EE346 NLO

1/13/21, #3 slide 1

3_Crystal Optics

EE 346 Nonlinear Optics

M.M. Fejer
fejer@stanford.edu
01/13/21
 EE346 NLO
1/13/21, #3 slide 2
Last time
Studied second harmonic generation as prototypical nonlinear interaction
Eω ( z ) = Eω 0
χ (2) E2ω ( L) = ? matching length of
crystal instead
z=0 z=L much
phasematched case still gives
conversion than local Max
Found that phase velocity mismatch ∆k was a keyhigher
parameter in the efficiency:
4π
∆k = k2ω − 2kω = ( n2ω − nω )
λω
1 η
I ( L) ∆k L
η ≡ 2ω = η PM ,0 sinc 2 ηPM
Iω (0) 2
sinc( x ) ≡ sin( x ) / x

2π 2 Z 0 χ (2)2 0.5
η PM ,0 = Iω 0 L2
n2ω nω λω
2 2

need ∆k << π/L

0
−5 -10 -5 0 5 10 ∆kL / 2
How to obtain n2ω − nω ~ 10 ?
leads to study of birefringent media
 EE346 NLO
1/13/21, #3 slide 3
Today

• Crystal symmetry and the dielectric tensor

• Formalism for plane waves in anisotropic media

• Specific results for eigenpolarizations and refractive indices in

uniaxial media

• Brief discussion of biaxial media

• Double refraction, Poynting-vector walkoff

• Reading
Harris Ch.2 pp 1-37
Yariv and Yeh 4.1-4.6
Yariv 5.2-5.4
 EE346 NLO
1/13/21, #3 slide 4
Dielectric Tensor

• Dielectric tensor relates displacement and electric field:

D = ε 0ε : E
– notation: use ↔
to indicate tensor of any rank
use : to indicate suitable contraction
– here ε relates two vectors, hence a second rank tensor
• Basic properties of dielectric tensor:
– can show ε Hermitian in lossless media (Harris, Ch. 2, app. A)
– if in addition medium is non-gyrotropic (no optical activity or
magneto-optic effects) ε is real
clear discussion of gyrotropic cases in Yariv and Yeh
• Consider lossless nongyrotropic case here
– most general form consistent with these assumptions:

ε xx ε xy ε xz
ε = ε xy ε yy ε yz
ε xz ε yz ε zz
 EE346 NLO
1/13/21, #3 slide 5
Symmetries of Dielectric Tensor

ε xx ε xy ε xz ε XX 0 0
ε = ε xy ε yy ε yz ε= 0 ε YY 0
#3.4 ⇒ real symmetric tensor
ε xz ε yz ε zz ⇒ real eigenvalues in 0 0 ε ZZ
real orthogonal basis

• Basis vectors referenced to crystallographic axes

ˆ ,Y
basis: X
t
{
ˆ ,Z
ˆ }
– notation: X {
ˆ ,Y ˆ ,Z }
ˆ for crystal frame diagonalizes E
{xˆ , yˆ , zˆ} for lab frame
• Symmetry of dielectric tensor related to crystal point group
– isotropic or cubic: εXX= εYY= εZZ, principal axes arbitrary
optically isotropic, can use a scalar dielectric constant ε: D = εε0E
– hexagonal, tetragonal, trigonal: εXX= εYY, X ˆ ,Y { }
ˆ arbitrary in plane ⊥ Ẑ
Ẑ along six-fold, four-fold, three-fold rotation axis, respectively
known as “uniaxial” crystals
ˆ ,Y
– orthorhombic: εXX≠ εYY ≠ εZZ, X {
ˆ ,Z }
ˆ all fixed to crystal axes
known as “biaxial”
ˆ ,Y
– monoclinic, triclincic: εXX≠ εYY ≠ εZZ, X ˆ ,Z{ }
ˆ depend on wavelength
“biaxial”, “dispersion of the axes”
 EE346 NLO
1/13/21, #3 slide 6
Effect of Crystal Symmetry
• All crystals belong to 1 of 32 point groups
– symmetry of dielectric tensor controlled by point group
Z Z
Z
hexagonal Z tetragonal
cubic trigonal 4
4 6
3

