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Introduction
Electromagnetic waves travel without interaction amongst themselves in a material with a linear optical response. There would be no energy exchange between
the waves. On the other hand, if the material exhibits a signicant optical
nonlinearity, that would enable energy transfer between the waves. We refer to
such energy transfer as a wave mixing process. Depending on the order of the
nonlinearity, the mixing may involve three waves, four waves or more. Three
wave mixing results in optical parametric amplication and second harmonic
generation. Four wave mixing produces, among other things, third harmonic
generation and optical phase conjugation. To set the stage for discussing these
eects, we rst review the basics of electromagnetism in linear dielectrics and
then show how nonlinear polarization changes the propagation of the waves and
provides coupling between them, ringing about this wave mixing.
Elements of Electromagnetism
The left hand side is convertible into a volume integral according to the
divergence theorem:
I
Z
! !
! !
r E dV
(2)
E dS =
S
The right hand side of Eq. 1 can also be written as a volume integral:
Z
1
1
qencl =
dV
0
(3)
Being true for any volume, the integrands on either side of the above equation
must therefore be equal:
! !
r E =
(5)
0
In a polarized material, the charge density has two parts: (a) a free charge
density f and (b) a bound charge density b . We can consider how the bound
!
charge density is related to the polarization P . To see this, let us write the
!0
potential at a point !
r due to a dipole !
p located at the point r :
V (!
r)=
p rb
1 !
4 0 r2
2
(6)
where rb =
!
0
!
r r
r ,
r
r= !
!0
r ; dening the the unit vector in the direction
of the position vector of the eld point relative to the source dipole. Now if
there is a volume distribution of dipoles in a material, then the potential due
to such a distribution is given by
V (!
r)=
1
4
!
Z !
P r0
r2
rb
dV 0
(7)
! ! !
because the dipole moment in the volume element dV 0 at r0 is P r0 dV 0 .
!
Since r0 1r = rrb2 ( the dierentiation being with respect to the source position
!0
r ), this can be written out as
Z
! !0 1
1
!
P :r
dV 0
(8)
V (r)=
4 0 v
r
Now we have
0
r:
!!
!!
P
= P :r0
r
1! !
+ r0 P
r
1
r
(9)
(10)
(11)
The rst term on the right hand side of the above equation is the potential
due to a surface charge of density
b
!
= P :b
n
(12)
! !
r P
(13)
+
0
(14)
f
and
(15)
Using the expression for the bound charge density given by Eq.13, this results
in
!
r
0E
!
+P =
(16)
!
thereby leading to the concept of the electric displacement D dened by
!
D=
0E
!
+P
(17)
modifying the Gauss law for electric elds in the presence of the polarizable
dielectrics to
! !
r D= f
(18)
For linear dielectrics, of course, we have
!
!
P = 0 E
!
!
!
D = 0 (1 + ) E = E
= r 0
r =1+
(19)
(20)
(21)
(22)
In free space devoid of any material, there is no charge. Maxwells equations for
the elds take the form
! !
r E =0
!
r
!
r
!
E =
!
B =0
!
r
!
B =
(23)
!
@B
@t
(24)
(25)
!
@E
0
@t
(26)
We now wish to develop the dierential equation for the travelling electric
and magnetic elds. Toward this, we use the vector identity
!
r
!
r
!
! ! !
E =r r E
!2 !
r E
(27)
!
r
!
E =
4
!
r2 E
(28)
Taking the curl of the right hand side of the Eq.4.20b, and making use of
Eq.26, we get
!
r
!!
@B
=
@t
!
@ r
!
B
=
@t
!
@2 E
0
@t2
(29)
Thus sing Eq. 28 for the left hand side and Eq.29 for the right hand side,
Eq.24 transforms to
!
!
@2 E
r2 E = 0 0 2
(30)
@t
In a similar way, we transform Eq.26 to give
!
r2 B =
!
@2 B
0
@t2
(31)
These are the two wave equations for the electric and magnetic elds, propagating at the common wave velocity of magnitude
c= p
(32)
0 0
As solutions of the wave equations for the electric and magnetic elds as
given above, let us consider a monochromatic plane wave travelling in the +X
direction with the elds given by
!
