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

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Ref. p. 187]

4.1 Frequency conversion in crystals

147

Z

Optic axis

Z

nX

nY

nY

Optic axis

nX

nX

nZ Y

nZ

nX Y

nY

nZ

n

Y

nZ

X

X

a

b

Fig. 4.1.3. Dependence of refractive index on light propagation direction and polarization (index surface) in biaxial crystals: (a) nX < nY < nZ , (b) nX > nY > nZ .

For a positive biaxial crystal the bisectrix of the acute angle between optical axes coincides with nmax and for a negative one the bisectrix coincides with nmin .

Equations for calculating phase-matching angles upon propagation in principal planes of biaxial crystals are given in Table 4.1.2 [87Nik, 99Dmi].

4.1.2.4 E ective nonlinearity

Miller delta formulation [64Mil]:

ε0Ei(ω3) = δijk Pj (ω1)Pk (ω2) ,

(4.1.11)

where the Miller coe cient,

1

χijk(2) (ω3)

δijk =

,

(4.1.12)

2ε0

χii(1)(ω1) χjj(1)(ω2) χkk(1)

(ω3)

has small dispersion and is almost constant for a wide range of crystals.

For anisotropic media the coe cients χ(1) and χ(2) are, in general, the secondand third-rank tensors, respectively. In practice, the tensor

dijk =

1

χijk

(4.1.13)

2

is used instead of χijk . Usually, the “plane” representation of dijk in the form dil is used, the relation between l and jk is:

jk

l

11

↔

1

22

↔

2

33

↔

3

23 or 32

↔

4

31 or 13

↔

5

12 or 21

↔

6

Landolt-B¨ornstein

New Series VIII/1A1

B¨ornstein-Landolt

VIII/1A1 Series New

Table 4.1.2. Equations for calculating phase-matching angles in biaxial crystals upon light propagation in the principal planes [87Nik, 99Dmi].

(a) nX < nY < nZ

Principal

Type of

Equations

Notations

plane

interaction

1 − U

U =

A + B

2

; W =

A + B

2

ooe

tan2 ϕ =

; A =

nZ1

; B =

nZ2

; C =

nY 3

; F =

nX3

W − 1

C

F

λ1

λ2

λ3

λ3

XY

≈

W − R

U =

C

2

; W =

F

2

D + B

2

; B =

λ2

; C = λ3

; D = λ1

; F =

λ3

; R =

; A = λ1

eoe

tan2

ϕ

1 − U

A + B

2

A + B

2

A

+ B

2

nY

1

nZ2

nY 3

nX1

nX3

≈

W − Q

U =

C

; W =

F

; A = λ1

; B = λ2

; C = λ3

; E = λ2

; F =

λ3

; Q =

A + E

oee

tan2

ϕ

1 − U

A + B

A + B

A

+ B

nZ1

nY 2

nY 3

nX2

nX3

≈

U − S

U =

C

2

2

λ1

; B =

λ2

; C =

λ3

; D =

λ1

; E =

λ2

; S = D + E

; A =

eeo

tan2

θ

1 − U

A + B

A

+ B

nY 1

nY 2

nX3

nZ1

nZ2

Y Z

V − Y

V =

C − A

2

; Y =

E

2

; B = λ2

; C = λ3

; E =

λ2

; A = λ1

oeo

tan2 θ =

1 − V

B

2

B

2

nX1

nY

2

nX3

nZ2

T − Z

T =

; Z = D

; B = λ2

; C = λ3

; D = λ1

C − B

; A = λ1

eoo

tan2 θ =

1 − T

A

A

nY 1

nX2

nX3

nZ1

XZ

W − 1

U =

C

2

; W =

F

2

λ1

; B =

λ2

; C =

λ3

; F =

λ3

; A =

ooe

tan2 θ =

1 − U

A + B

A + B

nY 1

nY 2

nX3

nZ3

θ < VZ

≈

W − R

U =

C

2

; W =

F

2

D + B

2

; B =

λ2

; C = λ3

; D = λ1

; F =

λ3

; R =

; A = λ1

eoe

tan2

θ

1 − U

A + B

2

A + B

2

A

+ B

2

nX1

nY 2

nX3

nZ1

nZ3

≈

W − Q

U =

C

; W =

F

; A = λ1

; B = λ2

; C = λ3

; E = λ2

; F =

λ3

; Q =

A + E

oee

tan2

θ

1 − U

A + B

A + B

A

+ B

nY 1

nX2

nX3

nZ2

nZ3

XZ

≈

U − S

U =

C

2

2

λ1

; B =

λ2

; C =

λ3

; D =

λ3

; E =

λ2

; S = D + E

; A =

eeo

tan2

θ

1 − U

A + B

A

+ B

nX1

nX2

nY 3

nZ1

nZ2

θ > VZ

V − Y

V =

C − A

2

; Y =

E

2

; B = λ2

; C = λ3

; E =

λ2

; A = λ1

oeo

tan2 θ =

1 − V

B

2

B

2

nY 1

nX2

nY 3

nZ2

T − Z

T =

; Z = D

; B = λ2

; C = λ3

; D =

λ1

C − B

; A = λ1

eoo

tan2 θ =

1 − T

A

A

nX1

nY 2

nY 3

nZ1

(continued)

148

Fundamentals 2.1.4

187 .p .[Ref

B¨ornstein-Landolt

VIII/1A1 Series New

Table 4.1.2 continued.

