Physical Optics of Iridescent

Multilayered Plastic Films

T. ALFREY, JR., Plastic Materials and Products Laboratory,
Dow Chemical Company, Midland, Michigan

E. F. GURNEE, Physical Research Laboratory,

Dow Chemical Company, Midland, Michigan

W. J. SCHRENK, Plastic Materials and Products Laboratory,

Dow Chemical Company, Midland, Michigan

The physical optics of iridescent multilayered plastic films

are analyzed theoretically relating the layer thickness, layer
arrangement, and refractive index difference between layers
to the reflection spectra for light at normal incidence. Very
vivid iridescent and metallic-appearing films may be made by
proper control of layer distribution.

INTRODUCTION tion. The wave-length of the first-order reflection

ultilayer plastic films containing hundreds of (for normal incidence) is given by:
M layers of two or more different thermoplastic
polymers can be produced by co-extrusion. If the
A1 = 2( nodd d o d d f
deven)
neven (1)
component polymers have different refractive indices, For example, if the thicknesses of the odd and even
and if the layer-thicknesses are properly adjusted, layers are set at 700 A and 746.5 A, respectively:
vivid optical effects can result. Some wave-lengths of nodCldocid = 1.6 X 700 = 1120.
light are strongly reflected, while others are trans-
mitted through the film. In this paper we shall dis- n,,,,CZ,,,~ = 1.5X 746.5 = 1120.
X I = 2 (1120 + 1120) = 4480 A.
cuss how reflection spectra of multilayer films are
determined by the layer arrangements.
This simple calculation, using Eq. 1, can be useful
SIMPLE THEORY
Consider, for example, a 201-layer film containing
101 odd layers and 100 even layers. The odd layers . !I !I26

have a refractive index of 1.6, and the even layers a

refractive index of 1.5. (Polystyrene and polymethyl- no= 1.0
I
methacrylate are close to these values.) If all the nlE1.6
layers are of equal optical thickness, the wave-lengths 112'1.5
of strong reflections can be calculated by a very n, = 1.6
172'1.5
simple procedure. I
Figure 1 is a schematic drawing of such a multi- I
layer film. When a beam of light, of wavelength A, I
I
shines upon the film, partial reflection occurs at each
of the many interfaces. The reflections at the inter-
faces of increasing refractive index suffer a phase
reversal. Since the layers differ only by 0.1 in refrac-
tive index, the individual reflections are weak. How-
ever, if reflections from the different interfaces all no=I.O
leave the film in phase with each other, the con-
structive interference yields a high intensity reflec- Fig. 1. Reflection of light from multilayer films.

400 POLYMER ENGINEERING AND SCIENCE, NOVEMBER, 1969, Vol. 9, No. 6

 Physical Optics of Iridescent Multilayered Plastic Films

in the design of multilayer plastic films with specific simple theory). At this wavelength, the reflectance
desired optical responses. On the other hand, there is 85%. Reflectance is > 50% over a wave-length
are many important questions which Eq. 1 does not region of about 250 A. This main reflection peak is
answer: the intensity and width of the reflection flanked by a series of weak bands with reflectance
peak; the wave-lengths and intensities of higher varying from zero to 20%.
order reflections; the reflection spectra of films with
systematically varying layer thicknesses; etc. For this
reason, the simple theory must be augmented by the
more comprehensive analysis presented in the fol-
lowing section.

GENERAL THEORY
Francon ( 1 ) and Vasicek ( 2 ) describe a matrix n,.,=1.500 d.”..= 746.5A
method for calculating the reflectivity of a nonab- 0.6 -
sorbing multilayer system, taking into account mul-
tiple reflections. This method follows: 0.4 -
The ith layer has thickness d , and refractive index
ni. These quantities determine the incremental phase
angle ai,of the ithlayer:
2 T nidi
ai = - DO
A h-dl

A 2 x 2 matrix (complex numerical) characterizing
the optical behavior of the ith layer can now be de-
fined :
where j = drl
A matrix ( Q ) , characterizing the entire multilayer
film, can now be calculated. ( Q ) is the matrix prod-
uct of the N individual layer matrices:
(Q) = (14)( 2 4 ) ( 8 4 ) - . -
Fig. 2. Reflection spectrum for a 50-layer film hauing layers
of uniform optical thickness.
In Fig. 3 is presented the calculated reflection
spectrum for a 100-layer film made up of the same
alternating layers as above. The peak reflectance,
which again occurs at 4480 A, is 99%. The low side-
bands are closer together and more numerous than
in the previous case.
Similar calculations for films containing 250, 400,

r
* ( N q ) (4)
Q is a complex 2 x 2 matrix.
The reflectance (fraction of incident light re-
flected by the multilayer film) can now be com- N=100LAYERS
puted from the formula: nodd= 1.600 d , d ~ = l O O A

