Thin Solid Films, 100(1983) 155-167 ELECTRONICSAND OPTICS

155

A M E T H O D FOR T H E D E T E R M I N A T I O N OF THE C O M P L E X R E F R A C T I V E I N D E X OF N O N - M E T A L L I C T H I N F I L M S U S I N G P H O T O M E T R I C M E A S U R E M E N T S AT N O R M A L I N C I D E N C E

J. I. CISNEROS,G. B. REGO, M. TOMYIAMA,S. BILAC,J. M. GON~'ALVES,A. E. RODRIGUEZ* AND Z. P. ARGOELLO

Departamento de Fisica do Estado S~'~lido e Cidncia dos Materiais, lnstituto de Fisica, Unit;ersidade Estadual de Campinas, 13.100 Campinas, Sdo Paolo ( Bracil)

(Received March 29, 1982: accepted September 13, 1982) A method is proposed for the determination of the complex refractive index of non-metallic thin films using photometric measurements at normal incidence over an extended wavelength interval. A necessary condition for the applicability of the method is the existence of maxima and minima in the reflectance due to interference effects. The problem of multiple solutions is analysed and the optical thicknesses at the extrema are used for choosing the correct solutions. For absorbing films two alternative procedures are described. One procedure requires an approximate value of the film thickness to start with and refines it during the calculation. The other procedure does not depend on a previous knowledge of the thickness but gives it as a result together with n(2) and k(2). A separate procedure is proposed for transparent and almost transparent films. An application of the method is carried out in which excellent agreement is obtained between calculated and experimental results.

1. INTRODUCTION Several methods have been developed for the determination of the complex refractive index N = n + i k of a thin absorbing film deposited onto a transparent substrate ~, 2 using reflection and transmission measurements. Some researchers 3 7 have proposed the determination of N and the film thickness h using experimental values of the transmittance T a n d the reflectances R and R' (measured from the film and substrate sides respectively) at normal incidence. However, the application of this type of calculation usually leads to multiple solutions 8 ~l, i.e. several pairs of values (n, k) can be found for each set of experimental results T, R and R'. It is necessary then to apply an efficient criterion in order to identify the correct solution ~2,13 This problem cannot be considered "as completely solved to date. As has been pointed out by Carey e t al. 14 some computer programs used to calculate N from photometric data can produce wrong solutions if the initial values are not properly chosen. A detailed analysis of the properties of the reflectance and transmittance of * Permanent address: Instituto de Fisica, Universidad de La Plata, La Plata, Argentina. 0040-6090/83/0000-0000/$03.00 Elsevier Sequoia/Printed in The Netherlands

156

J.i. CISNEROSet al.

absorbing and transparent films has permitted us to conclude that the optical thicknesses at the extrema in the reflectance of non-metallic thin films can be used to remove the indeterminacy b r o u g h t about by the existence of multiple solutions in a simple and straightforward way. The m e t h o d proposed in this paper permits the calculation of n(2) and k(,;.), and in most cases the thickness h, using as initial data experimental curves of the reflectance and transmittance over a range of wavelengths. In Sections 2 and 3 we review some basic results in order to define the nomenclature; Section 4 is devoted to analysis of the problem, and the method we are proposing is described in Section 5 and applied to an actual experimental situation in Section 6.
2. BASIC FORMULAE AND CONVENTIONS

The formulae to be used in the calculations correspond to the reflectances and transmittance of a plane-parallel absorbing film b o u n d e d by two transparent semiinfinite media ~5:
R = rlz-r32exp(i2fl)

{1)

1 - r 12r32 exp(i2fl)
R'= r-32--rlaexp(i2fl) 1 - r3z q 2 exp(i2fi) T = n~ t32tlzexp(ifl)

(2)

t3)

n3 1 -- r32r 12 exp(i2fl)

The indices 1, 2 and 3 correspond to air, film and substrate respectively; ri,i and tii are the Fresnel coefficients, which for normal incidence are 2N~
tii Ni + Nj

(4) (5)