Y Y Y Y

X X X X
ε XX 0 0
isotropic 0 ε XX 0 ε XX 0 0
0 0 ε XX uniaxial 0 ε XX 0
0 0 ε ZZ
biaxial, X and Z
triclinic
Z orthorhombic Y biaxial, X, Y and Z
axes dispersive
biaxial monoclinic axes dispersive
2 2 ε XX 0 ε XZ
ε XX 0 0 ε XX ε XY ε XZ
0 ε YY 0
0 ε YY 0 ε XY ε YY ε YZ
ε XZ 0 ε ZZ
0 0 ε ZZ ε XZ ε YZ ε ZZ
X Z
Y see D.A. Roberts, IEEE J. Quantum Electron. 28, pp.2057-74 (1992)
X regarding confused conventions for biaxial crystals
 EE346 NLO
1/13/21, #3 slide 7
Plane Waves in Anisotropic Media
consider uniaxial E ρ D
crystal S
ρ
⊗ k
B H
• Consider plane wave in linear, uniform anisotropic medium
– propagates as e
i ( k ⋅r −ωt )
⇒ ∇ → ik , ∂ / ∂t → −iω
• Maxwell equations become:
∇ × E = −∂B / ∂t → k × E = ωB 1 ⇒ B ⊥ E, k
∇ × H = ∂D / ∂t → k × H = −ω D 2 ⇒ D ⊥ H, k
∇⋅D = 0 → k ⋅D = 0 3 ⇒D ⊥ k
∇⋅B = 0 → k ⋅B = 0 4 ⇒ B⊥k
anisotropic
for
media
nonmagnetic: B = µ0 H ⇒ B H

E in plane ⊥ B, but not necessarily || D. Angle ρ depends on E = ε 0 ε : D

−1
A will be parallel only in special cases (#3.8)
E not transverse, in general
Poynting vector: S = E × H ⇒ S ⊥ (E, H )
energy flow in general is not along k
 EE346 NLO
1/13/21, #3 slide 8
When Is E Parallel to D?
in principal axis frame #3.5 ⇒

E ρ D ε XX
−1
0 0 DX
S E = ε 0−1ε −1 : D = ε 0
−1
0 ε YY−1 0 DY
ρ
⊗ k 0 0 ε ZZ
−1
DZ
B H

• Isotropic media: ε XX = ε YY = ε ZZ ≡ ε ⇒ E = ε 0ε D
−1

⇒ E D⇒ ρ = 0
J ∈ ( X, Y , Z )
• If D along a principal axis of ε , result is simple: E = EJ Jˆ = ε 0−1ε JJ−1 DJ Jˆ
⇒ E D⇒ ρ = 0
– like an isotropic case, but |ε| depends on polarization: E X = DX / ε 0ε XX
EY = DY / ε 0ε YY
EZ = DZ / ε 0ε ZZ
• General case: D not along a principal axis of ε
⇒ E = ε 0−1 ε XX
−1
( ˆ + ε −1 D Y
DX X YY Y
ˆ + ε −1 D Z
ZZ Z
ˆ )
⇒ E not parallel to D, ρ ≠ 0
 EE346 NLO
1/13/21, #3 slide 9
Polarization Eigenvalues and Eigenvectors

• How to determine dispersion relations and eigenpolarizations in

anisotropic media?
and displacementfield
– i.e. orientations of electric field that propagate unchanged
• Return to relation derived from Maxwell equations in #2.4:
∂2D
∇ ( ∇ ⋅ E ) − ∇ E = − µ0 2
2

∂t
– for our plane wave ~ Eei ( k ⋅r −ωt ) and D = ε 0 ε : E ⇒
k ( k ⋅ E ) − k 2 E = −(ω 2 / c 2 ) ε : E

( )
let k ≡ kkˆ , k ≡ nω / c ⇒ n 2 kˆ kˆ ⋅ E − E = − ε : E polarization eigenvalue equation
eigenvalue n to be determined

