Quantitative Mueller Matrix Polarimetry With Diverse Applications

Quantitative Mueller Matrix Polarimetry
with diverse applications

Harsh Purwar
(07MS-76)
Department of Physical Sciences,
Indian Institute of Science Education and Research, Kolkata
Email: harshpurwar@hotmail.com
Thesis Supervisor
Dr. Nirmalya Ghosh
April 26, 2012
Harsh Purwar (DPS, IISER-K) Quantitative MM Polarimetry April 26, 2012 1 / 41
Outline
1
Introduction
2
Motivation
3
MM Measurement Methods
4
Our MM Measurement Strategy
5
Experimental Setup
6
Eigenvalue Calibration Method
7
Mueller Matrix Decomposition Scheme
8
Results
9
Initial Applications on Biological Tissues
10
Applications towards nano-plasmonics
11
Conclusions
Introduction
Introduction
What is it?
Several calculi have been developed for analysing polarization, including those based on the
Jones matrix, coherency matrix, Mueller matrix, and other matrices
1
.
Stokes Mueller Formalism:
The Stokes parameters are a set of values that describe the polarization state of the
electromagnetic radiation rst introduced by George G. Stokes in 1852.
S =
_
_
_
_
S
0
S
1
S
2
S
3
_
_
_
_
=
_
_
_
_
I
Q
U
V
_
_
_
_
=
_
_
_
_
I
H
+ I
V
I
H
I
V
I
P
I
M
I
L
I
R
_
_
_
_
Degree of polarization (DOP) is a quantity used to describe the portion of an electromagnetic
wave which is polarized. In Stokes formalism we have,
DOP =
_
S
2
1
+ S
2
2
+ S
2
3
S
0
1
Shurcli, 1962; Gerrard and Burch, 1975; Theocaris and Gdoutos, 1979; Azzam and Bashara, 1987; Coulson,
1988; Egan, 1992.
Introduction
Introduction
Mueller Calculus
Mueller matrix (M) for a polarization-altering device is dened as the matrix which transforms
an incident Stokes vector S into the exiting (reected, transmitted, or scattered) Stokes vector
S
,
S
41
= M
44
S
41
Mueller matrices of some common optical elements with corresponding Stokes vectors:
For an ideal quarter waveplate with its fast axis oriented at an angle of 45
:
_
_
_
_
1 0 0 0
0 0 0 1
0 0 1 0
0 1 0 0
_
_
_
_
_
_
s
0
s
1
s
2
s
3
_
_
=
_
_
_
_
s
0
s
3
s
2
s
1
_
_
For an ideal linear polarizer, transmission axis 0
:
_
_
_
_
1 1 0 0
1 1 0 0
0 0 0 0
0 0 0 0
_
_
_
_
_
_
s
0
s
1
s
2
s
3
_
_
=
_
_
_
_
s
0
+ s
1
s
0
+ s
1
0
0
_
_
Motivation
Motivation
Why are we interested?
MM contains information about all the polarization properties of the sample and
thus has been very useful in the following areas of (but not limiting to) science
and technology.
Material characterization,
Measuring the thickness and refractive indices of thin lms (ellipsometry),
Tissue characterization & dierentiation, monitoring of Glucose levels in
blood, etc.,
Remote sensing of the earth and astronomical bodies,
Applications in Metrology, Astronomy, Ophthalmology, Radar polarimetry
etc.
2
Stokes Mueller calculus is applicable to randomly, fully or partially polarized
light.
2
Handbook of Optics, Chapter 22, R.A. Chipman
Some commonly used approaches...
Several MM measurement methods have been proposed so far. Some of the most
