Phase Matching in High

Harmonic Generation
A step towards attosecond spectroscopy…

Submitted by,
Ganguly Smita Omkarnath
M.Sc. Photonics and Biophotonics,
National Centre for Ultrafast
Processes,
University of Madras.
Preface
This project report contains a summary of the work carried out at the
Physical and Inorganic Chemistry Department, Indian Institute of Science,
Bengaluru during the Summer Fellowship Programme (2017) held by the
Indian Academy of Sciences. This project aims to study the phase matching
techniques of High Harmonic generation (HHG) theoretically. In HHG an
intense ultrashort pulsed laser is focussed on a dilute gas with high
ionization potential; the atoms in the gas get ionized and radiate high
harmonics of the incident light. The photon flux generated by this process is
used for attosecond time-resolved spectroscopic studies. The first two
chapters provide the needed theoretical background of nonlinear optics and
HHG. Chapter 3 enlists the results of the simulations conducted for various
experimental parameters and establishes the importance of phase matching
for high efficiency HHG.

Acknowledgements
I would like to thank my guide Dr. Atanu Bhattacharya and my co-
guide Sankhabrata Chandra for their guidance during the project; and the
Indian Academy of Sciences for this excellent opportunity.

1
Contents
1 Introduction to Nonlinear optics . . . . . . . . . . 2
2 Phase Matching in High Harmonic Generation. . . . . 7
3 Phase Matching in HHG using Semi-infinite gas cell :
Simulations . . . . . . . . . . . . . . . . . . . 27
4 Bibliography . . . . . . . . . . . . . . . . . . . . . 37

2
Chapter 1
Introduction to Nonlinear optics
Nonlinear optics is an important branch of physics that studies the optical properties of
matter in the presence of an intense beam of light. In 1960, Maiman invented the first laser that
led to the discovery of second-order harmonic generation by Franken et al in 1961. These
optical properties are ‘nonlinear’ in the sense that they show nonlinear dependence on the
applied field. The nonlinear polarization of a material is given by,
P(t )   0 (  (1) E(t )   (2) E(t )2   (3) E(t )3  ...) (1.1)
Here, P(t) is the nonlinear polarization defined as the number of dipole moments per
unit volume,
 0 is the permittivity in free space and E(t) is the applied electric field.  (1) is the

called linear susceptibility;  and 

(2) (3)
are the second and third order susceptibilities
respectively. Thus P(t) has a nonlinear relationship with E(t). Note that for centrosymmetric
crystals i.e. crystals having inversion symmetry  is equal to zero.
(2)

An example of nonlinear optical process is Second-order Harmonic generation (SHG).

In this process, an incident laser beam of frequency 𝛚 is up-converted to frequency 2𝛚 using
a non-centrosymmetric crystal.

𝛚 𝛚
 (2)
2𝛚

Consider a laser beam, whose electric field is represented as

E (t )  Eeiwt  c.c. (1.2)

is incident on a crystal having nonzero second order susceptibility 

(2)
.The nonlinear
polarization created in the crystal is given by P (2) (t )   0  (2) E 2 (t ) or

P(2) (t )  2 0  (2) EE*   0  (2) E 2ei 2t  c.c. (1.3)

The first term in the above equation does not lead to generation of electromagnetic radiation
(as its second derivative is zero) while the second term contributes a frequency of 2𝛚 that leads
to the generation of second order harmonics in the crystal.

3
 SHG can be physically interpreted as the destruction of two photons of frequency 𝛚
leading to generation of one photon of frequency 2𝛚 in a quantum mechanical process.

The energy level description of the SHG process.

The need for phase matching in SHG arises due to interference between harmonic fields
generated at different positions in the crystal. (blue represents the harmonic field and red
represents the fundamental laser beam)

SHG in a crystal and destructive interference between harmonic fields (inset)

Phase matching condition in SHG:
Let the applied electric field of the laser be a plane wave described by the equation,

E  t   E0ei (0t k0 z ) (1.4)

The nonlinear polarization term generating second harmonics in the crystal is given by,

   
2 2
P(2) (t )   0  (2) E0ei (0t k0 z )   0  (2) E02 ei (0t k0 z )   0  (2) E02ei (20t 2 k0 z ) (1.5)

Now the electric field of the second harmonic beam generated in the crystal by P(2)(t) is given
by,

E  t   E0ei (1t k1z )  E0ei (20t k1z ) (1.6)

Here 2k0 is the wave vector of the nonlinear polarization field and k1 is wave vector of
the second harmonic field. If the k1=2k0 or

4
 k  k1  2k0  0
(1.7)
then the system is said to be phase-matched. Here ∆k is the phase mismatch between the non-
linear polarization field and the harmonic field at position z in the crystal. Now the wave
vectors can be expressed in terms of refractive index as,
0 20
k0  n 0  , k1  n  20  (1.8)
c c
Where n(𝛚) is the refractive index for light having frequency 𝛚. Thus, the phase matching
condition can be written as:
20 
k  k1  2k0  n  20   2 0 n 0   0
c c

k  n  20   n 0   0

 n  20   n 0  (1.9)

However, the refractive index vs 𝛚 plot suggests that the phase matching condition cannot be
achieved due to normal dispersion.

Dispersion of refractive indices of a negative uniaxial crystal

Anomalous dispersion (i.e. the decrease in refractive index with increasing frequency)
can be used to cancel normal dispersion in principle. However, in experiments birefringent
crystals are used to achieve phase matching in SHG. Birefringence is the dependence of the
refractive index on the direction of polarization of the optical radiation. Phase matching is
achieved in birefringent crystals by making the highest frequency wave polarized in a direction
such that it has the smaller of the two possible refractive indices. In a negative uniaxial crystal
the highest frequency wave has extraordinary polarization. Phase matching in birefringent
crystals is further classified as Type I and Type II Phase matching. Consider the nonlinear
conversion process 3  1  2 (for SHG 3 is the second harmonic frequency and 2  1
is the applied frequency). In Type I Phase matching the two lower-frequency waves ( 2 and
1 ) have the same polarization, while in Type II their polarizations

5
are orthogonal. The refractive indices at the three optical frequency must be carefully
controlled. The two most commonly used techniques for phase matching are angle tuning and
temperature tuning.

Angle tuning: In this method the angle of incidence of the fundamental laser beam with respect
to the optical axis ĉ of the uniaxial crystal is fine tuned to achieve the phase matching condition.
Light polarized perpendicular to the plane containing the propagation vector k and the optic
axis is called the ordinary polarization and it experiences the ordinary refractive index no. Light
polarized in the plane containing k and the optic axis is called the extraordinary polarization
and experiences a refractive index ne(θ) that depends on the angle θ between the optic axis and
k according to the relation:
1 sin 2  cos 2 
  (1.10)
ne ( ) 2 ne2 n02

Here ne is the principal value of the extraordinary refractive index. Note that ne(θ) is equal to
the principal value ne for θ = 90 degrees and is equal to no for θ = 0. Phase matching is achieved
by adjusting the angle θ to obtain the value of ne(θ) for which the condition ∆k = 0 is satisfied.

Geometry of angle-tuned phase matching of second-harmonic generation for the case of a

negative uniaxial crystal.

