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by Tsukanov Roman
1
Outline
1. Introduction and definitions
2. Perturbation solution for 1st 2nd and 3rd
order susceptibilities
3. Density matrix formalism
4. Density matrix calculation for 1st and 2nd
order susceptibility
5. Expansion terms representation by
Feynman diagrams
2
Introduction
• Nonlinear optics – field which studies the phenomena which occurs as
a consequence of the modification of the optical properties of a material
by the presence of light
• Only laser light is sufficiently intense to modify the opt. properties of
material system
~ ~ () ~ ()
En En E n
Where
~ () ~ ( ) ~ ( )*
E n E n e i n t En En E n* e imt
by requiring complex conjugate we get the physical field E to be real 4
Formal Definition of the Nonlinear
Susceptibility
definition: An-slowly varying field amplitude
E n An e ikn r
Then the total field
~
E (r , t ) ' An e i ( kn r nt )
n
new notation:
En E ( n ) An A( n )
En ( n ) E * ( n ) An ( n ) A* ( n )
using new notations we can write the field in the more compact form
~ ~
E (r , t ) E ( n )e int A( n )e i ( kn r nt )
n n
5
Formal Definition of the Nonlinear
Susceptibility
According to the new definitions, the field is given by
~
E (r , t ) cos( k r t )
where
1 ikr 1 ikr
E ( ) e , E ( ) e
2 2
1 1
A( ) , A( )
2 2
In similar way we define the nonlinear polarization
~
Pn (r , t ) P( n )e int where the summation runs over the
positive and negative frequencies
n
And finally we define the components of the second order susceptibility as const.
of proportionality relating the amplitude to the product of field amplitude
Pi ( n m ) ijk
( 2)
( n m , n , m ) E j ( n )E k ( m )
jk nm
6
Motivation
Our goal is to calculate explicit expressions for the
Nonlinear optical susceptibility.
7
Schematic representation of the interaction
processes
We may consider the interaction in terms of the exchange of photons between
The various frequency components of the field
Solid lines represents the eigenlevels of the atom and dashed lines –virtual
levels. They represent the combined energy of one of the energy eigenstates
of the atom and of one or more photons of the radiation field.
8
Schematic representation of the interaction
processes
Example – enhancing the efficiency of the 3rd harmonic
generation
(a) – one photon transition Is nearly resonant, (b) – two photon transition is
Nearly resonant, (c) – the three photon transition is nearly resonant
We assume that all of the properties of the atomic system can be described in terms of
the atomic wave function (r,t), which is the solution to the time-dependent
Schrödinger equation
i Hˆ
t
Hˆ Hˆ 0 Vˆ (t )
Hˆ 0 is a free atom Hamiltonia n,Vˆ (t ) the int eraction
of the atom with the electromagnetic field
ˆ ~
V (t ) E (t )
ˆ
erˆ(t )
~
E (t ) E ( p )e p
iw t
p
The sum runs over the positive and negative frequency components 10
Energy Eigenstates
The solution:
i n t
n ( r , t ) u n ( r )e
After substituting to the Shrodinger equation we see that un(r) must
satisfy the eigenvalue equation (time independent S. equation)
Hˆ 0 un (r ) En un (r ), En n
m n r mn
* 3
u u d
11
Perturbation solution to Shrodinger Equation
After substitution we require that the Schrödinger eq. will be fulfilled for
Each order separately. We obtain the set of equations:
( 0)
i Hˆ 0 ( 0)
t( N )
i Hˆ 0 ( N ) Vˆ ( N 1) N 1, 2, 3, ......
