Selected Topics in Advanced Optics

Week 3 – part 1

Olivier J.F. Martin

Nanophotonics and Metrology Laboratory
 Module 2: Material properties and optical constants
• B.E.A. Saleh & M.C. Teich, Fundamental of photonics 2nd Ed. (Wiley, Hoboken,
2007), Chapters 5 & 6.
• C.F. Bohren & D.R. Huffman, Absorption and scattering of light by small particles
(Wiley, New York, 1983).
• Optical Society of America, Handbook of optics,2nd Ed. (Mc Grawn Hill, New York,
1995), Vol. II, Chapter 33.

Olivier J.F. Martin

Maxwell’s equations without sources
• This is the form generally used in optics
∂B ( r, t )
∇ × E ( r, t ) = − ∇ ⋅ D ( r, t ) = 0
∂t
∂D ( r, t )
= ∇ × H ( r, t ) ∇ ⋅ B ( r, t ) 0
=
∂t
• The electric and magnetic properties of the medium are
described by the constitutive relations:
D= ε 0 E + P= ε 0 E + ε 0 χ E= ε 0 (1 + χ )E= ε 0ε r E
B = µ0 H + µ0 M = µ0 µ r H P : polarization density
M : magnetization density
• P and M depend on the applied fields E and H. This dependence describes the
response of the medium
• Although the matter is neutral, it does not mean that charges cannot respond to the
applied fields ! Olivier J.F. Martin
Classical theories of optical constants
• Two sets of quantities are used to describe the optical properties: the complex
refractive index N= n= n + jk
and the complex dielectric function (or relative permittivity) ε r= ε ′ + jε ′′
• We assume non-magnetic materials ( µ r = 1)
• Both quantities are related:
ε ′2 + ε ′′2 + ε ′
n=
ε=′ n − k
2 2
2
ε ′′ = 2nk ε ′2 + ε ′′2 − ε ′
k=
2

Olivier J.F. Martin

 Selected Topics in Advanced Optics

Week 3 – part 2

Olivier J.F. Martin

Nanophotonics and Metrology Laboratory
Electromagnetic waves in dielectric media
• Most phenomena relevant to optics concern dielectric materials (i.e. magnetic
effects can be neglected)
• In response to an applied electric field E, a dielectric medium creates a polarization
density P:

• This response characterizes the medium:

– Linear (linear relation between E and P)
– Nondispersive: instantaneous response
– Homogeneous: relation between E and P independent of the position
– Isotropic: relation between E and P independent of the direction of E, the vectors E and P
must be parallel
– Spatially nondispersive: the relation between E and P is local; i.e. P is only influenced by
E at the same point (optically active materials are spatially dispersive).

Olivier J.F. Martin

Linear, nondispersive, homogeneous, isotropic media
• P and E are parallel and proportional:

P ( r, t ) = ε 0 χ E ( r, t ) χ : electric susceptibility
• Maxwell’s equations become:
D ( r, t ) =+
ε 0 (1 χ ) E ( r, t ) =
ε 0ε r E ( r , t ) =
ε E ( r, t )

∂H ( r, t )
∇ × E ( r, t ) = − µ ∇ ⋅ E ( r, t ) = 0 ε = ε 0ε r
∂t
∂E ( r, t ) µ = µ0 µ r
∇ × H ( r, t ) ε
= ∇ ⋅ H ( r, t ) 0
=
∂t
• Wave equation for each field component:

1 ∂ 2
u 1 c0 εµ
∇ 2u − 2 2 = 0 with c = and n = =
c ∂t εµ c ε 0 µ0
Olivier J.F. Martin
Inhomogeneous media
• Inhomogeneous wave equations:

1 E ( r, t )
2
ε0 ∂
∇ × ( ∇ × E ( r, t ) ) = − 2
ε (r ) c0 ∂t 2
 ε0  1 H ( r, t )
2
∂
∇ ×  ∇ × H ( r, t )  = − 2
 ε ( r )  c0 ∂t 2

