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Luca Cipelletti,* Marina Carpineti,† and Marzio Giglio‡

Dipartimento di Fisica and Istituto Nazionale per la Fisica della Materia, Università di Milano, Via Celoria 16, 20133 Milano, Italy

~Received 11 July 1997!

We have measured by means of a charge-coupled device sensor the space correlation function between two

speckle fields at different wavelengths. The fields are generated from the scattering of a two-color laser beam

from a stationary, three-dimensional sample. In general, the speckle fields attain their maximum degree of

correlation when the scattering angles are properly scaled according to a grating dispersion rule. The degree of

correlation, however, depends both on the thickness of the sample and on its turbidity. At a given angle, the

degree of cross-correlation diminishes as the thickness is increased, and it also decreases as the turbidity grows.

Working formulas are derived, and we show that the dependence from the sample turbidity is related to the

spread in photon paths. A comparison with the photon path spread calculated by means of a multiple-scattering

Monte Carlo simulation will be presented. The connection between the present work and studies on polychro-

matic light diffraction from random two-dimensional transparencies and microwave transmission through thick

samples will also be presented. @S1063-651X~98!15502-2#

mation on physical properties of the sample is actually con-

It is well known that the scattered radiation exhibits time tained in the space correlation function. Statistical optics

fluctuations and shows high contrast intensity space varia- teaches that the space correlation function is solely related to

tions, as vividly evidenced by the presence of speckles in the the actual intensity distribution of the scattering volume, as

scattered pattern @1,2#. At a fixed point, the time correlation observed by the region where the speckle pattern is collected

function of the intensity scattered by a sample is simply re- @1#.

lated to the dynamic properties of the scatterers. This is the It has been shown, however, that polychromatic speckle

operating principle of dynamic light scattering, a well estab- techniques can be used to characterize rough surfaces, i.e.,

lished technique that has been successfully used in countless two-dimensional ~2D! samples. Theory and experiments

applications. Sophisticated digital correlators are commer- show that when a rough surface is illuminated by polychro-

cially available, and their use is quite widespread to tackle matic light, the speckle pattern exhibits a radial structure

problems in physics, chemistry, biological science, and revealing a correlation between speckle fields at different

medicine. wavelengths. Furthermore, a measure of the intensity cross-

Present day technology makes it possible to record the correlation provides information on the surface roughness

intensity distribution of a speckle field by means of a charge- @4–7#. In fact, the degree of correlation is related to the sta-

coupled device ~CCD! sensor. The advantage offered by the tistical properties of the scatterer through the rms value s h of

CCD over conventional recording techniques is that they its height fluctuation. When s h is increased, a gradual deco-

provide digitized images of the scattering pattern, which may rrelation is observed and ultimately the polychromatic field

be directly processed while running the experiment. For pro- loses completely its radial structure.

cesses that are slow enough, a new instrumental procedure In the present work we study two-color spatial cross-

for dynamic light scattering measurements has been gener- correlation in three-dimensional ~3D! static samples. We

ated, since parallel correlation function algorithms allow one measure the spatial cross-correlation g I varying the sample

to determine the time correlation functions as evaluated ~in turbidity t and we observe that the cross-correlation function

parallel! at various points in the scattered intensity pattern is almost insensitive to the increase in turbidity until t

@3#. The use of a CCD sensor is very intriguing and very reaches very high values. In fact, at low turbidity the speckle

good quality ~equal time! space correlation functions should patterns are strongly correlated and, only when the samples

be obtainable, thanks to the good averaging properties of the become really turbid, the speckle fields finally start to deco-

process. In view of the fact that time correlation functions rrelate. We will show that the loss of chromatic correlation

give information of great interest, one could ask if the space can be interpreted as due to the spread in photon paths in

correlation function would also yield any valuable informa- getting out of the sample, caused by the presence of strong

multiple scattering. In fact, rampant multiple scattering—

inevitably associated with very high turbidities—causes an

*Present address: Department of Physics, University of Pennsyl- increase in the width s l of the photon path length distribu-

vania 209 S 33rd Street, Philadelphia, PA 19104-6396. Electronic tion p l (l). This spread is responsible for the wave front

address: lucacip@dept.physics.upenn.edu phase modulation imposed on the beam. We find that, in

†

Electronic address: marina.carpineti@mi.infn.it analogy with the 2D case, substantial decorrelation is at-

‡

Electronic address: marzio.giglio@mi.infn.it tained when the typical depth of the wave front modulation

3486 LUCA CIPELLETTI, MARINA CARPINETI, AND MARZIO GIGLIO 57

index of refraction, Dk5k 1 2k 2 , and k 1,252 p /l 1,2 , l 1,2 be-

ing the vacuum wavelength of the two colors. A test of the

above relation has been done by calculating p l (l) and its

standard deviation s l via a Monte Carlo simulation of the

photon propagation @8#. We find good agreement, although

only qualitative, with the proposed model.

