Professional Documents
Culture Documents
J. M. BENNETT
Michelson Laboratory, Naval Weapons Center, China Lake, CA 93555 (U.S.A.)
(Received August 13, 1984; accepted November 2, 1984)
1. INTRODUCTION
* Paper presented at the Sixth International Conference on Thin Films, Stockholm, Sweden, August
13-17, 1984.
2. SCATTERING
1
CATTEREOL,O,,
SCATTE R ED LIGHT
~ MgF2
AI
LONG RANGE (mm) EFFECT
COLUMNAR STRUCTURE,
INHOMOGENEITY IN FILM tI ~ t2 ~ t3
INTERFERENCE EFFECTS CAN CONTRIBUTE STRONGLY TO
CROSS CORRELATION EFFECTS NEAR-ANGLE SCATTERING
BETWEEN ROUGH SURFACES
Fig. 1. Schematic diagram of microirregularity-induced scattering from transparent and opaque films.
very close to the specular beam can sometimes be determined from a modulation
transfer function measurement of the blur circle of the specular beam.
or
2
6 ~ - T I S 1/2 (lb)
where 2 is the wavelength. The TIS is the ratio of the total light scattered by the
surface (total hemispherical scattering) divided by the sum of the specularly reflected
plus scattered light. Since for smooth surfaces the scattered light is a small fraction of
the specularly reflected light, the ratio becomes as shown in Fig. 2 and is thus
independent of the sample reflectance. For measurements in the visible spectral
region, the instrument can be conveniently calibrated using a white lambertian
scatterer such as polytetrafluoroethylene1°, BaSO~, Kodak white giowder, Kodak
white reflecting paint or other material. The TIS method for obtaining an effective
surface roughness forms the basis for an ASTM draft roughness standard 6, and
HEMISPHERICAL
COLLECTING MIRROR DETECTOR
//"~ f (SCATTERED
DETECTOR ¢/ f //RADIATION)
(REFLECTED BEAM)I / / J'~
DETECTOR
(INCIDENT BEAM)
Fig. 2. Schematic diagram of an instrument for measuring TIS (from ref. 6):
V sample, scattered = /4~rms/ 2
TIS V sample, specular
where 6,~, is the effective r.m.s, roughness. Hence
2
6rm, = - - TISI/2
4n
30 J.M. BENNETT
roughness values for polished surfaces obtained from TIS measurements have been
shown to correlate with roughnesses measured interferometrically ~~
The TIS can be measured as a function of wavelength for checking the validity
of the scalar scattering theory in the visible and UV spectral regions 7 or plotted at a
single wavelength as a function of position on the sample surface (Fig. 3). The
advantage of the three-dimensional plot is that a low scatter portion of the surface
may be selected if the illuminated area on the mirror is small compared with the total
mirror area.
SCATTERING
(xlO-4)
Fig. 3. Scattering from an aluminized superpolished fused quartz mirror plotted as a function of position
on the mirror surface (wavelength, 6471 A; r.m.s, roughness, 5/~): average scattering, 1 x 10-4; maximum
scattering, 8.5 x 10 -4.
TIS can also be used to measure the effect of scratches, digs, dust and other
particulates, particularly in the IR where scattering from small isolated surface
defects dominates because of the 1/22 dependence of microirregularity scattering 7.
Scratches have irregular cross-sectional profiles 12 and widths in the micrometer
range, but their effects can easily be measured by a laser beam whose diameter is of
the order of 1 ram, as shown in Fig. 4, even on an uncoated surface 12. Surface
plasmon effects can also give rise to scattering from silver-and aluminum-coated
surfaces ~'4. Evanescent surface waves can couple into the surface roughness to
produce absorption and subsequent re-radiation of light that looks like scattered
light.
~"='e..o._
e'°f./~
8,0 ~
6.0
4.0 4.0
2.0
0
2.0 i
-I,0 1.0
0
X (mm) ,0 -' 0
Y (mm)
~'-~.0
(a) (b)
Fig. 4. Scattering from uncoated scratch standards plotted as a function of position on the surface
(wavelength, 6471 A) (from ref. 12): (a) number 60 scratch width, 5.4 Ixm (31r, scratch; A , background); (b)
number 20 scratch width, 2.6 ~ n .
which gives the scattering per unit solid angle as a function Of wavelength, angles of
incidence and scattering, optical constants of the surface, polarization of the incident
and scattered light and surface roughness parameters is summarized in Appendix A.