Temperature Tuning: There is one serious drawback to the use of angle tuning.
Whenever the angle θ between the propagation direction and the optic axis has a value other
than 0 or 90 degrees, the Poynting vector S and the propagation vector k are not parallel for
extraordinary rays. As a result, ordinary and extraordinary rays with parallel propagation
vectors quickly diverge from one another as they propagate through the crystal. This walkoff
effect limits the spatial overlap of the two waves and decreases the efficiency of any nonlinear
mixing process involving such waves.
For some crystals, notably lithium niobate, the amount of birefringence is strongly temperature-
dependent. As a result, it is possible to phase-match the mixing process by holding θ fixed at
90 degrees and varying the temperature of the crystal. Hobden and Warner (1966) have given
the temperature dependence of the refractive indices of lithium niobate.

6
Chapter 2
Phase Matching in High Harmonic
Generation
High-harmonic generation (HHG) is a nonlinear process and is one of the most studied
aspects of strong-field physics. HHG is an upconversion process that generates XUV or soft
X-rays from visible and near IR radiation. HHG produces temporally and spatially coherent
radiation and it produces photons with energy as high as 1 keV. It produces laser pulses with
durations in the timescale of femtoseconds and attoseconds. It is also called a table-top laser
system. Applications of HHG include surface and molecular dynamics studies, high-resolution
imaging and attosecond dynamics.
Three step model:
The mechanism of HHG can be explained using a quasi-classical three step model. This
model describes the interaction between the atoms and applied intense laser field. In this model,
the bound electrons first tunnel through the potential barrier under the influence of the applied
oscillating laser field, and thus the atoms get ionized. Then the free electrons are accelerated in
the presence of the laser field in the first half cycle, in the second half cycle the accelerated
electrons are pulled back and they finally recombine with parent ions to emit high-energy
photons.

Three step model of High Harmonic Generation

ADK Model:
Ammosov, Delone and Krainov (ADK model) studied the rate of ionization in HHG for
hydrogen like atoms. The rate of ionization in ADK model is given by,

2 n 1
2  2E   2 E * 
*
3E (t )
wADK  | Cn |   I p exp   (2.1)
 E*  E (t )   3E (t ) 

7
 3
Here E(t) is the applied laser field, Ip is the ionization potential of the atom, E  (2 I p ) and
* 2

1

n  Z (2 I p ) where Z is the residual ion charge after ionization. Here Cn is a constant defined
2

*
22 n
as | Cn | 
2
.
n* (n*  1) n*
In addition, the ionization fraction or probability is calculated from wADK using the expression,

  1  exp(  wADK (t )dt ) (2.2)


Phase matching:
The conversion efficiency of HHG is limited due to the phase mismatch between the
polarization field and the harmonic field due to dispersion in the nonlinear medium. Because
of this phase mismatch, the phase of the fundamental field will shift by π rad relative to the
harmonic field as it propagates. This means that harmonic light generated early in the nonlinear
medium will be exactly out of phase with harmonic light generated a certain propagation
distance later. This dephasing distance is called the coherence length. This destructive
interference limits the total achievable coherent build-up of the harmonic field. In HHG, the
situation becomes complicated for generation at high photon energies (200 eV and above).
Because the laser generating the harmonic light also ionizes the medium, a large dispersion
results from the free electrons. Once the fraction of ionization increases above about 5%,
conventional phase matching techniques are no longer possible. Typical coherence lengths
range from a few millimeters at lower photon energies to a few microns at the highest observed
photon energies. New techniques for raising the conversion efficiency for HHG are crucial to
extending this source to high photon energies. The density of free electrons can also change
rapidly, both in time and in space. In time, the ionization fraction can ramp up rapidly during
the ultrafast pulse. In space, the intensity can vary strongly due to refraction of the plasma and
other nonlinear effects. The dynamic nature of the phase mismatch is difficult to model
accurately, and even more difficult to compensate accurately. In this project phase matching
condition for different dispersion and absorption effects in the medium is discussed. Quasi-
phase matching (QPM) is an alternative method for compensating for the phase mismatch to
improve conversion efficiency.
In experimental High harmonic generation, the photon flux of the XUV beam depends
significantly on the degree of phase matching achieved. In this chapter, the phase matching
condition in high harmonic generation (HHG) is discussed. In the interaction region of the
HHG, there is significant number of gas molecules present. Let us consider a typical interaction
region, where the length of the interaction region is 5 mm long and the diameter is about 50
microns. The length of the interaction region is mainly the Rayleigh length i.e. the length from
the focus position where the beam waist is increased by a factor of √2. The diameter of the
interaction region is depending upon the focal length of the lens so the diameter of the
interaction region is actually the beam waist. With this dimension the volume of the gas cell is
2
 50 106 
 r h  3.14  
2 3 12
  5 10  9.8110 m
3

 2 

8
Assume that the density of the gas in the target cell is 1023/m3. The target gas density is
depending upon the gas pressure of the gas source which can be semi-infinite gas cell, gas jet
or capillary. So in the above example the number of atoms in the interaction region is
9.811012 1023  1012 atoms. Now if each atom emits photon then total number of photon will
12
be 10 . Let’s assume that the energy of each photon is 25 eV then the total pulse energy will
be 25 1012 eV  2.5 1013 eV 4 J . So from this simple calculation we say that if we increase
the number density of the atom (by increasing pressure) then the output pulse energy will also
be increased. But in general if one want to increase the number density of the atom then the
absorption by the atom will also increase and as a result we shall get the energy of the
harmonics in nJ order. Generally the conversion efficiency decreases with harmonic order. For
example conversion efficiency of 15th harmonics is 6.4x10-5 which means if we use 3mJ per
pulse for HHG then the energy will be 3 103  6.4 105 J  192 nJ .

The wave equation:

The harmonics field emitted by atoms at different position in the propagation direction must
be in phase for constructive interference on the detector. The condition for such superposition
is called phase matching. The length over which the harmonic fields are phase matched is
called the ‘coherent length’. The phase of XUV fields is found by solving wave equation for
the field. The medium under consideration is homogenous, isotropic and non-magnetic with no
free charge and no free current. The Maxwell equation for such a medium are

   B 
 E ( r , t )   ( r , t) (2.3)
t

   D 
 B( r , t )  0 ( r , t) (2.4)
t
     
 D ( r , t )  0 or  E ( r , t )  0 (2.5)
  
 B( r , t )  0 (2.6)
   
Where E ( r , t ) is the electric field and B ( r , t ) is the magnetic field, including both the
 
fundamental laser beam and the high harmonic field contribution. D ( r , t ) is the electric
       
polarization which can be written as D( r , t )   0 E ( r , t )  P( r , t ) . Here P ( r , t ) is the electric
polarization. Taking curl of Maxwell first equation we get,

        
   E ( r , t )      B ( r , t )  (2.7)
  t  

 


      
2
  D  
   E( r , t)    E( r , t)   0 ( r , t)
  t  t 
 

9
  

2     D  
 E( r , t)  0 ( r , t) (2.8)
t  t 
 
 
Now using equation (2.8) and definition of D ( r , t ) we can write,

2   2     

 E ( r , t )  0 
2  0
E ( r , t )  P (r ,t) 
t  
2   2   2  
 E ( r , t )  0 0 E ( r , t )   P( r , t ) (2.9)
t 2 t 2
0