The present work is somehow related with two different sets

of papers. In the first one @9–12#, two wavelength correlation

techniques have been used to eliminate from large-angle dy-

namic light scattering measurements the contributions due to

multiple scattering. In spite of the existence of some analogy,

this line of research is quite far from that discussed here, as

will be clarified in the following. Much stronger connections

can be found with the second set of papers @13–16#, in which

correlation measurements of microwaves in random media

are performed as a function of the frequency shifts.

The paper is organized as follows. In Sec. II we describe the

experimental setup and the sample. In Sec. III we present FIG. 1. Schematic diagram of the small-angle static light scat-

both the basic theory and the experimental results for the tering setup for studying the two-color speckle field cross-

single scattering regime at low turbidity values. Finally, in correlation.

Sec. IV we deal with the two-color decorrelation in highly

turbid samples and we briefly discuss the connections be- lected by lens L1. In its focal plane S, a small mirror M is

tween the present work and the experiments described in the placed, forming an angle of 45° with the incident beams. The

two sets of papers mentioned above @9–12,13–16#. transmitted beams are focused by lens L1 onto the mirror

and then reflected to photodiode PD. The lens L2 is posi-

tioned so as to realize a reduced image of the L1 focal plane

II. PRINCIPLE OF OPERATION S onto the CCD sensor. With this optical scheme, each CCD

AND EXPERIMENTAL SETUP pixel corresponds to a different scattering wave vector q,

where q54 p n s l 21 sin u /2, u being the scattering angle.

Spatial cross-correlation measurements are performed as Wave vectors of the same magnitude are mapped to pixels

follows. Two laser beams of different wavelengths are lying on a circumference centered around the optical axis

brought to a sample. Each one generates a speckle field. The position. In the present configuration, the speckle linear di-

spatial cross-correlation g I (r1 ,r2 ) is calculated by multiply- mension is about four CCD pixels and we collect light over

ing the intensity at one point r1 of one speckle pattern by the a range of angles between 0.4° and 10°. Two shutters, driven

intensity of the other one at point r2 ~here and in the follow- by the personal computer ~PC!, are placed in front of the

ing r1,2 describe the points in the far field plane, r50 being lasers and allow to select the speckle field of interest. The

the position occupied by the center of the beam when the CCD images are digitized and acquired by the PC via an

diffuser is removed!. If, as in the present case, the sample is 8-bit frame grabber.

isotropic, the cross-correlation is invariant under rotation As the CCD sensor is a black and white one, the speckle

around the optical axis. Therefore, the cross-correlation func- patterns of the two colors are separately recorded in se-

tion is obtained by averaging over all points lying on a circle quence, and the two-color spatial intensity cross-correlation

of radius r 1 . We will show that at low angle, the maximum function is then calculated. In order to reduce the noise of the

of the cross-correlation function is expected for k 1 r1 cross-correlation function, we average over many pairs of

5k 2 r2 , similarly to the case of 2D samples. This indicates frames ~typically 100!. Before recording each pair of frames,

that if the two speckle fields are perfectly correlated, then the cell is moved in the xy plane for obtaining statistically

they can be exactly superimposed by rescaling the lengths independent speckle patterns, as we used static samples. The

according to r2 5(k 1 /k 2 )r1 5(l 2 /l 1 )r1 , where the ratio calculation of the intensity cross-correlation function g I is

l 2 /l 1 between the wavelengths is the dilation factor of the performed according to the following definition:

speckle fields.

The experimental setup is sketched in Fig. 1. Two linearly ^ I~ q 1 , f 1 !I~ q 2 , f 2 !& q1

polarized He-Ne laser beams of different wavelengths, g I ~ q1 ,q2 ! 5 g I ~ q 1 ,q 2 ,D f ! 5 21.

namely, l 1 [l g 5543.5 nm ~green! and l 2 [l r 5632.8 nm ^ I ~ q 1 , f 1 ! & q1^ I ~ q 2 , f 2 ! & q2

~red!, are combined by the beam splitter cube BS, pass ~1!

through a spatial filter, and impinge onto the sample cell.

The setup is arranged so that the size of the beam spot on the In Eq. ~1!, I(q i , f i ) is the intensity of the speckle pattern of

cell is the same for the two colors. The cell is mounted on a the ith color at a wave vector magnitude q i and at an azi-

xy translator whose movement is controlled by a computer muthal scattering angle f i , D f 5 f 1 2 f 2 , and ^ ••• & q i indi-

guided stepping motor. The optical scheme for the collection cates an azimuthal average over pixels with the same wave

of the scattered light is similar to that described by Ferri vector magnitude q i , i.e., pixels lying on a circumference of

@17#. Both the scattered and the transmitted light are col- radius r i . Note that the intensity cross-correlation may also

57 TWO-COLOR CROSS-CORRELATION IN SMALL-ANGLE . . . 3487

color speckle fields can be recorded in sequence without any

requirement on the CCD and frame grabber speed.

