Model-free extraction of refractive index

from measured optical data

A Tool for Refractive InDex Simulation

Martina Schmid, Guanchao Yin, Phillip Manley

Helmholtz-Zentrum Berlin,
Nanooptical concepts for photovoltaics
Motivation

Thin film optics

having to deal with multiple reflections

and requiring refractive indices
often only rely on optical measurements.
Contents

• Basic Principles
• Transfer Matrix Method
• Multilayer Stack
• Comparison to Experiment
• Advanced Features
• Surface Roughness
• Inhomogeneous Layers
• Effective Medium
• User Interface
• Outlook

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 Basic Principles – Transfer Matrix Method
Basic Principles: Transfer Matrix Method Advanced Features User Interface

one wave with positive direction(E+)

Superposition of electric field -
one wave with negative direction(E )

Propagating through an interface:

𝐸𝑖 + 1 1 𝑟𝑖,𝑗 𝐸𝑗 +
− = −
𝐸𝑖 𝑡𝑖 𝑗
,
𝑟𝑖,𝑗 1 𝐸𝑗
𝑁 −𝑁 2𝑁 2𝑁𝑗
𝑟𝑖,𝑗 =-𝑟𝑗,𝑖 =𝑁𝑖+𝑁𝑗, 𝑡𝑖,𝑗 = 𝑁 +𝑁𝑖 , 𝑡𝑗,𝑖 =𝑁 +𝑁 ;
𝑖 𝑗 𝑖 𝑗 𝑖 𝑗

𝑟, 𝑡 are, respectively, the complex amplitude reflection and

transmission Fresnel coefficients; 𝑁 is the complex
refractive index of the layer

Propagating within a layer:

𝐸𝑖 + Φ−1 o E,i+ 2𝜋
− = Φ=𝑒 −𝑖 𝜆 𝑁𝑖𝑑
𝐸𝑖 o Φ E,i−
Propagation through
mediums at Where d is the thickness of medium, ω is the frequency of
the propagating light and c is the speed of light
normal incidence 4
 Oblique incidence
Basic Principles: Transfer Matrix Method Advanced Features User Interface

𝞱𝑖 𝞱𝑖 En la interfaz Dentro de la capa

Medio i

P polarization:
Medio j
𝞱𝑗 𝑁𝑗 𝑐𝑜𝑠𝞱𝑖 − 𝑁𝑖 𝑐𝑜𝑠𝞱𝑗
𝑟𝑖,𝑗 =
𝑁𝑗 𝑐𝑜𝑠𝞱𝑖 + 𝑁𝑖 𝑐𝑜𝑠𝞱𝑗
2𝑁𝑖 𝑐𝑜𝑠𝞱𝑖
𝑡𝑖,𝑗 =
𝑁𝑗 𝑐𝑜𝑠𝞱𝑖 + 𝑁𝑖 𝑐𝑜𝑠𝞱𝑗
2𝜋
−𝑖 𝜆 𝑁𝑚 𝑑/𝑐𝑜𝑠𝞱𝑗
Φ=𝑒
S polarization:
𝑁𝑖 𝑐𝑜𝑠𝞱𝑖 − 𝑁𝑗 𝑐𝑜𝑠𝞱𝑗
𝑟𝑖,𝑗 =
𝑁𝑖 𝑐𝑜𝑠𝞱𝑖 + 𝑁𝑗 𝑐𝑜𝑠𝞱𝑗
2𝑁𝑖 𝑐𝑜𝑠𝞱𝑖
𝑡𝑖,𝑗 =
𝑁𝑖 𝑐𝑜𝑠𝞱𝑖 + 𝑁𝑗 𝑐𝑜𝑠𝞱𝑗

Coeficientes de Fresnel
para incidencia oblicua
 Coherent Layers – Interference Effects
Basic Principles: Multilayer Stack Advanced Features User Interface

Validity condition:
𝑑
n << 1
∆𝜆𝐶𝑜ℎ𝑒𝑟𝑒𝑛𝑐𝑒
θ

Phase difference between

transmission orders:
2𝜋
𝛿= 2𝑛𝑑 cos 𝜃
𝜆

When δ = 2𝑚𝜋 , 𝑚 ∈ ℕ there will

be constructive interference in T
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 Incoherent Layers & Substrate Layers
Basic Principles: Multilayer Stack Advanced Features User Interface

To removed coherency, calculate the

Intensity instead of the Electric Field

෤ ෤
𝐼 = 𝐸 ∗ 𝐸 = |𝐸0 |2 𝑒 𝑖𝑘𝑛𝑑 𝑒 −𝑖𝑘𝑛𝑑 = |𝐸0 |2

phase information
𝑡
>> 1
∆𝜆𝐶𝑜ℎ𝑒𝑟𝑒𝑛𝑐𝑒

Phase relationships between

interior reflections is destroyed –
therefore there is no interference
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Multilayer Stack
Basic Principles: Multilayer Stack Advanced Features User Interface