   (1)   ( NL )   (1) 
Now P ( r , t )  P ( r , t )  P ( r , t ) where P ( r , t ) is the linear component and it can be
 (1)         ( NL ) 
written as P ( r , t )   0  (1) E ( r , t ) . So we can write P( r , t )   0  (1) E ( r , t )  P ( r , t ) . Now
1
substitute this and c 2  in equation (2.9) to get,
 0 0

2   1 2   2     ( NL )  
 E ( r , t )  2 2 E ( r , t )  0 2   0  E ( r , t )  P ( r , t ) 
(1)

c t t  
2   1 2   2   
  2   ( NL )  
 E ( r , t )  2 2 E ( r , t )  0 2   0  E ( r , t )   0 2  P ( r , t ) 
(1)

c t t   t  
2   1 2   (1) 
2  
 2  ( NL ) 
 E( r , t)  E ( r , t )     E ( r , t )   P ( r , t)
c 2 t 2 t 2 t 2
0 0 0

2    (1)  2    2  ( NL ) 
 E ( r , t )  2 2 E ( r , t )  0 2 P ( r , t ) (2.10)
c t t

1 1  (1)
      , here  is the dielectric constant.
(1)
Where we have used 2
 0 0
(1)
 2 
1  (1)
  2
c c c

 2  ( NL )
In equation (2.10), the term 0 P is source of HHG. This equation is difficult to solve as
t 2
it has four variables. It is easier to deal with in the frequency domain. Fourier series is used to
transform the equation (2.10) from the time domain to frequency domain. The fundamental
laser is considered to be an infinity long monochromatic light.
Using Fourier series the electric field and non-linear polarization can be written as
  qc  
E ( r , t )   Eq ( r , t ) (2.11)
q 1

where qc is the cutoff harmonic order

10
   qc  
P( r , t )   Pq ( r , t ) (2.12)
q 1

Here the qth harmonics components are,

   
iq t
Eq ( r , t )   q ( r )e (2.13)
   
iq t
Pq ( r , t )  pq ( r )e (2.14)

where q  q and  is the angular frequency of the fundamental laser. Putting this in the
Fourier series equation we get,
  qc  
E ( r , t )    q ( r )e
iq t

q 1

  qc  
P ( r , t )   Pq ( r )e
iq t

q 1

Now using equation (2.13) and (2.14) we get,

2
   i t         

   q ( r )e q     0   0 E ( r , t )  P ( r , t )  
  t  t  

2
   i t         i t     
   q ( r )e q     0   0   q ( r )e q   P ( r , t )  
  t  t    
2
   i t   2    i t   2    i t 
   q ( r )e q    0 0 2   q ( r )e q   0 2  Pq ( r )e q ) 
  t   t  
Solving this we get,

         
 2 (1)
   q ( r )   2 (iq )2   q ( r )   0 (iq ) 2  Pq ( r ) 
  c    

         
 2 (1)
   q ( r )   2 q 2   q ( r )    0q 2  Pq ( r )  (2.15)
  c    
 
 (1) is a function of  q so it can be written as  (1) (q ) . P ( r , t ) is generally depends upon total
 
electric field E ( r , t ) and not on the harmonic field.

Equation (2.15) represents the qth harmonic field. Now this equation is modified for linearly
polarized field. In linearly polarized field the Laplacian can be separated for transverse and
longitudinal components with respect to propagation direction. Also in such fields the
polarization and fields are scalar so the modified equation becomes,

11
   2  2       (1) 2     2
 


 T  
2  q
( r )    
q  q ( r )     
0 q  q (r )
P
 z    c
2
   

 2
            
2
T   q ( r )   2   q ( r )   kq 2   q ( r )    0q 2  Pq ( r ) 
  z      

 (1)
Where kq2  2
q 2 is the propagation constant of the qth harmonics. ‘z’ is considered to be
c
the propagation direction. For each harmonic component in a linearly polarized field we can
write,
 2
       2
 
 2
 

2
T   q ( r )   2   q ( r )   kq   q ( r )    0q  Pq ( r )  (2.16)
  z      
This equation can be further simplified by Paraxial approximation. In Paraxial approximation
   
 ikq z
the field and polarization components are represented as,  q ( r )  Aq ( r )e and
   
 ikq z
Pq ( r )  pq ( r )e . The polarization depends on the driving field having propagation constant
k. substitute these in the above equation for a particular harmonics we get,
 2
   ik z      ik z     ik z     ik z 
2
T  Aq ( r )e q   2  Aq ( r )e q   kq 2  Aq ( r )e q    0q 2  Pq ( r )e q 
  z      
 2
 ikq z       ik z       ik z     ik z     ik z 
e T  Aq ( r )    e q Aq ( r )  Aq ( r )(ik q )e q   kq 2  Aq ( r )e q    0q 2  Pq ( r )e q 
  z  z     
 2
       ik z   ikq z 
2      
 ikq z  ik z 2  ikq z
e T  Aq ( r )   Aq ( r )(ikq )e q  e q A ( r )  ik e A ( r )  Aq ( r )( ik q ) e 
  z z z
2 q q q

    ik z      ik z 
kq 2  Aq ( r )e q    0q 2  Pq ( r )e q 
   
Solving this we get,
 2
         i ( k  qk ) z 
T  Aq ( r )   2ikq Aq ( r )   0q 2  Pq ( r )e q 1  (2.17)
  z  

2  
This equation represents the amplitude and phase of the harmonic field at r. here Aq ( r ) is
z 2
ignored since it has value smaller than the other terms.

Phase matching for plane waves:

The wavefont of the laser and harmonic beam is considered as plane wavefont. For plane wave
  
 2
T  Aq ( r )   0 , so equation (2.17) becomes,
 

12
       i ( k  qk ) z 
2ikq Aq ( z )  0q 2  Pq ( A1 )e q 1  (2.18)
z  

Here r is replaced by z and since Aq only depends on z and Pq depends on driving field A1.
Also the propagation constant is written as complex form to include absorption as,
q q
kq   (1) (q )   nR (q )  inI (q )  (2.19)
c c 
nR and nI are the real and imaginary part of the reflective index. Now go back to the equation
(2.18) and doing integration we get
z
   0q 2 z
 

0 z  pq ( A1 )e
i ( kq  qk1 ) z
Aq ( z )dz  i dz
2k q 0

  0q 2 z  
ikq z  q z
Aq ( z )  i
2k q  pq ( A1 )e
0
e dz (2.20)

 q 
 
Where i kq  qk1  i   nR (q )  inI (q )   qk1 
 c 

 q  q
i  kq  qk1   i  nR (q )  qk1   inI (q )  ikq   q
 c  c

Here  q is the absorption coefficient. Since the conversion efficiency of the fundamental laser
    
field to the harmonic field is low, A1 ( z )  0 . Hence the phase of A1 ( z ) does not change with
z
   
z, so the phase of A1 ( z ) is set to be zero and A1 ( z ) is replaced by real quantity A1 ( z ) . The
variation of qth harmonic field amplitude in the propagation direction can be calculated as,

