cmic department “giulio natta” soft matter lab

95
Statistical Optics in colloid science Roberto Piazza CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB International School of Physics “Enrico Fermi” Course CLXXXIV

Upload: others

Post on 07-Jun-2022

3 views

Category:

Documents


0 download

TRANSCRIPT

Page 1: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

Statistical Optics in colloid science

Roberto Piazza

CMIC DEPARTMENT “Giulio Natta”

SOFT MATTER LAB

International School of Physics “Enrico Fermi”

Course CLXXXIV

Page 2: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

MOTIVATION: A PARADOX ● Exploting optical methods has always been crucial for the development of soft matter physics. When I was young, scattering played the leading role. Now that I am growing a little bit older it is the turn of advanced microscopy. Yet these two worlds (real and reciprocal space) are intimately related. To appreciate this, a solid background in statistical optics is crucial

● When I was young, there was no way to enter the soft matter community without a good training in optics, allowing you to build instruments. Now that I am not anymore that young, youngsters have little time to study optics, not to say building your own stuff.

THIS IS A SCHOOL: THE RIGHT PLACE AND TIME TO START -  For experimentalists, to really grasp what they are doing -  For theoreticians, to understand how experimentalists can cheat them

Page 3: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

A VERY BASIC COURSE (If you get bored, the lake is just 50 m away )

1) A brief review of Fourier and statistical optics

2) Light Scattering and Intensity Correlation Spectroscopy

3) Statistical optics in imaging and “mixed” techniques

SUMMARY TIME SCHEDULE TEMPO

Page 4: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

1. BASICS OF FOURIER

AND STATISTICAL OPTICS

Page 5: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

A general (scalar) diffraction problem:

Incident plane wave

“Screen” (any obstacle

to propagation)

Amplitude and phase modulated diffracted wave

])(exp[),,(),,( x,y,zizyxUzyxU ϕ=

z

Page 6: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

?

● FUNDAMENTAL: NO PHYSICAL “EMITTER”!

● TECHNICAL: how do we take the relative phases of the “secondary sources”?

HUYGENS’ PRINCIPLE “Each element of the wave front can be regarded as the centre of a secondary disturbance which

gives rise to a spherical wavelet. The position of the wave front at later time is the

envelope (interference) of all such wavelets”

t0 t1

Page 7: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

THE ANGULAR SPECTRUM

● Fourier decomposition along x, y just beyond the screen

⎪⎩

⎪⎨⎧

+=

+−=

∫∫

)](2exp[)0,,()0,,(

)](2exp[)0,,()0,,(

yfxfiffAdfdfyxU

yfxfiyxdxdyUffA

yxyxyx

yxyx

π

π

● Many of the basic aspects of diffraction, and in general of Fourier optics can be easily grasped by selecting a “main” propagation direction (say, z), and expanding the wave front in terms of plane waves propagating with specific components of the wave-vector k along x and y.

Page 8: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

Direction cosines are interrelated! 221 βαγ −−=

PHYSICAL MEANING

)exp(),,()(exp[);,,( tizyxPtiitzyxp ωω −=−⋅= rk● SIMPLE MONOCHROMATIC PLANE WAVE

⎪⎩

⎪⎨⎧

++=

++=

)(2zyx

zyx zyx

uuuk

uuur

γβαλπ

x cos-1 α

cos-1 β

cos-1 γ

y z

k

)ˆexp()](exp[),,( zikyxikzyxP γβ+α=

Introducing director cosines (α,β,γ)

Thus, across the plane z= 0, exp[2πι(fxx+fyy)] may be seen as a plane wave traveling with director cosines α =λfx, β =λfy

Page 9: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

PROPAGATION OF THE ANGULAR SPECTRUM

PROBLEM: find the relation between )0,,( βαA and ),,( zA βα

SOLUTION: U(x,y,z) satisfy the Helmholtz equation: ( ) 0),,(22 =+∇ zyxUk

zikeAzA γβα=βα )0,,(),,(

( ) 0),,(1),,( 2222

2

=−−+∂∂ zAkzAz

βαβαβα

Page 10: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

122 ≤+ βα● For: REAL Simply a change of the relative phases of the components of the angular spectrum (each wave travels different distances between z-planes → phase delay)

PROPAGATING AND EVANESCENT WAVES

γλ ⇒≤+ − )( 222yx ff

122 >+ βα● For: IMAGINARY α and β cannot anymore be interpreted as direction cosines. We have an EVANESCENT wave, with an amplitude decaying as

α

β Propagating waves

Evanescent waves

12 22 −β+απ=γ=µ ikwhere:

● Evanescent waves do not carry energy away from the aperture (like in a waveguide driven below cutoff)

γλ ⇒>+ − )( 222yx ff

)exp( zµ−

Page 11: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

PROPAGATION AS A LINEAR SPATIAL FILTER

)0;,();,();,( yxyxyx ffAzffHzffA =

( )⎩⎨⎧ <+−−

=otherwise0

1)()(if)()(1exp),(2222

YxYxyx

ffffikzffH λλλλ

In terms of spatial frequencies:

where:

is the FREE SPACE TRANSFER FUNCTION

● Propagation can therefore be regarded as a linear dispersive spatial filter with a finite bandwidth. ● Transmission is zero outside a circular region C of radius λ-1 in the frequency plane. ● Within C, | H( fx, fy ) |= 1, but with a frequency-dependent phase shift, which is most significant at high f.

Page 12: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

)ˆ(0 rU

r̂Original disturbance

)(0 ρA

ρFull angular spectrum

)ˆ(0 rU

)ˆ(0 rU

r̂Propagating part Evanescent part

= +

EXAMPLE: FREE-SPACE PROPAGATION (DIFFRACTION) FROM A CIRCULAR APERTURE

)(0 ρA

ρ

)(0 ρA

ρρ < 1 ρ > 1

= +

Page 13: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

FRAUNHOFER DIFFRACTION – A SIMPLE VIEW (NO HF PRINCIPLE)

● Fraunhofer diffraction just concerns the far–field behavior of the radiation emitted by a planar source, hence the directions of the diffracted waves. Basically, it amounts to determining the propagating part of the angular spectrum ● “Principle of inverse interference” (G. Toraldo di Francia)

If we can find a system of plane waves {Wj} in S2 with suitable amplitudes and phases that, coming from S1 and interfering on Σ, would reproduce exactly A(P) and ϕ(P), then these waves yield exactly the angular spectrum of the far–field Fraunhofer diffraction pattern originated by Σ.

Page 14: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

How does it practically work?

