Some Basics of Nonlinear Optical Frequency Conversion (Contd)

Phase-Matching:
It refers to the tendency, when propagating through a nonlinear medium, of the
generated wave to become out of phase with the induced polarization after some
distance.It involves precise control of the indices of the three frequencies involved in the
mixing process to match the velocities of propagation of the polarization waves and the
electromagnetic wave which they generate.It can be seen that the generated signal is
90out of phase with the polarization wave when k=0. It can be shown that this makes it
possible to couple the energy from the polarization wave into the generated wave. But for
k0 this favorable condition exists only at L=0 and after one coherence length
(Lc=/k) the phase of the signal will change exactly by 90. Thus power flow
changes sign. So if L=2Lc no generation will occur!!!!.

Angle Phase-Matching:
In this method the crystal birefringence is utilized to compensate the dispersion. Too
small birefringence will not be able to make such compensation as shown below.

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In the figure below it can be seen that in the given negative uniaxial nonlinear medium
one can achieve the generation of 532 nm, the second harmonic of 1064 nm radiation, by
equating the phase-velocities of ordinarily polarized 1064 nm beam and that of the
extraordinarily polarized 532 nm beam by rotation of wave propagation angle θ which the
interacting beams make with the crystal optic axis inside the crystal. And since,

n
ord
 no
1
cos2  sin 2  2

n
ext
n e
()   2  2 
 n o ne 
Hence, the phase-matching condition for above interaction will be
n1o= n2e(θ)

n SHG is critically phase-matched

FHG is noncritically phase-matched (= 90o)

n2o
n1o
n2e()
n2e no
ne

266 532 1064
nm nm nm

However if the condition be such that n1o= n2e then the phase-matching angle θ will be
90 as is the case shown for second harmonic generation of 532 nm in the above figure.
In such case the interaction is said to be non-critically phase-matched. SHG of 532 nm is
obviously fourth harmonic of 1064 nm and hence it is denoted as FHG in the above
figure. The SHG of 1064 nm is shown by index-matching is figure below as well.

PM Conditions for negative uniaxial crystals:

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For sum frequency generation SFG: (1/1 + 1/2 = 1/3) 1>2>3
Type-I Type-IIA Type-IIB
ooe eoe oee

For difference frequency generation DFG: (1/1 1/2 = 1/3) 1<2<3

Type-I Type-IIA Type-IIB
eoo eoe eeo

For positive uniaxial crystal the conditions can be obtained simply by changing
the ordinary polarization by extraordinary and vice-versa. For example, for SFG,
the conditions will be eeo, oeo and eoo respectively for Type-I, Type-IIA and Type-IIB.

Critical issues of Material Selection:

1. Nonlinear Coefficient must be high. [ deff2].
2. Higher Damage Threshold is always an important advantage for improving
conversion efficiency. [ 1/r2]
3. The crystal should have enough birefringence to allow phase-matching for
different interactions.
4. The crystal should have large Transparency Range.
5. The Crystal length is an important parameter as the conversion efficiency
increases by L2. So it is important that the crystal can be available in large size.
[ L2]
6. Stability is very important since if the crystal is hygroscopic then its polished
surfaces will easily become opaque and thus it can not be used. Of course thermal
ovens can be used to tackle such problems, but it will mean additional cost and
extra care.
7. Optical Homogeneity of the crystal is very essential for getting high conversion
efficiency.

Nonlinear optical materials will be the key elements for future photonic technologies
based on the fact that photons are capable of processing information with the speed of
light. The search for new and efficient materials in which to carry out nonlinear optical
processes has been very active since SHG was first observed in single crystal quartz by
Franken and co-workers in 1961. In the beginning, studies were concentrated on
inorganic materials such as quartz, potassium dihydrogen phosphate (KDP), lithium
niobate (LiNbO3), and its analogues, potassium titanyl phosphate (KTP) and its
analogues, Beta Barium Borate (β-BaB2O4, BBO), generators to provide coherent laser
radiation with high frequency conversion efficiency in the new region of the spectrum
inaccessible by other nonlinear crystal conventional sources.