0q 2  z
ikq z  q z
Aq ( z )  i pq ( A1 )  e e dz (2.21)
2k q 0

Special Phase matching conditions:

Perfect phase matching in lossless media:
For high harmonic generation below the ionization threshold of the gas target, the absorption
due to linear photoionization is zero. When absorption and other losses are zero then  q  0 .
The propagation constant then becomes
q
kq  nR (q )
c

13
 q
Consider the general condition kq  nR (q )  qk1 varies with z, equation (2.21) under the
c
condition of  q  0 and the above condition can be written as

0q 2  z
pq ( A1 )  e
ikq ( z ) z
Aq ( z )  i dz (2.22)
2k q 0

The perfect phase matching condition is

d
dz
 kq ( z ) z    p ,q ( z )  q ( z )   0
d
dz
(2.23)

q
Where  p ,q ( z )  nR (q , z ) z is the phase of polarization responsible for generating the qth
c
q
harmonics by the dipoles at position z. q ( z ) z is the phase of the harmonic field generated
c
in front of z when the fundamental field arrives at z. the phase velocities of polarization field
q q
is and the two velocities of fields are the same when
d d
 p ,q ( z ) q ( z )
dz dz
d
 p ,q ( z )  q ( z )   0 . Under this condition the newly generated harmonic wave by non-
dz 
linear polarization at position z is always in phase with the one produces in front of z. the
constructive superposition leads to linear increase of wave amplitude as (from equation 10),

0q 2 
Aq ( z )  i pq ( A1 ) z (2.24)
2k q

Equation 11 is obtained by setting e

ikq ( z ) z
as constant since
d
dz
 kq z   0 then
z

e
 ikq ( z ) z  ikq ( z ) z
e z . in some cases kq does not change in z direction. In this case the parfect
0

phase matching condition becomes k q  0 or kq  qk1  0 . The phase velocities of qth

q q1
harmonic wave is then vq  . so vq  and the phase velocity of the driving laser is
kq kq
1 q1
v1   . If condition kq  qk1  0 is satisfied then the phase velocities are same. Now
k1 qk1
 
the non-linear polarization is pq ( A1 )  d q ( A1 ) N a i.e. the number of dipole moment per unit

volume. d q ( A1 ) is the dipole moment of single atom, Na is the gas density in the gas target. In
high harmonic generation, ionization of gas is unavoidable which turns the medium into a
mixture of plasma and neutral atoms. Thus the atomic density Nais not constant. It is
N a  N (1  p) where N is the field free gas density and p is the ionization probability. The work
amplitude can be written as from (2.24)

14
 kq 
Aq ( z )  i d q ( A1 ) N (1  p ) z (2.25)
2 0

0q 2 0 kq 2 0 kq kq
Here   
2k q 2kq c 2 2 0 0 2 0

The intensity of the qth harmonic is

c 0
I q ( NL)  A *q ( z ) Aq ( z ) (2.26)
2
*
c  kq    kq  
I q ( NL)  0  i d q ( A1 ) N (1  p) z   i d q ( A1 ) N (1  p) z 
2  2 0   2 0 
2
c  kq   
2
 2
I q ( NL)  0    q 1  N (1  p) L
d ( A ) 2 2

2  2 0   

Here we have taken z=L which is the length of gas target.

 ckq2    2
 2
I q ( NL)   d ( A ) N (1  p) 2 L2
 8   q 1 
(2.27)
 0

Intensity increases quadratically with density length product I q   NL  . Experimentally N is

2

 2

easier to change than to vary L. using strong field approximation d q ( A1 )  1010 a.u. which

yield intensity of 107 w/cm2 for N=108 /cm3 and L =1cm. the dipole moment calculated is not
accurate. Also as gas pressure is easily measured in experiment pressure-length product is used
instead of density-length product. The gas density N is directly proportional to pressure P,
I q ( PL)   PL  .
2

Plasma Dispersion:
In HHG due to continuous ionization of the atoms in the gas chamber, plasma is created. Plasma
is electrically neutral i.e. the density of free electrons is equal to the density of positive ions.
While studying phase matching in HHG thus one must consider the dispersion of the fields due
to the free electrons in plasma. The free electrons in plasma undergo oscillatory motion due to
the positive ion field, this phenomenon is called plasma oscillations. The refractive index of
2
 p 
plasma is n p (q )  1    where  p is the plasma angular frequency such that
 q 
N ee2
 p2  where me is the mass of the electron and Ne=Np is the free electron density. Here
 0 me
p 1 i.e.  p q hence the refractive index equation can be approximated as,

15
 2
1  e2 N e
n p (q )  1   p   1  (2.28)
2  q  2 0 me q2

Thus for very high q, n p (q )  1 and the phase velocity of the qth harmonic vq  c . The index
of refraction of the neutral atom is given by

e2 Ne
n p (q )  1   1  na (2.29)
2 0 me r  q2
2

r is the resonance frequency of atom and is determined by excitation energy between the
ground state and first excitation level, Ie.
For harmonics with photon energy much higher than Ie i.e. q r , nq (q )  1 . Finally the
total index of refraction of the gas medium for the driving laser is

e2  N a N 
nr (1 )  1   2  2e 
2 0 me  r  1 1 
2

e2 N  1  p p 
nr (1 )  1   2  2 (2.30)
2 0 me  r  1 1 
2

For harmonic the total refractive index nr (q )  np (q )  nq (q )  1 if q 1.

To fulfill the phase matching condition nr (1 )  nr (q ) i.e. nr (q )  nr (1 )  1 this is possible

1 p p e2 N  1  p p 
only when   0 . Setting  2  2   0 we get,
r  1 1
2 2 2
2 0 me  r  1 1 
2

1
p (2.31)
N  2 2 0 me
1 0 1
na (1 ) e 2

Where N 0  2.5  1019 atoms/cm3 is the gas density of standard gas at room temperatire and
atomospheric pressure. Alternatively one can set the laser intensity such that the ionization
2 2
     
probability p   1  i.e. p   ' 1  . I e'  r is the effective excitation energy. The
 r   Ie 
resonant frequency r can be treated as fitting parameter to match the measured refractive
index.

Pressure (plasma) gradient gas target:

In case of high ionization probability the phase matching is achieved by varying the gas density
in propagation direction. The refractive index of plasma for the driving laser is

16
 e2  N ( z ) p 
nr (1 , z )  1    (2.32)
2 0 me  12 

q q
kq ( z )  nR (1 )  qk1   nR (1 )  1
c c

q
e2  N ( z ) p 
kq ( z )     (2.33)
c 2 0 me  12 

N0 q e 2  N 0 p 
One can design a gas target such that N ( z )  such that kq ( z ) z    which
z c 2 0 me  12 
is independent of z,using this to modify equation (2.21) we get
 q e 2  N 0 P  
0q 2  z i  
 c 2  0 me   2    z
Aq ( z )  i pq ( A1 )  e   1  q
e dz
2kq 0

 q e 2  N 0 P  
0q 2 i 

1  e 
 
 c 2  0 me   2    q z
Aq ( z )  i pq ( A1 )e   1 
(2.34)
2kq

The phase matching is perfect for all harmonics. In this case the phase velocities of polarization
are
q q

d
 p ,q ( z ) d  q z  e 2 N ( z ) P  
 1  
dz dz  c  2 0 me12  

q c

d
 p ,q ( z ) d   e2 N 0 P  
 
c 1  
dz dz   2 0 me12 z  

Hence, in an ionized target the phase velocity of polarization wave is same as c. the pressure
gradient gas target for phase matching is feasible for petawatt level laser. The gas density
decreases in the propagation direction, an array of targets with different applied pressure is
used.

