Second-harmonic generation,

Phase-matching bandwidth, and

Group velocity mismatch (GVM)
Phase-matching in SHG
Phase-matching bandwidth
Group-velocity mismatch
Nonlinear-optical crystals
Practical numbers for SHG
Electro-optics

Phase-matching in Second-Harmonic
Generation

How does phase-matching affect SHG? Its a major effect,

one of the most important reasons why you just dont see SHG
every day.

First Demonstration of Second-Harmonic

Generation
P.A. Franken, et al, Physical Review Letters 7, p. 118 (1961)

The second-harmonic beam was very weak because the process

was not phase-matched.

First demonstration of SHG: The Data

The actual published results
The second harmonic

Input beam

Note that the very weak spot due to the second harmonic is missing.
It was removed by an overzealous Physical Review Letters editor,
who thought it was a speck of dirt.

Sinusoidal Dependence of SHG Intensity

on Length
Large k

Small k

The SHG intensity is sharply maximized if k = 0.

Phase-matching Second-Harmonic Generation

So were creating light at sig = 2.
The k-vector of the second-harmonic is: k sig =
And the k-vector of the polarization is:
The phase-matching condition is:

sig
c0

n(sig ) =

k pol = 2 k = 2

c0

(2 )
n(2 )
c0

n( )

ksig = k pol

n(2 ) = n( )
Unfortunately, dispersion prevents
this from ever happening!

Refractive
index

which will only be satisfied when:

Frequency

Phase-matching Second-Harmonic
Generation using Birefringence

We can now satisfy the

phase-matching condition.
Use the extraordinary polarization
for and the ordinary for 2.

no (2) = ne ()

Refractive index

Birefringent materials have different refractive indices for different

polarizations. Ordinary and extraordinary refractive indices
can be different by up to ~0.1 for SHG crystals.

ne

no

Frequency

ne depends on propagation angle, so we can tune for a given .

Some crystals have ne < no, so the opposite polarizations work.

Noncollinear SHG phase-matching

x

G
k = k cos z k sin x
G
k = k cos z + k sin x

G
G G
k pol = k + k = 2 k cos z
k pol = 2
But:

ksig

2
=
n(2 )
co

c0

n( ) cos
So the phase-matching
condition becomes:

n(2 ) = n( ) cos

Phase-Matching Bandwidth
Refractive index

Recall that the intensity out of an

SHG crystal of length L is:

I sig ( L) ( L / ) 2 sinc 2 (k L / 2)

ne

where:

n ( / 2) n ( )

no

Wavelength

0
2

k ( ) =

[ n( ) n( / 2)]

Phase-matching only works exactly for one wavelength, say 0.

Since ultrashort pulses have lots of bandwidth, achieving
approximate phase-matching for all frequencies is a big issue.
The range of wavelengths (or frequencies) that achieve approximate
phase-matching is the phase-matching bandwidth.

Phase-matching efficiency vs.

wavelength for BBO
Phase-matching efficiency vs. wavelength for the nonlinear-optical
crystal, beta-barium borate (BBO), for different crystal thicknesses:
10 m

100 m

1000 m

These curves also take into account the (L/)2 factor.

Note the huge differences

in phase-matching
bandwidth and efficiency
with crystal thickness.

While the curves are scaled in arbitrary units, the

relative magnitudes can be compared among the
three plots. (These curves dont, however, include the
nonlinear susceptibility, (2)).

Phase-matching efficiency vs.

wavelength for KDP
Phase-matching efficiency vs. wavelength for the nonlinear-optical
crystal, potassium dihydrogen phosphate (KDP), for different
crystal thicknesses:
10 m

The huge differences in

phase-matching bandwidth
and efficiency with crystal
thickness occur for all
crystals.

100 m

1000 m

The curves for the thin crystals dont fall to zero

at long wavelengths because KDP
simultaneously phase-matches for two
wavelengths, that shown and a longer (IR)
wavelength, whose phase-matching ranges
begin to overlap when the crystal is thin.