The surface parameters enter as the r.m.s, roughness and the Fourier transform of
the surface autocovariance function 14. The angle-resolved scattering equations can
be integrated to yield the correct TIS expression under most conditions. This subject
has been discussed by Elson e t al. ~5 There can be excellent agreement between
theoretically predicted and experimentally measured angle-resolved scattering, as
shown in Figs. 5(a) and 5(b) for scattering from a multilayer dielectric-coated
surface ~. However, there are still unexplained differences between theory and
experiment for retroscattering at large angles of incidence and scaling of near-angle
scattering to IR wavelengths 13'16. A refinement of the vector theory allows the
optical constants to depend on the position in the plane of the surface 17. This helps
to explain large'-angle retroscattering discrepancies, but still does not predict cross-
polarized scattering (s-(p-) polarized incident light produces small amounts of
p- (s-) polarized scattered light, while all first-order theories predict none).
Since the scattering per unit solid angle is greatest for angles close to the
specular direction, it is reasonable to assume that most of the accumulated scattered
light also occurs at very small scattering angles. This is not true for conventionally
polished surfaces, as is shown in Fig. 6. Even though the scattering per unit solid
angle is less at angles in the middle range (10°-60°), the increase in the total solid
angle dominates, so that the total cumulative scattering is more than that at smaller
angles. In the particular case shown in Fig. 6, 72% of the total scattered light occurs
in this middle range. Diamond-turned surfaces and polished molybdenum surfaces,
which have a well-defined surface texture caused by the polycrystalline nature of the
material, have long surface spatial wavelength components on the surface that give
rise to large amounts of near-angle scattering. In some cases, as much as 85% of the
total scattered light can occur at angles between 0.3 ° and 3 ° from, the specular
direction ~8. ~9.
32 J.M. BENNETT
l l l | l l l l l l l l l l l l l
-3 #t
/I
%
~-E
q
-6
f
i i l l l l l l i l l l l i i l l
-80 -~ 40 -20 0 20 ~ 60 80
(a) 6, DEGREES
I I I I I I I I I I I I I I I I I
-3
~---4
II ~!
II ~
eL
%
~..... ~
ff
q
-6
t'
-7 t I I t I I I I I 1 I I I I I I !
-80 -60 --40 -20 0 20 40 60 80
(b) e, DEGREES
Fig. 5. Calculated (- - -) (uncorrelated roughness between layers) and experimental ( ) carves for the
angle-resolved scattering from a multilayer dielectric stack (angle of incidence, 30 °) (from ref. 5): (a)
p-polarized incident and scattered light; (b) s-polarized incident and scattered light'.
3. SURFACE MICROSTRUCTURE
Since scattering from high quality surfaces is to a large extent produced by the
microroughness of the substrate and/or films, it is necessary to characterize this
roughness statistically.The important parameters are the r,m.s, heights of the
SCATTERING AND ABSORPTION LOSSES AT INTERFACES AND IN FILMS 33
2.0 I I ; ; t I '; ,I i
.I -__
2
z_
i - _
71 _8 %
_ ~ , II "10-60°" " "-
(J
_,- , .+-, , , ,
00" 10 20 30 40 50 60 70 80 90
SCATTERING ANGLE (DEGREES FROM SPECULAR)
Fig. 6. Cumulative scattering from aluminized fused quartz (normal incidence) (from ref. 12).
surface microirregularities and their correlation lengths. Both these parameters are
incorporated into the autocovariance function t 1.2o. For both the scalar and vector
scattering theories, the r.m.s, heights of the microirregularities are assumed to be
small compared with the wavelength, and their correlation or autocovariance
lengths are assumed to be equal to or longer than the wavelength is. Three different
types of technique are available for different correlation lengths.
For predicting extreme-UV and UV scattering, the lateral resolution obtain-
able in electron micrographs is appropriate. Recently, a technique has been
developed 16 for obtaining micrographs of silver films without the need for a surface
replica, using a new versatile electron microscope at the University of Southern
California. Figure 7 shows scanning electron micrographs of the surfaces of several
sputtered silver films taken with this instrument. The internal structure of parts of
these same films non-destructively removed from the substrates is shown in Fig. 8.
Using a technique developed by Rasigni e t al. 21 at the Universit~ Aix-Marseille III,
Marseille, France, it is now possible to obtain autocovariance functions for film and
substrate surfaces from electron micrographs using microdensitometer scans of the
micrographs. One such autocovariance function is shown in Fig. 9.