!
E = E0 ei(!t
kx)
(33)
!
!
B = B0 ei(!t kx)
(34)
!
!
where the eld amplitudes E0 and B0 are complex and have no variation in
!
!
!
!
! !
E0
E0
B0
B0
x
the Y Z plane. @@y
= @@z
= 0, @@y
= @@z
= 0. Since r E = 0, @E
@x = 0,
@Ey
@y
= 0,
@Ez
@z
E0 i !t !
k !
r
e
c
Taking the real parts, the elds of the wave are given by
!
! !
B ( r ; t) = k
eb
! !
E ( r ; t) = ebE0 cos !t
!
! !
B ( r ; t) = k
eb
! !
k r
E0
cos !t
c
! !
k r
(36)
(37)
(38)
3.1
Per unit volume of space, the energy available in the combined electric and
magnetic elds is given by
u=
p
Since B = Ec and
the total energy density
0 0
1
1 B2
2
0E +
2
2 0
(39)
0E
(40)
On using the real part of the electric eld as given by Eq.37, we have
u=
2
0 E0
cos2 (!t
kx)
(41)
!
Poynting vector S representing the energy transport dened by
!
S =
!
E
!
B
(42)
0
becomes now
or
! b
S = ic 0 E02 cos2 (!t
kx)
! b
S = icu
(43)
(44)
The linear momentum density of the eld (per unit volume) equals
u!
!
p = i
c
Averaging over one cycle of the wave ( cos2 (!t
ties are given by
1
hui = 0 E02
2
D!E 1
S = c 0 E02bi
2
1
2!
h!
pi=
0 E0 i
2c
The intensity of the wave is given by
I = hSi =
1
c 0 E02
2
(45)
kx) = 1=2) these quanti(46)
(47)
(48)
(49)
(50)
! !
r B =0
(51)
!
! !
@B
r E =
@t
!
! ! @D
r H =
@t
For a linear material medium, we have
(52)
(53)
!
!
D= E
(54)
!
!
B
H =
(55)
!
r
!
E =
!
@ r
!
B
@t
(60)
!
r
!
E =
7
@
@t
!
@E
@t
(61)
(62)
This is the wave equation for the electric eld propagating in a linear material
characterized by the linear properties and . There is also a similar equation
!
for the magnetic eld B . The velocity of the waves has the magnitude given by
1
=p
(63)
If, further the material is non-magnetic (i.e. non-ferromagnetic, nonantiferromagnetic, non-ferrimagnetic!), i.e. diamagnetic or paramagnetic, with
close to 0 , we have the wave speed given by
v=p
1
0 r 0
c
=p
(64)
r
p
The refractive index n of the material dened by n = c is thus equal to
r.
The energy density, the Poynting vector and the intensity of the wave now are
given by
1 B2
1
(65)
u = E2 +
2
2
! !
E B
!
S =
(66)
I=
1
2
E02
(67)
5.1
We revert to the Maxwells equations given by Eq.??. Taking the curl of Eq.58,
we have
! !
!
!
@ r B
@ r
H
!
! !
r
r E =
=
(68)
@t
@t
Using Eq.59, this gives
!
!
! !
@2 D
r
r E =
(69)
@t2
or on using the earlier vector identity27, we have
!
!
@2 D
r2 E =
@t2
8
(70)
(71)
!
Since our material now is nonlinear, we write the polarization P as a sum
!
!
of the linear part P (1) and the higher order nonlinear contributions P (N ) :
!
!
!
!
P (N ) = P (2) + P (3) + P (4) + :::
(72)
Thus Eq.71 is re-written as
2!
r E =
!
!
!
@2 E
@ 2 P (1)
@ 2 P (N )
+
+
0
@t2
@t2
@t2
(73)
The rst two terms on the right hand side of the above equation can be
combined and brought to the left hand side as
!
!
!
@ 2 P (N )
@2 E
=
(74)
r2 E
0
0
@t2
@t2
This is the wave equation valid for nonlinear materials. Note that we changed
to 0 , as the materials we choose are nonmagnetic. This nonlinear wave
equation diers from the linear wave equation in the occurrence of the term on
!
the right hand arising from the nonlinear polarization P (N ) . It is this term acting
as source responsible for energy transfer between the coupled propagating
waves.