• Introduce amplitude density of propagating waves A(α,β). Total contribution of waves propagating in dΩ = dαdβ/(1-α2-β2)1/2:

βαβ−α−

βα γβ+α ddee1

),( i)(i22

zkyxkA

• Amplitude generated by these waves when “back-propagated” to z=0:

∫ βαβ−α−

βα=Σ β+α dde

1),()( )(i22

yxkAv

• Developing the original disturbance a(x,y) in Fourier components and equating the coefficients:

∫+π

λβ−α−

=βα yxyxaA yfxf yx dde),(1),( )(i22

22

Page 15: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

THE POINT SOURCE

● Tiny aperture of size a → a(x,y) = A0. Since ϑ=β−α− cos1 22

ϑλ

=ϑ cos)( 20

aAAThis is the radiation pattern by any aperture, when its size goes to 0: we call it the absolute point source (PS).

● Substituting the real aperture on the screen with a source having this amplitude distribution would not change anything. This source is nothing but the Airy disk produced by a circular aperture, and has an central spot of radius ρ ≈0.61λ. THIS “MINIMAL CENTRIC” IS THE MIN. PHYSICAL SOURCE.

● Radiation pattern from a PS (propagating part): ∫ <βα

β+α βαλ

=1|||,|

)(i20 dde yxkaAA

ρπρ

λ=ρ

)2()( 10

JaAA(some calculation)

Page 16: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

DIFFRACTION (GENERAL) ● STRATEGY: Find the IMPULSE RESPONSE FUNCTION h(x,y,z) (inverse FT of the free-space transfer function), starting from Weyl expansion of a spherical wave in planar components: [ ] βαγ+β+α

γπ= ∫ dd)(iexp12ii

zyxkkre kr

[ ] βαβ+αγ=⎟⎠

⎞⎜⎝

⎛∂∂π

− ∫ dd)(iexp)iexp(e2 i

2 yxkzkrzk

kr

[ ]rerz

krezyxh

ikrzk

⎟⎠⎞

⎜⎝⎛ −λ=ℑ= γ− i1),,( i1

Derive w.r. z

● HUYGENS’ WAVELETS For r >> λ the IRF is a spherical wave:

rzyxh

kri2/i ecose),,( ϑλ≈ π

PHASE SHIFT (QUADRATURE)

r

z ϑ

OBLIQUITY FACTOR

Page 17: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

● RAYLEIGH-SOMMERFELD DIFFRACTION FORMULA Total disturbance in r = convolution of the amplitude beyond the screen with the IRF

yxeUU z

k

ʹ′ʹ′ʹ′−

ʹ′λ

−= ∫ʹ′−

dd),cos()(i)(i

0 uurr

rrrr

Σ P0

z P1

r01

ξ η

x y

APERTURE PLANE (ξ, η)

OBSERVATION PLANE (x, y)

Σ

ϑ

● STANDARD GEOMETRY 222

01 )()( η−+ξ−+= yxzr

∫Σ

Σλ

= drikrPU

izPU 2

01

0110

)exp()()(

● FRESNEL APPROXIMATION

⎪⎩

⎪⎨

⎧⎥⎦

⎤⎢⎣

⎡⎟⎠⎞

⎜⎝⎛ η−

+⎟⎠⎞

⎜⎝⎛ ξ−

+≈

zzy

zxzr

22

01 21

211 in phase

factor in denominator

⎪⎩

⎪⎨

⎥⎦⎤

⎢⎣⎡ +

λ=

η−ξ−ηξηξ= ∫∫)(

2iexp

ie),(

),(),(dd),(

22i

yxzk

zyxh

yxhUyxUkz

Convolution of the amplitude at the aperture with a quadratic IRF

Page 18: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

First-order approximation the exact free-space transfer function for

● TRANSFER FUNCTION IN FRESNEL APPROXIMATION

[ ] ( )[ ]22exp),(),( yxikz

yx ffzieyxhffH +−=ℑ= πλ

FRESNEL REGIME → SMALL ANGLES (PARAXIAL APPROX.)

11, −− λ<<λ<< yx ff

● ACCURACY OF THE FRESNEL APPROXIMATION Main contribution to the convolution integral comes from a square region of size Δξ ~Δη ~ 4(λz)1/2 centered in ξ = x, η = y (Notice that receding from the aperture, this region GROWS!)

In fact, Fresnel approx. is quite good even very close

to the aperture

Page 19: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

FRAUNHOHER DIFFRACTION ● If we are REALLY far from the aperture, so that: we can further approximate the diffraction integral as:

MAXkz )(2

22 η+ξ>>

∫∫ ⎥⎦⎤

⎢⎣⎡ η+ξ

λπ

−ηξηξλ

=+

)(2iexp),(ddi

ee),(2/)(ii 22

yxz

Uz

yxUzyxkkz

WARNING! A very stringent condition! Circular aperture, r =1 cm → z >> 500 m! (but see what follows…)

● Aside from a multiplicative phase factor (which does not affect INTENSITY), the amplitude in the observation plane is simply the FOURIER TRANSFORM of the aperture amplit. distribution

evaluated at frequencies: zyf

zxf yx λλ

== ;

( )yx ffU ,~

● FRESNEL NUMBER

⎩⎨⎧

>>

≤⇒

λ=

112

F

FF N

NzDN

full Fresnel regime (“near field”) Fraunhofer regime (“far field”)

Page 20: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

FRAUNHOFER DIFFRACTION FROM A CIRCULAR APERTURE (radius a )

⎥⎦⎤

⎢⎣⎡

λ=

zakrzakrJ

zArU

zkrkz

/)/(2

iee)( 1

2/ii 2 21

2

/)/(2)( ⎥⎦⎤

⎢⎣⎡

⎟⎠⎞

⎜⎝⎛=

zakrzakrJ

zArIλ

1 - 1 2 3 -2 -3

Normalized Intensity

1

0.5

(2a/λz)r

r = 1.22(λ/a) z

“Airy pattern”

a/2.1 λϑ ≈

Page 21: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

FOURIER OPTICS & IMAGING ● FROM FRESNEL TO FRAUHOFER Aperture illuminated by a spherical wave, converging towards P=(0, 0, z0) on the z axis. ● Writing the spherical wave in paraxial approximation, the field at a

point Q = (ξ, η, 0) is: ⎥⎦

⎤⎢⎣

⎡η+ξ−ηξ≈ηξ )(

2exp),(),( 22

00 z

iktUU

P Q

∫∫+

+

=)(2

00

)(2

0

22

0

),(),(ηξ

λπ

ηξηξλ

yxz

iyx

zki

etUddzi

eyxU

On the plane parallel to the aperture and containing P, we have the Fraunhofer diffraction pattern of the amplitude transmittance. Thus, by turning a plane wave into a converging spherical wave, the Fraunhofer regime is “pulled back” close to the aperture.

THIS IS EXACTLY WHAT A LENS DOES

● Using the Fresnel diffraction formula:

Page 22: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

FOURIER-TRANFORMING PROPERTIES OF A LENS

f

A) Object placed against a lens with finite extent

LENS PUPIL ⎩⎨⎧

=01

),( yxPInside the lens aperture

Otherwise

( )⎥⎦⎤

⎢⎣

⎡+= ∫∫

+

yvxuf

iyxPyxdxdyUfi

evuUvu

fki

f λπ

λ2exp),(),(),(

)(2

22

● If the object is much smaller than the lens aperture, we can neglect the effect of the lens finite size. Thus, apart from a phase factor (which does not affect intensity), the amplitude distribution in the focal plane is the FT, i.e., the Fraunhofer diffraction pattern of the amplitude transmitted by object.