• Consider first the simple case where D is along a principal axis, Ĵ

– then (#3.8) E D and kˆ ⋅ E = 0 ⇒ n 2 E = ε : E
n 2 E Jˆ = ε E Jˆ ⇒ n = ε JJ
2
J JJ J

• For example, for k Xˆ , there are two transverse polarization eigenmodes:

E Y ˆ ⇒ n2 = ε E Zˆ ⇒ n2 = ε
YY ZZ
 EE346 NLO
1/13/21, #3 slide 10
Polarization Eigenvalues and Eigenvectors II

• For the general case where E is not parallel to D, more complicated

• Consider simplest (and most common) case, a uniaxial crystal (ε YY = ε XX )
ε XX 0 0
ε= 0 ε XX 0
0 0 ε ZZ

• Assume a plane wave propagating along ẑ, at an angle θ to Ẑ

Y y
rotate tensor into lab frame:
ε xx 0 0 ε xx = ε XX
Ẑ
ε= 0 ε yy ε yz ε yy = ε XX cos 2 θ + ε ZZ sin 2 θ
θ
⊗ zˆ , k 0 ε yz ε zz
X, x ε zz = ε XX sin 2 θ + ε ZZ cos 2 θ
Lab and crystal frames In lab frame ε yz = ( ε ZZ − ε XX ) sin θ cosθ

(#3.9) ⇒ ( )
n 2 kˆ kˆ ⋅ E − E = − ε : E n 2 [ E − Ez zˆ ] = ε : E
kˆ = zˆ
 EE346 NLO
1/13/21, #3 slide 11
Polarization Eigenvalues and Eigenvectors III

• Take Cartesian components of n 2 [ E − Ez zˆ ] = ε : E from (#3.10) :

ε xx = ε XX a
n 2 Ex = ε xx Ex 1 ε xx 20 0 E2 x
ε yy = ε XX cos θ + ε ZZ sin θ b
n 2 E y = ε yy E y + ε yz Ez 2 ε= 0 ε ε E
ε zz = ε XX sin 2 θyy + ε ZZyz cos 2 yθ c
0 = ε yz E y + ε zz Ez 3 0 ε ε E
ε yz = ( ε ZZ − ε XXyz ) sinzzθ cosθz d

one trivial solution:

1 & a ⇒ n = ε XX ≡ no
2 2 ˆ
E = Eo X “ordinary wave”

propagation constant independent of θ. Electric field ⊥ k.

second solution requires more work: E-field may not be transverse:

ε yz E = E y yˆ + Ez zˆ ŷ
3 ⇒ Ez = − Ey 4 Ŷ
E
ε zz “extraordinary wave” ρ
Ẑ
walkoff angle ρ: 4 ⇒ θ
⊗ zˆ , k
tan ρ = E z / E y = −ε yz / ε zz ˆ , xˆ , E
X x

c & d ⇒ =
(ε XX − ε ZZ ) sin θ cosθ Electric field not ⊥ k unless θ = 0 or π/2.
ε XX sin θ + ε ZZ cos θ
2 2
 EE346 NLO
1/13/21, #3 slide 12
Polarization Eigenvalues and Eigenvectors IV

relate ne (θ ) to crystal properties ε XX , ε ZZ :

2

eliminate Ez from 2 with 4 :

⇒ n = ε yy − ε yz / ε zz ≡ ne (θ ) 5
2 2 2
(#3.11) 4 in 2

ε yy ε yz ε XX 0
e (
5 ⇒ n (θ ) = ε yyε zz − ε
2 2
yz ) / ε zz = ε
yz ε zz
=
0 ε ZZ
= ε XX ε ZZ
determinant indep.
of rotation