N i -- N j rij - N i -k N j

Further, if we write N e = n + ik with n and k real functions of)., the complex angle fl is given by
fl-2nhN ;[ -2r~hn .2~hk /~ -I-I V {6)

where 2 is the v a c u u m wavelength of the incident radiation. The refractive indices N~ = nl and N3 = na are real since the surrounding media are supposedly transparent; n3 is assumed to be a k n o w n function of the wavelength. In the different steps of the calculations T, R and R' are considered as functions of either the quantities (nl, n3, h, n, k, )4) or the quantities (nL, n3, d, n, k, 2). In the second set the optical thickness d = nh is used instead of h. The measured values of the transmittance and reflectance include naturally the effect of the (thick) substrate. In order to obtain the corresponding values of R, R'

DETERMINATION OF THE REFRACTIVE INDEX OF N O N - M E T A L L I C FILMS

157

and T we used the following f o r m u l a e based on the t r e a t m e n t given by Knittl 16 but with the n o t a t i o n established in Fig. 1 :
R' Rs-p

(7) R~)

1-p(2-

T-

0 -p)Ts
1 -- p ( 2 - - ns)
pT 2

(8)
(9)

R = Rt

l -pR'

w h e r e p = ]r13] 2.
Air nI Film n*ik Substrate n~ Air nI

-/

\\ \,

TS ~ c - -

~/~

\"

~ ~s

Fig. 1. Conventions adopted for the measurements of the reflectances Rf and R~ and the transmittance 7~ = T~of a thin film deposited onto a transparent substrate of finite thickness.

3. SOME PROPERTIES OF T R A N S P A R E N T AND ABSORBING FILMS I n t r o d u c i n g the a b s o r p t a n c e A = 1 - R - T t h e film is classified as t r a n s p a r e n t , a l m o s t t r a n s p a r e n t o r a b s o r b i n g respectively when A vanishes, is very small or is not very small c o m p a r e d with unity. F o r the ideal case of a film of thickness h m a d e with a t r a n s p a r e n t a n d n o n - d i s p e r s i v e m a t e r i a l (k = 0, n constant), the reflectances R and R' are identical a n d the wavelengths c o r r e s p o n d i n g to their e x t r e m a ( m a x i m a and m i n i m a ) satisfy the c o n d i t i o n 4rid

).m

-- mn

(10)

where m = 1, 2, 3 . . . . is the o r d e r n u m b e r a n d 2m is the wavelength c o r r e s p o n d i n g to the e x t r e m u m of o r d e r m. F i g u r e 2 shows the reflectance a n d t r a n s m i t t a n c e c a l c u l a t e d for a p a r t i c u l a r film of this kind. The values of the e x t r e m a of the reflectance, which d e p e n d neither on the wavelength n o r on the film thickness, are
= (|--n3"] R .... 2

\1 +n3f
= (n3--r/2~ 2

(l la)

Rod. \n-~--~!

(1 lb)

158

J . I . CISNEROS et

aL

where "even" and "odd" refer to the order numbers and n I was put equal to unity. We see that R .... coincides with the reflectance of the air-substrate interface independently of the values of n and h. For transparent but dispersive films eqn. (10) is exact for even order numbers but only approximate for odd numbers. (This can be readily seen by solving dR/d2 = 0 with n = n()~) and k = 0.) Consequently the optical thicknesses determined using that equation are more accurate at the even-order extrema. Considering the more general case of an absorbing and dispersive film in which both n and k are functions of the wavelength, the following effects are observed: R and R' no longer coincide and their representative curves differ from the typical shape of Fig. 2, the extrema being shifted from the positions predicted by eqn. (10), and in some extreme cases, i.e. strong absorption or very thick film, the maxima and minima disappear.
R,T! 06 290

R,T r

0.8 ~
j
0.6-

/rli
/

i I
I I
# I

49s

/
\ /

\
\ /

04 ~V ~ i
02 ~
O0 L I 8 2 3 4

02

/
/

kl~m)

),Auml

Fig. 2. Reflectance ( - - - ) and t r a n s m i t t a n c e ( - - ) as functions of wavelength for an ideally t r a n s p a r e n t and non-dispersive film d e p o s i t e d o n t o a t r a n s p a r e n t and non-dispersive s u b s t r a t e (n - 3.0; k = 0; n~ = 1.5; h = 1.0 ~tm). O r d e r n u m b e r s are indicated at the extrema. Fig. 3. Reflectance ( - - ) and t r a n s m i t t a n c e ( - - - - - ) of an a b s o r b i n g film calculated with nl,;D = 4.0 - 0 . 2 ( 2 - 2 . 0 ) , k ( 2 ) = 0 . 6 - 0 . 2 ( 2 - 2 . 0 ) and the following p a r a m e t e r s : n~ = 1.0; n 3 - 1.5: h = 1.0~tm. Values of 4d/). are indicated at the e x t r e m a in R, s h o w i n g that eqn. (10) is a p p r o x i m a t e l y satislied.

