Материал: Weber H., Herziger G., Poprawe R. (eds.) Laser Fundamentals. Part 1 (Springer 2005)(263s) PEo

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142

4.1.1 Introduction

[Ref. p. 187

4.1.1.1.2 Abbreviations

av cw DFG

DROPO ERR FIHG FOHG ICDFG ICSHG IR

mid IR NC NCSHG OPA OPO SFG SH SHG SIHG

SP OPO SROPO SRS THG TROPO TWOPO UV

4.1.1.1.3 Crystals

Chemical formula

Ag3AsS3

AgGaS2

AgGaSe2

Ag3SbS3

Ba2NaNb5O15 β−BaB2O4 CdGeAs2 CdSe

CsB3O5 CsH2AsO4 CsLiB6O10 C6H6N2O3 C8H8O3

C10H11N3O6 C10H13N3O3

C11H14N2O3

CsD2AsO4 GaSe

average continuous wave

di erence frequency generation doubly resonant OPO

external ring resonator fifth harmonic generation fourth harmonic generation

intracavity di erence frequency generation intracavity second harmonic generation infrared

middle infrared noncollinear

noncollinear second harmonic generation optical parametric amplifier

optical parametric oscillator sum frequency generation second harmonic

second harmonic generation sixth harmonic generation synchronously pumped OPO singly resonant OPO stimulated Raman scattering third harmonic generation triply resonant OPO traveling-wave OPO ultraviolet

Symbol

Crystal name

Proustite

Silver Thiogallate

Silver Gallium Selenide

Pyrargyrite

Barium Sodium Niobate (Banana)

BBO

Beta-Barium Borate

Cadmium Germanium Arsenide

Cadmium Selenide

CBO

Cesium Borate

CDA

Cesium Dihydrogen Arsenate

CLBO

Cesium Lithium Borate

POM

3-Methyl-4-Nitro-Pyridine-1-Oxide

MHBA

4-Hydroxy-3-Methoxy-Benzaldehyde (Vanillin)

MAP

Methyl N-(2,4-Dinitrophenyl)-L-Alaninate

DAN

N-[2-(Dimethylamino)-5-Nitrophenyl]-Acetamide

NPP

N-(4-Nitrophenyl)-(L)-Propinol

DCDA

Cesium Dideuterium Arsenate

Gallium Selenide

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4.1 Frequency conversion in crystals

143

HgGa2S4

α−HIO3

KB5O8 4D2O

KB5O8 4H2O

KD2AsO4

KD2PO4

KH2PO4

KNbO3

KTiOAsO4

KTiOPO4

LiB3O5

LiCOOH H2O

LiIO3

LiNbO3

LiNbO3:MgO

(NH2)2CO

NH4H2AsO4

NH4H2PO4

NO2C6H4NH2

RbH2AsO4

RbH2PO4

RbTiOAsO4

Te

Tl3AsSe3

ZnGeP2

Mercury Thiogallate

α−Iodic Acid

DKB5

Potassium Pentaborate Tetradeuterate

KB5

Potassium Pentaborate Tetrahydrate

DKDA

Potassium Dideuterium Arsenate

DKDP

Potassium Dideuterium Phosphate

KDP

Potassium Dihydrogen Phosphate

Potassium Niobate

KTA

Potassium Titanyl Arsenate

KTP

Potassium Titanyl Phosphate

LBO

Lithium Triborate

LFM

Lithium Fomate

Lithium Iodate

Lithium Niobate

Mg:O-doped Lithium Niobate

Urea

ADA

Ammonium Dihydrogen Arsenate

ADP

Ammonium Dihydrogen Phosphate

mNA

meta-Nitroaniline

RDA

Rubidium Dihydrogen Arsenate

RDP

Rubidium Dihydrogen Phosphate

RTA

Rubidium Titanyl Arsenate

Tellurium

Thallium Arsenic Selenide

Zinc Germanium Phosphide

4.1.1.2 Historical layout

The pioneering work of Franken et al. [61Fra] on second harmonic generation of ruby laser radiation in quartz and invention of the phase-matching concept [62Gio, 62Mak] generated a new direction in the freshly born field of nonlinear optics: frequency conversion in crystals. Sum frequency generation by mixing the outputs of two ruby lasers in quartz was already realized in 1962 [62Mil, 62Bas]. Zernike and Berman [65Zer] were the first to demonstrate di erence frequency mixing. Optical parametric oscillation was experimentally realized in 1965 by Giordmaine and Miller [65Gio]. First monographs on nonlinear optics by Akhmanov and Khokhlov [64Akh] and Bloembergen [65Blo] greatly stimulated development of the nonlinear frequency converters. At present the conversion of laser radiation in nonlinear crystals is a powerful method for generating widely tunable radiation in the ultraviolet, visible, near, mid, and far IR regions.