No one crystal is ideal. Phosphates provide the largest nonlinear crystals: KDP
(potassium dihydrogen phosphate), KD*P (deuterated potassium dihydrogen phosphate)
and ADP (ammonium dihydrogen phosphate) are all grown in water-solution to very

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large size, and are quite impervious to optical damage, although hygroscopic. KDP is
being grown in tremendous sizes for the inertial confinement fusion laser at Livermore
Laboratories in California. The phosphates have transparency to below 200 nm and out to
2 m, but their nonlinear coefficient is quite small: deff~ 0.4 pm/V (pm  picometer =
10-12m). By comparison, KTP (potassium titanyl phosphate) and KTA (potassium titanyl
arsenate) have an order of magnitude higher nonlinearity: deff ~ 4 pm/V and are non-
hygroscopic, but they are hard to grow and only small crystals are available. KTP is
commonly used today to frequency-double diode-pumped solid state lasers. However, if
the optical power becomes too high, KTP shows photo-induced “gray-tracks.”

Lithium niobate has large nonlinearities with a transparency range from 420 nm out to
4.8m and a very high nonlinearity (deff = 5.8 pm/V) but exhibits debilitating photo-
refractive effects unless heated or doped with oxides. Magnesium oxide doping is
commonly used. Zinc oxide doping increases the nonlinearity to 16 pm/V and has better
optical quality and lower absorption, but is limited to 250 MW/cm2 of light intensity.
Eighty times improvement in damage threshold is obtained with zirconium oxide doping,
at the expense of roughly half the nonlinearity. Lithium Tantalate (LiTaO3) has less
optical damage than LN and doesn’t require doping, but its nonlinearity is half that of
LN. Potassium niobate (KNbO3) has high nonlinearity and high damage threshold, which
sounds ideal, but it has only a small temperature range of phase-matching, and, more
importantly, shaking or stressing the crystalcan cause domain changes, so it must be
handled “smoothly,” limiting its use.

Borates form another class of nonlinear crystals, transparent into the UV, with a high
threshold to optical damage, but with considerably lower nonlinearity: LBO (lithium
triborate) is transparent to 150 nm, but deff ~ 0.8 pm/V, roughly twice KDP. BBO (bet
barium borate) has a more respectable deff ~ 2 pm/V. Bismuth Borate (BiBO) has deff~
3.3pm/V and the highest damage threshold. These crystals are excellent for high-power
applications: with a large acceptance angle and small walk-off angle and suitable for
temperature-controllable non-critical phase-matching.

Research is underway on organic crystals for frequency doubling, but they have not yet
proven more reliable than the above-mentioned crystals.

In the infrared, a different set of crystals has been developed, with higher nonlinearities
but much lower damage thresholds. These include AGS (AgGaS2), transparent over 0.5 -
13 m; AGSe (AgGaSe2) transparent over 0.7 - 18 m; also HGS (HgGa2S4) and Zinc
germanium diphosphide (ZnGeP2).

The Borate group of crystals, namely, -BaB2O4 (beta Barium Borate, BBO),
LiB3O5 (Lithium Triborate, LBO), CLBO (Cesium Lithium Borate, CsLiB6O10),
Li2B4O7 (Lithium Tetraborate, LB4) etc had proved to be very important addition
to the list of UV-VIS-NIR transmitting crystals that provides one with very high
nonlinear frequency conversion not only in harmonic generation of Nd:YAG laser
radiation (1064 nm) but also for generation of tunable source from ultraviolet to
near infrared region of the spectrum.

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Characteristics of some Nonlinear crystals:

Crystal KDP BBO LiNbO3 AgGaS2 ZnGeP2

(-ve (-ve (-ve (-ve (+ve
name uniaxial) uniaxial) uniaxial) uniaxial) uniaxial)

Transparency
0.18 – 1.6 0.19 – 3.2 0.45 – 4.8 0.5 – 13 0.74 – 12
(m)
Birefringence
0.04 0.11 0.09 0.06 + 0.04
RefractiveI
ndex
1.5 1.6 2.2 2.3 3.1
deff(pm/V)
0.39 2.2 6 13.5 70

Damage
threshold
(GW/cm2)
1 2 0.2 0.02 0.06
Chemical hygroscopic hygroscopic non non non
property hygroscopic hygroscopic hygroscopic

For BBO,

Reference Books:
1. Handbook of Nonlinear Optics by R.L. Sutherland
2. Solid State Laser Engineering by W Koechner(Chapter X)

Problem:
Calculate the phase-matching angle for Type-I sum frequency
mixing of 1064 and 565 nm radiations in a BBO crystal.