Coherent Stack
• Includes interference
• Typical thickness 0 ~ 2000 nm

Incoherent Layer
• Interference “turned off”
• Typical thickness 1 mm

• 9 Total layers implemented in RefDex

• Combine coherent and incoherent layers in any order

• For R,T calculation, d, n and k must be known for all layers

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Input Spectrum – R and T
Basic Principles: Comparison to Experiment Advanced Features User Interface

Absorbing Region

• Reflection loses
coherency peaks
• Transmission
drops to zero due
to absorption

Transparent Region

• R and T both show

coherency peaks
• R does not drop to
0 due to reflection
from glass
substrate

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Comparison to Experiment
Basic Principles: Comparison to Experiment Advanced Features User Interface

An example:

thin film
on substrate

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Problem of Uniqueness
Basic Principles: Comparison to Experiment Advanced Features User Interface

𝑅𝑐𝑎𝑙 𝑛 λ , 𝑘 λ − 𝑅𝑒𝑥𝑝 λ =0 Choose the n, k values

which minimise the
difference between our
𝑇𝑐𝑎𝑙 𝑛 λ , 𝑘 λ − 𝑇𝑒𝑥𝑝 λ =0 model and experiment

𝐹 𝑛, 𝑘 = 𝑅𝑐𝑎𝑙 𝑛 λ , 𝑘 λ − 𝑅𝑒𝑥𝑝 λ Adding these equations

together we get a function 𝐹
+ 𝑇𝑐𝑎𝑙 𝑛 λ , 𝑘 λ − 𝑇𝑒𝑥𝑝 λ which takes n and k as input

Problems arise because two

𝐹 𝑛′, 𝑘′ = 𝐹 𝑛′ ′, 𝑘′′ = 0 different n,k input pairs can both
equal zero!

One Physically Many Unphysical

Meaningful Solution Solutions
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Problem of Uniqueness – Physical Picture
Basic Principles: Comparison to Experiment Advanced Features User Interface

Spurius solution branches

Physically meaningful solution

Results need to be
interpreted – More
on this Later!

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 Determination of optical constants in multiple-layer configuration
Basic Principles: Comparison to Experiment Advanced Features User Interface

Take the configuration of CIGSe/TCO/glass substrate as an example:

G. Yin et al., Influence of substrate and its temperature on the optical constants
of CuIn1-xGaxSe2 thin films, accepted for Journal of Physics D: Applied Physics 13
Surface Roughness – Effect on R and T
Basic Principles Advanced Features: Surface Roughness User Interface

Absorbing Region

• Reflection Strongly
Reduced
• Transmission Slightly
Reduced

Transparent Region

• R and T reduced
prefferentially at
coherency peaks

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 Modified Transfer Matrix Method – Scalar Scattering Theory
Basic Principles Advanced Features: Surface Roughness User Interface

Scalar Scattering Theory

Rough Interface
′
𝑟𝑖,𝑗 = 𝑟𝑖,𝑗 𝑒𝑥𝑝 −2(2𝜋𝜎/𝜆)2 𝑛𝑖 2
Medium a
′
𝑟𝑗,𝑖 = 𝑟𝑗,𝑖 𝑒𝑥𝑝 −2(2𝜋𝜎/𝜆)2 𝑛𝑗 2
Modified
2
′ 2𝜋𝜎
Fresnel 𝑡𝑖,𝑗 = 𝑡𝑖,𝑗 𝑒𝑥𝑝 − (𝑛𝑖 − 𝑛𝑗 )2 /2
𝜆
coefficients
Medium b 2
′ 2𝜋𝜎
𝑡𝑗,𝑖 = 𝑡𝑗,𝑖 𝑒𝑥𝑝 − (𝑛𝑗 − 𝑛𝑖 )2 /2
𝜆

• 𝜎 is the interface roughness

• Gives us the loss of specular beam
intensity due to interface roughness

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 Modified Transfer Matrix Method - Examples
Basic Principles Advanced Features: Surface Roughness User Interface

Determination of
G. Yin et al.,The effect of surface
optical constants roughness on the determination of
optical constants of CuInSe2 and
CuGaSe2 thin films, J. Appl. Phys.,
133, 213510 (2013)

σ = 9nm σ = 20nm

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Inhomogeneous Layers – Effect on R and T
Basic Principles Advanced Features: Inhomogeneous Layers User Interface

Absorbing Region

• Small reduction in
R and T

Transparent Region

• Coherency
reduced for both R
and T
• Transmission
strongly reduced

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 Inhomogeneous Layers – Coherent / Incoherent Decomposition
Basic Principles Advanced Features: Inhomogeneous Layers User Interface

a)

b)
e)

c)

d)

a) 2D slice through the 3D inhomogeneous film

b) Overlay a rectangular grid
c) The resulting discretised representation of the film
d) Layers containing voids can be modelled incoherently allowing the use of
average layer thicknesses
e) This reduces the number of transfer matrix calculations to 4 18
 Inhomogeneous Layers – Coherent / Incoherent Decomposition
Basic Principles Advanced Features: Inhomogeneous Layers User Interface

