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Aluminium Nitride Thin Films Deposited by DC Reactive Magnetron Sputtering
Aluminium Nitride Thin Films Deposited by DC Reactive Magnetron Sputtering
Aluminium Nitride Thin Films Deposited by DC Reactive Magnetron Sputtering
Pergamon
PII: S0042207X(98)00150X
Vacuum/volume 51/number 2/pages 161 to 164/1998 1998 Elsevier Science Ltd All rights reserved. Printed in Great Britain 0042207X/98 $19.00+.00
AlN-lms prepared by dc reactive magnetron sputtering. AlN in an Ar+N2 gas mixture have been prepared and their microstructure, hardness, refractive index and IR transmittance examined. At l = 640 nm the refractive index was 1.93 and k = 3103; high transmission occurred between [??] structure and oxygen on microhardness is discussed. 1998 Elsevier Science Ltd. All rights reserved
0[ Introduction The widespread technological application of nitride thin _lms is the reason for increasing interest in the investigation of these compounds[ In particular AlN is an attractive material because of its high melting point "1399>C#\ thermal conductivity "159 Wm0K0#\ extreme hardness "about 1092 kgf mm1#\ chemical and thermal stability\ and high electrical resistivity "r 0980900 Vm# et al[02 AlN is an interesting optical _lm material with a high refractive index "n 0[71[1#3 and low absorption "k092#4[ Its thin _lms are transparent in the visible\ infrared and ultra!violet regions with high optical transmission between 9[101[4 mm4[ It is also a promising material for optical applications in corrosive and high temperature environments5\6[ Aluminium nitride is not an easy material to study because its growth of good quality AlN thin _lms requires a high purity source and an oxygen!free environment\ because of the alu! minium reactivity[ The _lms have been deposited by several tech! niques] molecular beam epitaxy "MBE#7\8\ reactive sputtering2\09\00\ chemical vapour deposition "CVD#01\02 etc[ A most common deposition method is d[c[ reactive magnetron sput! tering\ because of its simplicity\ relatively low cost and the ability to obtain _lms of a good quality[ In this work polycrystalline AlN!_lms were deposited on glass\ monocrystal KCl and low carbon steel substrates by the d[c[ reactive magnetron sputtering[ The microstructure\ morphology\ microhardness\ refractive index and transmission in the IR region of the _lms were studied using TEM\ microhardness tester\ optical and IR transmission spectrophotometers respectively[
1[ Experimental details 1[0[ Thin _lm deposition[ AlN!_lms\ 215255 nm thick\ were deposited by d[c[ reactive magnetron sputtering of a water cooled aluminium target in a gas mixture of argon and nitrogen[ The diameter of aluminium target was 09 cm and the Al purity was 88\84)[ The vacuum chamber was evacuated to 67[093 Pa and high purity argon introduced up to 0[090 Pa[ The target was cleaned at 329 W for 04 minutes[ The vacuum chamber was then evacuated again and nitrogen "88[88)# was introduced with partial pressures of 0[4091 Pa "regime I# and 8092 Pa "regime II#[ Afterwards argon was continuously admitted in addition to the nitrogen until the total pressure "N1Ar# reached 2091 Pa "regime I# and 6091 Pa "regime II#[ Each regime was established for 04 minutes[ During deposition the total pres! sure and the d[c[ power were kept constant[ AlN!_lms were deposited on glass\ KCl and low carbon steel substrates\ because of the speci_c requirements of TEM\ IR spectral analysis and the possibility of various AlN applications[ The deposition times were 1 h "regime I# and 0[4 h "regime II#[ The substrate was unheated and its temperature depended on heating from the plasma[ The substrate to target distance was 029 mm[ 1[1[ Structure[ Structural details of the _lms were revealed by transmission electron microscopy "TEM#[ Films for these inves! tigations were deposited onto monocrystal KCl substrates for 09 minutes and afterwards detached dissolving the substrates in distilled water[ 1[2[ Microhardness[ Microhardness measurements were made with a PMT!2 tester equipped with a diamond Knoop pyramid[ By applying increasing loads to the indenter\ it was possible to gather information on layer hardness at increasing penetration
161
To whom all correspondence should be addressed[ $Paper presented at the 09th International School on Vacuum Electron and Ion technologies\ 1116 September 0886\ Varna\ Bulgaria[
V. Dimitrova et al.: Aluminium nitride thin lms deposited by DC reactive magnetron sputtering
depths[ Ten impressions were made at each load and the average microhardness values were taken[ The statistic error did not exceed 5)[ 1[3[ Optical properties[ The optical transmittance was measured as a function of the wavelength "9[29[7 mm# by a spec! trophotometer {Specord UV VIS|[ The refractive index n of the layers was determined from the interference maxima and minima in the visible spectral region of the transmittance spectra accord! ing to Swanepoel 03[ The region of high optical transmission and absorption IR band were studied by means of IR transmission spectroscopy using a spectrophotometer {Specord 64 IR|[
2[ Results and discussion 2[0[ Structure[ Figure 0 shows the microstructure of AlN _lms\ deposited on KCl substrates at a N1 pressure of 0[4091 Pa and total sputtering pressure of 2091 Pa "regime I#[ It can be seen that the _lms have a relatively smooth\ homogeneous\ uncracked surface and a uniform microstructure[ The TEM photograph picture\ taken normal to the _lm surface\ shows that the _lm surface is composed of crystals with a di}erent size and high density[ The polycrystalline hexagonal structure of all investigated AlN _lms was con_rmed by electron beam di}raction "EBD#[ Figure 1 shows the electron di}raction pattern of AlN _lms deposited at a nitrogen partial pressure of 8092 Pa and total sputtering pressure of 6091 Pa "regime II#[ In this EBD pattern the pres! ence of "009#\ "091#\ "991# and "099# rings can be seen clearly\ which indicates once again a polycrystalline structure of the _lms[ The presence of a weak a!Al1O2 ring is due to oxygen in the residual gas in the vacuum chamber[ On the EBD pattern many single re~ections can be seen\ which con_rm the results from TEM analysis[ The results from EBD and TEM analysis are in good agreement with the observations of other authors 00[ TEM photographs and EBD patterns clearly showed that all investigated AlN thin _lms had a microcrystalline structure "Fig! ures 0 and 1#[