However, in many experimental situations, even in cases with appreciable absorption, the reflectance presents maxima and minima in a sequence similar to that observed in non-dispersive and non-absorbing films, as can be seen in Fig. 3. In these cases eqn. (10) is approximately satisfied at each extremum, allowing us to attribute order numbers to all of them. 4.
MULTIPLE SOLUTIONS

The reflectance and transmittance given by eqns. (1) and (3), for fixed values of nl, n3, h and )~, define two functions of n and k which when equated to the experimental values Rex p and Texp respectively give two curves in the (n, k) plane. These curves usually intersect in several points as can be seen in Fig. 4, which was calculated using Rexp and T~xp measured at one of the extrema in the reflectance of

DETERMINATION OF THE REFRACTIVE INDEX OF N O N - M E T A L L I C FILMS

159

the film used in Section 6 to illustrate the application of the method. Each intersection corresponds to a possible solution 8'9' 17 but further information is necessary to identify the correct solution. The measurement of R' may be considered in order to solve the problem, but this works only in some cases. In fact, for transparent films R' = R and no new information is added. It can be shown that even in absorbing films the knowledge of R' may prove useless for the selection of the correct solution. However, if the optical thickness d of the film can be determined and h is known we shall be able to calculate an approximate value ofn and then to choose the correct solution as that which best agrees with this value. When h is not known a priori the knowledge of the optical thickness is also useful. Fixing ns, n3, d and 2, in eqns. (1) and (3) we obtain two functions o f n and k which when equated to the experimental values Rexp and Texprespectively define two curves. Figure 5 shows two examples of this new type of curve computed for a m a x i m u m and a minimum in the reflectance of the film used in Section 6. We observe that by fixing the optical thickness we keep constant the real part of fl which is the main cause for the modulations in Fig. 4. Thus the new curves are quite different from those in Fig. 4, giving in general only two intersections. Figure 5(a) and Fig. 5(b) respectively are typical examples for odd- and even-order extrema in the reflectance of moderately absorbing films. For transparent films we find that curves computed at the odd-order extrema still look like those shown in Fig. 5(a) but those calculated for even orders both

k 08
2

06

(a)
04

0.2

/ ./I1

/ I ,

(b)
8

I 4. n

I 6

Fig. 4. C u r v e s for R(n,k)h ........ = Re,i, ( - - ) (eqn. (18a)) and T(n,k)h ........ = Texp(--.--) (eqn. (18b)) c a l c u l a t e d at the e x t r e m u m 23 = 1.301am, (m = 3, m a x i m u m ) with h = 0.225p-m. The multiple intersections give several pairs of s o l u t i o n s (n, k) c o m p a t i b l e with Rex o and T~xp. Fig. 5. C u r v e s for R(n,k)n ........ = Rex p ( ) (eqn. (15a)) and T(n,k)a ........ = To,p ( - - . - - ) (eqn. (15b)) c o m p u t e d at two consecutive e x t r e m a : (a) m = 3 ( m a x i m u m ) , ) . 3 = 1.30/am, d = 0.958 I.tm; (b) m = 4 (minimum), 24 = 0.99 p-m, d = 0.973 p-m. The two intersections give the following results: n 3' = 0.31 (h a' = 3.05 p-m), k 3' = 0.018, n3" = 4.26 (ha" = 0.224 p-m), k3" = 0.321; n 4' = 0.15 (h 4' = 6.43 p-m), k,,' = 0.009, n4" = 4.16 (h,," = 0.230 p_m), k,," = 0.485.