t
under assumption that initially the atom is in the ground state, we get
iEg t /
( 0)
(r , t ) u g (r )e
The Nth order contribution to the wave function may be represented as
(remember the Schrödinger picture)
l
13
Perturbation solution to Shrodinger Equation
Then
i a l( N ) u l ( r )e il t l
a ( N 1) ˆ
V u l ( r ) e i l t
l l
We multiply each side of the equation by u* and integrate over all space,
The result is
a m( N ) (i) 1 al( N 1)Vml e
i t ml
,
l
ml m l
Vml um Vˆ ul
As we see – once al(N-1) are determined, by integration we can get the next order
t
a m( N ) (t ) (i ) 1 dt 'Vml (t ' ) al( N 1) e iml t '
l
14
Perturbation solution to Schrödinger Equation
We are interested to determine the linear, second order and third order optical
Susceptibilities. For this we need to determine the probability amplitudes
1 mg E ( p ) i (mg p ) t
a (1)
(t ) e
p mg p
m
1 [ nm E ( q )][ mg E ( p )]
i ( n g p q ) t
a ( 2)
(t ) 2 e
( ng p q )( mg p )
m
pq m
15
Linear Susceptibility
1 gm [ mg E ( p )] i t [ mg E ( p )] mg i t
p (1)
~ ( e p
p
e )
p m mg p mg p
1 gm [ mg E ( p )] [ mg E ( p )] mg i t
p
~ (1)
( )e p
p m mg p mg p
16
Linear Susceptibility
Linear polarization ~
P (1) N ~
p (1)
~
P (1) P (1) ( p ) exp( i p t )
p
Linear susceptibility defined through the relation
Pi (1) ( p ) ij(1) E j ( p )
j
then
N gm
i
mg
j
gm
j
mg
i
ij ( p )
(
m mg p
*
mg p
)
The first and the second terms are the resonant and anti resonant
Contributions to the susceptibility
17
Second Order Susceptibility
~
p 2 0 ˆ 2 1 ˆ 1 2 ˆ 0
Then
Now we may replace q by -q in the second term, q by -q and p by -p in the
third term
18
Second Order Susceptibility
We perform similar steps like we did while deriving 1st order:
~
P ( 2) N ~
p ( 2)
~
P ( 2) P ( 2) ( r ) exp( i r t )
r
After introducing into the standard definition of the 2nd order susceptibility
Pi ( 2) ijk
( 2)
( p q , q , p ) E j ( q )E k ( p )
jk pq
For the case of highly non resonant excitation ng and mg can be taken
To be real, and the expression can by simplified further
Where we used the full permutation operator, defined as the expression summed
Over all permutations of the frequencies p , q and -
The statement that can be made is: the non linear susceptibility of a lossless
Medium possesses full permutation symmetry 20
Third Order Susceptibility
Now we want to treat the 3rd Order.
The dipole moment per atom, correct to third order in perturbation theory is
~
p 3 0 ˆ 3 1 ˆ 2 2 ˆ 1 3 ˆ 0
Then
21
Third Order Susceptibility
We can replace the values of p, q and r by their negatives in those
Expressions where the complex conjugate of a field amplitude appears.
Then
22
Third Order Susceptibility
Like before we let ~
P ( 3) N ~
p ( 3)
~
P (3) P (3) ( s ) exp( i s t )
s
The definition of the 3rd
order susceptibility
Pk ( p q r ) kji
( 3)
( , r , q , p ) E j ( r ) Ei ( q ) E h ( p )
hij pqr
23
Third Order Susceptibility
The illustration of the locations of the resonances we may see in the figure
24
Density Matrix Formalism
25
Density Matrix Formalism
26
Density Matrix Formalism - Introduction
Hˆ Hˆ 0 Vˆ (t )
Where H0 - - the Hamiltonian for a free atom and V(t) – an interaction
field-atom. We make explicit use of the fact that the energy eigenstates
of the free atom Hamiltonian H0 form a complete set of basis functions.
s (r , t ) C ns (t )u n (r ),
n
Hˆ 0 u n (r ) E n u n (r ), m n r mn
u *
u d 3
27
Density Matrix Formalism - Introduction
The coefficient C(t) gives the probability evolution that the atom,
Which is known to be in state s, is in energy eigenstate n at time t.
To determine the time evolution we introduce the expansion into
The Schrödinger equation to obtain
dCns (t )
i u n (r ) Cns (t ) Hˆ u n (r )
n dt n
A *s Aˆ d 3 r s Aˆ s s A s
s
28
Density Matrix Formalism - Introduction
Amn u m Aˆ u n u m * Aˆu n d 3 r
As long as the initial state of the system and the Hamiltonian operator H
For the system are known, the formalism described above is capable of
Providing a complete description of time evolution of the system and all of
Its observable properties.