IN THE SINGLE SCATTERING REQIME:

THEORY AND EXPERIMENTAL RESULTS

starting with a brief discussion of the main features of the

intensity cross-correlation function. As we anticipated, a sig-

nificant degree of correlation between the two-color speckle

FIG. 2. Scattering vector diagram. The incident kin , the final fields is expected when d q5q1 2q2 '0. The dependence of

ksc , and the scattering q wave vectors of the two colors are shown. g I on d q can be worked out with simple calculations. In

The difference d q between q1 and q2 is enlarged to show its trans- analogy to Ref. @11#, it can be easily shown that the expres-

verse d qt and parallel d qp components, with respect to the incom- sion for g I (q1 ,q2 ) for single scattering alone is

U U

ing beams direction.

E

2

g I ~ q1 ,q2 ! ' ~2!

E

polar coordinates ~in the sensor plane! r 1 , r 2 , D f : g I ,

5 g I (r 1 ,r 2 ,D f ). Although, as already pointed out, the sta- d 3 xu P ~ x! u 2

tistical properties of the speckle fields are invariant under

rotation about the optical axis, they are not invariant under where u P(x) u 2 is the incident intensity distribution of the

space translation. It follows that g I depends on both r 1 and scattering volume. If we assume that the sample has thick-

r 2 , while it depends on the azimuthal angles f 1 and f 2 only ness d and that the incident beam has a Gaussian profile with

through the angular lag D f , as evidenced in writing Eq. ~1!. radius w at 1/e 2 , then

S D SD

In practice, for a given radius r 1 , we restrict the calculation

of g I to those values of Dr and D f for which a significant 2x 2t xp

u P ~ x! u 2 }exp 2 rect , ~3!

degree of correlation is expected, i.e., when the green and red w d

q vectors approximately coincide.

It is to be pointed out that, with the arrangement shown in where xt and xp are the x components transverse and parallel

Fig. 1, it is not possible to collect exactly the same q vector to the incidence direction and

for the two colors, as the two beams impinge onto the cell

along the same direction ~see Fig. 2!. At low angle, however,

the difference d q between the two scattering wave vectors is

rect x5 H 1, u x u <1

0, u x u .1.

very small. In particular, d q can be considered negligible if it By substituting Eq. ~3! in Eq. ~2!, one obtains

S D

is less than the uncertainty associated to each q mode. In

fact, there is a natural uncertainty in the measure of q—due d q 2t w 2 d q pd

to the finite size of the scattering volume—that is associated g I ~ q 1 ,q 2 ,D f ! 5exp 2 sinc2 , ~4!

4 2

with the finite speckles size @18#. It is useful to decompose

d q into two components d qp and d qt parallel and transverse where sincx5sinx/x, and d q t and d q p depend on q1 and q2

to the incident beam, respectively ~see Fig. 2!. We will show only through their magnitudes and their relative azimuthal

in Sec. III that, with the present arrangement, to maximize orientation, due to the rotational symmetry mentioned above.

chromatic correlation the transverse components of the red From Eq. ~4! it is now possible to determine under which

and green wave vectors must be the same, i.e., d q t 50. conditions the maximum intensity cross-correlation may be

Moreover, as will be demonstrated in the following, to ob- observed. First of all, from simple geometrical arguments it

serve a significant degree of cross-correlation, d qp must be follows that for a given pair of scattering wave vectors q1

less than the typical uncertainty in the parallel component of and q2 , d q is minimum @and therefore g I is maximum, see

q, which is inversely proportional to the sample thickness Eq. ~4!# when both wave vectors have the same azimuthal

@18#. As a consequence, in order to have small enough d qp direction, i.e., for D f 50. Second, for a typical small-angle

one needs to work with thin enough samples. setup the Gaussian term in Eq. ~4! is always narrower than

The samples are microporous membrane filters ~Sarto- the other one, and it rapidly decays to zero. This is evident in

rius!, which have been characterized in a previous work @19#, Fig. 3, where the calculated behavior of the two factors in

and whose features fit very well the experimental require- Eq. ~4! is sketched as a function of the scattering angle for

ments. First of all, the membranes are quite thin, their thick- the red light u r , for three different values of u g , the green

ness being 14065 mm. Moreover, while in air they look light scattering angle. As a consequence, the Gaussian term

perfectly opaque, their transmittivity can be increased by fixes the position of the maximum of the cross-correlation

permeating them by a properly chosen, quasi-index-matching function at d q t 50, and its width at d q t '1/w, which is the

solvent. Therefore, it is possible to gradually vary the sample typical uncertainty in q associated to the speckle size @1,18#.

turbidity t by slightly changing the solvent index of refrac- By working out the dependence of d q t on the scattering

tion. Finally, membranes are static samples, so that the scat- angles, it can be easily shown that, at low angle, the condi-

tered speckle pattern does not change in time. This allows tions D f 50 and d q t 50 yield tan umax r 5(lr /lg)tanug @see

3488 LUCA CIPELLETTI, MARINA CARPINETI, AND MARZIO GIGLIO 57

lag Dr5r r 2r g and of the angular lag D w , both expressed in pixel.