Calculation of Phase-Matching Bandwidth

The phase-mismatch is:

k () =

[n( ) n( / 2)]

Assuming the process is phase-matched at 0, lets see what the

phase-mismatch will be at = 0 +

But the process is phase-matched at 0

4
k ( ) =
1
0 0

n
(

n
(

)
n
(

/
2)
n
(

/
2)
0
0
0
0

because, when the input wavelength changes by , the secondharmonic wavelength changes by only /2.

k ( ) =

4
1

n
n
(

)
(

/
2)

0
0

0
2

to first order
in

Calculation of Phase-Matching Bandwidth (contd)

sinc2(kL/2)

sinc2

The
curve will decrease by a
factor of 2 when k L/2 = 1.39.
So solving for the wavelength
range that yields |k | < 2.78/L
yields the phase-matching
bandwidth.

I
FWHM

-2.78/L

2.78/L

4
1

)
(

/
2)
n
n
2.78 / L <

< 2.78 / L
0
0

0
2

FWHM

0.44 0 / L
=
n(0 ) 12 n(0 / 2)

Phase-Matching Bandwidth
The phase-matching bandwidth is usually too small, but it increases as
the crystal gets thinner or the dispersion decreases (i.e., the
wavelength approaches ~1.5 microns).
BBO

KDP

The theory breaks down, however, when the bandwidth

approaches the wavelength.

Group-Velocity Mismatch
Inside the crystal the two different wavelengths have different group
velocities.
Define the Group-Velocity
Mismatch (GVM):

GVM

1
v g (0 / 2)

1
v g (0 )

Second harmonic created

just as pulse enters crystal
(overlaps the input pulse)

As the pulse
enters the crystal:

Crystal

As the pulse
leaves the crystal:

Second harmonic pulse lags

behind input pulse due to GVM

Group-Velocity Mismatch
Calculating GVM:

v g ( ) =

c0 / n( )

n( )
1
n ( )

So:

1
n ( )
=
v g ( )
c0

1 n( ) n ( )

1
GVM

v g (0 / 2) v g (0 )

xx

x x
x

n(0 )

n(0 / 2)
0 / 2
0
=
n(0 / 2)
n(0 )
1
1
c0
c0 n(0 )
n(0 / 2)

But we only care about GVM when

n(0/2) = n(0)

0
1

GVM =
n
(
)
n
(
/
2)

0
0

c0

Group-velocity
mismatch lengthens
the SH pulse.
Crystal

Assuming that a very short pulse

enters the crystal, the length of the ,
SH pulse, t, will be determined by
the difference in light-travel times
through the crystal:

L
t =

= L GVM
v g ( 0 / 2) v g ( 0 )
We always try to satisfy:

L GVM << p

Group-velocity mismatch pulse lengthening

Second-harmonic pulse shape for different crystal lengths:

LD
L /LD
Input
pulse
shape

p
GVM

LD is the crystal
length that
doubles the
pulse length.

Its best to use a very thin crystal. Sub-100-micron crystals are common.

Group-velocity mismatch numbers

Group-velocity mismatch limits bandwidth.

Lets compute the second-harmonic bandwidth due to GVM.
Take the SH pulse to have a Gaussian intensity, for which t = 0.44.
Rewriting in terms of the wavelength,

t = t [d/d]1 = 0.44 [d/d]1 = 0.44 2/c0

where weve neglected the minus sign since were computing the
bandwidth, which is inherently positive. So the bandwidth is:

FWHM

0.44 02 / c0
0.44 02 / c0

=
t
L GVM

FWHM

GVM =

0
1

n
(
)
n
(
/
2)

0
0

c0

0.44 0 / L

n(0 ) 12 n(0 / 2)

Calculating the bandwidth by considering the GVM yields the same

result as the phase-matching bandwidth!

SHG efficiency
The second-harmonic field is given by:

E 2 ( L, t ) = i

0 2 L
2k

P exp(ikL 2) sinc(kL 2)

The irradiance will be:

0 2 ( (2) ) 2 ( I ) 2 L2
2

2c0 n3

sinc 2 (kL 2)

Dividing by the input irradiance to obtain the SHG efficiency:

I 2 2 0 2 d 2 I L2
=
I
c0 2 n 3
Substituting in typical numbers:

I 2
2
8

[5

10
/
W
]
I
L

Take k = 0
d (2), and includes
crystal additional
parameters.