(b) nX > nY > nZ

Principal

Type of

Equations

Notations

plane

interaction

≈

U − S

U =

C

2

2

λ1

; B =

λ2

; C =

λ3

; D =

λ1

; E =

λ2

; S = D + E

; A =

eeo

tan2

ϕ

1

− U

A + B

A

+ B

nY 1

nY 2

nZ3

nX1

nX2

XY

V − Y

V =

C − A

2

; Y =

E

2

; B = λ2

; C = λ3

; E =

λ2

; A = λ1

oeo

tan2

ϕ =

1

− V

B

B

nZ1

nY 2

nZ3

nX2

2

2

T − Z

T =

; Z = D

; B = λ2

; C = λ3

; D =

λ1

C − B

; A = λ1

eoo

tan2

ϕ =

1

− T

A

A

nY 1

nZ2

nZ3

nX1

W − 1

U =

C

2

; W =

F

2

λ1

; B =

λ2

; C = λ3

; F = λ3

; A =

ooe

tan2

θ =

1

− U

A + B

A + B

nX1

nX2

nY 3

nZ3

2

2

2

Y Z

≈

W − R

U =

C

; W =

F

; A = λ1

; B =

λ2

; C =

λ3

; D = λ1

; F =

λ3

; R =

D + B

eoe

tan2

θ

1

− U

A + B

A + B

A

+ B

nY 1

nX2

nY 3

nZ1

nZ3

2

2

2

≈

W − Q

U =

C

; W =

F

; A = λ1

; B =

λ2

; C =

λ3

; E = λ2

; F =

λ3

; Q =

A + E

oee

tan2

θ

1

− U

A + B

A + B

A

+ B

nX1

nY 2

nY 3

nZ2

nZ3

XZ

≈

U − S

U =

C

2

2

λ1

; B =

λ2

; C =

λ3

; D =

λ1

; E =

λ2

; S = D + E

; A =

eeo

tan2

θ

1

− U

A + B

A

+ B

nX1

nX2

nY 3

nZ1

nZ2

θ < VZ

V − Y

V =

C − A

2

; Y =

E

2

; B = λ2

; C = λ3

; E =

λ2

; A = λ1

oeo

tan2

θ =

1

− V

B

B

nY 1

nX2

nY 3

nZ2

2

2

T − Z

T =

; Z = D

; B = λ2

; C = λ3

; D =

λ1

C − B

; A = λ1

eoo

tan2

θ =

1

− T

A

A

nX1

nY

2

nY 3

nZ1

XZ

W − 1

U =

C

2

; W =

F

2

λ1

; B =

λ2

; C =

λ3

; F = λ3

; A =

ooe

tan2

θ =

1

− U

A + B

A + B

nY 1

nY 2

nX3

nZ3

θ > VZ

≈

W − R

U =

C

2

; W =

F

2

2

; A = λ1

; B =

λ2

; C =

λ3

; D = λ1

; F =

λ3

; R =

D + B

eoe

tan2

θ

1

− U

A + B

A + B

A

+ B

nX1

nY 2

nX3

nZ1

nZ3

≈

W − Q

U =

C

2

; W =

F

2

2

; A = λ1

; B =

λ2

; C =

λ3

; E = λ2

; F =

λ3

; Q =

A + E

oee

tan2

θ

1

− U

A + B

A + B

A

+ B

nY 1

nX2

nX3

nZ2

nZ3

187] .p .Ref

crystals in conversion Frequency 1.4

149

150 4.1.2 Fundamentals [Ref. p. 187

Kleinman symmetry conditions [62Kle]: d21 = d16 , d24 = d32 , d31 = d15 , d13 = d35 , d14 = d36 , d25 = d12 = d26 , d32 = d24 are valid in the case of non-dispersion of electron nonlinear polarizability. The equations for calculating the conversion e ciency include the e ective nonlinear coe cients de , which comprise all summation operations along the polarization directions of the interacting waves and thus reduce the calculation to one dimension. E ective nonlinearities de for di erent crystal point groups under valid Kleinman symmetry conditions are presented in Table 4.1.3.

The conversion factors for SI and CGS-esu systems are given in Table 4.1.4.