The data were taken at r g 5100 pixels for a low turbidity sample, a

Sartorius membrane filter permeated by a quasi-index-matching sol-

FIG. 3. Calculated behavior of the two factors in Eq. ~4! as a vent. The peak at Dr516 pixels and D w 50 reveals the radial

function of the red light scattering angle u r , for three different scaling of the speckle fields when changing the incoming radiation

values of the green light scattering angle u g ~see text for more wavelength, according to r r /r g 5l g /l r '1.16.

details!. The solid line is the exp(2dq2t w2/4) factor, the dashed line

is the sinc2 d q p d/2 factor. The tick on the upper x axes indicates which the two-color intensity cross-correlation may be ob-

d q t 50. The intensity cross-correlation g I is the product of the two served. Moreover, we note from Eq. ~5! that, as anticipated,

terms plotted above, and is maximum for d q t 50. The two factors

g max

I is significantly greater than 0 for d q p !2 p /d, i.e., when

were calculated using the same parameters as in the experiment:

l r 5632.8 nm, l g 5543.5 nm, w5250 mm, d5140 mm, n s 51.49.

the magnitude of the parallel component of d q is less than

the typical uncertainty p /d of q p due to the finite thickness d

of the scattering volume.

Appendix A, Eq. ~A3!#, where u max r is the scattering angle of

In Fig. 4 a typical example of an intensity cross-

the red light at which the maximum of g I (q 1 ,q 2 ,D f ) is correlation function obtained with a sample at low turbidity

observed for a given u g . Note that, since r r,g }tan ur,g , the is shown. The cross-correlation function refers to a green

above relation may be written as r r 5(l r /l g )r g , as antici- radius r g 5100 pixel ~corresponding to a scattering angle u g

pated in Sec. II. This means that, as in the case of rough of about 1.4°!, and it is plotted as a function of both the

surfaces, for 3D samples in the single scattering regime the radial and the angular lag, expressed in pixel units. The peak

red speckle field is an omothetic version of the green one, the of the cross-correlation shown in Fig. 4 reflects the fact that,

dilation factor being the ratio of the wavelengths l r /l g . It is as discussed above, the red speckle field is the omothetic

to be pointed out that this is the typical scaling law observed version of the green one with a dilation factor given by

when illuminating diffraction gratings with polychromatic l r /l g '1.16. In fact, we observe that the maximum correla-

light. tion is at D f 50, and at Dr516 pixel, in good agreement

We turn now to discuss the second factor in Eq. ~4!, with what was expected as Dr5r r 2r g 5r g l r /l g 2r g . The

which has no analog in the case of rough surfaces. We note width of the peak, that indicates the linear speckle size, is

~see Fig. 3! that the height g max I of the peak of cross- roughly 4 pixels.

correlation is determined by the value of the sinc2 d q p d/2 In Fig. 5 the behavior of the radial part of the cross-

factor in correspondence to the maximum of the Gaussian correlation function (D f 50) is shown for different values

term: of the green radius r g ~the data shown in Fig. 5 refer to the

g max

I 5sinc

2

S DU

d q pd

2 d q t 50

. ~5!

same sample as in Fig. 4!. As already pointed out, the cross-

correlation depends both on r g and on r r and this is evident

by noticing that the peak position moves towards larger r r as

r g increases. The peak position of the data in Fig. 5 has been

As a consequence, it follows that the cross-correlation is compared with the theoretical prediction and the result is

gradually lost when increasing the sample thickness d, for a shown in Fig. 6, where a plot of tanumax r versus tan ug is

given pair of scattering angles u r and u g —i.e.,for d q p fixed, presented. Note the remarkably good agreement between the

see Appendix A, Eq. ~A1!. Conversely, given d, g max I de- experimental data and the theoretical curve tanumax r

creases moving towards larger angles, due to the fact that 5(lr /lg)tanug , where no adjustable parameters have been

d q p u d q t 50 grows with u g @see Appendix A, Eq. ~A4!#. This used. With reference to Fig. 5, there is another interesting

sets a limit on the angular range and sample thickness for feature to notice, namely that the peak height decreases as r g

57 TWO-COLOR CROSS-CORRELATION IN SMALL-ANGLE . . . 3489

enough to prevent any decrease in the peak height due to the

sample thickness. This deviation from the theory arises from

the data acquisition process. There are two main problems

that must be taken into account. The first one is that the CCD

pixels have a finite size, while g maxI 51 is calculated in the

hypothesis of pointlike sensors. The effect of the detectors’

finite size is just that of reducing both the auto-correlation

and the cross-correlation of the speckle fields @1,2#. The sec-

ond problem is associated with digitalization and saturation

effects following from the peculiarities of speckle fields.

Speckles appear as very bright spots on a dark background.