adopted among them are:
1
Modulation-based methods:
Uses electro-optic, magneto-optic or photoelastic modulators to rapidly
change polarization states and a lock-in based detection.
Advantages: Single measurement is sucient to determine complete
MM with very high precession and accuracy.
Major Drawback: Spectral and imaging measurements are not
possible.
2
Direct Measurements, using dual rotating polarizers and retarders.
Advantages: Suits well for imaging and/or spectral measurements.
Major Drawbacks: Measurements are not very accurate and are
prone to huge errors.
Our Measurement Strategy
Heres what we did...!
Dual rotating retarder approach:
Consists of two rotating quarter wave plates and two xed linear polarizers to generate sixteen
elliptically polarized states.
Polarization State Generator (W) comprises of a xed linear polarizer (P
1
) followed by a
rotatable quarter wave plate (Q
1
). It, in general can be used to generate any polarization state.
_
_
_
_
1 0 0 0
0 C
2
1
+ S
2
1
C
1
C
1
(1 C
) S
1
S
0 S
1
C
1
(1 C
) S
2
1
+ C
2
1
C
1
S
0 S
1
S
1
S
_
_
_
_
.
M
Retarder
_
_
_
_
1 1 0 0
1 1 0 0
0 0 0 0
0 0 0 0
_
_
_
_
.
M
Pol
at Horizontal
_
_
_
_
1
0
0
0
_
_
_
_
.
Unpol.
W
1
=
_
1 C
2
1
+ S
2
1
C
1
S
1
(1 C
) S
1
S
_
T
For four dierent input polarizations we have,
W =
_
_
_
_
1 1 1 1
C
2
1
+ S
2
1
C
C
2
2
+ S
2
2
C
C
2
3
+ S
2
3
C
C
2
4
+ S
2
4
C
1
S
1
(1 C
) C
2
S
2
(1 C
) C
3
S
3
(1 C
) C
4
S
4
(1 C
)
S
1
S
2
S
3
S
4
S
_
_
_
_
Our Measurement Strategy
Polarization State Analyser (A) comprises of a rotatable quarter wave plate (Q
2
) followed by a
xed linear polarizer (P
2
) crossed with P
1
. It is dedicated to the measurement of an unknown
Stokes vector.
_
_
_
_
1 1 0 0
1 1 0 0
0 0 0 0
0 0 0 0
_
_
_
_
.
M
Pol
at Vertical
_
_
_
_
1 0 0 0
0 C
2
1
+ S
2
1
C
1
C
1
(1 C
) S
1
S
0 S
1
C
1
(1 C
) S
2
1
+ C
2
1
C
1
S
0 S
1
S
1
S
_
_
_
_
.
M
Retarder
PSA is followed by an intensity based detector, which just records total intensity or the very rst
element/row of the Stokes vector. Hence,
A
1
=
_
1 C
2
1
S
2
1
C
1
C
1
(1 C
) S
1
S
_
Similarly for four dierent angles we have,
A =
_
_
_
_
_
1 C
2
1
S
2
1
C
1
C
1
(1 C
) S
1
S
1 C
2
2
S
2
2
C
2
C
2
(1 C
) S
2
S
1 C
2
3
S
2
3
C
3
C
3
(1 C
) S
3
S
1 C
2
4
S
2
4
C
4
C
4
(1 C
) S
4
S
_
_
_
_
_
Criteria for Stable Mueller Matrix
From A (PSA) and W (PSG) matrices, Mueller matrix of the sample M
s
is calculated as
follows. We know that,
M = A M
s
W
Hence if we dene,
Q
1616
= A
44
W
T
44
= (M
s
)
161
= Q
1
1616
M
161
(M
s
)
161
is then reshaped to a 4 4 matrix. The samples Mueller matrix is then decomposed
using Polar Decomposition scheme to get its basic polarization properties. Choice of orientation
angles of retarders (QWPs) is:
very crucial to get a stable and physically realizable MM.
made by maximizing the determinant of matrix Q.
For simplicity same four angles (35
, 70
, 105
& 140
) were chosen for both the QWPs.