Effect of absorption:
Under the perfect phase matching condition i.e. k q  0 , when the absorption of harmonics by
the gas is taken into account the amplitude is

0q 2 
Aq ( z )  i
2k q
pq ( A1 ) 1  e
 z
 q
 (2.35)

17
 1
The absorption coefficient  q  is for the qth harmonic. La is the absorption length defined
2 La
1
as the distance over which the transmission of light power is reduced by  0.368 .
e
1 1
La   where  q is the absorption cross section for qth harmonic.
2 q N q

0q 2   
z

Aq ( z )  i pq ( A1 ) La 1  e 2 La  (2.36)
kq  
 

For z La , Aq ( z ) is maximum.

Absorption limit: the maximum value of harmonic intensity is called the absorption limit and
is given by

 ckq2    2
 2
I q (max)   N (1  p) 2 La 2
 8   q 1 
d ( A ) (2.37)
 0

 ck 2   2

Or, I q (max)   q   d q ( A1 )  (1  p) 2 2
1
 8    q
 0
Where  q  2req f2 (q ) the photo-ionization cross section, here is f 2 (q ) is imaginary part of
atomic scattering factor and re is classical electronic radius. The absorption length-density
1
product defined as La N  or absorption length pressure product defined as
q
N 1
La P  La  . Both the products depend only on the type of atom and harmonic order
N0 N0 q
and don’t depend on target parameter like size and pressure. The dependence of harmonic
intensity on the length pressure product is given by,
LP LP
 
I ( LP )  I max (1  e La P
 2e 2 La P
) (2.38)

Makers Fringes:
In lossless media when kq  0 and kq does not change with z

0q 2  z
pq ( A1 )  e dz
k z
Aq ( z )  i q

2k q 0

0q 2   eikq z  1 
Aq ( z )  i pq ( A1 ) 
 ik 
(2.39)
2k q  q 

18
 q e 2  p 1 p 
Where kq   2 2  N , the corresponding intensity is
c 2 0 me  1 r  12 

c 0
I q ( NL)  A *q ( z ) Aq ( z )
2
*
c 0  0q   eikq z  1    0q 2   eikq z  1  
2

I q ( NL)   i pq ( A1 )    i 
 ik  
pq ( A1 ) 
2  2k q  2 k  ik  
 q   q  q 

c 0  0 q  *  eikq z  1  eikq z  1 
2 4

I q ( NL)  i  pq ( A1 ) z (i ) pq ( A1 ) z  
2  2kq2  i k z  ik z 
 q  q  zL

After putting z=L we get,

2
 q 
ik L ikq L

eikq L
 1  e 1  1  e
 ikq L
e
ikq L  ikq L
1 e 2 e 2  2
kq L 
 
        sin c  2 
 ikq L  ikq L  kq2 L2  kq L   
 

 ck 2   2
 k L 
So, I q (max)   q   d q ( A1 )  N 2 (1  p) 2 La 2 sin c 2  q  (2.40)
 8   
 0  2 

The dependence of normalized harmonic intensity on density-length product is called Maker


Fringe. The dephasing effects show up when the medium length L  Lc  . The coherent
kq
length and pressure product is given by
P 
( LP ) c   (2.41)
k q  q e 2  P 1 P  
  2 2 2 
N0 
 c 2 0 me  1 r  1  
The harmonic intensity is given by

 ckq2    
2
  LP 
I q ( LP)     d q ( A1 )  N 0 2 (1  p) 2 ( LP) 2 sin c 2   (2.42)
 8   
 0  2 ( LP)c 

Maker Fringes are obtained in second harmonic generation crystal. In HHG Iq changes with
pressure when L is fixed.

Rule of thumb for optimizing XUV photon:

When both phase mismatch and absorption effect are considered, assuming kq is independent
of z,

0q 2  z
 i ( k  ) z
Aq ( z )  i pq ( A1 )  e q q
dz
2k q 0

19
 0q 2   eikq z e q z  1 
Aq ( z )  i pq ( A1 ) 
 ik   
(2.43)
2k q  q q 
Now the harmonic intensity I q  A*q ( z ) Aq ( z ) and considering ,

e ikq L  q L
e 1 e   ikq L  q L
e 
1  e
2 q L
e
ikq L
.e
 q L
e
 ikq L  q L
e 1

 1
Using k q  and  q  we get,
Lc 2 La

L
 i L i L
 L
  
 
ikq L  q L  ikq L  q L
e e 1 e e 1  e La
  e Lc  e Lc  e 2 La  1
 
 

L 
L L

e  
 
i k q L   q L  i k q L   q L
e 1 e e 1  1 e La
 2e 2 La
cos   (2.44)
 Lc 

  
  
 i.e.  ikq   q  ikq   q  we get,
1 1
and solving  
 i   1  i   1 
 L 2 L  L 2 L 
 c a  c a 

4 L2a
 ik q   q  ik q   q   2
(2.45)
L 
1  4 2  a 
 Lc 
From equations (2.43), (2.44) and (2.45) one can conclude that I q  A*q ( z ) Aq ( z ) can be written
as,

 
LP

LP
  LP  
I q ( LP)  I max ' 1  e La P
 2e 2 La P
cos   (2.46)
  ( LP)c  

 
 
 1 
Where I max '  I max  2 
(2.47)
 1  4 2  La P  
   
  ( LP)c  

From the plot of output photon flux versus La for different values of Lc it is apparent that

1. The medium length L  Lc

2. Lc  5La by improving phase matching
3. Point 1 and 2 are rule of thumb to generate more than 50% of the maximum photon flux

For a given target gas density the absorption length is determined by the high harmonic photon
energy.

20
Intensity distribution effects in the propagation direction:
According to the strong field approximation the dipole moment can be expressed as
 
d q ( I1 )  d q ( I1 ) eiin ( I1 ) (2.48)

Where I1 is the intensity of the laser and in is the intrinsic dipole phase that depends on I1.
Now the phase variation of polarization can compensate for the phase change due to ionization.
Taking in consideration the variation of laser intensity in z direction in a lossless media
( q  0) the intensity for the qth harmonics can be written as,

0q 2 z 
 pq  I1 ( z )  e dz
ik z
Aq ( z )  i q

2k q 0

0q 2 z 
N  1  P( z )  d q  I1 ( z )  ei e dz
ik z
Aq ( z )  i in q
(2.49)
2k q 0

Perfect phase matching occurs when the total phase in  I1 ( z )   kq z is independent of z i.e.
constant. The intrinsic phase is expressed as in   I1 . the proportionality constant  depends
on the quantum trajectories. In high ionized gas the refractive index for 1 is predominantly
from plasma contribution.

e2 N e
n p (1 )  1 
2 0 me 12

q e2 P 
kq  N this we have obtained from kq  1 nR 1   qk1
c 2 0 me 1 c

For perfect phase matching condition of harmonic order q, the laser intensity is controlled so
that it decreases linearly with z i.e.
I1 ( z )  I1 (0) 1   z  and  I1 (0)  kq

q e 2 PN 1
 (q) 
c 2 0 me 1  I1 (0)

In this case the phase velocity of polarization are

q q

d
 p ,q ( z ) d  q  e2 N 0 P  
 I1 ( z )  1   z
dz dz  c  2 0 me12 z  

21
 q q
 c (2.50)
d
 p ,q ( z ) d  q  e2 N 0 P  
 I1 (0) 1   (q) z    1  2  
z
 2 0 me1 z  
dz dz  c

Here P is independent of z. quasi phase matching is possible in HHG by using a second weak
beam with opposite propagation direction.