+ n~+iQiz)- n =1.500 d ~746.5A

c
dQii (Q21+ ~N+IQZZ) 0.6
R=
[ + + +
n0(Q11 n~+1Q12) (421

where no and nN+ in our case ordinarily correspond

to 1.0 (the refractive index of air).
0.4 I 11
This matrix method was used to calculate the re- 0.2

flection spectra R ( A ) for a large number of multi-

layer films, in order to evaluate the effects of layer 0
4,000 4,500 5,000 5,500 6,000 6,500 7,000 7,500
arrangement and refractive index differences upon A-IA)
the optical response. Dispersion was ignored in the
Fig. 3. Reflection spectrum for a 100-layer film.
following calculations; the same value of refractive
index was used for all wavelengths.
and 600 layers yield the results shown in Fig. 4 : re-
REFLECTION SPECTRA OF FILMS WITH flectance approaching 100% throughout the wave-
UNIFORM LAYER THICKNESS length region A = 4480 *
100 A; and closely spaced
The complete reflection spectrum R ( A ) calculated side-bands which averaged out to about 10% re-
for a 50 layer film ( nodd = 1.6; neven= 1.5; dodd = flectance outside of this main band.
700 A; d,,, = 746.5 A) is shown in Fig. 2. The peak With a larger refractive index contrast, a given
reflectance occurs at 4480 A (as predicted from the degree of reflectivity can be attained with a smaller

POLYMER ENGINEERING AND SCIENCE, NOVEMBER, 1969, Vol. 9, No. 6 401

 T . Alfrey, Jr., E . F . Gurnee, and W. J. Schrenk

The simplest pattern of systematic layer thickness

variation is a linear function:
d&d=doodd+ a m (6)
deven = doeven
where m is the number of the layer. Such a variation
+ P m, (7)
in layer thickness is shown in Fig. 5. Keeping the
total number of layers constant, we can broaden the
wavelength region of strong reflectance by increasing
the value of a and P. However, if a and P are made
too large, the reflectance values throughout the band
will fall off.
Reflectance spectra were calculated for a series of
multilayer films, using the following parameters :
0 I I I I I I
4.000 4,500 5,000 5,500 6,000 6,500 7,000 7,500 nodd = 1.6 neven= 1.5
x-tlr
doodd = 700 A doeven= 746.5 A
Fig. 4 . Equivalent square wave of the reflection spectrum for P = 1.066 a
films having 250,400, and 600 layers.
A typical reflectance spectrum, for a = 0.5, N =
500, is shown in Fig. 6. In this case, R > 0.5 over
the range 4460 < A < 6100, and is > 0.95 over most
of this range. Similar spectra, differing in the upper
and lower cut-off frequencies and in peak reflec-
tivity, were obtained for other values of a and N .
Figure 7 shows upper and lower cut-off wavelengths

I
II
LAYER NUMBER-m

Fig. 5. Multilayer films with linear variation of layer thickness.

number of layers. Thus, if ?%odd= 1.6 and n,,,, = 1.4,

the peak reflectivity is > 99% for a 50-layer film.
04 -

FILMS WITH LINEARLY VARYING

LAYER THICKNESSES 0.2 -

As shown above, films with uniform optical thick-

0 ‘ b l I I I I
ness of the layers can exhibit very strong reflectance, 30
but only in a narrow wavelength band. To develop
vivid reflection colors, it is necessary to have high
Fig. 6 . Reflection spectrum of a 500-layer film having linearly
reflectance over a broader range of wavelengths. We increasing layer thickness.
can expect the most vivid impressions of color to
arise if the band of strong reflectance extends be-
tween two complementary wavelengths.
Bouma ( 3 ) refers to a reflection spectrum with R
= 1.0 throughout a wavelength band and R = 0.0
‘-1
l,oL I LOW h CUT-OFF , HIGH A CUT-OFF

elsewhere as an “ideal” color. A special class of

“ideal” colors, the “C-colors,” are characterized by BROAD BAND WIDTH
-REDUCE0 PEAK
the fact that the two jumps in reflectance ( 0 += 1.0 -
REFLECTION

and 1.0 + 0 ) occur at complementary wavelengths. NARROWER BAN0 WIDTH

0.6 -HIGH PEAK REFLECTION
Bouma shows that the most vivid color sensation
achievable by selective reflectance-the optimum
compromise between the contradictory requirements 0.4
I / N = 2 5 0 LAYERS
of brightness and purity (hue)-will closely cor- nodd = 1.600 new,”= 1.500
respond to a “C-color”.
Furthermore, strong reflectance over the entire d,,,,=746.5+ 1.066 am
visible spectrum results in a metallic appearance.
Such broad reflection bands require the use of 00

varying layer thickness through the multilayer plastic

film. Fig. 7 . Breadth of strong reflection versus 01.