Chosen angles were veried using a more rigorous approach.
Verication of Chosen Angles (
i
s) using SVD
The Singular Value Decomposition of an mn real or complex matrix S is a factorization of the
form,
S = UDV
where U is a m m and V is a n n unitary matrices. D is a m n rectangular diagonal

matrix. The diagonal entries of D are known as singular values of matrix S.
The angles of the polarizers and QWPs should be chosen so that
the corresponding Stokes vectors are distributed evenly inside the
Poincare sphere.
x y
z
1
This is achieved by making sure that the singular values obtained
after SVD of the PSG and PSA matrices are non-zero. We dene
the condition number for PSG and PSA matrices as,
C# =
Min{singular values}
Max{singular values}
Poincare sphere showing Stokes
vectors constituting PSG and
PSA matrices.
Experimental Setup
Experimental Setup
Our hard work!
Setup 1: Schematic of the experimental setup Setup 2: Schematic of the experimental setup
for elastic scattering. for inelastic (uorescence) scattering.
Need for Calibration
How does it help?
The polarizers and QWPs do not behave ideally (i.e. not as a perfect diattenuator
and as a perfect /2 retarder) over the entire spectral range. And hence the PSG
and PSA matrices constructed earlier will change with wavelength.
Eigenvalue Calibration,
provides exact PSG (W) and PSA (A) matrices over the entire spectral
range.
hence automatically corrects for the non-ideal behaviour of the involved
optical elements.
requires at least two extra measurements with samples whose form of the
MM is known.
Eigenvalue Calibration
Mathematical Formulation
Lets choose the two reference samples to be blank (no sample) and a diattenuating retarder and
call these measurements as b
0
and b respectively. Hence,
b
0
= aw, b = amw
= c = b
1
0
b = w
1
mw, c
= bb
1
0
= ama
1
By denition c, m & c
are similar matrices and hence have same eigenvalues. We do not know
m explicitly yet, but it has the following form,
m =
_
_
_
_
1 cos 2 0 0
cos 2 1 0 0
0 0 sin 2 cos sin 2 sin
0 0 sin 2 sin sin 2 cos
_
_
m has four eigenvalues (2 real & 2 imaginary),
R
1
= 2 cos
2
,
R
2
= 2 sin
2
C
1
= sin 2e
i
,
C
2
= sin 2e
i
Eigenvalue Calibration
A little more mathematics!
Hence,
=

R
1
+
R
2
2
, = tan
1
_
R
1
R
2
, = log
_
C
2
C
1
Mueller matrix m for the reference sample (diattenuating retarder) is constructed back from
these eigenvalues.
Now, consider the following two matrix equations,
mX Xc = 0, mX
= 0
with solutions: X = w and X
= a since, c = w
1
mw and c
= ama
1
.
Solving
3
these two linear equations gives us our PSG (w) and PSA (a) matrices.
3
Eric Compain, et. al., Applied Optics, Vol. 38, Issue 16, 1999.
Eigenvalue Calibration Results
PSG Matrix
Figure: Polarization State Generator Matrix (W) as a function of wavelength ().
PSA Matrix
Figure: Polarization State Analyser Matrix (A) as a function of wavelength ().
Condition Number for PSG & PSA Matrices
Figure: Plot of condition number for the PSG and PSA Matrices as a function of wavelength
(). Clearly, condition number > 0.25 .
Error Estimate
Figure: Plot of an estimate of error as a function of wavelength ().
Results
Mueller Matrix (blank)
Figure: Mueller Matrix (M) for blank (no sample) as a function of wavelength ().
Results
Null Elements from the MM for a quarter waveplate
Figure: Null (zero) elements of the Mueller matrix for a quarter waveplate plotted as a
function of wavelength () showing elemental error 0.01.
Mueller Matrix Decomposition Scheme
MM Decomposition
Polar Decomposition
Mueller matrix reects lumped eects hindering their unique interpretation.
Measured MM (4 4) is decomposed into three 4 4 matrices using Polar
decomposition scheme:
M = M
M
R
M
D
,
leading to three basic polarization properties diattenuation (D), retardance (R)
and depolarization ().
Depolarization (): If an incident state is 100% polarized and the exiting state
has a degree of polarization less than unity, then the system is said to be
depolarizing.
Retardance (R) is the phase dierence between the two orthogonal polarizations
of light for both linear and circular polarizations.
Diattenuation (D) is the dierential attenuation of orthogonal polarizations for
both linear and circular polarization states.
Results
Results
Diattenuation (D) for a wide-band linear polarizer
500 520 540 560 580 600 620 640 660 680 700
0.88
0.9
0.92
0.94
0.96
0.98
1
1.02
1.04
1.06
1.08
Wavelength (nm)
D
i
a
t
t
e
n
u
a
t
i
o
n