• Often the equation for the electric field is written:

 1  ∂ 2
E ( r, t )
∇ E ( r, t ) + ∇ 
2
∇ε ( r ) ⋅ E ( r, t )  − µ0ε ( r ) =0
 ε (r )
2
 ∂t
• For a medium varying slowly in space:

∂ 2
E ( r, t )
∇ E ( r , t ) − µ 0ε ( r )
2
2
0
∂t
Olivier J.F. Martin
Anisotropic media
• Tensorial susceptibility and permittivity:

=Pi ∑=
ε χ E
j
0 D ∑ε
ij j i
j
ij Ej

 Dx   ε xx ε xy ε xz   Ex 
     
= Dy   ε yx ε yy ε yz  ⋅  E y 
D  ε ε zy ε zz   Ez 
 z  zx

• E and D are not parallel !

• Most crystals (including semiconductors) are anisotropic

Olivier J.F. Martin

Anisotropic media – Refractive indices
• Permittivity tensor Di = ∑ ε ij E j
j

• Can be represented by an ellipsoid (because it is a symmetric tensor of second

rank)

∑ε
ij
x xj =1
ij i quadratic representation

ε1 x12 + ε 2 x22 + ε 3 x32 =

1 in the principal coordinate system
(ε ij is diagonal)
D1 ε=
= 11 E1 ε1 E1 =
D2 ε 22
= E2 ε 2 E2 =
D3 ε =
33 E3 ε 3 E3

=n1 ε1 / ε 0
= n2 ε2 / ε0
= n3 ε3 / ε0
principal refractive indexes Olivier J.F. Martin
Anisotropic media – Refractive indices
• Biaxial crystal: n1 ≠ n2 ≠ n3
• Uniaxial crystal: n1 = n2 ≠ n3 n1 = no ordinary index
n2 =
n3 = ne extraordinary index
positive uniaxial : ne > no
negative uniaxial : ne < no
z - axis ( no for propagation along z ) = optical axis
• Isotropic crystal: n=
1 n=
2 n3
1
• Impermeability tensor: E = ε −1 ⋅ D = η⋅ D
ε0
• Index ellipsoid:

∑η
ij
x xj =1
ij i ellipsoid of
revolution for a
x12 x22 x32 uniaxial crystal
2
+ 2+ 2 =1
n1 n2 n3 Olivier J.F. Martin
Anisotropic media – Propagation/polarization along the principal axes
• Linear polarized plane wave traveling along one of the principal axes ( x, y, z ) and
polarized parallel to another principal axis:

• The polarization direction of the electric field determines the phase velocity
• These 3 waves keep their velocities and polarizations:
normal modes of the crystal

Olivier J.F. Martin

Nonlinear media
• The relation between P and E is nonlinear.
• The superposition principle is not valid anymore !
• For a nonlinear, but homogeneous isotropic medium, one can derive the following
wave equation:

1
∇ E ( r, t ) − 2
2 ∂ 2
E ( r , t ) µ0
=
∂ 2
P ( r, t )
2
c0 ∂t ∂t 2
• For nondispersive, nonmagnetic media, the polarization
density can be written as a nonlinear function of E ;
for example:
P ψ (E
= = ) a1E + a2E 2

1
∇ E ( r, t ) − 2
2 ∂ 2
E ( r , t ) µ0
=
∂ 2
ψ (E)
2
c0 ∂t ∂t 2
Olivier J.F. Martin
Nonlinear media

• A nonlinear medium is characterized by a nonlinear relation between P and E

• The relation between P and E is linear when the field E is small, but becomes
nonlinear when E becomes comparable with the interatomic electric field
(E ~ 105 – 108 V/m)
• Macroscopic description: P=Np (p: individual dipole moment induced by the applied
field); either N or p can be nonlinear

P = ε 0 ( χ E + χ (2) E 2 + χ (3) E 3 +)

• In principle the higher order susceptibilities are tensors!

