below we study the steady states and their stabilities as a function of the beam intensity

I.

We first consider the simplest anchoring conditions: 0 0Lφ φ= = . For this anchoring

condition, ( ) ( )0 . . 0z i e wφ = =

is always a steady state solution (trivial branch) for any

beam intensity I. Another branch of steady state solution appears at 0.210578I = and

is stable. The trivial branch ( )0w =

remains stable beyond 0.210578I = ; it becomes

unstable at 0.214293I = . The phase diagram is shown in Figure 5. In the figure, the

vertical coordinate is the maximum orientation angle: ( ) ( )max / / 2z

zφ π . There is a

small interval for the beam intensity I in which both the trivial branch and the

non-trivial branch are stable. The system has a hysteresis behavior: when the beam

intensity is increased from a low value the transition from the trivial branch to the

non-trivial branch occurs at 0.214293I = ; when the beam intensity is reduced from a

high value the transition from the non-trivial branch to the trivial branch occurs at

0.210578I = . Figure 6 shows the details of the phase diagram in the small interval for

the beam intensity I where both trivial branch and the non-trivial branch are stable.

5. Conclusion and Future Perspective

The Fredericks transition plays an important role in nonlinear optics and it can

occur under magnetic or electric effects. Even though it has been studied extensively

both experimentally and theoretically, there are still many problems that remain to be

solved. For example, a rigorous mathematical proof on the hysteresis of the Fredericks

transition is still unavailable; the transition for the mismatched boundary conditions

38

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Optical Fredericks Transition in a Liquid Crystal Layer

needs further investigation. To conclude, Fredericks transition will continue to be an

active research subject.

Acknowledgment and Disclaimer

Hong Zhou would like to thank the Office of Naval Research (ONR) for

supporting this work. The views expressed in this document are those of the authors

and do not reflect the official policy or position of the Department of Defense or the

U.S. Government.

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44

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Optical Fredericks Transition in a Liquid Crystal Layer

Figure 1: An illustration of the three common geometries.

45

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Hong Zhou, Eric P. Choate and Hongyun Wang

Figure 2: The solution ( )zφ with respect to / 2π for different values of

dimensionless magnetic field strength / cH H using the one-constant

approximation.

46

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Optical Fredericks Transition in a Liquid Crystal Layer

Figure 3: Phase diagram of the classical Fredericks transition in the one-constant

approximation.

47

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Hong Zhou, Eric P. Choate and Hongyun Wang

(a)

(b)

Figure 4: A schematic diagram of an incident beam on a nematic liquid crystal

layer.

48

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Optical Fredericks Transition in a Liquid Crystal Layer

Figure 5: Phase diagram for the anchoring condition 0 0Lφ φ= = .

( ) ( )0 . . 0z i e wφ = =

is always a steady state solution. A second branch of steady

solution appears at 0.210578I = and is stable. The trivial branch ( )0w =

remains stable beyond 0.210578I = ; it becomes unstable at 0.214293I = .

49

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Hong Zhou, Eric P. Choate and Hongyun Wang

Figure 6: Details of the phase diagram in the small interval where

both the trivial branch and the non-trivial branch are stable.

50


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