AMPLITUDE ON THE LENS FOCAL PLANE

Page 23: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

f d

B) Object placed in front of the lens

● Propagation over d in Fresnel approximation yields (neglecting pupil):

⎟⎠

⎞⎜⎝

⎛λλλ

=

+⎟⎠

⎞⎜⎝

⎛−

fv

fuU

fvuU

vufd

fk

f ,~i

e),()(1

2i 22

● d = f → EXACT FT between amplitude transmitted by the object and the amplitude in the back focal plane. f f

F.T. pair planes

f

OBJECT

F. T. F.

T.

OBJECT

POINT SOURCE

● Other Fourier-transforming geometries

Two equal lenses separated by their common focal length

An object illuminated by a spherical wave emanating from a point source

The F. T. plane is always the plane

where the source is imaged.

Page 24: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

IMAGING PROPERTIES OF A LENS

● PROBLEM: Under what conditions is the field Ui(x, y) in the image plane a “faithful copy” of the field Uo(x, y) leaving the object?

● Wave propagation is linear → ∫∫= ),(),;,(),( ηξηξηξ oi UvuhddvuU

Response in (x, y) due to a unit-amplitude point source in (ξ, η) (POINT SPREAD FUNCTION)

),;,( ηξvuh

● Restating the problem: Under what conditions: ( )ηξδηξ MvMuMvuh ±±= ,),;,(

⎟⎠⎞

⎜⎝⎛=

Mv

MuU

MvuU ii ,1),( M = magnification

),( ηξoU ),( yxUi

z1 z2

Page 25: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

A) Neglect phase factors (irrelevant for intensity)

B) Assume that z1 and z2 satisfy: (Lens Law in geom. optics)

THE POINT SPREAD FUNCTION Consider a δ -function (point source) in (ξ, η). If we:

fzz111

21

=+

[ ]∫∫ ⎭⎬⎫

⎩⎨⎧

η−+ξ−λπ

−λ

=ηξ 22

2212 )()(2iexp),(dd1),;,( MvMu

zyxyPx

zzvuh

),( ηξ MvMu ==

● The PSF is the Fraunhofer diffraction pattern of the pupil centered on the image coordinate ((aside from a scaling factor 1/λz1)

● The effect of diffraction is then of convolving the ideal image with the diffraction pattern of the lens pupil (for monochomatic illumination)

Page 26: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

PLAYING WITH THE FOURIER TRANSFORM

z1 z2

F fzz111

21

=+

Page 27: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

STOCHASTIC PHENOMENA IN OPTICS

SOURCE Spectrum and temporal fluctuations

Size and spatial fluctuations

“SYSTEM” Random static structure Fluctuation dynamics

PROPAGATION Refractive index fluctuations

DETECTOR Photodetection

statistics

2) STATISTICAL OPTICS

Page 28: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

TEMPORAL COHERENCE

SPECTRUM OF THE SOURCE A PHYSICAL PROBLEM

SPATIAL COHERENCE

EXTENSION OF THE SOURCE

A GEOMETRICAL PROBLEM

(almost always…)

Page 29: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

TEMPORAL COHERENCE (first order)

TEMPORAL FLUCTUATIONS OF THE SIGNAL AMPLITUDE

NON-MONOCHROMATICY

FREQUENCY VIEW TIME VIEW

ω

u(ω)

MICHELSON INTERFEROMETRY

FOURIER-TRASFORM SPECTROSCOPY

POWER SPECTRUM CORRELATION FUNCTION ℑ

t

u(t)

COHERENCE TIME τc FINITE BANDWIDTH Δω ωπ

τΔ

=2

c

Page 30: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

DESCRIPTION OF QUASI-MONOCHROMATIC FIELDS: ● Complex representation of a monochromatic field:

)cos()( 0 φ−ω= tAtuR ( )[ ]φ−ω−= tAt 0iexp)(u

[ ] [ ])()(2

)( 00 ωωδωωδ φφ −++=ℑ − iiR eeAtu

+ω0 -ω0

A / 2

[ ] )()(u 0ωωδφ −=ℑ iAet

+ω0

A

a)  Suppress the negative frequency components b)  Double the strength of the positive frequency components

● Non monochromatic signal with FT Associated analytic signal:

)(tuR [ ] )(~)( ωRR utu =ℑ

∫∞

ω−ωωπ

=0

i)(~d1ˆ)( tR eutu

[ ]

[ ]⎪⎩

⎪⎨

−π=

=

∫∞+

∞− tzzuzt

tutR

R

)(d1)(Im

)()(Re

u

u

(no more info!)

-

Page 31: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

NARROWBAND SIGNALS: COMPLEX ENVELOPE

● Real signal having a narrow spectrum centered around ω0 and of width Δω << ω0:

[ ])(cos)()( 0 tttUtuR φω −=

Slowly-varying envelope and phase ⎭

⎬⎫)()(ttU

φ

t

uR( t )

ω + ω0 - ω0

Δω ● Associated analytic signal:

tt eetUt 0i)(i)()( ω−φ=u

tiett 0)()( ω−= Uu

)()()( tietUt φ=UComplex envelope

ω + ω0

Page 32: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

TEMPORAL PROPERTIES OF LIGHT SOURCES A) NARROW BAND THERMAL SOURCE (e.g. a spectral lamp, or even, to a good approximation, a

multimode laser) Many microscopic independent emitters, such as a collection of thermally excited atoms. Each atom emits at a single frequency ω0, but collisions induce abrupt phase jumps.

t

● Total signal amplitude (complex envelope) for N identical emitters:

∑∑ =====

N

i

tiN

i iti

NiUetetUt

1

)(

1

)( )()()( φφ UU

A N-step random walk in the complex plane. For large N, r = Re(U) = U cos(φ) and i = Im(U)= U sin(φ) have a joint Gaussian statistics:

i

r

UN

⎟⎟⎠

⎞⎜⎜⎝

⎛ += 2

22

2 2exp

21),(

σπσirirp UN=σwith

Page 33: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

● Prob. density for U is a Rayleigh distribution

⎪⎩

⎪⎨

⎧≥

⎟⎟

⎜⎜

⎛−

=

otherwise0

022

2exp2)(

UUUUpU σσ

0

0.2

0.4

0.6

0.8

1.0

0 1 2 3 4 5U / σ

p U(U

)

● STATISTICS OF THE INTENSITY

)0(2

exp21)( 22 >⎟

⎠⎞

⎜⎝⎛−= IIIpI σσ

0

0.2

0.4

0.6

0.8

1.0

0 1 2 3 4 5I / <I>

p( I

))0(exp1)( >⎟⎟

⎞⎜⎜⎝

⎛−= III

IIpI

22σ=I

Page 34: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

TIME VIEW ● MAIN MESSAGE: To a finite signal bandwidth unavoidably correspond TEMPORAL FLUCTUATIONS of the signal