Olivier J.F. Martin
 Selected Topics in Advanced Optics

Week 3 – part 3

Olivier J.F. Martin

Nanophotonics and Metrology Laboratory
Dispersive media
• The relation between P and E is
not instantaneous, it is dynamic and depends on the history of the system. The
polarization density can be expressed as a convolution:
+∞
P ( t ) ε 0 ∫ χ ( t − t ′ )E ( t ′ ) dt ′
=
−∞

 The function ε 0 χ ( t ) represents the impulse response function

of the system.
 Alternatively, one can go to Fourier space and look at the transfer
function of the system : ε 0 χ (ν ) .
 A dispersive medium has a frequency - dependent susceptibility.
 Every material is dispersive!

Olivier J.F. Martin

Dispersive media
• Waves of different wavelengths are refracted differently:

• The frequency-dependent speed of light produces different time delays for the
different spectral components (e.g. low frequency components travel faster than
high frequency ones):

Olivier J.F. Martin

Kramers-Kronig relations
• Absorption and dispersion are related
• A material with a frequency-dependent refractive index must be absorptive (and
conversely)… every material is dispersive!
• Kramers-Kronig relate the real and imaginary parts of the susceptibility:
2 s χ ′′ ( s )
∞
χ ′ (ν ) = ∫ 2 ds
π 0 s −ν 2

(ν ) χ ′ (ν ) + j χ ′′ (ν )
χ=
2 νχ ′ ( s )
∞
χ ′′ (ν ) = ∫ 2 2 ds
π 0ν − s

• Hilbert transform pair: χ ′ (ν ) and χ ′′ (ν ) are analytic in the upper complex plane
(related to causality)
• The real part can be computed from the imaginary one and vice-versa

Olivier J.F. Martin

Absorption
• Complex dielectric susceptibility: χ= χ ′ + j χ ′′
ε ε 0 (1 + χ )
• Complex permittivity:=
• ∇ 2U + k 2U =
0 is still valid, but with a complex wavenumber:

k= ω εµ0= k0 1 + χ= k0 1 + χ ′ + j χ ′′

1
k = β − j α = k0 1 + χ ′ + j χ ′′
2

• β : propagation constant of the wave (phase change rate)

• α : absorption coefficient (if α < 0, then γ = -α : gain)
• The sign depends on the convention chosen for exp(+ jωt )
a forward propagating wave: exp(+ jωt − jkr ) will decay if α > 0

Olivier J.F. Martin

Transmission window

Olivier J.F. Martin

A very useful reference
http://refractiveindex.info

Olivier J.F. Martin

 Selected Topics in Advanced Optics

Week 3 – part 4

Olivier J.F. Martin

Nanophotonics and Metrology Laboratory
Lorentz model
(book by Bohren and Huffman)
• Now we assume the following time-dependence: exp(− jωt )
• The electrons and ions in matter are treated as simple harmonic oscillators (springs)
• The applied force is given by the local electric field
• Equation of motion:
x + bx + Kx =
m eE

• Solution (oscillatory part):

x=
(e / m) E
=ω02 K=
/m γ b/m
ω02 − ω 2 − jγω
• If γ≠0, the proportionality factor between x and E is complex
→ the displacement and field are usually not in phase
1  γω 
x ( e=
/ m ) EAe with A
jΘ
= Θ arctan  2 2 
ω − ω
(ω02 − ω 2 ) + γ 2ω 2
2
 0 
Olivier J.F. Martin
Lorentz model

• The amplitude is maximum for ω = ω0 and the width inversely proportional to γ

• At low frequency the oscillator is in-phase ( Θ =0 ) and at high frequency it is out of
phase by 180o. The change occurs at ω  ω0
• The induced dipole moment of a single oscillator is p = ex
• For a collection of n oscillators per volume unit, the polarization is P = nex
ω p2
P = ε 0 E plasma frequency : ω 2
p ne 2
/ mε 0
ω0 − ω − jγω
2 2