For theoretical and experimental details of nonlinear frequency conversions in crystals, see monographs by Zernike and Midwinter [73Zer], Danelyus, Piskarskas et al. [83Dan], Dmitriev and Tarasov [87Dmi], Shen [84She], Handbook of nonlinear optical crystals (by Dmitriev, Gurzadyan, Nikogosyan) [91Dmi, 99Dmi], Handbook of nonlinear optics (by Sutherland ) [96Sut]. For frequency conversion of femtosecond laser pulses, see also [88Akh]. For linear and nonlinear optical properties of the crystals, see [77Nik, 79Kur, 84Jer, 87Nik, 87Che, 96Sut, 99Dmi, 00Cha, 00Sas]. For related nonlinear phenomena, see [96Sut]. For the historical perspective of the nonlinear frequency conversion over the first forty years, see [00Bye]. In the following section, Sect. 4.1.2, we present some basic equations which may be useful for simple calculations of frequency converters.

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4.1.2 Fundamentals

[Ref. p. 187

4.1.2 Fundamentals

4.1.2.1 Three-wave interactions

Dielectric polarization P (dipole moment of unit volume of the substance) is related to the field E by the material equation of the medium [64Akh, 65Blo] (Chap. 1.1):

P (E) = ε0 (χ(1) E + χ(2) E2 + χ(3) E3 + . . . )

(4.1.1)

with

ε0 = 8.854 × 10−12 CV−1m−1 : dielectric permittivity of free space,

χ(1) = n2 − 1 : the linear, and χ(2) , χ(3) etc.: the nonlinear dielectric susceptibilities.

In the present chapter, Chap. 4.1, we consider only three-wave interactions in crystals with square nonlinearity (χ(2) = 0). The following nonlinear frequency conversion processes are considered:

Second Harmonic Generation (SHG):

ω + ω = 2 ω ,

(4.1.2)

Sum-Frequency Generation (SFG) or up-conversion:

ω1 + ω2 = ω3 ,

(4.1.3)

Di erence-Frequency Generation (DFG) or down-conversion:

ω3

− ω2 = ω1 ,

(4.1.4)

Optical Parametric Oscillation (OPO):

ω3

= ω2 + ω1 .

(4.1.5)

For e cient frequency conversion phase matching should be fulfilled:

k1

+ k2 = k3

(4.1.6)

with

ki : the wave vectors for ω1 , ω2 , ω3 , respectively.

Two types of phase matching are introduced:

type I: o + o → e or e + e → o , type II: o + e → e or o + e → o ,

or with shortened notations:

ooe: o + o → e or e → o + o , eeo: e + e → o or o → e + e , eoe: e + o → e or e → e + o , oeo: o + e → o or o → e + o .

In the shortened notation (ooe, eoe, . . . ) applies: ω1 < ω2 < ω3, i.e. the first symbol refers to the longest-wavelength radiation, and the latter to the shortest-wavelength radiation. Here, o-beam, or ordinary beam, is the beam with polarization normal to the principal plane of the crystal, i.e.

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Ref. p. 187]

4.1 Frequency conversion in crystals

145

the plane containing the wave vector k and crystallophysical axis Z (or optical axis, for uniaxial crystals). The e-beam, or extraordinary beam, is the beam with polarization in the principal plane.

The methods of angular and temperature phase-matching tuning are used in frequency converters. Angular tuning is rather simple and more rapid than temperature tuning. Temperature tuning is generally used in the case of 90 ◦ phase matching, i.e., when the birefringence angle is zero. This method is mainly used in crystals with a strong temperature dependence of phase matching: LiNbO3, LBO, KNbO3, and Ba2NaNb5O15.