● Time autocorrelation function of the analytic signal:

ttt )()(*)( ττ +=Γ uu

● Normalizing Γ to its zero-time value Itt==Γ 2)()0( u

Ittg )()(*

)0()()(1

τττ

+=

ΓΓ

=uu

“FIELD TIME-CORRELATION FUNCTION

● The envelope of an optical signal with bandwidth Δω does not appreciably change on a time scale τ << τc = 2π / Δω.   τc plays than the role of the COHERENCE TIME of the optical signal.  

tiett 0)()( ω−= Uu

Page 35: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

CORRELATION AND SPECTRUM ● Power spectrum. uR( t ) cannot usually be F. T, but still has a finite average power, so we can define

TuPRT

TRu

)(~lim)( ωω ∞→=

SPECTRAL DENSITY (or POWER SPECTRUM)

● THE FUNDAMENTAL LINK: WIENER-KINTCHINE THEOREM

Defining a normalized power spectrum of the real signal as:

⎪⎪⎩

⎪⎪⎨

⎧>

= ∫∞

otherwise0

0)(

)(

)(0

ωωω

ω

ω Ru

Ru

Pd

P

P

[ ][ ]⎩

⎨⎧

ℑ=

ℑ=− )()(

)()(1

1

1

ωτ

τω

Pg

gP

Page 36: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

COLLISION-BROADENED THERMAL SOURCE

● Each emitter is independent, so we have:

Therefore: )()0()()0()()0()( *

1

** tNttt iiN

i iiNN uuuuUU ===Γ ∑ =

jitji ≠= 0)()0(* uu

The total correlation function coincides therefore with the correlation function for a single emitter: [ ])0()()(

110)()( φφω −−=≡ titii eetgtg

● The phases φ(0) and φ(t) will be correlated only if the atom does not undergo collisions in t. The phase correlation function will then be proportional to the probability p(t’ > t) of colliding at any t’ > t.

( )τω /exp)( 01 ttitg −−=Time-correlation function for a collision-broadened thermal source

● POWER SPECTRUM. Fourier-trasforming g1( t ):

( )220 /1)(11)(

τωωπτω

+−=P (Lorentzian lineshape)

Page 37: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

TEMPORAL COHERENCE AND INTERFEROMETRY

D

M1

BS

M2

CP

L1

L2

S

Δl ● Qualitatively, the two beams can interfere only if the difference between the optical paths Δl = l2-l1 is smaller than the coherence length of the source lc.

● Quantitatively, the detected intensity is proportional to the real part of the time correlation function, evaluated at the delay

[ ]( ) clgII /)(Re1 10 Δττ =+=

cl /Δτ =

[ ]CeII τττω /00 )cos(1 −+=

● THERMAL SOURCE

0

0.5

1.0

1.5

2.0

0 1 2 3

τ / τc

I / I 0

ce ττ /−FRINGE

VISIBILITY

Page 38: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

SPATIAL COHERENCE: LASER SPECKLES

DIFFUSER e.g.: “magic” Scotch tape

● When a diffuser is illuminated by a laser, a highly “maculated” pattern forms on the screen

(“SPECKLE PATTERN”)

● If we put a lens and enlarge the laser beam, the speckles become smaller.

F ● Conversely, if we move the diffuser towards the lens focus, the speckle pattern becomes much coarser. (a great way to find the real lens focus)

F Why the speckles?

Why their size depends on the beam spot on the diffuser?

Page 39: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

SPATIAL COHERENCE: YOUNG’S INTERFEROMETER

● POINT SOURCE (quasi-monochomatic)

d P

α ∼ λ/a

Fringes with a spatial period: dx /λ=Δ

Form in the overlap region of the diffraction patterns generated by the two pinholes of radius a.

D d

z

Rd

≈ϑ

● EXTENDED SOURCE made of independent point emitters

λϑ <<≈zDdD

Fringes form only when:

Page 40: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

● If P1 and P2 are very close (so that u1 ≈ u2, v1 ≈ v2 ), the fields

⎩⎨⎧

+=

+=

222

111

)()(

vuUvuU

PP

will be strongly correlated, even if the fields u and v are fully uncorrelated . That is, propagation INDUCES spatial correlations .

P1 P2 U

V

u1 u2 v1

v2

PROPAGATION AND SPATIAL CORRELATIONS

● However, if P2 is moved apart from P1, the phases of the fields coming from U and V change differently:

⎪⎩

⎪⎨

−≈−ʹ′=Δ

+≈−ʹ′=Δ

zdDrrr

zdDrrr

vvv

uuu

If we want: Dzdrr vu /λλ <<⇒<<Δ−Δ

P1

P2 V

U

ru’ rv rv’

d z D ru

Page 41: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

2/ zD=Ωʹ′Δ D

Conversely, the solid angle under which the source is seen is:

'

2

ΔΩ≈λ

cAΔΩ’

z

To the source is then associated a “coherence cone” with solid angle at vertex: which corresponds to an angular aperture: , just like a diffraction pattern!

2)/( Dλ≈ΔΩD/2 λα ≈

EXAMPLES ● Thermal source: D = 1mm, λ =0.5 µm, R = 1m → Ac ≈ 0.25 mm2

● SUN: Ang. diam. 2α ≈ 32’→ ΔΩ’ ≈ 7x10-5 sr → Ac ≈ 0.004 mm2

● STAR (Betelgeuse): 2α ≈ 0.047’’→ ΔΩ’ ≈ 4x10-14 sr → Ac ≈ 6 m2

(TWINKLE TWINKLE LITTLE STAR…)

● Hence, the pinholes must lie within a

2

22

DzAcλ

≈COHERENCE AREA D ΔΩ α

Ac

Page 42: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

SMALL PINHOLES SPACING

S1

S2

● S1 and S2 form two displaced sets of fringes ● However, since fringe oscillation is coarse (low frequency), the shift is a small fraction of the period and the sum of the two interferograms still shows fringes

LARGE PINHOLES SPACING

S1

S2

● Fringe oscillation is rapid. ● Therefore, the two sets are in counter-phase and the two interferograms cancel out.