For predicting scattering in the visible region, the lateral resolution should be
equal to the wavelength of the light used for the measurements, or approximately
0.5 lam. This resolution can be obtained using a profiling instrument with a diamond
stylus of radius 4 ttm or less. A computer-controlled surface profiling instrument
based on the Talystep is one possibility, and autocovariance functions measured
with this instrument are shown in ref. 20. Interferometric profiling instruments
generally have lateral resolutions of 1-2 ~tm or greater and, thus, cannot give
information about angular scattering for angles larger than about 18° (wavelength,
6328 A; normal incidence; lateral resolution, 2 ttm) 2°.
Near-angle scattering in the visible and IR regions at all angles can be
calculated from autocovariance functions measured with interferometric profiling
instruments such as the Mireau heterodyne interferometer (manufactured by Wyko
Optical Inc., 655 North Alvernon Way, Suite 123, Tucson, AZ 85711, U.S.A.), an
4~
Z
Z
Z
©
CJo
,...]
>
Z
! !
(a) (b) (c) (d) (e) 0.5
Fig. 8. Transmission electronmicrographs showing the internalmicrostructureof the same sputteredfilmsas in Fig. 7:(a)unbaked;(b)50°C;(c)100°C;(d) 200°C;
(e)250 °C. The filmshave been removed non-destructivelyfrom the substrates(from ref.16).
L~
36 J. M. BENNETT
(a)
(b) I I
s00o
0.5
(¢) ~ ~Ios
Fig. 9. (b) Surface topography and (c) autocovariance function (r.m.s. roughness, 37 ~; autocovarianc¢
length, 317 A) for an evaporated silver film obtained from microdensitometerscans of (a) a transmission
electron micrograph single-stagereplica of the surface(fromref. 16).
STYLUS (4~-10~m)
PROFILOMETER
* DEPENDS ON TYPE
OF INSTRUMENT
INTERFERO - | (10- 2500~1
METER
OPTICAL (4 -- 1000~)
HETERODYNE I
PROFILOMETER
MIREAU (4-3ooo
HETERODYNE I
INTERFEROMETER
( 5 - 350~ rms)
TOTAL I (100~-- HEIGHTS
INTEGRATED L 0.6tJm rms) ". ,I UNRESOLVED
SCATTERING
I I I I I I
10 100 I000~ 1 10ran
0.1 1 10 100 1000pro
SPATIAL WAVELENGTHS
Fig. 10. Surface spatial wavelength ranges of instruments and techniques for measuring surlacc
microroughness. Values in parentheses are the range of heights that can be measured with each
instrument or technique.
TABLE I
SUMMARYOF ROUGHNESSMEASUREMENTSON BALZERSROUGHNESSSTANDARDS(FROM REF. 23)
there is no one "r.m.s. roughness" (or autocovariance length) for each surface. In ref.
23 the reasons for the differences in roughness values are discussed.
4. ABSORPTION
20
18
16
~o 14
X 12
z lO
O
0 I I I I I I I
0 0.1 0.2 0.3 0.4 0.5 0.6 0.7
THICKNESS, /am
Fig. 11. Absorptance of a sodium fluoride film on calcium fluoride (AC-107, S-19) measured by the
wedged-film calorimetric technique (from ref. 25): ~7, 2.87 pro, 14 crn- t; ©, 2.72 ~ a , 3.5 c m - t.
eoI
5.5
5.0
4.5 I
4"0 I
X 3.5
Z 3.0
~2.5
~2.0
<
1.5
1.0 ~
0.5
0.0 I I I I I
0.0 0.4 0.8 1.2 1.6 2.0 2.4
SAMPLE THICKNESS (cm)
Fig. 12. Absorptanceofprism-shaped samplesoffusion-cast calcium fluoride measured byacalorimetdc
technique (from ref. 27): I-q, 2.87 pm, ct = 1.93 x 1 0 - , crn - 1; C), 2.705 p.m, ~t = 1.41 x 10-4 era- z.
internal reflections (Fig. 13). The sensitivity of the method depends on the state of
polarization (s or p), the angle of incidence, the refractive indices of the film and
prism, and the number of reflectiojns 2s. If a contamination layer is present in a
multilayer stack, it can usually be detected by profiling Auger, ESCA or SIMS
measurements. A peak in the carbon spectrum will occur in the profiling sequence to
show the presence of the contamination layer.
Photoacoustic spectroscopy is a specialized technique for detecting small
40 J. M. BENNETT
amounts of absorption in thin films as a function of position on the film 29. It has
been used to pinpoint locations on a film which are likely to be damaged when the
sample is irradiated with an intense laser beam, as shown in Fig. 14. Many of the
locations show no visible defects before exposure to the laser beam.
i i 1 i i i i i i i
100
I-
z
uJ
80
cc
u.I
n.
6O -OH?