⇒ ne2 (θ ) = ε XX ε ZZ / ε zz ⇒ ne−2 (θ ) = ε zz / ε XX ε ZZ

(#3.11) c : ε zz = ε XX sin θ + ε ZZ cos θ

2 2

−1/2
} ⇒
1
ne2 (θ )
=
sin 2

ε ZZ
θ
+
cos 2

ε XX
θ

sin θ cos θ
2 2
notation: ε XX ≡ no2
ne (θ ) = 2
+
ne no2
ε ZZ ≡ ne2
equation for an ellipse
easily confused with ne2 (θ )

special cases:
ŷ E E isotropic E
Ŷ ρ
Ŷ y θ = 0 : ne (0) = no Ẑ y θ = 90° : ne (90°) = ne
Ẑ
θ zˆ , k Ẑ ˆ
zˆ , k , −Y
x̂⊗ zˆ , k x⊗ x⊗
 EE346 NLO
1/13/21, #3 slide 13
Normal Surface

• Convenient geometric construct for interpreting anisotropic

propagation: “normal surface”
– note that extraordinary index is polar expression for an ellipse
uniaxial: −1/2 no2 = ε XX
ε XX sin θ cos θ
2 2
0 0 ne (θ ) = + “ordinary” index
0 ε XX 0 ne2 no2 ne2 = ε ZZ
0 0 ε ZZ “extraordinary” index
Z
no (θ ) = no no ne (θ )
k̂

θ
ne
X

Positive uniaxial:
ne > no

Z known as “optical axis”

 EE346 NLO
1/13/21, #3 slide 14
Normal Surface II

• Other useful geometrical interpretations associated with index surface

– state without proof here. see Yariv and Yeh for good discussion
• Eigenpolarization given by tangent to surface
• Poynting vector given by normal to surface

E ~ E j ei (ωt −k j r)
Z ne (θ ) Se
ωn j no
kj = k̂
c
So Ee
j = ( o, e ) θ ⊗ D , E De ρ
o o ne
X

Ez ( ε XX − ε ZZ ) sin θ cosθ
tan ρ ≡ =
E y ε XX sin 2 θ + ε ZZ cos 2 θ

convenient form for walkoff angle: ⇒ ρ ≈ no − ne sin(2θ )

first order in ne-no n
n = (ne + no ) / 2
 EE346 NLO
1/13/21, #3 slide 15
Typical Normal Surfaces
Uniaxial ne2 = ε ZZ
Z no2 = ε XX = ε YY
positive: ne > no no negative: ne < no Z n
o

ne ne
X X

Biaxial nZ > nY > nX similar concepts to uniaxial; see Harris ch. 2 or Yariv and Yeh for details
n = ε ZZ
2
Z
Z n = ε XX
2
X
Z Y
nY nZ
nY2 = ε YY
nY nX
nX
nX
nZ nZ nY
Y X X
 EE346 NLO
1/13/21, #3 slide 16
Poynting-Vector Walkoff

• Consider an e-wave and an o-wave with same k-vector direction

– will see that this is common in phasematched NLO

Eo k̂
⊗

Ee
– associated Poynting vectors are in general not parallel
kˆ , Sˆ
ρ
o S = E×H
Sˆ e

• Finite diameter beams will separate after a characteristic distance

ρ no longer interact

• Will see that this effect has major impact on wave-mixing efficiency
 EE346 NLO
1/13/21, #3 slide 17
Some Phenomena Associated with Crystal Optics
• Reflection and refraction become more complicated
x̂ boundary conditions require:
Z
ne , no α k in ⋅ xˆ = k out ⋅ xˆ
X ordinary wave:
k in φ ω ω
“bireflection” in no sin(φin ) = no sin(φout ,o )
φout , o c c
k out ,o φout ,e ⇒ φin = φout ,o
k out ,e but for extraordinary wave:
ω ω
ne (θin )sin(φin ) = ne (θ out )sin(φout )
Glan-Thompson prism c c
sin(φout ,e ) n (θ ) n (φ + α )
⇒ = e in = e in
sin(φin ) ne (θ out ) ne (φout − α )
angle of reflection not necessarily equal
Wollaston prism
to angle of incidence

similar considerations lead to

more than one refracted beam
“double refraction”
Figs from Wikipedia
 EE346 NLO
1/13/21, #3 slide 18
Next

• Use of birefringent crystals for phasematching

• Classical model for dipole susceptibilities