Consequently, in an experimental recording, the highest in-

tensity value can largely exceed the average value, and it is

likely that an appreciable number of pixels reaches the satu-

ration level, even at fairly low average intensity. Therefore,

FIG. 5. The radial part of the cross-correlation g I as a function the contrast is underestimated and g max is lower than ex-

I

of r r , for various r g . The sample is the same as in Fig. 4. Note that pected. One might overcome this problem by reducing the

the peak position shifts towards larger r r when increasing r g , ac- incident beam power. However, at very low average inten-

cording to the radial scaling of the speckle fields of the two colors. sity levels, significant distortions in the measured speckle

At the largest values of r g , the peak height is reduced due to the

pattern arise from the dark current noise and the digitaliza-

thickness of the sample.

tion process @20#. We measured the average intensity and the

speckle contrast as a function of the incident laser intensity,

increases. This result is a direct consequence of the fact that and the best choice of the latter has been determined on the

the difference in q vectors d q increases as the scattering basis of these tests. We stress that measurements are very

angle grows, and that ultimately, when matching the trans- reproducible, in spite of the reduced value of g max I with re-

verse component ( d q t 50), d q p becomes even larger than spect to the theoretical value. Therefore, we think that the

the usual uncertainty in the parallel component of q. limitations intrinsic in the use of finite-size detectors and due

As a final comment, let us consider the maximum mea- to digitalization do not severely affect the results.

surable peak height of the cross-correlation function. From

the definition of g I @see Eq. ~1!#, it follows that the upper

limiting value of l max

I is the square of the ~monochromatic! IV. CHROMATIC DECORRELATION

speckle field contrast, C5 s I / ^ I & , where s I is the standard IN HIGHLY TURBID SAMPLES:

deviation of I. It is well known that the theory predicts C EXPERIMENTAL RESULTS AND DISCUSSION

51 @1#. Actually, from Fig. 4 and from the lower r g curves We have performed measurements of the cross-

in Fig. 5 we observe that g maxI '0.6, which is significantly correlation function for different sample turbidities. As al-

ready explained, it is possible to vary the turbidity by using

solvents with different index of refraction n s . We used ac-

etate of cellulose membranes ~Sartorius SM 123 03! with an

index of refraction n'1.47 permeated by solvents of in-

creasing n s , with n s .n. In Fig. 7 a plot of the maximum of

the intensity cross-correlation g max

I as a function of n s , is

shown. All the measurements of g I have been performed

max

sponding to q g 52100 cm21, which is small enough to pre-

vent a significant decorrelation due to sample thickness.

From Fig. 7 it is evident that the cross-correlation peak value

decreases as the optical mismatch—and therefore the

turbidity—increases.

In order to explain the observed loss of cross-correlation,

it is useful to reconsider the basic results of the works per-

formed on 2D samples @4–7#. Two-color speckle fields gen-

erated by rough surfaces are highly correlated when Dk(n

21) s h ,1, where n is the refractive index of the diffuser

and s h is the rms value of its height fluctuations. When the

surface roughness is increased, the fields start to significantly

decorrelate. In particular, it can be shown @4,5# that the in-

FIG. 6. The peak position of the data shown in Fig. 5. Note the tensity cross-correlation function is given by

very good agreement between the experimental data ~filled squares!

and the theoretical line, where not adjustable parameters have been

used. g I ~ q1 ,q2 ! 5 u F h ~ d q p ! u 2 u m ~ d qt ! u 2 , ~6a!

3490 LUCA CIPELLETTI, MARINA CARPINETI, AND MARZIO GIGLIO 57

creasing the spread in path lengths. The analogy with the

case of rough surfaces suggests that the chromatic decorre-

lation is determined by the spread in path lengths. To be

more explicit, the analogous of (n21) s h for 3D samples is

the spread n s s l of the photon optical path length distribution

inside the sample, s l being the standard deviation of the

geometrical photon path distribution p l (l). Consequently,

we expect that the fields will start to significantly decorrelate

when

Dkn s s l >1. ~8!

A similar result was obtained in the past in works on

microwave propagation in random media @13–16#. The au-

thors performed cross-correlation measurements varying the

FIG. 7. The intensity cross-correlation peak height g max I as a wave frequency and they relate the decorrelation to the

function of the refractive index of the solvent. The refractive index spread in photon travel times through the sample. Further-

of the sample is n'1.47. The cross-correlation is gradually lost more, they show that the intensity-intensity correlation as a

when increasing the refractive index mismatching, and therefore the function of frequency shift is the squared modulus of the

sample turbidity. The letters in the figure are for future reference. Fourier transform of the photon time-of-flight distribution

@15#. We recall that Eqs. ~6a! and ~6b! link the two-color

where m ( d qt ) is the so-called complex coherence factor, and intensity cross-correlation to the Fourier transform of the

F h ( d q p ) is the characteristic function of the height probabil- photon optical path distribution. Therefore, there is a strong

ity density p h (h) @1#: analogy between the results reported in Ref. @15# in the time

domain for microwave propagation, and those described in

E

the space domain for light scattered by 2D samples. It is

d 3 xu P ~ x! u 2 exp~ ix• d qt ! quite remarkable that the two descriptions that apply to quite

m ~ d qt ! 5 different electromagnetic spectral regions have the same

E

,

physical root.

d 3 xu P ~ x! u 2 We will now compare the loss of cross-correlation with

~6b! the spread of the photon path length distribution, calculated

F h~ d q p ! 5 E dhp h ~ h ! exp~ ih d q p ! .