Figure 1[ Electron di}raction pattern of AlN _lms deposited on KCl substrates at a nitrogen partial pressure of 8092 Pa and a total pressure of 6091 Pa[
2[1[ Microhardness depth pro_les of AIN thin _lms[ The variation of the measured composite hardness Hc of the investigated sam! ples "regime I# with the identation height\ i[e[ the penetration depth\ h\ is given in Figure 2[ The penetration depth is expressed by h d:29[41\ where d is the identation diagonal[ The micro! hardness of the low carbon steel substrate\ Hs\ was measured on an uncovered sample[ Its variation with h is also shown in the same _gure[ The results of this measurement show\ that the Hs vs[ h plot is typical for a system\ in which the layer is harder than the used substrate material[ As shown in Figure 2\ with the indenter tip approaching the interface both curves tend to con! verge and coincide beneath the interface Hc and Hs[ To separate the _lm hardness\ Hf\ from that of the composite Hc the model proposed by Jonson and Hogmark 04 for metallic bilayer and veri_ed by Navratil and Stejskalova 05 for semi! conductor bilayer systems is used[ The following expression for hard ductile _lms on softer substrates applies]
Figure 0[ TEM picture "magni_cation 4093# of a reactively dc mag! netron sputtered AlN thin _lm "N1 partial pressure of 0[4091 Pa and total pressure of 2091 Pa# taken normal to the _lm surface[ 162
Figure 2[ Microhardness Hk of an AlN thin _lm on a low carbon steel substrate as a function of the identation depth h[
V. Dimitrova et al.: Aluminium nitride thin lms deposited by DC reactive magnetron sputtering
Hf
Hs
HcHs t t 1C C1 h h
01
"0#
where C sin 061> 29?\ for hard ductile _lm and t is the layer thickness[ The calculated Hf values varying with h are given also in Figure 2[ The three curves from this _gure show an expected character of varying[ It is well known that the microhardness doesn|t depend on the load P used and penetration depth h respectively[ But in practice there is a load dependence particularly for small load "indentation!size e}ect#[ The experimental points were _tted with the function Hk Hkoexp "k:L#\ where Hk is the measured microhardness\ L is the load\ K is a constant for every speci_c sample and Hko is the load independent bulk microhardness[ The load independent micro! hardness of the low carbon steel substrate obtained here is 105[147 kg[mm1[ The so called bulk microhardness value of the AlN layer "255 nm# is about 634[277 kg[mm1[ This value is lower than the one measured for AlN monocrystalline thin _lms reported in the literature\ according to Refs[ 5\ 06 and 07\ the Knoop microhardness of AlN thin _lms is in the range 0199 0799 kg[mm1[ In our case the lower value of microhardness is normal for microcrystalline structure of the grown layers[ Ano! ther reason for the lower layer hardness could be the presence of a small oxygen amount "8)# in the _lms from the residual gas in the chamber[ 2[2[ Optical properties[ Figures 3 and 4 show an optical trans! mission spectrum T"l# of AlN _lms\ which are deposited at a nitrogen partial pressure of 8092 Pa and a total sputtering pressure of 6091 Pa "regime II#\ and the relationship between the calculated _lm refractive index and the wavelength of light n"l# respectively[ It can be seen in Figure 3\ that the interference maxima are not located very close to the uncoated substrate transmittance curve Ts"l# and this indicates\ that the _lms have
observable absorption[ In our case\ the average value of AlN transmission is about 79) at a glass substrate transmission 89)[ The refractive index n"l# was calculated using envelope curves of transmittance maxima and minima according to Swanepoel 03[ The results are shown in Figure 4[ At a wavelength of 539 nm the _lm refractive index n was found to be 0[82[ The extinction coe.cient for these _lms in the visible range is k 2092 at l 539 nm[ The _lm thickness obtained by Swanepoel|s method is 215 nm[ These results are in accordance with the ones reported for a refractive index and coe.cient of extinction of poly! crystalline AlN _lms 0\3 and con_rm the possibility for the depo! sition of AlN thin _lms with the expected optical properties by dc reactive magnetron sputtering[ An infrared transmission spectrum of AlN _lms grown on KCl substrates "regime II# is shown in Figure 5[ This spectrum displays the strong absorption band at 569 cm0[ The deposited _lms have an IR characteristic of AlN[ The region of high IR transmission was found to be between 1[4 and 01 mm[ 3[ Conclusions The AlN thin _lms produced in this study are polycrystalline with a smooth surface and a dense\ homogeneous microstructure[ The measured microhardness values of the grown layers are nor! mal for microcrystalline AlN[ The _lms are found to have good optical properties!refractive index\ extinction coe.cient and high transmission in the visible and IR regions\ depending on the deposition conditions[ The mentioned above results of this work con_rm the possi! bility for the production of AlN thin _lms with a polycrystalline microstructure\ good optical and mechanical characteristics by d[c[ reactive magnetron sputtering[ Further work is necessary to determine the in~uence of process parameters like nitrogen pressure\ current power and target!sub! strate distance on the composition\ structure\ morphology\ electrical\ mechanical and optical properties of the _lms[
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V. Dimitrova et al.: Aluminium nitride thin lms deposited by DC reactive magnetron sputtering
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