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Roberts - South Bay Technology Scott D. Walck , John T. Grant - Materials Directorate , Wright Lab, WPAFB, Ohio. Nestor J. Zaluzec - Materials Science Div., Argonne National Laboratory 36@d0dd0d@d0d3d0d@d0d6d0dG H_$ x( `\$LL+@d}Microstructural observations are not sufficient to characterize all the features which are encountered during characterization of materials. Using a combination of analytical spectroscopies such as XEDS, and EELS we can gain additional insight into the factors controlling or affecting materials properties beyond that which can be determined using standard imaging tools. During these analytical studies focussed probes are frequently employed to determine local compositions, however, subtle processes which involve the specimen, the electron beam and any mobile species on the sample surface frequently cause the build up of hydrocarbon contamination layers. O y@ddd}#@d}M5 ^dd Introduction    dd È G  (($ x( JhLE@d}While serving to indicate the location of the electron probe, the contamination obliterates the area of the specimen being analyzed and adversely affects all quantitative microanalysis methodologies. A variety of methods including: UV, electron beam flooding, heating and/or cooling can decrease the rate of contamination, however, none of these methods directly attack the source of specimen borne contamination. Research has shown that reactive gas plasmas may be used to clean both the specimen and stage for AEM, in this study we report on quantitative measurements of the reduction in contamination rates in an AEM as a function of operating conditions and plasma gases. @dddd@dddd@ddd}d}M5 ^dd Background    ddT(xG  ,D$ hx , Px@ 1 ?L2d}Example: The figure at the right shows the results of contamination formed when a 300 kV probe is focussed on the surface of a freshly electropolished 304 SS TEM specimen. The dark deposits mainly consist of hydrocarbons which diffuse across the surface of the specimen to the immediate vicinity of the electron probe. The amount of the contamination is a function of the time spent at each location. Here the time was varied from 15 - 300 seconds.   dddddd@d}d}@d}M[ nddNReactive Gas Plasma Processing Applications to Analytical Electron Microscopy NNNdd/ddA'G $ ( \ =] P h P8 0M5 ndd Experimental    ddZBddTEM specimens Electropolished 304 Stainless Steel Chemically polished Silicon Crushed CaZrTiO3 on Holey Carbon Film Microscopy Philips CM30T at ANL Materials Science Div. 300 kV, LaB6 Gun, 20 nm/0.7 nA probe RT DT Be Stage, LN2 Cold Trap Used EDAX PowerMX - XEDS System Gatan 666 PEELS System Plasma Cleaning System Model : PC-150 South Bay Technology Power: 10 W, Gas Pressure 200 mT. Gases: nominally pure Argon & Oxygen mixed as needed in Model 150  P cB@dd%dddd&dddd @dd,dd%dd#dddddddd@dd$dd"dd%dd(dddd G! (p\$ hx `\ P  ;5`@ p((M[ ndd Experimental    ddX u ddI0 ddLEsddQTo measure the rate of contamination we employed electron energy loss spectroscopy (EELS) and monitored the rate of change of the intensity of the zero loss (I0) to the total integrated intensity in the spectrum (IT). This ratio is directly proportional to the local thickness of the specimen. t = l * ln (Io// IT) l = mean free path Q6UQ@ddddL@dddddd'$b%&G#( $ hx ] N= ^ PK 8 PPM[ ndd Data Analysis    ddk N@d Individual Electron Energy Loss Spectra are measured as a function of time Spectra are then individually analyzed and the value of t/l is determined. The instantaneous contamination rate is given by d (t/l)/dT  $  L@dN@d<@d.+.hx,-G*/ P  ``J$ hx G rG Rư 2atddM[ ndd#Results from Electropolished 304 SSd ####dd8RUP dd Untreated     ddI5W ddArgon Proccessed - 5 min  ddJg ddOxygen Processed - 5 min  ddLC&@ddUntreated Specimens exhibit severe contamination Argon gas processing for 5 minutes @ 10 W/200 mT reduces the contamination rate ~ 50 x. Additional treatment of sample with pure Oxygen (5 minutes) reduces the contamination rate further to > 500x. pT1@ddddR@dd ddddo@dd52,=34G|16 P` 8 =KD avD4$ 8H ZX 0<6@PPP@H(@ TT@  H@X@\\@Hdd@\@\ZUf dd!After 5 minutes Argon Processing !!!!