light and matter tim freegarde school of physics & astronomy university of southampton the...
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Light and MatterTim Freegarde
School of Physics & Astronomy
University of Southampton
The tensor nature of susceptibility
2
Birefringence
• asymmetry in crystal structure causes polarization dependent refractive index
• ray splits into orthogonally polarized components, which follow different paths through crystal• note that polarization axes are not related to plane of incidence
3
Anisotropic media
• difference in refractive index (birefringence) or absorption coefficient (dichroism) depending upon polarization
• recall that EEP 100 2
2
21
ciwhere
• susceptibility cannot be a simple scalar
• difference in or implies difference
in
1
2
EP
4
Linear dichroism
• fields normal to the conducting wires are transmitted
• current flow is not parallel to field
WIRE GRID POLARIZER
• susceptibility not a simple scalar
• fields parallel to the conducting wires are attenuated
I
5
Birefringence – mechanical model
x
y
z• springs attach electron cloud to fixed ion• different spring constants for x, y, z axes• polarization easiest along axis of weakest spring
• polarization therefore not parallel to field• susceptibility not a simple scalar
6
Susceptibility tensor
• the Jones matrix can map
• similarly, a tensor can describe the susceptibility of anisotropic media
y
x
y
x
a
a
aa
aa
a
a
2221
1211
JONES MATRIX
ya
xa
ya
xa ,,
EP
333231
232221
131211
0
SUSCEPTIBILITY TENSOR
• e.g. zyxx EEEP 1312110
7
Diagonizing the susceptibility tensor
• if the polarization axes are aligned with the principal axes of birefringent crystals, rays propagate as single beams• the susceptibility tensor is then diagonal
EP
33
22
11
0
00
00
00
DIAGONAL SUSCEPTIBILITY
TENSOR
• a matrix may be diagonalized if symmetrical:
jiij • the optical activity tensor is not
symmetrical; it cannot be diagonalized to reveal principal axes
8
The Fresnel ellipsoid
• surface mapped out by electric field vector for a given energy density
FRESNEL ELLIPSOID
• symmetry axes x’,y’,z’ are principal axes
UDE
zzyyxx
1,
1,
1• semi-axes are
xE
yE
zE
9
The Fresnel ellipsoid
• allows fast and slow axes to be determined:
FRESNEL ELLIPSOID
xE
yE
zE
• establish ray direction through Poynting vector
• electric field must lie in normal plane
• fast and slow axes are axes of elliptical cross-section
• axis lengths are
slowfast
1,
1
S
• allows fast and slow axes to be determined:
10
The optic axis
• if the cross-section is circular, the refractive index is independent of polarization
FRESNEL ELLIPSOID
xE
yE
zE
S• the Poynting vector then defines an optic axis• if , the single optic axis lies
along (uniaxial crystals)
yyxx z
• if , there are two, inclined, optic axes (biaxial crystals)
yyxx
11
Uniaxial crystals
FRESNEL ELLIPSOID
xE
yE
zE
S
• the single optic axis lies alongz optic axis
• one polarization is inevitably perpendicular to the optic axis (ordinary polarization)• the second polarization will be orthogonal to both the ordinary polarization and the Poynting vector
(extraordinary polarization)• positive uniaxial: oe • negative uniaxial: eo
12
Poynting vector walk-off
• Poynting vector obeys 0SE• wavevector vector obeys 0kD• in anisotropic media, and are not
necessarily parallelE D
• the Poynting vector and wavevector may therefore diverge
S
E
D
kwavevector
Poynting vector Fresnel
ellipsoid
13
How light interacts with matter
• atoms are polarized by applied fields
• Lorentz model: harmonically bound classical particles
220
2x
mEP 0 EPED
10
0
xmx
Vxm 2
0d
d
xV
x
E
14
Quantum description of atomic polarization
1
tie 02