402 POLYMER ENGINEERING AND SCIENCE, NOVEMBER, 1969, Vol. 9, No. 6

 Physical Optics of Iridescent Mukilayered Plastic Films

for various values of a, for films having a total of 250 various orders are determined entirely by the sum of
layers. It is apparent that to achieve very high reflec- optical thicknesses of the two adjacent layers, the
tivity over a very broad wavelength band, either N relative intensities of the various orders are strongly
must be greater than 250 or A n must be greater than dependent upon the ratio between the two optical
0.1. However, strong reflectance throughout a lo00 A thicknesses.
band would be possible with 250 layers alternating
between n = 1.5 and n = 1.6.
A rough estimate of the maximum and minimum
cutoff wavelengths for the case of linearly varying
layer-thickness can be obtained from the following In Fig. 9, we see the dependence of relative reflec-
simple equations (without going through a complete tance upon f, for the first four orders. Equal optical
optical analysis) : thickness ( f = 0.5) results in complete vanishing of
all even orders, and very strong reflections at all odd
h*min =2 ( % I d dodd + neven deven)min (8) orders. If the odd layer comprises y4 of the total opti-
h"max = 2 (nodd
dodd neven deven)max +
(9) cal thickness (or 3,4), the second-order reflection is
very strong, but the fourth-order vanishes. Higher
Predicted cutoff wavelengths obtained from Eq. 8 order reflection behaviors corresponding to several
and 9 are shown as broken lines in Fig. 8. other values of f are listed below:
HIGHER ORDER REFLECTIONS f = 0.15 to 0.2; first four orders present;
I11 strong.
In addition to the first-order reflection and its low
side-bands, discussed above, a multilayer plastic film f = 0.33; I11 vanishes.
can exhibit higher order reflections. The wavelengths
at which reflections of various orders appear are f = 0.4; I and IV strong.
given by the following equations: The above relationships might be useful in design-
ing multilayer films with certain desired reflection
1.2 spectra in the infrared and/or ultraviolet region as
well as the visible region. If on2y the visible region
-
1.0
is of interest, design can be made utilizing first-order
reflections only.
El
08 -

0.6 -
W W

il M
0.4 - 0 V
N.250 LAYERS z 2
n.rc ~1.600nSlll= 1.500
a 3
t
V u
0.2 - d,dd = 700 + am W
A
W
A
d,,, = 746.5 + 1.066 an LL LL
W W
a a
0 I I Y Y
4,000 4,500 5,000 5,500 6,000 6,500 7,000 7,' a a
W W
A-lil n n
. .25 50 75 1.0
Fig. 8. Calculated cutoff wavelengths for films having linearly 0 .5 I .o
increasing layer thickness. f f
( a ) FIRST ORDER ( b ) SECOND ORDER

XI = 2 ( nod, dodd + neven deven) ( )

&I =-
2
2
(%id dodd + neven deven) ( lob)

!!!fb
W
0
2
h r I = - ( nodd
3
dodd + neven deven) ( lot)
2
3
V
W
A
LL
W W
a a
Y Y
a U
W
W
n0 .33 .67 1.0 n

0 .25 .50 .75 1.0

f f
( c ) THIRD ORDER ( d ) FOURTH ORDER
where hMis the Mth order reflection.
Although the spectral locations of reflections of Fig. 9. Peak reflectance of higher order rgections.

POLYMER ENGINEERING AND SCIENCE, NOVEMBER, 1969, Vol. 9, No. 6 403

 T . Alfrey, Jr., E . F . Gurnee, and W. J . Schrenk
SUMMARY AND CONCLUSIONS
1. Thin multilayer plastic films can exhibit irides-
cence resulting from constructive reinforcement of
radiation reflected from the many layer interfaces.
The character of the reflection spectrum depends
upon the refractive index mismatch of the two phases,
the number of layers, and the thicknesses of the
various layers.
2. Narrow reflection bands can be developed in
films where all odd layers are identical and all even
layers are identical. The peak reflectance (first order)
occurs at the wavelength x I :
A1 2 (nodd dodd+neven
The peak reflectance is 99% for 100 layers, with
refractive indices of 1.5 and 1.6, and increases
strongly with increasing number of layers and in-
creasing refractive index mismatch.
3. Broad reflectance spectra require some syste-
404
matic variation of layer thicknesses through the film.
Color effects approaching “C-colors” can be devel-
oped with 250 layers, An = 0.1, and a linearly vary-
ing pattern of layer thickness. To achieve very high
reflectance over the entire visible spectrum would
require more layers or greater refractive index mis-
match.
4. Relative intensities of the various higher order
reflections depend upon the ratios of optical thickness
of the adjacent layers.
REFERENCES
1. M. Francon, “Interscience Tracts,” 13, 7, John Wiley, New
York (1963).
2. A. Vasicek, “Optics of Thin Films,” North-Holland Publish-
ing Co., Interscience Publishers, Inc., New York, N. Y.
(1960).
3 . P. J. Bouma, “Physical Aspects of Colour,” 140, Elsevier
Book Co., New York, N. Y. (1947).
POLYMER ENGINEERING AND SCIENCE, NOVEMBER, 1969, Vol. 9, No. 6