BUT there are circumstances under which the state of system is not known
In a precise manner.
We define the elements of the density matrix of the system by
nm p(s)Cms*Cns Cm* Cn
s
29
Density Matrix Formalism
30
Density Matrix Formalism
The Density matrix formalism is useful because it can be used to
Calculate the expectation value of any observable quantity
A nm Amn
nm
nm
nm Amn ( nm Amn ) ( ˆAˆ ) nn tr ( ˆAˆ )
n m n
then
A tr ( ˆAˆ )
31
Density Matrix Formalism
s
And we will get
s s*
dp( s) s* s dC dC
nm Cm C n p( s)(Cms* n
m Cns )
s dt s dt dt
Now we assume that p(s) does not vary in time, so the first term vanishes
and use the Schrödinger equation for the probability amplitudes for the
second term evaluation
dC ns i s*
C s*
m C m H n Cs ,
dt
dC ms* i s
C s
n C n Hm Cs* .
dt
32
Density Matrix Formalism
After substitution
i
nm p( s) p ( s )( C s
C
n
s*
H m C s* s
m C H n )
s
Using the density matrix notation we may write
i
nm
( n Hm H n m )
nm
i ˆ ˆ
( ˆH Hˆ ) nm
i ˆ
H , ˆ
nm
The last equation describes how the density matrix evolves in time as the
Result of interactions that are included in H
33
Density Matrix Formalism
•Till now we found how the DM evolves in time as a result of interactions
that are included in H.
• But in addition there are interactions that change the state of the system
and cannot conveniently be included in H.
• One of the ways to include such an effects in the formalism is to add
phenomenological damping terms to the equation of motion. Then
nm
i ˆ
H , ˆ
nm nm ( nm eq
nm )
And the meaning Is that nm relaxes to its equilibrium value nmeq
with decay rate
The additional physical assumption is that
nm
eq
0, for n m
This means that thermal excitation is incoherent process and cannot produce
any coherent superpositions of atomic states 34
Density Matrix - Example
Two-Level Atom:
There are only two atomic states a and b interacting appreciably with the
incident optical field.
The wave function describing s state is given by
35
Density Matrix - Example
DM for the atom is given by
tr( ˆˆ ) ab ba ba ab
As seen the expectation of the dipole moment depend upon the off-diagonal
Elements of the density matrix 36
Perturbation Solution of the Density Matrix
Equation of Motion
The density matrix equation of motion with phenomenological inclusion of
Damping is
nm
i ˆ
H , ˆ
nm nm ( nm nm
eq
)
This equation cannot be solved exactly for physical systems of interest and
We should use the perturbavite technique for solving it:
nm nm
(0)
nm
(1)
2 nm
( 2)
...
Hˆ Hˆ 0 Vˆ (t ),
We suppose that V is
ˆ ~
V ˆ E (t ), given by the electric
dipole approximation
ˆ erˆ
37
Perturbation Solution of the Density Matrix
Equation of Motion
We require that the expansion of will be the solution of the original equation
For any value of the parameter , so the coefficients of each power of must
Satisfy the equation separately (for derivation see Appendix 1). Then
nm
( 0)
inm nm
( 0)
nm ( nm
(0)
nm
eq
)
(1)
nm
(1)
nm
i ˆ ( 0)
(inm nm ) V , nm
( 2) ( 2)
i ˆ (1)
nm (inm nm ) nm V , nm
38