Phase matching for Gaussian Beams:

For beams with small divergence angles, under the paraxial approximation and assuming the
laser light is monochromatic, the equation for the fundamental wave is,

  
 2    
T  A1 ( r )   2ik  A1 ( r )   0
  z  
The laser beam is considered to be a Gaussian beam to describe the fundamental laser
propagation and neglect the plasma defocusing. The electric field is then expressed as
r2 r2
    ( z ) i
A1 (r , z )  A0 0 e   e 2 R ( z ) ei ( z )
2
(2.51)
 ( z)

A0 is the amplitude of the field at the laser focus and on the axis, 0 and  ( z ) are the radius
of the beam at the focus and at position z respectively, R( z ) is the radius of curvature of
02
wavefont and  ( z ) is the Gouy phase. By introducing the Rayleigh length, z R  also
1
 z 
2
 z 
2
r
z 2 i
 ( z )  0 1    , R( z )  z  R and  ( z )  tan 1   . The term e 2 R ( z ) is the radial
 zR  z  zR 
phase factor it accounts for phase shift due to measuring a spherical surface along a plane.
When the laser beam is Gaussian the harmonic field should have axial symmetry. The wave
equation for the qth harmonic is rewritten as

 q  
2
d  i  2   ikq z
Aq (r , z )   T  Aq (r , z )   i  Pq (r , z )  e
dz 2k q   2k q  

 0q
2
d  i  2     ik z
Aq (r , z )   T  Aq (r , z )   i N (1  p)  d q  A1 (r , z )   e q (2.52)
dz 2k q   2k q   

Where the dipole moment is

r2

    i I ,( r , z ) iqk1 2 R ( z ) iq ( z )
d q  A1 (r , z )   d q  A1 (r , z )  e in  e e
   

On axis phase matching without plasma and gas dispersion:

Consider the atoms placed on the axis. The phase difference between the polarization
wave and harmonic field is

22
  p ,q ( z )  q ( z )  in  I1 ( z )  q ( z)  kq ( z) z (2.53)

For the Gaussian beam

 I0  z 
 p ,q ( z )  q ( z )   q tan 1    kq ( z ) z
2
(2.54)
 z   zR 
1  
 zR 

q e 2  P ( z ) 1  P ( z )  d  z 
Where kq ( z )   2  2 2 
N . since q tan 1    0 thus Gouy phase
c 2 0 me  1 r  1  dz z 
 p
increase the phase velocity of polarization wave. The degree of phase matching can be
d
 p ,q ( z )  q ( z )  . Now ignoring the phase mismatch due to
dz 
evaluated by the magnitude of

plasma and neutral atom dispersion , i.e. kq ( z )  0 , the derivative of phase is,

d 2 z I 0 q
 p ,q ( z )  q ( z )     (2.55)
dz   z 2 
2
  z 2 
 1     z r  1     zr
2
  zR     zR  
   
2
d  
If  p ,q ( z )  q ( z )   0 then it implies 2 z I 0  qzr  q  z  zr  0
dz  zR 
2
 z  2 I 0 z
i.e.    1  0 (2.56)
 zR  q zR

2 2
 z  I I 
The solution to equation (2.56) is    0   0   1 this gives the location of gas
 zR  q  q 
q
target for phase matching. In this equation I 0  is the condition for the solution to be real.

Now for short trajectories   110 cm / w . Thus the peak intensity of the fundamental
14 2

q
laser I 0 must be higher than  q  10 w / cm for a working solution. For the long trajectories
14 2


  25 10 cm / w the peak intensity must be higher than q 1013 w / cm2 . Thus at the same
14 2

laser intensity, the order at which the harmonics is phase matching is different for the
trajectories. This provides a scheme for selecting the contribution of a particular quantum
q
trajectory. The lowest required intensity for perfect phase matching is I 0  which implies

z  z R . This means that the target should be located on Rayleigh range away from the laser
focus. When a finite gas target is located after the laser focus, the intrinsic dipole phase decrease
with z whereas the Gouy phase increases with z. these phases tend to cancel with each other on
the contribution to the total polarization phase, which results in good phase matching. When a
thin target is placed in the laser focus i.e. z  0 ,

23
 d q
 p ,q ( z )  q ( z )  
dz   z 2 
 1     zr
  zR  
 

This is independent of  , i.e. phase matching is the same for long and short trajectories
implying that z  0 is the best location to observe emission from both trajectories. For z  0

  z 2 
 1     zr
   zR  
q   0
d I z
 p ,q ( z )  q ( z )   0
(2.57)
dz   z   2 2
  z  2

1     z r 2  1     zr 2
  zR     zR  
   

This larger than that for z  0 . Thus, the harmonic generation in this region is not efficient.

On axis phase matching without neutral gas dispersion:

Consider the case such that the ionization probability is high enough so that the effect of plasma
dispersion is much larger than the neutral gas. Then,

q e 2  N 
kq ( z ).z    p( z ) z (2.58)
c 2 0 me  12 

d  e2  N  d
So,  kq ( z ).z   q    p( z ) z  (2.59)
dz c 2 0 me  12  dz

Now p( z ) strongly depends on I1 ( z ) . I1 ( z ) decreases with z for z  0 hence the product p ( z ) z

d
decreases as z increases. ( p( z ) decreases drastically as z increases hence  kq ( z ).z   0 )
dz 
Therefore the plasma dispersion and intrinsic phase work together to cancel out the phase
mismatch effects cause by Gouy phase (>0). Thus when plasma contribution is included, lower
laser intensity is required for phase matching. [without plasma dispersion I0 was estimated to
be  10 w / cm for perfect phase matching]. Now the Gouy phase,
14 2

 z 
 ( z )  tan 1   (2.60)
z
 p 
d 1 1
q 2
(2.61)
dz zR  z 
1  
 zR 

24
 d 1 d
Now at z  z R , q . Experiments have zR  2.5mm typically. This gives  0.2q
dz 2 zR dz
e2 N 1
mm . For   800nm and 1 torr gas pressure,
-1
   0.074mm .
2c 0 me  1 

d d
 kq ( z ) z   0.074qP  p ( z ) z  / mm (2.62)
dz dz
d
Here P is in torr. If P  p( z ) z   1 then plasma dispersion can efficiently cancel Gouy phase
dz
effects.