5.2
!
The rate at which work is done by an electric eld E in creating the polarization
!
P of a material is given by
*
!+
! dP
dW
= E
(75)
dt
dt
where the averaging is over one cycle of the alternating electric eld. The
real parts of the electric eld and polarization may be written as
i
! !
!
1 h! !
E ( r ; t) =
E ( r ) e i!t + E (!
r ) e+i!t
(76)
2
i
! !
!
1 h! !
P ( r ; t) =
P ( r ) e i!t + P (!
r ) e+i!t
(77)
2
Note the amplitudes of the eld and polarization are written as complex and
position-dependent (which could come from the nonlinear wave coupling). The
equation for the average power now becomes on use of the above two equations,
dW
1
= ha + b + c + di
dt
4
9
(78)
!
( i!) P (!
r )e
i!t
i!t
(79)
!
!
b = E (!
r ) e i!t (i!) P (!
r ) e+i!t
!
!
c = E (!
r ) e+i!t ( i!) P (!
r ) e i!t
!
!
d = E (!
r ) e+i!t (+i!) P (!
r ) e+i!t
(80)
(81)
(82)
Of the four terms on the right, two of them (the rst and the last) have
angular frequencies 2! and 2!. On averaging over a cycle these give vanishing
contributions. The second term (b) and the third term (c) are the ones which
need to be considered. Then
! !E
i! D! !
dW
=
E P
E P
(83)
dt
4
In a linear material, the polarization has the same frequency as the electric
eld that creates it so that both the above terms give zero contribution. That
is not however the case with a nonlinear material. We have learnt in an earlier
chapter how to write the Fourier components of polarization of the n - th order
due to a number of electric elds:
!(n) !
P
( r ; !) =
(n)
!
!
i k 1 +:: k n
!
r
(84)
! !
E ( r ; ! i ) = ebi Ei e
ib
ki r
b
(85)
and the angular frequency ! of the polarization satises the photon energy
conservation law:
! = ! 1 + ! 2 + ::: + ! n
(86)
For eective energy transfer to occur over the non-linear material sample,
! !
! !
E P should not be a varying
the power which is proportional to E P
!
function of position r . In other words, the wave vector k should satisfy the
linear momentum conservation condition:
!
!
!
!
k
k 1 + k 2 + :: + k n = 0
(87)
r E =
!
@2 E
+
@t2
10
!
@ 2 P (N )
0
@t2
(88)
(! 1 )
Pi
(x; t) =
+ c:c:
(92)
To come back to the nonlinear wave equation, the term r2 E1i (x; t) of the
nonlinear wave equation, we may note that since the plane wave is travelling
in the x direction, there would be no variation with the y and z directions:
@
@
@y E1i (x; t) = @z E1i (x; t) = 0, with the result
@2
@2 1
E1i (x; t) =
E1i (x) ei(!1 t
2
@x
@x2 2
or
r2 E1i =
1 @ 2 E1i
2 @x2
k12 E1i
2ik1
11
k1 x)
+ c:c:
@E1i i(!1 t
e
@x
k1 x)
(93)
+ c:c:
(94)
6.1
An Approximation
k1
@E1i
@x
(95)
Thus in Eq.94, we omit the @@xE21i term in comparison to the rst derivative
term. The nonlinear wave equation Eq.88 has the left hand side then given by
!
r2 E1i =
1 2
@E1i i(!1 t
k E1i + 2ik1
e
2 1
@x
k1 x)
+ c:c:
(96)
We turn to the terms on the right hand side of Eq.88: The rst term is
0 1
!
@ 2 E 1i
=
@t2
=
i
@ 1h
i! 1 E1i ei(!1 t k1 x) + c:c:
@t 2
i
1h
2
i(! 1 t k1 x)
!
E
e
+
c:c:
1
1i
1
2 0
(97)
0 1
(98)
have
2
0 1 !1
!