160

J.I. C1SNEROSel a].

coincide with the straight line k = 0. We arrive at the same result by analysing eqns. (ll), which indicate that each value of Roda has only two positive values of n associated with it while R .... may be associated with any value ofn. The criteria used to choose the correct solution depend on whether the film is absorbing or transparent and will be discussed in Section 5.
5. DESCRIPTION OF THE METHOD

5.1. Calculation of the optical thicknesses Assuming small variations in the optical thickness from one extremum to the nearest neighbours, we have
dm 1 ~ d " ~d,.+x
or

(m--1)2m 1 ~ m 2 , . ~ (m+l).,tm+ 1 Consequently the following alternative formulae for m are obtained: m~ m~ m~

(12)

)~m 1--2,.
'~m+ l

(13a) (13b) (13c)

2m--2"+ 1 2,. 1+2"+1

2,. 1--2,.+l

Using the approximate values given by eqns. (13) and the fact that the orders of the maxima and minima have definite and opposite parities (for transparent films odd integers correspond to maxima when Rma x > R~ub~ and to minima when Rmi n < Rsubs ; the same rule also holds for moderately absorbing films) we can choose the correct integer values of m. It is now possible to calculate, to a first approximation, the optical thicknesses at the extrema:

d,. (1) = m2.,/4

(14)

5.2. Absorbingfilms 5.2.1. Procedure A In this procedure the film thickness is initially unknown and is computed together with n and k. For each extremum in the reflectance at wavelength 2,. and optical thickness d,, ~11,approximate values n,, I1) and k,, I1) are calculated as solutions of the following coupled equations: R(nl,n3, d,n,k, .'~)-- Rexp(2 ) = 0 T(nx,n3, d,n,k, 2) - Texp()o = 0 )
(15a) (15b)

The solutions of eqns. (15) can be found numerically or graphically from the intersection of the two curves given by eqns. (15a) and (15b) plotted in the (n, k) plane.

DETERMINATION OF THE REFRACTIVE INDEX OF N O N - M E T A L L I C FILMS

161

As was mentioned in Section 4, there are in general two intersections. In order to decide which solution is the correct one we must use one of the following alternative criteria. (a) We call (n,,', k,,') and (n,,", k,,") the two solutions for the mth order extremum, with n,,' < n,,". We then calculate the two sets of thicknesses h,,' = d,,(1)/ n,.' and h,," = d,,(1)/n,, '' and their mean square deviations. The set with the smaller dispersion must correspond to the correct set of solutions, because it should give for very precise m e a s u r e m e n t s the true h for all 2,. values. This is clearly shown iv. Fig. 5 for two consecutive extrema. (b) If R'~x p is available we take as the correct solution that for which the calculated R' best agrees with the measured value. (c) We choose the solution which is nearest to an a p p r o x i m a t e value of n such as the bulk value or a value obtained by introducing a rough estimate of h in eqn. (17). Once the correct solutions (n,, (~), k,, (1)) have been chosen we determine the set h,, ~1~, the average h (L~ of which is taken as the first a p p r o x i m a t i o n to the film thickness. The next step is the correction of the dr, (1~obtained initially. For this purpose we need the values o f n and k in the n e i g h b o u r h o o d of the extrema. We plot two curves, n versus 2 and k versus 2, with the n,, (~) and k,, (1' already determined plus additional values if necessary, obtained by solving eqns. (l 5) for selected wavelengths 2j with j = 1,2,3 .... and interpolated optical thickness dj (~) The functions represented by these curves will be called nIle(2) and k(l~(2). Calculating the reflectance as a function of h (1~, n(~)(2), k(~(2) and 2 in a n e i g h b o u r h o o d of each e x t r e m u m of order m we obtain curves with extrema at ).,,~) usually different from 2,,. Whenever a difference between these two wavelengths is found, changes in the thicknesses h,, ") are introduced in order to shift the e x t r e m u m of the calculated curve until it occurs at 2 = )~,, for each m separately. (This is equivalent to the use of the condition dR/'d2 = 0 at the extrema in R.) If hm (l~* denotes the value corresponding to this condition, the improved optical thicknesses
are

d,, 2) = nl)(2m)h,, 1~*

(16)

We now iterate the whole procedure, using this time the values d,. (2) in place of d,, lj. A n u m b e r of iterations is performed in order to improve the agreement between the calculated and experimental values of R and Tuntil the differences between ),s) and 2,,, for all m, become less than a predetermined value, Let the f t h iteration be the last; then the final results will be h (f), n,, f) and k,, ~f) obtained from eqns. (15) at the extrema, plus n (I) and k I~ for 2 )~,,, obtained also from the same equations while using optical thicknesses dj (f) determined by interpolation or extrapolation from the dr, ~I). 5.2.2. P r o c e d u r e B Besides the reflectances R and R' and the transmittance T, we use in this procedure an a p p r o x i m a t e value happr of the film thickness, determined by an independent measurement. Dividing the optical thicknesses d,, (~ by this value we obtain
nm appr =

dmll)/happr

(17)