by means of a Monte Carlo simulation of the photon propa-

gation. The Monte Carlo multiple-scattering code is de-

scribed in detail in Ref. @8#. We simply recall here that the

simulation consists in tracking the path of a great number of

@Incidentally, we note that for a Gaussian incident beam, the

photons through the sample. For each launched photon, track

u m ( d qt ) u 2 term in Eqs. ~6a! and ~6b! is exactly the same as

is kept of the length of the path in getting out of the sample,

the Gaussian factor in Eq. ~4!.# From Eqs. ~6a! and ~6b!, it so that the photon path length distribution p l (l) can be cal-

follows that g I depends on the diffuser only through the culated for all q vectors of interest. The main required input

characteristic function F h ( d q p ). In the hypothesis of a parameters are the single scattering differential cross section

Gaussian distribution of the diffuser height, it can be shown and the turbidity t of the sample or, equivalently, its trans-

that at small angles F h does not depend on d q p @20#: mission T. The differential scattering cross section was that

obtained, for the same sample, in Ref. @8#. The measurement

F h 5exp@ 2Dk 2 ~ n21 ! 2 s 2h # , ~7! of the sample transmission deserves a brief comment. At low

turbidity, T can be directly measured thanks to the photodi-

Since F h is independent from q1 and q2 , it can be easily ode PD ~see Fig. 1!, by dividing the transmitted beam power

understood that for 2D samples m ( d qt ) fixes the peak posi- in the presence of the sample by that with the cell filled with

tion of g I (q1 ,q2 ) at d q t 50, while the second factor in Eq. the solvent alone. For highly turbid samples, however, the

~6a!, F h , is responsible of its height. The validity of Eqs. transmitted power can be comparable to, or even lower than,

~6a! and ~7! has been verified both qualitatively @4,6# and the power of the light scattered at extremely low angle, col-

quantitatively @7# in the past. lected together with the transmitted beam by the tiny mirror

It is to be noted that it is impossible to distinguish M , due to its finite size. Therefore, there is a comparatively

whether the wave front deformations of the scattered field high spurious signal on PD that leads to a significant over-

immediately after the cell have been introduced by a 2D or estimation of T. The correct value of the transmission can be

by a 3D sample. What is actually different is the physical recovered by iteratively running the simulation program.

mechanism that generates the phase variations, although in One starts with a guess for T to obtain the simulated total

both cases they depend on the differences in photon optical light collected by M ~scattered light plus transmitted beam!.

path lengths for crossing the sample. For 3D samples, the The initial estimate is then refined by comparing the result of

different path length of the photons is determined by the the simulation with the experimental data, and a corrected

amount of multiple scattering. In fact, photons that undergo a value of T is input for a second run. The entire process is

few scattering events travel a shorter path when compared to repeated until the simulated power converges to the mea-

those scattered many times. Moreover, we point out that, as sured one. Thanks to this procedure, it has been possible to

the turbidity grows, multiple scattering of higher orders be- estimate the transmission even for the more turbid samples,

57 TWO-COLOR CROSS-CORRELATION IN SMALL-ANGLE . . . 3491

index n s , the measured cross-correlation peak height g max I and the

ratio between the single and total scattering intensity, I s /I t , calcu-

lated via the Monte Carlo simulation. In the last column, we show

the ratio g max 2

I /(Is /It) , which would be constant if multiple scattering

contributions were uncorrelated. The enormous increase in

g max 2

I /(Is /It) clearly indicates that in the present case also multiply

scattered photons contribute to the cross-correlation.

ns g max

I I s /I t g max

I /(Is /It)

2

1.5028 0.54 0.61 1.45

1.5074 0.48 0.41 2.86

1.5144 0.37 0.18 11.4

1.5216 0.29 0.03 322

1.5290 0.20 0.02 500

1.5385 0.10 ,131024 .107

tering contributions by cross-correlating the scattered light of

two wavelengths, collected at different angles chosen so that

FIG. 8. Photon path length distribution p l (l), calculated via the the single scattering wave vectors exactly coincide. It can be

Monte Carlo simulation described in the text, for different values of shown that the time dependence of the cross-correlation

the sample turbidity t . The curves are labeled with the same letters function is solely due to single scattering. The two tech-

as the points in Fig. 7. niques, however, are substantially different. In particular, we

stress that in the present experiment the loss of cross-

for which a direct measurement of T would not have been correlation when the sample turbidity increases cannot be

feasible. As a check for the correction procedure, we have explained by assuming that the multiply scattered contribu-

also estimated t for the most turbid samples by extrapolating tions are uncorrelated. It can be shown ~see Appendix B!

the low refractive index dependence of the turbidity versus that, if the singly scattered contributions were the only cor-

n s . The corrected data are in reasonable agreement with the related ones, then g max would be proportional to (I s /I t ) 2 ,

I

extrapolated ones, the maximum deviation being less than where I s and I t are the single and the total scattered intensity,

30%. respectively. The ratio I s /I t for the data shown in Fig. 7 has

We have calculated the photon path length distributions been calculated by means of the simulation program de-

p l (l) and their standard deviation value s 1 for each experi-

mental point shown in Fig. 7 but the last one, for which T

was too high to be estimated in a sensible way, even via the

Monte Carlo simulation. Figure 8 shows some examples of

the calculated p l (l), for different values of the turbidity.