e2 N e2  PN 0  1
Here       0.074mm here P is in Pascal
2c 0 me  1  2c 0 me  1P0 

Let us assume
m
 I ( z )  I th 
p( z )   1  (2.63)
 I s  I th 

Where I th and I s are the threshold and saturation intensities respectively. When m  4 ,
Is
I th  , for z  z R
10

I 0 dI1 ( z )  2 
I1 ( z )   ( z  z R )  I 0 1  
2 dz zR  2 zR 

Is  2 
When I th  and I1 ( z )  I 0 1   we have
10  2 zR 
m m
 zI 0 I s   z 
 I 0  2 z  10   I  0.1I I0
2 zR 
p( z )   R
  0 s
 
 Is  s
I   0.9 I s 0.9 I s 
   
 10   
m m
 I   0.1I s z 
p( z )   0  1    (2.64)
 0.9 I s   I0 2 zR 

 I 0   0.1I s z  
m m m 1
d z   1   0.1I s
p( z )     1     m   z  1    
dz zR  0.9 I s   I0 2 zR   2 zR   I0 2 zR  
 z  zR

 I 0   1 0.1I s  m  1 0.1I s  
m m m 1
d
p( z )             0.1
dz zR  0.9 I s   2 I0  2 2 I0  


25
Thus the effect of plasma dispersion is comparable to the Gouy phase effects for P  10torr

Off axis phase matching:

For atoms located off axis we need to take into account the dipole phase change in the radial
direction.
r2
02  
in (r , z )    I1 (r , z )    I 0 2 e
2
(z)
(2.65)
 ( z)

02 02 2
i.e. in (r , z )   I 0   I r
 2 ( z) 0
 4 ( z)
the second term is a parabolic phase that makes the harmonic beam diverge as increases. As
 for short trajectories is less than long trajectories, the beam emitted by the short trajectories
is more concentrated near axis (less diverged) and can be filtered out by using an iris. Assuming
0
kq  q is constant for harmonic beam i.e. harmonic beam is close to plane wave. In this
c
case,

 I0  I0  z   1  2
 p ,q ( z )  q ( z )    r 2  q tan 1    kq (r , z ) z   qk1
2 R( z ) 
r
  z     z  
2 2
 zR  
1     1    
  zR     zR  
   
When the gas is significantly ionized by the laser, a plasma gradient is formed transverse to the
propagation axis. The on axis plasma density is higher than the off axis region. The variation
of index of refraction due to plasma changes  p,q ( z)  q ( z)  . In case of terawatt and petawatt
laser is used to generate attosecond pulses the focal spot is sufficiently large. One can vary the
gas density distribution in both transverse and propagation direction to optimize
 p,q ( z)  q ( z)  for phase matching over large spatial region.

26
Chapter 3
Phase Matching in HHG using Semi-infinite
gas cell : Simulations
The phase matching conditions discussed in Chapter 2 are used for simulations in this
chapter. The harmonic intensity is calculated under different experimental conditions for the
semi-infinite gas cell method of HHG.

Simulations for Plane Waves:

The calculations in this section are done for the following experimental parameters and
assumptions:
 The fundamental laser has wavelength 800nm and output intensity ∼ 1014W/cm2.
 The gas medium used is Argon having ionization potential 15.759 eV.
 The laser beam is assumed to have a plane wavefront.
 The gas density in the target is assumed to be uniform.
 The value of dipole moment for an atom is taken from the Strong-field approximation
result |dq(A1)|2∼10-10 atomic unit.

The results of the study for Plane waves are listed below:
I. For a lossless medium, harmonic intensity Iq is plotted for different harmonic orders q
using the equation,

 ckq2    2
 2
I q ( NL)   N (1  p) 2 L2
 8   q 1 
d ( A ) (3.1)
 0
qw1
where kq  nR ( wq ), wq  qw1
c
The values used for the plot are:
2
 
For Argon, p  0.038 ,  d q ( A1 )   1010 a.u.  8.4778 10 40 Cm , N is taken as 1014m-3,
 
L  1cm , w1  2.356 10 Hz and nR ( wq )  1
15

After substituting the above values the equation reduces to,

I q  (2.0494 1017 )q 2

27
The plot of normalised harmonic intensity (Iq) versus harmonic order (q):

1.0

Harmonic Intensity (Normalized)

0.8

0.6

0.4

0.2

0.0

0 20 40 60 80 100
Harmonic order

II. For a lossless medium, harmonic intensity Iq versus harmonic order q is plotted for
different gas pressures P using the equation,

 ckq2    
2

I q ( P)   ( N 0 P) 2 (1  p) 2 L2
 8   q 1 
d ( A ) (3.2)
 0
qw1
where kq  nR (q ), q  q1
c
The values used for the plot are:
2
 
For Argon, p  0.038 ,  d q ( A1 )   1010 a.u.  8.4778 10 40 Cm , N 0  2.5  1019 atom / cm3 ,
 
L  1cm , 1  2.356 10 Hz and nR (q )  1
15

The plot of harmonic intensity Iq versus the harmonic intensity q for different values of gas
pressure P (100 torr, 150 torr and 200 torr):

P=100 torr
P=150 torr
P=200 torr
1.0
Harmonic Intensity (Normalized)

0.8

0.6

0.4

0.2

0.0

0 20 40 60 80 100
Harmonic order

28
III. For a medium having absorption length La the harmonic intensity Iq is given by,
2
c q 210  
L

Iq    
2 2 2 2 2 La ( Eq )
| d ( A ) | N P L ( E ) 1 e (3.3)
2 1  nI2 ( Eq )
q 1 0 a q
 
 
1 1
Where nI ( Eq )  and La ( Eq )  ,  q ( Eq ) is the photo-absorption cross
La ( Eq ) PN 0 q ( Eq )
section calculated using an empirical formula and Eq  1q .

The values used for the plot are:

2
 
For Argon, P  200torr  26664.4Pa ,  d q ( A1 )   1010 a.u.  8.4778 10 40 Cm ,
 
N 0  2.5  10 atom / cm , L  25cm and 1  2.356  1015 Hz .
19 3

The intensity Iq versus harmonic order q plot considering only effect of absorption (no phase
mismatch) by the medium is as follows:

1.0
Normalised Harmonic Intensity

0.8

0.6

0.4

0.2

0.0

0 20 40 60 80 100
Harmonic order

IV. Using the Rule of Thumb for optimizing HHG signal, the harmonic intensity in a
medium having absorption length La and coherent length Lc is given by,

 
 
c0 q 212    LP  
LP LP
2 2 4 L2a  
I q ( LP)  2
| d q ( A1 ) | N 0 P  2 
1 e La P
 2e 2 La P
cos  
8
 1  4 2  L P   
  ( LP)c  
  
a

  ( LP ) c  

(3.4)

29
The values used for the plot are:
2
 
For Argon, P  200torr  26664.4Pa ,  d q ( A1 )   1010 a.u.  8.4778 10 40 Cm ,
 
1
N 0  2.5  1019 atom / cm3 , L  25cm , 1  2.356  1015 Hz and La ( Eq )  ,  q ( Eq ) is
PN 0 q ( Eq )
the photo-absorption cross section calculated using an empirical formula and Eq  1q .