@ 2 E 1i
=
1
@t2
1h 2
k E1i ei(!1 t
2 1
k1 x)
i
+ c:c
(99)
This is just equal to the rst term on the right hand side of Eq.96. Since
these appear on either side of the nonlinear wave equation they cancel each
other. Now what is left to be considered is the second term on right hand side
of the wave equation Eq.88. Using Eq.92, we have
0
@ 2 P1i
=
@t2
0 0 ijk E3j
2
0 0 ! 1 ijk E3j
! 2 )g eif(!3
+ c:c:
(100)
! 2 )t (k3 k2 )xg
+ c:c:
(101)
@E1i i(!1 t
e
@x
k1 x)
+ c:c: =
2
0 0 ! 1 ijk E3j
(k3 k2 )xg
+ c:c:
(102)
12
2
0 0 !1
ik1
ijk E3j
i(k3 k2 k1 )x
(103)
i kx
(104)
In a similar manner we derive the gradients of the elds for the other two
waves, using the same approximations and the same mathematical manipulations:
r
@E2k
0
i kx
= i! 2
(105)
0 kij E1i (x) E3j (x) e
@x
2
r
@E3j
0
i kx
= i! 3
(106)
0 jik E1i (x) E2k (x) e
@x
3
In arriving at the above equations, we used the relations ! 1 = ! 3 ! 2 in
the equation for the wave 1, ! 2 = ! 1 ! 3 in the equation for the wave 2 and
! 3 = ! 1 + ! 2 in the equation for the wave 3.
13
Integration yields
E3j = E3j (0)
i2!
ei kx x
j
jik E1i E2k
i k 0
(109)
If at the input end, x = 0, there is zero second harmonic eld, E3j (0) = 0.
To obtain the wave intensity, we need the square of the eld amplitude:
E3j (x) E3j (x) = 4! 2
0 2 2
2
2
0 jik E1i E2k
3
2
E3j
(x) = 4! 2
ei
kx
i k
2
kx
0 2 2
2
2 2 sin
2
E
E
x
0 jik 1i 2k
kx 2
3
2
i kx
i k
(110)
(111)
We can now write down the intensity of second harmonic wave as a function
of position:
r
1
3
2
I2! =
E2!
(112)
2
0
Eq.111 then gives
r
I2! = 2
2
kx
2 2
2
2 2 sin
2
E
E
x
0 jik 1i 1k
kx 2
2
!2
(113)
We note that for a given length x of the crystal sample, the e ciency of
conversion is proportional to 2 , the square of the nonlinear susceptibility and
to the intensity I! of the fundamental wave. Further, the e ciency oscillates as
a function of the position x for k 6= 0. Maximum e ciency is realized if the
phase matching condition k = 0 is satised. Since k = k3 k2 k1 = k3 2k1 ,
the phase matching condition may be phrased as
k2! = 2k!
(116)
2!
(n2!
c
14
n! )
(117)
2!
v2!
lc =
2!c
n2!
n2!
(118)
n!
What is this coherence length? We can see that when the phase matching
condition is not satised, the length of the crystal over which we can realize the
maximum cumulative energy transfer, is the spatial period of the oscillations
arising due the factor f .
7.1
(119)
There are two schemes, denoted as Scheme I and Scheme II, possible for
realizing the phase matching condition. First we detail Scheme I.
Scheme I
In this scheme, the optical anisotropy of uniaxial crystals is exploited. In
a negative uniaxial crystal, like KH2 P O4 , the refractive index of the extraordinary ray is less than that of the ordinary ray at any wavelength for a given
direction of travel. As may be expected, in normal dispersion, the refractive
index (for both the rays) increases with increasing frequency. As a consequence,
when both the fundamental and harmonic waves are both of the same kind (either ordinary or extraordinary), phase matching can not occur. However, if we
launch one of the waves, say, the pump wave as an ordinary ray, and the second
harmonic wave is extraordinary ray, then the refractive indices can be matched
for a certain direction in the crystal, because the speed of the ordinary ray is
isotropic whereas the extraordinary ray speed depends on the direction of travel
in the crystal. Let be the angle made by the rays with the optical axis of the
crystal. Then the refractive index of the extraordinary ray ne ( ) depends on
the angle according to the relation
1
2
fne ( )g
cos2
2
(n0 )
15
sin2
2
(ne )
(120)
c
2
(n02! )
sin2
c
2
(ne2! )
sin
c,
1
(n0! )2
1
fn0! g
(121)
we nd that
1
2
(n02! )
1
2
(n02! )
1
2
(ne2! )
(122)
o
k2;!
e
k1;!