4.1.2.2 Uniaxial crystals

For uniaxial crystals the di erence between the refractive indices of the ordinary and extraordinary beams, birefringence ∆n , is zero along the optical axis (crystallophysical axis Z) and maximum in the normal direction. The refractive index of the ordinary beam does not depend on the direction of propagation, however, the refractive index of the extraordinary beam ne(θ) is a function of the polar angle θ between the Z axis and the vector k (but not of the azimuthal angle ϕ) (Fig. 4.1.1):

1

ne (θ) = no

1 +

1 + tan2 θ

θ

2

(4.1.7)

no 2 tan2

,

ne

where no and ne are the refractive indices of the ordinary and extraordinary beams in the plane normal to the Z axis and termed as corresponding principal values. Note that if no > ne , the crystal is negative, and if no < ne , it is positive. For an o-beam the indicatrix of the refractive indices is a sphere with radius no , and an ellipsoid of rotation with semiaxes no and ne for an e-beam (Fig. 4.1.2). In the crystal the beam, in general, is divided into two beams with orthogonal polarizations; the angle between these beams ρ is the birefringence (or walk-o ) angle.

Equations for calculating phase-matching angles in uniaxial crystals are given in Table 4.1.1 [86Nik, 99Dmi].

Z

k

Y

X

Fig. 4.1.1. Polar coordinate system for description of refraction properties of uniaxial crystals (k is the light propagation direction, Z is the optic axis, θ and ϕ are the coordinate angles).

4.1.2.3 Biaxial crystals

For biaxial crystals the optical indicatrix has a bilayer surface with four points of interlayer contact which correspond to the directions of two optical axis. In the simple case of light propagation in

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4.1.2 Fundamentals

[Ref. p. 187

Z

Z

no > ne

no

z

ne > no

no

ne ( )

ne ( )

z

0

0

ne

no X (Y )

no

ne X (Y )

a

b

Fig. 4.1.2. Dependence of refractive index on light propagation direction and polarization (index surface) in uniaxial crystals: (a) negative: no > ne and (b) positive: ne > no .

Table 4.1.1. Equations for calculating phase-matching angles in uniaxial crystals [86Nik, 99Dmi].

Negative uniaxial crystals

Positive uniaxial crystals

tan2

θpmooe = (1

−

U )/(W

−

1)

tan2 θpmeeo

≈

(1

−

U )/(U

−

S)

2

eoe

(1

U )/(W

R)

tan

2

oeo

V )/(V

Y )

tan

θpm

≈

−

−

2

θpm

= (1

−

−

2

oee

tan

eoo

= (1

tan

θpm

≈ (1 − U )/(W − Q)

θpm

− T )/(T − Z)

Notations:

U = (A + B)2/C2 ; W = (A + B)2/F 2 ; R = (A + B)2/(D + B)2 ;

Q = (A + B)2

E)2 ; S = (A + B)2/(D + E)2 ; V = B2/(C

−

A)2 ;

2

/E

2

/(A +2

2

2

/D

2

;

Y = B

; T = A

/(C − B) ; Z

= A

A = no1/λ1 ; B = no2/λ2 ; C = no3/λ3 ;

D = ne1/λ1 ; E = ne2/λ2 ; F = ne3/λ3 .

These expressions can

be generalized

to

noncollinear phase matching. In this

case, for example,

the phase-matching angle θpmooe is determined from the above presented equation using the new coe cients U and W :

U = (A2 + B2 + 2AB cos γ)/C2 , W = (A2 + B2 + 2AB cos γ)/F 2 ,

where γ is the angle between the wave vectors k1 and k2 .

the principal planes XY , Y Z, and XZ the dependencies of refractive indices on the direction of light propagation represent a combination of an ellipse and a circle (Fig. 4.1.3). Thus in the principal planes a biaxial crystal can be considered as a uniaxial crystal, e.g. a biaxial crystal with nZ > nY > nX in the XY plane is similar to a negative uniaxial crystal with no = nZ and

ne (ϕ) = nY 1 + (nY /nX )2

tan2

1

(4.1.8)

ϕ .

1 + tan2

ϕ

2

The angle VZ between the optical axis and Z axis for the case nZ > nY > nX can be found from:

nY

nZ2

− nX2

1

sin VZ =

nZ

nY2

− nX2

2

(4.1.9)

and for the case nX > nY > nZ :

nY

nX2

− nZ2

1

cos VZ =

nX

nY2

− nZ2

2 .

(4.1.10)

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