𝑅𝑐𝑎𝑙𝑐 𝑛, 𝑘 = 𝑤𝑐 𝑅𝐶 + 𝑤𝐼 𝑅𝐼 (Same equations for T

not shown here)

Standard Calculation

Replace propagation operator inside inhomogeneous layer with:

෡ 𝑖 = ς𝑀 ෡𝑛 𝑚 𝑫 𝑚 ,𝑛 𝑚−1 ෡ 𝑛(0)
෡ 𝑛𝑚,𝑚−1
𝑷 𝑚=1 𝑷𝑚 𝑷0 , 𝑛 𝑚 = ቊ 𝑛 0 , 𝑚 = 𝑒𝑣𝑒𝑛, 𝑚 ≠ 0
¬𝑛 0 , 𝑚 = 𝑜𝑑𝑑

𝑛 0 = 𝑛𝑖∗ or 𝑛 0 = 𝑛𝑣∗

• Void scattering as from a rough surface. (Slide 13)

• Requires statistical knowledge of 3D void distribution as input

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 Inhomogeneous Layers – Modelling Distribution of Voids
Basic Principles Advanced Features: Inhomogeneous Layers User Interface

• Measurement of real 2D surface

used to generate 3D distribution

• From 3D distribution we obtain

inputs for the RefDex calculation

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 Inhomogeneous Layers – Recalculating n and k
Basic Principles Advanced Features: Inhomogeneous Layers User Interface

n k data from an inhomogeneous CISe2 film is in good agreement to the n k data

from a homogeneous film using the inhomogeneous layer feature.
P. Manley et al.,A method for calculating the complex refractive index of inhomogeneous thin films, 21
(submitted)
 Effective Medium Approximation - Background
Basic Principles Advanced Features: Effective Medium User Interface

Volume Fraction Approximation

𝑛𝑒𝑓𝑓 = 𝑤ℎ 𝑛ℎ + 𝑤𝑖 𝑛𝑖
𝑘𝑒𝑓𝑓 = 𝑤ℎ 𝑘ℎ + 𝑤𝑖 𝑘𝑖
• Direct mixing of the two materials via
the volume fraction
• Does not consider polarisation
effects arrising due to mixing

Maxwell Garnett Approximation

𝜀𝑒𝑓𝑓 − 𝜀ℎ 𝜀𝑖 − 𝜀ℎ
= 𝑤𝑖 • Based on elementary electrostatics
𝜀𝑒𝑓𝑓 + 2𝜀ℎ 𝜀𝑖 + 2𝜀ℎ • Assumes spatially separated
polarisable particles

Bruggeman Approximation
𝜀ℎ − 𝜀𝑒𝑓𝑓 𝜀𝑖 − 𝜀𝑒𝑓𝑓 • Assumes two kinds of spherical
𝑤ℎ = −𝑤𝑖
𝜀ℎ + 2𝜀𝑒𝑓𝑓 𝜀𝑖 + 2𝜀𝑒𝑓𝑓 particles randomly arranged.
• Spatial separation between
particles should be small (i.e. 𝑤𝑖 is
large)
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 ELLIPSOMETRY MODE

𝒓𝒑
= 𝐭𝐚𝐧𝚿 𝒆𝒊∆
𝒓𝒔

Type equation here.

𝒓𝒑 • Ellipsometric parameters Ψ and Δ simulated by RefDex

= 𝐭𝐚𝐧𝚿 𝒆𝒊∆ • Useful for highly absorbing substrates
𝒓𝒔 • Currently incompatable with roughness and
inhomogeneity advanced features 23
n k Data from Ellipsometry – Example of Mo film

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Main Interface
Basic Principles Advanced Features User Interface

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Advanced options
Basic Principles Advanced Features User Interface

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 Data Extraction Process
Basic Principles Advanced Features User Interface

• Interactive fitting
process

• Place nodes which

are automatically
connected by a
smooth function

• User selects
physically meaningful
solutions from multiply
degenerate solution
space

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Summary and Outlook

RefDex
•
𝒓
calculates T, R (n,k) for a multilayer stack 𝒑 = 𝐭𝐚𝐧𝚿 𝒆𝒊∆
→ extracts n,k from T, R
𝒓𝒔
• considers surface roughness
Type equation here.
• applies to inhomogeneous layers
• has also basic features for ellipsometry
...
• is freely available from
http://www.helmholtz-berlin.de/forschung/oe/enma/nanooptix/index_en.html

Impulse and Networking Fond: VH-NG-928

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