162

J. i, CISNEROSet al.

(We note that if an approximate value of n is available, e.g. its bulk value, we may also apply this procedure when R, R' and T are measured for only a few discrete wavelengths.) We have to solve the following system of equations:

R ( n l , n 3 , n , k , h , 2)-Rexp().) = 0
T ( / I I , n 3 , n, k , h, A) Texp()~ ) = 0

(18a) (1 8b)

for all 2,. and for h in the n e i g h b o u r h o o d of h,rpr. We keep the solution which has n nearest to n m appr" Because of experimental errors we require only that eqns. (18) be approximately satisfied. Several researchers 8'9' ~s have proposed to determine n and k by using numerical methods to minimize some convenient function of Ie~a~ - R~pl and IT ~ r~pl. The procedure that we adopted consists in finding n and k which minimize IR~al~-R~vl while at the same time satisfying eqn. (18b). For several n values in a n e i g h b o u r h o o d of nmappr we obtain the corresponding k(n) by solving eqn. (18b). These values enable us to calculate R as a function of n which is then c o m p a r e d with Rex p in order to find the m i n i m u m in IR~.,~- Rexpl. This is illustrated in Fig. 6. For curves a and b we find only one value ofn and an associated value of k; for curve c we have two solutions and we choose that for which R ' ~ is closest t o R ' e x p. ,. The solutions found in this way depend on h and for this reason will be called nm(h) and kin(h). In order to use the measured values of R' for improving h, n and k, we define
-

A(h) = ~ lR'.,(h)- R'., ox~l

rn

(~ 9)

where R'm(h) is calculated with h. n.,(h) and kin(h).

r

019

Rex~ O.18
I

2.9

3 0 n

3.1

Fig. 6. M i n i m i z a t i o n o f IRc,]~-R~xpl in p r o c e d u r e B. T h e f u n c t i o n R(n) is p l o t t e d for t h r e e v a l u e s of h c o r r e s p o n d i n g to t h e t h r e e p o s s i b l e c a s e s a n a l y s e d in t h e text: c u r v e a, h - 0.99; c u r v e b, h - 0.9989; c u r v e e, h = 1.01. Rexp ( - - ) a n d Texv c o r r e s p o n d to a n ideal film w i t h n = 3.0, k = 0.2, h - 1.0 p,m, ,;. - 2.0 p m , n~ - 1 . 0 a n d n.~ = 1.5.

DETERMINATION

OF THE REFRACTIVE

INDEX OF

NON-METALLICF I L M S

163

Repeating the calculation for different values of h and plotting A(h) we take as the final film thickness the value he for which A is a minimum. In the case of ideally precise measurements of a perfect film we should have Amen = 0, but when using actual measurements on real films we usually obtain Ami n ~ 0 because of experimental errors and possible film inhomogeneities and imperfections. We finally repeat the calculation using h = hr. The corresponding results n,,(hr) and k,,(hf) give the best agreement with the experimental measurements at the extrema. In order to determine n(Z) and k(2) for ). 2=, the calculation described to obtain n,,(h) and k,,(h) is performed using hf, the experimental values corresponding to 2 and as approximate values o f n the n,, appr for the nearest ,;,,,.

5.3. Transparent and almost transparent.films

The procedures proposed in Section 5.2 are not completely applicable to transparent films: procedure A can only be performed at the odd-order extrema and procedure B cannot be applied at all because R and R' are equal. When there is experimental evidence that the film is transparent, i.e. when R + T = 1 or R .... is equal to the reflectance Rsubs of the air-substrate interface, we simply solve eqn. (! lb). The two positive roots are

n'

~n3(l-Rad1/2)~1/2
-j

12Oa)
(20b)

n" = n3/n'

It should be noted that eqns. (20) are strictly valid only for a dispersion-free film and substrate but actual deviations are very small. In order to choose the correct solution we m a y use one of the following criteria. (a) W h e n the optical thicknesses at the extrema have been determined, a rather crude value of h m a y be sufficient for choosing the correct n. It is clear that a better value o f h is obtained from the optical thickness and the calculated n. (b) An approximate value of n can be used, such as that for the bulk material. F o r films of mixed composition we can sometimes use an average of the indices of the components. (c) T w o films of the same material deposited onto different substrates can be used. Writing the index of the second substrate as ~3, with ~' and if' the ~ corresponding roots, we m a y write according to eqn. (20b)
n t n r' ~ n3

if'if" = if3

(21 )