Perturbation Solution of the Density
Matrix Equation of Motion
We use the same assumtion we used before incoherenc e of the thermal exitation precesses :
nm
(0)
nm
eq
nm
eq
0 for n m
nm
(1)
(t ) S nm
(1)
(t )e (i nm nm ) t
nm
(1) (1) ( i
(t ) (i nm nm ) S nm e nm nm ) t
S nm
(1) ( i nm nm ) t
e
then after substitution
S nm
(1)
i ˆ (0)
V , ˆ nm e (i )t nm nm
Or
i ˆ
t
ˆ e (inm nm )t ' dt '
(1) (0)
S nm V (t ' ), nm
39
Perturbation Solution of the Density Matrix
Equation of Motion
Then after substitution S into
i ˆ
t
(t )
(1)
nm V (t ' ), ˆ ( 0) nm e ( inm nm )( t ' t )
dt '
nm
(1)
(t ) nm
(q)
(t ) on the left hand side
ˆ (0) ˆ ( q 1) on the right hand side
40
Density Matrix of the Linear Susceptibility
i ˆ
t
( i n m n m ) t ( i n m n m ) t '
(t ) e
(1)
nm V (t ' ),
ˆ (0)
nm e dt '
Easy to show
i p t
nm E ( p )e
nm
(1)
(t ) 1 ( mm
(0)
nn )
( 0)
p ( nm p ) i nm
41
Density Matrix of the Linear Susceptibility
i p t
mn [ nm E ( p )]e
ˆ (t ) tr ( ˆ (1) ˆ ) nm
(1)
mn ( mm nn )
1 (0) (0)
nm nm p ( nm p ) i nm
We may decompose the dipole moment int o the frequency components :
ˆ (t ) ( p ) e
i p t
nm ( nm p ) i nm
42
Density Matrix of the Linear Susceptibility
N an
i
naj na
i
anj
( p )
(1)
ij
n ( ) i ( ) i
na p na na p na
As we may see the first term is resonant for positive frequencies p .
The second one is antiresonant and can be dropped when p is
Close to one of the resonance frequencies of the atom. Then to good
Approximation the linear susceptibility is given by
N i
j
N i j ( na p ) i na
ij ( p )
(1) an na
an na
( na p ) i na ( na p ) 2 na
2
43
Density Matrix Calculation of the
Second Order Susceptibility
i ˆ
t
( i nm nm ) t
( 2)
nm (t ) e V (t ' ),
ˆ (1)
nm e (inm nm )t ' dt '
( 0) nn
(0)
[ n E ( p )][ m E ( p )]
e i ( ) t
p q
2
[( nm p q ) i nm ][( n p ) i n ]
K nm e
i ( p q ) t
pq
ˆ nm mn
nm
ˆ ( r ) e ir t
r
44
Density Matrix Calculation of the
Second Order Susceptibility
We will with to look at atomic dipole moment oscillating at frequency p+ q
ˆ ( p q ) K nm mn
nm pq
Pi ( 2) ijk
( 2)
( p q , q , p ) E j ( q )E k ( p )
jk pq
45
Density Matrix Calculation of the Second
Order Susceptibility
By comparison of the equalities we obtain
46
Density Matrix Calculation of the Second
Order Susceptibility
47
Density Matrix Calculation of the Second
Order Susceptibility
ˆ
nm n ˆ m
48
References
1. R. W. Boyd, Nonlinear Optics (1992)
2. A. Maitland and M.H. Dunn, Laser
Physics (1969)
49
APPENDIX 1
Perturbation Solution of the Density Matrix
Equation of Motion
nm
i ˆ
H , ˆ nm nm ( nm eq
nm )
Hˆ Hˆ 0 Vˆ (t )
H 0,nm E n nm
Hˆ , ˆ
0 nm
( Hˆ 0 ˆ ˆHˆ 0 ) nm Hˆ 0,n ˆm ˆ n Hˆ 0,m
( E n n m n m E m ) E n nm E m nm
( E n E n ) nm
En Em
nm
i
nm inm nm n m n m nm nm nm )
(V V ) ( eq
nm nm
(0)
nm
(1)
2 nm
( 2)
... 50
APPENDIX 1
Perturbation Solution of the Density Matrix
Equation of Motion
( 0)
nm eq
nm
nm
eq
0 for n m
nm (0)
nm (1)
nm 2 ( 2)
nm ...
nm
( 0)
inm nm
( 0)
nm ( nm
(0)
nm
eq
)
(inm nm ) V , nm
(1)
nm
(1)
nm
i ˆ ( 0)
nm
( 2)
(inm nm ) nm
( 2)
i
Vˆ , (1) nm
51
Appendix 2
Centrosymmetric medium
52