U
Z ' -OH
<
E 40 -OH
' ~ "
Z
< 2O : /
n,,
I ! I
2.5 3 4 5 6 7 8 9 10 12 15 20
WAVELENGTH (MICRONS)
(S-POk)
Y
Fig. 13. I n t e r n a l reflection spectroscopy m e a s u r e m e n t s of the a b s o r p t i o n in a silicon m o n o x i d e film
(angle of incidence, 30 °) (from ref. 28): , s p o l a r i z e d ; - - -, p polarized.
A nuclear resonance method has been used by Donovan et al. a° to detect water
vapor in the form of hydrogen in a film or at the film-substrate interface. A nuclear
reaction between 19F and hydrogen yields 4He and ~ rays which can be detected
with a scintillation counter. The energy of the incoming fluorine atoms is uniformly
varied to change the penetration depth into the material so that the location of the
hydrogen atoms can be determined.
Allen et al. 31 have developed a new technique for detecting adsorbed gases or
liquids on a surface by exposing it to increasingly intense pulses of laser radiation.
The laser beam heats the surface, allowing materials to desorb and be detected in a
mass analyzer. Figure 15 shows data from such a desorption experiment.
One of the most important factors in obtaining high quality, low absorption,
defect-free films is a clean surface. It is very difficult to see particulate matter on the
surface of transparent substrates before they are coated, and it is also difficult to see
defects in transparent films. Temple 32 has developed a sensitive method for
observing the surfaces of transparent materials by total internal reflection micros-
copy (TIRM). Figure 16 shows how defects in a transparent SiO~ film are made
visible by this technique when they do not show under Nomarski illumination.
SCATTERING AND ABSORPTION LOSSES AT INTERFACES AND IN FILMS 41
~"UNDAMAGED SCRATCH
SUBSEQUENT LASER
DAMAGE
Z
t/)
_u $ Se •
8,<
O o| •
I-
O FILM
[ ABSORPTION
o.o13 _t_
l-
UNIDENTIFIED
ANt)
~T
uJ UNDAMAGED
GC
THIN FILM _, S U B S T R A T E
i-- -j - mI
o 7.5 13.0
POSITION (mm)
Fig.14. Photoacoustic spectroscopy measurements of thin film absorbing defects that were subsequently
damaged in a C O t laser beam (from ref. 29). The conclusions were as follows: all sites which were later
damaged were detected by photoacoustic spectroscopy; not all photoacoustic spectroscopy sites were
damaged, there was a poor correlation between the peak height and the damage level; not all
photoacoustic spectroscopy sites were identifiable using a microscope.
I ! i
l/1 MINIMUM
D A M A G E L E V E L "-D"
~6
I ¢qM
i
i
.J
¢.1
m
I 111 D A M A G E ~
~4 r THRESHOLD~ uu
Z
es
LU 2OO •
Z t~
gl
Z
O0
~2 DATA AVERAGED
OVER 4 SITES 10o
:S
0 i I I I I J I I 0
o ; 2 4 5 e
SHOT NUMBER
Fig. 15. Laser-stimulated desorption of water from calcium fluoride at 2.7 p m (data averaged over four
sites) (from ref. 31): - - -, energy density (each shot); - - , cumulative water signal.
42 J.M. BENNETT
5. CONCLUSIONS
I n c o n c l u s i o n , we h a v e d i s c u s s e d s c a t t e r i n g a n d a b s o r p t i o n in t h i n films a n d
s u b s t r a t e s a n d h a v e also d e s c r i b e d t e c h n i q u e s for m e a s u r i n g statistical p r o p e r t i e s o f
s u r f a c e s in o r d e r to p r e d i c t scattering.
REFERENCES
APPENDIX A
The equation for the differential power scattered per unit solid angle as a
function of optical and surface parameters is as follows AI.
ldP 16re2 | /32/ Zo 2 ,~ )
/~ ~ = - ~ c ° s 0 ° c ° s 2 0 - ~iq'--~qel2 ~ Iq 12 g(k-k°)
where P0 is the incident power, dP/df2 is the power scattered per solid angle, 00 is the
angle of incidence, 0 is the scattering angle, 8 is the dielectric constant of the surface
(~ --- N 2 where N = n - i k is the complex refractive index), g ( k - ko) is the surface
power spectral density function, k o and k are the incident and scattered wave vectors
given by
2~
ko = -~- sin 0o
44 J.M. BENNETT
2~
k = - f sin 0
and
2n
qo =-~-cOS0o
2~
q =-~--COS0
q' = e - k2~
qo' = e - ko2~
2n ~
~qo' sin tp cos 4' (2n/2) cos ~bsin ~b']
Z* =--2-(" -qo'
- ' - +qo
'--~ qo' +qo
For scattering in the plane of incidence the general equations become
(q' qo'-- kko) cos 4'
Zo = qo' + qo e