As the true solutions must evidently coincide, we conclude that the wrong solutions for r~3 and n3 must yield a ratio ff3/n3 which may be chosen to be appreciably different from unity. (d) If we find n' < 1 and n" > n3, we can reasonably reject the first root as n is usually greater than unity for the frequencies used in optical work. O n l y a few values o f n can be determined in this way since eqn. (1 l b) requires m to be odd. If m o r e information is needed about n(2) the method indicated below for almost transparent films m a y be used.

164

J.i. CISNEROS

Ct {ll.

W h e n the film is not completely transparent, n and k can be determined by using a modified version of procedure A which takes into account the difficulties found in the case of transparent films. First we determine the optical thicknesses d,,, t~ at the even-order extrema using eqn. (10) and then at the odd-order extrema by interpolation. We execute procedure A normally for odd extrema and for intermediate values of 2. It should be noted that out of the three criteria given in Section 5.2.1 for choosing the correct solution, only (c) can safely be applied. In contrast, in almost transparent films dispersion is small and consequently the optical thickness given by eqn. (10) are rather precise, which means that the recommended iterations may prove unnecessary.
6. EXAMPLE

We describe in this section the application of the method, using procedure A, to a PbS film deposited onto a quartz substrate by standard chemical techniques. Procedure B gave the same results when applied to the same film. The experimental photometric curves are shown in Fig. 7. Using the ";-mof the extrema of R(),), we determined the order numbers m (Table I) and, using eqn. (10), the optical thicknesses d,, I1~ presented in Table II, together with n3(2,,), Rexp{).m) and

L,p(;.m)"
06

7 /

04 .o o~

f . ,~..
0.2

\k
k\
/

~ //
/
f

/ /"
/

/\\\
\
X
\.

/-1"

0 0.75

I
I00

]
125 '~ (tJm)

I
1.50

I
175

Fig. 7. CurvesforthereflectancesR( )andR'( - ) and the transmittance T( .. )ofaPbSfilm measured at normal incidence: 0, the corresponding values calculated at selected wavelengths, using the final results of Table IV. These values were then used to find n,, Ill and k,, ul by solving eqns. (15). We found it necessary to calculate n and k for a few more values of 2 in order to plot the approximate curves nH~(),) and k u)(),) used for correcting d,, t~ and thus obtaining d,, ~2~, and later, in a similar way, d,, ~3~. The calculation was iterated twice; as we found 2,, 131 = ),,, for all m, no further iteration was necessary. All the results are condensed in Table III.

DETERMINATION OF THE REFRACTIVE INDEX OF N O N - M E T A L L I C FILMS

165

TABLE I DETERMINATION OF THE ORDER NUMBERS 2,, (~tm) Cah'ulated order number Eqn. (13a) 0.81 0.99 1.30 1,9l 5.50 4.19 3.13 -Eqn. (13h) -4.50 3.19 2.13 Eqn. ( 13c j 5 4 3 2

4.31 3.15

T A B L E II OPTICAL THICKNESSES AND EXPERIMENTAL DATA

Am
0am) 0.81 0.99 1.30
a

dmtl)
(p.m) . 1.012 0.990 0.975

Rexp
0.435 0.299 0.564

T~.xp
0.033 0.134 0.175

tl3 a

1.453 1.450 1.447

Refractive index of q u a r t z t a k e n from a c a t a l o g furnished by Amersil Inc., Hillside, N J, U.S.A.

TABLE Ill RESULTS OF THE PERFORMED ITERATIONS )'m = 0.81 ton dm(l) (/am) d,, (2) (tam) d,, (3) (lam) h,, I1) (p.m) hm12) (~m) hm (3) (gm) n,, (1)
rt,n t2)

)~m = 0.99 itm 0.990 0.973 0.973 0.227 0.227 0.227 4.36 4.29 4.29 0.481 0.498 0.486

).,,, = 1.30 j~nl 0.975 0.949 0.953 0.231 0.222 0.224 4.24 4.27 4.27 0.316 0,325 0,321

n,,,TM k,, (1) km 12l km(3)