@dd*D< dd1After 5 minutes of additional Oxygen Processing 1111@ddMU+ ndd-Comparision Results on Electropolished 304 SS ----ddj ddUntreated Specimen @dd<9 K@:;GL8=  @ _$ hx G P@! (}*](b`$(}* Dt(  LM[ ndd#Results from Electropolished 304 SS? ####ddT dd 5 min Argon     dd( E dd 10 min Argon     dd dd 15 min Argon      dd* dd +5 min Oxygen     ddL] V@d0d#Successive 5 minute processing of the same specimen with Argon continuously reduces the contamination rate but does not completely eliminate the problem A final 5 minute treatement in pure Oxygen always reduced the rate to lower levels. Regardless of the length of time of Argon processing ###@d0dd0dd0d@d0dC@GABGD?D 80]$ hx F PPu H (]`(Pl(}*]XXM[ ndd(Results from Chemically Polished Silicon ((((dd: dd Untreated     ddev ddArgon Prccessede  dd  ddOxygen Processed   ddLUd0dInitial Contamination rates of Silicon are less than 304SS Argon alone is very efficient in Silicon Oxygen has a small but measurable effect and always reduces the contamination rate, however, the difference is much less than in 304 SS ;@d0dd0d)@d0dd0d@d0dJGWWHIGFK H$ hx  P  x (8(R<z zM[ ndd0Results from Crushed Zirconolite on Holey Carbon 0000dd0[ dd#Crushed Zirconolite on Holey Carbon ####d0d)u dd Untreated     dd)5 ddArgon Processed 5 mink  ddL+d0dnContamination of the Zirconolite is due to suspension of crushed mineral in solvents. A drop of the crushed mineral is then deposited on the H.C. film to make the sample. This leave organic residue on the sample and the Holey Carbon film. Argon treatment greatly reduces the contamination rate, a final treatment in pure Oxygen further decreases the problem. n! yn@d0dd0dy@d0dQNOPGMR x`p$ hx  P0H  ?M[ nddResults from Holey Carbon Filmse ddLC6@d0dTContamination of theHoley Carbon is due to suspension of crushed mineral in solvents. A drop of the crushed mineral is then deposited on the H.C. film to make the sample. This leave organic residue on the sample and the Holey Carbon film. Long processing (~ 15minutes) can effect the Holey Carbon support film and should be avoided. T_T@d0dd0dd0d_@d0dXU? ? ? ?VWGTY  D$ hx  PpP X F ( X(<~M[ nddGas Mixing Results ddc dd(Normalized Contamination Rate on Silicon ((((dd* ddArgon/Oxygen Mixture (50/50)  ddvD dd'Argon - 5 Minutes + Oxygen 5 MnustesA '' 'ddddL^d0dIn all cases tested the most effective cleaning occured when a two step process was carried out. 5 Min pure Argon followed by 5 Min pure Oxygen This was more effective and reduced the contamination rate more than using a Ar/O2 mixture (50/50)  a@d0dd0dd0dd0dd0dc@d0dd0d_\]^Gt[` hb@$ hx a P M[ nddHeating Effects of the Plasma ddLk@d0d-Using a conventional thermocouple in an AEM stage, the temperature rise of a SS sample and stage was measured as a function of input power to the plasma. Compared to a 150W flood lamp the increase in temperature is insignificant ~ 5-6 Co for the typical conditions used for cleaning (10 W @ 5 min). ->-@d0dd0d@d0dfc'8deGDbg  ޜ$ hx  P0h  ^ P@  0h 5U P=(`4@ !Kޤ03 dd Using XPS deposition of surface layers of material, were detected. This occurs only when cleaning conditions are set incorrectly.  d0d@d0dM[ nddAnalytical Results dds ddUsing XEDS & EELS in the AEM no measurable redeposition of plasma chamber materials or oxide formation was observed on the Silicon or SS samples. @d0dR8 dd'Silicon Sample after Ar & O2 Processing '    'ddddc dd2(Silicon Sample after Ar & O2 Processing (    ((dd2> dd O K = 532 eV      ddmj 5klGin $ hx ڼ ^ xxM[ ndd Conclusions    dd" fddeReactive Gas Plasmas are an effective means of mitigating the problem of hydrocarbon contamination in an AEM for a wide range of specimen types. When using a capacitive coupled parallel plate geometry optimal conditions are centered around a power rating of 10 W and a gas pressure of 200 mT at a DC bias ~ 40 V. The best results are obtained by using a 2 step processing of pure Argon followed by pure Oxygen for a time interval of 5 minutes each. No AEM detectable species are deposited on the specimen under cleaning conditions. 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