=0
(123)
Since the refractive index of the extraordinary ray depends on the direction
of propagation, which makes an angle wit the optic axis of the crystal, this
condition may be written as
e
o
e
k2!
( ) = k2;!
+ k1;!
( )
!n
c ,
(124)
this becomes
!
!
2! e
n2! ( ) = no! + ne! ( )
c
c
c
or
(125)
1 o
[n + ne! ( )]
(126)
2 !
Substituting the expressions for the angle-dependence of the refractive indices in the above equation yields as the matching condition of Scheme II as
"
# 1=2
(
"
#) 1=2
2
2
cos2 c
sin2 c
1
cos
sin
c
c
=
no! +
(127)
2 +
2
2 +
2
2
fno2! g
fne2! g
fno! g
fne! g
ne2! ( ) =
16
7.2
We have solved the coupled equations Eq.??, describing three wave mixing under
the approximation that the depletion of the pump wave is negligible. We shall
now remove this unnecessary limitation and solve the equations more generally
with the pump wave transferring appreciable amounts of energy to the harmonic
wave.
In order to facilitate an easy handling of the equations, we introduce new
eld terms F1 ; F2 ; F3 dened by
r
r
r
n1
n2
n3
E1 ; F 2 =
E2 ; F 3 =
E3
(128)
F1 =
!1
!2
!3
We recall that the intensity of a wave is the energy per unit area owing
per second. Therefore intensity is also equal to the photon ux multiplied by
photon energy. Photon ux is the number of photons per unit area passing per
second. As such, intensity is proportional to photon ux at a given frequency.
!2
Intensity being proportional to the square of the eld amplitude E , we see
2
our new eld variables are such that F 2 / E! and so are proportional to the
photon ux!
In terms of these new variables F , we may re-write the coupled wave equations Eq.??:
r
dF1
0 !1 !2 !3
i kx
= i
(129)
0 F1 F3 e
dx
n1 n2 n3
r
dF2
0 !1 !2 !3
i kx
=i
(130)
0 F1 F3 e
dx
n 1 n 2 n3
r
dF3
0 !1 !2 !3
i kx
= i
(131)
0 F1 F2 e
dx
n1 n2 n3
Introducing the parameter
r
0 !1 !2 !3
(132)
=
0
n1 n2 n3
the above equations may appear as
dF1
= i F1 F3 e i kx
(133)
dx
dF2
= i F1 F3 ei kx
(134)
dx
dF3
= i F1 F2 ei kx
(135)
dx
For analyzing second harmonic generation, we know that we need to consider only the rst and last of the above three equations. Further, if the phase
matching condition is met, i.e. k = 0, then these equations become
dF1
=
dx
i F1 F3
17
(136)
dF3
= i F12
(137)
dx
Let us choose the pump wave at the input end (x = 0) to be real. Then
F1 (0) and hence F1 (x) become real giving
dF1
=
dx
i F1 F3
(138)
dF3
= i F12
dx
To obtain the solutions of these equations, we set S3
equations become then
dF1
= F 1 S3
dx
dS3
=
F12
dx
These are consistent with
(139)
iF3 . The two above
(140)
(141)
d
F 2 + S32 = 0
dx 1
(142)
(143)
or
since there is no harmonic eld at the input end (S32 (0) = 0). This results
in the equation
dS3
=
F12 (0) S32
(144)
dx
or
dS3
=
dx
(145)
2
F1 (0) S32
Integrating from x = 0, S3 (0) = 0, to x = x, S3 (x), we have
1
tanh
F1 (0)
or
S3 (x) = F1 (0)
S32
F12 (0)
(146)
p
tanh ( xF1 (0))
(147)
jS3 (x)j
jF1 (0)j
= tanh2 [ F1 (0) x]
(148)
18