Page 43: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

⎟⎠⎞

⎜⎝⎛ −+⎟

⎠⎞

⎜⎝⎛ −=

crtPK

crtPKtQ 2

221

11 ,,),( uuu

COMPLEX DEGREE OF COHERENCE ● The field at a point Q on the screen is the superposition of the diffraction pattern from the two pinholes. For a narrowband source, this is simply related to fields on the pinholes at earlier times:

● INTENSITY: ⎥⎦

⎤⎢⎣

⎡⎟⎠⎞

⎜⎝⎛ −

Γ++=crrKKQIQIQI 12

1221)2()1( Re2)()()(

),(),(*)( 2112 ττ +=Γ tPtP uu

MUTUAL COHERENCE FUNCTION

Γ12(τ) is like Γ(τ), but evaluated at two different point in space, so it is a space-time correlation function that, in terms of the positions of P1 and P2, can be written: ),(),(*);,( 2121 ττ +=Γ tt rururr

Page 44: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

● To separate out effects purely due to spatial coherence, let us consider a quasi-monochomatic source, such that all delays are Then, we can write with:

cτ<<ωττ ieJ −=Γ 1212 )(

),(),(*),(),(* 212112 tttPtPJ rUrUuu ==

( ) ( )21

12

PIPIJ

=µ DEGREE OF SPATIAL COHERENCE

Normalized:

MUTUAL INTENSITY

P1

P2

Q1

Q2

Σ

SOURCE

( )∫∫ Σ

−−

ΣΣΣ=

21

21)(2121221

)cos()cos(,1),( 21

rrePPJddQQJ rrik ϑϑ

λ

PROPAGATION OF THE MUTUAL INTENSITY

Using Fresnel diffraction for both fields, one finds:

This looks rather terrific, but…

Page 45: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

THE VAN CITTERT-ZERNIKE THEOREM ● Suppose that the source S is fully spatially incoherent, so that:

)()(),( 211021 PPPCIPPJ −= δ

( )∫Σ−− Σ= d

rrePICQQJ rrik

21

21)(1221

)cos()cos(),( 21 ϑϑλ

● In paraxial approximation:

( ) ( )∫Σ−

⎥⎦⎤

⎢⎣⎡ Δ+Δ= yxz

iIddz

CeQQJi

ηξλπ

ηξηξλ

ψ 2exp,)(

),( 0221

Σ

η

ξ

y

x P

Q1 Q2

● Therefore, apart from a scaling and phase factor: The mutual intensity is the Fourier transform of the intensity distribution across the source

(van Cittert-Zernike theorem)

Page 46: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

● The VCZ theorem may “resemble” the expression for Fraunhofer diffraction, but this is just a formal analogy. Indeed:

a)  The physical quantities are totally different (mutual intensity as FT

of the source intensity, rather than field on a screen as FT of the field at the source)

b) The range of validity is very different! The VCZ theorem is solely based on the paraxial approximation, and holds true also in the Fresnel regime!

∫∫ΔΔ

==ΔΔ−

ηξηξ

λλ

ηξηξµ

ψ

ddI

zyzxIe

ddIC

QQJyxi

),(

)/,/(~

),(

),(),( 21

● From the VCZ theorem, the spatial degree of coherence is then :

Page 47: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

● From the VCZ theorem:

2

2

22

2

),(

)()(),(~

)(),(

)()()/,/(~

∫∫

∫∫

=ΔΔΔΔ

=

dxdyyxI

fdfdffIz

dxdyyxI

ydxdzyzxIA

yxyx

c λλλ

COHERENCE AREA

( )∫∞+

∞−ΔΔΔΔ= )()(,ˆ 2 ydxdyxAc µ● We shall formally define:

but from the properties of the FT (Parseval’s theorem):

∫∫ =⇒= dxdyyxIfdfdffIyxIffI yxyxyx22),()()(),(~),(),(~

2

22

2

2

2 )(

),(

),()(

II

Az

dxdyyxI

dxdyyxIzA

Sc

λλ ==

∫∫ Where AS is the

area of the source

Page 48: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

EXAMPLE: UNIFORMLY BRIGHT SOURCE

AS

● If we have an incoherent source (or illuminated aperture) of area AS with uniform intensity I0:

20

22 III == ( )S

c AzA2λ

=

which will therefore correspond to the typical speckle size at distance z, consistently with what we qualitatively found previously.

But…Does a fully incoherent source REALLY exist? A fully incoherent wave field would have an infinitesimally fine spatial structure. Therefore its angular spectrum would consist only of evanescent waves, and cannot propagate! Then, there must be correlation at least on the scale of λ. Writing: is than a limiting approximation, valid for an optical system that cannot resolve structures finer than λ

)(),( 2121 PPPPJ −∝δ

Page 49: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

THE SPECKLE FIELD ● The field at each point P on the screen is a random sum of contributions from each point of the source, so has a Gaussian statistics for the field components (similarly to a chaotic source).

● Around P there is a correlated region of average size AC and random shape.

● The INTENSITY statistics of the speckles is exponential, that is “most speckles are dark”.

0

0.2

0.4

0.6

0.8

1.0

0 1 2 3 4 5I / <I>

p( I

)

● The “granular” speckle pattern depends only on the geometry of the source.

NOT ALWAYS TRUE, AS WE WILL SEE!

Page 50: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

● We define the (normalized) intensity correlation function (or “degree of second order temporal coherence”) as:

222)()(*

)()()(*)(*

)(

)()()(

t

t

t

t

tttttt

tItItI

guu

uuuu ττττ

++=

+=

PROPERTIES

[ ]

[ ]

[ ]1)(0)0()(0)

1)0(1)0()

*)()()()()

122

12

2

2

1122

≤≤≤≤

=≥=

=−=−

ττ

ττττ

gggiii

gI

Igii

ggggi

For a monochromatic source, obviously: 1)(2 ≡τg

INTENSITY CORRELATION (Second order temporal coherence)

Page 51: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

CHAOTIC SOURCE

● However, due to the independence of the emitters, a given term averages to zero, unless the containing only products of a field times its complex conjugate relative to the same emitter.

∑ =++=+

N

jijiji tttttItI

1,)()()(*)(*)()( uuuu τττ

● We should evaluate the double sum:

+++=+ ∑iiiii tttttItI )()()(*)(*)()( uuuu τττ

[ ]∑≠++++++

jijjiijjii tttttttt )()(*)()(*)()(*)()(* uuuuuuuu ττττ

● Since all emitters are identical:

[ ]22 )()(*)()(*)1(

)()()(*)(*)()(

τ

τττ

++−+

+++=+

ttttNN

ttttNtItI

iiii

iiii

uuuu

uuuu

Where we split the averages because of independence

Page 52: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

● For large N, the first term can be neglected, and N(N - 1) ≈ N2 :

[ ]222 )()(*)()(*)()( ττ ++=+ ttttNtItI iiii uuuu

222 )()(*)( ttNtI ii uu=

212 )(1)( ττ gg += SIEGERT RELATION

● For a collision-broadened thermal source:

● Therefore, for a chaotic source, g2(τ ) does not yield any additional information, and can be directly obtained from |g1(τ )|

( )cg τττ /||2exp1)(2 −+=

● More generally, defining a second order complex degree of coherence:

tt

t

PIPItPItPI)()(),(),(

)(21

21)2(12

ττγ

+=

2211221

)2(12 );,(1);,( τγτγ rrrr +=then, for a chaotic source:

Page 53: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

2. LIGHT SCATTERING AND INTENSITY CORRELATION

SPECTROSCOPY

Page 54: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

LIGHT SCATTERING BASICS Scattered radiation - wave-vector ks - frequency ωs - detected along V/H axis by setting analyzer A

Scattering plane defined by (ki, ks)

Incident radiation - wave-vector ki - frequency ωi - polarized along V/H axis by setting polarizer P

SCATTERING WAVE-VECTOR q For quasi-elastic scattering (ωi ≈ ωs) 2

sin42

sin2||0

ϑλπ

==nkq q

0

2||||λπ

===nkis kk

Page 55: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

MOLECULAR SCATTERING (Rayleigh) ● Single molecule (or particle with size a <<λ) Scattered field Es can depend only on: -  incident field E0 -  particle polarizability α (prop. to particle volume V) -  particle and surrounding medium refractive indices np, ns -  distance from detector (in far-field must decrease as R-1)

ip

sip

s Inn

fRVIE

nn

fRVE ⎟

⎞⎜⎝

⎛λ

∝⇒⎟⎠

⎞⎜⎝

⎛λ

∝ 242

2

2

~ a6 Dimensional analysis

● Full electromagnetic treatment - Incident plane wave Ei=E0eik.rni -  Induced dipole P =aEi Radiation zone

R>>λ

Diff. scattering cross-section

4

2

20

2

dd

λα

ε

⋅π=

Ωfiσ nn

Page 56: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

NO FLUCTUATIONS NO SCATTERING ● Perfectly uniform medium (no refractive index fluctuations)

For each volume element v… …There is always a v’ that scatters with the same amplitude and Δφ=π/2

● Ideal gas: Poisson fluctuations Here (and only here) Is prop. to N

Attractive interactions ↓

Stronger fluctuations ↓

more scattering

Repulsive interactions ↓

weaker fluctuations ↓

less scattering

Page 57: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

SCATTERING FROM A FLUCTUATING MEDIUM

● Generic medium with a fluctuating dielectric tensor : )()( ,t,t rδεIrε +ε=

tifif

ssif tt

RIkI ω

∞+

∞−

δεδεεπ

−=ω ∫ i*20

230

2e),()0,(d

32),( qqqSpectral density:

220

230

2)(

32)( qq if

ssif R

IkI δεεπ

−=Total scatt. intensity: Probe of mean-square fluctuations at q

[ ] t

ji

tifif

sif

ijttII ω−⋅∞+

∞−∑∫ αα=ω i

,

)0()(i*0 ee)()0(d),( rrqq

( )[ ]∑ −⋅α=ji

ijifsif II

,

20 iexp||)( rrqq

● DISCRETE MOLECULAR POSITIONS ⎟⎠⎞

⎜⎝⎛ −δ=ρ ∑1

)()( i,t rrr

),()(),( 20 ωα⋅=ω qnnq SII fi

sif

)()()( 20 qnnq SII fi

sif α⋅=scalar α

Page 58: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

PARTICLE SCATTERING

SCATTERING AMPLITUDE S(θ,φ) (Vertical incid. polariz/Vertical detection)

),(ie),(

ie),(),(

)(i

0

)(i

tzEkr

SEkr

StrE i

zrktkr

s

−ω−

ϕϑ=ϕϑ=

)(i0e),( tkz

i EtzE ω−=θ

φ

● S is in general a complex quantity: ),(e),(),( ϕϑαϕϑ=ϕϑ iFS

Scattered intensity: 022

2 ),(),;( Irk

FrI ϕϑ=ϕϑ

● Scattering cross section σs(by equating total scattered power to

the incident power falling a surface area): ∫ Ωϕϑ= d),(1σ 22s Fk

● In general, the particle may scatter and absorb, with an absorption

cross-sect ion σa → EXTINCTION cross-section: σext = σs + σa

Page 59: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

THE OPTICAL THEOREM ● Whatever the illuminating source, the scattering pattern from the particles contains a faithful reproduction of the incident field that spatially overlaps with the transmitted radiation, but with a different phase ● It is the interference between this “copy” of the incident field and the transmitted beam that yields both the power reduction of the transmitted field and its phase delay in traversing the medium.

INCIDENT PLANE WAVE

z=0

In the forward direction, all contributions add in phase

SUM FIELDS, NOT INTENSITIES! ∑= i iSS )0()0(

[ ])0(Re42 Skext

πρσ −=

[ ]

[ ]⎪⎩

⎪⎨

−=

+=

)0(Re2'

)0(Im21

2

2

Sk

n

Sk

n

πρ

πρ REFRACTION

ABSORPTION

Complex refr. index 'i~ nnn +=

Extinction cross section

Page 60: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

LORENZ - MIE SCATTERING ● Scattering from a spherical particle (exact)

[ ]∑∞

=

+++

=1

)(cos)(cos)1(12

nnnnnVV ba

nnnE ϑτϑπ

● Expansion coefficients very complicated! (combination of Riccati-Bessel functions) However…

⎪⎩

⎪⎨

=

=

ϑϑ

ϑτ

ϑϑ

ϑπ

d)(cosd)(cos

sin)(cos)(cos

)1(

)1(

nn

nn

P

P● Angular functions

By increasing n, the angular pattern becomes “richer”

Page 61: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

● Mode amplitude depends only on x =ka, m=np/n, and decreases fast with x. Hence, for small particles, we need only the lowest order terms.

)()1(45

)(21

94

)2()1)(2(

52i

21

32i

7521

76

2

2

25

22

223

2

2

1

xOxmib

xOxmmx

mmmx

mma

+−−=

+⎟⎠

⎞⎜⎝

⎛+−

++

−−−

+−

−=

Dipole First real term

● By increasing a/λ, more and more mode superimpose. the contributions from different modes tend to cancel each other, except in the forward direction, where all of them present a maximum with the same sign, and, to a lesser extent, in the backward direction, where signs from successive modes alternate.

● In the limit of a very large particle, we would expect the extinction cross section to coincide with the are of the beam geometrically intercepted by the particle, hence that Q = σext/πa2 →1. Instead one finds Q = σext/πa2 →1. This “paradox” comes from the fact that half of the scattering is contained in a strongly peaked diffraction cone (ovlp. with transmitted!)

Page 62: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

Special scattering regimes ● Rayleigh-Gans-Debye (RGD a) x(m-1) = ka(np/n -1)<< 1 → The phase shift of the field in passing

+ through the particle is negligible b) m ≈ 1 → No reflections or refractions

Each volume element of the particle “sees” the external field

Simply integrate over volume elements field (a “collection” of Rayleigh scatterers)

23i

22

42

0

de1)(

)()(4

)(

∫ ⋅=

−=

V

p

rV

kP

kPnnrkVIqI

rq

π

FORM FACTOR

Homogeneous sphere

A curious story with the Optical Theorem (read!)