ω p2
• Since P =ε 0 χ E → ε r =1 + χ =1 + 2
ω0 − ω 2 − jγω Olivier J.F. Martin
Lorentz model

• The real part and the imaginary part of the permittivity are then
ω p2 (ω02 − ω 2 ) ω p2γω
ε ′ =+
1 χ ′ =+
1 ε ′′ =χ ′′ =
(ω 2
0 −ω )
2 2
+γ ω
2 2
(ω 2
0 −ω )
2 2
+ γ 2ω 2

• A region of anomalous dispersion exists around the resonance

• High frequency limits: ω p2 γω p2
(ω  ω0 ) ε ′  1 − 2 ε ′′  3
ω ω
ω p2 ε ′′ γω 2
p
n  ′
ε 1 − k  
2ω 2 2 2ω 3
ω p2 γω p2ω
• Low frequency limits: ( ω  ω0 ) ε ′  1 + 2 ε ′′  4
ω0 ω0 Olivier J.F. Martin
Multiple oscillator model
• The Lorentz model can be extended for a broad range of materials by considering
several resonances (i.e. several oscillators):
ω pj2
ε=
r ε∞ + ∑ 2
j ω j − ω 2
− jγ jω

• ε ∞ represents the effect of all oscillators at high frequency, if

all oscillators are included in the summation, then ε ∞ = 1

Olivier J.F. Martin

Multiple oscillator model
• MgO crystal: reflectance data are well fitted using two oscillators (in this spectral
region)

ω pj2
ε=
r ε∞ + ∑ 2
j ω j − ω − jγ jω
2

ε ∞ = 3.01
=ω1 401cm
= −1
γ 1 7.62 cm −1=
ω p21 / ω12 6.6
=ω2 640
= cm −1 γ 2 102.4 cm=
−1
ω p2 2 / ω22 0.045
Olivier J.F. Martin
Multiple oscillator model
• The permittivity of hemoglobin depends on the oxygen level

Olivier J.F. Martin

Multiple oscillator model
• A simple model with three oscillators reproduces this permittivity very well, but the
oscillators are different for the oxygenated and de-oxygenated states:

Olivier J.F. Martin

Drude model (for metals)
• The spring constant is set to zero K = 0
• As a result: ω0 = 0
ω p2
εr = 1−
ω 2 + jγω

ω p2 ω p2γ
ε′ =
1− 2 ε ′′ =
ω +γ 2
ω (ω 2 + γ 2 )

• The real part of the permittivity is negative !

• The following website gathers parameters for the Drude model for many metals:
http://www.wave-scattering.com/drudefit.html
• For one metal, there are often different possible fits, depending on the wavelength
range of interest !

Olivier J.F. Martin

Plasmonic metals
• Coinage metals (noble metals, group 11): Cu, Ag, Au
• The plasma frequency determines the optical range where plasmonic effects can be
excited
• Further plasmonic metals include Al, W, Pt

Olivier J.F. Martin

 Selected Topics in Advanced Optics

Week 3 – part 5

Olivier J.F. Martin

Nanophotonics and Metrology Laboratory
Spectral line shapes
• It is often useful to fit a function on the spectral response of a system
• There are three such main functions
• Lorentzian: • Gaussian: • Voigt:
1 p − p0 ∞
=L( x) = x G ( x) = e −( ln 2 ) x 2
V ( x; σ , γ )
= ∫ G ( x '; σ ) L ( x − x '; γ ) dx '
1 + x2 w/2 −∞

w = FWHM σ , γ = half-widths

wikipedia Olivier J.F. Martin

Spectral line shapes
• In most cases, on can safely use a Lorentzian curve
• A complex spectrum can be decomposed into a collection of simple lines

The spectrum is the sum of two Lorentzians

wikipedia Olivier J.F. Martin