The plot of intensity Iq versus harmonic order q taking into account both phase mismatch and
absorption is shown below:

1.0
Normalised Harmonic Intensity

0.8

0.6

0.4

0.2

0.0

0 20 40 60 80 100
Harmonic order

Simulations for position dependency of different dispersion terms:

For phase matching it is necessary to consider all the factors causing dispersion in the
medium. The dispersion factors for the 23rd harmonic order of argon are calculated for
different laser focus positions. The total phase mismatch ∆k can be expressed as:
k  k g  k p  kd  kn (3.5)

4
2.0x10

4
1.5x10

1.0x10
4 kd
5.0x10
3
kg
)

0.0
kn
-1
k (m

3
-5.0x10
kp
4
-1.0x10

4
k
-1.5x10

4
-2.0x10

4
-2.5x10
-10 -5 0 5 10
Position z (mm)

30
 Where,
1 q
kg   2
(3.6)
 z  zr
1  
 zr 

-2000

-4000
kg(m )
-1

-6000

-8000

-10000

-12000
-10 -5 0 5 10
Position z (mm)

∆kg is the phase mismatch due to Gaussian beam phase gradient, here z is the displacement
from the focus position of the laser beam, zr is the Rayleigh length and q is the harmonic
order.

P q2 1
k p   N atm re 0 (3.7)
Patm q

-1050

-1100
kp(m )
-1

-1150

-1200

-10 -5 0 5 10
Position z (mm)

∆kp is the phase mismatch is due to plasma dispersion, here  is the ionization fraction,
N atm is the atomic number density at standard temperature, re is the classical electron radius,
P is the gas pressure, 0 is the wavelength of the fundamental laser, Patm is the atmospheric
pressure.

31
 2 q P
kn   (1   ) (3.8)
0 Patm n

3900

3800

3700
 kp(m-1)

3600

3500

3400

3300

-10 -5 0 5 10
Position z (mm)

∆kn is the phase mismatch is due to neutral gas dispersion, here  n is the difference in
refractive indices for fundamental and harmonic wavelengths.
8z
kd  2
q I0 (3.9)
  2 z 2 
b 1    
2

  b  

20000

15000

10000

5000
kd (m )
-1

-5000

-10000

-15000

-20000
-10 -5 0 5 10
Position z (mm)

∆kd is the phase mismatch is due to atomic dipole phase, here  q is the coefficient related
to electron trajectories and I 0 is the intensity of the fundamental laser.

32
Simulations for Gaussian beam:
The Gaussian beam is assumed to have electric field,

E (t )  E0 cos(t )e  at
2
(3.10)

2 ln 2
Where a  , t is the FWHM of the pulse. In the simulations, t  40 fs and
t
  2.35 1015 s 1 .
The calculations are done for a Gaussian beam having electric field and temporal intensity
profile as follows:

1.00E+011

8.00E+010
Electric field E(t) (V/m)

6.00E+010

4.00E+010

2.00E+010

0.00E+000

-2.00E+010

-4.00E+010

-6.00E+010

-8.00E+010

-1.00E+011
-100 -50 0 50 100

Time t (fs)

1.0

0.8
Intensity profile

0.6

0.4

0.2

0.0

-100 -50 0 50 100

Time t (fs)

The ionization rate and ionization fraction for Argon atom are calculated using the ADK model.
The rate of ionization in ADK model is given by,

33
 2 n 1
3E (t )  2E*   2 E * 
wADK  | Cn |2   I p exp   (3.11)
E *
 E (t )   3E (t ) 
3
Here E(t) is the applied laser field, Ip is the ionization potential of the atom, E *  (2 I p ) 2 and
1

n  Z (2 I p ) 2 where Z is the residual ion charge after ionization. Here Cn is a constant defined
*
22 n
as | Cn | 
2
.
n* (n*  1) n*
For argon, | Cn |2  4.11564 and I p  15.759eV  0.5791hartree .
In addition, the ionization fraction or probability is calculated from wADK using the expression,
t'
 (t ' )  1  exp(  wADK (t )dt ) (3.12)

Where the lower limit is -100 fs and the upper limit t’ is changed from -100 fs to +100 fs.
The results of the simulations are:

2.00E+012
Ionization rate WADK(t)

1.50E+012

1.00E+012

5.00E+011

0.00E+000

-100 -50 0 50 100

Time t (fs)

1.0

0.8
Ionization fraction 

0.6

0.4

0.2

0.0

-100 -50 0 50 100

Time t (fs)

34
 Then the dispersion terms are calculated using the formulas listed above, and coherent

length is given by Lc  . The results of the simulations are:
| k|

5000
0

4000 -1000
neutral atom dispersion (m )
-1

plasma dispersion (m )
-1
-2000
3000

-3000
2000

-4000

1000
-5000

0 -6000

-100 -50 0 50 100 -100 -50 0 50 100

Time t (fs) Time t (fs)

-9400

-9600
14000

geometric phase dispersion (m )

-1
dipole phase dispersion (m )
-1

-9800

-10000
13500
-10200

-10400
13000
-10600

-10800
12500
-11000

-11200
12000
-11400
-100 -50 0 50 100 -100 -50 0 50 100
Time t (fs) Time t (fs)

8000 0.014

0.012
6000
total dispersion (m )

0.010
-1

4000
coherent length (m)

0.008

2000
0.006

0 0.004

-2000 0.002

0.000
-4000
-100 -50 0 50 100 -100 -50 0 50 100
Time t (fs) Time t (fs)

Next using the one-dimensional model the number of photons emitted on axis per unit time
and area is given by,

 
 
   LP 
LP LP
2 2 4 L2a  
N out  P Aq  2 
1 e La P
 2e 2 La P
cos   (3.13)
 1  4 2  La P     ( LP)c  
   
  ( LP)c  

35
 Using the above equation, the pressure dependence of harmonic intensity is plotted for
different medium lengths for the 23rd harmonic order in argon.

Lmed=0.005m
4000

3500

3000

Harmonic intensity
2500

2000

1500

1000

500

-500
0 20 40 60 80 100

P(torr)

Lmed=0.05m
80

70

60
Harmonic intensity

50

40

30

20

10

-10
0 20 40 60 80 100

P(torr)

36
Bibliography
 Fundamentals of Attosecond Optics -CRC Press (2011) by Zenghu Chang.
 Nonlinear Optics (Third Edition) by Robert Boyd.
 Bellini, M., C. Corsi, and M. C. Gambino. "Neutral depletion and beam defocusing in
harmonic generation from strongly ionized media." Physical Review A 64.2 (2001):
023411.
 Niu, Yong, et al. "Pressure-dependent phase matching for high harmonic generation of
Ar and N 2 in the tight focusing regime." Optics Communications 397 (2017): 118-121.
 Wang, Feng, et al. "Time-dependent phase matching of high-order-harmonic
generation." Physical Review A 92.6 (2015): 063839.
 Steingrube, Daniel S., et al. "Phase matching of high-order harmonics in a semi-infinite gas cell."
Physical Review A 80.4 (2009): 043819.
 Constant, E., et al. "Optimizing high harmonic generation in absorbing gases: Model
and experiment." Physical Review Letters 82.8 (1999): 1668.
 Gibson, Emily A., et al. "High-order harmonic generation up to 250 eV from highly
ionized argon." Physical Review Letters 92.3 (2004): 033001.

37