Table 4.1.3. Expressions for de in nonlinear crystals when Kleinman symmetry relations are valid.

(a) Uniaxial crystals

Point group

Type of interaction

ooe, oeo, eoo

eeo, eoe, oee

4, 4mm

d15 sin θ

0

6, 6mm

d15 sin θ

0

¯

d 22

cos θ sin (3ϕ)

d22 cos

2

θ cos ϕ

6m2

3m

d 15

sin θ − d22 cos θ sin (3ϕ)

d22 cos2 θ cos (3ϕ)

2

¯

(d11 cos (3ϕ) − d22 sin (3ϕ)) cos θ

(d11 sin (3ϕ) + d22 cos (3ϕ)) cos2

θ

6

sin θ

3

(d

11

cos (3ϕ)

−

d

22

sin (3ϕ)) cos θ + d

(d11

sin (3ϕ) + d

22

cos (3ϕ)) cos

θ

32

15

2

d 11

cos θ cos (3ϕ)

d11 cos

θ sin (3ϕ)

¯

(d14 sin (2ϕ) + d15 cos (2ϕ)) sin θ

(d14 cos (2ϕ) − d15 sin (2ϕ)) sin (2θ)

4

¯

d 36

sin θ sin (2ϕ)

d36 sin (2θ) cos (2ϕ)

42m

(b) Biaxial crystals (assignments of crystallophysical and crystallographic axes: for mm2 and 222 point groups: X, Y, Z → a, b, c ; for 2 and m point groups: Y → b )

Point

Principal

Type of interaction

group

plane

ooe, oeo, eoo

eeo, eoe, oee

2

XY

d23 cos ϕ

d36 sin (2ϕ)

Y Z

d21 cos θ

d36 sin (2θ)

XZ

0

d21 cos2 θ + d23 sin2 θ − d36 sin (2θ)

m

XY

d13 sin ϕ

d31 sin2 ϕ + d32 cos2 ϕ

Y Z

d31 sin θ

d13 sin2 θ + d12 cos2 θ

XZ

d12 cos θ − d32 sin θ

0

mm2

XY

0

d31 sin2 ϕ + d32 cos2 ϕ

Y Z

d31 sin θ

0

XZ

d32 sin θ

0

222

XY

0

d36 sin (2ϕ)

Y Z

0

d36 sin (2θ)

XZ

0

d36 sin (2θ)

Landolt-B¨ornstein

New Series VIII/1A1

Ref. p. 187]

4.1 Frequency conversion in crystals

151

Table 4.1.4. Units and conversion factors.

Nonlinear coe cient

MKS or SI units

CGS or electrostatic units

χ(1)

1

(SI, dimensionless)

=

1

(esu, dimensionless)

ij

4 π

dij or χ(2)

1

V−1m

=

3 × 104

(erg−1 cm3) 21

ijk

4 π

4 π

1

δij

1

C−1m2

=

(erg−1 cm3) 2

3 × 105

Note that in SI units P (n)

=

ε0 χ(n)E n (with P (n)

expressed in C m−2 ), whereas in CGS or esu

units P (n) = χ(n)E n (with P (n)

expressed in esu).

4.1.2.5 Frequency conversion e ciency

4.1.2.5.1 General approach

The conversion e ciency of a three-wave interaction process for the case of square nonlinearity

P nl = ε0 χ(2)E2

(4.1.14)

can be determined from the wave equation derived from Maxwell’s equations [64Akh, 65Blo, 73Zer, 99Dmi], see also (1.1.4)–(1.1.7),

× × E +

(1 + χ(1)) ∂2E

= −

1

∂2P nl

(4.1.15)

c2

∂t2

ε0 c2

∂t2

with the initial and boundary conditions for the electric field E .

An exact calculation of the nonlinear conversion e ciency for SHG, SFG, and DFG generally requires a numerical calculation. In some simple cases analytical expressions are available. In order to choose the proper method, the contribution of di erent e ects in the nonlinear mixing process should be determined. For this purpose the following approach is introduced [99Dmi]:

–Consider the e ective lengths of the interaction process:

1.Aperture length La:

La = d0 ρ−1 ,

(4.1.16)

where d0 is the beam diameter.

2. Quasistatic interaction length Lqs:

Lqs = τ ν−1 ,

(4.1.17)

where τ is the radiation pulse width and ν is the mismatch of reverse group velocities. For SHG

ν = uω−1 − u2−ω1 ,

(4.1.18)

where uω and u2ω are the group velocities of the corresponding waves ω and 2ω .

3.

Di raction length Ldif :

L

= k d2 .

(4.1.19)

dif

0

4.

Dispersion-spreading length Lds:

Lds = τ 2g−1 ,

(4.1.20)

Landolt-B¨ornstein

New Series VIII/1A1

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