D
Ideal Value = 1.0
Figure: Polar decomposition derived Diattenuation (D) for a wide-band Glan-Thomson linear
polarizer as a function of wavelength ().
Results
Results
Linear Retardance () for a quarter waveplate
Figure: Polar decomposition derived Linear Retardance () for a 633 nm quarter waveplate
plotted as a function of wavelength (). At = 633 nm, measured = 1.54 rad.
Results
Advantages of Our Measurement Strategy
Independent of source and detector (spectrometer) polarization responses.
Simultaneous spectroscopic and spatial mapping (imaging). Can be
incorporated with microscopic arrangement.
Exact PSG and PSA matrices and their wavelength dependence need not be
known.
Is fully automated. Takes just a few minutes for measurement of complete
spectral (400 800 nm) MM.
Mueller matrix elemental error < 0.01.
Capable of detecting small polarization signal even in presence of large
background depolarization noise.
Applications towards Tissue Characterization
Fluorescence MM Polarimetry
Challenges & Prospects
1
Signicant change in tissue uorescence from normal to malignant stage.
2
Collagen and NADH identied as biomarkers for cancer.
3
Tissue uorescence spectra convolution of spectra of various uorophores.
4
Diagnostic parameters: Spectra, Yield & Decay Kinetics.
5
Only spectral signature can not be used to distinguish between the normal and cancerous
tissues for the following few reasons.
Spectral signatures of these biomolecules vary from patient to patient and also
depend on the region we are probing.
Are hugely inuenced by the absorption of light from absorbers like blood. Hence
not suited for in-vitro examination.
Also the emission and absorption bands of NADH and Collagen overlap to an extent
that it is not practically possible to study them separately.
Fluorescence MM on the other hand can bring out the structural dierences by targeting
specic molecules. The brous structure of collagen gives large diattenuation as opposed
to NADH, which is isotropic.
Hence this can be used as a tool for Cancer Diagnosis.
Preliminary Results
M
11
Element of Fluorescence MM for Human Cervical Cancer Biopsy Slides
Collagen Em. Spectra
NADH Em. Spectra
Figure: M
11
element of uorescence Mueller matrix (un-normalized) measured from the Human
cervical tissue biopsy slides (thickness few m) shown as a function of wavelength ().
Preliminary Results
Fluorescence MM for Human Cervical Cancer Biopsy Slides
Figure: Individual elements of uorescence Mueller matrix measured from the Human cervical
tissue biopsy slides (thickness few m) shown as a function of wavelength ().
Preliminary Results
Diattenuation for Human Cervical Cancer Biopsy Slides
Figure: Diattenuation measured from the Human cervical tissue biopsy slides (thickness few
m) with dierent stages of cancer shown as a function of wavelength ().
Introduction to SPR
Surface Plasmon Resonance
Plasmon resonance: Collective oscillations of free electrons at the metal-dielectric interface in
resonance with the incident electromagnetic (EM) eld.
Can be propagating as on the planar metal-dielectric interfaces as well as localized as on metal
nanoparticles.
Numerous practical applications:
Contrast enhancement in optical imaging.
Ultra-high sensitive chemical and biomedical sensing, bio-molecular manipulation,
labelling, detection.
Surface enhanced spectroscopy (Raman and uorescence).
Development of new optical devices: Plasmonic wave guiding nano-devices, optical
information processing and data storage.
Methodology
The scattering matrices for Ag (silver)
nanoparticles and similar dielectric
particles were generated in its surface
plasmon spectral region
( = 380 600 nm).
Reported values of n and k (real &
imaginary part of refractive index)
were used in the calculation.
Decomposition analysis was performed
on S() (T-matrix computed) for
randomly oriented spheroidal
nano-particles (metal & dielectric) to
study the depolarization behaviour.
Similar decomposition analysis
performed on S() for preferentially
oriented spheroidal nano-particles to
understand the underlying mechanism
of depolarization.
Results
Depolarization for randomly oriented metal nanoparticles
Depolarization characteristics show distinct spectral features with a peak at around
380 410 nm.
Figure: For r = 20 nm and varying .
Results
Longitudinal & Transverse plasmon resonances in spheroids
The magnitude of depolarization peaks around the overlap spectral region of the two
dipolar plasmon bands.
Figure: For r = 20 nm and varying .
Results
Enhanced Retardance and Diattenuation in preferentially oriented metal nanoparticles
Parameters
Estimated values for the polarization parameters
at = 400 nm, = 45
and = 1.5.
Spheroidal metal Spheroidal dielectric Spherical metal
nanoparticle nanoparticle nanoparticle
d 0.435 0.388 0.333
0 0 0
(rad.) 1.99 0 0.011
Magnitude of linear retardance () peaks
around the overlap spectral region of the two
dipolar plasmon bands ().
Stronger diattenuation (D
metal
> D
dielectric
).
No depolarization 0.
For r = 20 nm, = 45
and varying .
Results
Retardance of preferentially oriented metal nanoparticles
Dielectric nanoparticle: Usual behaviour
Phase reversal ( >