Filled squares refer to the case t 53.4 mm21, corresponding

to T562%, for which the maximum cross-correlation peak

value has been measured. As can be seen, p l (l) vanishes for

l.140 mm—i.e., for photon paths longer than the sample

thickness—in agreement to what is expected due to the fact

that single scattering prevails ~see Table I!. As the turbidity

increases, multiple scattering becomes appreciable and this

leads to a larger standard deviation s l of p l (l) ~see curves

B, C, and D in Fig. 8!. As discussed above, we expect that

the increase in the photon path length spread is responsible

of the cross-correlation loss and that the speckle fields of the

two colors significantly decorrelate for Dkn s s l >1. In order

to verify this statement, we have plotted in Fig. 9 the experi-

mentally measured maximum value of the cross-correlation

function g max

I as a function of Dkn s s I . Note that the behav-

ior of g max

I is in good agreement with the one qualitatively

expected, as it is significantly reduced when Dkn s s l >1. FIG. 9. The measured intensity cross-correlation peak height

As a final point, let us consider the analogies between the g max

I as a function of Dkn s s l , where s l has been calculated via the

present experiment and a two-wavelength cross-correlation Monte Carlo photon propagation simulation. The cross-correlation

technique, proposed in the past for large-angle dynamic light between the two-color speckle fields is substantially lost when

scattering measurements of very turbid samples @9–12#. In Dkn s s l >1.

3492 LUCA CIPELLETTI, MARINA CARPINETI, AND MARZIO GIGLIO 57

scribed above and is reported in Table I, together with scattered at small angles by thin 3D samples. We have used

g max

I /(Is /It) . It can be noted that the ratio g I /(Is /It) enor-

2 max 2 an experimental setup that allows to record the intensity dis-

mously increases with the amount of multiple scattering, thus tribution of the speckle fields, thanks to a CCD sensor. We

demonstrating that single scattering contributions are not the have shown that, in order to observe a significant degree of

only correlated ones. cross-correlation, it is necessary for the difference between

The main differences between the two techniques are the the scattering wave vectors to be small compared with the

following. First, we do not collect light so that the scattering natural uncertainty in q associated with the finite sample

q vector is exactly the same for the two wavelengths, as in thickness. Furthermore, we have observed that cross-

the two-color dynamic light scattering apparatus. Second, we correlation is gradually lost when the sample turbidity is in-

collect light at small angles and use samples with a differen- creased. We have suggested that this effect is associated with

tial scattering cross section strongly peaked near the forward the spread in photon path lengths caused by multiple scatter-

direction @19#, while in a typical two-color dynamic light ing. We have tested this guess thanks to a Monte Carlo simu-

scattering setup measurements are performed at much larger lation of photon propagation, and a qualitative good agree-

angles @12#, and using small scatterers, which diffuse light ment between the model and the experimental data has been

almost isotropically. As a consequence, for the dynamic light found.

scattering experiment the two-color wave vectors associated

to each intermediate scattering event are generally much dif-

ferent, and the only significantly correlated are the singly ACKNOWLEDGMENTS

scattered ones. Conversely, in the present experiment the dif-

The authors thank D. A. Weitz for useful discussions and

ferences between the intermediate scattering vectors for the

for bringing to their attention the papers by A. Z. Genack

two colors are so small that they turn out to be comparable to

et al. They also wish to thank F. Ferri for suggestions in

the unavoidable difference d q between the final wave vec- designing parts of the instrument. This work was partially

tors. Therefore, even light scattered more than once probes supported by the Ministero dell’Università e della Ricerca

essentially the same fluctuation Fourier modes for the two Scientifica e Tecnologica ~MURST! and by the Agenzia Spa-

colors. Note that the same reason for which we are able to ziale Italiana ~ASI!.

observe correlation with the present configuration—i.e., that

d q is smaller than the natural uncertainty in q—is respon-

sible for the correlation between multiply scattered contribu- APPENDIX A

tions. Only when a large number of scattering events occurs,

the small differences in the intermediate wave vectors may In this appendix we work out the dependence of d q p and

sum up and finally overcome d q, giving rise to a significant d q t on the wave vectors k 1 and k 2 of the two-color incident

loss of cross-correlation. light, and on the scattering angles u 1 and u 2 for the two

To summarize, we have performed measurements of two- colors. We will refer to the case D f 50 shown in Fig. 2.

wavelength spatial cross-correlation between the intensities From simple geometrical calculations, one gets

d q p 5n s 5 , ~A1!

A11tan2 u 1 A11tan2 u 2

k 1 tanu 1 A11tan2 u 2 2k 2 tanu 2 A11tan2 u 1

d q t 5n s . ~A2!