1.012 0.998 0.989 0.230 0.224 0.225 4.38 4.41 4.40 0.718 0.738 0.736

T A B L E IV FINAL VALUES OF r/ AND k CALCULATED FOR SEVERAL WAVELENGTHS 2 (tam) 0.75 0.81 0.90 0.99 1.15 1.30 1.50 1.70 n k

4.30 4.40 4.40 4.29 4,34 4.27 4.25 4.26

0.937 0.736 0.585 0.486 0.390 0.321 0.283 0.267

166

J. 1. CISNEROS '1 HI.

Additional points for nl3t().) and k31(2) were calculated using interpolated and extrapolated values of the optical thickness and eqn. (15). Table IV contains the final results. The final value h 3~ = 0.225 ~tm was obtained by averaging the h,,, ~~ values. As a check of these results, we used them to calculate R(2), R'(2) and T(,;.) and represented the results in Fig. 7 for comparison with the experimental values. Thc agreement is very good in all three curves, including R'().) which was not used in the calculations. We have not attempted here to evaluate the accuracy of the results as determined by the accuracy of the experimental values. They can, however, be estimated using for instance the method of Ward and Nag ~2. 7.
CONCLUDING REMARKS

The method proposed in this paper proved to be simple and efficient as can be seen in the example of Section 6. When using procedure A only two iterations were needed for achieving the desired accuracy, In the case of procedure B a good agreement between calculated and experimental values was also quickly attained. The calculations are simple enough to allow the use of a programmable desk {or even a pocket) calculator. For routine work a computer is recommended. It should be noted that procedure A can be performed either with the pair R, T as proposed or with R', 7". The combination R, R' may not be convenient because the curves R(n, k) = Rex p and R'(n, k) = R'ex p usually form small angles at their crossing points, thus introducing large errors in the determination of n and k, especially in almost transparent films. Furthermore, procedures A and B may also be combined in the following way: the first is used to obtain approximate values n,/! }, k,, ~1} and h~ which are then used to carry on the calculations applying procedure B.
ACKNOWLEDGMENTS

We acknowledge the financial support for this work by the Financiadora de Estudos e Projetos-lnstituto de Atividades Espaciais, Fundaqfio de Amparo t'~ Pesquisa do Estado de Silo Paulo, Conselho Nacional de Desenvolvimento Cientifico e Tecnol6gico and Banco Interamericano de Desenvolvimento. One of us (A.E.R.) also wishes to acknowledge financial support from the Argentine Consejo Nacional de Investigaciones Cientificas y Tecnol6gicas. We also wish to thank Drs. R. Luzzi and L. C. M. Miranda for fruitful discussions.
REFERENCES 1 O.S. Heavens, Phys. Thin Films, 2 (1964) 193 238. 2 F. Abeles, Phys. Thin Films, 6 (1971) 151--204.

3
4 5

6
7 8 9

D. Ma16, C.R. Acad. Sci.,230(1950) 1349. D. Mal6, Ann. Phys. (Paris), 9 (1954) 10. D. Mal6, J. Phys. (Paris), 25 (1964) 74. J.F. Hall, Jr.,andW. F.C. Ferguson, J. Opt. Soc. Am.,45(1955)714. A.M. Goodman, Appl. Opt., 17 (1978) 2779. P.O. Nilsson, Appl. Opt., 7 (1968) 435. F. Abel6s and L. M. Theyc, Sur[i Sci., 5 (1966) 325.

DETERMINA]'ION OF THE REFRACTIVE INDEX OF NON-METALLIC FILMS

167

10 11 12 13 14 15 16 17 18

R.E. Denton, R.D. CampbellandS. G. Tomlin, J. Phys. D, 5(1972) 852. L, Ward, A. NagandL. C.W. Dixon, J. Phys. D, 2(1969) 301. L, W a r d a n d A . Nag, J. Phys. D, 3(1970)462. R.K. Cook and R. W. Christy~ J. Appl. Phws., 51 (1980) 668. R. Carey, B. W. J. Thomas and D. M. Newman, Thin Solid Fibns, 66 ( [980) 139. M. Born and E. Wolf, Principles ~['Optics, Pergamon, New York, 5th edn., 1975, pp. 61 66,
628-632. Z. Knittl, Optics ~/'Thin Fihns, Wiley, New York, 1976, pp. 480 484. R.D. Bringans, J. Phys. D, lO (1977) 1855.

J.M. BennetandM. J. Booty, Appl. Opt.,5(1966)41.