Amazing second-harmonic generation

Frequency-doubling
KDP crystals at
Lawrence Livermore
National Laboratory
These crystals convert
as much as 80% of the
input light to its second
harmonic. Then
additional
crystals produce the
third harmonic with
similar efficiency!
These guys are
serious!

Difference-Frequency Generation: Optical

Parametric Generation, Amplification, Oscillation
Difference-frequency generation takes many useful forms.
1
3

2 = 3 1

1
3

Parametric Down-Conversion
(Difference-frequency generation)
1

Optical Parametric
Generation (OPG)

"idler"
By convention:
signal > idler

2
mirror

Optical Parametric
Amplification (OPA)

"signal"

Optical Parametric
Oscillation (OPO)

mirror

Optical Parametric Generation

Equations are just about identical to those for SHG:
2

1 
(2) 1
 * E eik z
E
+
E1 = i
2 3
2

v
2
z
t
c
k
1
g1

2

1 
(2) 2
 * E eik z
E
+
E2 = i
1 3
2

v
2
z
t
c
k
2
g2

1 
(2)
3
 E e ik z
E
+
E3 = i
1 2
2

v
2
z
t
c
k
3
g3

where:
ki = wave vector of ith wave
k = k1 + k2 - k3
vgi = group velocity of ith wave

The solutions for E1 and E2

involve exponential gain!

OPAs etc. are ideal uses of ultrashort pulses, whose intensities are high.

Phase-matching applies.
We can vary the crystal angle in the usual manner, or we can vary
the crystal temperature (since n depends on T).

Free code to perform OPO,

OPA, and OPG calculations
Public domain software maintained by Arlee Smith at
Sandia National Labs. Just web-search SNLO.
You can use it to select the best nonlinear crystal for your particular
application or perform detailed simulations of nonlinear mixing
processes in crystals.
Functions in SNLO:
1. Crystal properties
2. Modeling of nonlinear crystals in various applications.
3. Designing of stable cavities, computing Gaussian focus parameters
and displaying the help file.

Optical
Parametric
Generation
signal:
Recent results
using the nonlinear
medium,
periodically poled
RbTiOAsO4
idler:

Sibbett, et al., Opt. Lett., 22, 1397 (1997).

An Ultrafast Noncollinear OPA (NOPA)

Continuum generates an
arbitrary-color seed pulse.

NOPA Specs

Crystals for far-IR generation

With unusual crystals,
such as AgGaS2,
AgGaSe2 or GaSe,
one can obtain
radiation to
wavelengths as long
as 20 m.
These long
wavelengths are
useful for vibrational
spectroscopy.

Wavelength
10 m

1 m

Gavin D. Reid, University of Leeds, and Klaas Wynne, University of Strathclyde

Differencefrequency
generation in
GaSe

Angle-tuned
wavelength

Elsaesser, et al., Opt.

Lett., 23, 861 (1998)

Another 2nd-order process: Electro-optics

Applying a voltage to a crystal changes its refractive indices and
introduces birefringence. In a sense, this is sum-frequency
generation with a beam of zero frequency (but not zero field!).
A few kV can turn a crystal into a half- or quarter-wave plate.

Pockels cell
(voltage may be
transverse or
longitudinal)

Polarizer

If V = 0, the pulse
polarization doesnt
change.
If V = Vp, the pulse
polarization switches to its
orthogonal state.

Abruptly switching a Pockels cell allows us to switch a pulse into or out

of a laser.

The Pockels Cell (Q-Switch)

The Pockels effect is a type of second-order nonlinear-optical effect.
Before switching
0 Polarizer

Mirror

Pockels cell as
wave plate w/
axes at 45

After switching
0 Polarizer

Mirror

Pockels cell as
wave plate w/
axes at 0 or 90

The Pockels effect involves the simple second-order process:

sig = + 0
dc field
The signal field has the orthogonal polarization, however.