Page 63: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

● Anomalous Diffraction (AD) “Tenuous” particles (common situation in microscopy of biological objects) Take into account phase changes, but: m ≈ 1 → No reflections or refractions a >> l → almost ray-tracing

For a large particle, in general: SCATTERING = DIFFRACTION + REFRACTIONS/REFLECTIONS But for low optical contrast, this regime is reached very slowly

)1(2

)cos1(2sin212 2

−=

⎥⎦

⎤⎢⎣

⎡ −+−=

mkapp

pppQ

Normalized extinction (exact):

Page 64: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

Dynamic Light Scattering (DLS)

Quasi-Elastic Light Scattering (QELS)

Laser Light Scattering (LLS)

Photon Correlation Spectroscopy (PCS)

Self-Beating Spectroscopy (SBS)

Bosons are particles that differ from fermions because they behave differently

Corriere della Sera, 3/7/2012

Intensity Correlation Spectroscopy (ICS)

How physicists (re)discover the radio!

Page 65: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

ICS vs. INTERFEROMETRY (OR STANDARD SPECTROSCOPY)

Note: a quadratic detector does not measure the instantaneous intensity, but rather its time-average over many optical cicles!

)()()( * tEtEtI = (actually an irradiance)

Page 66: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

The scattering volume: another “chaotic” source:

● Total scattered field: ∑ =

⋅=M

jv

sjAE

1)(iti ee rqω Again a sum of

random phasors!

V

vj

● Split V into M>>1 small volumes, which have anyway a large size compared to sample spatial correlation

-  Es has a gaussian distribution -  The intensity has an exponential distribution (speckle field) BEWARE!

a)  The scattered field is gaussian only provided it is fully fluctuating (does not work for non-ergodic samples)

b)  If the number of particles N in each sub-volume is small, the Siegert relation must be corrected for number fluctuations:

22

12)()0(

)(1)(N

tNNtgg

δδτ ++=

Page 67: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

g1(t) → Physics of Brownian motion

● Langevin equation: )(1dd t

mtRvv

+−= γ

● Velocity autocorrelation and particle displacement: ( )⎪

⎪⎨

−−=

=

t

tB

DDttRmTkt

γ

γ

γe166)(

e3)()0(

2

vv

ttD d)()0(31

0∫∞

= vv● Self-diffusion coefficient:

● Intermediate scattering function (time- FT of dynamic structure factor):

[ ]2||i

21-i ee),(

R(0)R(t)R(0)R(t)q −−⋅ ==q

s tqF

(this is not trivial, and requires the process to be gaussian!)

● Correlation functions: ⎩⎨⎧

−=

=Γ−

−Γ−

t

tt

gg

22

i1

e1)(ee)(

τ

τ ω 2Dq=Γ

Decay rate

Page 68: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

TIME FOR NUMBERS DLS measurement on: -  Small surfactant micelles (radius a ≈2 nm → D ≈ 1.1x10-10 m2/s ) -  Using a blu laser (λ = 488 nm), at max q = 3.4x107 nm-1

Δω = Dq2 ≈ 130 kHz LUDICROUSLY SMALL! No conventional spectroscopic measurement can resolve such a small broadening, because it is much smaller than the source bandwidth (even for a well-stabilized single-mode laser, it is very hard to reduce the bandwidth to less than 1MHz)!

●THE SOLUTION: Forget usual spectroscopic or interferometric methods, which are related to the field correlation function, and look for intensity correlation, the ultimate spectroscopy (no lower brodening limit!)

Page 69: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

THE MAGIC OF ICS: TIME VIEW

( ) )(),()(e)(),( 00)(i tEtqBtEqbtqE

i

tis

i ==∑ ⋅rq

Fluctuations in the incident field E0(t) and Brownian fluctuation embodied in B(q,t) are statistically independent. Hence, the full correlation function factorizes as: ),(),(),( 111 tqgtqgtqg sourcesample=

0),(0),( 11BcB tt

source tqgtqgτττ <<<<>>

→⇒→ BAD NEWS! But:

● FIELD CORRELATION SPECTROSCOPY (INTERFEROMETRY)

● Scattered field:

0

0.2

0.4

0.6

0.8

1.0

0.001 0.01 0.1 1τ

g 1(τ)

CHAOTIC SOURCE & SAMPLE

samplec

sourcec ττ 1.0=

)(1 τg

)()(1 τSg

)()( 1)(

1 ττ gg SC.F. “dies out” before g1(τ ) starts decaying

Page 70: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

● INTENSITY CORRELATION SPECTROSCOPY

DECAYS TO 1! )(2 tg source ),(),( 22 tqgtqg sample

t Bc ττ <<<<→

1

2

3

4

0.001 0.01 0.1 1!

g 2(!)

samplec

sourcec ττ 01.0=

This is exactly what we are looking for! After a short time, we can forget about the source and we see only sample correlations!

Ideal monochromatic sources would be a DISASTER for DLS!

Page 71: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

FREQUENCY VIEW (or, how physicists re-discovered the radio)

Crystal radio (no battery!)

Antenna (HF input)

Headset (Audio output)

Tunable resonant filter

Rectifier

QUADRATIC DETECTOR

Cat-whisker Impurity

Galena crystal (lead sulfide)

Page 72: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

AMPLITUDE MODULATION (not Marconi, but Fessenden!) [ ] ttmfAtv cωcos)(1)( +=

tmAtmtAtv mmcm ωωωω cos)(2cos2cos1[)( 222 +±++=

2ωc ωm

QUADRATIC DETECTION

cm

mttfωω

ω

<<

= cos)(

[ ]ttmAtAtv mcmcc )cos()cos(2

cos)( ωωωωω −+++=

ωc

Low-pass filter

tmAtv mfilt ωcos)( 22 =

DLS: )()()( tvtftv c= (carrier-suppressed AM)

Page 73: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

DLS AND SPATIAL COHERENCE ● Illumination: What matters is only the power the source emits in a single coherence area → A single transversal mode laser (a practical need)

● Detection: No more than one speckle (more just lowers the contrast)

D

● First (and rather dull) way: two pinholes

● Later (more clever): imaging by a stopped-down lens on a controllable slit GIVE SPECKLES THE SIZE YOU LIKE!

(and select the scattering volume) D

● Today: monomode fiber TOTALLY DIFFERENT (ask Jaro Rička)

D

Page 74: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

Again about radios: Heterodyne detection and Doppler Velocimetry

Signal

Local Oscillator at ωc

● Superheterodyne detection (E. Amstrong) Mix the incoming AM signal with a LOCAL OSCILLATOR at the carrier frequency ωc

{ } tAAttAAtvtvtV mLmmLLO ωωω cosR.F.atsignalscos)cos1()()()( 2 +=+==

Again the modulating audio signal, but amplified by vLO!

● Similar trick in DLS, by mixing the scattered light with a tiny fraction of the incident beam (|ELO|2 >> |Es|2) We get the real part of g1(t), not its modulus square!