A11tan2 u 1 A11tan2 u 2

served for d q t 50. Accordingly, to find the relation between

In this appendix we will show that, if multiple scattering

u 1 and u 2 at the g I peak position, we set the numerator of

contributions to the two-color scattered field were uncorre-

Eq. ~A2! to zero, we expand in Taylor series in tanu1 and

lated, then g max would be proportional to (I s /I t ) 2 , where I s

tanu2 up to the first order, and we solve for tanu1 : I

and I t are the single and the total ~single plus multiple! scat-

k1 l2 tered intensity, respectively.

tanu 2 u d q t 50 [tanu max

2 5 tanu 1 5 tanu 1 . ~A3! We start by recalling that the Siegert relation @10# allows

k2 l1

us to express g I (q1 ,q2 ) through the field cross-correlation

Finally, we calculate the d q p value at the cross-correlation g A (q1 ,q2 ):

peak position. Substitution of Eq. ~A3! into Eq. ~A1! yields,

up to the second order in tanu1 ,

g I ~ q1 ,q2 ! 5 u g A ~ q1 ,q2 ! u 2 , ~B1!

1 k2

d q p u d q t 50 5 n ~ k 2k ! tan2 u 1 . ~A4!

2 k2 s 1 2 where

57 TWO-COLOR CROSS-CORRELATION IN SMALL-ANGLE . . . 3493

^ A ~ q1 ! A * ~ q2 ! & I s~ q 1 ! I s~ q 2 !

g A ~ q,q2 ! 5 , ~B2! g I ~ q,q2 ! 5 u g A,s ~ q1 ,q2 ! u 2 . ~B4!

AI ~ q 1 ! I ~ q 2 ! I t~ q 1 ! I t~ q 2 !

and A(q) is the scattered field. If we assume, as in Ref. @11#, Since the maximum intensity cross-correlation is observed

that only single scattering contributes to g A , then in the pres- for q 1 'q 2 [q, from Eq. ~B4! we obtain

ence of multiple scattering

~B3!

g max

I ~ q ! 5 u g A,s ~ q ! u

2

S DI s~ q !

I t~ q !

2

. ~B5!

In Eq. ~B3! subscripts s and t refer as usual to single and For a given sample thickness and a given scattering wave

total scattering, respectively, and g A,s is the field cross- vector q, g A,s is a constant and does not depend on the

correlation that would have been observed if single scatter- amount of multiple scattering. Therefore, Eq. ~B5! shows

ing alone were present @see Eq. ~B2!#. Equations ~B1!, ~B2!, that the cross-correlation peak height is proportional to the

and ~B3! yield square of the fraction of single scattering intensity.

@1# J. W. Goodman, in Laser Speckle and Related Phenomena, @11# K. Schätzel, J. Mod. Opt. 38, 1849 ~1991!.

edited by J. C. Dainty ~Springer-Verlag, Berlin, 1975!; J. W. @12# P. N. Segrè, W. Van Megen, P. N. Pusey, K. Schätzel, and W.

Goodman, Statistical Optics ~Wiley, New York, 1985!. Peters, J. Mod. Opt. 42, 1929 ~1995!.

@2# See, for example, B. J. Berne and R. Pecora, Dynamic Light @13# A. Z. Genack, Phys. Rev. Lett. 58, 2043 ~1987!.

Scattering ~Wiley, New York, 1976!. @14# N. Garcia and A. Z. Genack, Phys. Rev. Lett. 63, 1678 ~1989!.

@3# A. P. Y. Wong and P. Wiltzius, Rev. Sci. Instrum. 64, 2547 @15# A. Z. Genack and M. Drake, Europhys. Lett. 11, 331 ~1990!.

~1993!. @16# A. Z. Genack, N. Garcia, and W. Polkosnik, Phys. Rev. Lett.

@4# G. Parry, Opt. Commun. 12, 75 ~1974!. 65, 2129 ~1990!.

@5# G. Parry, in Laser Speckle and Related Phenomena ~Ref. @1#!. @17# F. Ferri, Rev. Sci. Instrum. 68, 2265 ~1997!.

@6# G. Tribillon, Opt. Commun. 11, 172 ~1974!. @18# See, for example, G. B. Benedek, in Statistical Physics, Phase

@7# M. Giglio, S. Musazzi, and U. Perini, Opt. Commun. 28, 166 Transition and Superfluidity, edited by M. Chretien, E. P.

~1978!. Gros, and S. Deser ~Brandeis University, Waltham, MA,

@8# L. Cipelletti, Phys. Rev. E 55, 7733 ~1997!. 1966!, Vol. 2.

@9# G. D. J. Phillies, J. Chem. Phys. 74, 260 ~1981!. @19# L. Cipelletti, M. Carpineti, and M. Giglio, Langmuir 12, 6446

@10# J. K. G. Dhont and C. G. De Kruif, J. Chem. Phys. 79, 1658 ~1996!.

~1983!. @20# L. Cipelletti, Ph.D. thesis, University of Milan, Italy, 1997.

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