tibat 0exp21, r
energy
0
0
1 2
• harmonic oscillator• two-level atom
2exp1,0
tit
r • electron density depends upon relative phase of superposition components
• weak electric field
15
Quantum description of atomic polarization
x/a0 x/a0
2exp1,0
tit
r
1 2
• electron density depends upon relative phase of superposition components
1
tie 02
energy
0
0• harmonic
oscillator• two-level atom
• weak electric field
16
Optical nonlinearity
• potential is anharmonic for large displacements
43220
2cxbxx
mxV
xV
x
220
2x
m
332210 EEEP
• polarization consequently varies nonlinearly with field
• in quantum description, • uneven level spacing• distortion of
eigenfunctions• higher terms in perturbation
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Optical nonlinearity
• potential is anharmonic for large displacements
43220
2cxbxx
mxV
xV
x
332210 EEEP
• polarization consequently varies nonlinearly with field
• in quantum description, • uneven level spacing• distortion of
eigenfunctions• higher terms in perturbation
x
V
d
d
18
Electro-optic effect
• nonlinearity mixes static and oscillatory fields
332210 EEEP
x
x
V
d
d
EEEP 320
20
10 32
• susceptibility at hence controlled by 0E
• exploit the nonlinear susceptibility
• Pockels effect; Kerr effect
0E
19
Second harmonic generation
x
x
V
d
d
332210 EEEP
• again exploit the nonlinear susceptibility
• distortion introduces overtones (harmonics)
2210 EEP
where 22cos1cos 22 tEtE
20
Nonlinear tensor susceptibilities
• nonlinear contributions to the polarization depend upon products of electric field components
• each product corresponds to a different susceptibility coefficient
zyxkj
kjijkzyxj
jiji EEEP,,,
2
,,
10
e.g. zyxjzyxiEEEE ji ,,;,,,2,121
• terms in the susceptibility expansion are therefore tensors of increasing rank
• the induced polarization has three components (i =x,y,z):
21
Nonlinear tensor susceptibilities
• the susceptibility depends upon the frequencies of the field and polarization components
213 23
113
1
0
1 :: EEP
e.g. if , 21 EEE
2211 223
2113
2 ,:,: EEEE
1221 1232
2132 ,:,: EEEE
• any susceptibility unless 0,: 2132 213
22
Symmetry in susceptibility
• the susceptibility tensor may be invariant under certain symmetry operations
e.g. • rotation• reflection
• the symmetries of the susceptibility must include – but are not limited to – those of the crystal point group
• optically active materials fall outside the point group description (nonlocality)
• materials showing inversion symmetry have identically zero terms of even rank
• inversion zyxzyx ,,,,
23
Properties of susceptibility
• depends upon frequency
• dispersion and absorption in material response
• depends upon field orientation
• anisotropy in crystal and molecular structure
• depends upon field strength
• anharmonicity of binding potential hence nonlinearity
• tensor nature of susceptibility
• series expansion of susceptibility
24
Pockels (linear electro-optic) effect
x
x
V
d
d
• nonlinearity mixes static and oscillatory fields
0E
EEχEχP 021
0 0,: 02 ,0: EEχ
• applying intrinsic permutation symmetry,
021 0,:21 Eχχε 2
03 0,0,:3 Eχ
• in non-centrosymmetric materials, dominates
2χ
25
Kerr (quadratic electro-optic) effect
x
x
V
d
d
• nonlinearity mixes static and oscillatory fields
0E
EEχEχP 021
0 0,: 02 ,0: EEχ
• applying intrinsic permutation symmetry,
021 0,:21 Eχχε 2
03 0,0,:3 Eχ
• in centrosymmetric materials, 02 χ
26
Pockels cell
polarizer
polarizermodulation voltage
• voltage applied to crystal controls birefringence and hence retardance
• mounted between crossed linear polarizers
• longitudinal and transverse geometries for modulation field• allows fast intensity modulation and beam switching