[ ])(Re1)( 12 tgCtg h +=

)exp()cos(1)()exp()iexp(),( 22

21 tDqtCtgtDqttqg h −⋅+=⇒−⋅= VqVq● Particles in a moving fluid:

WE DETECT ABSOLUTE MOTION (impossible with homodyne)!

Page 75: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

ϕ

z

d SPECKLE SIZE generated by d: ξ

λλξλ

== zz

zd

So the speckle size coincides with the CORRELATION LENGTH! (and we obtain the PHYSICS of the source)

NEAR FIELD

EFFECTIVE SOURCE SIZE: ξλzd =

“STRUCTURED” SOURCES: NEAR FIELD SPECKLES

ξλ

ϕ ≈ξ D

(M. Giglio, 2000)

● A source with correlations extending for ξ

COHERENCE AREA DIFFRACTION PATTERN

FAR FIELD

(just geometry…)

ϕλ

ϑ <<≈D

Page 76: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

● PUZZLE: This seems to violate the VCZ theorem (saying that the speckle size should vanish for z → 0). Where is the catch?

IN THE ASSUMPTION OF A FULLY INCOHERENT SOURCE!

● Generalized VCZ theorem for sources with finite spatial coherence (R. Cerbino, 2007)

“Deep Fresnel region” (DFR) ⎟⎟

⎞⎜⎜⎝

⎛=<<=<< !

2

λλξ DzDzz Fc

“Usual” Fresnel region

-  In the DFR (z<<zc) :

-  z>>zc → Usual VCZ

[ ]),(.F.T),(),( 2211*

yx qqIyxEyxEJ ==Σ

Far-field scattering pattern from the source

Page 77: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

Mutual Intensity does not change

in the DFR

(Cerbino R., Vailati A., 2009)

Page 78: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

FOURIER PLANE

CCD

IMAGE PLANE

BEAM STOP

● Sensitive to misalignment (hard to suppress incident beam) ● Suffers from stray-light

SMALL-ANGLE LIGHT SCATTERING (“TRADITIONAL”)

SPECKLE FIELD

CCD

MAGNIFIED SPECKES

OBJECTIVE

NEAR-FIELD SCATTERING

● Optically simple ● FREE from stray light (heterodyning) ● Unfortunately, does not work for fully non-ergodic systems

Page 79: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

IMAGE DIFFERENCE → SPECKLE FIELD SOURCE CORRELATIONS

SCATTERED INTENSITY STRUCTURE (OR FORM) FACTOR

Page 80: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

3. A FEW WORDS

ABOUT IMAGING

At this point…

Page 81: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

Photon Correlation Imaging (PCI) (L. Cipelletti, 2009)

Imaging through a stopped-down lens

“Speckled” image of the beam

FT plane

z1 z2

f

All regions correspond to the same q (nothing to do with FT of image plane)

Page 82: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

Front f.p.

Back f.p.

Image plane

1st F.T.

2nd F.T.

AN APPARENTLY STUPID QUESTION: Why do we see (large) non absorbing particles under the microscope?

A phase object

A phase object

(with border)

● If a 3D sphere can be shown to be equivalent to a 2D disk with a suitable refractive index profile, no chance! ● In the anomalous diffraction approximation, rigorously true (so, we just see cell borders)

Page 83: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

The microscope: a paradise of Fourier optics

“SOURCE” PLANES

“OBJECT” PLANES

F. T. PAIRS

Page 84: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

RESOLVING POWER ● INCOHERENT IMAGING: RAYLEIGH CRITERION We shall say that two incoherent point sources, imaged by a lens with pupil w, are “barely resolved” if the center of the Airy pattern of one point coincides with the first minimum of the second.

≈0.73

1

Minimum resolvable separation: wziλ

δ 61.0≈

● EXAMPLE: astronomical telescope Sources are always mutually incoherent and, since they are at ∞, the are imaged on the focal plane. Than, is the angular separation of the stars and

f/δϑ =

ϑ 61.0min ≈

ϑ

zi = f

2w

∞ δ

Page 85: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

● COHERENT IMAGING The result depends on relative phase of the two point sources. Indeed, we can write (in normalized image coordinates):

[ ] [ ]211

)61.0()61.0(2

)61.0()61.0(2)(

++

+−−

=xxJe

xxJxI i

ππ

ππ ϕ

b) Sources in quadrature (ϕ = π/2): identical to incoherent

a) Sources in phase (ϕ = 0): NO DIP at all!

c) Sources in counter-phase (ϕ = π): 100% DIP! (resolution doubles)

Page 86: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

RESOLVING POWER: MICROSCOPE ● Microscope optics is definitely NOT paraxial. The Rayleigh criterion in the non-paraxial case becomes:

ONAnλ

θλ

δ 22.1)sin(

22.1 =≈θ = angle subtended by the exit pupil viewed from the image plane NAO = numerical aperture of the objective.

Specimen

Condenser

Objective

Back focal plane

● However, the degree of spatial coherence is controlled by the numerical aperture of the condenser NAC (see next) ● Full coherent illumination for NAC → 0.

● Maximum resolution is obtained when the NA of condenser and objective are comparable

Page 87: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

Try to look at a dilute suspension (3%) of 100 nm PS particles

CERBINO & TRAPPE EXPERIMENT (a replica by Eleonora Secchi)

● Standard microscope in white light ● High N.A. objective (no stop-down tricks), but ● Moderately stopped-down condenser

DDM

BUT NOW TAKE THE DIFFERENCE BETWEEN TWO IMAGES AT SLIGHTLY DIFFERENT TIMES (OR WITH THE TIME AVG.)

Page 88: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

Scattering (3D) and image (2D) q-vectors

⎥⎥⎦

⎢⎢⎣

⎡⎟⎠

⎞⎜⎝

⎛+=

2||2

||2

21

kq

qq

2nd term O(θ)→ for small θ: 2||

2 qq ≈

POLYCHROMATIC In general different q may correspond to the same q||, but negligible for:

||

1q

<<Δλ

Page 89: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

KÖHLER ILLUMINATION

APERTURE STOP Controls the size of the illuminated area

FIELD STOP Controls the spatial

coherence of the source

Page 90: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

A “coherence mosaic” source:

● Scattering from tiny uncorrelated volumes (little problems with turbidity)

Actually, a 3D mosaic!

● Allows for (moderate) z-scan

wt wl

λπ 2

lt

ww ≈

Page 91: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

E.G: Approaching the metastable critical point of a depleted colloid

Page 92: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

GHOST PARTICLE IMAGE VELOCIMETRY (GPIV) Tracing flow with d=50 nm PS tracers

Page 93: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

Flux

Coarse-graining in regions of interest

Page 94: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

FLOW RECONSTRUCTION

Page 95: CMIC DEPARTMENT “Giulio Natta” SOFT MATTER LAB

0

200

400

600

0 200 400 600 800

Δz= 5um Δz= 20um

velocity [um/s]

z [u

m]

z scan

A 3-D TECHNIQUE