2
rad.) in
backscattering > 90
.
(for any value of ) is either close to
zero or .
Metal nanoparticle at 400 nm: Phase reversal or
helicity ipping even in forward scattering angles
( >

2
rad. < 90
)
Additional scattering-induced due the inherent
phase retardation between the two orthogonal
dipolar plasmon polarizabilities.
Longitudinal and the transverse dipolar plasmon
polarizabilities oscillating with a phase dierence.
For r = 20 nm, = 1.5 at specic s.
Prospective Applications & Outlook
Quantitative MM Plasmon Polarimetry: Prospective
applications & Outlook
Quantitative dierences in intrinsic polarization parameters of non-spherical
metal nanoparticles & background tissue (cell) dielectric structures.
Polarization can be used as additional contrast mechanism to discriminate
against background Rayleigh / Mie scattering (with optimal choice of ).
Can be exploited in combination with other spectroscopic approaches
(Fluorescence & Raman).
In-situ monitoring and controlling of size & shape of nanoparticles during
synthesis.
May have implications in bio-sensing exploiting polarization to enhance
sensitivity.
Conclusions
Conclusions
A highly sensitive automated spectral Mueller matrix polarimeter for both
elastic and inelastic scattering (uorescence) has been developed and
calibrated using Eigenvalue Calibration method.
It had initially been used to characterize human cervical cancer tissues.
It had also been used to study the characteristics of some of the uorescent
dyes like Coumarin 102 and Coumarin 152.
Nano-plasmonics
Enhanced depolarization (and its spectral characteristics ()) for randomly
oriented spheroidal metal nanoparticles originates from the presence of
strong linear retardance () eect in the individual oriented nanoparticles.
Enhanced diattenuation d & linear retardance for preferentially oriented
spheroidal metal nanoparticles.
Acknowledgement
Acknowledgement
Dr. Nirmalya Ghosh, IISER-Kolkata.
Prof. Asima Pradhan, IIT-Kanpur.
Dr. Ayan Banerjee, IISER-Kolkata.
Dr. Uday Kumar, IISER-Kolkata.
I am also very thankful to my friends Jalpa Soni, Sayantan Ghosh, Satish Kumar,
Harshit Lakhotia, Shubham Chandel, Nandan K. Das and Subhasri Chatterjee for
numerous healthy discussions and for their constant help, motivation and support
throughout the project.
Publications
Publications
...in last one year!
Included in Thesis
Development and Eigenvalue calibration of an automated spectral Mueller matrix system
for biomedical polarimetry H. Purwar, et. al., Proc. of SPIE, Vol. 8230 No. 823019,
2012. (Full length manuscript is under preparation).
Quantitative polarimetry of plasmon resonant spheroidal metal nanoparticles: A Mueller
matrix decomposition study J. Soni, et. al., Optics Communications, Vol. 285 Issue 6,
2011.
Enhanced polarization anisotropy of metal nano-particles and their spectral
characteristics in the surface plasmon resonance band J. Soni, et. al., Proc. of SPIE,
Vol. 8096 No. 809624, 2011.
Other related Publications
Diering self-similarity in light scattering spectra: A potential tool for pre-cancer
detection S. Ghosh, et. al. Optics Express, Vol. 19 No. 20, 2011. Selected for further
impact by Virtual Journal for Biomedical Optics, Vol. 6 Issue 10, 2011.
A comparative study of dierential matrix and polar decomposition formalisms for
polarimetric characterization of complex turbid media S. Kumar, et. al. to be submitted
to Optics Communications.
Thank you for your time.
Harsh Purwar
07MS-76
Department of Physical Sciences,
Indian Institute of Science Education and Research, Kolkata
Email: harshpurwar@hotmail.com

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) were chosen for both the QWPs.

where U is a m m and V is a n n unitary matrices. D is a m n rectangular diagonal

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